Chuanyao Sun, Pengfei Qiu, Xinjie Yuan, Kelin Shen, Yi Wu, Xuefeng Zhao, Jiawei Zhang, Shiqi Yang, Lidong Chen, Xun Shi
Thermoelectric (TE) technology can convert human body heat into useful electricity, providing a promising solution to develop self-powered wearable electronics, in which both high output voltage density and power density are urgently required. However, the existing TE devices usually possess low voltage density in the wearing condition, greatly limiting their real applications. In this work, we propose a novel highly integrated blade structure, which can achieve ultrahigh output voltage and power densities. The finite element simulation gives the optimal geometric dimensions and integration numbers of the TE legs for the blade structure. In the experiment, we successfully fabricated the blade TE device by using the recently discovered Ag-based ductile inorganic TE materials with the TE leg density and aspect ratio of 300 cm−2 and 1250 cm−1, respectively. Such high values have not been simultaneously achieved for the TE devices reported before. An ultrahigh voltage density of up to 869.6 mV cm−2 is achieved when the blade device is worn on the human body, which is at least one order of magnitude higher than the existing TE devices. Likewise, the blade TE devices also exhibit high power density up to 114.1 µW cm−2, among the highest values reported so far. The electricity converted from body heat by the blade TE device can directly power an electronic watch, showing great potential to be used in real applications.
热电（TE）技术可以将人体热量转化为有用的电能，为开发迫切需要高输出电压密度和高功率密度的自供电可穿戴电子产品提供了一个有希望的解决方案。然而，现有的TE器件在磨损状态下通常具有较低的电压密度，极大地限制了其实际应用。在这项工作中，我们提出了一种新的高度集成的叶片结构，可以实现超高的输出电压和功率密度。有限元仿真给出了叶片结构中TE支腿的最优几何尺寸和积分数。在实验中，我们利用新发现的ag基延展性无机TE材料，成功制备了叶片TE器件，TE支腿密度为300 cm−2，长径比为1250 cm−1。如此高的数值并没有同时达到之前报道的TE设备。当叶片器件佩戴在人体上时，可实现高达869.6 mV cm−2的超高电压密度，比现有TE器件高出至少一个数量级。同样，叶片TE器件也具有高达114.1 μ W cm−2的高功率密度，是迄今为止报道的最高值之一。刀片TE装置将人体热量转化为电能，可以直接为电子表供电，在实际应用中显示出巨大的潜力。
{"title":"A highly integrated blade structure for thermoelectric devices with ultra-high output voltage and power densities","authors":"Chuanyao Sun, Pengfei Qiu, Xinjie Yuan, Kelin Shen, Yi Wu, Xuefeng Zhao, Jiawei Zhang, Shiqi Yang, Lidong Chen, Xun Shi","doi":"10.1039/d5ee06920c","DOIUrl":"https://doi.org/10.1039/d5ee06920c","url":null,"abstract":"Thermoelectric (TE) technology can convert human body heat into useful electricity, providing a promising solution to develop self-powered wearable electronics, in which both high output voltage density and power density are urgently required. However, the existing TE devices usually possess low voltage density in the wearing condition, greatly limiting their real applications. In this work, we propose a novel highly integrated blade structure, which can achieve ultrahigh output voltage and power densities. The finite element simulation gives the optimal geometric dimensions and integration numbers of the TE legs for the blade structure. In the experiment, we successfully fabricated the blade TE device by using the recently discovered Ag-based ductile inorganic TE materials with the TE leg density and aspect ratio of 300 cm<small><sup>−2</sup></small> and 1250 cm<small><sup>−1</sup></small>, respectively. Such high values have not been simultaneously achieved for the TE devices reported before. An ultrahigh voltage density of up to 869.6 mV cm<small><sup>−2</sup></small> is achieved when the blade device is worn on the human body, which is at least one order of magnitude higher than the existing TE devices. Likewise, the blade TE devices also exhibit high power density up to 114.1 µW cm<small><sup>−2</sup></small>, among the highest values reported so far. The electricity converted from body heat by the blade TE device can directly power an electronic watch, showing great potential to be used in real applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"72 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146056969","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}
Monolithic perovskite/silicon tandem solar cells have emerged as a compelling route, combining the certified power conversion efficiencies exceeding 34% for laboratory-scale devices with more cost-effective manufacturing compared to market-established silicon photovoltaics. Despite deployment in pilot processing lines beyond the lab stage, this technology still faces scaling challenges from perovskite sub-cells, such as the incompatibility with contemporary mass production lines and the upscaling efficiency deficit, that are expected to be resolved within a few years to achieve commercial viability. Here, we comprehensively elaborate the scalable deposition and drying methods of perovskite sub-cells on silicon substrates and review their recent advanced progress. We assess the merits and limitations of these competing methods, providing a systematic framework for achieving efficient and durable large-area perovskite/silicon tandem solar cells suitable for industrial production.
