Non-Newtonian Electrolytes: A Sustainable Pathway to Improve Dye-Sensitized Solar Cell Technology by Enhancing Ionic Conductivity in the Electrolyte

Non-Newtonian Electrolytes: A Sustainable Pathway to Improve Dye-Sensitized Solar Cell Technology by Enhancing Ionic Conductivity in the Electrolyte | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article Non-Newtonian Electrolytes: A Sustainable Pathway to Improve Dye-Sensitized Solar Cell Technology by Enhancing Ionic Conductivity in the Electrolyte R. P. Chandrika, N. G. A. Karunathilaka, Kapila Wijayaratne, M. A. K. L. Dissanayake, and 3 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7956216/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 04 Apr, 2026 Read the published version in Journal of Materials Science: Materials in Electronics → Version 1 posted You are reading this latest preprint version Abstract This study explores the role of non-Newtonian gel-polymer electrolytes, infused with TiO 2 nanofillers, in improving the performance of dye-sensitized solar cells (DSSCs). The key focus was understanding how these nanofillers alter the electrolyte's ionic conductivity and influence the DSSC efficiency, and to study the transient nature of the conductivity in non-Newtonian electrolytes. By introducing TiO 2 nanofillers, the polymer chains undergo structural rearrangements, transitioning into a more amorphous state. This shift enhances ionic mobility within the electrolyte, a characteristic behavior of non-Newtonian fluids where viscosity and flow properties change under stress or temperature. This behavior is confirmed by analyzing the transient nature of the electrolyte’s conductivity. The FTIR and UV-Vis spectroscopy confirmed chemical stability and light-harvesting capability, respectively, without introducing unwanted reactions. The research found a distinct optimum in performance at 15.0 wt.% TiO 2 content beyond which the performance decreased due to nanoparticle aggregation and polymer chain immobilization. Key electrochemical analyses, including Nyquist plots and temperature-dependent conductivity measurements, reveal that ionic conductivity exhibits non-Arrhenius behavior, indicating complex, thermally activated transport within the gel matrix. The conductivity peaked at 9.73 mS cm − 1 at 80°C for the 15% TiO 2 sample, confirming the non-Newtonian dynamic nature of the electrolyte. AC conductivity, dielectric constant variations, and polarization microscopy provided further evidence of improved amorphous character and charge transport. In terms of DSSC performance, the electrolyte sample containing 15.0 wt.% TiO 2 yielded a power conversion efficiency (PCE) of 7.18%, a 26.0% increase over the TiO 2 -free baseline. This improvement is linked to increased iodide ion mobility, reduced charge recombination, longer electron diffusion lengths, and enhanced photoelectron lifetimes, as shown through EIS analysis. Conclusively, TiO 2 nanofiller–infused non-Newtonian gel-polymer electrolytes significantly enhance DSSC stability, conductivity, and efficiency. This work presents a viable pathway toward developing high-performance, stable, and sustainable solar cells using solid-state electrolyte technologies. Non-Newtonian Fluid Gel polymer electrolyte Ionic conductivity Nanofiller Composite Electrolyte Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 Figure 10 1.0 Introduction Non-Newtonian gel-polymer electrolytes (GPEs) can be utilized to improve the performance of dye-sensitized solar cells (DSSCs). The addition of nanofillers into such polymer electrolytes can enhance the electrolyte's ionic conductivity which can be utilized to improve the photovoltaic conversion efficiency of DSSCs [ , ]. The gel-polymer electrolytes used in DSSCs are primarily based on polymers such as polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), poly(methyl methacrylate) (PMMA), and polyacrylonitrile (PAN), which serve as polymer hosts combined with plasticizers or solvents. In general, with the introduction of nanofillers such as TiO 2 , SiO 2 or Al 2 O 3 the polymer chains undergo significant structural rearrangements, transitioning into a more amorphous state enhancing the ionic mobility within the electrolyte [ , ]. In addition, these electrolytes behave like non-Newtonian fluids [ , , , ]. Non-Newtonian fluids are materials whose viscosity varies in response to applied shear stress or shear rate, in contrast to Newtonian fluids that maintain a constant viscosity under all flow conditions and with time. This behavior arises due to structural rearrangements, molecular interactions, or time-dependent effects such as viscoelasticity and thixotropy. Common examples include household materials like ketchup, toothpaste, and paint, but these complex rheological properties are increasingly engineered into functional materials for energy devices such as photoelectrochemical solar cells, secondary batteries and super capacitors. Among the different types of non-Newtonian behaviors, shear-thinning (pseudoplastic), shear-thickening (dilatant), Bingham plastic, and thixotropic or rheopectic shear-thinning are particularly important for energy applications. These properties allow materials to flow more easily under mechanical stress during the assembly, while solidifying into a stable structure once fixed, making them ideal for use in gel-polymer electrolytes in dye-sensitized solar cells (DSSCs) [ , ]. Non-Newtonian electrolytes, typically found in quasi-solid-state or gel-polymer systems, exhibit dynamic flow properties influenced by temperature, electric fields, and mechanical agitation and they are time-varying. In DSSCs and other electrochemical devices, this tunable rheology offers some benefits: enhanced interfacial contact with porous electrodes, minimized leakage, and improved operational stability [ ]. Thixotropic gels, for instance, are solid-like at rest but liquefy under shear, allowing precise injection into solar cells during fabrication and re-solidification for long-term stability and portability. The incorporation of polymers in GPEs, such as PEO, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and poly(methyl methacrylate) (PMMA), often displays non-Newtonian behavior due to chain entanglement and ionic coordination [ , , ]. These systems are inherently stable and safer than liquid electrolytes, and particularly advantageous in portable and flexible DSSCs. Their pseudoplastic or thixotropic nature allows excellent mechanical integrity and ease of sealing during cell assembly [ ]. In addition, the performance of non-Newtonian electrolytes can be significantly enhanced by incorporating nanofillers. Materials such as titanium dioxide (TiO 2 ), silica (SiO 2 ), alumina (Al 2 O 3 ) and graphene oxide (GO) disrupt the polymer matrix, reduce crystallinity, and establish additional pathways for ionic transport. TiO 2 nanoparticles, in particular, are attractive due to their high surface area, dielectric constant, thermal stability, and chemical compatibility with the TiO 2 photoanode [ , ]. These properties promote better dye regeneration, reduce charge recombination, and facilitate uniform ion distribution. When introduced into GPEs, nanofiller improve ionic conductivity and mechanical strength through Lewis acid-base interactions and microstructural rearrangement [ , ]. The resulting nanocomposite electrolytes exhibit shear-thinning behavior, facilitating better penetration into porous photoanodes and more stable charge transport under operational conditions. The enhanced electrolyte-electrode interface contributes to reduced recombination losses and higher power conversion efficiency (PCE). Finally, when it comes to solar cells, photovoltaic (PV) technologies based on silicon dominate the market due to their high PCE (> 20%) [ ]. However, they suffer from energy-intensive fabrication, rigidity, and cost-related scalability issues [ ]. DSSCs, by contrast, offer an eco-friendly, low-cost alternative with decent efficiency, particularly in low-light environments. Since the groundbreaking work of O’Regan and Grätzel [ ], DSSCs have attracted extensive research attention, with over 30,800 publications recorded by October 2025 (Scopus). Despite the promise, liquid electrolytes traditionally used in DSSCs are prone to evaporation, leakage, and thermal degradation, compromising long-term reliability [ , , , ]. Non-Newtonian GPEs address these challenges by offering solid-like behavior at rest and fluidity during application. This not only enhances stability but also simplifies encapsulation processes, making DSSCs more practical for real-world applications [ ]. While more than 1,700 publications up to now focus on polymer electrolyte-based DSSCs, only a small fraction, 43 studies, cover the incorporation of nanofillers, with merely 12 specifically employing TiO 2 nanofillers (Scopus, October 2025). Nevertheless, the results are compelling: PCEs as high as 9.09% have been achieved using TiO 2 nanofillers with acrylonitrile-based polymers [ ]. The present work shows, a non-volatile, non-toxic PEO-based GPE incorporated with 13 nm TiO 2 nanoparticles demonstrates enhanced PCE and long-term device stability. This underscores the vast untapped potential of non-Newtonian nanocomposite electrolytes in fabricating efficient, scalable, and durable DSSCs. 2.0 Experimental Section 2.1 Preparation of Multi-Layer TiO 2 Photoanodes The DSSCs developed in this study were fabricated using highly porous, multi-layer TiO 2 photoanodes sensitized with commercially available ruthenium-based dye, N719 (Solaronix® SA). The photoanodes were constructed on fluorine-doped tin oxide (FTO) glass substrates (sheet resistance ~ 10 Ω cm − 2 ) by successive spin-coating of TiO 2 nanoparticle dispersions, followed by thermal annealing. The first photoanode layer was prepared by dispersing 0.5 g of TiO 2 nanoparticles (Evonik AEROXIDE® P90; avg. particle size: 13 nm) in 2 mL of 0.1 M HNO 3 . The resulting slurry was spin-coated onto pre-cleaned FTO glass at 2300 rpm for 2 minutes. After air drying for ~ 5 hours, the coated substrate was sintered at 450°C for 30 minutes. The same procedure was repeated to fabricate the second layer. To deposit the third layer, 0.5 g of TiO 2 nanoparticles with a relatively larger average particle size (21 nm; Evonik AEROXIDE® P25) was dispersed in 2 mL of 0.1 M HNO 3 . This dispersion was spin-coated at a relatively slower rate (1000 rpm for 2 minutes) and subsequently annealed at 450°C. Identical conditions were used to apply the fourth, fifth, and sixth layers, thereby forming a graded, multi-layer TiO 2 architecture as optimized in previous studies [ 2, ]. The assembled multilayer films were then immersed in a 0.5 mM ethanolic solution of N719 dye for 24 h to ensure complete sensitization. After dye adsorption, the photoanodes were rinsed with ethanol to remove any loosely bound dye or particulates. These sensitized anodes were later paired with platinum-coated counter electrodes, and a gel-polymer electrolyte was inserted between the two to complete the DSSC assembly. 