Energy & Environmental Materials最新文献

{"title":"Time-Resolved Oxidation State Changes Are Key to Elucidating the Bifunctionality of Perovskite Catalysts for Oxygen Evolution and Reduction","authors":"Casey E. Beall,&nbsp;Emiliana Fabbri,&nbsp;Adam H. Clark,&nbsp;Vivian Meier,&nbsp;Nur Sena Yüzbasi,&nbsp;Benjamin H. Sjølin,&nbsp;Ivano E. Castelli,&nbsp;Dino Aegerter,&nbsp;Thomas Graule,&nbsp;Thomas J. Schmidt","doi":"10.1002/eem2.12737","DOIUrl":"10.1002/eem2.12737","url":null,"abstract":"<p>In a unified regenerative fuel cell (URFC) or reversible fuel cell, the oxygen bifunctional catalyst must switch reversibly between the oxygen reduction reaction (ORR), fuel cell mode, and the oxygen evolution reaction (OER), electrolyzer mode. However, it is often unclear what effect alternating between ORR and OER has on the electrochemical behavior and physiochemical properties of the catalyst. Herein, operando X-ray absorption spectroscopy (XAS) is utilized to monitor the continuous and dynamic evolution of the Co, Mn, and Fe oxidation states of perovskite catalysts Ba_0.5Sr_0.5Co_0.8Fe_0.2O_3-δ (BSCF) and La_0.4Sr_0.6MnO_3-δ (LSM), while the potential is oscillated between reducing and oxidizing potentials with cyclic voltammetry. The results reveal the importance of investigating bifunctional catalysts by alternating between fuel cell and electrolyzer operation and highlight the limitations and challenges of bifunctional catalysts. It is shown that the requirements for ORR and OER performance are divergent and that the oxidative potentials of OER are detrimental to ORR activity. These findings are used to give guidelines for future bifunctional catalyst design. Additionally, it is demonstrated how sunlight can be used to reactivate the ORR activity of LSM after rigorous cycling.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12737","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High Seebeck Coefficient Thermally Chargeable Supercapacitor with Synergistic Effect of Multichannel Ionogel Electrolyte and Ti3C2Tx MXene-Based Composite Electrode","authors":"Zhongming Chen,&nbsp;Zhijian Du,&nbsp;La Li,&nbsp;Kai Jiang,&nbsp;Di Chen,&nbsp;Guozhen Shen","doi":"10.1002/eem2.12756","DOIUrl":"10.1002/eem2.12756","url":null,"abstract":"<p>Thermally chargeable supercapacitors can collect low-grade heat generated by the human body and convert it into electricity as a power supply unit for wearable electronics. However, the low Seebeck coefficient and heat-to-electricity conversion efficiency hinder further application. In this paper, we designed a high-performance thermally chargeable supercapacitor device composed of ZnMn₂O₄@Ti₃C₂T_<i>x</i> MXene composites (ZMO@Ti₃C₂T_<i>x</i> MXene) electrode and UIO-66 metal–organic framework doped multichannel polyvinylidene fluoridehexafluoro-propylene ionogel electrolyte, which realized the thermoelectric conversion and electrical energy storage at the same time. This thermally chargeable supercapacitor device exhibited a high Seebeck coefficient of 55.4 mV K⁻¹, thermal voltage of 243 mV, and outstanding heat-to-electricity conversion efficiency of up to 6.48% at the temperature difference of 4.4 K. In addition, this device showed excellent charge–discharge cycling stability at high-temperature differences (3 K) and low-temperature differences (1 K), respectively. Connecting two thermally chargeable supercapacitor units in series, the generated output voltage of 500 mV further confirmed the stability of devices. When a single device was worn on the arm, a thermal voltage of 208.3 mV was obtained indicating the possibility of application in wearable electronics.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12756","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Stable Organic Solar Cells Enabled by Simultaneous Hole and Electron Interlayer Engineering","authors":"Wisnu Tantyo Hadmojo,&nbsp;Furkan H. Isikgor,&nbsp;Yuanbao Lin,&nbsp;Zhaoheng Ling,&nbsp;Qiao He,&nbsp;Hendrik Faber,&nbsp;Emre Yengel,&nbsp;Roshan Ali,&nbsp;Abdus Samad,&nbsp;Ryanda Enggar Anugrah Ardhi,&nbsp;Sang Young Jeong,&nbsp;Han Young Woo,&nbsp;Udo Schwingenschlögl,&nbsp;Martin Heeney,&nbsp;Thomas D. Anthopoulos","doi":"10.1002/eem2.12712","DOIUrl":"10.1002/eem2.12712","url":null,"abstract":"<p>The development of high-performance organic solar cells (OSCs) with high operational stability is essential to accelerate their commercialization. Unfortunately, our understanding of the origin of instabilities in state-of-the-art OSCs based on bulk heterojunction (BHJ) featuring non-fullerene acceptors (NFAs) remains limited. Herein, we developed NFA-based OSCs using different charge extraction interlayer materials and studied their storage, thermal, and operational stabilities. Despite the high power conversion efficiency (PCE) of