{"title":"Scalable deposition and drying methods toward large-area monolithic perovskite/silicon tandem solar cells","authors":"Chenxia Kan, Chao Luo, Yi Hou","doi":"10.1039/d5ee06772c","DOIUrl":"https://doi.org/10.1039/d5ee06772c","url":null,"abstract":"Monolithic perovskite/silicon tandem solar cells have emerged as a compelling route, combining the certified power conversion efficiencies exceeding 34% for laboratory-scale devices with more cost-effective manufacturing compared to market-established silicon photovoltaics. Despite deployment in pilot processing lines beyond the lab stage, this technology still faces scaling challenges from perovskite sub-cells, such as the incompatibility with contemporary mass production lines and the upscaling efficiency deficit, that are expected to be resolved within a few years to achieve commercial viability. Here, we comprehensively elaborate the scalable deposition and drying methods of perovskite sub-cells on silicon substrates and review their recent advanced progress. We assess the merits and limitations of these competing methods, providing a systematic framework for achieving efficient and durable large-area perovskite/silicon tandem solar cells suitable for industrial production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"50 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034081","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}
To advance the practical application of potassium-ion batteries (PIBs), the lack of robust electrolytes must be addressed, as the prevailing fluorinated solvents present a cost-prohibitive and environmentally unsustainable solution. Here, we propose an asymmetric alkylation strategy to overcome this limitation, engineering a fluorine-free, high-flash-point, and green ether-based electrolyte. This design reconstitutes the solvent coordination geometry through dual steric hindrance, which concurrently weakens cation-solvent binding and modulates the electronic structure of the solvation cluster. Consequently, the designed electrolyte demonstrates exceptional interfacial compatibility, enabling the high-voltage K2Mn[Fe(CN)6]||graphite and K2Mn[Fe(CN)6]||hard carbon full-cells to achieve capacity retention rates of 75.75% after 1400 cycles at 0.33 C and 80.09% after 1500 cycles at 0.5 C, respectively. Moreover, this stability is preserved under elevated temperatures, with both full-cells exhibiting stable operation over hundreds of cycles. This work establishes an effective electrolyte design strategy for realizing high-performance, cost-effective, and environmentally friendly PIBs.
{"title":"Solvation Geometry Engineering for Stable High-Voltage Potassium-Ion Batteries","authors":"Zhe Zhang, Wenli Qi, Shiwan Zhang, Jiacheng Zhu, Linlin Wang, Yue Bai, Jiale Chen, Yifan Chen, Guangqiang Hou, Xiaogang Niu, Xuefeng Wang, Ji-Tao Chen, Xiao Ji, Yujie Zhu","doi":"10.1039/d5ee07550e","DOIUrl":"https://doi.org/10.1039/d5ee07550e","url":null,"abstract":"To advance the practical application of potassium-ion batteries (PIBs), the lack of robust electrolytes must be addressed, as the prevailing fluorinated solvents present a cost-prohibitive and environmentally unsustainable solution. Here, we propose an asymmetric alkylation strategy to overcome this limitation, engineering a fluorine-free, high-flash-point, and green ether-based electrolyte. This design reconstitutes the solvent coordination geometry through dual steric hindrance, which concurrently weakens cation-solvent binding and modulates the electronic structure of the solvation cluster. Consequently, the designed electrolyte demonstrates exceptional interfacial compatibility, enabling the high-voltage K<small><sub>2</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>]||graphite and K<small><sub>2</sub></small>Mn[Fe(CN)<small><sub>6</sub></small>]||hard carbon full-cells to achieve capacity retention rates of 75.75% after 1400 cycles at 0.33 C and 80.09% after 1500 cycles at 0.5 C, respectively. Moreover, this stability is preserved under elevated temperatures, with both full-cells exhibiting stable operation over hundreds of cycles. This work establishes an effective electrolyte design strategy for realizing high-performance, cost-effective, and environmentally friendly PIBs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"32 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146021855","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}
Suo Li, Libo Li, Hang Yang, Zhixuan Wang, Xiangrui Deng, Wenyi Lu, Wenhao Xu