2.2 Preparation of Gel-Polymer Electrolytes with TiO 2 Nanoparticles All reagents used in the preparation of the electrolytes were procured from Sigma-Aldrich® with purities above 99%. Lithium iodide (LiI) and tetrahexylammonium iodide (Hex 4 NI) were vacuum dried at ~ 50°C for 2 hours before use. The electrolyte was synthesized by sequentially mixing ethylene carbonate (EC), propylene carbonate (PC), 4-tert-butylpyridine (4TBP), 1-methyl-3-propylimidazolium iodide (MPII), Hex 4 NI, and LiI in a sealed vial, following a previously optimized method. The mixture was heated to 100°C, after which polyethylene oxide (PEO) was added and stirred until fully dissolved. Upon cooling to ~ 40°C, the respective amount of iodine (I 2 ) was added under continuous stirring to complete the redox gel polymer electrolyte formulation. The final electrolyte composition was based on the molar ratio: PEO(10):EC(40):PC(40):MPII(0.25):4TBP(0.85):Hex 4 NI(0.8):LiI(1.2):I 2 (0.2). To investigate the effect of nanofiller concentration, a series of gel-polymer electrolytes were prepared by incorporating TiO 2 nanoparticles (13 nm, Evonik AEROXIDE® P90) at concentrations ranging from 0.0 to 25.0 wt.%. These were added after PEO dissolution while the mixture was still warm and thoroughly stirred to ensure homogenous dispersion. The weight and weight percentage of the constituents of each sample are tabulated in Table 1 . Table 1 Composition of gel-polymer electrolyte samples with varying TiO₂ content. Electrolyte sample TiO₂ (wt.%) TiO₂ (mg) PEO (mg) A 0.00 0.00 50.00 B 5.00 2.50 47.50 C 10.00 5.00 45.00 D 15.00 7.50 42.50 E 20.00 10.00 40.00 F 25.00 12.50 37.50 2.3 Characterization Techniques The photovoltaic performance of the fabricated DSSCs was measured using a PEC-LO1 solar simulator under AM 1.5G illumination (1000 W m − 2 ) and a Peccell® potentiostat. The effective active area of each cell was 0.19 cm 2 . Current-voltage ( J - V ) characteristics were recorded under continuous light exposure. Electrochemical impedance spectroscopy (EIS) and DC polarization studies were carried out using a Metrohm® Autolab PGSTAT128N over a frequency range of 0.1 Hz to 1 MHz. These tests were conducted at temperatures from 20 to 80°C using gel-electrolyte discs (about 1 mm thick, 9 mm in diameter) sandwiched between stainless steel blocking electrodes. To measure the variation in conductivity over time, EIS measurements were taken immediately after preparing the electrolyte: every 5 minutes during the first 30 minutes, every 10 minutes during the second 30 minutes, every 15 minutes over the following two hours, and every 30 minutes during the subsequent hours. The final measurement was taken one hour after the previous measurement. These measurements were taken for the sample series. In total, EIS measurements for electrolyte samples were conducted over a period of 5 hours. To probe the chemical and morphological properties of the electrolytes, Fourier-transform infrared (FTIR) spectroscopy was performed using a JASCO® FT/IR-6700 spectrometer. Optical microscopy analysis was conducted using a ZEISS® AXIO Lab.A1 Polarizing Microscope. UV-Visible spectroscopy (Shimadzu UV-1800) was used to assess the optical absorbance of the gel electrolytes across the visible spectrum. 3.0 Results and Discussion This study explores the role of non-Newtonian gel-polymer electrolytes, infused with titanium dioxide (TiO 2 ) nanofillers, in improving the performance of DSSCs. Figure 1 shows photographic images of the gel-polymer electrolyte series with various amounts of added TiO 2 , in inverted bottles (a) after equilibrating for 6 h and (b) just after stirring for 3 minutes. The images confirm that the flow properties of the electrolytes depend on the mechanical disturbance given and the period given to equilibrate the sample. After equilibration, the electrolyte sample did not flow even when the bottles were inverted vertically. However, when mechanically disturbed by magnetic stirring, it began to flow slowly even when the bottles were inclined as shown in Fig. 1 , confirming the non-Newtonian behavior of the electrolyte. 3.1 Electric and Dielectric Properties Nyquist plots of the gel-polymer electrolyte series prepared by adding various amounts of TiO 2, are shown in Fig. 2 . Because of the high conductivity of the samples, only the linear part of the complex impedance is visible within the measurement frequency window. Inclined and slightly curved spikes specify a restricted diffusion in the transport process, in this electrochemical cell [ , ]. In particular, the inclined spike that arises from the limited movement of ions or reactants to the electrode surface can be due to the high viscosity of the samples. Furthermore, the results indicate that ion transport increases with rising temperature, which can be attributed to the enhancement of charge transport dynamics with increasing temperature. The temperature dependence of the conductivity is shown in Fig. 3 by plotting (a) conductivity Arrhenius plot and (b) the VTF (Vogel-Tammann-Fulcher) plot. Temperature-dependent conductivity measurements revealed that ionic transport follows non-Arrhenius behavior, indicating a complex, thermally activated ionic transport in the gel matrix. The conductivity variation exhibits the VTF behavior, as shown in Fig. 3 (b). It was revealed that the highest conductivity occurs at 15 wt% of TiO 2 composition. The conductivity peaked at 9.73 mS cm − 1 at 80°C for the 15.0% TiO 2 sample, confirming the non-Newtonian dynamic nature of the electrolyte. The ambient temperature conductivity of this sample is 4.58 mS cm − 1 . The gel-polymer electrolyte used in this study is based on PEO, which consists of a crystalline phase and an amorphous phase. However, by introducing TiO 2 nanofillers, the polymer chains could undergo structural rearrangements, increasing the amorphous phase content in the electrolyte. This structural change would have enhanced the ionic mobility within the gel electrolyte. Additionally, as shown in many previous studies, the conductivity in this type of nano-filler added electrolytes increases due to the formation of high conducting pathways for ions [ , , , ]. The gradual increase of conductivity up to 15.0 wt.% TiO 2 can be attributed to these two effects. However, higher TiO 2 loading may lead to nanoparticle agglomeration and cluster formation, thereby decreasing the ion mobility due to the blocking effect. An additional contribution could also come from the reduced effective gel electrolyte medium, thus reducing the overall ionic mobility [16]. AC conductivity and dielectric constant variations, and polarization microscopy were analyzed for the detailed characterization of this gel polymer electrolyte series. Complex AC Conductivity Generally, the AC conductivity has real and imaginary components. These components of conductivity in an electrolyte give information about polarization in the electrolyte. For instance, there can be dipole, ionic, electronic, space charge and electrode polarizations [ ,]. In addition, the ion transport and dielectric properties of an electrolyte depend on the dynamics of ions and dipoles in the electrolyte [ , , ]. Frequency dependence of the real part of the AC conductivity of the gel-polymer electrolyte series prepared by varying the amount of TiO 2 is given in Fig. 4 at different temperatures ranging from 20 ℃ to 80 ℃. The inset in Fig. 4 shows the low-frequency variation of the real part of the AC conductivity, revealing a characteristic exponential increase that reflects the underlying charge transport dynamics in this frequency range, which is not visible in the main curve. All the electrolytes show a similar behavior, reaching a plateau at higher frequencies and visibly another plateau at lower frequencies. The real part of the AC conductivity increases with the increase in frequency as a result of enhanced polarization dynamics with increasing frequency of the applied signal. The poor conductivity in the low-frequency dispersion region indicates electrode polarization, which arises from the accumulation of ions due to the slow periodic reversal of the applied electric field [ , ]. These polarization effects gradually diminish with increasing frequency. The upward shift of the curves with increasing temperature can also be attributed to the enhanced dynamics of ions and dipoles at elevated temperatures. At high frequencies, the AC conductivity approaches the DC plateau resulting from long-range diffusion of ions. These corresponding values closely match the DC conductivity extracted from Nyquist plot analysis, as illustrated in Fig. 3 (a). The AC conductivity values at 10 5 Hz for all electrolyte samples are tabulated in Table 2 . Table 2 AC conductivity values at 10 5 Hz for electrolyte samples A–F infused with TiO 2 nanofillers over a temperature range from 20℃ to 80℃. Temperature ( T ) AC conductivity at 10 5 Hz ( σ / mS cm − 1 ) T /℃ T /K TiO 2 NFs added gel-polymer electrolyte sample A B C D E F 20 293.15 1.18 1.37 1.49 1.61 1.61 1.38 30 303.15 1.34 1.68 1.72 1.92 1.77 1.47 40 313.15 1.65 1.89 2.05 2.27 2.05 1.59 50 323.15 1.91 2.11 2.38 2.58 2.31 1.79 60 333.15 2.13 2.39 2.66 2.84 2.54 2.02 70 343.15 2.35 2.64 2.93 3.15 2.70 2.32 80 353.15 2.57 2.91 3.13 3.39 2.85 2.55 The imaginary part of the AC conductivity ( σ ʺ) for all samples exhibits a clear frequency dependence (curves are given in supplementary Fig. S1 ). The σʺ exhibits a distinct peak as a function of frequency, which indicates a dielectric relaxation process within the electrolyte. This peak arises when the frequency of the applied electric field reaches the characteristic relaxation frequency of charge carriers or dipoles. The peak in σ ʺ emerges and grows, corresponding to a characteristic frequency f ₘₐₓ at which maximum electrode polarization occurs [38]. This peak is related to the maximum energy storage and delayed response, and in terms of conductivity, it is an energy loss process. A similar behavior is observed in all curves (a to f). σ ʺ shows a peak in the frequency range 1000 to 10,000 Hz, and the peak magnitude of σʺ increases systematically with rising temperature. When the charged species follows the frequency (at higher and lower frequencies), σʺ is minimum as seen in Fig. S1 . The σ ʺ peak is related to the frequency at which a specific charge transport mechanism becomes inefficient, while the capacitive (energy storage) contribution becomes most significant. Dielectric Properties The dielectric behavior and polarization effects of an electrolyte can be studied by analyzing the real ( ɛ ʹ) and imaginary ( ɛ ʺ) parts of the dielectric function. The real and imaginary parts of the dielectric function were calculated as described in the literature using complex impedance data [2]. The real part of the dielectric function for the gel-polymer electrolyte series, prepared with varying amounts of TiO 2 , is shown in Fig. 5 (a)–(f) as a function of frequency at different temperatures ranging from 20 to 80°C. The complex dielectric function ( ɛ ʺ (ω) = ɛ ʹ+ ɛ ʺ ) represents the energy stored in an electrolyte material while ɛ ʹ and ɛ ʺ are specifies polarization and energy loss as a function of the frequency of the applied electric field. The elevated ɛʹ observed at low frequencies in Fig. 5 is indicative of marked dielectric polarization behavior generally observed in polymer electrolyte systems. This polarization originates primarily from (i) the dissociation of the salt into free cations and anions, and (ii) the presence of polar ether (-O-) groups in the PEO matrix. The dissociated ions in the electrolyte contribute to electrode polarization as they migrate under an applied electric field and accumulate at the electrode–electrolyte interfaces due to the use of blocking electrodes, resulting in a space charge region. The ether groups in PEO undergo conformational reorientation in response to the electric field, leading to additional dipolar polarization. The combined effect of these two mechanisms accounts for the high dielectric