{"title":"Highly Deformable, Ion-Conductive Borohydride-Substituted Sulfide Electrolyte for Superior Performance at Low Stack Pressure.","authors":"Shunsuke Kawaguchi,Naomi Fukiya,Kei Ehara,Tomoyuki Ichikawa,Manami Yoshimura,Eishi Iso,Yuji Sasaki,Yuhei Horisawa,Yoshiteru Mizukoshi,Masaki Shimada,Naoya Ishida,Minoru Kuzuhara,Koji Kawamoto,Takuhiro Miyuki","doi":"10.1002/adma.202507963","DOIUrl":"https://doi.org/10.1002/adma.202507963","url":null,"abstract":"All-solid-state batteries (ASSBs) are promising next-generation energy storage systems that can replace conventional lithium-ion batteries. Further enhancement in battery performance requires the formation of a stable physical interfacial contact between the active material (AM) in the electrode and the solid electrolyte (SE). However, reducing the resistance at the AM-SE interface remains a key challenge. This study focuses on Li3PS4-xLiBH4 (LPSBH), a sulfide-based SE with an argyrodite structure, synthesized by mechanical milling. Although LPSBH is known for its high ionic conductivity, its mechanical properties are not thoroughly examined. Here, the deformability of LPSBH is evaluated by demonstrating that it can be formed at low pressures to achieve high relative density. A quantitative evaluation of the AM-SE interfacial contact using symmetric cells demonstrates the formation of a good AM-SE interfacial contact within the electrode layer. A 13 mAh-class laminated cell with LPSBH stacked onto the negative electrode achieves 6C charging at 25 °C under a low stacked pressure of 5 MPa, along with significant cycle stability, which retains ≈70% capacity after 1000 cycles under 1C/1C conditions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"94 1","pages":"e07963"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Meng Xiao,Jianping Meng,Hulin Zhang,Zhiyi Wu,Zhou Li
{"title":"Ionic Gels for Low-Grade Heat Energy Harvesting and Thermal Sensing.","authors":"Meng Xiao,Jianping Meng,Hulin Zhang,Zhiyi Wu,Zhou Li","doi":"10.1002/adma.202506436","DOIUrl":"https://doi.org/10.1002/adma.202506436","url":null,"abstract":"Harvesting the low-grade heat energy from the environment and the human body remains an underutilized energy. Ionic thermoelectric (i-TE) gels have garnered significant attention in the fields of energy harvesting and sensing due to their exceptional stretchability, adaptability, ease of large-scale fabrication, and excellent thermoelectric performance. This review aims to provide a comprehensive overview of the recent progress of i-TE gels in application of temperature sensing and low-grade heat energy harvesting. The narration begins with the introduction of the synthetic and natural polymer for i-TE gels. Then, various methods are discussed to enhance the mechanical performance (stretchability, self-healing, and mechanical durability) to satisfy the flexible device based on i-TE gels. Noticeably, this work emphatically summarizes the improvement methods of thermopower for i-TE gels, including the preparation of n-type i-TE gels and the bidirectional modulation of their thermopower. Finally, this work explores the diverse applications of i-TE gels, including low-grade heat harvesting, sensing, human-machine interfaces, and biomedical applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"22 1","pages":"e06436"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669525","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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 Bioinspired Piezoelectric Stress Buffer Layer for SiOx-Based Electrodes Toward High-Energy Lithium Batteries.","authors":"Xing Chen,Wenru Li,Cizhen Luo,Huanrui Zhang,Chenhui Gao,Chenghao Sun,Rongxian Wu,Yifan Gong,Pengzhou Mu,Zhaolin Lv,Guanglei Cui","doi":"10.1002/adma.202504360","DOIUrl":"https://doi.org/10.1002/adma.202504360","url":null,"abstract":"High-specific-capacity silicon suboxide (SiOx, 0 < x < 2) anodes have long faced the problems of huge volume expansion, fast capacity decay and unsatisfied rate performance. To overcome these bottlenecks, the volume expansion resistance and electrogenic Na+ transport functions of common rain frog (Breviceps adspersus) epidermis are introduced into the design philosophy of stress buffers for SiOx electrodes. Thereupon, a mechanically robust, piezoelectric (MP) stress buffer layer comprised of ferroelectric tetragonal BaTiO3 nanoparticles and a novel homopolymer (PCM) binder of cyanoethyl carbamate-containing methacrylate is developed. It is demonstrated that MP stress buffer layer with superior mechanical properties effectively inhibits excessive volume expansion and stabilizes the solid electrolyte interface along with much suppressed electrolyte decomposition. Meanwhile, MP stress buffer layer helps expedite the dealloying reaction kinetics of SiOx electrodes in half-cells, mainly owing to the generation of a stress-induced built-in electric field within MP stress buffer layer, conducive to improving battery rate performance. As a result, unprecedented cycling and rate performance can be realized in coin and home-made soft package cells with SiOx and SiOx/graphite composite electrodes. Such a design philosophy of stress buffer layers marks an important milestone in developing high-energy lithium batteries with SiOx-based anodes.