{"title":"Smart Quasi-Solid-State Electrolytes with the “Dual Insurance” Mechanism for Thermal Safety and Autonomous Operation in Flexible Energy Storage Devices","authors":"Yanqing Wang, Yanli Zhang, Picheng Chen, Yu Ding, Yuetao Liu, Chuanhui Gao","doi":"10.1002/aenm.202500591","DOIUrl":"https://doi.org/10.1002/aenm.202500591","url":null,"abstract":"The thermal effect crisis poses a significant challenge to large-scale application of energy storage devices. Hydrogel electrolytes are regarded as promising substrates for these applications due to the ionic conductivity and safety. This work presents a quasi-solid-state electrolyte with a dual thermal insurance mechanism based on the unique structural, designed for the long-term safe operation of energy devices. The first protection involves microspheres embedded in the matrix and the hydrogel network, which initiate a dual-linkage effect and accelerate the hydrophilic-to-hydrophobic state transition in response to heat accumulation. This process rapidly closes the ion transport channels. Complementing this mechanism, water evaporation further impedes ion migration, forming the second thermal insurance. Due to the thermal reversibility of hydrogel network, the device's initial capacity can be restored upon cooling. Moreover, the regenerative behavior of electrolyte dynamically regulates matrix's water content, ensuring the recovery of ion transport capacity. Theoretical simulations and experiments demonstrate that the designed hydrogel electrolyte offers a broad and tunable temperature protection range. Notably, this thermally reversible protection can be repeated multiple times without compromising electrochemical performance, facilitating autonomous operation. The prepared hydrogels also demonstrate self-healing capabilities and mechanical flexibility, thereby enhancing the durability of self-heating protected energy storage devices.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841729","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}
Yanxin Shang, Nan Chen, Yuejiao Li, Shi Chen, Li Li, Feng Wu, Renjie Chen
{"title":"Decoding the Entropy-Performance Relationship in Aqueous Electrolytes for Lithium-Ion Batteries","authors":"Yanxin Shang, Nan Chen, Yuejiao Li, Shi Chen, Li Li, Feng Wu, Renjie Chen","doi":"10.1002/aenm.202406118","DOIUrl":"https://doi.org/10.1002/aenm.202406118","url":null,"abstract":"Developing aqueous low-temperature electrolytes aligns with the societal demand for lithium batteries in extreme climates and environments. However, the main challenges include high thermodynamic freezing points, slow ion diffusion, and instability at the interface under low temperatures, resulting in low energy density and poor cycle performance. Here, the role of mixing entropy ΔS<sub>mix</sub>, hydrogen bonding, and electrostatic interactions in achieving an optimal electrolyte composition is explored. By systematically varying the ethyl acetate (EA)/H<sub>2</sub>O ratio, a critical “mixing entropy optimal point” at a molar ratio of 3.91, where the electrolyte exhibits the best balance between molecular disorder and interfacial stability is identified. At this optimal point, EA molecules with polar ester group (-COO-) effectively break the hydrogen-bond network of water, enhancing the ΔS<sub>mix</sub> and lowering the freezing point to −106.95 °C. Furthermore, the stable interfacial chemistry derived from entropy-driven solvation structure effectively suppress hydrogen evolution and expand the electrochemical window to 6.2 V. Full aqueous Li-ion batteries with LiMn<sub>2</sub>O<sub>4</sub>-Li<sub>4</sub>Ti<sub>5</sub>O<sub>12</sub> full cell delivered an initial discharge specific capacity of 135.1 mAh g<sup>−1</sup> for 1000 cycles under rapid 10 C rate. The results provide a promising thermodynamic foundation for designing high-performance aqueous electrolytes, with implications for next-generation low-temperature aqueous lithium-ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841732","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}
Guanzhi Wang, Haoyi Li, Finn Babbe, Andrew Tricker, Ethan J. Crumlin, Junko Yano, Rangachary Mukundan, Xiong Peng
