Hsi Chen, Yung‐An Chen, Chen Chang, Frances M. Ross, Yimeng Huang, Ju Li
Disordered rocksalt cathodes (DRX) represent a compelling platform for cobalt‐ and nickel‐free high‐energy density lithium‐ion batteries. Yet their scalable synthesis remains challenging, especially for metastable DRX chemistries that have been predominantly developed via mechanochemical routes. A prominent example is polyanion‐integrated DRX (DRXPS) cathodes, which rank among the best DRX cathodes reported to date in terms of reversible energy density, but have thus far been synthesized only mechanochemically via low‐temperature ball milling. Here we demonstrate a coprecipitation–enabled solid‐state synthesis of a DRXPS cathode, Li 1.67 Mn 1.5 P 0.17 O 4 , translating a mechanochemical route into a scalable process that is compatible with established cathode manufacturing infrastructure. The workflow programs precursor chemistry via coprecipitation of Mn 2+ with HPO 42− and OH − , followed by a eutectic lithium‐salt‐assisted solid‐state reaction, enabling low‐thermal‐budget DRXPS formation (450°C, 30 min) in air. The reduced thermal budget suppresses particle coarsening and yields a mixed micro‐/nanoscale particle morphology, thereby eliminating the need for post‐synthesis particle pulverization. The resulting cathodes deliver 324 mAh g −1 (935 Wh kg −1 ), demonstrating that high‐energy density DRXPS can be realized within a manufacturing‐compatible workflow. This work establishes a direct pathway toward scalable production of metastable high‐energy density DRXPS cathodes and identifies precursor engineering as the key enabler.
无序岩盐阴极（DRX）为无钴和无镍高能量密度锂离子电池提供了一个令人信服的平台。然而，它们的可扩展合成仍然具有挑战性，特别是对于主要通过机械化学途径开发的亚稳态DRX化学物质。一个突出的例子是聚阴离子集成DRX （DRXPS）阴极，就可逆能量密度而言，它是迄今为止报道的最好的DRX阴极之一，但迄今为止只能通过低温球磨机械化学合成。在这里，我们展示了一种共沉淀法固态合成DRXPS阴极Li 1.67 Mn 1.5 P 0.17 o4，将机械化学路线转化为可扩展的工艺，与现有的阴极制造基础设施兼容。工作流程通过将Mn 2 +与HPO 2 -和OH -共沉淀，然后进行锂盐辅助的共晶固态反应，从而在空气中形成低热预算DRXPS（450°C， 30分钟），从而对前驱化学进行编程。减少的热收支抑制了颗粒的粗化，产生了混合的微/纳米级颗粒形态，从而消除了合成后颗粒粉碎的需要。所得到的阴极提供324 mAh g - 1 (935 Wh kg - 1)，表明高能量密度DRXPS可以在制造兼容的工作流程中实现。这项工作为大规模生产亚稳态高能量密度DRXPS阴极建立了一条直接途径，并确定了前体工程是关键的推动因素。
{"title":"Coprecipitation‐Enabled Scalable Synthesis of High‐Energy Density Polyanion‐Integrated Disordered Rocksalt Cathodes for Lithium‐Ion Batteries","authors":"Hsi Chen, Yung‐An Chen, Chen Chang, Frances M. Ross, Yimeng Huang, Ju Li","doi":"10.1002/aenm.71730","DOIUrl":"https://doi.org/10.1002/aenm.71730","url":null,"abstract":"Disordered rocksalt cathodes (DRX) represent a compelling platform for cobalt‐ and nickel‐free high‐energy density lithium‐ion batteries. Yet their scalable synthesis remains challenging, especially for metastable DRX chemistries that have been predominantly developed via mechanochemical routes. A prominent example is polyanion‐integrated DRX (DRXPS) cathodes, which rank among the best DRX cathodes reported to date in terms of reversible energy density, but have thus far been synthesized only mechanochemically via low‐temperature ball milling. Here we demonstrate a coprecipitation–enabled solid‐state synthesis of a DRXPS cathode, Li <jats:sub>1.67</jats:sub> Mn <jats:sub>1.5</jats:sub> P <jats:sub>0.17</jats:sub> O <jats:sub>4</jats:sub> , translating a mechanochemical route into a scalable process that is compatible with established cathode manufacturing infrastructure. The workflow programs precursor chemistry via coprecipitation of Mn <jats:sup>2</jats:sup> <jats:sup>+</jats:sup> with HPO <jats:sub>4</jats:sub> <jats:sup>2</jats:sup> <jats:sup>−</jats:sup> and OH <jats:sup>−</jats:sup> , followed by a eutectic lithium‐salt‐assisted solid‐state reaction, enabling low‐thermal‐budget DRXPS formation (450°C, 30 min) in air. The reduced thermal budget suppresses particle coarsening and yields a mixed micro‐/nanoscale particle morphology, thereby eliminating the need for post‐synthesis particle pulverization. The resulting cathodes deliver 324 mAh g <jats:sup>−1</jats:sup> (935 Wh kg <jats:sup>−1</jats:sup> ), demonstrating that high‐energy density DRXPS can be realized within a manufacturing‐compatible workflow. This work establishes a direct pathway toward scalable production of metastable high‐energy density DRXPS cathodes and identifies precursor engineering as the key enabler.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149298599","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}