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"14 1","pages":"e04360"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"The Synergy Between In Situ Gradient Polymerization and Phase Separation Enables Practical Solid-State Ni-Rich Lithium-Ion Batteries.","authors":"Hao Zhang,Yalan Zhang,Xiaofan Du,Xuesong Ge,Zhixiang Yuan,Shijie Zhang,Duo Wang,Zhaolin Lv,Xinhong Zhou,Jianjun Zhang,Guanglei Cui","doi":"10.1002/adma.202507621","DOIUrl":"https://doi.org/10.1002/adma.202507621","url":null,"abstract":"Solid polymer electrolytes (SPEs) have garnered significant attention due to their exceptional safety property. However, most of the previously reported SPEs cannot well match with high-loading and high-voltage cathodes due to their low ionic conductivity and limited anodic stability. Herein, a SPE with superior compatibility with high-loading Ni-rich cathodes is generated by in situ gradient polymerization of a deep eutectic electrolyte. Besides, a polymerization-induced petaloid phase separation structure enhances interfacial ion transport, resulting in a high room temperature ionic conductivity of 1.5 × 10-3 S cm-1. As a result, the as-assembled high-loading (19.5 mg cm-2) NCM811||graphite full battery exhibites a high capacity retention of 85.3% after 200 cycles and outstanding rate performance (1 C). Industrial 1.2 Ah NCM811||SiOx pouch cell demonstrates unprecefented energy density of 382 Wh kg-1. Moreover, this SPE also exhibits significantly enhanced safety characteristics, delaying the onset temperature of heat release from 157 °C to 266 °C and thermal runaway temperature from 198 °C to 312 °C. This study provides a general and practical avenue to high-energy-density lithium-ion batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"94 1","pages":"e07621"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669604","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Macromolecular Boron-Based Salt Enables Dense Interphases for Long-Cycling Lithium-Sulfur Batteries.","authors":"Dejie Qu,Tao Liu,Youlong Sun,Yuewei Yan,Chuanchuan Li,Zili Cui,Chuanwei Gao,Shuaice Kong,Zengqi Zhang,Zhiming Liu,Shu Zhang,Shitao Wang,Zhaolin Lv,Gaojie Xu,Guicun Li,Guanglei Cui","doi":"10.1002/adma.202505762","DOIUrl":"https://doi.org/10.1002/adma.202505762","url":null,"abstract":"Lithium-sulfur (Li-S) batteries represent a compelling next-generation energy storage system with practical energy densities exceeding 700 Wh kg-1, offering a promising pathway beyond current lithium-ion technology. However, their commercial viability remains constrained by deleterious interfacial reactions between lithium metal anodes and polysulfide-containing electrolytes. Herein, it is presented a molecular engineering approach through a novel boron-based salt, lithium perfluoropinacolatoborate (LiFPB), strategically designed to reinforce the solid electrolyte interphase (SEI) for long-cycling Li-S batteries. LiFPB anions, featuring higher specific charge (mass-to-charge ratio) and larger steric bulk compared to conventional salts, demonstrate enhanced resistance to Helmholtz double-layer repulsion and increased susceptibility to lithium metal reduction, promoting the formation of a robust SEI enriched with LiF and LiBxOy species. The LiFPB-containing electrolyte exhibits superior lithium metal compatibility, achieving a high coulombic efficiency of 99.59%. Consequently, Li-S cells demonstrate markedly improved capacity retention from 50.9% to 75.7% over 200 cycles. This strategy has been successfully scaled to Ah-level Li-S pouch cells, achieving practical energy densities of 408 Wh kg-1 with stable cycling over 75 cycles. This work presents an effective approach to developing long-cycling Li-S batteries through the rational design of electrolyte salt.