Evaluation of Various Combination Ratios of Polymer-Based Dyes from Mangosteen Pericarp and Ti Plant for Grätzel Cell Efficiency Using Response Surface Methodology

Evaluation of Various Combination Ratios of Polymer-Based Dyes from Mangosteen Pericarp and Ti Plant for Grätzel Cell Efficiency Using Response Surface Methodology | 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 Evaluation of Various Combination Ratios of Polymer-Based Dyes from Mangosteen Pericarp and Ti Plant for Grätzel Cell Efficiency Using Response Surface Methodology Tristan Roy Panaligan, Alyza Anzano, Bruce Benjamin De Leon, Ronesse Angel Rellin, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6462691/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract This study investigates the performance of combining polymer-rich natural dyes from Mangosteen pericarp and Ti plant leaves as sensitizers for Grätzel cells. The mangosteen pericarp is rich in natural polymers, including polyphenols, anthocyanins, and polysaccharides. These compounds enhance light absorption, electron transfer, film formation, and dye adhesion on the TiO 2 surface. The Ti plant leaves contain a high amount of chlorophyll. These compounds are well-known for their ability to capture light and act as photosensitizers, especially for Grätzel cells. Using Response Surface Methodology (RSM) with a Box-Behnken Design, the research evaluates the effects of dye combination ratios, dye soaking time (DST), and light soaking time (LST) on Grätzel cell efficiency. UV-Vis spectrophotometry was employed to analyze the light absorption characteristics of the natural dyes, revealing that a 2:8 ratio (20% Mangosteen pericarp dye and 80% Ti plant dye) exhibited the highest peak absorbance of 0.4685 at 665.452 nm. Grätzel cells with this 2:8 ratio achieved the highest average efficiency of 0.1989% under optimal conditions of 48 hours DST and 2.55 hours LST. While extended DST improved efficiency, longer LST and a higher proportion of Ti plant dye negatively impacted stability and performance. Statistical analysis indicated significant interactions among the parameters, with varying efficiency based on the dye composition and soaking durations. Grätzel cell Combination Ratio Dye Soaking Time Light Soaking Time Response Surface Methodology Figures Figure 1 Figure 2 Figure 3 1 Introduction The global energy crisis, primarily driven by the unsustainable reliance on fossil fuels, presents a critical challenge that aggravates climate change and threatens environmental stability. In the Philippines, as Concepcion et al. [ 1 ] stated, coal accounts for approximately 70% of energy consumption, while renewable sources contribute only about 10%. This reliance on non-renewable energy sources significantly increases carbon emissions and hastens global warming, highlighting the critical need for alternative and sustainable energy options. Additionally, the finite nature of fossil fuel reserves and the deterioration of aging energy infrastructure further highlight the vulnerability and unsustainability of traditional energy systems. A study by Ye et al. [ 2 ] mentioned that solar energy, a renewable and environmentally friendly resource, represents a favorable path for addressing these challenges. Among the various solar technologies, dye-sensitized solar cells (DSSCs), commonly referred to as Grätzel cells, have emerged as a compelling alternative to conventional silicon-based photovoltaic systems. DSSCs are particularly attractive due to their cost-effectiveness, reduced toxicity, and the potential to utilize abundant, naturally derived materials as sensitizers. By employing natural dyes to capture sunlight, these cells align with sustainable energy production goals and reduce dependence on synthetic and resource-intensive materials. The primary objective of this study was to maximize the efficiency of dye-sensitized solar cells (DSSCs) using natural dye extracts from Mangosteen pericarp (MP) and Ti plant (TP) leaves. These locally abundant yet underutilized resources in the Philippines present a cost-effective and environmentally sustainable alternative to conventional synthetic dyes and silicon-based photovoltaic systems. Examples of natural dyes used for DSSCs come from Mangosteen pericarp and Ti plant leaves. According to Pedraza-Chaverri et al. [ 3 ] and Wathoni et al. [ 4 ], the Mangosteen pericarp is a valuable source of natural polymers and dyes, including polyphenols (xanthones and tannins), anthocyanin, polysaccharides (pectin and cellulose). At the same time, according to Gabrielsen [ 5 ], the Ti plant leaves are particularly rich in chlorophyll (a porphyrin-based compound). In addition, recent research has demonstrated that combining natural dyes from multiple sources can enhance DSSC efficiency, often outperforming single-dye systems. This study employed Box-Behnken Design (BBD), a statistical tool within the Response Surface Methodology (RSM) framework, to systematically optimize key parameters—contributing directly to the achievement of several United Nations Sustainable Development Goals (SDGs) through its emphasis on clean energy innovation, sustainable resource use, and climate action. Primarily, it supports SDG 7: Affordable and Clean Energy by developing an eco-friendly and cost-effective alternative to conventional solar cell materials using natural dyes from Mangosteen pericarp and Ti plant extracts. By harnessing renewable resources to optimize Grätzel cell efficiency, the research fosters innovation in sustainable energy technologies, aligning with SDG 9: Industry, Innovation, and Infrastructure. Furthermore, the use of abundant, biodegradable materials addresses resource efficiency and reduces environmental impact, contributing to SDG 12: Responsible Consumption and Production. Lastly, this work aligns with SDG 13: Climate Action by promoting renewable energy solutions that help mitigate carbon emissions and combat global warming, supporting the global transition toward sustainable energy systems. 