{"title":"Probing Electrode Transformation under Dynamic Operation for Alkaline Water Electrolysis","authors":"Guanzhi Wang, Haoyi Li, Finn Babbe, Andrew Tricker, Ethan J. Crumlin, Junko Yano, Rangachary Mukundan, Xiong Peng","doi":"10.1002/aenm.202500886","DOIUrl":"https://doi.org/10.1002/aenm.202500886","url":null,"abstract":"Alkaline water electrolyzers (AWEs) play a pivotal role in the realm of large-scale hydrogen production. However, AWEs face significant challenges in electrode degradation particularly under dynamic operating conditions, induced by reverse current phenomenon during frequent startup/shutdown. Herein, this study aims to rationalize the degradation mechanisms of AWEs under these conditions. A three-electrode membrane electrode assembly (MEA) setup is first utilized to decouple polarization behaviors of anode and cathode in AWEs. Following a proposed accelerated stress testing protocol, the setup allows for tracking individual electrode performance transformations during frequent reverse current operation. Integrating <i>operando</i> cell studies with in situ and post-mortem characterizations, it is showed that continuous formation of highly active species, nickel (oxy)hydroxides, improves the anode performance for oxygen evolution reaction. On the contrary, irreversible oxidation of nickel to β-nickel hydroxide results in a severe degradation of cathode, leading to material dissolution, poor electrical conductivity and loss of catalytic activity for hydrogen evolution reaction. These results provide insights in nickel-based electrode transformation mechanisms for alkaline water electrolysis and indicate that cathode with higher redox reversibility can potentially improve durability of AWEs under dynamic conditions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841727","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}
Zhiying Lai, Jun Long, Yong Lu, Fenqiang Luo, Lingxing Zeng, Wenbin Lai, Yixin Li, Qingrong Qian, Qinghua Chen, Kai Zhang, Zhenhua Yan, Jun Chen
{"title":"Direct Recycling of Retired Lithium-Ion Batteries: Emerging Methods for Sustainable Reuse","authors":"Zhiying Lai, Jun Long, Yong Lu, Fenqiang Luo, Lingxing Zeng, Wenbin Lai, Yixin Li, Qingrong Qian, Qinghua Chen, Kai Zhang, Zhenhua Yan, Jun Chen","doi":"10.1002/aenm.202501009","DOIUrl":"https://doi.org/10.1002/aenm.202501009","url":null,"abstract":"Among various recycling lithium-ion batteries (LIBs) methods, direct recycling consumes far less energy and fewer chemical agents. Most direct regeneration approaches become the specialized process of repairing individual materials due to the different degraded levels of spent materials. This review summarized the solid-state sintering, hydrothermal, eutectic salt, electrochemical, and other emerging methods used for directly repairing various retired power batteries, with a particular focus on their universality when repairing electrodes. Recent progress of different direct recycling methods for retired power batteries (LiFePO<sub>4</sub>, LiCoO<sub>2</sub>, LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>z</sub>O<sub>2</sub>) are outlined, the progress of pretreatment and removal of impurities are also summarized, emphasizing the importance of improving the technical stability of direct recycling of retired LIBs. A series of challenges and corresponding potential solutions are also proposed for guiding the development of direct recycling methods toward practical application. Developing a direct repairing technology that can adaptively replenish lithium (Li) resources in spent cathode might be an important target in the future. With the development of direct recycling, the economic, universal, and advanced strategies will be applied by fully understanding the repairing mechanism in the foreseeable future.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"108 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841728","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}
Qi Mai, Yiwen Mai, Yiwen Zhong, Ruichang Xue, Baohua Jia, Xinwei Guan, Wubin Du, Hongge Pan, Yitong Li, Zhenfang Zhang, Lingfeng Zhu, Xiaoning Li, Peng Li, Tianyi Ma
{"title":"Intermetallic Electrocatalysts for Small-Molecule Fuel Oxidation","authors":"Qi Mai, Yiwen Mai, Yiwen Zhong, Ruichang Xue, Baohua Jia, Xinwei Guan, Wubin Du, Hongge Pan, Yitong Li, Zhenfang Zhang, Lingfeng Zhu, Xiaoning Li, Peng Li, Tianyi Ma","doi":"10.1002/aenm.202500415","DOIUrl":"https://doi.org/10.1002/aenm.202500415","url":null,"abstract":"Intermetallic compounds with well-ordered crystal structures and precise stoichiometry are emerging as a transformative class of electrocatalysis. Existing reviews have primarily focused on intermetallic compounds for specific electrocatalytic reactions or their synthesis strategies, while a comprehensive perspective on how ordered structures contribute to performance across different electrochemical applications that share similarity remains underexplored. In this review, the recent progress is examined in intermetallic compounds, particularly focusing on their structure–property-performance correlations in four critical small-molecule