Photoelectrochemical water oxidation is limited not simply by light absorption, but by inefficient hole routing and utilization at the semiconductor‐electrolyte interface, together with severe defect‐mediated recombination. Here, a self‐reconstructed crystallinity‐differentiated interface is developed to program hole utilization in photoanodes. A one‐step hydrothermal synthesis creates an interlocked architecture in which highly crystalline In 2 S 3 pyramids are coupled with a disordered mixed‐anion nanosheet domain, generating a spatially polarized reaction field for directed hole accumulation and transfer. This reconstructed interface lowers the work function, redistributes the local coordination environment around In sites, and induces a spatially heterogeneous photovoltage landscape that promotes interfacial charge separation. Mild Ar annealing further serves as a defect‐selective activation step, suppressing recombination‐active defects while preserving the beneficial interfacial polarization, thereby accelerating charge injection and oxygen evolution kinetics. The optimized photoanode reaches 8.74 mA cm −2 at 1.23 V RHE , establishing interlocked crystallinity‐differentiated architecture engineering combined with defect‐selective activation as an effective strategy for sulfide photoanodes.
光电化学水氧化不仅受到光吸收的限制，还受到半导体-电解质界面上低效的空穴布线和利用，以及严重的缺陷介导的复合的限制。在这里，开发了一个自重构的结晶度分化界面来规划光阳极的空穴利用。一步水热合成创造了一个互锁结构，其中高度结晶的in2s3金字塔与无序的混合阴离子纳米片畴耦合，产生一个空间极化的反应场，用于定向孔积累和转移。这种重构的界面降低了功函数，重新分配了In位点周围的局部协调环境，并诱导了空间异质性的光电压景观，促进了界面电荷分离。轻度Ar退火进一步作为缺陷选择性活化步骤，抑制复合活性缺陷，同时保留有益的界面极化，从而加速电荷注入和析氧动力学。优化后的光阳极在1.23 V RHE下达到8.74 mA cm−2，建立了结合缺陷选择性激活的互锁结晶度分化结构工程作为硫化物光阳极的有效策略。
{"title":"Directing Hole Utilization Through Self‐Reconstructed Crystallinity Differentiation for Photoelectrochemical Water Oxidation","authors":"Tianyun Liu, Linxing Meng, Dongniu Wang, Yuyang Kang, Yutao Xing, Xuefei Liu, Zhenhao He, Liang Li","doi":"10.1002/aenm.71781","DOIUrl":"https://doi.org/10.1002/aenm.71781","url":null,"abstract":"Photoelectrochemical water oxidation is limited not simply by light absorption, but by inefficient hole routing and utilization at the semiconductor‐electrolyte interface, together with severe defect‐mediated recombination. Here, a self‐reconstructed crystallinity‐differentiated interface is developed to program hole utilization in photoanodes. A one‐step hydrothermal synthesis creates an interlocked architecture in which highly crystalline In <jats:sub>2</jats:sub> S <jats:sub>3</jats:sub> pyramids are coupled with a disordered mixed‐anion nanosheet domain, generating a spatially polarized reaction field for directed hole accumulation and transfer. This reconstructed interface lowers the work function, redistributes the local coordination environment around In sites, and induces a spatially heterogeneous photovoltage landscape that promotes interfacial charge separation. Mild Ar annealing further serves as a defect‐selective activation step, suppressing recombination‐active defects while preserving the beneficial interfacial polarization, thereby accelerating charge injection and oxygen evolution kinetics. The optimized photoanode reaches 8.74 mA cm <jats:sup>−2</jats:sup> at 1.23 V <jats:sub>RHE</jats:sub> , establishing interlocked crystallinity‐differentiated architecture engineering combined with defect‐selective activation as an effective strategy for sulfide photoanodes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"111 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149298597","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}
Nan Sun, Binbin Xu, Gaosheng Huang, Yuehui Li, Karsten Bittkau, Eunseo Noh, Sercan Aslan, Andreas Lambertz, Sang Il Seok, Michael Saliba, Christoph J. Brabec, Thomas Kirchartz, Kaining Ding
Surface texturing in crystalline silicon solar cells imposes a fundamental trade‐off in perovskite‐silicon tandems: micrometer‐scale pyramids enable efficient light trapping but limit the conformal deposition of thin perovskite films with sub‐micrometer thickness, whereas reduced texture heights improve compatibility at the expense of optical performance and interfacial quality of the tandem device. Here, we address this challenge by combining precisely controlled submicron texturing with an ozone‐assisted chemical rounding treatment. The resulting silicon substrates feature smoothly rounded, symmetric submicron textures that suppress micro‐terrace formation and partial epitaxy at the amorphous silicon/crystalline silicon interface, while promoting more spatially uniform optoelectronic properties in the subsequently integrated top‐cell stack. The morphology‐engineered texture yields a monolithic perovskite–silicon tandem device with a power conversion efficiency of 33.25%, demonstrating that multiscale morphological control provides a powerful pathway to simultaneously improve the optical performance and interfacial quality of tandem solar cells.
