Use of CoNi-ZIF-derived Bimetallic-Doped Nitrogen-Rich Porous Carbon (CoNi-NC) Composite Bi 2 S 3 in Lithium-Sulfur Batteries

Use of CoNi-ZIF-derived Bimetallic-Doped Nitrogen-Rich Porous Carbon (CoNi-NC) Composite Bi 2 S 3 in Lithium-Sulfur Batteries | 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 Use of CoNi-ZIF-derived Bimetallic-Doped Nitrogen-Rich Porous Carbon (CoNi-NC) Composite Bi 2 S 3 in Lithium-Sulfur Batteries Zhifeng Zhao, Wangjun Feng, Yueping Niu, Wenting Hu, Wenxiao Su, and 2 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4636248/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 14 You are reading this latest preprint version Abstract Lithium-sulfur batteries have not been widely commercialized due to issues with poor conductivity of the active material and the shuttle effect, both of which are effectively addressed in this study. The porous carbon CoNi-NC, derived from high-temperature carbonization of the cobalt-nickel metal-organic framework CoNi-ZIF, was utilized as the carbon substrate. It exhibits excellent specific surface area and a well-developed pore structure, thereby optimizing the conductivity and sulfur-loading capacity of the material. The incorporation of polar Bi 2 S 3 effectively adsorbs polysulfides, retards the shuttle effect, and enhances the reaction kinetics of lithium-sulfur batteries. Electrochemical tests revealed that the CoNi-NC@Bi 2 S 3 electrode achieved a specific discharge capacity of 1107 mAh/g at a current density of 0.1 C, demonstrating excellent rate capability. Moreover, the cathode material maintained a specific discharge capacity of 796.5 mAh/g after 200 cycles at 0.2 C, indicating robust cycling stability. lithium-sulfur battery Bi2S3 Porous carbon Shuttle effect Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 1. Introduction Due to rising demand for electric vehicles and portable electronics, lithium-sulfur batteries, known for their ultra-high energy density, excellent theoretical specific capacity, and low production costs, have emerged as one of the most promising alternatives to conventional lithium-ion batteries. Nevertheless, the low conductivity of cathode materials and discharge products (LiS 2 /Li 2 S 2 ), coupled with the dissolution of intermediate lithium polysulfides during the reaction process, contribute to sluggish redox reaction kinetics and rapid capacity decay. These challenges pose significant hurdles for the practical application of lithium-sulfur batteries [ 1 ] . To mitigate these drawbacks, researchers have explored diverse materials to serve as hosts for elemental sulfur, aiming to attenuate shuttle effects and enhance the conductivity of cathode materials. For instance, materials such as graphene [ 2 ] , porous carbon materials [ 3 , 4 ] , metal phosphides [ 5 ] , metal oxides [ 6 , 7 ] , and metal selenides [ 8 , 9 ] have been demonstrated to suppresses polysulfide dissolution and thereby enhance the electrochemical performance of batteries. Among these, porous carbon is extensively employed in electrode and catalytic materials due to its excellent conductivity and cost-effectiveness in fabrication. However, nonpolar porous carbon materials exhibit weak interaction with polar polysulfides, leading to ineffective adsorption and insufficient suppression of the shuttle effect, thereby limiting their ability to enhance the electrochemical performance of batteries [ 10 , 11 ] . In recent years, heteroatom-doped porous carbon materials derived from direct calcination of MOF precursors have garnered significant interest. This is because the porous carbon synthesized via pyrolysis of MOF precursors possesses a distinct microporous structure that enhances elemental sulfur loading. Secondly, heteroatom-doped porous carbon materials enhance the conductivity of carbon-based materials and accelerate the reaction kinetics in lithium-sulfur batteries. The integration of metal compounds with advantageous catalytic and adsorption properties into MOF materials can effectively mitigate polysulfide dissolution and the shuttle effect, thus significantly prolonging the cycle life of lithium-sulfur batteries [ 12 – 14 ] . Metal sulfides have garnered significant attention owing to their abundant electronic structure and excellent semiconductor properties. When employed as cathode materials in lithium-sulfur batteries, they can engage in Lewis acid-base interactions with intermediate polysulfide products to mitigate the shuttle effect [ 15 , 16 ] . Among these, the N-type semiconductor material Bi 2 S 3 exhibits excellent chemical stability and catalytic activity, effectively mitigating the formation of the shuttle effect [ 17 ] . Nevertheless, the low conductivity of Bi 2 S 3 results in a sluggish ion transfer rate during the reaction process, thereby affecting the electrochemical performance of lithium-sulfur batteries relative. When CoNi-ZIF (Co-Ni zeolitic imidazolate framework) derived bimetal-doped nitrogen-rich porous carbon (CoNi-NC) is employed as a carbon-based material, its abundant pore size structure and excellent specific surface area effectively mitigate the volume expansion effect induced by the reaction [ 18 – 20 ] . Therefore, Bi 2 S 3 and CoNi-NC have been selected as cathode materials for lithium-sulfur batteries. On one hand, the superior specific surface area and conductivity of CoNi-NC enhance the loading of active substances and effectively mitigate the conductivity issues of Bi 2 S 3 . On the other hand, Bi 2 S 3 efficiently suppresses the shuttle effect of polysulfides. This composite material significantly enhances the electrochemical performance of lithium-sulfur batteries. 2 Experimental Procedure 2.1 Synthesis of CoNi-NC 6 mmol of Co(NO 3 ) 2 ·6H 2 O and Ni(NO 3 ) 2 ·6H 2 O were dissolved in 80 mL of methanol solution, stirred for 15 minutes, and designated as solution A. 24 mmol of 2-methylimidazole was dissolved in 80 mL of methanol and designated as solution B. Subsequently, the two solutions were mixed thoroughly by magnetic stirring and left to stand at room temperature for 18 hours. The supernatant was decanted, and the purple precipitate was collected. The CoNi-MOF sample was obtained after several washes with ethanol. The CoNi-MOF was placed in a nitrogen-filled tube furnace, heated to 800°C at a rate of 4°C/min, and maintained at this temperature for 4 hours. The resulting samples were designated as CoNi-NC. 2.2 Synthesis of CoNi-NC@Bi 2 S 3 composites Solution A was prepared initially by dispersing 0.15 g of CoNi-NC in 15 mL of deionized water under magnetic stirring. Additionally, 0.970 g of Bi(NO 3 ) 2 ·5H 2 O and 0.902 g of thioacetamide were dissolved in 60 mL of deionized water and stirred vigorously to form solution B. The two solutions were thoroughly mixed and transferred to a reaction vessel, where they were heated at 180°C for 24 hours. After allowing the reaction products to cool, they were washed multiple times with deionized water and absolute ethanol, followed by drying in an oven at 60°C for 18 hours. Subsequently, the samples were collected to obtain CoNi-NC@Bi 2 S 3 composites 2.3 Synthesis of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S composite cathode materials were synthesized via the melt diffusion method. CoNi-NC and CoNi-NC@Bi 2 S 3 were mixed with elemental sulfur in a mass ratio of 3:7 and ground thoroughly for thirty minutes. Afterwards, the ground product was transferred to an argon-filled glove box for 30 minutes to ensure thorough oxygen exchange within the reaction vessel. Subsequently, the reaction vessel was sealed and maintained at 155°C for 18 hours. This process yielded the CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S composite cathode materials. 2.4 Test characterization methods The crystal structure of the synthesized material was characterized using X-ray diffraction analysis (XRD) with a scanning angle range of 5° to 90°. X-ray photoelectron spectroscopy (XPS) was employed to analyze the chemical valence states of the composites. Simultaneously, the topography of the composite materials was examined using scanning electron microscopy (SEM), while transmission electron microscopy (TEM) was employed to investigate their finer structure. Furthermore, to determine the sulfur loading capacity of the composite, thermogravimetric analysis (TGA) was conducted. Additionally, Brunauer-Emmett-Teller (BET) specific surface area measurements were conducted to obtain pore size information of the material 2.5 Battery assembly and electrochemical testing The sulfur-containing composite electrode material, conductive agent (Super P), and binder (PVDF) were thoroughly mixed in a mass ratio of 7:2:1 to prepare a homogeneous slurry. Afterwards, the cathode slurry was coated onto carbon-coated aluminum foil using a coater, followed by drying at 60°C for 12 hours to produce the cathode electrode for the lithium-sulfur battery. The coin cell battery was assembled in an argon-filled glove box following this sequence: cathode casing, cathode material, electrolyte-soaked separator, electrolyte, metallic lithium foil, metallic spacer, metallic spring, and anode casing. After assembly, the battery was sealed using a button battery packaging machine and subsequently underwent electrochemical testing following a resting period. The galvanostatic charge-discharge (GCD) test was conducted using the Blue Electric CT3001A battery test system to analyze the battery's charge-discharge curves, cycle stability, and long-cycle performance under constant current conditions. The voltage range tested ranged from 1.7 V to 2.8 V. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were performed using the CS350H Electrochemical workstation by Wuhan Cosid. The cyclic voltammetry (CV) test analyzed the battery's redox processes over a voltage range of 1.7 V to 2.8 V, with a scan rate of 0.1 mV/s. Electrochemical impedance spectroscopy (EIS) was conducted using frequencies from 10 mHz to 100 kHz, applying a sinusoidal perturbation signal with an amplitude of ± 5 mV. 3. Results and discussion Figure 2 presents the X-ray diffraction (XRD) patterns of the CoNi-NC and CoNi-NC@Bi 2 S 3 composites. In Fig. 2 a, three distinct diffraction peaks for CoNi-NC are observed at 44.3°, 51.5°, and 76.1°, corresponding to the (111), (200), and (220) crystallographic planes as per the standard cards for Co (PDF#15–0806) and Ni (PDF#01-1258). Figure 2 b depicts the XRD pattern of CoNi-NC@Bi 2 S 3 , revealing a significant overlap with the standard card for Bi 2 S 3 (PDF#84–0279), indicating the successful synthesis of CoNi-NC@Bi 2 S 3 composites [ 21 ] . The specific surface area and pore structure of CoNi-NC@Bi 2 S 3 cathode materials were characterized using BET analysis. Figure 2 c displays the nitrogen adsorption-desorption isotherm of CoNi-NC@Bi 2 S 3 , which exhibits type IV isotherms, indicating that the composite primarily consists of mesopores [ 22 ] . Figure 2 d illustrates that the pore size distribution of CoNi-NC@Bi 2 S 3 material predominantly ranges from 2 to 7 nm. Incorporating mesoporous materials during the multiphase conversion of lithium-sulfur batteries enhances electron transfer rates, thereby improving the rate performance and cycling stability of these batteries [ 23 ] . Figure 3 a reveals that the CoNi-NC porous carbon material, obtained through high-temperature calcination, exhibits a polyhedral structure with a concave surface, enhancing its capability to support sulfur elements. Figure 3 b presents the scanning electron microscope image of CoNi-NC@Bi 2 S 3 , revealing rod-shaped Bi 2 S 3 clusters adhered to the surface of CoNi-NC. This observation indicates the successful preparation of the CoNi-NC@Bi 2 S 3 composite cathode material. The lattice structure and elemental distribution of CoNi-NC@Bi 2 S 3 materials were examined using transmission electron microscopy (TEM). As depicted in Fig. 3 c, the TEM images confirm the topography of CoNi-NC@Bi 2 S 3 observed via SEM. Figure 3 d presents the results obtained from high-resolution transmission electron microscopy (HR-TEM), depicting the (021) plane of Bi 2 S 3 with a lattice spacing of 0.325 nm. Figures 3 e-k depict the energy-dispersive X-ray spectroscopy (EDS) element mapping images of CoNi-NC@Bi 2 S 3 , revealing uniform distribution of Co, Ni, N, C, Bi, and S elements corresponding to their morphology. This observation further confirms the hydrothermal growth of Bi 2 S 3 on the surface of CoNi-NC. The sulfur loading capacity of the CoNi-NC@Bi 2 S 3 composite cathode materials was assessed via thermogravimetric analysis. As illustrated in Fig. 4 a, the sulfur loading capacity of CoNi-NC@Bi 2 S 3 was measured at 67.24%, which is conducive to enhancing the specific capacity and energy storage capability of lithium-sulfur batteries. The elemental bonding and binding energies of CoNi-NC@Bi 2 S 3 were analyzed using X-ray photoelectron spectroscopy. Figures 4 b-f illustrate the chemical bonds of Co 2p, Ni 2p, C 1s, N 1s, Bi 4f, and S 2p along with their respective binding energies. Figure 4 b depicts the X-ray photoelectron spectroscopy (XPS) spectrum of Co 2p, revealing six distinct peaks. The peaks at 806.3 eV and 786.8 eV are attributed to satellite peaks. Additionally, the peaks at 799.2 eV and 782.9 eV correspond to the spin-orbit components Co 2p 3/2 and Co 2p 1/2 , respectively, indicative of Co 2+ . Furthermore, spectral peaks at 794.9 eV (Co 2p 3/2 ) and 780.2 eV (Co 2p 1/2 ) are characteristic of Co 3+[ 24 , 25 ] . At the same time, the high-resolution spectra of Ni 2p exhibit six peaks, corresponding to two spin-orbit components and two satellite peaks. The first pair of doublets at 879.8 eV and 861.7 eV are attributed to the nickel satellite peaks. The second pair of doublets at 874.3 eV and 870.6 eV correspond to the Ni 2p 1/2 spin-orbit component. Additionally, the spectral peaks at 861.6 eV and 856.4 eV correspond to the Ni 2p 3/2 spin-orbit components, indicative of Ni 2+ and Ni 3+ , respectively [ 26 , 27 ] . Figure 4 d illustrates the X-ray photoelectron spectroscopy (XPS) spectrum of C 1s, displaying three spectral peaks at 284.7 eV, 285.3 eV, and 288.9 eV, corresponding to C-C, C-N, and O = C-O bonds, respectively [ 28 ] . Figure 4 e presents a high-resolution spectrum of N 1s in a CoNi-NC@Bi 2 S 3 material, where nitrogen atoms are doped into a carbon matrix in the forms of pyridinic N (399.8 eV), pyrrolic N (401.7 eV), and graphitic N (402.7 eV) [ 29 ] . Figure 4 f illustrates the spectral peaks of Bi 4f and S 2p. The binding energies of Bi 4f are observed at 164.0 eV (Bi 4f 7/2 ) and 158.7 eV (Bi 4f 5/2 ), while those of S 2p are found at 162.5 eV (S 2p 3/2 ) and 161.4 eV (S 2p 1/2 ). These findings are consistent with previous reports [ 30 ] . To investigate the electrochemical performance of CoNi-NC and CoNi-NC@Bi 2 S 3 as cathode materials, batteries were assembled in an argon-filled glove box. The rate performance and charge-discharge curves were evaluated using the Blue Electric CT3001A battery test system. Figures 5 a-b comprehensively illustrate the charge-discharge curves of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S composites at various magnifications. At a current density of 0.1 C, the discharge capacity of CoNi-NC@Bi 2 S 3 /S reaches 1107 mAh/g, whereas that of CoNi-NC is only 786 mAh/g. This difference suggests that incorporating transition metal sulfides onto the porous carbon surface effectively enhances the reaction kinetics of lithium-sulfur batteries. Moreover, Fig. 5 b reveals that the CoNi-NC@Bi 2 S 3 /S material maintains a distinct double discharge platform even at high rates, suggesting excellent cycling stability of the material [ 31 ] . Through analysis of the charge-discharge curves depicted in Fig. 5 a-b, three primary capacity plateaus can be distinguished. In the charge curve, the prominent plateau observed at 2.3V corresponds to the oxidation process from Li 2 S to S 8 (labeled as A 1 ) [ 32 ] . In the discharge curve, plateaus at 2.3V and 2.1V signify the reduction reactions from S 8 to soluble long-chain polysulfides (such as Li 2 S 4 , labeled as C 1 ) and from soluble polysulfides to Li 2 S (labeled as C 2 ), respectively [ 33 ] . The shuttle effect of soluble long-chain polysulfides (LiSPs) diminishes the capacity of the 2.1V plateau, resulting in subsequent capacity loss during cycling [ 34 ] . Thus, mitigating the shuttle effect and enhancing polysulfide conversion efficiency are crucial for improving the capacity and cycling stability of lithium-sulfur batteries. Figure 5 c compares the charge/discharge curves of the CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S electrodes at a current density of 0.1 C (where 1 C = 1672 mAh/g). The charge-discharge curve of lithium-sulfur batteries provides two fundamental metrics for assessing polysulfide conversion: the polarization potential (ΔE), which denotes the voltage difference between the discharge and charge platforms, and the specific capacity ratio of these two platforms during discharge [ 31 ] . Compared to CoNi-NC (ΔE = 258 mV), the CoNi-NC@Bi 2 S 3 /S electrode exhibited a reduced polarization potential (ΔE = 215 mV), attributable to its enhanced electrocatalytic activity in facilitating soluble long-chain polysulfides (LiPSs) conversion. At the same time, we also observed that the capacity of CoNi-NC@Bi 2 S 3 /S at the second discharge plateau significantly increased compared to porous carbon materials without Bi 2 S 3 , indicating enhanced conversion of long-chain polysulfides to Li 2 S. This is due to the adsorption and binding of soluble polysulfides by Bi 2 S 3 , which catalyzes their transformation into insoluble Li 2 S [ 35 ] . Figure 5 d compares the discharge specific capacities of two electrode materials at different rates. The test results demonstrate that the CoNi-NC@Bi 2 S 3 /S material exhibits excellent rate performance, achieving discharge capacities of 1107, 898, 701, 599, and 526 mAh/g at current densities of 0.1 C, 0.2 C, 0.5 C, 1 C, and 2 C, respectively. When the current density is returned to 0.1 C, the specific discharge capacity of the CoNi-NC@Bi 2 S 3 /S electrode remains at 908 mAh/g, with a capacity retention rate of 82.1%. In contrast, the CoNi-NC electrode shows a capacity retention rate of only 72.4%, indicating superior cycling stability of CoNi-NC@Bi 2 S 3 /S. To further investigate the cycling stability of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S