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"96 1","pages":"e05762"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Kilogram-Scale Production of Ultrafast-Charging Micro-Expanded Graphite Anode toward High-Power and Long-Life Ah-Level Pouch Batteries.","authors":"Yangyang Liu,Haodong Shi,Mingzhe Yang,Haodong Wang,Yuxin Ma,Xiaofeng Li,Daokuan Jin,Changde Ma,Zhihao Ren,Xiaoyu Shi,Feng Zhou,Zhong-Shuai Wu","doi":"10.1002/adma.202506584","DOIUrl":"https://doi.org/10.1002/adma.202506584","url":null,"abstract":"The exponential growth of electric vehicle industry necessitates to rapidly develop fast-charging technology for lithium-ion batteries. However, the mainstream graphite anode encounters significant challenges in fast-charging scenarios, including capacity decay and shortened lifespan caused by the sluggish lithiation kinetics and unstable solid electrolyte interphase. Herein, the kilogram-level scalable production of ultrafast-charging anode (C@MEG) consisting of micro-expanded graphite coated by an ultrathin disordered carbon layer (5 nm) is reported, which simultaneously compensates for the conventional limitation of internal lithium diffusion kinetics and reconfigures the external electrode-electrolyte interface. This uniqueness endows rapid surface-to-bulk lithium transport, with minimized electrode polarization, enhanced pseudocapacitive behavior, and reduced interface impedance. At an ultrafast-charging rate of 10 C, this Li||C@MEG cell exhibits an ultrahigh capacity of 157 mAh g-1, superior to pristine graphite (71 mAh g-1) and previously reported graphite anodes. Moreover, this assembled 1 Ah-level C@MEG||LiCoO2 pouch battery delivers remarkable fast-charging cyclability, showcasing 92% capacity retention after 1000 cycles under 3 A, together with high power density around 1500 W kg-1 under 10 A, corresponding to a short charging time of only 4.2 min, demonstrative of applicability. This work presents a practical scalable fast-charging anode toward high-energy, high-power and long-life batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":"e06584"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiamin Zhang,Zhixin Zhang,Xiuyang Zou,Zheng Shi,Mingqing Shan,Zhe Sun,Siyu Guo,Feng Yan
{"title":"Tailoring COFs with Water and Oxygen Pathways for Efficient Catalyst Interfaces in PEMFCs.","authors":"Jiamin Zhang,Zhixin Zhang,Xiuyang Zou,Zheng Shi,Mingqing Shan,Zhe Sun,Siyu Guo,Feng Yan","doi":"10.1002/adma.202509000","DOIUrl":"https://doi.org/10.1002/adma.202509000","url":null,"abstract":"Proton exchange membrane fuel cells (PEMFCs) have gained significant attention due to their high efficiency and clean emissions. However, reducing platinum (Pt) loadings in PEMFCs remains challenging due to the high mass transport resistance near the catalyst surfaces. This study investigates phosphorylated covalent organic frameworks (P-rCOFs) as ionomers in PEMFCs, aiming to optimize the three-phase interface at the catalyst surface. Through the protonation of tertiary amine sites and precise structural engineering of side chains within the COF framework, well-defined transport channels are created to enhance water and oxygen mass transfer. The results demonstrate that P-rCOF-C4 significantly improves the catalytic performance of commercial Pt/C catalysts, with a half-wave potential 37 mV higher than Nafion. Furthermore, a PEMFC incorporating P-rCOF-C4 as an ionomer binder achieves a peak power density of 2.40 W cm-2 at 0.1 mg cm-2 catalyst loading, a 1.5 fold increase over Nafion. This work underscores the potential of P-rCOFs in optimizing the three-phase interface, offering a promising pathway for more efficient and cost-effective PEMFCs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"35 1","pages":"e09000"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669520","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Achieving Abnormal Evaporation Behavior Using Melanin/Cellulose-Based Solar Evaporators via Salt Ion Enrichment.","authors":"Yanhu Shi,Shang Liu,Yi Zhao,Heng Zhang,Yifan Hou,Xiaoyong Deng,Yijun Xie","doi":"10.1002/adma.202508192","DOIUrl":"https://doi.org/10.1002/adma.202508192","url":null,"abstract":"Solar-driven interfacial evaporation technology has emerged as a promising solution for seawater desalination, offering a potential remedy to the global water crisis. However, its widespread application is hindered by reduced performance in high-salinity brines and limited evaporator lifetimes. Inspired by natural melanins, amino acid-doped poly(norepinephrine) nanoparticles (PNE NPs) are developed as photothermal materials, encapsulated in a cellulose-based aerogel to form a 3D bilayer porous structure with salt ion enrichment effects. The interaction between the enriched ions in the aerogel weakens the hydrogen bonds between water molecules, reducing evaporation enthalpy and enhancing evaporation rates. Under one sun illumination, the evaporator achieves an evaporation rate of 4.06 kg m-2 h-1 in high-concentration saline, surpassing the rate in pure water (3.51 kg m-2 h-1), with the rate increasing further as salt concentration rises. Notably, even the blank control group without photothermal materials shows an evaporation rate of 1.70 kg m-2 h-1, demonstrating the aerogel's strong intrinsic evaporation performance. The aerogel maintains its performance over five months of immersion in water without significant degradation. This low-cost, cellulose-based aerogel offers a promising solution to the issue of evaporation performance degradation in high-salinity brines, making large-scale solar desalination a feasible and effective option.