{"title":"Chemical Rounding Suppresses Morphology‐Induced Interfacial Losses in Perovskite–Silicon Tandem Solar Cells","authors":"Nan Sun, Binbin Xu, Gaosheng Huang, Yuehui Li, Karsten Bittkau, Eunseo Noh, Sercan Aslan, Andreas Lambertz, Sang Il Seok, Michael Saliba, Christoph J. Brabec, Thomas Kirchartz, Kaining Ding","doi":"10.1002/aenm.71784","DOIUrl":"https://doi.org/10.1002/aenm.71784","url":null,"abstract":"Surface texturing in crystalline silicon solar cells imposes a fundamental trade‐off in perovskite‐silicon tandems: micrometer‐scale pyramids enable efficient light trapping but limit the conformal deposition of thin perovskite films with sub‐micrometer thickness, whereas reduced texture heights improve compatibility at the expense of optical performance and interfacial quality of the tandem device. Here, we address this challenge by combining precisely controlled submicron texturing with an ozone‐assisted chemical rounding treatment. The resulting silicon substrates feature smoothly rounded, symmetric submicron textures that suppress micro‐terrace formation and partial epitaxy at the amorphous silicon/crystalline silicon interface, while promoting more spatially uniform optoelectronic properties in the subsequently integrated top‐cell stack. The morphology‐engineered texture yields a monolithic perovskite–silicon tandem device with a power conversion efficiency of 33.25%, demonstrating that multiscale morphological control provides a powerful pathway to simultaneously improve the optical performance and interfacial quality of tandem solar cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"21 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149298598","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}
Junghye Lee, Kwang Min Kim, Seongbin Ga, Hyeonmyeong Oh, Jungki Ryu
The hydrogen economy is commonly organized around four separate tasks: production, storage, transport, and release. This Perspective redefines decoupled water electrolysis (DWE) as a framework in which these functions can be integrated within a single electrochemical redox loop. By using a proton‐coupled redox mediator to decouple hydrogen and oxygen evolution in time and space, DWE stores hydrogen equivalents in a charged mediator phase and releases H 2 electrochemically or catalytically at the point of use. This architecture shifts part of hydrogen logistics from pressure‐ or temperature‐intensive processes toward ambient‐condition electrochemical operation. DWE can therefore be viewed not merely as an alternative electrolyzer architecture, but as an integrated hydrogen‐carrier platform. Within this broader framework, this Perspective focuses primarily on solution‐phase proton‐coupled mediators because their charged inventories can function as transportable liquid‐phase carriers. Although current solution‐phase DWE mediators remain disadvantaged in gravimetric capacity relative to ammonia and liquid organic hydrogen carriers (LOHCs), their system‐level value lies in ambient‐condition storage, low‐temperature on‐site H 2 release, independent scaling of power (electrolyzer stack) and energy capacity (mediator inventory), and flexible coupling to intermittent renewable electricity. We therefore propose carrier‐relevant benchmarks including full‐system capacity, storage‐and‐release efficiency, mediator retention, gas quality, delivered cost, and closed‐loop logistics.