the OSCs (17.54%), we found that cells featuring self-assembled monolayers (SAMs) as hole-extraction interlayers exhibited poor stability. The time required for these OSCs to reach 80% of their initial performance (T₈₀) was only 6 h under continuous thermal stress at 85 °C in a nitrogen atmosphere and 1 h under maximum power point tracking (MPPT) in a vacuum. Inserting MoO_x between ITO and SAM enhanced the T₈₀ to 50 and ~15 h after the thermal and operational stability tests, respectively, while maintaining a PCE of 16.9%. Replacing the organic PDINN electron transport layer with ZnO NPs further enhances the cells' thermal and operational stability, boosting the T₈₀ to 1000 and 170 h, respectively. Our work reveals the synergistic roles of charge-selective interlayers and device architecture in developing efficient and stable OSCs.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12712","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927184","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Amphoteric Supramolecular Nanofiber Separator for High-Performance Sodium-Ion Batteries","authors":"Yuping Zhang,&nbsp;Hongzhi Zheng,&nbsp;Xing Tong,&nbsp;Hao Zhuo,&nbsp;Wu Yang,&nbsp;Yuling Chen,&nbsp;Ge Shi,&nbsp;Zehong Chen,&nbsp;Linxin Zhong,&nbsp;Xinwen Peng","doi":"10.1002/eem2.12735","DOIUrl":"10.1002/eem2.12735","url":null,"abstract":"<p>The separator is an essential component of sodium-ion batteries (SIBs) to determine their electrochemical performances. However, the separator with high mechanical strength, good electrolyte wettability and excellent electrochemical performance remains an open challenge. Herein, a new separator consisting of amphoteric nanofibers with abundant functional groups was fabricated through supramolecular assembly of natural polymers for SIB. The uniform nanoporous structure, remarkable mechanical properties and abundant functional groups (e.g. −COOH, −NH₂ and −OH) endow the separator with lower dissolution activation energy and higher ion migration numbers. These metrics enable the separator to lower the barrier for desolvation of Na⁺, accelerate the migration of Na⁺, and generate more stable solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). The battery assembled with the amphoteric nanofiber separator shows higher specific capacity and better stability than that assembled with glass fiber (GF) separator.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12735","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Organic X-Ray Image Sensors Using a Medium Bandgap Polymer Donor with Low Dark Current","authors":"Jong-Woon Ha,&nbsp;Seung Hun Eom,&nbsp;Bo Kyung Cha,&nbsp;Seyeong Song,&nbsp;Hyeong Ju Eun,&nbsp;Jong H. Kim,&nbsp;Jong Mok Park,&nbsp;BongSoo Kim,&nbsp;Byoungwook Park,&nbsp;Seo-Jin Ko,&nbsp;Sung Cheol Yoon,&nbsp;Changjin Lee,&nbsp;In Hwan Jung,&nbsp;Do-Hoon Hwang","doi":"10.1002/eem2.12750","DOIUrl":"10.1002/eem2.12750","url":null,"abstract":"<p>The development of portable X-ray detectors is necessary for diagnosing fractures in unconscious patients in emergency situations. However, this is quite challenging because of the heavy weight of the scintillator and silicon photodetectors. The weight and thickness of X-ray detectors can be reduced by replacing the silicon layer with an organic photodetectors. This study presents a novel bithienopyrroledione-based polymer donor that exhibits excellent photodetection properties even in a thick photoactive layer (~700 nm), owing to the symmetric backbone and highly soluble molecular structure of bithienopyrroledione. The ability of bithienopyrroledione-based polymer donor to strongly suppress the dark current density (<i>J</i>_d ~ 10⁻¹⁰ A cm⁻²) at a negative bias (−2.0 V) while maintaining high responsivity (<i>R</i> = 0.29 A W⁻¹) even at a thickness of 700 nm results in a maximum shot-noise-limited specific detectivity of <i>D</i>_sh* = 2.18 × 10¹³ Jones in the organic photodetectors. Printed organic photodetectors are developed by slot-die coating for use in X-ray detectors, which exhibit <i>D</i>_sh* = 2.73 × 10¹² Jones with clear rising (0.26 s) and falling (0.29 s) response times upon X-ray irradiation. Detection reliability is also proven by linear response of the X-ray detector, and the X-ray detection limit is 3 mA.