Shabab Hussain, Yufeng Wu, Zhifu Chen, Zhiyong Luo, Fei Zhong, Yu Chen, Chunmei Gao, Lei Wang
{"title":"Siloxane engineered polydiketopyrrolopyrrole derivatives with improved crystallinity and doping efficiency for thermoelectric power generation","authors":"Shabab Hussain, Yufeng Wu, Zhifu Chen, Zhiyong Luo, Fei Zhong, Yu Chen, Chunmei Gao, Lei Wang","doi":"10.1039/d4ta07160c","DOIUrl":"https://doi.org/10.1039/d4ta07160c","url":null,"abstract":"Siloxane side engineered conjugated polymers exhibit good film forming capabilities and have been reported for a variety of advanced energy applications. However, their potential for regulating polymer crystallinity to achieve high thermoelectric (TE) properties remains unexplored. In this study, the siloxane side-chained diketopyrrolopyrrole polymers (PDPPSix, where x is the molar ratio of siloxane side chain) and its corresponding FeCl3-doped films were designed and synthesized by solution-processed drop-casting method to improve the thermoelectric properties. The results show that the addition of siloxane side chains enhance the crystallinity and doping efficiency of the DPPSix polymers, and thus improves the conductivity and TE performance. It is worth noting that the 5-min FeCl3-doped PDPPSi50 film exhibits excellent thermoelectric properties, with an electronic conductivity of 66.29 S cm-1 and a maximum power factor (PF) of 38.6 μW m-1 K-2, which are about 7-fold and 3-fold higher than that of polymer film without siloxane side chains, respectively. The synergistic effect between siloxane side chains and FeCl3 doping significantly increases the charge carrier concentration and mobility, enhances the conductivity and thermoelectric efficiency of DPP-based TE polymers. This study highlights the potential of solution-processed, inorganic-doped, and side chain engineered conjugated polymer films for enhancing thermoelectric power generation.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589146","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junli Chen, Xinyi Jin, Xinli Yang, Lei Deng, Zhiqiang Zhang, Li Feng Han, Feilong Gong, Yonghui Zhang
{"title":"Plasmonic Mo-doped HNb3O8 nanosheets with tunable energy band structures for photothermal catalytic H2 evolution in Full Solar Spectrum","authors":"Junli Chen, Xinyi Jin, Xinli Yang, Lei Deng, Zhiqiang Zhang, Li Feng Han, Feilong Gong, Yonghui Zhang","doi":"10.1039/d4ta06164k","DOIUrl":"https://doi.org/10.1039/d4ta06164k","url":null,"abstract":"Ultrathin Mo-HNb3O8 nanosheets were synthesized by a facile hydrothermal process. Introducing low-valence Mo and oxygen vacancies into the pristine HNb3O8 nanosheets can modulate the band structure and induce the localized surface plasmon resonance (LSPR), which not only efficiently promotes the separation and transfer of photo-generated carriers, but also improves the high utilization rate of solar energy in photothermal catalytic hydrogen evolution in all solar spectrum. The optimized MoNb-10 exhibits the highest H2 evolution rate (220.4 μmol h-1 g-1), which is approximate 7.7 times higher than that of the HNb3O8 nanosheet. The current work not only deepens our understanding LSPR effects generated from the Mo dopant and OVs on the surface of transition metal oxide nanosheets, also provides clues for exploring new photothermal catalyst to promote future solar energy conversion.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589147","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dan Wang, Yuan Chu, Youzheng Wu, Mengkang Zhu, Lin Pan, Ruopeng Li, Yukai Chen, Wenchang Wang, Naotoshi Mitsuzaki, Zhidong Chen