cathode materials, assembled coin cell batteries were tested through 200 cycles at 0.2 C. As depicted in Fig. 6 a, the specific discharge capacity of the CoNi-NC@Bi 2 S 3 /S cathode material after 200 cycles is 796.5 mAh/g. Compared to CoNi-NC/S, CoNi-NC@Bi 2 S 3 /S exhibits superior cycling stability. This improvement is primarily attributed to the ability of Bi 2 S 3 to mitigate the shuttle effect and enhance the utilization rate of the cathode materials. The unique polyhedral structure of CoNi-NC effectively mitigates volume expansion effects, synergistically enhancing the electrochemical performance of lithium-sulfur batteries. The catalytic effect and ion transfer rate of the electrodes during cycling were further evaluated through cyclic voltammetry (CV) testing. Figure 6 b illustrates the CV curves of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S obtained at a scan rate of 0.1 mV/s. In a typical lithium-sulfur battery CV curve, there are two reduction peaks and one oxidation peak. The two reduction peaks at 2.3 V and 2.1 V correspond to the processes C 1 and C 2 in the discharge curve, where S 8 is reduced to the discharge product Li 2 S during multiphase conversion. Additionally, the oxidation peak at 2.4 V corresponds to the reverse multiphase conversion process, where Li 2 S oxidizes to the discharge product S 8 , reflecting the A 1 process in the charge curve [ 32 – 34 ] . Upon comparing the CV curves of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S, it is evident that the voltage gap (0.40 V) between the reduction and oxidation peaks of CoNi-NC@Bi 2 S 3 /S is significantly smaller than that of the CoNi-NC electrode (0.45 V). This indicates that the polarization effect of the CoNi-NC@Bi 2 S 3 /S electrode during the reaction is minimal. Furthermore, the lithium-ion diffusion coefficients of CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S during electrochemical reactions can be calculated using the Randles-Sevick equation (Eq. 1) [ 7 , 36 ] , and the results are presented in Table 1 . The results indicate that the addition of Bi 2 S 3 significantly enhances the ion diffusion rate of the battery. This suggests that the CoNi-NC@Bi 2 S 3 /S composite cathode material effectively enhances the electrochemical reaction performance of lithium-sulfur batteries. $$\begin{array}{c}{\text{I}}_{\text{p}}\text{=}\text{2.69}\text{×}\text{1}{\text{0}}^{\text{5}}{\text{n}}^{\frac{\text{3}}{\text{2}}}\text{A}{\text{D}}^{\frac{\text{1}}{\text{2}}}{\text{v}}^{\frac{\text{1}}{\text{2}}}\text{C}\#\left(\text{1}\right)\end{array}$$ where I p is the peak current, n is the number of electrons, A is the electrode area, D is the lithium-ion diffusion coefficient, C is the concentration of lithium ions in the electrolyte, and v is the scanning rate. Table 1 Calculated value of lithium-ion diffusion coefficient ( cm 2 /s ) CoNi-NC@Bi 2 S 3 CoNi-NC A1 3.38×10 − 8 1.38×10 − 8 C1 2.12×10 − 9 1.88×10 − 9 C2 8.54×10 − 9 1.41×10 − 9 The electron migration and electrode interface structure of lithium-sulfur batteries when using CoNi-NC@Bi 2 S 3 /S as the cathode material were further analyzed through AC impedance testing (EIS). Figure 7 a presents the EIS curves for CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S, characterized by semicircular arcs in the high-frequency region and oblique lines in the low-frequency region. These correspond to charge transfer resistance and Warburg diffusion resistance, respectively [ 37 ] . Comparing the curves of the samples reveals that the resistance of CoNi-NC@Bi 2 S 3 /S in the high-frequency region is lower than that of CoNi-NC/S, suggesting that CoNi-NC@Bi 2 S 3 /S exhibits higher charge transfer kinetics. Additionally, the real part and the reciprocal square root of the angular frequency of the impedance spectra for CoNi-NC/S and CoNi-NC@Bi 2 S 3 /S were subjected to linear fitting, facilitating the evaluation of ion diffusion rates during the reaction processes based on the fitting results. From Fig. 7 b, it is evident that the CoNi-NC@Bi 2 S 3 /S composites exhibit a low fitting slope, suggesting excellent ion diffusion characteristics. This property effectively enhances the reaction kinetics of lithium-sulfur batteries [ 38 , 39 ] . Conclusion In this study, CoNi-NC@Bi 2 S 3 composites were successfully synthesized via the hydrothermal method for application as cathodes in lithium-sulfur batteries. Through physical characterization and electrochemical measurements, it has been observed that CoNi-NC porous carbon exhibits excellent specific surface area and conductivity. These properties enable the composites to achieve high sulfur loading and excellent conductivity. Moreover, the mesoporous structure provided by the composites enhances electron transfer rates during the multiphase conversion process of lithium-sulfur batteries. Additionally, the polar Bi 2 S 3 effectively promotes the conversion of soluble polysulfides (LiPS), reduces capacity loss due to the shuttle effect, and enhances cycling stability. The synergistic effect of these two components demonstrates robust cycling stability and excellent reversible discharge specific capacity. When the CoNi-NC@Bi 2 S 3 /S electrode is cycled at a current density of 0.2 C for 200 cycles, the capacity retention remains at 88.7%, demonstrating that the incorporation of Bi 2 S 3 effectively enhances the cycling stability of lithium-sulfur batteries. Declarations Statement of Interest. The authors do not have any conflicts of interest that could affect the integrity of this paper. Author Contribution Zhifeng Zhao: Data curation and Writing—Original draft preparation. Wangjun Feng: Supervision. Yueping Niu: Investigation and Software. Wenting Hu: Investigation and Resources. Wenxiao Su: Investigation. Xiaoping Zheng: Project Administration. Li Zhang: Funding Acquisition. All authors reviewed the manuscript. Acknowledgements This work was supported by the National Natural Science Foundation of China (No. 21965019); HongLiu First-class Disciplines Development Program of Lanzhou University of Technology; Gansu College Innovation Fund Project of Gansu Provincial Department of Education (No.2022A-169). References Zhao H, Deng N, Yan J, et al (2018) A review on anode for lithium-sulfur batteries: Progress and prospects. Chemical Engineering Journal 347:343–365. https://doi.org/10.1016/j.cej.2018.04.112 Zhou G, Li L, Ma C, et al (2015) A graphene foam electrode with high sulfur loading for flexible and high energy Li-S batteries. 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ACS Appl Nano Mater 3:10914–10921. https://doi.org/10.1021/acsanm.0c02169 Asif M, Ali Z, Qiu H, et al (2020) Confined Polysulfide Shuttle by Nickel Disulfide Nanoparticles Encapsulated in Graphene Nanoshells Synthesized by Cooking Oil. ACS Appl Energy Mater 3:3541–3552. https://doi.org/10.1021/acsaem.0c00072 Zhao M, Hu J, Wu S, et al (2022) Hydrodeoxygenation of lignin-derived phenolics over facile prepared bimetallic RuCoN x /NC. Fuel 308:121979. https://doi.org/10.1016/j.fuel.2021.121979 Li P, Qiu Y, Liu S, et al (2019) Heterogeneous Mo 2 C/Fe 5 C 2 Nanoparticles Embedded in Nitrogen-Doped Carbon as Efficient Electrocatalysts for the Oxygen Reduction Reaction. Eur J Inorg Chem 2019:3235–3241. https://doi.org/10.1002/ejic.201900390 Ren S, Yang H, Zhang D, et al (2022) Excellent performance of the photoelectrocatalytic CO 2 reduction to formate by Bi 2 S 3 /ZIF-8 composite. Applied Surface Science 579:152206. https://doi.org/10.1016/j.apsusc.2021.152206 Zhang C, Biendicho JJ, Zhang T, et al (2019) Combined High Catalytic Activity and Efficient Polar Tubular Nanostructure in Urchin-Like Metallic NiCo 2 Se 4 for High‐Performance Lithium–Sulfur Batteries. Adv Funct Materials 29:1903842. https://doi.org/10.1002/adfm.201903842 Lei J, Liu T, Chen J, et al (2020) Exploring and Understanding the Roles of Li 2 S n and the Strategies to beyond Present Li-S Batteries. Chem 6:2533–2557. https://doi.org/10.1016/j.chempr.2020.06.032 Mikhaylik YV, Akridge JR (2004) Polysulfide Shuttle Study in the Li/S Battery System. J Electrochem Soc 151:A1969. https://doi.org/10.1149/1.1806394 Huang Y, Lin L, Zhang C, et al (2022) Recent Advances and Strategies toward Polysulfides Shuttle Inhibition for High-Performance Li–S Batteries. Advanced Science 9:2106004. https://doi.org/10.1002/advs.202106004 Li Y, Li T, Deng Y, et al (2024) Tuning the D-Band Center of Bi 2 S 3 MoS 2 Heterostructure Towards Superior Lithium‐Sulfur Batteries. Small 2401921. https://doi.org/10.1002/smll.202401921 Zhang X, Zheng J (2019) Controllable synthesis of highly active Au@Ni nanocatalyst supported on graphene oxide for electrochemical sensing of hydrazine. Applied Surface Science 493:1159–1166. https://doi.org/10.1016/j.apsusc.2019.07.136 Karakus A, Eroglu D (2019) Characterization of the Effect of Electrolyte-to-Sulfur Ratio on the Lithium-Sulfur Cell Resistance Using Electrochemical Impedance Spectroscopy Method. Meet Abstr MA2019-02:539–539. https://doi.org/10.1149/MA2019-02/6/539 Barchasz C, Leprêtre J-C, Alloin F, Patoux S (2012) New insights into the limiting parameters of the Li/S rechargeable cell. Journal of Power Sources 199:322–330. https://doi.org/10.1016/j.jpowsour.2011.07.021 Fu C, Venturi V, Kim J, et al (2020) Universal chemomechanical design rules for solid-ion conductors to prevent dendrite formation in lithium metal batteries. Nat Mater 19:758–766. https://doi.org/10.1038/s41563-020-0655-2 Additional Declarations No competing interests reported. Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Revision requested 20 Jul, 2024 Reviews received at journal 16 Jul, 2024 Reviews received at journal 14 Jul, 2024 Reviews received at journal 11 Jul, 2024 Reviewers agreed at journal 11 Jul, 2024 Reviews received at journal 05 Jul, 2024 Reviewers agreed at journal 03 Jul, 2024 Reviewers agreed at journal 03 Jul, 2024 Reviewers agreed at journal 03 Jul, 2024 Reviewers agreed at journal 03 Jul, 2024 Reviewers invited by journal 03 Jul, 2024 Editor assigned by journal 25 Jun, 2024 Submission checks completed at journal 25 Jun, 2024 First submitted to journal 25 Jun, 2024 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-4636248","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":327610637,"identity":"1e5aa657-bab3-4723-b88e-c0db652f96d1","order_by":0,"name":"Zhifeng Zhao","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Zhifeng","middleName":"","lastName":"Zhao","suffix":""},{"id":327610638,"identity":"62a25125-6ff0-4ce2-a5c3-b9d6c1dfccca","order_by":1,"name":"Wangjun Feng","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAy0lEQVRIiWNgGAWjYFCCgw+AhI0MmM1DnJbDBkAijYeBjXgtzCAth0nQYnDwMOPjgl/neQzuNzA+eNvGIG9OUMuBw8zGM/tu8xgcY2A2nNvGYLizgYAWswPnj0nz9oC1sEnztjEkGBwgqOUw+2/ennMgLUAGkVrYmHl+HADbwkyUFnugX6R5G5J5JI8lNkvOOSdhuIGQFskZhxk/8/yxk+M7fPjghzdlNvIEbWGQAKpgbAOxGBtAXELqgYAfpPAPEQpHwSgYBaNg5AIAWrVADkv34OEAAAAASUVORK5CYII=","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":true,"prefix":"","firstName":"Wangjun","middleName":"","lastName":"Feng","suffix":""},{"id":327610639,"identity":"a6d3efe0-c4e1-4f75-ab04-9a7717997368","order_by":2,"name":"Yueping Niu","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Yueping","middleName":"","lastName":"Niu","suffix":""},{"id":327610640,"identity":"f8e722e8-417b-4198-90c9-064b74484228","order_by":3,"name":"Wenting Hu","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Wenting","middleName":"","lastName":"Hu","suffix":""},{"id":327610641,"identity":"aa7fb76b-3fbf-41ba-bec6-e1355a37c2b3","order_by":4,"name":"Wenxiao Su","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Wenxiao","middleName":"","lastName":"Su","suffix":""},{"id":327610642,"identity":"e0f49637-32ec-4b2c-924b-06be0ccf5e89","order_by":5,"name":"Xiaoping Zheng","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Xiaoping","middleName":"","lastName":"Zheng","suffix":""},{"id":327610643,"identity":"d345a405-bb64-4588-a8a1-17456f4301fc","order_by":6,"name":"Li Zhang","email":"","orcid":"","institution":"Lanzhou University of Technology","correspondingAuthor":false,"prefix":"","firstName":"Li","middleName":"","lastName":"Zhang","suffix":""}],"badges":[],"createdAt":"2024-06-25 11:59:06","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4636248/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4636248/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":60485378,"identity":"21fb1546-3910-4d5c-9ff6-0461959087a8","added_by":"auto","created_at":"2024-07-17 09:24:42","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":373397,"visible":true,"origin":"","legend":"\u003cp\u003eFlow chart of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e synthesis\u003c/p\u003e","description":"","filename":"floatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/cee0ba81310b7b1b6e239a3b.png"},{"id":60486210,"identity":"fddd5310-d854-4a5b-8c1d-bfc129a62277","added_by":"auto","created_at":"2024-07-17 09:32:42","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":672912,"visible":true,"origin":"","legend":"\u003cp\u003eXRD plot of \u003cstrong\u003ea)\u003c/strong\u003e CoNi-NC, \u003cstrong\u003eb) \u003c/strong\u003eXRD plot of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, \u003cstrong\u003ec) \u003c/strong\u003enitrogen adsorption-desorption curve of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, and \u003cstrong\u003ed)\u003c/strong\u003e pore size distribution profile of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e","description":"","filename":"floatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/ee487d6813a5d5be84e1fd0c.png"},{"id":60485380,"identity":"0f3a717a-dcd4-4152-b19e-665acc809547","added_by":"auto","created_at":"2024-07-17 09:24:42","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":1228160,"visible":true,"origin":"","legend":"\u003cp\u003eSEM plot of \u003cstrong\u003ea)\u003c/strong\u003e CoNi-NC, \u003cstrong\u003eb) \u003c/strong\u003eSEM plot of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, \u003cstrong\u003ec-d)\u003c/strong\u003e TEM plot of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, and \u003cstrong\u003ee-k)\u003c/strong\u003e element distribution of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e","description":"","filename":"floatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/c9427ca8385f58de0bc60b79.png"},{"id":60486212,"identity":"e15d192e-285d-47cc-b86c-ced06d9bb592","added_by":"auto","created_at":"2024-07-17 09:32:42","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":1309174,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea)\u003c/strong\u003e TGA plot of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, XPS spectrum of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e \u003cstrong\u003eb) \u003c/strong\u003eCo 2p,\u003cstrong\u003e c) \u003c/strong\u003eNi 2p, \u003cstrong\u003ed) \u003c/strong\u003eC 1s, \u003cstrong\u003ee)\u003c/strong\u003e N 1s, \u003cstrong\u003ef)\u003c/strong\u003e Bi 4f and S 2p\u003c/p\u003e","description":"","filename":"floatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/c895267fcda2feb295746557.png"},{"id":60486785,"identity":"6b1e468b-d587-4095-b4a7-8ea3d64b5d7e","added_by":"auto","created_at":"2024-07-17 09:40:42","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":983007,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea)\u003c/strong\u003e the first charge-discharge curves of CoNi-NC at different discharge rates, \u003cstrong\u003eb) \u003c/strong\u003ethe first charge-discharge curves of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e at different discharge rates, \u003cstrong\u003ec) \u003c/strong\u003ethe first charge-discharge curves of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e at 0.1 C, and \u003cstrong\u003ed) \u003c/strong\u003ethe rate performance of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e","description":"","filename":"floatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/8f132c956e0516dc1c4f13a9.png"},{"id":60485383,"identity":"1d766ce1-9eec-4efd-b8ea-f0cf414d998b","added_by":"auto","created_at":"2024-07-17 09:24:42","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":494530,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea)\u003c/strong\u003e Cycling performance and Coulomb efficiency plots of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e at 0.2 C current density, \u003cstrong\u003eb)\u003c/strong\u003e CV curves of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e","description":"","filename":"floatimage6.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/4468409a43e9ccdd3834f79c.png"},{"id":60486209,"identity":"5989fbde-fc8e-4349-a495-ec832f463fb0","added_by":"auto","created_at":"2024-07-17 09:32:42","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":96364,"visible":true,"origin":"","legend":"\u003cp\u003e\u003cstrong\u003ea) \u003c/strong\u003eEIS curves of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e,\u003cstrong\u003e b)\u003c/strong\u003e fitting curves of the real part of the impedance of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e and the reciprocal square root of the angular frequency\u003c/p\u003e","description":"","filename":"floatimage7.png","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/1354ca3f8c228ef0ddc90453.png"},{"id":60487528,"identity":"2160fd8e-585e-4442-ba3d-de07bb19cd3b","added_by":"auto","created_at":"2024-07-17 09:48:46","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":6605045,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4636248/v1/9d54ceb9-542e-4c74-b7ba-e26c2f55dd51.