constant shown at low frequencies. The ε ʺ represents the dielectric loss, which corresponds to the energy dissipated as heat when a material is subjected to an alternating electric field. The variation of the ε ʺ as a function of frequency for all samples is given in supplementary Fig. S2 . A peak in the ε ʺ versus frequency plot typically signifies the occurrence of a dielectric relaxation process, wherein the polarization mechanisms such as dipolar reorientation, interfacial charge accumulation, or ionic hopping fail to follow the oscillating electric field [38,39, ]. This mismatch results in maximum energy dissipation at a characteristic frequency, often referred to as the relaxation frequency ( f ₘ). The frequency at which ε ʺ reaches its maximum is of particular importance, as it provides quantitative insight into the dynamic behavior of charge carriers or dipoles within the material. Specifically, it is inversely related to the relaxation time ( τ = 1/2π f ₘ), thereby reflecting the time scale over which the system responds to changes in the applied field [ ]. In addition, ε ʺ peak helps to recognize the dominant polarization mechanism ranging from atomic, dipolar or molecular relaxation at high frequencies to space charge or interfacial (Maxwell–Wagner) polarization at lower frequencies, and electrode polarization at very low frequencies [ , ]. The f ₘ is sensitive to various material parameters, including temperature, microstructure, defect states, ionic mobility, and interfacial effects. Transient Nature of Conductivity. Figure 6 shows the time dependence of the ionic conductivity. The time-dependent conductivity of this polymer electrolyte exhibits an initial dramatic drop followed by a steady plateau, which reflects non-Newtonian, viscoelastic nature of the electrolyte. This type of behavior can be exhibited due to structural relaxation and ion mobility hindrance caused by restructuring of the ion-polymer network. In the initial stage (immediately after preparing the electrolyte), the system is in a non-equilibrium state, where a large number of free carriers contribute to ionic conductivity. However, with time (aging), ionic relaxation processes, such as ion pairing, cluster formation, and coordination with polar functional groups in the polymer matrix, can take place. This can reduce the number of mobile ions available for conduction and their mobility, causing a dramatic initial decline of conductivity as seen in Fig. 6. This behavior is analogous to that of non-Newtonian fluids, where viscosity (or in this case, ionic mobility) changes with time or shear. Similar to how non-Newtonian fluids exhibit time-dependent shear thinning or thickening, the polymer electrolyte exhibits a transient ionic conductivity response before reaching a dynamic equilibrium. The final stabilization of ionic conductivity shown in Fig. 6 reflects the system’s transition to a steady-state, where the polymer matrix and ion distribution reach a quasi-equilibrium. This behavior underscores the complex interplay between ionic transport and polymer chain dynamics in a non-Newtonian polymer electrolyte. 3.2 Surface Morphology of Electrolytes Non-Newtonian fluids are characterized by a viscosity that varies in response to applied shear stress or strain rate. In this electrolyte system, the viscosity manifests as either shear-thinning or shear-thickening, depending on the TiO 2 concentration and the structural dynamics of the polymer matrix. Figures 7 (a)–(f) show the polarization microscope images of the TiO 2 -infused gel polymer electrolyte samples (A, B, C, D, E, F), while Fig. 7 (g) depicts the polarizing image of the spherulites formed by lamellar structures of the pure PEO sample. The incorporation of TiO 2 nanoparticles influences the microstructure and rheological properties of the gel polymer electrolyte, modifying its viscoelastic and non-Newtonian characteristics. At the optimal TiO 2 concentration of 15 wt.% (Sample D), the electrolyte exhibited improved ionic conductivity, likely due to a more amorphous polymer phase and enhanced ion mobility facilitated by the nanoparticle-induced dynamic rearrangement of polymer chains. This concentration may represent a balance between the modifications in polymer chain dynamics caused by the filler and the formation of conductive ion pathways. When the TiO 2 content exceeds 15 wt.%, a decline in conductivity is observed, attributed to nanoparticle aggregation as seen in samples E and F, which can increase rigidity and restrict ion transport. In addition, reduction of rich polymer phase which contributes to the ion transport at higher TiO 2 content can decrees the conductivity. The non-Newtonian gel nature of the electrolyte allows dynamic rearrangement of the polymer-nanoparticle network under shear or stress, thereby enhancing interface contact and supporting stable ionic conduction in quasi-solid-state DSSCs. 3.3 FTIR and UV-Visible spectroscopy Figure 8 (a) shows the UV-Visible absorption spectra of the electrolyte series prepared with varying TiO 2 concentrations from 0% to 25%. The absorption edge of the TiO 2 nanoparticles appears near 400 nm, and the results are consistent with their wide bandgap properties. An increase in light absorption is observed with an increase in TiO 2 nanofiller content. Figure 8 (b) presents the FTIR spectra of the electrolyte series, obtained in the wavenumber range of 500–3000 cm − 1 . The spectra show characteristic vibrational modes associated with the organic solvents ethylene carbonate (EC) and propylene carbonate (PC) present in the electrolyte. In particular, the in-plane ring stretching, asymmetric ring stretching, and C-O stretching vibrations are observed at 714.50 cm − 1 , 1069.34 cm − 1 , and 1770.33 cm − 1 , respectively. The peaks at 772.35, 1158.04 cm − 1 , and 1388.49 cm − 1 correspond to out-of-plane ring bending, C-H wagging, and C-H rocking vibrations, respectively. No unexpected peaks attributable to undesired species or byproducts are detected, confirming the chemical integrity and compatibility of the electrolyte system. Characterization of DSSCs Figure 9 shows the variation of current density and power density with cell potential for DSSCs assembled with this new electrolyte series. Figure 9 (a) and (b), which present the photocurrent density and power density variation with cell potential, were utilized to calculate the key performance parameters such as open-circuit voltage ( V oc ), short-circuit current density ( J sc ), fill factor ( FF ), and power conversion efficiency (PCE). The values of the respective parameters of each cell are given in Table 3 . Notably, every tested cell achieved an efficiency of over 5%. The observed high efficiencies in the quasi-solid state solar cells can be attributed to the high ionic conductivity of the electrolytes. The solar cell containing electrolyte sample D (TiO 2 , 15.0 wt.%) showed the highest power conversion efficiency (PCE) of 7.18%, which is a 26.0% increase compared to the TiO 2 -free reference sample. This cell that contains electrolyte with 15.0% TiO 2 (Sample D), reaches a J sc of 13.02 mA cm - ², a V oc of 0.78 V and an FF of 0.71. Table 3 The photoelectrochemical parameters of all DSSCs. Sample V oc / V J sc / mA cm − 2 ff η / % A 0.71 12.17 0.66 5.70 B 0.73 12.28 0.66 5.94 C 0.76 11.51 0.74 6.51 D 0.78 13. 02 0.71 7.18 E 0.78 13.20 0.66 6.83 F 0.78 12.64 0.64 6.26 The solar cell performance enhancement achieved by modifying the electrolyte with TiO 2 nanofillers can be better understood by studying the conductivity behaviour of the electrolytes. For a clearer comparison, Fig. 10 illustrates the correlation between the conductivity of the various electrolytes and the PCE of the DSSCs using these electrolytes. As observed in Fig. 10 , the improvement in efficiency for the cells fabricated with the improved electrolytes generally follows the trend in conductivity. However, the relationship is not strictly linear or one-to-one since other minor effects, such as transport number iodide/triiodides etc, can also influence the results. Finally, it can be concluded that the ionic conductivity of non-Newtonian polar electrolytes can be significantly enhanced by incorporating TiO 2 nanofillers. This improvement in conductivity can, in turn, contribute to enhanced PCE in DSSCs. 4.0 Conclusions Non-Newtonian gel and polymer electrolytes, especially when enhanced with TiO 2 nanofillers, offer a promising route toward the realization of sustainable, flexible, and low-maintenance solar energy technologies. This study reveals the effectiveness of TiO 2 nanofiller-infused non-Newtonian gel polymer electrolytes in enhancing the performance of quasi-solid state DSSCs. By incorporating TiO 2 into a PEO-based polymer matrix, the polymer can transform into a more amorphous structure, significantly improving ionic mobility and overall electrolyte conductivity. An optimal TiO 2 content of 15 wt.% was identified, yielding a maximum PCE of 7.18%, which marks a 29.0% improvement over the filler-free electrolyte. It can be concluded, the incorporation of TiO 2 nanofillers enhances the ionic conductivity of non-Newtonian polar electrolytes, thereby improving the power conversion efficiency of DSSCs. Electrochemical and spectroscopic analyses confirmed improved charge transport, reduced recombination, and maintained chemical stability. These findings highlight the potential of non-Newtonian gel-polymer electrolytes as a promising approach for developing high-efficiency and stable solid-state DSSCs. Declarations Author Contribution R. P.; Methodology, Formal analysis, Data Collection, Investigation, Writing, preparing Graphs and Figures.N. G. A.; Conceptualization, Data Collection, Methodology, Formal analysis, Writing and Investigation. K. W.; Investigation, Formal analysis and Review & Editing.M. A. K. L.; Conceptualization, Methodology and Review & Editing.G. S.; Conceptualization, Review & Editing and Supervision.T. H. W.; Conceptualization, Review & Editing and Supervision.T. M. W. J.; Conceptualization, Methodology, Formal analysis, Investigation, Writing - Review & Editing, Supervision and Project administration Acknowledgments Financial assistance was provided by the Research Grant No. PGIS/2022/12 from the Post-graduate Institute of Science, University of Peradeniya, Sri Lanka. Data Availability Research data will be provided on request References Kanimozhi, G., Naresh, N., Kumar, H., & Satyanarayana, N. (2022). Review on the recent progress in the nanocomposite polymer electrolytes on the performance of lithium‐ion batteries. International Journal of Energy Research , 46 (6), 7137-7174. Chandrika, R. P., Gunathilaka, S. M. S., Liyanage, J. P., Wijayaratne, K., Kumara, G. R. A., Karunathilaka, N. G. A., Ajith DeSilva., L., & Bandara, T. M. W. J. (2024). Effect of titanium dioxide nanofillers on the properties of gel-polymer electrolytes and power conversion efficiency of dye-sensitized solar cells. Journal of Solid-State Electrochemistry , 1-20. 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6","display":"","copyAsset":false,"role":"figure","size":4418992,"visible":true,"origin":"","legend":"\u003cp\u003eConductivity variation of the electrolyte series with time after preparation (aging) of the sample.\u003c/p\u003e","description":"","filename":"Figure6.png","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/d1fef7c343a749844ea08cca.png"},{"id":96252901,"identity":"f8aa05a2-1ade-418c-8119-cf4475e04c91","added_by":"auto","created_at":"2025-11-19 07:41:38","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":16585639,"visible":true,"origin":"","legend":"\u003cp\u003e(a) – (f) Polarizing micrographs of electrolyte sample series (A, B, C, D, E, F), (g) Polarizing micrographs of pure PEO polymer sample.