{"title":"Synergistic Coupling of CuNi Alloy with CoFe LDH Heterostructure on Nickel Foam toward High-Efficiency Overall Water Splitting","authors":"Dan Wang, Yuan Chu, Youzheng Wu, Mengkang Zhu, Lin Pan, Ruopeng Li, Yukai Chen, Wenchang Wang, Naotoshi Mitsuzaki, Zhidong Chen","doi":"10.1039/d4ta05681g","DOIUrl":"https://doi.org/10.1039/d4ta05681g","url":null,"abstract":"Accelerating the kinetics of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital for high-efficiency green hydrogen production. However, developing cost-effective and highly active bifunctional catalysts for overall water splitting electrolysis remains a huge challenge. Herein, CuNi/CoFe LDH heterostructure is synthesized in situ on the nickel foam (CuNi/CoFe LDH@NF) by a simple two-step electrodeposition process. The synergy of CuNi alloy and CoFe LDH optimizes the electron distribution at the interface and improves the intrinsic activity of HER/OER. Consequently, the optimal CuNi/CoFe LDH@NF bifunctional catalyst displays low overpotentials of 56 mV (10 mA cm−2) and 268 mV (50 mA cm−2) for HER and OER, respectively, along with high stability in alkaline electrolyte. Remarkably, CuNi/CoFe LDH@NF as the cathode and anode requires a low voltage (1.49 V) to achieve 10 mA cm−2 for overall water splitting. Meanwhile, it also displays favorable stability for operation for 17 h (50 mA cm−2) without obvious decline of cell voltage. Density functional theory calculations indicate that constructing heterojunction interfaces promotes the redistribution of interface electrons and optimizes the free energy of adsorbed intermediates, thereby reducing the energy barrier of the rate-determining step (from *O to *OOH).","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594192","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Elucidating the effects of carbon source on fluorination kinetics and the CFx structure to tailor the energy density of Li/CFx","authors":"Shixue Zhang, Yu Li, Hang Xu, Cong Peng, Lingchen Kong, Zhihao Gui, Wei Feng","doi":"10.1039/d4ta07119k","DOIUrl":"https://doi.org/10.1039/d4ta07119k","url":null,"abstract":"Li/CF<small><sub>x</sub></small> batteries are an essential energy source for advancing smart medicine and deep-space exploration, and increasing their energy density is crucial for large-scale applications. However, CF<small><sub>x</sub></small> cathode development is hindered due to the voltage–capacity trade-off when the actual synthesis is considered. To solve this problem, the mechanism of fluorination and key factors that affect the fluorine pattern must be determined. In this study, we propose a diffusion-controlled fluorination mechanism, and the critical role of the carbon source structure in the fluorination kinetics and fluorine pattern of the formed CF<small><sub>x</sub></small> is revealed. As a proof-of-concept, we prepared a series of hierarchical porous carbons (HPCs) and promoted fluorination kinetics with their well-developed hierarchical pore structure, resulting in a high fluorine content from full interior fluorination and an altered fluorine pattern. In addition, a HPCs enabled low fluorination temperature helped to maintain the skeleton structure and improve the conductivity, resulting in an excellent maximum energy density of 2902.45 Wh kg<small><sup>-</sup></small>1 (0.05 C). Orthogonal experiments, which facilitated the tailoring of battery performance, demonstrated the synergistic effect of the carbon source and fluorination temperature for the first time. This study provides theoretical and practical guidance for designing and implementing CF<small><sub>x</sub></small> cathodes for ultrahigh-energy-density Li/CF<small><sub>x</sub></small> batteries, and the results pave the way for various large-scale applications of Li/CF<small><sub>x</sub></small> batteries in the future.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A Novel Nano C@BaTiO3 Fibers/ Polar Trans-cyclohexane Modified Polyimide Composite Films with Enhanced Dielectric Properties and Energy Storage Density","authors":"xingwu jiang, Xiang Wang, Peifeng Liu, Jinzheng Huang","doi":"10.1039/d4ta06322h","DOIUrl":"https://doi.org/10.1039/d4ta06322h","url":null,"abstract":"Polyimide (PI), a kind of polymer with excellent heat resistance, processing, mechanical and electrical insulation performance, stands out as a prime candidate for advanced dielectric energy storage materials. However, the low dielectric constant of PI has hindered its broader development, requiring dielectric modification. In order to increase the dielectric constant of PI, PI with polar trans-cyclohexane structure was synthesis and characterized and then reinforced with nano C@BT-fibers to produce a novel nano fiber reinforced PI film. Experimental results demonstrate that polar trans-cyclohexane