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Use of CoNi-ZIF-derived Bimetallic-Doped Nitrogen-Rich Porous Carbon (CoNi-NC) Composite Bi 2 S 3 in Lithium-Sulfur Batteries","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eDue to rising demand for electric vehicles and portable electronics, lithium-sulfur batteries, known for their ultra-high energy density, excellent theoretical specific capacity, and low production costs, have emerged as one of the most promising alternatives to conventional lithium-ion batteries. Nevertheless, the low conductivity of cathode materials and discharge products (LiS\u003csub\u003e2\u003c/sub\u003e/Li\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e), coupled with the dissolution of intermediate lithium polysulfides during the reaction process, contribute to sluggish redox reaction kinetics and rapid capacity decay. These challenges pose significant hurdles for the practical application of lithium-sulfur batteries\u003csup\u003e[\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eTo mitigate these drawbacks, researchers have explored diverse materials to serve as hosts for elemental sulfur, aiming to attenuate shuttle effects and enhance the conductivity of cathode materials. For instance, materials such as graphene\u003csup\u003e[\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e]\u003c/sup\u003e, porous carbon materials\u003csup\u003e[\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e, \u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]\u003c/sup\u003e, metal phosphides\u003csup\u003e[\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]\u003c/sup\u003e, metal oxides\u003csup\u003e[\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]\u003c/sup\u003e, and metal selenides\u003csup\u003e[\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e, \u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]\u003c/sup\u003e have been demonstrated to suppresses polysulfide dissolution and thereby enhance the electrochemical performance of batteries. Among these, porous carbon is extensively employed in electrode and catalytic materials due to its excellent conductivity and cost-effectiveness in fabrication. However, nonpolar porous carbon materials exhibit weak interaction with polar polysulfides, leading to ineffective adsorption and insufficient suppression of the shuttle effect, thereby limiting their ability to enhance the electrochemical performance of batteries\u003csup\u003e[\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e, \u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eIn recent years, heteroatom-doped porous carbon materials derived from direct calcination of MOF precursors have garnered significant interest. This is because the porous carbon synthesized via pyrolysis of MOF precursors possesses a distinct microporous structure that enhances elemental sulfur loading. Secondly, heteroatom-doped porous carbon materials enhance the conductivity of carbon-based materials and accelerate the reaction kinetics in lithium-sulfur batteries. The integration of metal compounds with advantageous catalytic and adsorption properties into MOF materials can effectively mitigate polysulfide dissolution and the shuttle effect, thus significantly prolonging the cycle life of lithium-sulfur batteries\u003csup\u003e[\u003cspan additionalcitationids=\"CR13\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eMetal sulfides have garnered significant attention owing to their abundant electronic structure and excellent semiconductor properties. When employed as cathode materials in lithium-sulfur batteries, they can engage in Lewis acid-base interactions with intermediate polysulfide products to mitigate the shuttle effect\u003csup\u003e[\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e, \u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]\u003c/sup\u003e. Among these, the N-type semiconductor material Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e exhibits excellent chemical stability and catalytic activity, effectively mitigating the formation of the shuttle effect\u003csup\u003e[\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]\u003c/sup\u003e. Nevertheless, the low conductivity of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e results in a sluggish ion transfer rate during the reaction process, thereby affecting the electrochemical performance of lithium-sulfur batteries relative. When CoNi-ZIF (Co-Ni zeolitic imidazolate framework) derived bimetal-doped nitrogen-rich porous carbon (CoNi-NC) is employed as a carbon-based material, its abundant pore size structure and excellent specific surface area effectively mitigate the volume expansion effect induced by the reaction\u003csup\u003e[\u003cspan additionalcitationids=\"CR19\" citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]\u003c/sup\u003e. Therefore, Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e and CoNi-NC have been selected as cathode materials for lithium-sulfur batteries. On one hand, the superior specific surface area and conductivity of CoNi-NC enhance the loading of active substances and effectively mitigate the conductivity issues of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e. On the other hand, Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e efficiently suppresses the shuttle effect of polysulfides. This composite material significantly enhances the electrochemical performance of lithium-sulfur batteries.\u003c/p\u003e"},{"header":"2 Experimental Procedure","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Synthesis of CoNi-NC\u003c/h2\u003e \u003cp\u003e6 mmol of Co(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO and Ni(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026middot;6H\u003csub\u003e2\u003c/sub\u003eO were dissolved in 80 mL of methanol solution, stirred for 15 minutes, and designated as solution A. 24 mmol of 2-methylimidazole was dissolved in 80 mL of methanol and designated as solution B. Subsequently, the two solutions were mixed thoroughly by magnetic stirring and left to stand at room temperature for 18 hours. The supernatant was decanted, and the purple precipitate was collected. The CoNi-MOF sample was obtained after several washes with ethanol. The CoNi-MOF was placed in a nitrogen-filled tube furnace, heated to 800\u0026deg;C at a rate of 4\u0026deg;C/min, and maintained at this temperature for 4 hours. The resulting samples were designated as CoNi-NC.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Synthesis of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composites\u003c/h2\u003e \u003cp\u003eSolution A was prepared initially by dispersing 0.15 g of CoNi-NC in 15 mL of deionized water under magnetic stirring. Additionally, 0.970 g of Bi(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026middot;5H\u003csub\u003e2\u003c/sub\u003eO and 0.902 g of thioacetamide were dissolved in 60 mL of deionized water and stirred vigorously to form solution B. The two solutions were thoroughly mixed and transferred to a reaction vessel, where they were heated at 180\u0026deg;C for 24 hours. After allowing the reaction products to cool, they were washed multiple times with deionized water and absolute ethanol, followed by drying in an oven at 60\u0026deg;C for 18 hours. Subsequently, the samples were collected to obtain CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composites\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Synthesis of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S\u003c/h2\u003e \u003cp\u003eCoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S composite cathode materials were synthesized via the melt diffusion method. CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e were mixed with elemental sulfur in a mass ratio of 3:7 and ground thoroughly for thirty minutes. Afterwards, the ground product was transferred to an argon-filled glove box for 30 minutes to ensure thorough oxygen exchange within the reaction vessel. Subsequently, the reaction vessel was sealed and maintained at 155\u0026deg;C for 18 hours. This process yielded the CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S composite cathode materials.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e2.4 Test characterization methods\u003c/h2\u003e \u003cp\u003eThe crystal structure of the synthesized material was characterized using X-ray diffraction analysis (XRD) with a scanning angle range of 5\u0026deg; to 90\u0026deg;. X-ray photoelectron spectroscopy (XPS) was employed to analyze the chemical valence states of the composites. Simultaneously, the topography of the composite materials was examined using scanning electron microscopy (SEM), while transmission electron microscopy (TEM) was employed to investigate their finer structure. Furthermore, to determine the sulfur loading capacity of the composite, thermogravimetric analysis (TGA) was conducted. Additionally, Brunauer-Emmett-Teller (BET) specific surface area measurements were conducted to obtain pore size information of the material\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e2.5 Battery assembly and electrochemical testing\u003c/h2\u003e \u003cp\u003eThe sulfur-containing composite electrode material, conductive agent (Super P), and binder (PVDF) were thoroughly mixed in a mass ratio of 7:2:1 to prepare a homogeneous slurry. Afterwards, the cathode slurry was coated onto carbon-coated aluminum foil using a coater, followed by drying at 60\u0026deg;C for 12 hours to produce the cathode electrode for the lithium-sulfur battery.\u003c/p\u003e \u003cp\u003eThe coin cell battery was assembled in an argon-filled glove box following this sequence: cathode casing, cathode material, electrolyte-soaked separator, electrolyte, metallic lithium foil, metallic spacer, metallic spring, and anode casing. After assembly, the battery was sealed using a button battery packaging machine and subsequently underwent electrochemical testing following a resting period.