Lithium-sulfur (Li-S) batteries promise exceptional theoretical energy density but face persistent challenges, notably polysulfide shuttling and sluggish redox kinetics. High-entropy materials (HEMs), leveraging their distinctive configurational entropy and unparalleled compositional tunability, offer a transformative approach to engineer electrochemical interfaces and address these critical limitations. This review comprehensively surveys the recent advancements in the rational design and application of HEMs for Li-S batteries. We first analyze the structural and electronic characteristics of HEMs and clarify how they enhance sulfur utilization, suppress lithium polysulfides (LiPSs) shuttling by anchoring intermediates, and accelerate LiPSs redox reactions through tailored electronic structures. Subsequently, state-of-the-art design strategies are critically examined, including atomic-scale elemental selection, advanced synthetic methodologies, and multidimensional structural engineering. These strategies enable fabrication of components such as sulfur hosts with optimized adsorption and catalytic sites, separator modifiers that regulate ion-selective transport, and protective interlayers that mitigate lithium dendrite growth. Furthermore, we systematically review cutting-edge characterization techniques and computational methods that detail the mechanisms behind entropy-mediated improvements in battery performance. Finally, critical challenges and promising future research directions are highlighted for the development of next-generation HEM-based energy storage systems, and the insights presented in this review will guide the rational design and practical implementation of HEMs in advanced Li-S batteries.
{"title":"Breaking the boundaries of Li-S batteries with high-entropy engineered multifunctional materials","authors":"Suo Li, Libo Li, Hang Yang, Zhixuan Wang, Xiangrui Deng, Wenyi Lu, Wenhao Xu","doi":"10.1039/d5ee05863e","DOIUrl":"https://doi.org/10.1039/d5ee05863e","url":null,"abstract":"Lithium-sulfur (Li-S) batteries promise exceptional theoretical energy density but face persistent challenges, notably polysulfide shuttling and sluggish redox kinetics. High-entropy materials (HEMs), leveraging their distinctive configurational entropy and unparalleled compositional tunability, offer a transformative approach to engineer electrochemical interfaces and address these critical limitations. This review comprehensively surveys the recent advancements in the rational design and application of HEMs for Li-S batteries. We first analyze the structural and electronic characteristics of HEMs and clarify how they enhance sulfur utilization, suppress lithium polysulfides (LiPSs) shuttling by anchoring intermediates, and accelerate LiPSs redox reactions through tailored electronic structures. Subsequently, state-of-the-art design strategies are critically examined, including atomic-scale elemental selection, advanced synthetic methodologies, and multidimensional structural engineering. These strategies enable fabrication of components such as sulfur hosts with optimized adsorption and catalytic sites, separator modifiers that regulate ion-selective transport, and protective interlayers that mitigate lithium dendrite growth. Furthermore, we systematically review cutting-edge characterization techniques and computational methods that detail the mechanisms behind entropy-mediated improvements in battery performance. Finally, critical challenges and promising future research directions are highlighted for the development of next-generation HEM-based energy storage systems, and the insights presented in this review will guide the rational design and practical implementation of HEMs in advanced Li-S batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"43 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146021856","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}
Zinc–air batteries are considered promising candidates for the next generation of batteries due to their significant advantages in theoretical specific capacity, safety, and environmental friendliness. The combination of gel polymer electrolytes and zinc–air batteries further expands future energy storage applications. However, traditional alkaline gel zinc–air batteries are usually constructed by post-stacking methods, and their poor interfacial contact and weakened long-term durability in the ambient air hinders practical applications. Here, we synthesized a non-alkaline gel electrolyte with a liquid–solid phase transition mechanism utilizing agar, and constructed an integrated gel zinc–air battery by direct injection and encapsulation methods. This strategy realizes the integrated assembly of non-alkaline gel zinc–air full batteries, thereby obtaining all-round high stability. The agar gel electrolyte endows the battery with outstanding performance, including a high output specific capacity (706 mAh g Zn−1), a long discharge duration (270 h at 0.1 mA cm−2), and a significant operational life (850 h at 0.2 mA cm−2). Importantly, the integrated zinc–air pouch battery can achieve a high zinc utilization rate of over 80% in various discharge states and exhibit satisfactory cycling stability (>200 h at 0.1 mA cm−2). This technology alleviates the current challenges of gel zinc batteries, and highlights the direction for the development of non-alkaline gel zinc–air full batteries.