fuel oxidation reactions, including hydrogen oxidation reactions, formic acid oxidation reactions, methanol oxidation reactions, and ethanol oxidation reactions. These reactions are central to sustainable fuel-cell technologies due to their high theoretical energy densities, relatively benign byproducts, and scalability for clean energy production. This review begins by highlighting the advantages of intermetallic compound nanocrystals over metal alloys, such as their unique crystal structures, exceptional thermodynamic stability, enhanced durability, improved intrinsic activity, optimized distribution of active sites, and benign scalability. Subsequently, their applications in these small-molecule fuel oxidation reactions are comprehensively discussed in detail. This review concludes with an outlook on future directions for the synthesis and application of intermetallic nanocrystals, emphasizing their critical role in advancing sustainable energy technologies.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"17 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841730","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":"Rational Design of Carbon-Based Electrocatalysts for H2O2 Production by Machine Learning and Structural Engineering","authors":"Rong Ma, Gao-Feng Han, Feng Li, Yunfei Bu","doi":"10.1002/aenm.202500953","DOIUrl":"https://doi.org/10.1002/aenm.202500953","url":null,"abstract":"Electrochemical synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) represents an economically viable alternative to conventional anthraquinone processes. While noble metal catalysts have dominated this field, carbon-based materials are emerging as promising alternatives due to their low cost, abundant reserves, and tunable properties. This mini-review summarizes recent advances in computational methods, particularly the integration of density functional theory (DFT) with machine learning (ML), to accelerate the rational design of electrocatalysts by enabling rapid screening and structure-training predictions. Meanwhile, the optimization strategies of carbon-based electrocatalysts are systematically investigated, focusing on four key aspects: atomic-level heterochromatic doping, defect engineering, microenvironment control, and morphological design. Despite significant progress in achieving high selectivity and activity, challenges remain in scaling these materials for industrial applications. Moving carbon-based H<sub>2</sub>O<sub>2</sub> electrocatalysts will require multidisciplinary efforts combining advanced in situ characterization techniques, computational modeling, and process engineering to develop robust catalysts suitable for diverse operating conditions.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"8 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143841764","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}
Nathan James Pataki, Shubhradip Guchait, Badr Jismy, Nicolas Leclerc, Adrica Kyndiah, Martin Brinkmann, Mario Caironi
{"title":"A Label-Like Monolithic Organic Thermoelectric Generator Enabled by Local Inkjet Doping of Aligned Polymer Films (Adv. Energy Mater. 15/2025)","authors":"Nathan James Pataki, Shubhradip Guchait, Badr Jismy, Nicolas Leclerc, Adrica Kyndiah, Martin Brinkmann, Mario Caironi","doi":"10.1002/aenm.202570076","DOIUrl":"https://doi.org/10.1002/aenm.202570076","url":null,"abstract":"<p><b>Organic Thermoelectric Generators</b></p><p>In article number 2404656, Martin Brinkmann, Mario Caironi, and co-workers present a method for integrating aligned organic semiconductor films (P3HT and PBTTT-<sup>8</sup>O) into thin, label-like thermoelectric generators (TEGs). High-temperature rubbing induces advantageous structural anisotropy while local inkjet doping patterns the films on ultrathin substrates. The TEGs exhibit exceptional normalized power densities of 0.33 and 1.04 nW cm<sup>−2</sup> K<sup>−2</sup>, promising applications in healthcare and food packaging.