\u003c/p\u003e \u003cp\u003eThe galvanostatic charge-discharge (GCD) test was conducted using the Blue Electric CT3001A battery test system to analyze the battery's charge-discharge curves, cycle stability, and long-cycle performance under constant current conditions. The voltage range tested ranged from 1.7 V to 2.8 V.\u003c/p\u003e \u003cp\u003eCyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were performed using the CS350H Electrochemical workstation by Wuhan Cosid. The cyclic voltammetry (CV) test analyzed the battery's redox processes over a voltage range of 1.7 V to 2.8 V, with a scan rate of 0.1 mV/s. Electrochemical impedance spectroscopy (EIS) was conducted using frequencies from 10 mHz to 100 kHz, applying a sinusoidal perturbation signal with an amplitude of \u0026plusmn;\u0026thinsp;5 mV.\u003c/p\u003e \u003c/div\u003e"},{"header":"3. Results and discussion","content":"\u003cp\u003eFigure \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e presents the X-ray diffraction (XRD) patterns of the CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composites. In Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea, three distinct diffraction peaks for CoNi-NC are observed at 44.3°, 51.5°, and 76.1°, corresponding to the (111), (200), and (220) crystallographic planes as per the standard cards for Co (PDF#15–0806) and Ni (PDF#01-1258). Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003eb depicts the XRD pattern of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, revealing a significant overlap with the standard card for Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e (PDF#84–0279), indicating the successful synthesis of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composites\u003csup\u003e[\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe specific surface area and pore structure of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e cathode materials were characterized using BET analysis. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ec displays the nitrogen adsorption-desorption isotherm of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, which exhibits type IV isotherms, indicating that the composite primarily consists of mesopores\u003csup\u003e[\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed illustrates that the pore size distribution of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e material predominantly ranges from 2 to 7 nm. Incorporating mesoporous materials during the multiphase conversion of lithium-sulfur batteries enhances electron transfer rates, thereby improving the rate performance and cycling stability of these batteries\u003csup\u003e[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea reveals that the CoNi-NC porous carbon material, obtained through high-temperature calcination, exhibits a polyhedral structure with a concave surface, enhancing its capability to support sulfur elements. Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb presents the scanning electron microscope image of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, revealing rod-shaped Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e clusters adhered to the surface of CoNi-NC. This observation indicates the successful preparation of the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composite cathode material. The lattice structure and elemental distribution of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e materials were examined using transmission electron microscopy (TEM). As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ec, the TEM images confirm the topography of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e observed via SEM. Figure\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ed presents the results obtained from high-resolution transmission electron microscopy (HR-TEM), depicting the (021) plane of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e with a lattice spacing of 0.325 nm. Figures\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ee-k depict the energy-dispersive X-ray spectroscopy (EDS) element mapping images of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, revealing uniform distribution of Co, Ni, N, C, Bi, and S elements corresponding to their morphology. This observation further confirms the hydrothermal growth of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e on the surface of CoNi-NC.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eThe sulfur loading capacity of the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composite cathode materials was assessed via thermogravimetric analysis. As illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ea, the sulfur loading capacity of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e was measured at 67.24%, which is conducive to enhancing the specific capacity and energy storage capability of lithium-sulfur batteries. The elemental bonding and binding energies of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e were analyzed using X-ray photoelectron spectroscopy. Figures\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb-f illustrate the chemical bonds of Co 2p, Ni 2p, C 1s, N 1s, Bi 4f, and S 2p along with their respective binding energies. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003eb depicts the X-ray photoelectron spectroscopy (XPS) spectrum of Co 2p, revealing six distinct peaks. The peaks at 806.3 eV and 786.8 eV are attributed to satellite peaks. Additionally, the peaks at 799.2 eV and 782.9 eV correspond to the spin-orbit components Co 2p\u003csub\u003e3/2\u003c/sub\u003e and Co 2p\u003csub\u003e1/2\u003c/sub\u003e, respectively, indicative of Co\u003csup\u003e2+\u003c/sup\u003e. Furthermore, spectral peaks at 794.9 eV (Co 2p\u003csub\u003e3/2\u003c/sub\u003e) and 780.2 eV (Co 2p\u003csub\u003e1/2\u003c/sub\u003e) are characteristic of Co\u003csup\u003e3+[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e, \u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]\u003c/sup\u003e. At the same time, the high-resolution spectra of Ni 2p exhibit six peaks, corresponding to two spin-orbit components and two satellite peaks. The first pair of doublets at 879.8 eV and 861.7 eV are attributed to the nickel satellite peaks. The second pair of doublets at 874.3 eV and 870.6 eV correspond to the Ni 2p\u003csub\u003e1/2\u003c/sub\u003e spin-orbit component. Additionally, the spectral peaks at 861.6 eV and 856.4 eV correspond to the Ni 2p\u003csub\u003e3/2\u003c/sub\u003e spin-orbit components, indicative of Ni\u003csup\u003e2+\u003c/sup\u003e and Ni\u003csup\u003e3+\u003c/sup\u003e, respectively\u003csup\u003e[\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ed illustrates the X-ray photoelectron spectroscopy (XPS) spectrum of C 1s, displaying three spectral peaks at 284.7 eV, 285.3 eV, and 288.9 eV, corresponding to C-C, C-N, and O = C-O bonds, respectively\u003csup\u003e[\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ee presents a high-resolution spectrum of N 1s in a CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e material, where nitrogen atoms are doped into a carbon matrix in the forms of pyridinic N (399.8 eV), pyrrolic N (401.7 eV), and graphitic N (402.7 eV)\u003csup\u003e[\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]\u003c/sup\u003e. Figure\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003ef illustrates the spectral peaks of Bi 4f and S 2p. The binding energies of Bi 4f are observed at 164.0 eV (Bi 4f\u003csub\u003e7/2\u003c/sub\u003e) and 158.7 eV (Bi 4f\u003csub\u003e5/2\u003c/sub\u003e), while those of S 2p are found at 162.5 eV (S 2p\u003csub\u003e3/2\u003c/sub\u003e) and 161.4 eV (S 2p\u003csub\u003e1/2\u003c/sub\u003e). These findings are consistent with previous reports\u003csup\u003e[\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eTo investigate the electrochemical performance of CoNi-NC and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e as cathode materials, batteries were assembled in an argon-filled glove box. The rate performance and charge-discharge curves were evaluated using the Blue Electric CT3001A battery test system. Figures\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea-b comprehensively illustrate the charge-discharge curves of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S composites at various magnifications. At a current density of 0.1 C, the discharge capacity of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S reaches 1107 mAh/g, whereas that of CoNi-NC is only 786 mAh/g. This difference suggests that incorporating transition metal sulfides onto the porous carbon surface effectively enhances the reaction kinetics of lithium-sulfur batteries. Moreover, Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb reveals that the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S material maintains a distinct double discharge platform even at high rates, suggesting excellent cycling stability of the material\u003csup\u003e[\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003eThrough analysis of the charge-discharge curves depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea-b, three primary capacity plateaus can be distinguished. In the charge curve, the prominent plateau observed at 2.3V corresponds to the oxidation process from Li\u003csub\u003e2\u003c/sub\u003eS to S\u003csub\u003e8\u003c/sub\u003e (labeled as A\u003csub\u003e1\u003c/sub\u003e)\u003csup\u003e[\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]\u003c/sup\u003e. In the discharge curve, plateaus at 2.3V and 2.1V signify the reduction reactions from S\u003csub\u003e8\u003c/sub\u003e to soluble long-chain polysulfides (such as Li\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e4\u003c/sub\u003e, labeled as C\u003csub\u003e1\u003c/sub\u003e) and from soluble polysulfides to Li\u003csub\u003e2\u003c/sub\u003eS (labeled as C\u003csub\u003e2\u003c/sub\u003e), respectively\u003csup\u003e[\u003cspan citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e]\u003c/sup\u003e. The shuttle effect of soluble long-chain polysulfides (LiSPs) diminishes the capacity of the 2.1V plateau, resulting in subsequent capacity loss during cycling\u003csup\u003e[\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]\u003c/sup\u003e. Thus, mitigating the shuttle effect and enhancing polysulfide conversion efficiency are crucial for improving the capacity and cycling stability of lithium-sulfur batteries.