2 Materials and Methods 2.1 Preparation of Mangosteen Pericarp Dye Extract The preparation of dye extract from MP was adapted from the methods utilized by Al-Alwani et al. [ 6 ] and Ndeze et al. [ 7 ] with some modifications. Mangosteen pericarp, locally sourced, was thoroughly washed with distilled water to remove impurities. The cleaned MP was air-dried and subsequently oven-dried at 80°C until a constant weight was achieved. The dried MP was ground into fine particles using a Sonifer SF-3526 coffee grinder and sieved to achieve a particle size greater than 60 mesh. For dye extraction, 50 g of the ground MP was soaked in 500 mL of 95% ethanol in a 1 L amber glass bottle. The bottle was sealed and stored in a dark environment for 24 hours. The mixture was then stirred at 78.33°C for 45 minutes using a magnetic stirrer operating at 400–500 rpm. After cooling to room temperature, the solution was filtered, and the residue was discarded. The filtrate was concentrated using rotary evaporation at 50°C for 3 hours. The resulting MP extract was stored in a 250 mL amber glass bottle for subsequent use. 2.2 Preparation of Ti Plant Leaves Dye Extract The method for preparing dye extract from Ti plant leaves was based on the approaches described by Al-Alwani et al. [ 6 ] and Ndeze et al. [ 7 ], with certain variations. TP leaves were thoroughly washed with distilled water to remove surface impurities. The cleaned TP leaves were air-dried and further dried in an oven at 80°C until a constant weight was obtained. The dried leaves were ground using a Panasonic MX-900M blender and sieved through a 60-mesh screen. For dye extraction, 50 g of the ground TP leaves were combined with 500 mL of 95% ethanol in a 1 L amber glass bottle. The bottle was sealed and stored in a dark environment for 24 hours. The mixture was stirred at 78.33°C for 45 minutes using a magnetic stirrer set at 400–500 rpm. The filtrate was separated, and the residue was discarded. The filtrate was concentrated using rotary evaporation at 50°C for 3 hours. The concentrated TP leaf extract was stored in a 250 mL amber glass bottle for further use. 2.3 Preparation of Combination Ratios of Dye To create the dye combinations, extracts of Mangosteen pericarp and Ti plant leaves were mixed in predetermined ratios of 2:8, 6.8:3.2, and 8:2. For each combination, a 15 g solution was prepared in a beaker and thoroughly mixed for 5 minutes. A 1.5 g aliquot of each mixture was then transferred to a syringe for subsequent processes. 2.4 Preparation of Electrolyte The procedure for preparing electrolyte solution was based on Kabir et al. [ 8 ]. The electrolyte solution was prepared by dissolving 0.576 g of iodine and 7.47 g of potassium iodide in 90 mL of ethylene glycol. The mixture was stirred until the components were fully dissolved, and the solution was stored in a 250 mL amber glass bottle for later use. 2.5 Preparation of Titanium Dioxide Paste The methods utilized to prepare the titanium dioxide paste were from the studies of Munawaroh et al. [ 9 ], Prakash et al. [ 10 ], and Salimian et al. [ 11 ]. Titanium dioxide (TiO₂) paste was prepared by blending 65 g of TiO₂ powder with 130 mL of 95% ethanol in a mortar and pestle. The mixture was ground for 10 minutes until a lump-free, homogeneous paste was achieved. The prepared paste was covered with aluminum foil and set aside. 2.6 Fabrication of Grätzel Cells The procedure for fabricating the Grätzel cells was derived from the method outlined by Concepcion et al. [ 1 ], with specific modifications. The natural dye from mangosteen pericarp and Ti plant leaves is considered a soft, natural polymer requiring adapted methods to preserve its light-absorbing ability and enhance interaction with the conductive side. Fluorine-doped tin oxide (FTO) glass substrates were cleaned, and the non-conductive side was coated with TiO₂ paste to ensure a uniform application. The coated glass was sintered on a hot plate at 350°C for 30 minutes. After cooling, the glass was immersed in a petri dish containing 1 g of the prepared dye combination and allowed to soak for 12 hours. Unlike ordinary synthetic dyes, which bind quickly, natural dyes were allowed to soak for 12 hours to ensure sufficient dispersion and adsorption. This extended duration was implemented as a novel modification to accommodate binding in soft and biodegradable dyes. The counter electrode was prepared by coating the conductive side of a separate FTO glass with a carbon layer, achieved by passing the substrate through a candle flame. The working and counter electrodes were assembled with 0.5 mL of electrolyte solution placed between them and secured using binder clips. The process is repeated for each sample having different dye soaking and combination ratios. 2.7 Testing and Characterization The different combination ratios of natural dye are subjected to UV Vis spectrophotometry to determine the light absorption characteristics of each. Each combination ratio of dye is diluted, having a weight of dye (g) to volume of solvent ratio (mL) of 1:2500. An aliquot of each sample is transferred to a cuvette and subjected to UV-Vis Spectrophotometer. The fabricated Grätzel cells were exposed to a light source at varying light soaking time (LST). The methods for testing the fabricated Grätzel cells that were utilized are from the study of See et al. [ 9 ] The open-circuit voltage (E oc or V oc ) and short-circuit current (I sc ) were measured. The total resistance of the circuit connected to the Grätzel cell was calculated using Ohm’s law. The maximum power point current (I mp ) and voltage (E mp ) were determined using a circuit adjusted for different LST values. These parameters were then used to calculate the efficiency of the Grätzel cells using Eqs. (1) and (2). This process is repeated for all Grätzel cells having various light soaking times in each. $$\:FF=\frac{{E}_{mp}{I}_{mp}}{{E}_{oc}{I}_{sc}}\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\left(1\right)$$ $$\:\eta\:=\frac{{V}_{oc}{J}_{sc}FF}{{P}_{in}}\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\:\left(2\right)$$ 3 Results and Discussion The UV-Vis spectrophotometry results in Fig. illustrate the light absorption characteristics of the dye extracts across various combination ratios of MP and TP. The spectra highlight how the ratio of the two natural dye sources influences the absorbance at different wavelengths, which directly impacts the photoactive efficiency of the Grätzel cells. Notably, the 2:8 ratio exhibited the highest absorbance within the visible light range, particularly around 400–600 nm, which aligns with the spectral region where solar energy is most effectively harvested for dye-sensitized solar cells. This suggests that the 2:8 combination optimizes the synergistic effect of the two dyes, resulting in enhanced light capture and superior Grätzel cell efficiency. The findings suggest that the 2:8 ratio is a promising candidate for maximizing solar energy conversion efficiency in DSSCs. In contrast, the other ratios (0:10, 6.8:3.2, 8:2, and 10:0) demonstrated comparatively lower absorbance, which may explain their reduced cell performance. The decreased absorbance at critical wavelengths for these ratios implies suboptimal interaction or individual contributions of the dye components to the light-harvesting process. The efficiencies of the Grätzel cells across different dye combination ratios, DST, and LST are presented in Table 1 . The results consistently highlight the superior performance of the 2:8 dye ratio combined with a light soaking time of 2.55 hours, emphasizing the critical role of parameter optimization in enhancing cell