{"title":"Redefining Decoupled Water Electrolysis as an Integrated Hydrogen‐Carrier Platform","authors":"Junghye Lee, Kwang Min Kim, Seongbin Ga, Hyeonmyeong Oh, Jungki Ryu","doi":"10.1002/aenm.71763","DOIUrl":"https://doi.org/10.1002/aenm.71763","url":null,"abstract":"The hydrogen economy is commonly organized around four separate tasks: production, storage, transport, and release. This Perspective redefines decoupled water electrolysis (DWE) as a framework in which these functions can be integrated within a single electrochemical redox loop. By using a proton‐coupled redox mediator to decouple hydrogen and oxygen evolution in time and space, DWE stores hydrogen equivalents in a charged mediator phase and releases H <jats:sub>2</jats:sub> electrochemically or catalytically at the point of use. This architecture shifts part of hydrogen logistics from pressure‐ or temperature‐intensive processes toward ambient‐condition electrochemical operation. DWE can therefore be viewed not merely as an alternative electrolyzer architecture, but as an integrated hydrogen‐carrier platform. Within this broader framework, this Perspective focuses primarily on solution‐phase proton‐coupled mediators because their charged inventories can function as transportable liquid‐phase carriers. Although current solution‐phase DWE mediators remain disadvantaged in gravimetric capacity relative to ammonia and liquid organic hydrogen carriers (LOHCs), their system‐level value lies in ambient‐condition storage, low‐temperature on‐site H <jats:sub>2</jats:sub> release, independent scaling of power (electrolyzer stack) and energy capacity (mediator inventory), and flexible coupling to intermittent renewable electricity. We therefore propose carrier‐relevant benchmarks including full‐system capacity, storage‐and‐release efficiency, mediator retention, gas quality, delivered cost, and closed‐loop logistics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292691","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}
Zixuan Li, Katarzyna Sowa, Tomasz Kołodziej, Yi Yuan, Hewen Chen, Lijiang Song, Pawel Wróbel, Didier Wermeille, Paul Thompson, Paweł Korecki, Peter G. Bruce, Alex W. Robertson
Manganese dioxides are pervasive as cathode materials for aqueous zinc‐ion batteries; however, their energy storage mechanism has proven to be complex. Increasing evidence suggests that Mn dissolution contributes to cathode capacity via a reversible dissolution‐redeposition process, in addition to capacity from Zn 2+ /H + (de)intercalation. Understanding the role played by Mn 2+ in the electrolyte, particularly when introduced as an electrolyte additive, is important for diagnosing cathode degradation. Using operando X‐ray fluorescence (XRF) spectroscopy, we track Mn 2+ in operating cells to gain insights into the complexity of the MnO 2 cathode. While some suppression of cathode dissolution by the additive cannot be excluded, our measurements suggest that Mn 2+ electrolyte additives improve cycling performance by supplying extra redox‐active Mn during charge, rather than solely by suppressing Mn dissolution, thereby compensating for cathode degradation. Benefiting from operando XRF, we propose that a potential contributor to capacity fading is the incomplete dissolution of the MnO 2 cathode and incomplete redeposition of Mn 2+ from the electrolyte, and that this fading does not appear to be mitigated by using Mn 2+ additives. These findings underscore the necessity of directly tracking Mn 2+ evolution, and that improving reversibility requires addressing both the dissolution of MnO 2 and the redeposition of Mn 2+ .
{"title":"Diagnosing the Role of Mn Additives in Aqueous Zn/MnO 2 Batteries","authors":"Zixuan Li, Katarzyna Sowa, Tomasz Kołodziej, Yi Yuan, Hewen Chen, Lijiang Song, Pawel Wróbel, Didier Wermeille, Paul Thompson, Paweł Korecki, Peter G. Bruce, Alex W. Robertson","doi":"10.1002/aenm.71765","DOIUrl":"https://doi.org/10.1002/aenm.71765","url":null,"abstract":"Manganese dioxides are pervasive as cathode materials for aqueous zinc‐ion batteries; however, their energy storage mechanism has proven to be complex. Increasing evidence suggests that Mn dissolution contributes to cathode capacity via a reversible dissolution‐redeposition process, in addition to capacity from Zn <jats:sup>2+</jats:sup> /H <jats:sup>+</jats:sup> (de)intercalation. Understanding the role played by Mn <jats:sup>2+</jats:sup> in the electrolyte, particularly when introduced as an electrolyte additive, is important for diagnosing cathode degradation. Using operando X‐ray fluorescence (XRF) spectroscopy, we track Mn <jats:sup>2+</jats:sup> in operating cells to gain insights into the complexity of the MnO <jats:sub>2</jats:sub> cathode. While some suppression of cathode dissolution by the additive cannot be excluded, our measurements suggest that Mn <jats:sup>2+</jats:sup> electrolyte additives improve cycling performance by supplying extra redox‐active Mn during charge, rather than solely by suppressing Mn dissolution, thereby compensating for cathode degradation. Benefiting from operando XRF, we propose that a potential contributor to capacity fading is the incomplete dissolution of the MnO <jats:sub>2</jats:sub> cathode and incomplete redeposition of Mn <jats:sup>2+</jats:sup> from the electrolyte, and that this fading does not appear to be mitigated by using Mn <jats:sup>2+</jats:sup> additives. These findings underscore the necessity of directly tracking Mn <jats:sup>2+</jats:sup> evolution, and that improving reversibility requires addressing both the dissolution of MnO <jats:sub>2</jats:sub> and the redeposition of Mn <jats:sup>2+</jats:sup> .","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292623","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}
Epitaxial dielectric thin films have attracted considerable attention for better energy storage performance than bulks and polymers, yet their reported recoverable energy density ( Wrec ) commonly excludes the substrate, which limits its relevance to practical device‐level energy storage. Here, we develop a Si‐integrated BZT//S‐BZT multilayer capacitor to address this issue and simultaneously enhance polarization and breakdown strength ( Eb ). By directly integrating the oxide multilayer on Si‐based substrates, the contribution of the substrate to the effective device volume is substantially reduced, enabling a realistic energy density ( Wrec‐real ) of 105.51 J/cm 3 , exceeding that of the overwhelming majority of comparable systems. The BZT and S‐BZT sublayers exhibit small lattice mismatch but pronounced dielectric contrast, which induces strong interfacial polarization ( Pinter ) without introducing interfacial structural perturbation. Landau–Ginzburg–Devonshire theory and phase‐field simulations consistently verify the interface‐induced polarization enhancement and agree well with the experimental observations. To further improve E b , machine learning was employed to establish the relationship between the multilayer structural parameters and Eb and to identify the optimal starting‐layer thickness. Experimental results closely reproduce the predicted trend, leading to an optimized Big‐Mac‐ n architecture with a high Wrec of 131.21 J/cm 3 and an E b of 6.5 MV/cm. The multilayer also exhibits excellent fatigue, frequency, and temperature stability, together with ultrafast discharge capability. This work establishes a data‐driven interface‐engineering strategy for reliable, Si‐integrated dielectric energy‐storage capacitors.
