Advanced lithium-sulfur battery leveraging carbonized MoO3/T-CNF Composite Aerogels

Advanced lithium-sulfur battery leveraging carbonized MoO3/T-CNF Composite Aerogels | 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 Advanced lithium-sulfur battery leveraging carbonized MoO3/T-CNF Composite Aerogels Yane Liu, Mingang Zhang, Shengli Jia, Yifan Jiang, Qinghua Zhao This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4491545/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 Lithium-sulfur (Li-S) battery is one of the most promising high energy density energy storage systems due to its high theoretical energy density (2600 W h kg − 1 ) and specific capacity (1675 mA h g − 1 ). However, the poor conductivity of elemental sulfur and discharge final products Li 2 S 2 /Li 2 S, and the shuttle effect of lithium polysulfide are still important reasons for the capacity degradation of lithium-sulfur batteries. Herein, we propose to prepare MoO 3 /T-CNF composite aerogel materials by compounding TEMPO-oxidized cellulose nanofibers (T-CNF) and molybdenum trioxide (MoO 3 ) nanosheets through ultrasonic dispersion, directional freeze drying and high-temperature carbonization processes. When used as the cathode material for lithium-sulfur batteries, the aerogel material offers high electrical conductivity, a well-developed pore structure, and a large specific surface area. These properties enable it to effectively adsorb polysulfides, suppress their shuttle effect, and alleviate the volume expansion of electrode materials during charge and discharge cycles. Among them, the highest specific discharge capacity of MoO 3 /T-CNF-3 at 0.1C was 1721.8 mA h g − 1 , and the coulombic efficiency of 99.6% can still be maintained after 200 cycle. This demonstrates the benefits of the three-dimensional composite aerogel structure for Li-S battery cathode material applications, suggesting that the structural design of the material can enhance cycle stability while optimizing the specific capacity and multiplicative performance of Li-S batteries. Lithium-sulfur battery MoO3 Aerogel T-CNF Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 1 Introduction At present, compared with other energy storage and conversion devices, lithium-ion batteries have been widely used in portable electronic devices, new energy vehicles and energy storage devices due to their high energy density, long cycle life and low self-discharge rate [ 1 – 4 ]. Although compared with other commonly used batteries, lithium-ion batteries can reach 2 ~ 3 times their energy density and 4 ~ 5 times their power density [ 5 , 6 ]. However, with the rapid development of the new energy industry, there is an urgent need for energy storage systems with higher capacity, longer life, high efficiency and safety [ 7 – 11 ]. Therefore, it is especially important to develop a new generation of batteries with higher energy density and longer cycle life. Compared with conventional lithium-ion batteries, lithium-sulfur batteries (LSBs) have advantages of high theoretical energy density (2600 W h kg − 1 ), high safety and wide source of raw materials, and have received wide attention from scholars at home and abroad[ 12 – 15 ]. However, before commercial application, the development of lithium-sulfur batteries is constrained by many factors, such as the electronic insulation of sulfur and discharge products Li 2 S increases the internal resistance of the battery; the high solubility of polysulfide in organic ether electrolyte causes the "shuttle effect" greatly reduces the coulomb efficiency of the battery, the morphological change of the cathode material expands the volume of the battery and causes capacity decay, etc[ 16 – 20 ]. Therefore, it is still a great challenge to develop commercially available lithium-sulfur batteries. In recent years, many efforts have been made in the design of electrode materials for lithium-sulfur batteries. Among them, carbon materials have attracted much attention because of their high specific surface area, porous structure and controllable morphology[ 21 – 24 ]. In 2009, Nazar et al. developed a high-capacity sulfur cathode material by infusing molten sulfur into the ordered mesoporous carbon material CMK-3 [ 25 ]. Subsequently, functionalized carbon materials such as carbon nanotubes, graphene oxide and carbon nanorods appeared in lithium-sulfur batteries, which only further alleviated the problems of various defects in lithium-sulfur batteries. Natural biomass-derived carbon materials have been widely used to construct lithium-sulfur battery cathode materials because of their unique chemical composition, abundant resources, low cost and easy preparation, and their unique chemical composition makes it easy to obtain in situ heteroatom-doped porous carbon, which can effectively adsorb polysulfides, suppress shuttle effect and improve the electrochemical performance of lithium-sulfur batteries [ 26 – 29 ]. Magnacca et al. obtained biochar materials by heat-treating chitin at different temperatures, and studied the possibility of biochar as a sustainable and low-cost electrochemical energy storage device (such as lithium-sulfur batteries) [ 30 ]. Zhou et al. developed a biomimetic microbattery by utilizing Aspergillus niger, which has a dual concave structure similar to red blood cells, as the carrier [ 31 ]. They modified the black Aspergillus niger-derived dual concave surface hollow carbon (ADNC) by loading TiO 2 − x nanoparticles, resulting in a biomimetic ADNC/TiO 2 − x/S composite material with outstanding cycling stability and rate performance. After 500 cycles at a rate of 0.5C, the specific capacity reached 995 mA h g − 1 . Zhong et al. ingeniously designed a porous carbon material, referred to as expanded rice-derived carbon (PRC), by incorporating a metal foaming agent into rice and subsequently inducing its instantaneous expansion [ 32 ]. This resulted in a highly porous rice-derived carbon material with a high porosity (85.1%), high electrical conductivity (≈ 7.2×104 S/m), and high specific surface area (1492.2 m 2 /g). The carbon material exhibited a three-dimensional interconnected honeycomb-like structure composed of secondary carbon sheets, providing strong physical confinement for uniform sulfur distribution. Additionally, the embedded nickel nanoparticles offered short ion diffusion channels, reducing diffusion resistance, while the introduced metal/metal oxide (Ni/NiO) exhibited strong chemical adsorption on polysulfides, minimizing sulfur loss. The designed PRC/Ni/S composite electrode demonstrated excellent electrochemical performance, delivering a high capacity of 1257.2 mA h g − 1 at a rate of 0.2C, and maintaining a capacity of 821 mA h g − 1 after 500 cycles. Since then, the research on the application of porous carbon materials loaded with active materials as sulfur carriers has been rapidly developed in the field of lithium-sulfur batteries[ 33 – 37 ]. Therefore, in the current research, with the objectives of designing porous carrier materials, constructing adsorption sites for polysulfides, and improving the discharge capacity, multiplicative performance and cycle life of positive materials, a porous aerogel sulfur host material with uniformly encapsulated MoO 3 nanosheets was prepared by making TEMPO-oxidized cellulose nanofibers (T-CNF) as raw materials and MoO 3 nanosheets as active materials. The aerogel demonstrates not only effective polysulfide adsorption and shuttle effect suppression in lithium-sulfur batteries but also exhibits favorable initial discharge specific capacity and cycling performance, thereby reducing redundancy in language and enhancing clarity. When MoO 3 /T-CNF-3 aerogel was used as the main material of lithium-sulfur battery cathode sulfur, its highest specific discharge capacity is 1721.8 mA h g − 1 at 0.1C, and the coulombic efficiency of 99.6% can still be maintained after 200 cycles. This study highlights the benefits of employing a three-dimensional composite porous structure strategy for lithium-sulfur battery cathode material applications. It illustrates that optimizing the structure of the cathode material and its surface active sites can enhance both the specific capacity and overall performance of the battery, while also improving cycling stability. 