enables pure PI films to achieve a dielectric constant of 8.89 at 100 Hz. Meanwhile, the dielectric constant of C@BT-fibers/modified PI composite films indeed enhance up to 39.48 at 100 Hz and the energy storage density increases to 1.028 J/cm3 with only 1.0 wt% addition content of C@BT-fibers, increased 117.3% compared with pure PI (0.473 J/cm3).","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588613","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Shola: A 3D porous hydrophobic-oleophilic lignocellulosic material for efficient oil/water separation","authors":"Keya Mondal, Kushagra Advani, Snigdha Ghosh, Kadhiravan Shanmuganathan, Goutam Kulshi, Sivaram Swaminathan, Sayam Sen Gupta","doi":"10.1039/d4ta06463a","DOIUrl":"https://doi.org/10.1039/d4ta06463a","url":null,"abstract":"Transitioning from the fossil fuel era to a sustainable future requires increasing adoption of high-performing renewable materials in industrial applications. Natural polymers derived from lignocellulosic materials are often considered more environmentally friendly than their petroleum-based synthetic analogs. <em>Aeschynomene aspera</em>, commonly known as <em>Shola</em>, has been found to be a large source of amorphous cellulose and a useful sorbent for the removal of oil from water. The <em>Shola</em> pith, the pure white inner stem, is rich in cellulose and has an exquisite three-dimensional and hierarchical porous architecture created by nature. The pith consists of about 70 wt.% cellulose as the main chemical component, which is much higher than what is found in other lignocellulosic sources. In addition, the pith has about 12 wt.% hemicellulose, 2-3 wt.% pectin, 10 wt.% lignin, 2.5 wt.% wax, and 2 wt.% protein as other chemical components. It was observed that water has a high contact angle (135˚) on the surface of the pith, while oil droplets instantly spread on the surface, indicating excellent hydrophobic–oleophilic properties. Further studies reveal that <em>Shola</em> pith exhibits a fast and high sorption capacity of 40-60 g/g for various oils and organic liquids. Silicone oil shows a sorption capacity of about 166 g/g. When applied to oil-floating-over-water, the <em>Shola</em> pith exhibits high selectivity for the oil over the water; almost all oil on the surface could be removed, leaving no trace of oil on the water surface. <em>Shola</em> pith can also efficiently separate oil from an oil-in-water emulsion. This behavior is unprecedented in natural sorbents. The used material sorbs a considerable volume of the oil even after the 7th cycle. Furthermore about 95% of sorbed oil could be recovered from the material by solvent extraction. This study reveals for the first time some of the unique and interesting properties of <em>Shola</em>, a widely found biomass native to the eastern parts of the Indian subcontinent, and opens up possibilities of exploiting it for valuable applications.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
chao Wei, Ming Lu, Jing-Jing Li, Ze-Jiu Diao, Guoliang Liu, Xiao-Qin Liu, Lin-Bing Sun
{"title":"A doubly interpenetrated perylene diimide-based zirconium metal-organic framework for selective oxidation of sulfides powered by blue light","authors":"chao Wei, Ming Lu, Jing-Jing Li, Ze-Jiu Diao, Guoliang Liu, Xiao-Qin Liu, Lin-Bing Sun","doi":"10.1039/d4ta06294a","DOIUrl":"https://doi.org/10.1039/d4ta06294a","url":null,"abstract":"Perylene diimide (PDI) with its unique photoactive properties can be employed as an effective building block for synthesizing vigorous metal-organic frameworks (MOFs) and photocatalytic performance can be anticipated. Specifically, we introduce the fabrication of a zirconium-based MOF, Zr-PDI-Me, which is deliberately constructed using PDI units via a solvothermal process. The resulting Zr-PDI-Me exhibits a double interpenetrated topological structure and boasts a considerable specific surface area of up to 634 m2/g. Furthermore, its photoelectric response is satisfactory as evidenced by electrochemical characterizations. Consequently, Zr-PDI-Me has served as a photocatalyst to selectively oxidize sulfides, demonstrating its excellent versatility. Importantly, it retains initial catalytic activity even after 5 cycles. Studies on the mechanism revealed that both superoxide radicals (O<small><sub>2</sub></small><small><sup>•-</sup></small>) and singlet oxygen (<small><sup>1</sup></small>O<small><sub>2</sub></small>) promote the selective oxidation process to produce sulfoxides over Zr-PDI-Me. This work underscores the potential of incorporating photoresponsive organic functional groups into MOFs to create photoactive heterogeneous catalysts.