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 15","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570076","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Lattice Plainification Leads to High Thermoelectric Cooling Performance in Physically Vapor-Deposited N-Type PbSe Crystal","authors":"Zhiyao Zhang, Zhan Si, Yuxiang Wei, Yi Wen, Jiankun Kang, Pengpeng Chen, Yichen Li, Yixuan Hu, Jiayi Peng, Yang Jin, Shibo Liu, Haonan Shi, Xiang Gao, Dezheng Gao, Hongyao Xie, Li-Dong Zhao","doi":"10.1002/aenm.202501184","DOIUrl":"https://doi.org/10.1002/aenm.202501184","url":null,"abstract":"Thermoelectric materials enable solid-state cooling, which has drawn significant attention in the electronics industry. Current thermoelectric cooling devices rely on advanced Bi<sub>2</sub>Te<sub>3</sub> alloys. However, the scarcity of the Te element raises the price of thermoelectric devices and limits their widespread use. Therefore, developing high-performance, low-cost thermoelectric materials is a key focus in the field. In this work, a high-performance n-type PbSe crystal is developed through lattice plainification and physical vapor deposition. Adding trace amounts of Sn is found to compensate for intrinsic Pb vacancies, which effectively improves the crystal quality and significantly enhances the electron mobility from 1125 to 1550 cm<sup>2</sup> V<sup>−1</sup> s<sup>−1</sup>. This results in a high power factor of 37 µW cm<sup>−1</sup> K<sup>−2</sup> at room temperature for PbSe crystal, transforming this traditional mid-temperature power generation thermoelectric material into a solid-state refrigeration material. The 7-pairs PbSe-based module achieves a temperature difference of 52 K at room temperature, demonstrating a competitive coefficient of performance (COP) of 3.5 under 5 K cooling conditions. Single-leg efficiency tests also validate a 4.5% conversion efficiency at <i>T</i><sub>h</sub> = 773 K for the material. All of these results demonstrate the practical application value of the physically vapor-deposited PbSe crystal.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"2 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837046","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":"Host–Guest Complexation of α-Cyclodextrin and Triiodide Ions for Enhanced Performance of Ionic Thermoelectric Capacitors (Adv. Energy Mater. 15/2025)","authors":"Shih-Ting Kao, Ching-Chieh Hsu, Shao-Huan Hong, U-Ser Jeng, Chia-Hsin Wang, Shih-Huang Tung, Cheng-Liang Liu","doi":"10.1002/aenm.202570074","DOIUrl":"https://doi.org/10.1002/aenm.202570074","url":null,"abstract":"<p><b>Ionic Thermoelectric Capacitors</b></p><p>In article number 2405502, Cheng-Liang Liu and co-workers present an effective strategy using α-cyclodextrin/triiodide host-guest complexation for hydrogel-based ionic thermoelectric capacitors. With α-cyclodextrin side chains decorating the polyvinyl alcohol-based hydrogel, triiodide diffusion is restricted, enhancing its thermopower.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 15","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570074","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143836036","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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":"Solvent Engineering for Scalable Fabrication of High-Quality Formamidinium Cesium-Based Perovskite Films Toward Highly Efficient and Stable Solar Modules","authors":"Zhaoyi Jiang, Fumeng Ren, Qisen Zhou, Binkai Wang, Zhenxing Sun, Mengjie Li, Zhiguo Zhao, Zonghao Liu, Wei Chen","doi":"10.1002/aenm.202500598","DOIUrl":"https://doi.org/10.1002/aenm.202500598","url":null,"abstract":"Demonstrating the high efficiency and stability of large-area perovskite solar modules (PSMs) is crucial for the industrialization of this innovative photovoltaic technology. However, it remains challenging to achieve the controllable fabrication of high-quality perovskite films over large areas. Herein, a ternary solvent system composed of 2-methoxyethanol (2ME), N,N-dimethylformamide (DMF), and N-methyl-2-pyrrolidone (NMP), is thoroughly investigated to fine-tune the solubility, volatility, and coordination characteristics for formamidinium cesium (FACs) perovskite precursor solution. Initially, 2ME and DMF are employed to adjust the volatility and their coordination of Pb<sup>2+</sup> ions, thereby regulating perovskite nucleation rate. Following this, NMP is introduced as a chelating agent to facilitate the formation of stable intermediate phase, which could extend the processing time window for the solution coating and facilitate crystal growth in the subsequent annealing process. With the optimized solvent system, high-quality, large-area FACs perovskite films are successfully fabricated. The resultant inverted PSMs based on a sole NiO hole-transport layer achieved certified efficiencies of 18.73% and 14.62% with aperture areas of 100.15 and 2123.18 cm<sup>2</sup>. Furthermore, the encapsulated mini-module and sub-module retained 97.2% and 95.8% of their initial efficiencies with maximum power tracking, after aging for 1000 h under 1 and 0.5-sun equivalent white-light illumination, respectively.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"14 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837047","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}