performance. The findings emphasize the significance of the TP dye's proportion in the combination, as its higher percentage appears to enhance the efficiency of the cells. Supporting evidence from Hang [ 13 ] demonstrates that the efficiency of MP dye improves when combined with other extracts, such as Adenium obesum, achieving an efficiency of 0.37%, compared to 0.22% for Mangosteen pericarp alone. Similarly, the study by Isah Kimpa et al. [ 14 ] correlates the intensity of light absorbance in the UV-Vis spectrum with improved photoelectrochemical performance of DSSCs. Moreover, the optimal LST of 2.55 hours aligns with the results of Ndeze et al. [ 4 ], where Baobab leaf dye achieved its highest efficiency of 0.111% within 2 hours of light soaking. These comparisons suggest that the observed trends in this study are consistent with previously reported findings, further validating the effectiveness of the 2:8 ratio and the optimized LST in maximizing Grätzel cell efficiency. As noted by Panaligan et al. [ 15 ], Response Surface Methodology (RSM) is a statistical and mathematical technique used to model and optimize processes, particularly for complex systems. In this study, Box-Behnken Design (BBD), a type of RSM, was employed to optimize the factors influencing Grätzel cell efficiency. BBD is widely used for quadratic modeling, and it is especially advantageous when fewer experimental runs are needed compared to other RSM designs, such as Central Composite Design (CCD). Unlike CCD, BBD does not require experiments at extreme factor settings, which makes it a more cost-effective option while still providing valuable insights into factor interactions. Table 1 Percent Grätzel Cell Efficiency at Different Combination Ratios, DST, and LST Run No. Combination Ratio of MP to TP Leaves Extracts DST (hr) LST (hr) Efficiency (Trial 1) Efficiency (Trial 2) Average Efficiency 1 2:8 12 2.55 0.1328% 0.1775% 0.1551% 2 8:2 30 0.1 0.0229% 0.0158% 0.0193% 3 6.8:3.2 48 5 0.0978% 0.0839% 0.0909% 4 6.8:3.2 48 0.1 0.0522% 0.0830% 0.0676% 5 6.8:3.2 30 2.55 0.1553% 0.1113% 0.1333% 6 2:8 30 0.1 0.0119% 0.0145% 0.0132% 7 8:2 12 2.55 0.0768% 0.1011% 0.0889% 8 8:2 48 2.55 0.0788% 0.0921% 0.0855% 9 6.8:3.2 12 5 0.1545% 0.1944% 0.1744% 10 8:2 30 5 0.0410% 0.0480% 0.0445% 11 2:8 48 2.55 0.2153% 0.1825% 0.1989% 12 6.8:3.2 12 0.1 0.0500% 0.0336% 0.0418% 13 2:8 30 5 0.0430% 0.0428% 0.0429% The BBD approach enables efficient exploration of the parameter space with fewer design points, allowing for the identification of optimal conditions for Grätzel cell performance. The experimental design also facilitates the precise adjustment of factor levels based on the results of the parametric study. The surface plots in Fig. 2 illustrate the interactions between two factors and their effects on Grätzel cell performance, revealing how these interactions lead to variations in efficiency. These plots show that no specific interaction leads to substantial variation in cell efficiency, as supported by the results of the ANOVA in Fig. 3 . The P-values for each interaction exceed the 0.05 level of significance, suggesting that these interactions do not significantly influence Grätzel cell efficiency. 4 Conclusions This study explores the potential of using Mangosteen pericarp and Ti plant extracts as cost-effective, renewable dyes for dye-sensitized solar cells. The results demonstrate that these natural dyes have promise for sustainable energy production, providing an eco-friendly and economical alternative to conventional materials. By combining these extracts, this research aims to create a safer and more affordable solution for DSSC fabrication. The methodological innovation for soft materials, specifically natural polymers, utilizes the Response Surface Methodology with a Box-Behnken design to optimize dye ratios, soaking durations, and light exposure times, thereby maximizing photovoltaic performance. Presenting a novel and environmentally sustainable approach for DSSC fabrication. This approach highlights the viability of green materials in advancing solar cell technology through a systematic and scientifically rigorous testing strategy. Specifically, a 2:8 ratio of Mangosteen pericarp to Ti plant dye, 48 hours of dye soaking, and 2.55 hours of light exposure yielded the highest efficiency. Declarations Author Contribution A. A., B. B. D., and R. A. R. contributed to the conceptualization and experimental design of the study, carried out the laboratory work, collected the data, and performed data analysis and statistical optimization using Response Surface Methodology. T. R. P. and J. A. supervised the experimental phase, with T. R. P. reviewing the final manuscript and J. A. facilitating access to the research laboratory. All authors reviewed, edited, and approved the final version of the manuscript Acknowledgement This research was supported by the Department of Chemical Engineering of Mapúa Institute of Technology, Laguna (MITL) at Mapúa Malayan Colleges Laguna (MMCL), Cabuyao City, Laguna, 4025, Philippines References Concepcion, R., Alejandrino, J., Mendigoria, C. H., Dadios, E., Bandala, A., Sybingco, E., & Vicerra, R. R. (2021). Lactuca sativa leaf extract concentration optimization using evolutionary strategy as photosensitizer for TiO2-filmed Grӓtzel cell. Optik, 242. Ye, M., Wen, X., Wang, M., Iocozzia, J., Zhang, N., Lin, C., & Lin, Z. (2015). Recent advances in dye-sensitized solar cells: From photoanodes, sensitizers and electrolytes to counter electrodes. In Materials Today (Vol. 18, Issue 3, pp. 155–162). Elsevier B.V. Pedraza-Chaverri, J., et al. (2008). Medicinal properties of mangosteen (Garcinia mangostana). Food and Chemical Toxicology, 46(10), 3227–3239. Wathoni, N., et al. (2019). Characterization and antioxidant activity of pectin from Indonesian mangosteen (Garcinia mangostana L.) rind. Heliyon, 5(8), e02299. Gabrielsen, E. K. (1948). Effects of Different Chlorophyll Concentrations on Photosynthesis in Foliage Leaves. Physiologia Plantarum, 1(1), 5–37. Al-Alwani, M. A. M., Ludin, N. A., Mohamad, A. B., Kadhum, A. A. H., Baabbad, M. M., & Sopian, K. (2016). Optimization of dye extraction from Cordyline fruticosa via response surface methodology to produce a natural sensitizer for dye-sensitized solar cells. Results in Physics, 6, 520–529. Ndeze, U. I., Aidan, J., Ezike, S. C., & Wansah, J. F. (2021). Comparative performances of nature-based dyes extracted from Baobab and Shea leaves photo-sensitizers for dye-sensitized solar cells (DSSCs). Current Research in Green and Sustainable Chemistry, 4. Kabir, F., Bhuiyan, M. M. H., Hossain, M. R., Bashar, H., Rahaman, M. S., Manir, M. S., Ullah, S. M., Uddin, S. S., Mollah, M. Z. I., Khan, R. A., Huque, S., & Khan, M. A. (2019). Improvement of efficiency of Dye Sensitized Solar Cells by optimizing the combination ratio of Natural