\u003c/p\u003e","description":"","filename":"Figure7.png","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/0109fb374834565e49c25b32.png"},{"id":96251642,"identity":"05e9b5e9-e5ef-48f0-ab53-9daeb6f254b2","added_by":"auto","created_at":"2025-11-19 07:39:52","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":2399197,"visible":true,"origin":"","legend":"\u003cp\u003e(a) UV-Visible absorbance spectroscopy of the gel polymer electrolyte series, (b) FTIR transmittance spectroscopy of the gel polymer electrolyte series.\u003c/p\u003e","description":"","filename":"Figure8F.png","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/285531e836c192fcc001bfa0.png"},{"id":96208035,"identity":"393eeb16-0037-40e8-b6f8-a26fb520edd6","added_by":"auto","created_at":"2025-11-18 17:49:23","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":3806246,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Current density variation with cell potential for DSSCs assembled with electrolyte sample series, (b) Power density variation with cell potential for DSSCs assembled with electrolyte sample series.\u003c/p\u003e","description":"","filename":"Figure9F.png","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/61b7e0b2b1d031df83c6b866.png"},{"id":96208059,"identity":"f5c8709f-4d04-46eb-a20a-dbb98d542344","added_by":"auto","created_at":"2025-11-18 17:49:24","extension":"png","order_by":10,"title":"Figure 10","display":"","copyAsset":false,"role":"figure","size":1696414,"visible":true,"origin":"","legend":"\u003cp\u003eComparison of the ionic conductivity of the electrolytes with the energy conversion efficiency of the DSSCs.\u003c/p\u003e","description":"","filename":"Figure10.png","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/b52bf0ed0e5177f96a7a2e7d.png"},{"id":106343891,"identity":"8d796e7e-fc5a-4722-a58c-6e20479937fb","added_by":"auto","created_at":"2026-04-07 16:10:39","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":47527764,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/6779577b-ee6b-4808-b272-b4592d580f4f.pdf"},{"id":96208037,"identity":"6f707379-0592-42ad-8056-ed30da3fcc59","added_by":"auto","created_at":"2025-11-18 17:49:23","extension":"tif","order_by":3,"title":"","display":"","copyAsset":false,"role":"supplement","size":5245746,"visible":true,"origin":"","legend":"","description":"","filename":"FigureS1.tif","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/f6a864c832b0d3a5c01001ab.tif"},{"id":96208039,"identity":"45dc4328-dd95-4f90-9a04-9965be452821","added_by":"auto","created_at":"2025-11-18 17:49:23","extension":"tif","order_by":4,"title":"","display":"","copyAsset":false,"role":"supplement","size":3237242,"visible":true,"origin":"","legend":"","description":"","filename":"FigureS2.tif","url":"https://assets-eu.researchsquare.com/files/rs-7956216/v1/979791ff800431c8dc9b528d.tif"}],"financialInterests":"No competing interests reported.","formattedTitle":"Non-Newtonian Electrolytes: A Sustainable Pathway to Improve Dye-Sensitized Solar Cell Technology by Enhancing Ionic Conductivity in the Electrolyte","fulltext":[{"header":"1.0 Introduction","content":"\u003cp\u003eNon-Newtonian gel-polymer electrolytes (GPEs) can be utilized to improve the performance of dye-sensitized solar cells (DSSCs). The addition of nanofillers into such polymer electrolytes can enhance the electrolyte's ionic conductivity which can be utilized to improve the photovoltaic conversion efficiency of DSSCs [\u003ca class=\"FNLink\" href=\"#Fn1\" id=\"#FNLinkFn1\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn2\" id=\"#FNLinkFn2\"\u003e\u003c/a\u003e]. The gel-polymer electrolytes used in DSSCs are primarily based on polymers such as polyethylene oxide (PEO), polyvinylidene fluoride (PVDF), poly(methyl methacrylate) (PMMA), and polyacrylonitrile (PAN), which serve as polymer hosts combined with plasticizers or solvents. In general, with the introduction of nanofillers such as TiO\u003csub\u003e2\u003c/sub\u003e, SiO\u003csub\u003e2\u003c/sub\u003e or Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e the polymer chains undergo significant structural rearrangements, transitioning into a more amorphous state enhancing the ionic mobility within the electrolyte [\u003ca class=\"FNLink\" href=\"#Fn3\" id=\"#FNLinkFn3\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn4\" id=\"#FNLinkFn4\"\u003e\u003c/a\u003e]. In addition, these electrolytes behave like non-Newtonian fluids [\u003ca class=\"FNLink\" href=\"#Fn5\" id=\"#FNLinkFn5\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn6\" id=\"#FNLinkFn6\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn7\" id=\"#FNLinkFn7\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn8\" id=\"#FNLinkFn8\"\u003e\u003c/a\u003e]. Non-Newtonian fluids are materials whose viscosity varies in response to applied shear stress or shear rate, in contrast to Newtonian fluids that maintain a constant viscosity under all flow conditions and with time. This behavior arises due to structural rearrangements, molecular interactions, or time-dependent effects such as viscoelasticity and thixotropy. Common examples include household materials like ketchup, toothpaste, and paint, but these complex rheological properties are increasingly engineered into functional materials for energy devices such as photoelectrochemical solar cells, secondary batteries and super capacitors.\u003c/p\u003e\u003cp\u003eAmong the different types of non-Newtonian behaviors, shear-thinning (pseudoplastic), shear-thickening (dilatant), Bingham plastic, and thixotropic or rheopectic shear-thinning are particularly important for energy applications. These properties allow materials to flow more easily under mechanical stress during the assembly, while solidifying into a stable structure once fixed, making them ideal for use in gel-polymer electrolytes in dye-sensitized solar cells (DSSCs) [\u003ca class=\"FNLink\" href=\"#Fn9\" id=\"#FNLinkFn9\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn10\" id=\"#FNLinkFn10\"\u003e\u003c/a\u003e].\u003c/p\u003e\u003cp\u003eNon-Newtonian electrolytes, typically found in quasi-solid-state or gel-polymer systems, exhibit dynamic flow properties influenced by temperature, electric fields, and mechanical agitation and they are time-varying. In DSSCs and other electrochemical devices, this tunable rheology offers some benefits: enhanced interfacial contact with porous electrodes, minimized leakage, and improved operational stability [\u003ca class=\"FNLink\" href=\"#Fn11\" id=\"#FNLinkFn11\"\u003e\u003c/a\u003e]. Thixotropic gels, for instance, are solid-like at rest but liquefy under shear, allowing precise injection into solar cells during fabrication and re-solidification for long-term stability and portability.\u003c/p\u003e\u003cp\u003eThe incorporation of polymers in GPEs, such as PEO, poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and poly(methyl methacrylate) (PMMA), often displays non-Newtonian behavior due to chain entanglement and ionic coordination [\u003ca class=\"FNLink\" href=\"#Fn12\" id=\"#FNLinkFn12\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn13\" id=\"#FNLinkFn13\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn14\" id=\"#FNLinkFn14\"\u003e\u003c/a\u003e]. These systems are inherently stable and safer than liquid electrolytes, and particularly advantageous in portable and flexible DSSCs. Their pseudoplastic or thixotropic nature allows excellent mechanical integrity and ease of sealing during cell assembly [\u003ca class=\"FNLink\" href=\"#Fn15\" id=\"#FNLinkFn15\"\u003e\u003c/a\u003e]. In addition, the performance of non-Newtonian electrolytes can be significantly enhanced by incorporating nanofillers. Materials such as titanium dioxide (TiO\u003csub\u003e2\u003c/sub\u003e), silica (SiO\u003csub\u003e2\u003c/sub\u003e), alumina (Al\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e) and graphene oxide (GO) disrupt the polymer matrix, reduce crystallinity, and establish additional pathways for ionic transport. TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles, in particular, are attractive due to their high surface area, dielectric constant, thermal stability, and chemical compatibility with the TiO\u003csub\u003e2\u003c/sub\u003e photoanode [\u003ca class=\"FNLink\" href=\"#Fn16\" id=\"#FNLinkFn16\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn17\" id=\"#FNLinkFn17\"\u003e\u003c/a\u003e]. These properties promote better dye regeneration, reduce charge recombination, and facilitate uniform ion distribution. When introduced into GPEs, nanofiller improve ionic conductivity and mechanical strength through Lewis acid-base interactions and microstructural rearrangement [\u003ca class=\"FNLink\" href=\"#Fn18\" id=\"#FNLinkFn18\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn19\" id=\"#FNLinkFn19\"\u003e\u003c/a\u003e]. The resulting nanocomposite electrolytes exhibit shear-thinning behavior, facilitating better penetration into porous photoanodes and more stable charge transport under operational conditions. The enhanced electrolyte-electrode interface contributes to reduced recombination losses and higher power conversion efficiency (PCE).\u003c/p\u003e\u003cp\u003eFinally, when it comes to solar cells, photovoltaic (PV) technologies based on silicon dominate the market due to their high PCE (\u0026gt;\u0026thinsp;20%) [\u003ca class=\"FNLink\" href=\"#Fn20\" id=\"#FNLinkFn20\"\u003e\u003c/a\u003e]. However, they suffer from energy-intensive fabrication, rigidity, and cost-related scalability issues [\u003ca class=\"FNLink\" href=\"#Fn21\" id=\"#FNLinkFn21\"\u003e\u003c/a\u003e]. DSSCs, by contrast, offer an eco-friendly, low-cost alternative with decent efficiency, particularly in low-light environments. Since the groundbreaking work of O\u0026rsquo;Regan and Gr\u0026auml;tzel [\u003ca class=\"FNLink\" href=\"#Fn22\" id=\"#FNLinkFn22\"\u003e\u003c/a\u003e], DSSCs have attracted extensive research attention, with over 30,800 publications recorded by October 2025 (Scopus). Despite the promise, liquid electrolytes traditionally used in DSSCs are prone to evaporation, leakage, and thermal degradation, compromising long-term reliability [\u003ca class=\"FNLink\" href=\"#Fn23\" id=\"#FNLinkFn23\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn24\" id=\"#FNLinkFn24\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn25\" id=\"#FNLinkFn25\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn26\" id=\"#FNLinkFn26\"\u003e\u003c/a\u003e]. Non-Newtonian GPEs address these challenges by offering solid-like behavior at rest and fluidity during application. This not only enhances stability but also simplifies encapsulation processes, making DSSCs more practical for real-world applications [\u003ca class=\"FNLink\" href=\"#Fn27\" id=\"#FNLinkFn27\"\u003e\u003c/a\u003e]. While more than 1,700 publications up to now focus on polymer electrolyte-based DSSCs, only a small fraction, 43 studies, cover the incorporation of nanofillers, with merely 12 specifically employing TiO\u003csub\u003e2\u003c/sub\u003e nanofillers (Scopus, October 2025). Nevertheless, the results are compelling: PCEs as high as 9.09% have been achieved using TiO\u003csub\u003e2\u003c/sub\u003e nanofillers with acrylonitrile-based polymers [\u003ca class=\"FNLink\" href=\"#Fn28\" id=\"#FNLinkFn28\"\u003e\u003c/a\u003e]. The present work shows, a non-volatile, non-toxic PEO-based GPE incorporated with 13 nm TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles demonstrates enhanced PCE and long-term device stability. This underscores the vast untapped potential of non-Newtonian nanocomposite electrolytes in fabricating efficient, scalable, and durable DSSCs.