{"title":"High‐Density Energy Storage in Si‐Integrated Dielectric Multilayers Through Interfacial Polarization and ML‐Guided Structural Optimization","authors":"Jun Yang, Hongyu Yang, Zixiong Sun","doi":"10.1002/aenm.71783","DOIUrl":"https://doi.org/10.1002/aenm.71783","url":null,"abstract":"Epitaxial dielectric thin films have attracted considerable attention for better energy storage performance than bulks and polymers, yet their reported recoverable energy density ( <jats:italic>W</jats:italic> <jats:sub>rec</jats:sub> ) commonly excludes the substrate, which limits its relevance to practical device‐level energy storage. Here, we develop a Si‐integrated BZT//S‐BZT multilayer capacitor to address this issue and simultaneously enhance polarization and breakdown strength ( <jats:italic>E</jats:italic> <jats:sub>b</jats:sub> ). By directly integrating the oxide multilayer on Si‐based substrates, the contribution of the substrate to the effective device volume is substantially reduced, enabling a realistic energy density ( <jats:italic>W</jats:italic> <jats:sub>rec‐real</jats:sub> ) of 105.51 J/cm <jats:sup>3</jats:sup> , exceeding that of the overwhelming majority of comparable systems. The BZT and S‐BZT sublayers exhibit small lattice mismatch but pronounced dielectric contrast, which induces strong interfacial polarization ( <jats:italic>P</jats:italic> <jats:sub>inter</jats:sub> ) without introducing interfacial structural perturbation. Landau–Ginzburg–Devonshire theory and phase‐field simulations consistently verify the interface‐induced polarization enhancement and agree well with the experimental observations. To further improve <jats:italic> E <jats:sub>b</jats:sub> </jats:italic> , machine learning was employed to establish the relationship between the multilayer structural parameters and <jats:italic>E</jats:italic> <jats:sub>b</jats:sub> and to identify the optimal starting‐layer thickness. Experimental results closely reproduce the predicted trend, leading to an optimized Big‐Mac‐ <jats:italic>n</jats:italic> architecture with a high <jats:italic>W</jats:italic> <jats:sub>rec</jats:sub> of 131.21 J/cm <jats:sup>3</jats:sup> and an <jats:italic> E <jats:sub>b</jats:sub> </jats:italic> of 6.5 MV/cm. The multilayer also exhibits excellent fatigue, frequency, and temperature stability, together with ultrafast discharge capability. This work establishes a data‐driven interface‐engineering strategy for reliable, Si‐integrated dielectric energy‐storage capacitors.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"8 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292502","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}
Jianqi Sun, Juliane Fiates, Kohei Shimokawa, Qingsong Weng, Heng Wang, Zhuangnan Li, Su Jin Heo, Hooman Abbasi, Minfei Fei, Tianhao Wu, Yaogang Li, Hongzhi Wang, James A Dawson, Michael De Volder
Lithium (Li) metal anodes (LMAs) hold great promise to increase the energy density of batteries. This is especially true when using an energy‐dense cathode such as Ni‐rich layered transition metal oxides, but unfortunately, these lead to accelerated capacity loss when combined with LMAs. Ni‐rich cathodes suffer from surface reduction, which can be accelerated in contact with certain electrolyte solvents. This in turn leads to transition metal dissolution and shuttling, which poisons the solid electrolyte interphase (SEI) and complicates the anode stabilization. Here, we propose nitrile primary solvent combined with ether co‐solvent, diluent and two borate salts to suppress parasitic reaction. A competition in the ion coordination between solvents surrounded by diluents is achieved. This leads to the anions being preferentially decomposed in the SEI and enhanced reversibility. Using high cathode areal capacity (4.0 mAh cm −2 ), thin LMAs (N/p = 2.5), lean electrolyte (3 g Ah −1 ), and high charging voltages (≥4.4 V), we achieve a capacity retention of 80% over 250 cycles. With moderately high loading cathode (3.4 mAh cm −2 ) but higher upper voltage (4.6 V), the cells retain 87.5% capacity retention over 430 cycles. Finally, we demonstrate Ah‐level anode‐free pouch cells with a 78.7% capacity retention over 100 cycles.