Red and Yellow dyes. Optik, 179, 252–258. Munawaroh, H., adillah, G. F., Saputri, L. N. M. Z., Hanif, Q. A., Hidayat, R., & Wahyuningsih, S. (2016). The co-pigmentation of anthocyanin isolated from mangosteen pericarp ( Garcinia Mangostana L. ) as Natural Dye for Dye- Sensitized Solar Cells (DSSC). IOP Conference Series: Materials Science and Engineering, 107(1), 012061. Prakash, P., Janarthanan, B., Ubaidullah, M., Al-Enizi, A. M., Shaikh, S. F., Alanazi, N. B., Alkhalifah, R. I., & Ilyas, M. (2023). Optimization, fabrication, and characterization of anthocyanin and carotenoid derivatives based dye-sensitized solar cells. Journal of King Saud University - Science, 35(4). Salimian, J., Osfouri, S., Azin, R., & Jalali, T. (2022). Impacts of paste preparation methods on the porous TiO2nanostructure properties and naturally dye-sensitized solar cells performance. Journal of Materials Research and Technology, 18, 4816–4833. See, S. C., Mercado, M. M., Corpuz, J. Z., Balbin, J., & Chua, E. (2020). Characterization of Electrical Quantities of a Grape Dye-Sensitized Solar Cell. IOP Conference Series: Earth and Environmental Science, 581(1). Hang, C. O. (2015). Natural Dye For Dye Sensitized Solar Cells (DSSCs) Using Mangosteen Adenium Obesum. Isah Kimpa, M., Momoh, M., Uthman Isah, K., Nawawi Yahya, H., & Muhammed Ndamitso, M. (2012). Photoelectric Characterization of Dye Sensitized Solar Cells Using Natural Dye from Pawpaw Leaf and Flame Tree Flower as Sensitizers. Materials Sciences and Applications, 03(05), 281–286. Panaligan, T. R. L., Jr., Pagal, J. A. N., & Cancisio, S. J. J.(2023). Response Surface Methodology Design and Optimization of Inorganic Phosphate Removal from Simulated Wastewater Effluent Utilizing Caulerpa lentillifera Algal Powder. In Chemical Engineering Transactions (Vol. 106, pp. 61–66). Additional Declarations No competing interests reported. Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-6462691","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":444260332,"identity":"3db1cac5-474e-4c96-b381-21d62375608a","order_by":0,"name":"Tristan Roy 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Ratios.\u003c/p\u003e","description":"","filename":"1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6462691/v1/87c4bec60a44d67cec51a979.jpg"},{"id":81105461,"identity":"f4c1175d-7671-4405-a483-c22a79edfe0d","added_by":"auto","created_at":"2025-04-22 09:33:30","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":100927,"visible":true,"origin":"","legend":"\u003cp\u003eSurface Plot of (a) combination ratio and DST vs. Grätzel cell efficiency, (b) combination ratio and LST vs. Grätzel cell efficiency, and (c) DST and LST vs. Grätzel cell efficiency.\u003c/p\u003e","description":"","filename":"2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6462691/v1/9e441fe871ed293d2c7f3e6c.jpg"},{"id":81105466,"identity":"0f6f85d9-2623-4c67-a789-fb901cad6084","added_by":"auto","created_at":"2025-04-22 09:33:30","extension":"jpg","order_by":3,"title":"Figure 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Introduction","content":"\u003cp\u003eThe global energy crisis, primarily driven by the unsustainable reliance on fossil fuels, presents a critical challenge that aggravates climate change and threatens environmental stability. In the Philippines, as Concepcion et al. [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e] stated, coal accounts for approximately 70% of energy consumption, while renewable sources contribute only about 10%. This reliance on non-renewable energy sources significantly increases carbon emissions and hastens global warming, highlighting the critical need for alternative and sustainable energy options. Additionally, the finite nature of fossil fuel reserves and the deterioration of aging energy infrastructure further highlight the vulnerability and unsustainability of traditional energy systems.\u003c/p\u003e \u003cp\u003eA study by Ye et al. [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e] mentioned that solar energy, a renewable and environmentally friendly resource, represents a favorable path for addressing these challenges. Among the various solar technologies, dye-sensitized solar cells (DSSCs), commonly referred to as Gr\u0026auml;tzel cells, have emerged as a compelling alternative to conventional silicon-based photovoltaic systems. DSSCs are particularly attractive due to their cost-effectiveness, reduced toxicity, and the potential to utilize abundant, naturally derived materials as sensitizers. By employing natural dyes to capture sunlight, these cells align with sustainable energy production goals and reduce dependence on synthetic and resource-intensive materials.\u003c/p\u003e \u003cp\u003eThe primary objective of this study was to maximize the efficiency of dye-sensitized solar cells (DSSCs) using natural dye extracts from Mangosteen pericarp (MP) and Ti plant (TP) leaves. These locally abundant yet underutilized resources in the Philippines present a cost-effective and environmentally sustainable alternative to conventional synthetic dyes and silicon-based photovoltaic systems. Examples of natural dyes used for DSSCs come from Mangosteen pericarp and Ti plant leaves. According to Pedraza-Chaverri et al. [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e] and Wathoni et al. [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e], the Mangosteen pericarp is a valuable source of natural polymers and dyes, including polyphenols (xanthones and tannins), anthocyanin, polysaccharides (pectin and cellulose). At the same time, according to Gabrielsen [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e], the Ti plant leaves are particularly rich in chlorophyll (a porphyrin-based compound). In addition, recent research has demonstrated that combining natural dyes from multiple sources can enhance DSSC efficiency, often outperforming single-dye systems.\u003c/p\u003e \u003cp\u003eThis study employed Box-Behnken Design (BBD), a statistical tool within the Response Surface Methodology (RSM) framework, to systematically optimize key parameters\u0026mdash;contributing directly to the achievement of several United Nations Sustainable Development Goals (SDGs) through its emphasis on clean energy innovation, sustainable resource use, and climate action. Primarily, it supports SDG 7: Affordable and Clean Energy by developing an eco-friendly and cost-effective alternative to conventional solar cell materials using natural dyes from Mangosteen pericarp and Ti plant extracts. By harnessing renewable resources to optimize Gr\u0026auml;tzel cell efficiency, the research fosters innovation in sustainable energy technologies, aligning with SDG 9: Industry, Innovation, and Infrastructure. Furthermore, the use of abundant, biodegradable materials addresses resource efficiency and reduces environmental impact, contributing to SDG 12: Responsible Consumption and Production. Lastly, this work aligns with SDG 13: Climate Action by promoting renewable energy solutions that help mitigate carbon emissions and combat global warming, supporting the global transition toward sustainable energy systems.