\u003c/p\u003e"},{"header":"2.0 Experimental Section","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003ch2\u003e2.1 Preparation of Multi-Layer TiO\u003csub\u003e2\u003c/sub\u003e Photoanodes\u003c/h2\u003e\u003cp\u003eThe DSSCs developed in this study were fabricated using highly porous, multi-layer TiO\u003csub\u003e2\u003c/sub\u003e photoanodes sensitized with commercially available ruthenium-based dye, N719 (Solaronix\u0026reg; SA). The photoanodes were constructed on fluorine-doped tin oxide (FTO) glass substrates (sheet resistance\u0026thinsp;~\u0026thinsp;10 Ω cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e) by successive spin-coating of TiO\u003csub\u003e2\u003c/sub\u003e nanoparticle dispersions, followed by thermal annealing. The first photoanode layer was prepared by dispersing 0.5 g of TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles (Evonik AEROXIDE\u0026reg; P90; avg. particle size: 13 nm) in 2 mL of 0.1 M HNO\u003csub\u003e3\u003c/sub\u003e. The resulting slurry was spin-coated onto pre-cleaned FTO glass at 2300 rpm for 2 minutes. After air drying for ~\u0026thinsp;5 hours, the coated substrate was sintered at 450\u0026deg;C for 30 minutes. The same procedure was repeated to fabricate the second layer. To deposit the third layer, 0.5 g of TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles with a relatively larger average particle size (21 nm; Evonik AEROXIDE\u0026reg; P25) was dispersed in 2 mL of 0.1 M HNO\u003csub\u003e3\u003c/sub\u003e. This dispersion was spin-coated at a relatively slower rate (1000 rpm for 2 minutes) and subsequently annealed at 450\u0026deg;C. Identical conditions were used to apply the fourth, fifth, and sixth layers, thereby forming a graded, multi-layer TiO\u003csub\u003e2\u003c/sub\u003e architecture as optimized in previous studies [ 2,\u003ca class=\"FNLink\" href=\"#Fn29\" id=\"#FNLinkFn29\"\u003e\u003c/a\u003e].\u003c/p\u003e\u003cp\u003eThe assembled multilayer films were then immersed in a 0.5 mM ethanolic solution of N719 dye for 24 h to ensure complete sensitization. After dye adsorption, the photoanodes were rinsed with ethanol to remove any loosely bound dye or particulates. These sensitized anodes were later paired with platinum-coated counter electrodes, and a gel-polymer electrolyte was inserted between the two to complete the DSSC assembly.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\u003ch2\u003e2.2 Preparation of Gel-Polymer Electrolytes with TiO\u003csub\u003e2\u003c/sub\u003e Nanoparticles\u003c/h2\u003e\u003cp\u003eAll reagents used in the preparation of the electrolytes were procured from Sigma-Aldrich\u0026reg; with purities above 99%. Lithium iodide (LiI) and tetrahexylammonium iodide (Hex\u003csub\u003e4\u003c/sub\u003eNI) were vacuum dried at ~\u0026thinsp;50\u0026deg;C for 2 hours before use. The electrolyte was synthesized by sequentially mixing ethylene carbonate (EC), propylene carbonate (PC), 4-tert-butylpyridine (4TBP), 1-methyl-3-propylimidazolium iodide (MPII), Hex\u003csub\u003e4\u003c/sub\u003eNI, and LiI in a sealed vial, following a previously optimized method. The mixture was heated to 100\u0026deg;C, after which polyethylene oxide (PEO) was added and stirred until fully dissolved. Upon cooling to ~\u0026thinsp;40\u0026deg;C, the respective amount of iodine (I\u003csub\u003e2\u003c/sub\u003e) was added under continuous stirring to complete the redox gel polymer electrolyte formulation. The final electrolyte composition was based on the molar ratio: PEO(10):EC(40):PC(40):MPII(0.25):4TBP(0.85):Hex\u003csub\u003e4\u003c/sub\u003eNI(0.8):LiI(1.2):I\u003csub\u003e2\u003c/sub\u003e(0.2).\u003c/p\u003e\u003cp\u003eTo investigate the effect of nanofiller concentration, a series of gel-polymer electrolytes were prepared by incorporating TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles (13 nm, Evonik AEROXIDE\u0026reg; P90) at concentrations ranging from 0.0 to 25.0 wt.%. These were added after PEO dissolution while the mixture was still warm and thoroughly stirred to ensure homogenous dispersion. The weight and weight percentage of the constituents of each sample are tabulated in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e.\u003c/p\u003e\u003cp\u003e\u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab1\" border=\"1\"\u003e\u003ccaption language=\"En\"\u003e\u003cdiv class=\"CaptionNumber\"\u003eTable 1\u003c/div\u003e\u003cdiv class=\"CaptionContent\"\u003e\u003cp\u003eComposition of gel-polymer electrolyte samples with varying TiO₂ content.\u003c/p\u003e\u003c/div\u003e\u003c/caption\u003e\u003ccolgroup cols=\"4\"\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u003cp\u003eElectrolyte sample\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003eTiO₂ (wt.%)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003eTiO₂ (mg)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c4\"\u003e\u003cp\u003ePEO (mg)\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eA\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e0.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e50.00\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eB\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e5.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e2.50\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e47.50\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eC\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e10.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e5.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e45.00\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eD\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e15.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e7.50\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e42.50\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e20.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e10.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e40.00\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eF\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e25.00\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e12.50\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e37.50\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\u003ch2\u003e2.3 Characterization Techniques\u003c/h2\u003e\u003cp\u003eThe photovoltaic performance of the fabricated DSSCs was measured using a PEC-LO1 solar simulator under AM 1.5G illumination (1000 W m\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e) and a Peccell\u0026reg; potentiostat. The effective active area of each cell was 0.19 cm\u003csup\u003e2\u003c/sup\u003e. Current-voltage (\u003cem\u003eJ\u003c/em\u003e-\u003cem\u003eV\u003c/em\u003e) characteristics were recorded under continuous light exposure. Electrochemical impedance spectroscopy (EIS) and DC polarization studies were carried out using a Metrohm\u0026reg; Autolab PGSTAT128N over a frequency range of 0.1 Hz to 1 MHz. These tests were conducted at temperatures from 20 to 80\u0026deg;C using gel-electrolyte discs (about 1 mm thick, 9 mm in diameter) sandwiched between stainless steel blocking electrodes.\u003c/p\u003e\u003cp\u003eTo measure the variation in conductivity over time, EIS measurements were taken immediately after preparing the electrolyte: every 5 minutes during the first 30 minutes, every 10 minutes during the second 30 minutes, every 15 minutes over the following two hours, and every 30 minutes during the subsequent hours. The final measurement was taken one hour after the previous measurement. These measurements were taken for the sample series. In total, EIS measurements for electrolyte samples were conducted over a period of 5 hours.\u003c/p\u003e\u003cp\u003eTo probe the chemical and morphological properties of the electrolytes, Fourier-transform infrared (FTIR) spectroscopy was performed using a JASCO\u0026reg; FT/IR-6700 spectrometer. Optical microscopy analysis was conducted using a ZEISS\u0026reg; AXIO Lab.A1 Polarizing Microscope. UV-Visible spectroscopy (Shimadzu UV-1800) was used to assess the optical absorbance of the gel electrolytes across the visible spectrum.\u003c/p\u003e\u003c/div\u003e"},{"header":"3.0 Results and Discussion","content":"\u003cp\u003eThis study explores the role of non-Newtonian gel-polymer electrolytes, infused with titanium dioxide (TiO\u003csub\u003e2\u003c/sub\u003e) nanofillers, in improving the performance of DSSCs. Figure\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e shows photographic images of the gel-polymer electrolyte series with various amounts of added TiO\u003csub\u003e2\u003c/sub\u003e, in inverted bottles (a) after equilibrating for 6 h and (b) just after stirring for 3 minutes. The images confirm that the flow properties of the electrolytes depend on the mechanical disturbance given and the period given to equilibrate the sample. After equilibration, the electrolyte sample did not flow even when the bottles were inverted vertically. However, when mechanically disturbed by magnetic stirring, it began to flow slowly even when the bottles were inclined as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, confirming the non-Newtonian behavior of the electrolyte.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cdiv id=\"Sec7\" class=\"Section2\"\u003e\u003ch2\u003e3.1 Electric and Dielectric Properties\u003c/h2\u003e\u003cp\u003eNyquist plots of the gel-polymer electrolyte series prepared by adding various amounts of TiO\u003csub\u003e2,\u003c/sub\u003e are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. Because of the high conductivity of the samples, only the linear part of the complex impedance is visible within the measurement frequency window. Inclined and slightly curved spikes specify a restricted diffusion in the transport process, in this electrochemical cell [\u003ca class=\"FNLink\" href=\"#Fn30\" id=\"#FNLinkFn30\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn31\" id=\"#FNLinkFn31\"\u003e\u003c/a\u003e]. In particular, the inclined spike that arises from the limited movement of ions or reactants to the electrode surface can be due to the high viscosity of the samples. Furthermore, the results indicate that ion transport increases with rising temperature, which can be attributed to the enhancement of charge transport dynamics with increasing temperature.