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12750","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927270","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Water-in-Polymer Salt Electrolyte for Long-Life Rechargeable Aqueous Zinc-Lignin Battery","authors":"Divyaratan Kumar, Leandro R. Franco, Nicole Abdou, Rui Shu, Anna Martinelli, C. Moyses Araujo, Johannes Gladisch, Viktor Gueskine, Reverant Crispin, Ziyauddin Khan","doi":"10.1002/eem2.12752","DOIUrl":"https://doi.org/10.1002/eem2.12752","url":null,"abstract":"Zinc metal batteries (ZnBs) are poised as the next-generation energy storage solution, complementing lithium-ion batteries, thanks to their cost-effectiveness and safety advantages. These benefits originate from the abundance of zinc and its compatibility with non-flammable aqueous electrolytes. However, the inherent instability of zinc in aqueous environments, manifested through hydrogen evolution reactions (HER) and dendritic growth, has hindered commercialization due to poor cycling stability. Enter potassium polyacrylate (PAAK)-based water-in-polymer salt electrolyte (WiPSE), a novel variant of water-in-salt electrolytes (WiSE), designed to mitigate side reactions associated with water redox processes, thereby enhancing the cyclic stability of ZnBs. In this study, WiPSE was employed in ZnBs featuring lignin and carbon composites as cathode materials. Our research highlights the crucial function of acrylate groups from WiPSE in stabilizing the ionic flux on the surface of the Zn electrode. This stabilization promotes the parallel deposition of Zn along the (002) plane, resulting in a significant reduction in dendritic growth. Notably, our sustainable Zn-lignin battery showcases remarkable cyclic stability, retaining 80% of its initial capacity after 8000 cycles at a high current rate (1 A g⁻¹) and maintaining over 75% capacity retention up to 2000 cycles at a low current rate (0.2 A g⁻¹). This study showcases the practical application of WiPSE for the development of low-cost, dendrite-free, and scalable ZnBs.","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"24 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140927023","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":"Nanodiamond-Assisted High Performance Lithium and Sodium Ions Co-Storage","authors":"Xiaochen Sun,&nbsp;Xuan Gao,&nbsp;Chang Su,&nbsp;Wei Cheng,&nbsp;Nan Gao,&nbsp;Xin Zhang,&nbsp;Mengmeng Gong,&nbsp;Haobo Dong,&nbsp;Yuhang Dai,&nbsp;Guanjie He,&nbsp;Hongdong Li","doi":"10.1002/eem2.12749","DOIUrl":"10.1002/eem2.12749","url":null,"abstract":"<p>While lithium resources are scarce for high energy-dense lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), serving as an alternative, inherently suffer from low capacity and the high-cost use of non-graphite anodes. Combining Li- and Na-ions within a single battery system is expected to mitigate the shortcomings of both systems while leveraging their respective advantages. In this study, we developed and assembled a nanodiamonds (NDs)-assisted co-Li/Na-ion battery (ND–LSIB). This innovative battery system comprised a commercial graphite anode, an ND-modified polypropylene (DPP) separator, a hybrid lithium/sodium-based electrolyte, and a cathode. It is theoretically and experimentally demonstrated that the ND/Li co-insertion can serve as an ion-drill opening graphite layers and reconstructing graphite anodes into few-layered graphene with expanding interlayer space, achieving highly efficient Li/Na storage and the theoretical maximum of LiC₆ for Li storage in graphite. In addition, ND is helpful for creating a LiF-/NaF-rich hybrid solid electrolyte interface with improved ionic mobility, mechanical strength, and reversibility. Consequently, ND–LSIBs have higher specific capacities ~1.4 times the theoretical value of LIBs and show long-term cycling stability. This study proposes and realizes the concept of Li/Na co-storage in one ion battery with compatible high-performance, cost-effectiveness, and industrial prospects.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12749","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140835314","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pseudocapacitive Heteroatom-Doped Carbon Cathode for Aluminum-Ion Batteries with Ultrahigh Reversible Stability","authors":"Jiahui Li,&nbsp;Jehad K. El-Demellawi,&nbsp;Guan Sheng,&nbsp;Jonas Björk,&nbsp;Fanshuai Zeng,&nbsp;Jie Zhou,&nbsp;Xiaxia Liao,&nbsp;Junwei Wu,&nbsp;Johanna Rosen,&nbsp;Xingjun Liu,&nbsp;Husam N. Alshareef,&nbsp;Shaobo Tu","doi":"10.1002/eem2.12733","DOIUrl":"10.1002/eem2.12733","url":null,"abstract":"<p>Aluminum (Al)-ion batteries have emerged as a potential alternative to conventional ion batteries that rely on less abundant and costly materials like lithium. Nonetheless, given the nascent stage of advancement in Al-ion batteries (AIBs), attaining electrode materials that can leverage both intercalation capacity and structural stability remains challenging. Herein, we demonstrate a C₃N₄-derived layered N,S heteroatom−doped carbon, obtained at different pyrolysis temperatures, as a cathode material for AIBs, encompassing the diffusion−controlled intercalation and surface-induced capacity with ultrahigh reversibility. The developed layered N,S-doped corbon (N,S-C) cathode, synthesized at 900 °C, delivers a specific capacity of 330 mAh g⁻¹ with a relatively high coulombic efficiency of ~85% after 500 cycles under a current density of 0.5 A g⁻¹. Owing to its reinforced adsorption capability and enlarged interlayer spacing by doping N and S heteroatoms, the N,S-C900 cathode demonstrates outstanding energy storage capacity with excellent rate performance (61 mAh g⁻¹ at 20 A g⁻¹) and ultrahigh reversibility (90 mAh g⁻¹ at 5 A g⁻¹ after 10 000 cycles).