锌空气电池在理论比容量、安全性和环保性方面具有显著的优势，被认为是下一代电池的有希望的候选者。凝胶聚合物电解质和锌空气电池的结合进一步扩展了未来的储能应用。然而，传统的碱性凝胶锌-空气电池通常采用后堆叠方法构建，其界面接触差，在环境空气中的长期耐用性减弱，阻碍了实际应用。本研究利用琼脂合成了一种具有液固相变机理的非碱性凝胶电解质，并采用直接注射和包封的方法构建了一体化凝胶锌-空气电池。该策略实现了非碱性凝胶锌-空气全电池的集成化组装，从而获得全方位的高稳定性。琼脂凝胶电解质赋予电池优异的性能，包括高输出比容量（706 mAh g Zn−1），长放电时间（0.1 mA cm−2下270小时）和显著的使用寿命（0.2 mA cm−2下850小时）。重要的是，集成锌-气囊电池在各种放电状态下都能达到80%以上的锌利用率，并表现出令人满意的循环稳定性（0.1 mA cm−2下200小时）。该技术缓解了凝胶锌电池目前面临的挑战，为非碱性凝胶锌-空气全电池的发展指明了方向。
{"title":"A highly stable zinc–air battery based on a non-alkaline agar gel electrolyte","authors":"Pengfei Zhang, Xinjie Li, Ziyue Li, Jiayun Zhang, Qian Wen, Runjing Xu, Jinyu Yang, Mingxu Wang, Chaoxin Wu, Fengmei Wang, Ya Zhang, Zihao Zhang, Dalin Sun, Fang Fang, Qian Cheng, Fei Wang","doi":"10.1039/d5ee06236e","DOIUrl":"https://doi.org/10.1039/d5ee06236e","url":null,"abstract":"Zinc–air batteries are considered promising candidates for the next generation of batteries due to their significant advantages in theoretical specific capacity, safety, and environmental friendliness. The combination of gel polymer electrolytes and zinc–air batteries further expands future energy storage applications. However, traditional alkaline gel zinc–air batteries are usually constructed by post-stacking methods, and their poor interfacial contact and weakened long-term durability in the ambient air hinders practical applications. Here, we synthesized a non-alkaline gel electrolyte with a liquid–solid phase transition mechanism utilizing agar, and constructed an integrated gel zinc–air battery by direct injection and encapsulation methods. This strategy realizes the integrated assembly of non-alkaline gel zinc–air full batteries, thereby obtaining all-round high stability. The agar gel electrolyte endows the battery with outstanding performance, including a high output specific capacity (706 mAh g Zn<small><sup>−1</sup></small>), a long discharge duration (270 h at 0.1 mA cm<small><sup>−2</sup></small>), and a significant operational life (850 h at 0.2 mA cm<small><sup>−2</sup></small>). Importantly, the integrated zinc–air pouch battery can achieve a high zinc utilization rate of over 80% in various discharge states and exhibit satisfactory cycling stability (>200 h at 0.1 mA cm<small><sup>−2</sup></small>). This technology alleviates the current challenges of gel zinc batteries, and highlights the direction for the development of non-alkaline gel zinc–air full batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"31 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146042999","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}
Niklas H. Deissler, J. Bjarke V. Mygind, Valerie A. Niemann, Jakob B. Pedersen, Valentin Vinci, Shaofeng Li, Xianbiao Fu, Thomas F. Jaramillo, Jakob Kibsgaard, Jakub Drnec, Ib Chorkendorff
The lithium-mediated nitrogen reduction reaction (Li-NRR) is currently the most promising strategy for electrochemical ammonia synthesis. In this study, we present an operando grazing incidence wide angle X-ray scattering (GI WAXS) investigation using an improved electrochemical flow cell that enables hydrogen oxidation at the anode and thereby eliminates the need of a sacrificial proton donor. The improved cell design also increases nitrogen availability and mass transport, achieving ammonia faradaic efficiencies (FEs) up to 36%. This setup allows direct analysis of reaction intermediates and the solid electrolyte interphase (SEI) using state-of-the-art diglyme-based electrolytes. We identify lithium amide (LiNH2) as the only stable, crystalline intermediate, providing direct insight into the Li-NRR mechanism. Notably, in diglyme-based electrolytes, the SEI composition differs significantly from that in tetrahydrofuran-based systems, with reduced LiF content and the formation of previously unreported crystalline diglyme–lithium salt complexes. These species likely influence ammonia selectivity and long-term stability. Our findings highlight how the electrolyte composition and cell architecture govern Li-NRR selectivity and efficiency, offering a foundation for the rational design of next-generation SEI layers and solid electrolytes to enable scalable electrochemical ammonia synthesis.