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe temperature dependence of the conductivity is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e by plotting (a) conductivity Arrhenius plot and (b) the VTF (Vogel-Tammann-Fulcher) plot. Temperature-dependent conductivity measurements revealed that ionic transport follows non-Arrhenius behavior, indicating a complex, thermally activated ionic transport in the gel matrix. The conductivity variation exhibits the VTF behavior, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(b). It was revealed that the highest conductivity occurs at 15 wt% of TiO\u003csub\u003e2\u003c/sub\u003e composition. The conductivity peaked at 9.73 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 80\u0026deg;C for the 15.0% TiO\u003csub\u003e2\u003c/sub\u003e sample, confirming the non-Newtonian dynamic nature of the electrolyte. The ambient temperature conductivity of this sample is 4.58 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. The gel-polymer electrolyte used in this study is based on PEO, which consists of a crystalline phase and an amorphous phase. However, by introducing TiO\u003csub\u003e2\u003c/sub\u003e nanofillers, the polymer chains could undergo structural rearrangements, increasing the amorphous phase content in the electrolyte. This structural change would have enhanced the ionic mobility within the gel electrolyte. Additionally, as shown in many previous studies, the conductivity in this type of nano-filler added electrolytes increases due to the formation of high conducting pathways for ions [\u003ca class=\"FNLink\" href=\"#Fn32\" id=\"#FNLinkFn32\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn33\" id=\"#FNLinkFn33\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn34\" id=\"#FNLinkFn34\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn35\" id=\"#FNLinkFn35\"\u003e\u003c/a\u003e]. The gradual increase of conductivity up to 15.0 wt.% TiO\u003csub\u003e2\u003c/sub\u003e can be attributed to these two effects. However, higher TiO\u003csub\u003e2\u003c/sub\u003e loading may lead to nanoparticle agglomeration and cluster formation, thereby decreasing the ion mobility due to the blocking effect. An additional contribution could also come from the reduced effective gel electrolyte medium, thus reducing the overall ionic mobility [16]. AC conductivity and dielectric constant variations, and polarization microscopy were analyzed for the detailed characterization of this gel polymer electrolyte series.\u003c/p\u003e\u003cp\u003e\u003cem\u003eComplex AC Conductivity\u003c/em\u003e\u003c/p\u003e\u003cp\u003eGenerally, the AC conductivity has real and imaginary components. These components of conductivity in an electrolyte give information about polarization in the electrolyte. For instance, there can be dipole, ionic, electronic, space charge and electrode polarizations [\u003ca class=\"FNLink\" href=\"#Fn36\" id=\"#FNLinkFn36\"\u003e\u003c/a\u003e,]. In addition, the ion transport and dielectric properties of an electrolyte depend on the dynamics of ions and dipoles in the electrolyte [\u003ca class=\"FNLink\" href=\"#Fn37\" id=\"#FNLinkFn37\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn38\" id=\"#FNLinkFn38\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn39\" id=\"#FNLinkFn39\"\u003e\u003c/a\u003e]. Frequency dependence of the real part of the AC conductivity of the gel-polymer electrolyte series prepared by varying the amount of TiO\u003csub\u003e2\u003c/sub\u003e is given in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e at different temperatures ranging from 20 ℃ to 80 ℃. The inset in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e shows the low-frequency variation of the real part of the AC conductivity, revealing a characteristic exponential increase that reflects the underlying charge transport dynamics in this frequency range, which is not visible in the main curve.\u003c/p\u003e\u003cp\u003eAll the electrolytes show a similar behavior, reaching a plateau at higher frequencies and visibly another plateau at lower frequencies. The real part of the AC conductivity increases with the increase in frequency as a result of enhanced polarization dynamics with increasing frequency of the applied signal. The poor conductivity in the low-frequency dispersion region indicates electrode polarization, which arises from the accumulation of ions due to the slow periodic reversal of the applied electric field [\u003ca class=\"FNLink\" href=\"#Fn40\" id=\"#FNLinkFn40\"\u003e\u003c/a\u003e,\u003ca class=\"FNLink\" href=\"#Fn41\" id=\"#FNLinkFn41\"\u003e\u003c/a\u003e]. These polarization effects gradually diminish with increasing frequency. The upward shift of the curves with increasing temperature can also be attributed to the enhanced dynamics of ions and dipoles at elevated temperatures. At high frequencies, the AC conductivity approaches the DC plateau resulting from long-range diffusion of ions. These corresponding values closely match the DC conductivity extracted from Nyquist plot analysis, as illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e(a). The AC conductivity values at 10\u003csup\u003e5\u003c/sup\u003e Hz for all electrolyte samples are tabulated in Table\u0026nbsp;\u003cspan refid=\"Tab2\" class=\"InternalRef\"\u003e2\u003c/span\u003e.\u003c/p\u003e\u003cp\u003e\u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab2\" border=\"1\"\u003e\u003ccaption language=\"En\"\u003e\u003cdiv class=\"CaptionNumber\"\u003eTable 2\u003c/div\u003e\u003cdiv class=\"CaptionContent\"\u003e\u003cp\u003eAC conductivity values at 10\u003csup\u003e5\u003c/sup\u003e Hz for electrolyte samples A\u0026ndash;F infused with TiO\u003csub\u003e2\u003c/sub\u003e nanofillers over a temperature range from 20℃ to 80℃.\u003c/p\u003e\u003c/div\u003e\u003c/caption\u003e\u003ccolgroup cols=\"8\"\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c8\" colnum=\"8\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colspan=\"2\" nameend=\"c2\" namest=\"c1\"\u003e\u003cp\u003eTemperature (\u003cem\u003eT\u003c/em\u003e)\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colspan=\"6\" nameend=\"c8\" namest=\"c3\"\u003e\u003cp\u003eAC conductivity at 10\u003csup\u003e5\u003c/sup\u003e Hz (\u003cem\u003eσ\u003c/em\u003e / mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\" morerows=\"1\" rowspan=\"2\"\u003e\u003cp\u003e\u003cem\u003eT\u003c/em\u003e/℃\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\" morerows=\"1\" rowspan=\"2\"\u003e\u003cp\u003e\u003cem\u003eT\u003c/em\u003e/K\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colspan=\"6\" nameend=\"c8\" namest=\"c3\"\u003e\u003cp\u003eTiO\u003csub\u003e2\u003c/sub\u003e NFs added gel-polymer electrolyte sample\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003eA\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003eB\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003eC\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003eD\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003eE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003eF\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e20\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e293.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1.18\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e1.37\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e1.49\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e1.61\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e1.61\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e1.38\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e30\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e303.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1.34\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e1.68\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e1.72\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e1.92\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e1.77\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e1.47\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e40\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e313.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1.65\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e1.89\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e2.05\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e2.27\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e2.05\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e1.59\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e50\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e323.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e1.91\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e2.11\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e2.38\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e2.58\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e2.31\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e1.79\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e60\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e333.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e2.13\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e2.39\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e2.66\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e2.84\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e2.54\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e2.02\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e70\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e343.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e2.35\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e2.64\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e2.93\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e3.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e2.70\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e2.32\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003e80\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c2\"\u003e\u003cp\u003e353.15\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c3\"\u003e\u003cp\u003e2.57\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c4\"\u003e\u003cp\u003e2.91\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c5\"\u003e\u003cp\u003e3.13\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c6\"\u003e\u003cp\u003e3.39\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c7\"\u003e\u003cp\u003e2.85\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"left\" colname=\"c8\"\u003e\u003cp\u003e2.55\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eThe imaginary part of the AC conductivity (\u003cem\u003eσ\u003c/em\u003eʺ) for all samples exhibits a clear frequency dependence (curves are given in supplementary Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e). The \u003cem\u003eσʺ\u003c/em\u003e exhibits a distinct peak as a function of frequency, which indicates a dielectric relaxation process within the electrolyte. This peak arises when the frequency of the applied electric field reaches the characteristic relaxation frequency of charge carriers or dipoles. The peak in \u003cem\u003eσ\u003c/em\u003eʺ emerges and grows, corresponding to a characteristic frequency \u003cem\u003ef\u003c/em\u003eₘₐₓ at which maximum electrode polarization occurs [38]. This peak is related to the maximum energy storage and delayed response, and in terms of conductivity, it is an energy loss process. A similar behavior is observed in all curves (a to f). \u003cem\u003eσ\u003c/em\u003eʺ shows a peak in the frequency range 1000 to 10,000 Hz, and the peak magnitude of \u003cem\u003eσʺ\u003c/em\u003e increases systematically with rising temperature. When the charged species follows the frequency (at higher and lower frequencies), \u003cem\u003eσʺ\u003c/em\u003e is minimum as seen in Fig. \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e. The \u003cem\u003eσ\u003c/em\u003eʺ peak is related to the frequency at which a specific charge transport mechanism becomes inefficient, while the capacitive (energy storage) contribution becomes most significant.