2 Experimental 2.1 Chemical reagents The molybdenum trioxide (MoO 3 ) and Li 2 S 6 were purchased form Shanghai Titan Technology Co. Ltd. The TEMPO-oxidized cellulose nanofibers (T-CNF) was provided by Shanghai Maclin Biochemical Technology Co. Ltd. The above chemicals are reagent grade and do not require further purification. 2.2 Preparation of MoO 3 /T-CNF aerogel and cathodes First, First, MoO 3 and T-CNF were thoroughly mixed evenly, its schematic diagram is shown in Fig. 1 a-c. Following this, the uniformly mixed dispersion was transferred into a designated mold, frozen directionally using liquid nitrogen, and subsequently subjected to freeze-drying in a freeze dryer (Fig. 1 d). Finally, the freeze-dried aerogels underwent annealing at 600°C for 6 hours in an argon environment within a tube furnace (process from Fig. 1 d to Fig. 1 e). The prepared aerogel material was processed into an electrode sheet with a thickness of 100 µm and a diameter of 12 mm. Then, sulfur was loaded onto the aerogel by dropping Li 2 S 6 cathode electrolyte to prepare an aerogel cathode material, which was then tested as a cathode material for lithium-sulfur batteries (Fig. 1 f). More information about the electrodes and batteries can be found in the supporting materials. 2.3 Material characterization and Electrochemical test Scanning electron microscopy (SEM) mapping images were carried out through scanning electron microscopy (Hitachi S-4800, 15 kV). Infrared spectroscopy were used to test the chemical structure of materials. X-ray diffraction (XRD) patterns were obtained using a Rigaku 18 KWD/max-2550 instrument with Cu Kα radiation. The specific surface area and pore sizes were obtained by Surface Area and Porosimetry Analyzer. X-ray photoelectron spectroscopy (XPS) analysis was conducted using a Kratos Axis Ultra DLD X-ray photoelectron spectrometer. Electrochemical testing was carried out using the same methodology as previously described [ 38 ]. 3 Results and Discussion To characterize the microstructural features of the prepared MoO 3 /T-CNF composite aerogels, SEM was employed to observe different samples. As shown in Fig. 2 , compared to the smooth surface of pure T-CNF aerogel (Figure S1 ), significant changes in the pore structure and surface roughness were observed in the MoO 3 /T-CNF composite aerogels with varying ratios of MoO 3 and T-CNF. As shown in Fig. 2 a-c, when the proportion of MoO 3 increases and the proportion of T-CNF decreases, the porosity of the aerogel increases and the surface becomes rougher. This is attributed to the uniform spatial structure formed by the increased MoO 3 nanosheets and T-CNF, which prevents excessive accumulation caused by T-CNF. However, when there is an excessive amount of MoO 3 nanosheets, the enrichment of MoO 3 in the aerogel may result in reduced porosity and blockage of the porous structure, as shown in Fig. 2 d. Furthermore, as observed in Figure S2, the volume change of the prepared aerogel material is minimal before (a) and after (b) annealing. This intuitively proves that carbonization does not cause the material collapse. Furthermore, in Fig. 3 a, infrared spectroscopy analysis of MoO 3 nanosheets and MoO 3 /T-CNF-3 aerogel reveals that stretching vibration peaks of the C-O-C bonds in the cellulose pyranose ring (1042 cm − 1 ) and the stretching vibration peaks of Mo-O-Mo in MoO 3 (889 cm − 1 ) can be simultaneously detected in the infrared spectrum of MoO 3 /T-CNF-3 aerogel, indicating the successful composite of MoO 3 and T-CNF[ 39 ]. To delve deeper into the pore structure characteristics of the prepared material, we began by assessing its specific surface area using nitrogen adsorption-desorption testing. As shown in Fig. 3 b, compared to the pure T-CNF (105.50 m 2 /g) aerogel, the MoO 3 /T-CNF-3 aerogel exhibits a significantly higher specific surface area of 297.54 m 2 /g. This is attributed to the increased intermolecular interactions upon the introduction of MoO 3 , which effectively prevents the aggregation of nanoscale fiber materials. The linear T-CNF nanowires and planar MoO 3 nanosheets form a cross-linked structure, greatly enhancing the surface area and mechanical strength. In contrast, pure T-CNF shows a limited specific surface area because of the clustering of nanowires. To further confirm the successful formation of the composite of MoO 3 and T-CNF, we conducted X-ray diffraction (XRD) analysis on MoO 3 /T-CNF-1, MoO 3 /T-CNF-2, MoO 3 /T-CNF-3, MoO 3 /T-CNF-4, MoO 3 , and T-CNF, and the results are plotted in Fig. 4 . The analysis revealed distinct MoO 3 characteristic peaks at 12.8°, 23.4°, 25.7°, 27.4°, and 39.0° in the prepared composite aerogels, with the peak intensities gradually increasing with the increased amount of MoO 3 doping. Additionally, the broad peak around 22.8° signifies the successful integration of MoO 3 and T-CNF within the MoO 3 /T-CNF aerogel. Furthermore, X-ray photoelectron spectroscopy (XPS) was employed to determine the elemental composition of the composite aerogel films and analyze the composite of MoO 3 nanosheets and T-CNF in the MoO 3 /T-CNF-3 aerogel (Fig. 5 ). It is well known that cellulose is composed of a series of glucuronic acid units, which are connected through dehydration at the 1st and 4th positions, resulting in the presence of C-O and O-C-O bonds in the cellulose monomer. However, the appearance of a new C = O bond in the characteristic peak of C1s in Fig. 5 b indicates the selective formation of numerous C6 carboxylic acid groups on the surface of nanocellulose through TEMPO-mediated oxidation [118]. As shown in Fig. 5 a, characteristic peaks of Mo are observed in the MoO 3 /T-CNF-3 aerogel, and further confirmation of the successful preparation of the MoO 3 /T-CNF composite aerogel is obtained through fitting analysis of the characteristic peaks of O1s (Fig. 5 c) and Mo3d (Fig. 5 d), which is consistent with the XRD and FTIR analyses mentioned above. To investigate the electrochemical performance of the prepared materials, a series of tests were conducted. As shown in Fig. 6 a, cyclic voltammetry (CV) measurements were performed on the cathode materials of T-CNF and MoO 3 /T-CNF aerogels. The CV curves of T-CNF, MoO 3 /T-CNF-1, MoO 3 /T-CNF-2, MoO 3 /T-CNF-3, and MoO 3 /T-CNF-4 electrode materials after three cycles (Fig. 6 a) exhibit distinct oxidation-reduction peaks, indicating the redox reactions and transformations between elemental sulfur, polysulfides, and lithium sulfides. Notably, the integrated area of the CV curve for MoO 3 /T-CNF-3 is greater than