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"4 1","pages":"e08192"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669522","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Edge-Dislocated WO3 Photocathode Toward Efficient Photo-Assisted Li-O2 Batteries.","authors":"Meng Wang,Zhangliu Tian,Guanxing Li,Yukun Xiao,Ganwen Chen,Siyuan Li,Ruiqi Su,Baihua Cui,Chonglai Jiang,Zejun Sun,Haotian Yang,Yu Long,Hui Zhang,Yu Han,Hexing Li,Wei Chen","doi":"10.1002/adma.202501716","DOIUrl":"https://doi.org/10.1002/adma.202501716","url":null,"abstract":"The operation of rechargeable Li-O2 batteries critically depends on the highly reversible formation and decomposition of Li2O2 at the cathode. However, the intrinsic insulating nature of Li2O2 fundamentally restricts reaction kinetics, posing a core challenge to practical applications. Here, it is demonstrate that the insulating properties of Li2O2 can be effectively improved by photoexcitation, attributed to the generation of photo-induced charge carriers. It is inspired to develop photo-assisted Li-O2 batteries featuring Z-type photocathode@Li2O2 heterojunction, which serves as a charge modulation channel to regulate carrier dynamics through photocathode modifications. By employing edge-dislocated WO3 as the photocathode, sustained growth of Li2O2 films is observed with a thickness >18 µm, which is 2-3 orders of magnitude higher than typically reported values. Benefiting from the enhanced exciton dissociation of Li2O2 and improved oxidative capability of photocathode, the battery delivers an ultra-high discharge capacity of 31 800 mAh g-1 under a current density of 100 mA g-1 and a light-induced temperature of ≈60 °C. In addition, a low polarization overpotential of 0.04 V is achieved with high reversibility over 1 000 h. The grasp of photoexcited Li2O2 within Li-O2 batteries can drive solutions beyond state-of-the-art metal-air batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"35 1","pages":"e01716"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669532","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Visible Light-Driven Spatiotemporal-Resolved Proton Management by Harnessing Merocyanine-Integrated Hydrogels as Regenerative Photoacid Matrices.","authors":"Guodong Wang,Meiqing Yang,Ze Gong,Chuang Li","doi":"10.1002/adma.202508265","DOIUrl":"https://doi.org/10.1002/adma.202508265","url":null,"abstract":"Photomanipulation of the environmental pH plays a crucial role in modulating the reaction kinetics and engineering material functionalities. While conventional merocyanine photoacids offer pH modulability, their practical implementation is fundamentally constrained by aqueous dissolution and laborious regeneration. Here, a transformative strategy is reported through the covalent integration of merocyanine photoacids into hydrophilic polymer networks to construct regenerative photoacid matrices, which stably retain protons in the dark and spatiotemporally liberate them upon illumination. The photoacid matrix overcomes solubility constraints through adjustable merocyanine grafting density while simultaneously enhancing alkaline stability, thereby enabling shape-governed, diffusion-controlled proton release kinetics. The universality of this approach has been extensively verified in multiple polymer matrices with variable chemical compositions. Upon straightforward separation and acidic regeneration in the dark, the recovered matrices sustainably maintain robust photoactivated proton release capability. This not only enables programmable control over acid-base indicator discoloration but also guides hierarchical self-assembly of arylazopyrazole-based hydrogelators, yielding 3D supramolecular gel architectures with tailored complexity. Furthermore, spatially controlled directional proton liberation are established through synergistically addressing negative phototropic deformation within a low-density crosslinked photoacid matrix. This work creates a new paradigm for spatiotemporal pH manipulation in the development of autonomous materials through regenerative photoacid matrices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"94 1","pages":"e08265"},"PeriodicalIF":29.4,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669556","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}