{"title":"Unveiling the mechanism of lithium-mediated nitrogen reduction via operando X-ray scattering in a flow cell with hydrogen oxidation","authors":"Niklas H. Deissler, J. Bjarke V. Mygind, Valerie A. Niemann, Jakob B. Pedersen, Valentin Vinci, Shaofeng Li, Xianbiao Fu, Thomas F. Jaramillo, Jakob Kibsgaard, Jakub Drnec, Ib Chorkendorff","doi":"10.1039/d5ee06529a","DOIUrl":"https://doi.org/10.1039/d5ee06529a","url":null,"abstract":"The lithium-mediated nitrogen reduction reaction (Li-NRR) is currently the most promising strategy for electrochemical ammonia synthesis. In this study, we present an <em>operando</em> grazing incidence wide angle X-ray scattering (GI WAXS) investigation using an improved electrochemical flow cell that enables hydrogen oxidation at the anode and thereby eliminates the need of a sacrificial proton donor. The improved cell design also increases nitrogen availability and mass transport, achieving ammonia faradaic efficiencies (FEs) up to 36%. This setup allows direct analysis of reaction intermediates and the solid electrolyte interphase (SEI) using state-of-the-art diglyme-based electrolytes. We identify lithium amide (LiNH<small><sub>2</sub></small>) as the only stable, crystalline intermediate, providing direct insight into the Li-NRR mechanism. Notably, in diglyme-based electrolytes, the SEI composition differs significantly from that in tetrahydrofuran-based systems, with reduced LiF content and the formation of previously unreported crystalline diglyme–lithium salt complexes. These species likely influence ammonia selectivity and long-term stability. Our findings highlight how the electrolyte composition and cell architecture govern Li-NRR selectivity and efficiency, offering a foundation for the rational design of next-generation SEI layers and solid electrolytes to enable scalable electrochemical ammonia synthesis.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"48 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022030","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}
Hyun-Wook Lee, Woojin Jeong, Seong Soo Park, Ho-Jeong Ji, Ji-Su Woo, Juhyun Lee, Ye-Jin An, Yu-Chan Hwang, Dong-Ha Kim, Hongjun Chang, Minseok Kim, Mikang Jeong, Moonsu Yoon, Dongsoo Lee, Jongsoon Kim, Zheng-Long Xu, Taeseup Song, Janghyuk Moon, Junghyun Choi, Won-Jin Kwak
Dry-processed thick electrodes are a key strategy for increasing the energy density of batteries. However, thick dry electrodes, especially anodes, suffer from limited ion mobility, causing non-uniform solid-electrolyte interphase (SEI) formation and high irreversible capacity loss during the initial cycle. Moreover, the adhesive primer layer required during processing increases electrical resistance and necessitates additional wet-processing steps, thereby undermining both performance and process integrity. To address these issues, we propose an underlayer lithium-metal-configured prelithiation strategy for thick electrodes. Here, a lithium metal underlayer simultaneously functions as a primer, compensates for irreversible lithium loss during the initial cycle, and promotes uniform SEI formation through a chemical reaction. Consequently, this strategy enhances the initial Coulombic efficiency and cycle stability of high-energy-density silicon-graphite/NCM811 full-cells. By overcoming the limitations of conventional dry process, it enables a fully dry manufacturing process and advances the development of next-generation high-energy-density batteries.