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580713","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Rationally engineered smart automotive upholstery leather based on gradient feeding in situ one-pot reaction in microreactors of natural skin","authors":"Qingxin Han, Huishu Fan, Xuechuan Wang, Junli Zhang, Xinhua Liu, Xiaoyu Guan","doi":"10.1039/d4ta06569g","DOIUrl":"https://doi.org/10.1039/d4ta06569g","url":null,"abstract":"The smart automobile sector, a burgeoning industry today, demands high standards for the manufacturing and performance of smart automotive upholstery leather, driven by continuous innovations in smart technology, comfort, and aesthetics. Herein, natural leather is utilized as a multiscale microporous reactor to create the chemical environment necessary for the preparation of a new smart material (ACG leather), which combines the traditional tannery process with a “gradient feeding <em>in situ</em> one-step preparation strategy”. Leveraging the unique porous structure of attapulgite (ATP) with the incorporation of chitosan (CS) and glycerol triglycidyl ether (GTE), the ACG leather integrates radiation cooling performance (outdoor experiments demonstrate a temperature drop of 8.69 °C), color modulation properties, effective shielding against electromagnetic interference (EMI) (approximately 5.8 dB) and acoustic noise reduction (sound pressure level >22 dB in the frequency range of 992–6400 Hz). Additionally, the bactericidal properties of ACG leather (<em>E. coli</em> inhibition zone diameter = 14 mm, <em>S. aureus</em> inhibition zone diameter = 9 mm), yellowing resistance, mechanical properties (tensile strength of 24.40 MPa, tear strength of 73.52 N mm<small><sup>−1</sup></small>, elongation at break of 91.45%), flame retardancy (LOI = 29.3%), and biodegradability align with sustainable development goals. The advanced design and versatility of ACG leather demonstrate the possibilities for incorporating advanced materials into smart automotive upholstery design, breaking away from traditional manufacturing methods that rely on more material components and complex processes.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588619","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Diffusion Behaviors of Lithium Ions at the Cathode/Electrolyte Interface from Global Neural Network Potentials","authors":"Yufeng Sun, Cheng Shang, Yi-Bin Fang, Zhipan Liu, Xin-Gao Gong, Jihui Yang","doi":"10.1039/d4ta05530f","DOIUrl":"https://doi.org/10.1039/d4ta05530f","url":null,"abstract":"The diffusion of Li ions plays a vital role and has been the central topic of the Li-ion battery (LIB) research. However, the diffusion behaviors at the cathode/electrolyte interface still remain unclear due to the complexity of interfaces. Despite some progress achieved through ab initio molecular dynamics (AIMD) and classical molecular dynamics (MD) simulations, a full understanding of Li-ion diffusion behavior requires direct simulations of the entire interface. This remains challenging due to the inherent limitations of current simulation methods. Here, we develop a global neural network potential to reveal the Li ion diffusion behaviors at the interface between LiCoO<small><sub>2</sub></small> cathode and liquid electrolytes (EC, DMC and LiPF<small><sub>6</sub></small>) by performing long-term molecular dynamics simulations. We identify four kinds of interfacial diffusion behaviors by analyzing the trajectories of Li ions. While the inactive Li ions are immobile, the active Li ions can shuttle between the interface and solution regions, hop between different interfacial sites, or diffuse as they would in pure electrolytes. Among all diffusion behaviors, only those diffusion across the interface