that of the other materials, demonstrating the superior energy storage performance of the MoO 3 /T-CNF-3 composite aerogel among these electrode materials. Subsequently, galvanostatic charge-discharge (GCD) tests were conducted on the cathode materials of T-CNF and MoO 3 /T-CNF aerogels at rate ranging from 0.1C to 2C, and the results are shown in Fig. 6 (b-f). It can be observed that the voltage drop of the charge-discharge curves for MoO 3 /T-CNF-3 is relatively small, indicating longer discharge time and absence of significant polarization, demonstrating strong reaction kinetics. Due to the stable porous structure of MoO 3 /T-CNF-3 and effective anchoring of polysulfides at high current density, even at a rate of 2C, the discharge plateau remains distinct and stable. In addition to the GCD test at low rate, the test at high rate is also a characterization method to prove its excellent electrochemical performance. Therefore, as shown in Figure S3, galvanostatic charge-discharge tests (GCD) from 0.1C to 5C were performed on T-CNF (Figure S3a) and MoO 3 /T-CNF-3 (Figure S3b) aerogel electrode materials. When the rate is greater than 2C, the discharge time of MoO 3 /T-CNF-3 aerogel electrode material was still significantly better than that of T-CNF material, which proves the excellent electrochemical performance of MoO 3 /T-CNF-3 aerogel electrode material. In Fig. 7 a, the rate performance test of T-CNF and MoO 3 /T-CNF aerogel electrode materials at ranging from 0.1C to 2C demonstrates the superior reversible discharge specific capacity of the prepared MoO 3 /T-CNF-3 material, indicating its improved performance. At a rate of 0.1C, the reversible discharge specific capacity of MoO 3 /T-CNF-3 (1721.8 mA h/g) is significantly higher than that of T-CNF (776.7 mA h g − 1 ), MoO 3 /T-CNF-1 (1007.2 mA h g − 1 ), MoO 3 /T-CNF-2 (1222.8 mA h g − 1 ), and MoO 3 /T-CNF-4 (1188.1 mA h g − 1 ). Furthermore, for each electrode material, the reversible discharge specific capacity decreases as the current density increases, which is attributed to insufficient reaction at the electrode-electrolyte interface under high current density. Upon returning to a rate of 0.1C, the reversible discharge specific capacity of the electrode material recovers to its original level. This excellent performance is mainly attributed to the porous aerogel material's high adsorption efficiency, facilitating rapid lithium-ion transport and effective anchoring of polysulfides, thereby enhancing the kinetics of the redox reactions. Furthermore, in Fig. 7 b, the rate performance of T-CNF and MoO 3 /T-CNF-3 aerogel electrode materials at higher current densities were tested. The reversible discharge specific capacity variation is similar to that shown in Fig. 8 a, confirming the excellent stability of the MoO 3 /T-CNF-3 aerogel electrode material. Electrochemical impedance tests were carried out to analyze the conductivity of T-CNF and MoO 3 /T-CNF composite electrode materials, the result was shown in Fig. 8 a. In the high-frequency region, the intercept on the real axis represents the internal resistance (Rs) of the battery. From the graph, the internal resistances of T-CNF, MoO 3 /T-CNF-1, MoO 3 /T-CNF-2, MoO 3 /T-CNF-3, and MoO 3 /T-CNF-4 aerogel cathodes are determined to be 2.2 Ω, 5.9 Ω, 7.6 Ω, 3.1 Ω, and 2.9 Ω, respectively. Among which, the MoO 3 /T-CNF-4 aerogel cathode displays the lowest internal resistance due to increased incorporation of MoO 3 . This reduction decreases the ohmic resistance of the cathode material and enhances electronic conductivity. In the mid-frequency range, the semicircle illustrates the rate of charge transfer at the electrode-electrolyte interface, which correlates with the charge transfer resistance (Rct). Among the T-CNF, MoO 3 /T-CNF-1, MoO 3 /T-CNF-2, MoO 3 /T-CNF-3, and MoO 3 /T-CNF-4 aerogel cathodes, the MoO 3 /T-CNF-3 aerogel cathode shows the lowest charge transfer resistance. While Rs value of the MoO 3 /T-CNF-3 aerogel cathode isn’t the lowest, its superior ion transport structure and uniform coating contribute to a favorable pathway for rapid charge transfer at the electrode interface. This is also due to the high specific surface area and enhanced wetting effect of the MoO 3 /T-CNF-3 aerogel cathode. In the low-frequency region, the corresponding diagonal line reflects the diffusion process of lithium ions within the electrode, corresponding to the Warburg impedance (Wo). The consistent coating structure of MoO 3 in the MoO 3 /T-CNF-3 aerogel significantly enhances the speed of charge transfer at the interface and the diffusion pathway of ions. Cycle performance of T-CNF and MoO 3 /T-CNF composite electrode material was shown in Fig. 8 b. The discharge specific capacities of T-CNF, MoO 3 /T-CNF-1, MoO 3 /T-CNF-2, MoO 3 /T-CNF-3, and MoO 3 /T-CNF-4 aerogel cathodes at 0.1 C are 776.6, 1060, 1277.9, 1511.6, and 1116.8 mA h g − 1 , respectively. Following 200 cycles, the MoO 3 /T-CNF-3 aerogel cathode continues to sustain a capacity of 1282.4 mA h g − 1 , with a coulombic efficiency of 99.6%. In contrast, the pure C-CNF aerogel exhibits a capacity of only 17.1 mA h g − 1 after 200 cycles, significantly lower than that of the MoO 3 /T-CNF-3 aerogel. This indicates that the combination strategy of spatial structure and strong adsorption sites effectively enhances the cycling stability of lithium-sulfur batteries. 4 Conclusion In this study, we effectively prepared a three-dimensional porous aerogel material by combining MoO 3 and T-CNF, serving as a sulfur host material for lithium-sulfur batteries. The three-dimensional porous structure formed by T-CNF as the framework greatly facilitates rapid ion transport, and the enormous specific surface area of the composite material ensures effective adsorption of polysulfides. Among them, the MoO 3 /T-CNF-3 exhibits a highest specific discharge capacity of 1721.8 mA h g − 1 at 0.1C, and maintains a coulombic efficiency of 99.6% after 200 cycles. This illustrates the benefits of employing the three-dimensional composite aerogel structure in the utilization of positive electrode materials for lithium-sulfur batteries, indicating that the structural design of this material can enhance cycling stability while optimizing the specific capacity and rate capabilities of lithium-sulfur batteries. Declarations Compliance with Ethical Standards The authors declare adherence to ethical standards. Author Contribution Y. L. provided the specific program and financial support for the experiment, and she processed the data and wrote the paper. M. Z and S. J. put forward some suggestions to revise the paper. Y. J. and Q. Z. performed experimental operations. All authors reviewed the manuscript. 