</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12733","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140656437","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Low-Strain and High-Energy KVPO4F Cathode with Multifunctional Stabilizer for Advanced Potassium-Ion Batteries","authors":"Yongli Heng,&nbsp;Zhenyi Gu,&nbsp;Jinzhi Guo,&nbsp;Haojie Liang,&nbsp;Yan Liu,&nbsp;Wei Guo,&nbsp;Xinxin Zhao,&nbsp;Xiaotong Wang,&nbsp;Xinglong Wu","doi":"10.1002/eem2.12721","DOIUrl":"10.1002/eem2.12721","url":null,"abstract":"<p>KVPO₄F with excellent structural stability and high operating voltage has been identified as a promising cathode for potassium-ion batteries (PIBs), but limits in sluggish ion transport and severe volume change cause insufficient potassium storage capability. Here, a high-energy and low-strain KVPO₄F composite cathode assisted by multifunctional K₂C₄O₄ electrode stabilizer is exquisitely designed. Systematical electrochemical investigations demonstrate that this composite cathode can deliver a remarkable energy density up to 530 Wh kg⁻¹ with 142.7 mAh g⁻¹ of reversible capacity at 25 mA g⁻¹, outstanding rate capability of 70.6 mAh g⁻¹ at 1000 mA g⁻¹, and decent cycling stability. Furthermore, slight volume change (~5%) and increased interfacial stability with thin and even cathode–electrolyte interphase can be observed through in situ and ex situ characterizations, which are attributed to the synergistic effect from in situ potassium compensation and carbon deposition through self-sacrificing K₂C₄O₄ additive. Moreover, potassium-ion full cells manifest significant improvement in energy density and cycling stability. This work demonstrates a positive impact of K₂C₄O₄ additive on the comprehensive electrochemical enhancement, especially the activation of high-voltage plateau capacity and provides an efficient strategy to enlighten the design of other high-voltage cathodes for advanced high-energy batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 5","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12721","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140663853","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Lithium Salt Combining Fluoroethylene Carbonate Initiates Methyl Methacrylate Polymerization Enabling Dendrite-Free Solid-State Lithium Metal Battery","authors":"Xue Ye,&nbsp;Jianneng Liang,&nbsp;Baorong Du,&nbsp;Yongliang Li,&nbsp;Xiangzhong Ren,&nbsp;Dazhuan Wu,&nbsp;Xiaoping Ouyang,&nbsp;Qianling Zhang,&nbsp;Jianhong Liu","doi":"10.1002/eem2.12751","DOIUrl":"10.1002/eem2.12751","url":null,"abstract":"<p>This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate, lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate. The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism. LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte. Normally, lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer, a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization. However, the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant. The as-prepared poly-methyl methacrylate-based polymer electrolyte has a high ionic conductivity (1.19 × 10⁻³ S cm⁻¹), a wide electrochemical stability window (5 V vs Li⁺/Li), and a high Li ion transference number (<span></span><math>\u0000 <mrow>\u0000 <msub>\u0000 <mi>t</mi>\u0000 <msup>\u0000 <mi>Li</mi>\u0000 <mo>+</mo>\u0000 </msup>\u0000 </msub>\u0000 </mrow></math>) of 0.74 at room temperature (RT). Moreover, this polymerization-derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode, which enabled the Li symmetric cell to achieve a long-term cycling performance at 0.2 mAh cm⁻² for 2800 h. The LiFePO₄ battery with polymerization-derived polymer electrolyte-modified Li metal anode shows a capacity retention of 91.17% after 800 cycles at 0.5 C. This work provides a facile and accessible approach to manufacturing poly-methyl methacrylate-based polymerization-derived polymer electrolyte and shows great potential as an interphase in Li metal batteries.</p>","PeriodicalId":11554,"journal":{"name":"Energy & Environmental Materials","volume":"7 6","pages":""},"PeriodicalIF":13.0,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/eem2.12751","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140660835","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}