锂（Li）金属阳极（LMAs）在提高电池的能量密度方面具有很大的前景。当使用能量密集的阴极（如富镍层状过渡金属氧化物）时尤其如此，但不幸的是，当与lma结合时，这些阴极会加速容量损失。富镍阴极受到表面还原的影响，与某些电解质溶剂接触会加速表面还原。这反过来又导致过渡金属的溶解和穿梭，从而毒害固体电解质界面（SEI）并使阳极稳定复杂化。在此，我们提出了腈一级溶剂与乙醚共溶剂、稀释剂和两种硼酸盐结合来抑制寄生反应。被稀释剂包围的溶剂之间的离子配位发生竞争。这导致阴离子在SEI中被优先分解，增强了可逆性。采用高阴极面积容量（4.0 mAh cm−2），薄lma (N/p = 2.5)，稀薄电解质（3g Ah−1）和高充电电压（≥4.4 V），我们在250次循环中实现了80%的容量保持。在高负载阴极（3.4 mAh cm−2）和高电压（4.6 V）条件下，电池在430次循环中保持87.5%的容量。最后，我们展示了在100次循环中具有78.7%容量保持率的Ah级无阳极袋状电池。
{"title":"Locally Competitive Coordination Electrolyte for High‐Voltage Lithium‐Metal Batteries With Ni‐Rich Cathodes","authors":"Jianqi Sun, Juliane Fiates, Kohei Shimokawa, Qingsong Weng, Heng Wang, Zhuangnan Li, Su Jin Heo, Hooman Abbasi, Minfei Fei, Tianhao Wu, Yaogang Li, Hongzhi Wang, James A Dawson, Michael De Volder","doi":"10.1002/aenm.71779","DOIUrl":"https://doi.org/10.1002/aenm.71779","url":null,"abstract":"Lithium (Li) metal anodes (LMAs) hold great promise to increase the energy density of batteries. This is especially true when using an energy‐dense cathode such as Ni‐rich layered transition metal oxides, but unfortunately, these lead to accelerated capacity loss when combined with LMAs. Ni‐rich cathodes suffer from surface reduction, which can be accelerated in contact with certain electrolyte solvents. This in turn leads to transition metal dissolution and shuttling, which poisons the solid electrolyte interphase (SEI) and complicates the anode stabilization. Here, we propose nitrile primary solvent combined with ether co‐solvent, diluent and two borate salts to suppress parasitic reaction. A competition in the ion coordination between solvents surrounded by diluents is achieved. This leads to the anions being preferentially decomposed in the SEI and enhanced reversibility. Using high cathode areal capacity (4.0 mAh cm <jats:sup>−</jats:sup> <jats:sup>2</jats:sup> ), thin LMAs (N/p = 2.5), lean electrolyte (3 g Ah <jats:sup>−</jats:sup> <jats:sup>1</jats:sup> ), and high charging voltages (≥4.4 V), we achieve a capacity retention of 80% over 250 cycles. With moderately high loading cathode (3.4 mAh cm <jats:sup>−</jats:sup> <jats:sup>2</jats:sup> ) but higher upper voltage (4.6 V), the cells retain 87.5% capacity retention over 430 cycles. Finally, we demonstrate Ah‐level anode‐free pouch cells with a 78.7% capacity retention over 100 cycles.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"24 1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292617","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}
All‐solid‐state lithium batteries (ASSLBs) combining halide solid electrolytes (HSEs) with high‐nickel layered oxide cathodes offer great promise for high energy density, yet they suffer from severe interfacial issues such as oxidative decomposition, mechanical degradation, and chemical incompatibility with sulfide electrolytes. Herein, we report a Lewis‐acid‐induced surface‐softening strategy that constructs a nanoscale adaptive flexible interphase (AFI) via in situ polymerization of acrylonitrile (AN) on a representative halide electrolyte, Li 3 InCl 6 (LIC). The resulting AFI layer concurrently provides ionic conductivity, excellent oxidation stability (>4.8 V), and favorable viscoelasticity, thereby synergistically enhancing the electrochemical, chemical, and mechanical stability of the interface without compromising bulk ion transport. When paired with a single‐crystal ultrahigh‑nickel cathode LiNi 0.94 Co 0.05 Mn 0.01 O 2 (Ni94), the surface‑softened LIC (S‑LIC) enables ASSLBs delivering specific capacities of 223.8 and 209.5 mAh g −1 at 2 C and 4 C, respectively, retaining over 85% of the initial capacity after 2000 cycles at 2 C, and operate stably for more than 9000 cycles at 10 C. Even under an ultrahigh cutoff voltage of 4.8 V, a capacity retention of 81% is achieved after 800 cycles at 2 C. This work provides a broadly applicable and efficient interfacial engineering route for high‑voltage halide‑based ASSLBs.