{"title":"Integrated one-step dry process enabling prelithiated thick electrodes without primer coating for high energy density and initial Coulombic efficiency","authors":"Hyun-Wook Lee, Woojin Jeong, Seong Soo Park, Ho-Jeong Ji, Ji-Su Woo, Juhyun Lee, Ye-Jin An, Yu-Chan Hwang, Dong-Ha Kim, Hongjun Chang, Minseok Kim, Mikang Jeong, Moonsu Yoon, Dongsoo Lee, Jongsoon Kim, Zheng-Long Xu, Taeseup Song, Janghyuk Moon, Junghyun Choi, Won-Jin Kwak","doi":"10.1039/d5ee05739f","DOIUrl":"https://doi.org/10.1039/d5ee05739f","url":null,"abstract":"Dry-processed thick electrodes are a key strategy for increasing the energy density of batteries. However, thick dry electrodes, especially anodes, suffer from limited ion mobility, causing non-uniform solid-electrolyte interphase (SEI) formation and high irreversible capacity loss during the initial cycle. Moreover, the adhesive primer layer required during processing increases electrical resistance and necessitates additional wet-processing steps, thereby undermining both performance and process integrity. To address these issues, we propose an underlayer lithium-metal-configured prelithiation strategy for thick electrodes. Here, a lithium metal underlayer simultaneously functions as a primer, compensates for irreversible lithium loss during the initial cycle, and promotes uniform SEI formation through a chemical reaction. Consequently, this strategy enhances the initial Coulombic efficiency and cycle stability of high-energy-density silicon-graphite/NCM811 full-cells. By overcoming the limitations of conventional dry process, it enables a fully dry manufacturing process and advances the development of next-generation high-energy-density batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"71 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146021857","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}
Mitigating surface-initiated structural degradation that propagates inward and depletes all active particles is critical to improving the cycle lifespan of Co-free ultrahigh-Ni NMAs (LiNi 1-x-y Mn x Al y O 2 , 1-x-y-z ≥ 0.9) cathodes. Herein, an epitaxially grown lattice-coherent surface with stabilized low-Ni valence state and refined primary particles have been precisely implemented in LiNi 0.9 Mn 0.05 Al 0.05 O 2 by designing the internal composition distribution within secondary particles, simultaneously ameliorating surface chemistry and mechanical integrity. Key findings indicate that Mn 4+ retained on the particle crust facilitates a layer of localized coherent Li/Ni antisite defects on the periphery of the primary particles located on the surface of the secondary particle, which stabilizes the intrinsic nature of surface lattice. Meanwhile, thermally driven and inward diffusion of Mn during calcination, which acts as an oxygen carrier, ameliorates the local oxygen environment and suppresses interfacefusion intermediate phases (cation mixing) to refine the primary particles. The robust morphological integrity provided by refined primary particles prevents intergranular crack, confining interfacial parasitic reactions to the surface region of secondary particles protected by the lattice-coherent epitaxial surface. This universal approach optimally balances surface stabilization with charge transfer, significant enhancing capacity retention and rate capability for NMA cathode while opening new avenue for the next generation Co-free ultrahigh-Ni cathodes.