\u003c/p\u003e"},{"header":"2 Materials and Methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Preparation of Mangosteen Pericarp Dye Extract\u003c/h2\u003e \u003cp\u003eThe preparation of dye extract from MP was adapted from the methods utilized by Al-Alwani et al. [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e] and Ndeze et al. [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e] with some modifications. Mangosteen pericarp, locally sourced, was thoroughly washed with distilled water to remove impurities. The cleaned MP was air-dried and subsequently oven-dried at 80\u0026deg;C until a constant weight was achieved. The dried MP was ground into fine particles using a Sonifer SF-3526 coffee grinder and sieved to achieve a particle size greater than 60 mesh.\u003c/p\u003e \u003cp\u003eFor dye extraction, 50 g of the ground MP was soaked in 500 mL of 95% ethanol in a 1 L amber glass bottle. The bottle was sealed and stored in a dark environment for 24 hours. The mixture was then stirred at 78.33\u0026deg;C for 45 minutes using a magnetic stirrer operating at 400\u0026ndash;500 rpm. After cooling to room temperature, the solution was filtered, and the residue was discarded. The filtrate was concentrated using rotary evaporation at 50\u0026deg;C for 3 hours. The resulting MP extract was stored in a 250 mL amber glass bottle for subsequent use.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Preparation of Ti Plant Leaves Dye Extract\u003c/h2\u003e \u003cp\u003eThe method for preparing dye extract from Ti plant leaves was based on the approaches described by Al-Alwani et al. [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e] and Ndeze et al. [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e], with certain variations. TP leaves were thoroughly washed with distilled water to remove surface impurities. The cleaned TP leaves were air-dried and further dried in an oven at 80\u0026deg;C until a constant weight was obtained. The dried leaves were ground using a Panasonic MX-900M blender and sieved through a 60-mesh screen.\u003c/p\u003e \u003cp\u003eFor dye extraction, 50 g of the ground TP leaves were combined with 500 mL of 95% ethanol in a 1 L amber glass bottle. The bottle was sealed and stored in a dark environment for 24 hours. The mixture was stirred at 78.33\u0026deg;C for 45 minutes using a magnetic stirrer set at 400\u0026ndash;500 rpm. The filtrate was separated, and the residue was discarded. The filtrate was concentrated using rotary evaporation at 50\u0026deg;C for 3 hours. The concentrated TP leaf extract was stored in a 250 mL amber glass bottle for further use.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Preparation of Combination Ratios of Dye\u003c/h2\u003e \u003cp\u003eTo create the dye combinations, extracts of Mangosteen pericarp and Ti plant leaves were mixed in predetermined ratios of 2:8, 6.8:3.2, and 8:2. For each combination, a 15 g solution was prepared in a beaker and thoroughly mixed for 5 minutes. A 1.5 g aliquot of each mixture was then transferred to a syringe for subsequent processes.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Preparation of Electrolyte\u003c/h2\u003e \u003cp\u003eThe procedure for preparing electrolyte solution was based on Kabir et al. [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e]. The electrolyte solution was prepared by dissolving 0.576 g of iodine and 7.47 g of potassium iodide in 90 mL of ethylene glycol. The mixture was stirred until the components were fully dissolved, and the solution was stored in a 250 mL amber glass bottle for later use.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Preparation of Titanium Dioxide Paste\u003c/h2\u003e \u003cp\u003eThe methods utilized to prepare the titanium dioxide paste were from the studies of Munawaroh et al. [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e], Prakash et al. [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e], and Salimian et al. [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]. Titanium dioxide (TiO₂) paste was prepared by blending 65 g of TiO₂ powder with 130 mL of 95% ethanol in a mortar and pestle. The mixture was ground for 10 minutes until a lump-free, homogeneous paste was achieved. The prepared paste was covered with aluminum foil and set aside.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003e2.6 Fabrication of Gr\u0026auml;tzel Cells\u003c/h2\u003e \u003cp\u003eThe procedure for fabricating the Gr\u0026auml;tzel cells was derived from the method outlined by Concepcion et al. [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e], with specific modifications. The natural dye from mangosteen pericarp and Ti plant leaves is considered a soft, natural polymer requiring adapted methods to preserve its light-absorbing ability and enhance interaction with the conductive side. Fluorine-doped tin oxide (FTO) glass substrates were cleaned, and the non-conductive side was coated with TiO₂ paste to ensure a uniform application. The coated glass was sintered on a hot plate at 350\u0026deg;C for 30 minutes. After cooling, the glass was immersed in a petri dish containing 1 g of the prepared dye combination and allowed to soak for 12 hours. Unlike ordinary synthetic dyes, which bind quickly, natural dyes were allowed to soak for 12 hours to ensure sufficient dispersion and adsorption. This extended duration was implemented as a novel modification to accommodate binding in soft and biodegradable dyes.\u003c/p\u003e \u003cp\u003eThe counter electrode was prepared by coating the conductive side of a separate FTO glass with a carbon layer, achieved by passing the substrate through a candle flame. The working and counter electrodes were assembled with 0.5 mL of electrolyte solution placed between them and secured using binder clips.\u003c/p\u003e \u003cp\u003eThe process is repeated for each sample having different dye soaking and combination ratios.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003e2.7 Testing and Characterization\u003c/h2\u003e \u003cp\u003eThe different combination ratios of natural dye are subjected to UV Vis spectrophotometry to determine the light absorption characteristics of each. Each combination ratio of dye is diluted, having a weight of dye (g) to volume of solvent ratio (mL) of 1:2500. An aliquot of each sample is transferred to a cuvette and subjected to UV-Vis Spectrophotometer.