\u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec compares the charge/discharge curves of the CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S electrodes at a current density of 0.1 C (where 1 C = 1672 mAh/g). The charge-discharge curve of lithium-sulfur batteries provides two fundamental metrics for assessing polysulfide conversion: the polarization potential (ΔE), which denotes the voltage difference between the discharge and charge platforms, and the specific capacity ratio of these two platforms during discharge\u003csup\u003e[\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]\u003c/sup\u003e. Compared to CoNi-NC (ΔE = 258 mV), the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S electrode exhibited a reduced polarization potential (ΔE = 215 mV), attributable to its enhanced electrocatalytic activity in facilitating soluble long-chain polysulfides (LiPSs) conversion. At the same time, we also observed that the capacity of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S at the second discharge plateau significantly increased compared to porous carbon materials without Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, indicating enhanced conversion of long-chain polysulfides to Li\u003csub\u003e2\u003c/sub\u003eS. This is due to the adsorption and binding of soluble polysulfides by Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e, which catalyzes their transformation into insoluble Li\u003csub\u003e2\u003c/sub\u003eS\u003csup\u003e[\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFigure \u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed compares the discharge specific capacities of two electrode materials at different rates. The test results demonstrate that the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S material exhibits excellent rate performance, achieving discharge capacities of 1107, 898, 701, 599, and 526 mAh/g at current densities of 0.1 C, 0.2 C, 0.5 C, 1 C, and 2 C, respectively. When the current density is returned to 0.1 C, the specific discharge capacity of the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S electrode remains at 908 mAh/g, with a capacity retention rate of 82.1%. In contrast, the CoNi-NC electrode shows a capacity retention rate of only 72.4%, indicating superior cycling stability of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S.\u003c/p\u003e \u003cp\u003eTo further investigate the cycling stability of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S cathode materials, assembled coin cell batteries were tested through 200 cycles at 0.2 C. As depicted in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea, the specific discharge capacity of the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S cathode material after 200 cycles is 796.5 mAh/g. Compared to CoNi-NC/S, CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S exhibits superior cycling stability. This improvement is primarily attributed to the ability of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e to mitigate the shuttle effect and enhance the utilization rate of the cathode materials. The unique polyhedral structure of CoNi-NC effectively mitigates volume expansion effects, synergistically enhancing the electrochemical performance of lithium-sulfur batteries. The catalytic effect and ion transfer rate of the electrodes during cycling were further evaluated through cyclic voltammetry (CV) testing. Figure\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003eb illustrates the CV curves of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S obtained at a scan rate of 0.1 mV/s. In a typical lithium-sulfur battery CV curve, there are two reduction peaks and one oxidation peak. The two reduction peaks at 2.3 V and 2.1 V correspond to the processes C\u003csub\u003e1\u003c/sub\u003e and C\u003csub\u003e2\u003c/sub\u003e in the discharge curve, where S\u003csub\u003e8\u003c/sub\u003e is reduced to the discharge product Li\u003csub\u003e2\u003c/sub\u003eS during multiphase conversion. Additionally, the oxidation peak at 2.4 V corresponds to the reverse multiphase conversion process, where Li\u003csub\u003e2\u003c/sub\u003eS oxidizes to the discharge product S\u003csub\u003e8\u003c/sub\u003e, reflecting the A\u003csub\u003e1\u003c/sub\u003e process in the charge curve\u003csup\u003e[\u003cspan additionalcitationids=\"CR33\" citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e–\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]\u003c/sup\u003e. Upon comparing the CV curves of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S, it is evident that the voltage gap (0.40 V) between the reduction and oxidation peaks of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S is significantly smaller than that of the CoNi-NC electrode (0.45 V). This indicates that the polarization effect of the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S electrode during the reaction is minimal.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eFurthermore, the lithium-ion diffusion coefficients of CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S during electrochemical reactions can be calculated using the Randles-Sevick equation (Eq.\u0026nbsp;1)\u003csup\u003e[\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e, \u003cspan citationid=\"CR36\" class=\"CitationRef\"\u003e36\u003c/span\u003e]\u003c/sup\u003e, and the results are presented in Table\u0026nbsp;\u003cspan refid=\"Tab1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. The results indicate that the addition of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e significantly enhances the ion diffusion rate of the battery. This suggests that the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S composite cathode material effectively enhances the electrochemical reaction performance of lithium-sulfur batteries.\u003c/p\u003e\u003cdiv id=\"Equa\" class=\"Equation\"\u003e\u003cdiv format=\"TEX\" class=\"mathdisplay\" id=\"FileID_Equa\" name=\"EquationSource\"\u003e\n$$\\begin{array}{c}{\\text{I}}_{\\text{p}}\\text{=}\\text{2.69}\\text{×}\\text{1}{\\text{0}}^{\\text{5}}{\\text{n}}^{\\frac{\\text{3}}{\\text{2}}}\\text{A}{\\text{D}}^{\\frac{\\text{1}}{\\text{2}}}{\\text{v}}^{\\frac{\\text{1}}{\\text{2}}}\\text{C}\\#\\left(\\text{1}\\right)\\end{array}$$\u003c/div\u003e\u003c/div\u003e\u003cp\u003e\u003c/p\u003e \u003cp\u003ewhere \u003cem\u003eI\u003c/em\u003e\u003csub\u003e\u003cem\u003ep\u003c/em\u003e\u003c/sub\u003e is the peak current, \u003cem\u003en\u003c/em\u003e is the number of electrons, \u003cem\u003eA\u003c/em\u003e is the electrode area, \u003cem\u003eD\u003c/em\u003e is the lithium-ion diffusion coefficient, \u003cem\u003eC\u003c/em\u003e is the concentration of lithium ions in the electrolyte, and \u003cem\u003ev\u003c/em\u003e is the scanning rate.