\u003c/p\u003e\u003cp\u003e\u003cem\u003eDielectric Properties\u003c/em\u003e\u003c/p\u003e\u003cp\u003eThe dielectric behavior and polarization effects of an electrolyte can be studied by analyzing the real (\u003cem\u003eɛ\u003c/em\u003eʹ) and imaginary (\u003cem\u003eɛ\u003c/em\u003eʺ) parts of the dielectric function. The real and imaginary parts of the dielectric function were calculated as described in the literature using complex impedance data [2]. The real part of the dielectric function for the gel-polymer electrolyte series, prepared with varying amounts of TiO\u003csub\u003e2\u003c/sub\u003e, is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e(a)\u0026ndash;(f) as a function of frequency at different temperatures ranging from 20 to 80\u0026deg;C. The complex dielectric function (\u003cem\u003eɛ\u003c/em\u003eʺ\u003csub\u003e(ω) =\u003c/sub\u003e \u003cem\u003eɛ\u003c/em\u003eʹ+\u003cem\u003eɛ\u003c/em\u003eʺ\u003cem\u003e)\u003c/em\u003e represents the energy stored in an electrolyte material while \u003cem\u003eɛ\u003c/em\u003eʹ and \u003cem\u003eɛ\u003c/em\u003eʺ are specifies polarization and energy loss as a function of the frequency of the applied electric field.\u003c/p\u003e\u003cp\u003eThe elevated \u003cem\u003eɛʹ\u003c/em\u003e observed at low frequencies in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e is indicative of marked dielectric polarization behavior generally observed in polymer electrolyte systems. This polarization originates primarily from (i) the dissociation of the salt into free cations and anions, and (ii) the presence of polar ether (-O-) groups in the PEO matrix. The dissociated ions in the electrolyte contribute to electrode polarization as they migrate under an applied electric field and accumulate at the electrode\u0026ndash;electrolyte interfaces due to the use of blocking electrodes, resulting in a space charge region. The ether groups in PEO undergo conformational reorientation in response to the electric field, leading to additional dipolar polarization. The combined effect of these two mechanisms accounts for the high dielectric constant shown at low frequencies.\u003c/p\u003e\u003cp\u003eThe \u003cem\u003eε\u003c/em\u003eʺ represents the dielectric loss, which corresponds to the energy dissipated as heat when a material is subjected to an alternating electric field. The variation of the \u003cem\u003eε\u003c/em\u003eʺ as a function of frequency for all samples is given in supplementary Fig. \u003cspan refid=\"MOESM2\" class=\"InternalRef\"\u003eS2\u003c/span\u003e. A peak in the \u003cem\u003eε\u003c/em\u003eʺ versus frequency plot typically signifies the occurrence of a dielectric relaxation process, wherein the polarization mechanisms such as dipolar reorientation, interfacial charge accumulation, or ionic hopping fail to follow the oscillating electric field [38,39,\u003ca class=\"FNLink\" href=\"#Fn42\" id=\"#FNLinkFn42\"\u003e\u003c/a\u003e]. This mismatch results in maximum energy dissipation at a characteristic frequency, often referred to as the relaxation frequency (\u003cem\u003ef\u003c/em\u003eₘ). The frequency at which \u003cem\u003eε\u003c/em\u003eʺ reaches its maximum is of particular importance, as it provides quantitative insight into the dynamic behavior of charge carriers or dipoles within the material. Specifically, it is inversely related to the relaxation time (\u003cem\u003eτ\u003c/em\u003e\u0026thinsp;=\u0026thinsp;1/2π\u003cem\u003ef\u003c/em\u003eₘ), thereby reflecting the time scale over which the system responds to changes in the applied field [\u003ca class=\"FNLink\" href=\"#Fn43\" id=\"#FNLinkFn43\"\u003e\u003c/a\u003e]. In addition, \u003cem\u003eε\u003c/em\u003eʺ peak helps to recognize the dominant polarization mechanism ranging from atomic, dipolar or molecular relaxation at high frequencies to space charge or interfacial (Maxwell\u0026ndash;Wagner) polarization at lower frequencies, and electrode polarization at very low frequencies [\u003ca class=\"FNLink\" href=\"#Fn44\" id=\"#FNLinkFn44\"\u003e\u003c/a\u003e, \u003ca class=\"FNLink\" href=\"#Fn45\" id=\"#FNLinkFn45\"\u003e\u003c/a\u003e]. The \u003cem\u003ef\u003c/em\u003eₘ is sensitive to various material parameters, including temperature, microstructure, defect states, ionic mobility, and interfacial effects.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cem\u003eTransient Nature of Conductivity.\u003c/em\u003e\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eFigure 6 shows the time dependence of the ionic conductivity. The time-dependent conductivity of this polymer electrolyte exhibits an initial dramatic drop followed by a steady plateau, which reflects non-Newtonian, viscoelastic nature of the electrolyte. This type of behavior can be exhibited due to structural relaxation and ion mobility hindrance caused by restructuring of the ion-polymer network. In the initial stage (immediately after preparing the electrolyte), the system is in a non-equilibrium state, where a large number of free carriers contribute to ionic conductivity. However, with time (aging), ionic relaxation processes, such as ion pairing, cluster formation, and coordination with polar functional groups in the polymer matrix, can take place. This can reduce the number of mobile ions available for conduction and their mobility, causing a dramatic initial decline of conductivity as seen in Fig.\u0026nbsp;6. This behavior is analogous to that of non-Newtonian fluids, where viscosity (or in this case, ionic mobility) changes with time or shear. Similar to how non-Newtonian fluids exhibit time-dependent shear thinning or thickening, the polymer electrolyte exhibits a transient ionic conductivity response before reaching a dynamic equilibrium. The final stabilization of ionic conductivity shown in Fig.\u0026nbsp;6 reflects the system\u0026rsquo;s transition to a steady-state, where the polymer matrix and ion distribution reach a quasi-equilibrium. This behavior underscores the complex interplay between ionic transport and polymer chain dynamics in a non-Newtonian polymer electrolyte.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec8\" class=\"Section2\"\u003e\u003ch2\u003e3.2 Surface Morphology of Electrolytes\u003c/h2\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003eNon-Newtonian fluids are characterized by a viscosity that varies in response to applied shear stress or strain rate. In this electrolyte system, the viscosity manifests as either shear-thinning or shear-thickening, depending on the TiO\u003csub\u003e2\u003c/sub\u003e concentration and the structural dynamics of the polymer matrix. Figures\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003e(a)\u0026ndash;(f) show the polarization microscope images of the TiO\u003csub\u003e2\u003c/sub\u003e-infused gel polymer electrolyte samples (A, B, C, D, E, F), while Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e7\u003c/span\u003e(g) depicts the polarizing image of the spherulites formed by lamellar structures of the pure PEO sample.\u003c/p\u003e\u003cp\u003eThe incorporation of TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles influences the microstructure and rheological properties of the gel polymer electrolyte, modifying its viscoelastic and non-Newtonian characteristics. At the optimal TiO\u003csub\u003e2\u003c/sub\u003e concentration of 15 wt.% (Sample D), the electrolyte exhibited improved ionic conductivity, likely due to a more amorphous polymer phase and enhanced ion mobility facilitated by the nanoparticle-induced dynamic rearrangement of polymer chains. This concentration may represent a balance between the modifications in polymer chain dynamics caused by the filler and the formation of conductive ion pathways. When the TiO\u003csub\u003e2\u003c/sub\u003e content exceeds 15 wt.%, a decline in conductivity is observed, attributed to nanoparticle aggregation as seen in samples E and F, which can increase rigidity and restrict ion transport. In addition, reduction of rich polymer phase which contributes to the ion transport at higher TiO\u003csub\u003e2\u003c/sub\u003e content can decrees the conductivity. The non-Newtonian gel nature of the electrolyte allows dynamic rearrangement of the polymer-nanoparticle network under shear or stress, thereby enhancing interface contact and supporting stable ionic conduction in quasi-solid-state DSSCs.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec9\" class=\"Section2\"\u003e\u003ch2\u003e3.3 FTIR and UV-Visible spectroscopy\u003c/h2\u003e\u003cp\u003eFigure \u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e8\u003c/span\u003e(a) shows the UV-Visible absorption spectra of the electrolyte series prepared with varying TiO\u003csub\u003e2\u003c/sub\u003e concentrations from 0% to 25%. The absorption edge of the TiO\u003csub\u003e2\u003c/sub\u003e nanoparticles appears near 400 nm, and the results are consistent with their wide bandgap properties. An increase in light absorption is observed with an increase in TiO\u003csub\u003e2\u003c/sub\u003e nanofiller content. Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e8\u003c/span\u003e(b) presents the FTIR spectra of the electrolyte series, obtained in the wavenumber range of 500\u0026ndash;3000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. The spectra show characteristic vibrational modes associated with the organic solvents ethylene carbonate (EC) and propylene carbonate (PC) present in the electrolyte. In particular, the in-plane ring stretching, asymmetric ring stretching, and C-O stretching vibrations are observed at 714.50 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, 1069.34 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and 1770.33 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. The peaks at 772.35, 1158.04 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and 1388.49 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e correspond to out-of-plane ring bending, C-H wagging, and C-H rocking vibrations, respectively. No unexpected peaks attributable to undesired species or byproducts are detected, confirming the chemical integrity and compatibility of the electrolyte system.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cb\u003eCharacterization of DSSCs\u003c/b\u003e\u003c/p\u003e\u003cp\u003eFigure \u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e9\u003c/span\u003e shows the variation of current density and power density with cell potential for DSSCs assembled with this new electrolyte series. Figure\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e9\u003c/span\u003e (a) and (b), which present the photocurrent density and power density variation with cell potential, were utilized to calculate the key performance parameters such as open-circuit voltage (\u003cem\u003eV\u003c/em\u003e\u003csub\u003eoc\u003c/sub\u003e), short-circuit current density (\u003cem\u003eJ\u003c/em\u003e\u003csub\u003esc\u003c/sub\u003e), fill factor (\u003cem\u003eFF\u003c/em\u003e), and power conversion efficiency (PCE). The values of the respective parameters of each cell are given in Table\u0026nbsp;\u003cspan refid=\"Tab3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. Notably, every tested cell achieved an efficiency of over 5%. The observed high efficiencies in the quasi-solid state solar cells can be attributed to the high ionic conductivity of the electrolytes. The solar cell containing electrolyte sample D (TiO\u003csub\u003e2\u003c/sub\u003e, 15.0 wt.%) showed the highest power conversion efficiency (PCE) of 7.18%, which is a 26.0% increase compared to the TiO\u003csub\u003e2\u003c/sub\u003e-free reference sample. This cell that contains electrolyte with 15.0% TiO\u003csub\u003e2\u003c/sub\u003e (Sample D), reaches a \u003cem\u003eJ\u003c/em\u003e\u003csub\u003esc\u003c/sub\u003e of 13.02 mA cm\u003csup\u003e-\u003c/sup\u003e\u0026sup2;, a \u003cem\u003eV\u003c/em\u003e\u003csub\u003eoc\u003c/sub\u003e of 0.78 V and an \u003cem\u003eFF\u003c/em\u003e of 0.71.