全固态锂电池（asslb）结合了卤化物固体电解质（HSEs）和高镍层状氧化物阴极，为高能量密度提供了巨大的希望，但它们存在严重的界面问题，如氧化分解、机械降解和与硫化物电解质的化学不相容。在此，我们报道了一种Lewis酸诱导的表面软化策略，该策略通过丙烯腈（AN）在具有代表性的卤化物电解质li3incl6 （LIC）上的原位聚合，构建了纳米级自适应柔性界面（AFI）。由此产生的AFI层同时具有离子导电性、优异的氧化稳定性（>4.8 V）和良好的粘弹性，从而协同增强了界面的电化学、化学和机械稳定性，而不影响大块离子的传输。当与单晶超高镍阴极LiNi 0.94 Co 0.05 Mn 0.01 O 2 （Ni94）配对时，表面软化LIC （S - LIC）使asslb在2℃和4℃下分别提供223.8和209.5 mAh g - 1的比容量，在2℃下循环2000次后保持85%以上的初始容量，在10℃下稳定运行超过9000次，即使在4.8 V的超高截止电压下。在2℃下循环800次后，容量保持率达到81%。这项工作为高压卤化物asslb提供了广泛适用和高效的界面工程路线。
{"title":"Constructing an Adaptive Flexible Interphase on Halide Electrolytes by Lewis‐Acid‐Induced Polymerization for High‐Voltage All‐Solid‐State Lithium Batteries","authors":"Guo Tang, Yicheng Deng, Gengzhong Lin, Benchi Li, Kean Chen, Hui Li, Jiangfeng Qian, Yongjin Fang, Yuliang Cao, Xinping Ai","doi":"10.1002/aenm.71780","DOIUrl":"https://doi.org/10.1002/aenm.71780","url":null,"abstract":"All‐solid‐state lithium batteries (ASSLBs) combining halide solid electrolytes (HSEs) with high‐nickel layered oxide cathodes offer great promise for high energy density, yet they suffer from severe interfacial issues such as oxidative decomposition, mechanical degradation, and chemical incompatibility with sulfide electrolytes. Herein, we report a Lewis‐acid‐induced surface‐softening strategy that constructs a nanoscale adaptive flexible interphase (AFI) via in situ polymerization of acrylonitrile (AN) on a representative halide electrolyte, Li <jats:sub>3</jats:sub> InCl <jats:sub>6</jats:sub> (LIC). The resulting AFI layer concurrently provides ionic conductivity, excellent oxidation stability (>4.8 V), and favorable viscoelasticity, thereby synergistically enhancing the electrochemical, chemical, and mechanical stability of the interface without compromising bulk ion transport. When paired with a single‐crystal ultrahigh‑nickel cathode LiNi <jats:sub>0.94</jats:sub> Co <jats:sub>0.05</jats:sub> Mn <jats:sub>0.01</jats:sub> O <jats:sub>2</jats:sub> (Ni94), the surface‑softened LIC (S‑LIC) enables ASSLBs delivering specific capacities of 223.8 and 209.5 mAh g <jats:sup>−1</jats:sup> at 2 C and 4 C, respectively, retaining over 85% of the initial capacity after 2000 cycles at 2 C, and operate stably for more than 9000 cycles at 10 C. Even under an ultrahigh cutoff voltage of 4.8 V, a capacity retention of 81% is achieved after 800 cycles at 2 C. This work provides a broadly applicable and efficient interfacial engineering route for high‑voltage halide‑based ASSLBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292501","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}
Heng Huang, Yang Li, Xuekun Lu, Xinyu Liu, Yubai Li, Huanyue Zhang, Zhifu Zhou, Wei‐Tao Wu, Lei Wei, Chengzhi Hu, Linsong Gao, Yongchen Song
The fast‐charging capability of phase‐separating graphite electrodes is largely constrained by heterogeneous reaction kinetics and sluggish mass transport at both the particle and electrode scales, which increase the risk of parasitic lithium plating and associated safety concerns. A deeper mechanistic understanding of the interplay among phase‐separation dynamics, electrode microstructure, and lithium‐plating propensity is therefore essential for guiding the rational design of advanced electrode architectures and fast‐charging protocols. Here, we combine operando optical microscopy with three‐dimensional microstructure‐resolved phase‐field modeling to resolve the interplay between phase separation and lithium plating. Microscopy captures stages evolution, phase mode transitions and structural dynamics across the particle population and at the single‐particle level, which is driven by the slow interfacial reactions. Non‐equilibrium phase‐field simulations elucidate the kinetic control mechanisms governing phase transitions as the current varies. Importantly, a new mechanism of lithium plating associated with interfacial ohmic resistance is identified. Based on these insights, we evaluate particle‐size‐distribution design and use thermal activation as a mechanistic probe to resolve how temperature alters phase‐separation pathways and lithium‐plating behavior. These results may serve as a foundation for improving the physical understanding and driving optimization of fast charging protocols for lithium‐ion batteries.