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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-4491545","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":312181335,"identity":"dd86de2c-053c-408d-a226-c1e6bbc14fab","order_by":0,"name":"Yane Liu","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAwUlEQVRIiWNgGAWjYBACfvb+hw8SDCTk+NkbiNQi2XOG2eBBgYWxZM8BIrUY3PBhE3zwoSLR4EYCsbbM4D3GAHRYAsPNxxtvMNTYRBPUwi/dlwbySx7j7LRiC4ZjabkNBG2Zc8DcAKilmFk6x0yCseEwYS1AL5hJALUktkmeIVpLDkRLjwQPkVoke44lgxxmLMED9EsCMX7hZ28++PDHnzo5++OHN974UGNDWAuKI4FBTSIwkCBVxygYBaNgFIwMAAC9ZECNwAvW8gAAAABJRU5ErkJggg==","orcid":"","institution":"Lvliang University","correspondingAuthor":true,"prefix":"","firstName":"Yane","middleName":"","lastName":"Liu","suffix":""},{"id":312181336,"identity":"00cbbf3f-cc64-483b-b018-ed6886e27b8d","order_by":1,"name":"Mingang Zhang","email":"","orcid":"","institution":"Taiyuan University of Science and Technology","correspondingAuthor":false,"prefix":"","firstName":"Mingang","middleName":"","lastName":"Zhang","suffix":""},{"id":312181337,"identity":"684c9c81-fa9f-4ed1-872f-a16cf8ff32fe","order_by":2,"name":"Shengli Jia","email":"","orcid":"","institution":"Lvliang University","correspondingAuthor":false,"prefix":"","firstName":"Shengli","middleName":"","lastName":"Jia","suffix":""},{"id":312181338,"identity":"3a0b9426-cc2e-4048-b44e-070f886d2300","order_by":3,"name":"Yifan Jiang","email":"","orcid":"","institution":"Lvliang University","correspondingAuthor":false,"prefix":"","firstName":"Yifan","middleName":"","lastName":"Jiang","suffix":""},{"id":312181339,"identity":"20f1e6aa-d40f-45ae-89b2-ae7f3b55d8bf","order_by":4,"name":"Qinghua Zhao","email":"","orcid":"","institution":"Lvliang University","correspondingAuthor":false,"prefix":"","firstName":"Qinghua","middleName":"","lastName":"Zhao","suffix":""}],"badges":[],"createdAt":"2024-05-28 14:15:56","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-4491545/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-4491545/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":58121218,"identity":"374c3243-80fa-4348-9fe0-bfd60ed90400","added_by":"auto","created_at":"2024-06-11 12:03:19","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":108534,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic diagram of the preparation process of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF: (a-c) preparation of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF mixture suspension, (d) preparation of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogel, (e) carbonization of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF Aerogels, (f) schematic illustration of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF as cathode for lithium-sulfur battery.\u003c/p\u003e","description":"","filename":"floatimage1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/fc6325371f51a50e97a4eabc.jpg"},{"id":58121219,"identity":"02e44679-cc64-4222-b155-524605e44ee4","added_by":"auto","created_at":"2024-06-11 12:03:19","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":322485,"visible":true,"origin":"","legend":"\u003cp\u003eSEM images of (a) MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, (b) MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, (c) MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, and (d) MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4.\u003c/p\u003e","description":"","filename":"floatimage2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/1a2c3a38f4e64475266ef85d.jpg"},{"id":58121220,"identity":"534caf17-3c45-4d87-a8d6-8dbfa630b313","added_by":"auto","created_at":"2024-06-11 12:03:19","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":111044,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Infrared absorption curve of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel and the MoO\u003csub\u003e3\u003c/sub\u003e nanosheet. (b) The nitrogen adsorption-desorption isotherms of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogels.\u003c/p\u003e","description":"","filename":"floatimage3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/a738c4bb4a1e3f8b7ccb9dcd.jpg"},{"id":58122782,"identity":"217133fe-acd7-4179-85a4-db74a55c4989","added_by":"auto","created_at":"2024-06-11 12:27:19","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":648726,"visible":true,"origin":"","legend":"\u003cp\u003eXRD patterns of MoO\u003csub\u003e3\u003c/sub\u003e, T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4.\u003c/p\u003e","description":"","filename":"floatimage4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/dd568b86aec39ab11fb9d1c3.jpg"},{"id":58121661,"identity":"a6729b09-49c6-4d22-9271-13d35e054fe0","added_by":"auto","created_at":"2024-06-11 12:11:19","extension":"jpg","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":161979,"visible":true,"origin":"","legend":"\u003cp\u003eXPS spectrum of (a) MoO\u003csub\u003e3\u003c/sub\u003e and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3; and characteristic peaks of (b) the C1s, (c) the O1s and (d) the Mo3d.\u003c/p\u003e","description":"","filename":"floatimage5.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/f84be53c7aa541c3c7c0850f.jpg"},{"id":58122060,"identity":"a48eabea-da35-4f70-9258-15f0d000e4c1","added_by":"auto","created_at":"2024-06-11 12:19:19","extension":"jpg","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":219911,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Cyclic voltammetry at 0.1 mV s\u003csup\u003e-1\u003c/sup\u003e of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 cathodes after three cycles. (b-f) Galvanostatic charge and discharge curves of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 cathodes from 0.1 to 2 C, respectively.\u003c/p\u003e","description":"","filename":"floatimage6.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/5cc7a026ad0c717d14b8bf4b.jpg"},{"id":58121658,"identity":"50adb60d-1257-435d-9304-d809c6d27915","added_by":"auto","created_at":"2024-06-11 12:11:19","extension":"jpg","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":150865,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Rate capability of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 cathodes from 0.1 C to 2 C. (b) Rate capability of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 cathodes from 0.1 C to 5 C.\u003c/p\u003e","description":"","filename":"floatimage7.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/d6fdd59a6dda52b7b160bb9a.jpg"},{"id":58121225,"identity":"8b9d7579-083c-4189-8f69-edcdda219d6e","added_by":"auto","created_at":"2024-06-11 12:03:19","extension":"jpg","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":127875,"visible":true,"origin":"","legend":"\u003cp\u003e(a) Electrochemical impedance spectrums of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 aerogel electrodes. (b) Cycle performance of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 cathodes.\u003c/p\u003e","description":"","filename":"floatimage8.jpg","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/9eb9e1200ac9e9e45d00ef43.jpg"},{"id":58414060,"identity":"114de6bd-e115-49a7-a191-5b66ef9896e0","added_by":"auto","created_at":"2024-06-15 11:44:46","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2272764,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/d565788b-a714-4bad-8ef4-717518e8227a.pdf"},{"id":58121226,"identity":"1f707945-edec-4c58-876f-968069f94df5","added_by":"auto","created_at":"2024-06-11 12:03:19","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":1297929,"visible":true,"origin":"","legend":"","description":"","filename":"supportinginformation.docx","url":"https://assets-eu.researchsquare.com/files/rs-4491545/v1/8d9993df5ac753d5567caa78.docx"}],"financialInterests":"No competing interests reported.","formattedTitle":"Advanced lithium-sulfur battery leveraging carbonized MoO3/T-CNF Composite Aerogels","fulltext":[{"header":"1 Introduction","content":"\u003cp\u003eAt present, compared with other energy storage and conversion devices, lithium-ion batteries have been widely used in portable electronic devices, new energy vehicles and energy storage devices due to their high energy density, long cycle life and low self-discharge rate [\u003cspan additionalcitationids=\"CR2 CR3\" citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e]. Although compared with other commonly used batteries, lithium-ion batteries can reach 2\u0026thinsp;~\u0026thinsp;3 times their energy density and 4\u0026thinsp;~\u0026thinsp;5 times their power density [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e, \u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. However, with the rapid development of the new energy industry, there is an urgent need for energy storage systems with higher capacity, longer life, high efficiency and safety [\u003cspan additionalcitationids=\"CR8 CR9 CR10\" citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]. Therefore, it is especially important to develop a new generation of batteries with higher energy density and longer cycle life.