\u003c/p\u003e \u003cp\u003eThe fabricated Gr\u0026auml;tzel cells were exposed to a light source at varying light soaking time (LST). The methods for testing the fabricated Gr\u0026auml;tzel cells that were utilized are from the study of See et al. [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e] The open-circuit voltage (E\u003csub\u003eoc\u003c/sub\u003e or V\u003csub\u003eoc\u003c/sub\u003e) and short-circuit current (I\u003csub\u003esc\u003c/sub\u003e) were measured. The total resistance of the circuit connected to the Gr\u0026auml;tzel cell was calculated using Ohm\u0026rsquo;s law. The maximum power point current (I\u003csub\u003emp\u003c/sub\u003e) and voltage (E\u003csub\u003emp\u003c/sub\u003e) were determined using a circuit adjusted for different LST values. These parameters were then used to calculate the efficiency of the Gr\u0026auml;tzel cells using Eqs.\u0026nbsp;(1) and (2). This process is repeated for all Gr\u0026auml;tzel cells having various light soaking times in each.\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e\n$$\\:FF=\\frac{{E}_{mp}{I}_{mp}}{{E}_{oc}{I}_{sc}}\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\left(1\\right)$$\u003c/div\u003e\u003c/div\u003e\u003cdiv id=\"Equb\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equb\" name=\"EquationSource\"\u003e\n$$\\:\\eta\\:=\\frac{{V}_{oc}{J}_{sc}FF}{{P}_{in}}\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\:\\left(2\\right)$$\u003c/div\u003e\u003c/div\u003e\u003c/p\u003e \u003c/div\u003e"},{"header":"3 Results and Discussion","content":"\u003cp\u003eThe UV-Vis spectrophotometry results in Fig. illustrate the light absorption characteristics of the dye extracts across various combination ratios of MP and TP. The spectra highlight how the ratio of the two natural dye sources influences the absorbance at different wavelengths, which directly impacts the photoactive efficiency of the Gr\u0026auml;tzel cells.\u003c/p\u003e \u003cp\u003eNotably, the 2:8 ratio exhibited the highest absorbance within the visible light range, particularly around 400\u0026ndash;600 nm, which aligns with the spectral region where solar energy is most effectively harvested for dye-sensitized solar cells. This suggests that the 2:8 combination optimizes the synergistic effect of the two dyes, resulting in enhanced light capture and superior Gr\u0026auml;tzel cell efficiency. The findings suggest that the 2:8 ratio is a promising candidate for maximizing solar energy conversion efficiency in DSSCs.\u003c/p\u003e \u003cp\u003eIn contrast, the other ratios (0:10, 6.8:3.2, 8:2, and 10:0) demonstrated comparatively lower absorbance, which may explain their reduced cell performance. The decreased absorbance at critical wavelengths for these ratios implies suboptimal interaction or individual contributions of the dye components to the light-harvesting process.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe efficiencies of the Gr\u0026auml;tzel cells across different dye combination ratios, DST, and LST are presented in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The results consistently highlight the superior performance of the 2:8 dye ratio combined with a light soaking time of 2.55 hours, emphasizing the critical role of parameter optimization in enhancing cell performance. The findings emphasize the significance of the TP dye's proportion in the combination, as its higher percentage appears to enhance the efficiency of the cells.\u003c/p\u003e \u003cp\u003eSupporting evidence from Hang [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e] demonstrates that the efficiency of MP dye improves when combined with other extracts, such as Adenium obesum, achieving an efficiency of 0.37%, compared to 0.22% for Mangosteen pericarp alone. Similarly, the study by Isah Kimpa et al. [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e] correlates the intensity of light absorbance in the UV-Vis spectrum with improved photoelectrochemical performance of DSSCs.\u003c/p\u003e \u003cp\u003eMoreover, the optimal LST of 2.55 hours aligns with the results of Ndeze et al. [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e], where Baobab leaf dye achieved its highest efficiency of 0.111% within 2 hours of light soaking. These comparisons suggest that the observed trends in this study are consistent with previously reported findings, further validating the effectiveness of the 2:8 ratio and the optimized LST in maximizing Gr\u0026auml;tzel cell efficiency.\u003c/p\u003e \u003cp\u003eAs noted by Panaligan et al. [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e], Response Surface Methodology (RSM) is a statistical and mathematical technique used to model and optimize processes, particularly for complex systems. In this study, Box-Behnken Design (BBD), a type of RSM, was employed to optimize the factors influencing Gr\u0026auml;tzel cell efficiency. BBD is widely used for quadratic modeling, and it is especially advantageous when fewer experimental runs are needed compared to other RSM designs, such as Central Composite Design (CCD). Unlike CCD, BBD does not require experiments at extreme factor settings, which makes it a more cost-effective option while still providing valuable insights into factor interactions.\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\u003ePercent Gr\u0026auml;tzel Cell Efficiency at Different Combination Ratios, DST, and LST\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"7\"\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=\"char\" char=\".\" 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=\"char\" char=\".\" class=\"colspec\" colname=\"c5\" colnum=\"5\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c6\" colnum=\"6\"\u003e\u003c/div\u003e \u003cdiv align=\"char\" char=\".\" class=\"colspec\" colname=\"c7\" colnum=\"7\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eRun No.\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCombination \u003c/p\u003e \u003cp\u003eRatio of MP to TP Leaves Extracts\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eDST (hr)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eLST (hr)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c5\"\u003e \u003cp\u003eEfficiency\u003c/p\u003e \u003cp\u003e(Trial 1)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c6\"\u003e \u003cp\u003eEfficiency\u003c/p\u003e \u003cp\u003e(Trial 2)\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c7\"\u003e \u003cp\u003eAverage \u003c/p\u003e \u003cp\u003eEfficiency\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2:8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.1328%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.1775%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.1551%\u003c/p\u003e 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colname=\"c3\"\u003e \u003cp\u003e48\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0978%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0839%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0909%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e4\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6.8:3.