减轻表面引发的向内扩散并耗尽所有活性颗粒的结构降解对于提高无co超高ni nma （LiNi 1-x-y Mn x Al y O 2, 1-x-y-z≥0.9）阴极的循环寿命至关重要。本文通过设计二次粒子内部的成分分布，在LiNi 0.9 Mn 0.05 Al 0.05 o2中精确地实现了具有稳定的低ni价态和精炼一次粒子的外延生长晶格相干表面，同时改善了表面化学和机械完整性。主要研究结果表明：Mn - 4+在颗粒壳上的保留有利于在二次颗粒表面的一次颗粒外围形成一层局域相干Li/Ni反位缺陷，从而稳定了表面晶格的固有性质；同时，Mn作为氧载体，在煅烧过程中热驱动向内扩散，改善了局部氧环境，抑制了界面融合中间相（阳离子混合），细化了初生颗粒。精致的初级颗粒提供的强大的形态完整性防止了晶间裂纹，将界面寄生反应限制在由晶格相干外延表面保护的次级颗粒的表面区域。这种通用的方法最佳地平衡了表面稳定性和电荷转移，显著提高了NMA阴极的容量保持和速率能力，同时为下一代无co超高镍阴极开辟了新的途径。
{"title":"Lattice-Coherent Epitaxial Surface Engineering in Highly Stable Co-Free Ultrahigh-Ni Cathodes","authors":"Fuqiren Guo, Liangchi Yang, Shuli Zheng, Xianyan Qiao, Heng Zhang, Yong Ming, Fang Wan, Zhen Guo Wu, Lang Qiu, Xiaodong Guo","doi":"10.1039/d5ee07209c","DOIUrl":"https://doi.org/10.1039/d5ee07209c","url":null,"abstract":"Mitigating surface-initiated structural degradation that propagates inward and depletes all active particles is critical to improving the cycle lifespan of Co-free ultrahigh-Ni NMAs (LiNi 1-x-y Mn x Al y O 2 , 1-x-y-z ≥ 0.9) cathodes. Herein, an epitaxially grown lattice-coherent surface with stabilized low-Ni valence state and refined primary particles have been precisely implemented in LiNi 0.9 Mn 0.05 Al 0.05 O 2 by designing the internal composition distribution within secondary particles, simultaneously ameliorating surface chemistry and mechanical integrity. Key findings indicate that Mn 4+ retained on the particle crust facilitates a layer of localized coherent Li/Ni antisite defects on the periphery of the primary particles located on the surface of the secondary particle, which stabilizes the intrinsic nature of surface lattice. Meanwhile, thermally driven and inward diffusion of Mn during calcination, which acts as an oxygen carrier, ameliorates the local oxygen environment and suppresses interfacefusion intermediate phases (cation mixing) to refine the primary particles. The robust morphological integrity provided by refined primary particles prevents intergranular crack, confining interfacial parasitic reactions to the surface region of secondary particles protected by the lattice-coherent epitaxial surface. This universal approach optimally balances surface stabilization with charge transfer, significant enhancing capacity retention and rate capability for NMA cathode while opening new avenue for the next generation Co-free ultrahigh-Ni cathodes.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"31 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034082","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}
Thermal stability is a critical challenge limiting the practical deployment of thermoelectric materials in real-world energy conversion. This study presents a breakthrough by incorporating dense nanoscale twin boundaries into bismuth-telluride-based thermoelectrics, achieving concurrent improvements in thermoelectric efficiency, mechanical robustness, and operational longevity. The coherent twin interfaces, characterized by their crystallographic symmetry and minimal electron scattering, effectively reduce lattice thermal conductivity while preserving charge carrier mobility. Remarkably, the material maintains a high power factor and a low thermal conductivity even after extended thermal aging. Device-level testing confirms exceptional stability, with twin-engineered devices retaining >98% of their output power and conversion efficiency across repeated thermal cycles, alongside intact interfacial contacts and no observable microstructural degradation. These results highlight nanotwin boundary engineering as a robust microstructural design paradigm for developing high-performance, durable thermoelectric device applications.
{"title":"Nanotwin Engineering Enables Exceptional Thermal Stability in P-Type Bismuth Telluride Thermoelectrics","authors":"Chuandong Zhou, Jiaze Zhu, Shuxin Zhang, Zhen'ao Zhang, Zongwei Zhang, Jianfeng Cai, Qiang Zhang, Ruijie Li, Lianghan Fan, Jingtao Xu, Guoqiang Liu, Xiaojian Tan, Bo Liang, Jun Jiang","doi":"10.1039/d5ee06360d","DOIUrl":"https://doi.org/10.1039/d5ee06360d","url":null,"abstract":"Thermal stability is a critical challenge limiting the practical deployment of thermoelectric materials in real-world energy conversion. This study presents a breakthrough by incorporating dense nanoscale twin boundaries into bismuth-telluride-based thermoelectrics, achieving concurrent improvements in thermoelectric efficiency, mechanical robustness, and operational longevity. The coherent twin interfaces, characterized by their crystallographic symmetry and minimal electron