\u003c/p\u003e \u003cp\u003eCompared with conventional lithium-ion batteries, lithium-sulfur batteries (LSBs) have advantages of high theoretical energy density (2600 W h kg\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), high safety and wide source of raw materials, and have received wide attention from scholars at home and abroad[\u003cspan additionalcitationids=\"CR13 CR14\" citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]. However, before commercial application, the development of lithium-sulfur batteries is constrained by many factors, such as the electronic insulation of sulfur and discharge products Li\u003csub\u003e2\u003c/sub\u003eS increases the internal resistance of the battery; the high solubility of polysulfide in organic ether electrolyte causes the \"shuttle effect\" greatly reduces the coulomb efficiency of the battery, the morphological change of the cathode material expands the volume of the battery and causes capacity decay, etc[\u003cspan additionalcitationids=\"CR17 CR18 CR19\" citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]. Therefore, it is still a great challenge to develop commercially available lithium-sulfur batteries.\u003c/p\u003e \u003cp\u003eIn recent years, many efforts have been made in the design of electrode materials for lithium-sulfur batteries. Among them, carbon materials have attracted much attention because of their high specific surface area, porous structure and controllable morphology[\u003cspan additionalcitationids=\"CR22 CR23\" citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. In 2009, Nazar et al. developed a high-capacity sulfur cathode material by infusing molten sulfur into the ordered mesoporous carbon material CMK-3 [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e]. Subsequently, functionalized carbon materials such as carbon nanotubes, graphene oxide and carbon nanorods appeared in lithium-sulfur batteries, which only further alleviated the problems of various defects in lithium-sulfur batteries. Natural biomass-derived carbon materials have been widely used to construct lithium-sulfur battery cathode materials because of their unique chemical composition, abundant resources, low cost and easy preparation, and their unique chemical composition makes it easy to obtain in situ heteroatom-doped porous carbon, which can effectively adsorb polysulfides, suppress shuttle effect and improve the electrochemical performance of lithium-sulfur batteries [\u003cspan additionalcitationids=\"CR27 CR28\" citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e]. Magnacca et al. obtained biochar materials by heat-treating chitin at different temperatures, and studied the possibility of biochar as a sustainable and low-cost electrochemical energy storage device (such as lithium-sulfur batteries) [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. Zhou et al. developed a biomimetic microbattery by utilizing Aspergillus niger, which has a dual concave structure similar to red blood cells, as the carrier [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e]. They modified the black Aspergillus niger-derived dual concave surface hollow carbon (ADNC) by loading TiO\u003csub\u003e2\u003c/sub\u003e\u0026thinsp;\u0026minus;\u0026thinsp;x nanoparticles, resulting in a biomimetic ADNC/TiO\u003csub\u003e2\u003c/sub\u003e\u0026thinsp;\u0026minus;\u0026thinsp;x/S composite material with outstanding cycling stability and rate performance. After 500 cycles at a rate of 0.5C, the specific capacity reached 995 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e. Zhong et al. ingeniously designed a porous carbon material, referred to as expanded rice-derived carbon (PRC), by incorporating a metal foaming agent into rice and subsequently inducing its instantaneous expansion [\u003cspan citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e]. This resulted in a highly porous rice-derived carbon material with a high porosity (85.1%), high electrical conductivity (\u0026asymp;\u0026thinsp;7.2\u0026times;104 S/m), and high specific surface area (1492.2 m\u003csup\u003e2\u003c/sup\u003e/g). The carbon material exhibited a three-dimensional interconnected honeycomb-like structure composed of secondary carbon sheets, providing strong physical confinement for uniform sulfur distribution. Additionally, the embedded nickel nanoparticles offered short ion diffusion channels, reducing diffusion resistance, while the introduced metal/metal oxide (Ni/NiO) exhibited strong chemical adsorption on polysulfides, minimizing sulfur loss. The designed PRC/Ni/S composite electrode demonstrated excellent electrochemical performance, delivering a high capacity of 1257.2 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at a rate of 0.2C, and maintaining a capacity of 821 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e after 500 cycles. Since then, the research on the application of porous carbon materials loaded with active materials as sulfur carriers has been rapidly developed in the field of lithium-sulfur batteries[\u003cspan additionalcitationids=\"CR34 CR35 CR36\" citationid=\"CR33\" class=\"CitationRef\"\u003e33\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR37\" class=\"CitationRef\"\u003e37\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eTherefore, in the current research, with the objectives of designing porous carrier materials, constructing adsorption sites for polysulfides, and improving the discharge capacity, multiplicative performance and cycle life of positive materials, a porous aerogel sulfur host material with uniformly encapsulated MoO\u003csub\u003e3\u003c/sub\u003e nanosheets was prepared by making TEMPO-oxidized cellulose nanofibers (T-CNF) as raw materials and MoO\u003csub\u003e3\u003c/sub\u003e nanosheets as active materials. The aerogel demonstrates not only effective polysulfide adsorption and shuttle effect suppression in lithium-sulfur batteries but also exhibits favorable initial discharge specific capacity and cycling performance, thereby reducing redundancy in language and enhancing clarity. When MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel was used as the main material of lithium-sulfur battery cathode sulfur, its highest specific discharge capacity is 1721.8 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 0.1C, and the coulombic efficiency of 99.6% can still be maintained after 200 cycles. This study highlights the benefits of employing a three-dimensional composite porous structure strategy for lithium-sulfur battery cathode material applications. It illustrates that optimizing the structure of the cathode material and its surface active sites can enhance both the specific capacity and overall performance of the battery, while also improving cycling stability.