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e48\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e0.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0522%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0830%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0676%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6.8:3.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e30\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.1553%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.1113%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.1333%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e6\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2:8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e30\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e0.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0119%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0145%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0132%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e7\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e8:2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0768%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.1011%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0889%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e8:2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e48\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0788%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0921%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0855%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e9\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6.8:3.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.1545%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.1944%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.1744%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e10\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e8:2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e30\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0410%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0480%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0445%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e11\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2:8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e48\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e2.55\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.2153%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.1825%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.1989%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e6.8:3.2\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e12\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e0.1\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0500%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0336%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0418%\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e13\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e2:8\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c3\"\u003e \u003cp\u003e30\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e5\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c5\"\u003e \u003cp\u003e0.0430%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c6\"\u003e \u003cp\u003e0.0428%\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"char\" char=\".\" colname=\"c7\"\u003e \u003cp\u003e0.0429%\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 BBD approach enables efficient exploration of the parameter space with fewer design points, allowing for the identification of optimal conditions for Gr\u0026auml;tzel cell performance. The experimental design also facilitates the precise adjustment of factor levels based on the results of the parametric study.\u003c/p\u003e \u003cp\u003eThe surface plots in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e illustrate the interactions between two factors and their effects on Gr\u0026auml;tzel cell performance, revealing how these interactions lead to variations in efficiency. These plots show that no specific interaction leads to substantial variation in cell efficiency, as supported by the results of the ANOVA in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e. The P-values for each interaction exceed the 0.05 level of significance, suggesting that these interactions do not significantly influence Gr\u0026auml;tzel cell efficiency.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003e \u003c/p\u003e"},{"header":"4 Conclusions","content":"\u003cp\u003eThis study explores the potential of using Mangosteen pericarp and Ti plant extracts as cost-effective, renewable dyes for dye-sensitized solar cells. The results demonstrate that these natural dyes have promise for sustainable energy production, providing an eco-friendly and economical alternative to conventional materials. By combining these extracts, this research aims to create a safer and more affordable solution for DSSC fabrication. The methodological innovation for soft materials, specifically natural polymers, utilizes the Response Surface Methodology with a Box-Behnken design to optimize dye ratios, soaking durations, and light exposure times, thereby maximizing photovoltaic performance. Presenting a novel and environmentally sustainable approach for DSSC fabrication. This approach highlights the viability of green materials in advancing solar cell technology through a systematic and scientifically rigorous testing strategy. Specifically, a 2:8 ratio of Mangosteen pericarp to Ti plant dye, 48 hours of dye soaking, and 2.55 hours of light exposure yielded the highest efficiency.\u003c/p\u003e"},{"header":"Declarations","content":"\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eA. A., B. B. D., and R. A. R. contributed to the conceptualization and experimental design of the study, carried out the laboratory work, collected the data, and performed data analysis and statistical optimization using Response Surface Methodology. T. R. P. and J. A. supervised the experimental phase, with T. R. P. reviewing the final manuscript and J. A. facilitating access to the research laboratory. All authors reviewed, edited, and approved the final version of the manuscript\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThis research was supported by the Department of Chemical Engineering of Map\u0026uacute;a Institute of Technology, Laguna (MITL) at Map\u0026uacute;a Malayan Colleges Laguna (MMCL), Cabuyao City, Laguna, 4025, Philippines\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eConcepcion, R., Alejandrino, J., Mendigoria, C. H., Dadios, E., Bandala, A., Sybingco, E., \u0026amp; Vicerra, R. R. (2021). Lactuca sativa leaf extract concentration optimization using evolutionary strategy as photosensitizer for TiO2-filmed Grӓtzel cell. Optik, 242. \u003c/li\u003e\n\u003cli\u003eYe, M., Wen, X., Wang, M., Iocozzia, J., Zhang, N., Lin, C., \u0026amp; Lin, Z. (2015). Recent advances in dye-sensitized solar cells: From photoanodes, sensitizers and electrolytes to counter electrodes. In Materials Today (Vol. 18, Issue 3, pp. 155\u0026ndash;162). Elsevier B.V. \u003c/li\u003e\n\u003cli\u003ePedraza-Chaverri, J., et al. (2008). Medicinal properties of mangosteen (Garcinia mangostana). Food and Chemical Toxicology, 46(10), 3227\u0026ndash;3239.