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e\u003cdiv class=\"gridtable\"\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\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\u003eCalculated value of lithium-ion diffusion coefficient (\u003cb\u003ecm\u003c/b\u003e\u003csup\u003e\u003cb\u003e2\u003c/b\u003e\u003c/sup\u003e\u003cb\u003e/s\u003c/b\u003e)\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e\u003ccolgroup cols=\"3\"\u003e\u003c/colgroup\u003e\u003cthead\u003e\u003ctr\u003e\u003cth align=\"left\" colname=\"c1\"\u003e\u0026nbsp;\u003c/th\u003e\u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eCoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e \u003c/th\u003e\u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003eCoNi-NC\u003c/p\u003e \u003c/th\u003e\u003c/tr\u003e\u003c/thead\u003e\u003ctbody\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003eA1\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c2\"\u003e \u003cp\u003e3.38×10\u003csup\u003e− 8\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c3\"\u003e \u003cp\u003e1.38×10\u003csup\u003e− 8\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003eC1\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c2\"\u003e \u003cp\u003e2.12×10\u003csup\u003e− 9\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c3\"\u003e \u003cp\u003e1.88×10\u003csup\u003e− 9\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003c/tr\u003e\u003ctr\u003e\u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cb\u003eC2\u003c/b\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c2\"\u003e \u003cp\u003e8.54×10\u003csup\u003e− 9\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003ctd align=\"char\" char=\"×\" colname=\"c3\"\u003e \u003cp\u003e1.41×10\u003csup\u003e− 9\u003c/sup\u003e\u003c/p\u003e \u003c/td\u003e\u003c/tr\u003e\u003c/tbody\u003e\u003c/table\u003e\u003c/div\u003e \u003cp\u003e\u003c/p\u003e \u003cp\u003eThe electron migration and electrode interface structure of lithium-sulfur batteries when using CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S as the cathode material were further analyzed through AC impedance testing (EIS). Figure\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea presents the EIS curves for CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S, characterized by semicircular arcs in the high-frequency region and oblique lines in the low-frequency region. These correspond to charge transfer resistance and Warburg diffusion resistance, respectively\u003csup\u003e[\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e]\u003c/sup\u003e. Comparing the curves of the samples reveals that the resistance of CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S in the high-frequency region is lower than that of CoNi-NC/S, suggesting that CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S exhibits higher charge transfer kinetics. Additionally, the real part and the reciprocal square root of the angular frequency of the impedance spectra for CoNi-NC/S and CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S were subjected to linear fitting, facilitating the evaluation of ion diffusion rates during the reaction processes based on the fitting results. From Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb, it is evident that the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S composites exhibit a low fitting slope, suggesting excellent ion diffusion characteristics. This property effectively enhances the reaction kinetics of lithium-sulfur batteries\u003csup\u003e[\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e, \u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]\u003c/sup\u003e.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e "},{"header":"Conclusion","content":"\u003cp\u003eIn this study, CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e composites were successfully synthesized via the hydrothermal method for application as cathodes in lithium-sulfur batteries. Through physical characterization and electrochemical measurements, it has been observed that CoNi-NC porous carbon exhibits excellent specific surface area and conductivity. These properties enable the composites to achieve high sulfur loading and excellent conductivity. Moreover, the mesoporous structure provided by the composites enhances electron transfer rates during the multiphase conversion process of lithium-sulfur batteries. Additionally, the polar Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e effectively promotes the conversion of soluble polysulfides (LiPS), reduces capacity loss due to the shuttle effect, and enhances cycling stability. The synergistic effect of these two components demonstrates robust cycling stability and excellent reversible discharge specific capacity. When the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e/S electrode is cycled at a current density of 0.2 C for 200 cycles, the capacity retention remains at 88.7%, demonstrating that the incorporation of Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e effectively enhances the cycling stability of lithium-sulfur batteries.\u003c/p\u003e"},{"header":"Declarations","content":" \u003cp\u003e \u003cb\u003eStatement of Interest.\u003c/b\u003e The authors do not have any conflicts of interest that could affect the integrity of this paper.\u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eZhifeng Zhao: Data curation and Writing\u0026mdash;Original draft preparation. Wangjun Feng: Supervision. Yueping Niu: Investigation and Software. Wenting Hu: Investigation and Resources. Wenxiao Su: Investigation. Xiaoping Zheng: Project Administration. Li Zhang: Funding Acquisition. All authors reviewed the manuscript.\u003c/p\u003e\u003ch2\u003eAcknowledgements\u003c/h2\u003e \u003cp\u003eThis work was supported by the National Natural Science Foundation of China (No. 21965019); HongLiu First-class Disciplines Development Program of Lanzhou University of Technology; Gansu College Innovation Fund Project of Gansu Provincial Department of Education (No.2022A-169).\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eZhao H, Deng N, Yan J, et al (2018) A review on anode for lithium-sulfur batteries: Progress and prospects. 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Nat Mater 19:758\u0026ndash;766. \u003cspan class=\"ExternalRef\"\u003e\u003cspan class=\"RefSource\"\u003ehttps://doi.org/10.1038/s41563-020-0655-2\u003c/span\u003e\u003cspan address=\"10.1038/s41563-020-0655-2\" targettype=\"DOI\" class=\"RefTarget\"\u003e\u003c/span\u003e\u003c/span\u003e\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"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":"ionics","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":" Learn more about [Ionics](https://www.springer.com/journal/11581) ","snPcode":"11581","submissionUrl":"https://mc.manuscriptcentral.com/ionics","title":"Ionics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"lithium-sulfur battery, Bi2S3, Porous carbon, Shuttle effect","lastPublishedDoi":"10.21203/rs.3.rs-4636248/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4636248/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eLithium-sulfur batteries have not been widely commercialized due to issues with poor conductivity of the active material and the shuttle effect, both of which are effectively addressed in this study. The porous carbon CoNi-NC, derived from high-temperature carbonization of the cobalt-nickel metal-organic framework CoNi-ZIF, was utilized as the carbon substrate. It exhibits excellent specific surface area and a well-developed pore structure, thereby optimizing the conductivity and sulfur-loading capacity of the material. The incorporation of polar Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e effectively adsorbs polysulfides, retards the shuttle effect, and enhances the reaction kinetics of lithium-sulfur batteries. Electrochemical tests revealed that the CoNi-NC@Bi\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e3\u003c/sub\u003e electrode achieved a specific discharge capacity of 1107 mAh/g at a current density of 0.1 C, demonstrating excellent rate capability. Moreover, the cathode material maintained a specific discharge capacity of 796.5 mAh/g after 200 cycles at 0.2 C, indicating robust cycling stability.\u003c/p\u003e","manuscriptTitle":"Use of CoNi-ZIF-derived Bimetallic-Doped Nitrogen-Rich Porous Carbon (CoNi-NC) Composite Bi 2 S 3 in Lithium-Sulfur Batteries","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-07-17 09:24:38","doi":"10.21203/rs.3.rs-4636248/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-07-20T10:54:48+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-16T10:00:02+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-14T11:25:53+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-11T13:20:00+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"21307915042468979644270818490362942152","date":"2024-07-11T07:26:22+00:00","index":"hide","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-07-05T10:00:53+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"266137875708200401799292542043660722169","date":"2024-07-04T00:18:20+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"16002199588417555342157859457838340440","date":"2024-07-03T23:55:25+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"223004575468275353454231922174331171711","date":"2024-07-03T22:17:18+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"151129650441360662986517016249835651777","date":"2024-07-03T22:05:20+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2024-07-03T16:18:23+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-06-26T03:40:00+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-06-26T03:24:36+00:00","index":"","fulltext":""},{"type":"submitted","content":"Ionics","date":"2024-06-25T11:57:41+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"ionics","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":" Learn more about [Ionics](https://www.springer.com/journal/11581) ","snPcode":"11581","submissionUrl":"https://mc.manuscriptcentral.com/ionics","title":"Ionics","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"bcae0557-d955-4bb4-b515-5257a0a6e344","owner":[],"postedDate":"July 17th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2024-08-27T09:51:39+00:00","versionOfRecord":[],"versionCreatedAt":"2024-07-17 09:24:38","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4636248","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4636248","identity":"rs-4636248","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}