\u003c/p\u003e"},{"header":"2 Experimental","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e \u003ch2\u003e2.1 Chemical reagents\u003c/h2\u003e \u003cp\u003eThe molybdenum trioxide (MoO\u003csub\u003e3\u003c/sub\u003e) and Li\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e6\u003c/sub\u003e were purchased form Shanghai Titan Technology Co. Ltd. The TEMPO-oxidized cellulose nanofibers (T-CNF) was provided by Shanghai Maclin Biochemical Technology Co. Ltd. The above chemicals are reagent grade and do not require further purification.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec4\" class=\"Section2\"\u003e \u003ch2\u003e2.2 Preparation of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogel and cathodes\u003c/h2\u003e \u003cp\u003eFirst, First, MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF were thoroughly mixed evenly, its schematic diagram is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ea-c. Following this, the uniformly mixed dispersion was transferred into a designated mold, frozen directionally using liquid nitrogen, and subsequently subjected to freeze-drying in a freeze dryer (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed). Finally, the freeze-dried aerogels underwent annealing at 600\u0026deg;C for 6 hours in an argon environment within a tube furnace (process from Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ed to Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ee). The prepared aerogel material was processed into an electrode sheet with a thickness of 100 \u0026micro;m and a diameter of 12 mm. Then, sulfur was loaded onto the aerogel by dropping Li\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e6\u003c/sub\u003e cathode electrolyte to prepare an aerogel cathode material, which was then tested as a cathode material for lithium-sulfur batteries (Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003ef). More information about the electrodes and batteries can be found in the supporting materials.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec5\" class=\"Section2\"\u003e \u003ch2\u003e2.3 Material characterization and Electrochemical test\u003c/h2\u003e \u003cp\u003eScanning electron microscopy (SEM) mapping images were carried out through scanning electron microscopy (Hitachi S-4800, 15 kV). Infrared spectroscopy were used to test the chemical structure of materials. X-ray diffraction (XRD) patterns were obtained using a Rigaku 18 KWD/max-2550 instrument with Cu Kα radiation. The specific surface area and pore sizes were obtained by Surface Area and Porosimetry Analyzer. X-ray photoelectron spectroscopy (XPS) analysis was conducted using a Kratos Axis Ultra DLD X-ray photoelectron spectrometer. Electrochemical testing was carried out using the same methodology as previously described [\u003cspan citationid=\"CR38\" class=\"CitationRef\"\u003e38\u003c/span\u003e].\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e"},{"header":"3 Results and Discussion","content":"\u003cp\u003eTo characterize the microstructural features of the prepared MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite aerogels, SEM was employed to observe different samples. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e, compared to the smooth surface of pure T-CNF aerogel (Figure \u003cspan refid=\"MOESM1\" class=\"InternalRef\"\u003eS1\u003c/span\u003e), significant changes in the pore structure and surface roughness were observed in the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite aerogels with varying ratios of MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ea-c, when the proportion of MoO\u003csub\u003e3\u003c/sub\u003e increases and the proportion of T-CNF decreases, the porosity of the aerogel increases and the surface becomes rougher. This is attributed to the uniform spatial structure formed by the increased MoO\u003csub\u003e3\u003c/sub\u003e nanosheets and T-CNF, which prevents excessive accumulation caused by T-CNF. However, when there is an excessive amount of MoO\u003csub\u003e3\u003c/sub\u003e nanosheets, the enrichment of MoO\u003csub\u003e3\u003c/sub\u003e in the aerogel may result in reduced porosity and blockage of the porous structure, as shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003ed. Furthermore, as observed in Figure S2, the volume change of the prepared aerogel material is minimal before (a) and after (b) annealing. This intuitively proves that carbonization does not cause the material collapse.\u003c/p\u003e \u003cp\u003eFurthermore, in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003ea, infrared spectroscopy analysis of MoO\u003csub\u003e3\u003c/sub\u003e nanosheets and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel reveals that stretching vibration peaks of the C-O-C bonds in the cellulose pyranose ring (1042 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) and the stretching vibration peaks of Mo-O-Mo in MoO\u003csub\u003e3\u003c/sub\u003e (889 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) can be simultaneously detected in the infrared spectrum of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel, indicating the successful composite of MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF[\u003cspan citationid=\"CR39\" class=\"CitationRef\"\u003e39\u003c/span\u003e]. To delve deeper into the pore structure characteristics of the prepared material, we began by assessing its specific surface area using nitrogen adsorption-desorption testing. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003eb, compared to the pure T-CNF (105.50 m\u003csup\u003e2\u003c/sup\u003e/g) aerogel, the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel exhibits a significantly higher specific surface area of 297.54 m\u003csup\u003e2\u003c/sup\u003e/g. This is attributed to the increased intermolecular interactions upon the introduction of MoO\u003csub\u003e3\u003c/sub\u003e, which effectively prevents the aggregation of nanoscale fiber materials. The linear T-CNF nanowires and planar MoO\u003csub\u003e3\u003c/sub\u003e nanosheets form a cross-linked structure, greatly enhancing the surface area and mechanical strength. In contrast, pure T-CNF shows a limited specific surface area because of the clustering of nanowires.\u003c/p\u003e \u003cp\u003eTo further confirm the successful formation of the composite of MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF, we conducted X-ray diffraction (XRD) analysis on MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4, MoO\u003csub\u003e3\u003c/sub\u003e, and T-CNF, and the results are plotted in Fig.\u0026nbsp;\u003cspan refid=\"Fig4\" class=\"InternalRef\"\u003e4\u003c/span\u003e. The analysis revealed distinct MoO\u003csub\u003e3\u003c/sub\u003e characteristic peaks at 12.8\u0026deg;, 23.4\u0026deg;, 25.7\u0026deg;, 27.4\u0026deg;, and 39.0\u0026deg; in the prepared composite aerogels, with the peak intensities gradually increasing with the increased amount of MoO\u003csub\u003e3\u003c/sub\u003e doping. Additionally, the broad peak around 22.8\u0026deg; signifies the successful integration of MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF within the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogel.\u003c/p\u003e \u003cp\u003eFurthermore, X-ray photoelectron spectroscopy (XPS) was employed to determine the elemental composition of the composite aerogel films and analyze the composite of MoO\u003csub\u003e3\u003c/sub\u003e nanosheets and T-CNF in the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003e). It is well known that cellulose is composed of a series of glucuronic acid units, which are connected through dehydration at the 1st and 4th positions, resulting in the presence of C-O and O-C-O bonds in the cellulose monomer. However, the appearance of a new C\u0026thinsp;=\u0026thinsp;O bond in the characteristic peak of C1s in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003eb indicates the selective formation of numerous C6 carboxylic acid groups on the surface of nanocellulose through TEMPO-mediated oxidation [118]. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ea, characteristic peaks of Mo are observed in the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel, and further confirmation of the successful preparation of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite aerogel is obtained through fitting analysis of the characteristic peaks of O1s (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ec) and Mo3d (Fig.\u0026nbsp;\u003cspan refid=\"Fig5\" class=\"InternalRef\"\u003e5\u003c/span\u003ed), which is consistent with the XRD and FTIR analyses mentioned above.\u003c/p\u003e \u003cp\u003eTo investigate the electrochemical performance of the prepared materials, a series of tests were conducted. As shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea, cyclic voltammetry (CV) measurements were performed on the cathode materials of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogels. The CV curves of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 electrode materials after three cycles (Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003ea) exhibit distinct oxidation-reduction peaks, indicating the redox reactions and transformations between elemental sulfur, polysulfides, and lithium sulfides. Notably, the integrated area of the CV curve for MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 is greater than that of the other materials, demonstrating the superior energy storage performance of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 composite aerogel among these electrode materials.\u003c/p\u003e \u003cp\u003eSubsequently, galvanostatic charge-discharge (GCD) tests were conducted on the cathode materials of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogels at rate ranging from 0.1C to 2C, and the results are shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig6\" class=\"InternalRef\"\u003e6\u003c/span\u003e(b-f). It can be observed that the voltage drop of the charge-discharge curves for MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 is relatively small, indicating longer discharge time and absence of significant polarization, demonstrating strong reaction kinetics. Due to the stable porous structure of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 and effective anchoring of polysulfides at high current density, even at a rate of 2C, the discharge plateau remains distinct and stable. In addition to the GCD test at low rate, the test at high rate is also a characterization method to prove its excellent electrochemical performance. Therefore, as shown in Figure S3, galvanostatic charge-discharge tests (GCD) from 0.1C to 5C were performed on T-CNF (Figure S3a) and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 (Figure S3b) aerogel electrode materials. When the rate is greater than 2C, the discharge time of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel electrode material was still significantly better than that of T-CNF material, which proves the excellent electrochemical performance of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel electrode material.\u003c/p\u003e \u003cp\u003eIn Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003ea, the rate performance test of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF aerogel electrode materials at ranging from 0.1C to 2C demonstrates the superior reversible discharge specific capacity of the prepared MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 material, indicating its improved performance. At a rate of 0.1C, the reversible discharge specific capacity of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 (1721.8 mA h/g) is significantly higher than that of T-CNF (776.7 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1 (1007.2 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2 (1222.8 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 (1188.1 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). Furthermore, for each electrode material, the reversible discharge specific capacity decreases as the current density increases, which is attributed to insufficient reaction at the electrode-electrolyte interface under high current density. Upon returning to a rate of 0.1C, the reversible discharge specific capacity of the electrode material recovers to its original level. This excellent performance is mainly attributed to the porous aerogel material's high adsorption efficiency, facilitating rapid lithium-ion transport and effective anchoring of polysulfides, thereby enhancing the kinetics of the redox reactions.\u003c/p\u003e \u003cp\u003eFurthermore, in Fig.\u0026nbsp;\u003cspan refid=\"Fig7\" class=\"InternalRef\"\u003e7\u003c/span\u003eb, the rate performance of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel electrode materials at higher current densities were tested. The reversible discharge specific capacity variation is similar to that shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003ea, confirming the excellent stability of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel electrode material.\u003c/p\u003e \u003cp\u003eElectrochemical impedance tests were carried out to analyze the conductivity of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite electrode materials, the result was shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003ea. In the high-frequency region, the intercept on the real axis represents the internal resistance (Rs) of the battery. From the graph, the internal resistances of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 aerogel cathodes are determined to be 2.2 Ω, 5.9 Ω, 7.6 Ω, 3.1 Ω, and 2.9 Ω, respectively. Among which, the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 aerogel cathode displays the lowest internal resistance due to increased incorporation of MoO\u003csub\u003e3\u003c/sub\u003e. This reduction decreases the ohmic resistance of the cathode material and enhances electronic conductivity.\u003c/p\u003e \u003cp\u003eIn the mid-frequency range, the semicircle illustrates the rate of charge transfer at the electrode-electrolyte interface, which correlates with the charge transfer resistance (Rct). Among the T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 aerogel cathodes, the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel cathode shows the lowest charge transfer resistance. While Rs value of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel cathode isn\u0026rsquo;t the lowest, its superior ion transport structure and uniform coating contribute to a favorable pathway for rapid charge transfer at the electrode interface. This is also due to the high specific surface area and enhanced wetting effect of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel cathode.