can contribute to the effective conductivity and thus the device performance. Based on the above findings, we further study the influence of electrolyte concentration and interfacial compounds on the diffusion of interfacial Li ions. We show that 1 mol/L LiPF<small><sub>6</sub></small> has the largest conductivity across the interface, in agreement with the experimental results that 1 mol/L LiPF<small><sub>6</sub></small> is the most suitable electrolyte concentration. We further propose that Li<small><sub>2</sub></small>O could be used as interface coating to improve the Li ion conductivity across the interface. Our work provides deep atomic insights into the dynamics of Li ions at cathode/electrolyte interface and is expected to help the optimization of LIBs.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Alexandra D. Easley, Cheng-Han Li, Shih-Guo Li, Tan P. Nguyen, Kai-Hua Mick Kuo, Karen L. Wooley, Daniel P. Tabor, Jodie L. Lutkenhaus
{"title":"Electron transport kinetics for viologen-containing polypeptides with varying side group linker spacing","authors":"Alexandra D. Easley, Cheng-Han Li, Shih-Guo Li, Tan P. Nguyen, Kai-Hua Mick Kuo, Karen L. Wooley, Daniel P. Tabor, Jodie L. Lutkenhaus","doi":"10.1039/d4ta06766e","DOIUrl":"https://doi.org/10.1039/d4ta06766e","url":null,"abstract":"Studies investigating the influence of the length of linkers between redox-active moieties and peptide-based polymer backbones were conducted to advance fundamental knowledge toward the design and development of sustainably-sourced, recyclable, and degradable materials for energy applications. In this work, precursor polypeptides were synthesized through the ring-opening polymerizations of <em>N</em>-carboxyanhydrides decorated with varying lengths of alkylchloride side chain groups, followed by post-polymerization installation of the viologen moieties. Electrochemical interrogation of the viologen-based polypeptides provided estimates of the electron transfer rate constants, both heterogeneous (<em>k</em><small><sup>0</sup></small>) and electron self-exchange (<em>k</em><small><sub>ex</sub></small>), the apparent diffusion coefficient (<em>D</em><small><sub>ap</sub></small>), and their device-based energy storage performance. For the first redox couple (viologen dication state to viologen radical-cation state), it was found that the rate of electron transfer among the pendant groups in all viologen-based polypeptides, <em>k</em><small><sub>ex</sub></small>, was not significantly impacted by linker length. In contrast, for the second redox couple (viologen radical-cation state to the neutral viologen), <em>k</em><small><sub>ex</sub></small> varied with linker length and was fastest during reduction from the viologen radical-cation state to the neutral viologen. Most interestingly, a linear relationship was identified between log(<em>k</em><small><sup>0</sup></small>) and log(<em>k</em><small><sub>ex</sub></small>) with a slope of 1.85, indicating that electron transport in the viologen-based polypeptides followed most closely to Marcus–Hush theory with diffusion limitations or Laviron–Andrieux–Savéant (LAS) theory. Finally, the polypeptides were studied in lithium metal half cells to determine the relationship between <em>k</em><small><sub>ex</sub></small> and energy storage performance. The viologen-based polypeptide with the moderate length linker exhibited the highest capacity and lowest degree of swelling, but only moderate <em>k</em><small><sub>ex</sub></small>, demonstrating that the device performance was primarily influenced electrode swelling. Taken together, the viologen-polypeptide backbone dictated the mechanism of electron transfer, whereas the linker length could be used to alter the rate of electron transfer (<em>k</em><small><sub>ex</sub></small>). Balancing the rate of electron transfer (<em>k</em><small><sub>ex</sub></small>) and degree of swelling will be a major challenge to identify polymers for high performance energy storage devices.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":null,"pages":null},"PeriodicalIF":11.9,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588693","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}