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003cp\u003e\u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab3\" border=\"1\"\u003e\u003ccaption language=\"En\"\u003e\u003cdiv class=\"CaptionNumber\"\u003eTable 3\u003c/div\u003e\u003cdiv class=\"CaptionContent\"\u003e\u003cp\u003eThe photoelectrochemical parameters of all DSSCs.\u003c/p\u003e\u003c/div\u003e\u003c/caption\u003e\u003ccolgroup cols=\"5\"\u003e\u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e\u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u003cp\u003eSample\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e\u003cp\u003e\u003cem\u003eV\u003c/em\u003e\u003csub\u003eoc\u003c/sub\u003e / V\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e\u003cp\u003e\u003cem\u003eJ\u003c/em\u003e\u003csub\u003esc\u003c/sub\u003e / mA cm\u003csup\u003e\u0026minus;\u0026thinsp;2\u003c/sup\u003e\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c4\"\u003e\u003cp\u003e\u003cem\u003eff\u003c/em\u003e\u003c/p\u003e\u003c/th\u003e\u003cth align=\"left\" colname=\"c5\"\u003e\u003cp\u003e\u003cem\u003eη\u003c/em\u003e / %\u003c/p\u003e\u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eA\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.71\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e12.17\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.66\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e5.70\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eB\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.73\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e12.28\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.66\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e5.94\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eC\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.76\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e11.51\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.74\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e6.51\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eD\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.78\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e13. 02\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.71\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e7.18\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eE\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.78\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e13.20\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.66\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e6.83\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e\u003cp\u003eF\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c2\"\u003e\u003cp\u003e0.78\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e\u003cp\u003e12.64\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c4\"\u003e\u003cp\u003e0.64\u003c/p\u003e\u003c/td\u003e\u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e\u003cp\u003e6.26\u003c/p\u003e\u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/colgroup\u003e\u003c/table\u003e\u003c/div\u003e\u003c/p\u003e\u003cp\u003eThe solar cell performance enhancement achieved by modifying the electrolyte with TiO\u003csub\u003e2\u003c/sub\u003e nanofillers can be better understood by studying the conductivity behaviour of the electrolytes. For a clearer comparison, Fig.\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e10\u003c/span\u003e illustrates the correlation between the conductivity of the various electrolytes and the PCE of the DSSCs using these electrolytes. As observed in Fig.\u0026nbsp;\u003cspan refid=\"Fig9\" class=\"InternalRef\"\u003e10\u003c/span\u003e, the improvement in efficiency for the cells fabricated with the improved electrolytes generally follows the trend in conductivity. However, the relationship is not strictly linear or one-to-one since other minor effects, such as transport number iodide/triiodides etc, can also influence the results. Finally, it can be concluded that the ionic conductivity of non-Newtonian polar electrolytes can be significantly enhanced by incorporating TiO\u003csub\u003e2\u003c/sub\u003e nanofillers. This improvement in conductivity can, in turn, contribute to enhanced PCE in DSSCs.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e"},{"header":"4.0 Conclusions","content":"\u003cp\u003eNon-Newtonian gel and polymer electrolytes, especially when enhanced with TiO\u003csub\u003e2\u003c/sub\u003e nanofillers, offer a promising route toward the realization of sustainable, flexible, and low-maintenance solar energy technologies. This study reveals the effectiveness of TiO\u003csub\u003e2\u003c/sub\u003e nanofiller-infused non-Newtonian gel polymer electrolytes in enhancing the performance of quasi-solid state DSSCs. By incorporating TiO\u003csub\u003e2\u003c/sub\u003e into a PEO-based polymer matrix, the polymer can transform into a more amorphous structure, significantly improving ionic mobility and overall electrolyte conductivity. An optimal TiO\u003csub\u003e2\u003c/sub\u003e content of 15 wt.% was identified, yielding a maximum PCE of 7.18%, which marks a 29.0% improvement over the filler-free electrolyte. It can be concluded, the incorporation of TiO\u003csub\u003e2\u003c/sub\u003e nanofillers enhances the ionic conductivity of non-Newtonian polar electrolytes, thereby improving the power conversion efficiency of DSSCs. Electrochemical and spectroscopic analyses confirmed improved charge transport, reduced recombination, and maintained chemical stability. These findings highlight the potential of non-Newtonian gel-polymer electrolytes as a promising approach for developing high-efficiency and stable solid-state DSSCs.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eR. P.; Methodology, Formal analysis, Data Collection, Investigation, Writing, preparing Graphs and Figures.N. G. A.; Conceptualization, Data Collection, Methodology, Formal analysis, Writing and Investigation. K. W.; Investigation, Formal analysis and Review \u0026amp; Editing.M. A. K. L.; Conceptualization, Methodology and Review \u0026amp; Editing.G. S.; Conceptualization, Review \u0026amp; Editing and Supervision.T. H. W.; Conceptualization, Review \u0026amp; Editing and Supervision.T. M. W. J.; Conceptualization, Methodology, Formal analysis, Investigation, Writing - Review \u0026amp; Editing, Supervision and Project administration\u003c/p\u003e\u003ch2\u003eAcknowledgments\u003c/h2\u003e\u003cp\u003eFinancial assistance was provided by the Research Grant No. PGIS/2022/12 from the Post-graduate Institute of Science, University of Peradeniya, Sri Lanka.\u003c/p\u003e\u003ch2\u003eData Availability\u003c/h2\u003e\u003cp\u003eResearch data will be provided on request\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eKanimozhi, G., Naresh, N., Kumar, H., \u0026amp; Satyanarayana, N. (2022). Review on the recent progress in the nanocomposite polymer electrolytes on the performance of lithium‐ion batteries. \u003cem\u003eInternational Journal of Energy Research\u003c/em\u003e, \u003cem\u003e46\u003c/em\u003e(6), 7137-7174.\u003c/li\u003e\n\u003cli\u003eChandrika, R. P., Gunathilaka, S. M. S., Liyanage, J. P., Wijayaratne, K., Kumara, G. R. 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Maxwell\u0026ndash;Wagner polarization and interfacial charge at the multi-layers of thermoplastic polymers. \u003cem\u003eJournal of Electrostatics\u003c/em\u003e, \u003cem\u003e72\u003c/em\u003e(1), 91-97.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"Non-Newtonian Fluid, Gel polymer electrolyte, Ionic conductivity, Nanofiller, Composite Electrolyte","lastPublishedDoi":"10.21203/rs.3.rs-7956216/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7956216/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThis study explores the role of non-Newtonian gel-polymer electrolytes, infused with TiO\u003csub\u003e2\u003c/sub\u003e nanofillers, in improving the performance of dye-sensitized solar cells (DSSCs). The key focus was understanding how these nanofillers alter the electrolyte's ionic conductivity and influence the DSSC efficiency, and to study the transient nature of the conductivity in non-Newtonian electrolytes. By introducing TiO\u003csub\u003e2\u003c/sub\u003e nanofillers, the polymer chains undergo structural rearrangements, transitioning into a more amorphous state. This shift enhances ionic mobility within the electrolyte, a characteristic behavior of non-Newtonian fluids where viscosity and flow properties change under stress or temperature. This behavior is confirmed by analyzing the transient nature of the electrolyte\u0026rsquo;s conductivity. The FTIR and UV-Vis spectroscopy confirmed chemical stability and light-harvesting capability, respectively, without introducing unwanted reactions. The research found a distinct optimum in performance at 15.0 wt.% TiO\u003csub\u003e2\u003c/sub\u003e content beyond which the performance decreased due to nanoparticle aggregation and polymer chain immobilization. Key electrochemical analyses, including Nyquist plots and temperature-dependent conductivity measurements, reveal that ionic conductivity exhibits non-Arrhenius behavior, indicating complex, thermally activated transport within the gel matrix. The conductivity peaked at 9.73 mS cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 80\u0026deg;C for the 15% TiO\u003csub\u003e2\u003c/sub\u003e sample, confirming the non-Newtonian dynamic nature of the electrolyte. AC conductivity, dielectric constant variations, and polarization microscopy provided further evidence of improved amorphous character and charge transport. In terms of DSSC performance, the electrolyte sample containing 15.0 wt.% TiO\u003csub\u003e2\u003c/sub\u003e yielded a power conversion efficiency (PCE) of 7.18%, a 26.0% increase over the TiO\u003csub\u003e2\u003c/sub\u003e-free baseline. This improvement is linked to increased iodide ion mobility, reduced charge recombination, longer electron diffusion lengths, and enhanced photoelectron lifetimes, as shown through EIS analysis. Conclusively, TiO\u003csub\u003e2\u003c/sub\u003e nanofiller\u0026ndash;infused non-Newtonian gel-polymer electrolytes significantly enhance DSSC stability, conductivity, and efficiency. This work presents a viable pathway toward developing high-performance, stable, and sustainable solar cells using solid-state electrolyte technologies.\u003c/p\u003e","manuscriptTitle":"Non-Newtonian Electrolytes: A Sustainable Pathway to Improve Dye-Sensitized Solar Cell Technology by Enhancing Ionic Conductivity in the Electrolyte","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-11-18 17:49:14","doi":"10.21203/rs.3.rs-7956216/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"cedbcef8-21c3-4ab5-ba87-346f03b66c59","owner":[],"postedDate":"November 18th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2026-04-07T16:06:20+00:00","versionOfRecord":{"articleIdentity":"rs-7956216","link":"https://doi.org/10.1007/s10854-026-17067-5","journal":{"identity":"journal-of-materials-science-materials-in-electronics","isVorOnly":false,"title":"Journal of Materials Science: Materials in Electronics"},"publishedOn":"2026-04-04 15:59:12","publishedOnDateReadable":"April 4th, 2026"},"versionCreatedAt":"2025-11-18 17:49:14","video":"","vorDoi":"10.1007/s10854-026-17067-5","vorDoiUrl":"https://doi.org/10.1007/s10854-026-17067-5","workflowStages":[]},"version":"v1","identity":"rs-7956216","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7956216","identity":"rs-7956216","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}