\u003c/p\u003e \u003cp\u003eIn the low-frequency region, the corresponding diagonal line reflects the diffusion process of lithium ions within the electrode, corresponding to the Warburg impedance (Wo). The consistent coating structure of MoO\u003csub\u003e3\u003c/sub\u003e in the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel significantly enhances the speed of charge transfer at the interface and the diffusion pathway of ions.\u003c/p\u003e \u003cp\u003eCycle performance of T-CNF and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite electrode material was shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig8\" class=\"InternalRef\"\u003e8\u003c/span\u003eb. The discharge specific capacities of T-CNF, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-1, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-2, MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3, and MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-4 aerogel cathodes at 0.1 C are 776.6, 1060, 1277.9, 1511.6, and 1116.8 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively. Following 200 cycles, the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel cathode continues to sustain a capacity of 1282.4 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, with a coulombic efficiency of 99.6%. In contrast, the pure C-CNF aerogel exhibits a capacity of only 17.1 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e after 200 cycles, significantly lower than that of the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 aerogel. This indicates that the combination strategy of spatial structure and strong adsorption sites effectively enhances the cycling stability of lithium-sulfur batteries.\u003c/p\u003e "},{"header":"4 Conclusion","content":"\u003cp\u003eIn this study, we effectively prepared a three-dimensional porous aerogel material by combining MoO\u003csub\u003e3\u003c/sub\u003e and T-CNF, serving as a sulfur host material for lithium-sulfur batteries. The three-dimensional porous structure formed by T-CNF as the framework greatly facilitates rapid ion transport, and the enormous specific surface area of the composite material ensures effective adsorption of polysulfides. Among them, the MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 exhibits a highest specific discharge capacity of 1721.8 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at 0.1C, and maintains a coulombic efficiency of 99.6% after 200 cycles. This illustrates the benefits of employing the three-dimensional composite aerogel structure in the utilization of positive electrode materials for lithium-sulfur batteries, indicating that the structural design of this material can enhance cycling stability while optimizing the specific capacity and rate capabilities of lithium-sulfur batteries.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e \u003ch2\u003eCompliance with Ethical Standards\u003c/h2\u003e \u003cp\u003eThe authors declare adherence to ethical standards.\u003c/p\u003e \u003c/p\u003e\u003ch2\u003eAuthor Contribution\u003c/h2\u003e\u003cp\u003eY. L. provided the specific program and financial support for the experiment, and she processed the data and wrote the paper. M. Z and S. J. put forward some suggestions to revise the paper. Y. J. and Q. Z. performed experimental operations. All authors reviewed the manuscript.\u003c/p\u003e\u003ch2\u003eAcknowledgement\u003c/h2\u003e\u003cp\u003eThis work was supported by the Key Research and Development Projects for the Introduction of High-level Scientific and Technological Talents in Lvliang City (2022RC12), Lvliang College Youth Academic Backbone Project and Lvliang College Research Startup Fund.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\u003cli\u003e\u003cspan\u003eZhong, H.-Y., et al., \u003cem\u003eBimetallic alloy FexCo1-xPS3 with boosted lithium reaction kinetics for lithium-ion batteries\u003c/em\u003e. Chemical Engineering Journal, 2023. 475: p. 145990.\u003c/span\u003e\u003c/li\u003e \u003cli\u003e\u003cspan\u003eYin, Y.X., et al., \u003cem\u003eLithium\u0026ndash;sulfur batteries: electrochemistry, materials, and prospects\u003c/em\u003e. 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Fukuzumi, \u003cem\u003eTEMPO-oxidized cellulose nanofibers\u003c/em\u003e. The Royal Society of Chemistry, 2011(1).\u003c/span\u003e\u003c/li\u003e\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"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":"Lithium-sulfur battery, MoO3, Aerogel, T-CNF","lastPublishedDoi":"10.21203/rs.3.rs-4491545/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-4491545/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eLithium-sulfur (Li-S) battery is one of the most promising high energy density energy storage systems due to its high theoretical energy density (2600 W h kg\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e) and specific capacity (1675 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e). However, the poor conductivity of elemental sulfur and discharge final products Li\u003csub\u003e2\u003c/sub\u003eS\u003csub\u003e2\u003c/sub\u003e/Li\u003csub\u003e2\u003c/sub\u003eS, and the shuttle effect of lithium polysulfide are still important reasons for the capacity degradation of lithium-sulfur batteries. Herein, we propose to prepare MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF composite aerogel materials by compounding TEMPO-oxidized cellulose nanofibers (T-CNF) and molybdenum trioxide (MoO\u003csub\u003e3\u003c/sub\u003e) nanosheets through ultrasonic dispersion, directional freeze drying and high-temperature carbonization processes. When used as the cathode material for lithium-sulfur batteries, the aerogel material offers high electrical conductivity, a well-developed pore structure, and a large specific surface area. These properties enable it to effectively adsorb polysulfides, suppress their shuttle effect, and alleviate the volume expansion of electrode materials during charge and discharge cycles. Among them, the highest specific discharge capacity of MoO\u003csub\u003e3\u003c/sub\u003e/T-CNF-3 at 0.1C was 1721.8 mA h g\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, and the coulombic efficiency of 99.6% can still be maintained after 200 cycle. This demonstrates the benefits of the three-dimensional composite aerogel structure for Li-S battery cathode material applications, suggesting that the structural design of the material can enhance cycle stability while optimizing the specific capacity and multiplicative performance of Li-S batteries.\u003c/p\u003e","manuscriptTitle":"Advanced lithium-sulfur battery leveraging carbonized MoO3/T-CNF Composite Aerogels","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-06-11 12:03:14","doi":"10.21203/rs.3.rs-4491545/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":"b8514d70-3ad3-4a4b-a673-62bd8066ab93","owner":[],"postedDate":"June 11th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2024-06-15T11:36:39+00:00","versionOfRecord":[],"versionCreatedAt":"2024-06-11 12:03:14","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4491545","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4491545","identity":"rs-4491545","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}