\u003c/li\u003e\n\u003cli\u003eWathoni, N., et al. (2019). Characterization and antioxidant activity of pectin from Indonesian mangosteen (Garcinia mangostana L.) rind. Heliyon, 5(8), e02299.\u003c/li\u003e\n\u003cli\u003eGabrielsen, E. K. (1948). Effects of Different Chlorophyll Concentrations on Photosynthesis in Foliage Leaves. Physiologia Plantarum, 1(1), 5\u0026ndash;37. \u003c/li\u003e\n\u003cli\u003eAl-Alwani, M. A. M., Ludin, N. A., Mohamad, A. B., Kadhum, A. A. H., Baabbad, M. M., \u0026amp; Sopian, K. (2016). Optimization of dye extraction from Cordyline fruticosa via response surface methodology to produce a natural sensitizer for dye-sensitized solar cells. Results in Physics, 6, 520\u0026ndash;529. \u003c/li\u003e\n\u003cli\u003eNdeze, U. I., Aidan, J., Ezike, S. C., \u0026amp; Wansah, J. F. (2021). Comparative performances of nature-based dyes extracted from Baobab and Shea leaves photo-sensitizers for dye-sensitized solar cells (DSSCs). Current Research in Green and Sustainable Chemistry, 4. \u003c/li\u003e\n\u003cli\u003eKabir, F., Bhuiyan, M. M. H., Hossain, M. R., Bashar, H., Rahaman, M. S., Manir, M. S., Ullah, S. M., Uddin, S. S., Mollah, M. Z. I., Khan, R. A., Huque, S., \u0026amp; Khan, M. A. (2019). Improvement of efficiency of Dye Sensitized Solar Cells by optimizing the combination ratio of Natural Red and Yellow dyes. Optik, 179, 252\u0026ndash;258. \u003c/li\u003e\n\u003cli\u003eMunawaroh, H., adillah, G. F., Saputri, L. N. M. Z., Hanif, Q. A., Hidayat, R., \u0026amp; Wahyuningsih, S. (2016). The co-pigmentation of anthocyanin isolated from mangosteen pericarp ( Garcinia Mangostana L. ) as Natural Dye for Dye- Sensitized Solar Cells (DSSC). IOP Conference Series: Materials Science and Engineering, 107(1), 012061. \u003c/li\u003e\n\u003cli\u003ePrakash, P., Janarthanan, B., Ubaidullah, M., Al-Enizi, A. M., Shaikh, S. F., Alanazi, N. B., Alkhalifah, R. I., \u0026amp; Ilyas, M. (2023). Optimization, fabrication, and characterization of anthocyanin and carotenoid derivatives based dye-sensitized solar cells. Journal of King Saud University - Science, 35(4). \u003c/li\u003e\n\u003cli\u003eSalimian, J., Osfouri, S., Azin, R., \u0026amp; Jalali, T. (2022). Impacts of paste preparation methods on the porous TiO2nanostructure properties and naturally dye-sensitized solar cells performance. Journal of Materials Research and Technology, 18, 4816\u0026ndash;4833. \u003c/li\u003e\n\u003cli\u003eSee, S. C., Mercado, M. M., Corpuz, J. Z., Balbin, J., \u0026amp; Chua, E. (2020). Characterization of Electrical Quantities of a Grape Dye-Sensitized Solar Cell. IOP Conference Series: Earth and Environmental Science, 581(1). \u003c/li\u003e\n\u003cli\u003eHang, C. O. (2015). Natural Dye For Dye Sensitized Solar Cells (DSSCs) Using Mangosteen Adenium Obesum. \u003c/li\u003e\n\u003cli\u003eIsah Kimpa, M., Momoh, M., Uthman Isah, K., Nawawi Yahya, H., \u0026amp; Muhammed Ndamitso, M. (2012). Photoelectric Characterization of Dye Sensitized Solar Cells Using Natural Dye from Pawpaw Leaf and Flame Tree Flower as Sensitizers. Materials Sciences and Applications, 03(05), 281\u0026ndash;286. \u003c/li\u003e\n\u003cli\u003ePanaligan, T. R. L., Jr., Pagal, J. A. N., \u0026amp; Cancisio, S. J. J.(2023). Response Surface Methodology Design and Optimization of Inorganic Phosphate Removal from Simulated Wastewater Effluent Utilizing Caulerpa lentillifera Algal Powder. In Chemical Engineering Transactions (Vol. 106, pp. 61\u0026ndash;66).\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"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":"Grätzel cell, Combination Ratio, Dye Soaking Time, Light Soaking Time, Response Surface Methodology","lastPublishedDoi":"10.21203/rs.3.rs-6462691/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6462691/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThis study investigates the performance of combining polymer-rich natural dyes from Mangosteen pericarp and Ti plant leaves as sensitizers for Gr\u0026auml;tzel cells. The mangosteen pericarp is rich in natural polymers, including polyphenols, anthocyanins, and polysaccharides. These compounds enhance light absorption, electron transfer, film formation, and dye adhesion on the TiO\u003csub\u003e2\u003c/sub\u003e surface. The Ti plant leaves contain a high amount of chlorophyll. These compounds are well-known for their ability to capture light and act as photosensitizers, especially for Gr\u0026auml;tzel cells. Using Response Surface Methodology (RSM) with a Box-Behnken Design, the research evaluates the effects of dye combination ratios, dye soaking time (DST), and light soaking time (LST) on Gr\u0026auml;tzel cell efficiency. UV-Vis spectrophotometry was employed to analyze the light absorption characteristics of the natural dyes, revealing that a 2:8 ratio (20% Mangosteen pericarp dye and 80% Ti plant dye) exhibited the highest peak absorbance of 0.4685 at 665.452 nm. Gr\u0026auml;tzel cells with this 2:8 ratio achieved the highest average efficiency of 0.1989% under optimal conditions of 48 hours DST and 2.55 hours LST. While extended DST improved efficiency, longer LST and a higher proportion of Ti plant dye negatively impacted stability and performance. Statistical analysis indicated significant interactions among the parameters, with varying efficiency based on the dye composition and soaking durations.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e","manuscriptTitle":"Evaluation of Various Combination Ratios of Polymer-Based Dyes from Mangosteen Pericarp and Ti Plant for Grätzel Cell Efficiency Using Response Surface Methodology","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-04-22 09:33:26","doi":"10.21203/rs.3.rs-6462691/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":"06dc0deb-3d7b-42a0-bc9c-3937d9e5ad4d","owner":[],"postedDate":"April 22nd, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2025-09-29T09:39:12+00:00","versionOfRecord":[],"versionCreatedAt":"2025-04-22 09:33:26","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-6462691","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6462691","identity":"rs-6462691","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}