scattering, effectively reduce lattice thermal conductivity while preserving charge carrier mobility. Remarkably, the material maintains a high power factor and a low thermal conductivity even after extended thermal aging. Device-level testing confirms exceptional stability, with twin-engineered devices retaining >98% of their output power and conversion efficiency across repeated thermal cycles, alongside intact interfacial contacts and no observable microstructural degradation. These results highlight nanotwin boundary engineering as a robust microstructural design paradigm for developing high-performance, durable thermoelectric device applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"7 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022031","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}
Quan Zong, Xuelian Liu, Keyi Chen, Qi-Long Zhang, Haoran Yuan, Shuang Zhou, Guoying Wei, Gongxun Bai, Anqiang Pan
Aqueous zinc‐ion batteries (ZIBs) are promising candidates for large‐scale energy storage owing to their high safety, low cost, and environmental friendliness. However, the practical application of ZIBs remains challenged by low energy density and energy efficiency owing to the rapid capacity fading and voltage decay, large voltage polarization, and sluggish reaction kinetics. In this work, we introduce a ligand-field engineering strategy that couples pre-intercalated ions interaction with octahedral defects to inhibit energy loss in layered hydrated vanadium pentoxide (V2O5·nH2O, VOH) cathodes. Comprehensive experimental analyses reveal that the introduction of pre-intercalated ions and oxygen vacancies induces [VO6] octahedral distortion and V-O bond elongation, thereby tailoring the ligand field and lowering the V 3d orbital energy level. This structure modulation effectively narrows the voltage hysteresis, stabilizes the voltage plateau and enhances the energy efficiency. In addition, this ligand-engineering strategy in enhancing energy efficiency can be extended to low-temperature conditions and other similar systems. As a result, the Ov-Zn-VOH cathode delivers a high discharge capacity (536 mAh g−1 at 0.1 A g−1) coupled with high energy efficiency (86%) and an energy efficiency retention of 94% after 3000 cycles at 4 A g−1.
水锌离子电池（zib）具有高安全性、低成本和环境友好性，是大规模储能的理想选择。然而，由于容量衰减快、电压衰减快、电压极化大、反应动力学缓慢等原因，ZIBs的实际应用仍然面临能量密度和能量效率低的挑战。在这项工作中，我们引入了一种配体场工程策略，将预插层离子与八面体缺陷耦合，以抑制层状水合五氧化钒（V2O5·nH2O， VOH）阴极的能量损失。综合实验分析表明，引入预插层离子和氧空位可诱导[VO6]八面体畸变和V- o键延伸，从而裁剪配体场并降低V- o三维轨道能级。这种结构调制有效地缩小了电压滞回，稳定了电压平台，提高了能效。此外，这种提高能源效率的配体工程策略可以扩展到低温条件和其他类似的系统。因此，Ov-Zn-VOH阴极在0.1 a g−1下具有高放电容量（536 mAh g−1），高能量效率（86%），在4 a g−1下循环3000次后能量效率保持在94%。
{"title":"Ligand-field regulation enables high energy-efficiency cathodes for aqueous zinc-ion batteries","authors":"Quan Zong, Xuelian Liu, Keyi Chen, Qi-Long Zhang, Haoran Yuan, Shuang Zhou, Guoying Wei, Gongxun Bai, Anqiang Pan","doi":"10.1039/d5ee07175e","DOIUrl":"https://doi.org/10.1039/d5ee07175e","url":null,"abstract":"Aqueous zinc‐ion batteries (ZIBs) are promising candidates for large‐scale energy storage owing to their high safety, low cost, and environmental friendliness. However, the practical application of ZIBs remains challenged by low energy density and energy efficiency owing to the rapid capacity fading and voltage decay, large voltage polarization, and sluggish reaction kinetics. In this work, we introduce a ligand-field engineering strategy that couples pre-intercalated ions interaction with octahedral defects to inhibit energy loss in layered hydrated vanadium pentoxide (V2O5·nH2O, VOH) cathodes. Comprehensive experimental analyses reveal that the introduction of pre-intercalated ions and oxygen vacancies induces [VO6] octahedral distortion and V-O bond elongation, thereby tailoring the ligand field and lowering the V 3d orbital energy level. This structure modulation effectively narrows the voltage hysteresis, stabilizes the voltage plateau and enhances the energy efficiency. In addition, this ligand-engineering strategy in enhancing energy efficiency can be extended to low-temperature conditions and other similar systems. As a result, the Ov-Zn-VOH cathode delivers a high discharge capacity (536 mAh g−1 at 0.1 A g−1) coupled with high energy efficiency (86%) and an energy efficiency retention of 94% after 3000 cycles at 4 A g−1.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"9 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022034","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}
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