{"title":"Operando Mapping of Population Phase Separation and Lithium‐Plating Dynamics in Graphite Electrode Using Optical Microscopy and Microstructure Modeling","authors":"Heng Huang, Yang Li, Xuekun Lu, Xinyu Liu, Yubai Li, Huanyue Zhang, Zhifu Zhou, Wei‐Tao Wu, Lei Wei, Chengzhi Hu, Linsong Gao, Yongchen Song","doi":"10.1002/aenm.71762","DOIUrl":"https://doi.org/10.1002/aenm.71762","url":null,"abstract":"The fast‐charging capability of phase‐separating graphite electrodes is largely constrained by heterogeneous reaction kinetics and sluggish mass transport at both the particle and electrode scales, which increase the risk of parasitic lithium plating and associated safety concerns. A deeper mechanistic understanding of the interplay among phase‐separation dynamics, electrode microstructure, and lithium‐plating propensity is therefore essential for guiding the rational design of advanced electrode architectures and fast‐charging protocols. Here, we combine operando optical microscopy with three‐dimensional microstructure‐resolved phase‐field modeling to resolve the interplay between phase separation and lithium plating. Microscopy captures stages evolution, phase mode transitions and structural dynamics across the particle population and at the single‐particle level, which is driven by the slow interfacial reactions. Non‐equilibrium phase‐field simulations elucidate the kinetic control mechanisms governing phase transitions as the current varies. Importantly, a new mechanism of lithium plating associated with interfacial ohmic resistance is identified. Based on these insights, we evaluate particle‐size‐distribution design and use thermal activation as a mechanistic probe to resolve how temperature alters phase‐separation pathways and lithium‐plating behavior. These results may serve as a foundation for improving the physical understanding and driving optimization of fast charging protocols for lithium‐ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"120 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149292619","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}
Biomass‐based fiber materials, including cellulose, chitosan, bacterial cellulose, and their derivatives, have emerged as a distinctive class of structural and functional scaffolds, effectively bridging renewable materials chemistry with advanced energy storage technologies. This review systematically elucidates their hierarchical structural characteristics, classifications, and the intrinsic structural‐function‐application relationships that underpin their versatility. Furthermore, the critical roles of these materials as key components‐including solid‐state/liquid electrolytes, separators, electrodes, and binders‐in various metal battery systems, particularly lithium‐ and zinc‐based batteries, are comprehensively summarized. The discussion further highlights how the rational architectural design of biomass‐derived fibrous materials can significantly enhance ionic conductivity, interfacial stability, and mechanical integrity. By improving these fundamental properties, such materials provide effective strategies for addressing major challenges, including dendrite formation and cycling instability. Finally, the current challenges and future research perspectives are discussed, with particular emphasis on precise molecular‐level design, scalable fabrication technologies, and standardized evaluation protocols, all of which are essential for advancing the development of next‐generation green and sustainable energy storage devices.
{"title":"Sustainable Biomass‐Based Fiber Materials as Structural and Functional Scaffolds for Advanced Metal Batteries","authors":"Yifei Yan, Ziqing Ruan, Shukai Wu, Leixin Yang, Hongyao Wang, Nuo Xu, Jingwen Gao, Long Jiao, Yaping Kong, Yun Zheng, Jiujun Zhang, Bowen Cheng","doi":"10.1002/aenm.71747","DOIUrl":"https://doi.org/10.1002/aenm.71747","url":null,"abstract":"Biomass‐based fiber materials, including cellulose, chitosan, bacterial cellulose, and their derivatives, have emerged as a distinctive class of structural and functional scaffolds, effectively bridging renewable materials chemistry with advanced energy storage technologies. This review systematically elucidates their hierarchical structural characteristics, classifications, and the intrinsic structural‐function‐application relationships that underpin their versatility. Furthermore, the critical roles of these materials as key components‐including solid‐state/liquid electrolytes, separators, electrodes, and binders‐in various metal battery systems, particularly lithium‐ and zinc‐based batteries, are comprehensively summarized. The discussion further highlights how the rational architectural design of biomass‐derived fibrous materials can significantly enhance ionic conductivity, interfacial stability, and mechanical integrity. By improving these fundamental properties, such materials provide effective strategies for addressing major challenges, including dendrite formation and cycling instability. Finally, the current challenges and future research perspectives are discussed, with particular emphasis on precise molecular‐level design, scalable fabrication technologies, and standardized evaluation protocols, all of which are essential for advancing the development of next‐generation green and sustainable energy storage devices.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149274716","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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