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Mn[B(HFIP)4]2: A Weakly Coordinating Electrolyte for Mn Metal Batteries Mn[B(HFIP)4]2:锰金属电池弱配位电解质
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-08 DOI: 10.1021/acsenergylett.6c02094
Jian Zhang, Fang Chen, Bowen Liu, Liang Chen, Gang Wang
{"title":"Mn[B(HFIP)4]2: A Weakly Coordinating Electrolyte for Mn Metal Batteries","authors":"Jian Zhang,&nbsp;Fang Chen,&nbsp;Bowen Liu,&nbsp;Liang Chen,&nbsp;Gang Wang","doi":"10.1021/acsenergylett.6c02094","DOIUrl":"10.1021/acsenergylett.6c02094","url":null,"abstract":"<p>Mn metal batteries (MnMBs) are promising for stationary applications owing to the low cost and low working potential of Mn anodes. However, developing electrolytes that combine high ionic conductivity with low-overpotential Mn plating/stripping remains challenging because of the trade-off between salt dissociation and desolvation. Herein, we propose a weakly coordinating electrolyte, Mn[B(HFIP)<sub>4</sub>]<sub>2</sub> (HFIP: hexafluoroisopropyl), for advanced MnMBs. The [B(HFIP)<sub>4</sub>]<sup>–</sup> anion, featuring full electron delocalization and steric hindrance, promotes complete salt dissociation in low-dielectric-constant ethers, yielding a pure ether-coordinated Mn<sup>2+</sup> electrolyte with high ionic conductivity (4.7–8.5 mS/cm at 20 °C) and a wide electrochemical window (&gt;3 V). Weak ether-Mn<sup>2+</sup> coordination facilitates desolvation, affording a record-low Mn plating/stripping overpotential (&lt;100 mV at 0.5 mA/cm<sup>2</sup>) and dendrite-free 3D growth. Coupling Mn anodes with polytriphenylamine or activated carbon cathodes enables quick-charge full cells, demonstrating the potential of anion engineering for high-performance multivalent metal batteries.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6776–6782"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148908742","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}
引用次数: 0
Nonmonotonic Li-Content Evolution and Size-Dependent Lithium Accessibility in Degraded High-Nickel Cathodes 降解高镍阴极中锂含量的非单调演化和尺寸相关的锂可及性
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-08 DOI: 10.1021/acsenergylett.6c01660
Sungjae Seo, Sugeun Jo, Hwiho Kim, Juwon Kim, Munsoo Song, Chihyun Nam, Sung Pil Woo, Jongwoo Lim
{"title":"Nonmonotonic Li-Content Evolution and Size-Dependent Lithium Accessibility in Degraded High-Nickel Cathodes","authors":"Sungjae Seo,&nbsp;Sugeun Jo,&nbsp;Hwiho Kim,&nbsp;Juwon Kim,&nbsp;Munsoo Song,&nbsp;Chihyun Nam,&nbsp;Sung Pil Woo,&nbsp;Jongwoo Lim","doi":"10.1021/acsenergylett.6c01660","DOIUrl":"10.1021/acsenergylett.6c01660","url":null,"abstract":"<p>Understanding how degradation reshapes lithium (de)insertion pathways in high-nickel cathodes is crucial for extending battery lifetime. Here, we integrate operando synchrotron X-ray diffraction (sXRD) with electrode-level transmission X-ray microscopy (TXM) to quantitatively resolve how degradation redistributes lithium accessibility in Ni-rich NCA cathodes. Using a 26-state deconvolution framework, we show that degraded electrodes exhibit nonmonotonic Li-content population evolution: delithiation kinetics are initially suppressed, transiently synchronized, and ultimately diverge, leaving ∼7% discharge-like states and ∼13% intermediate Li-content states at the end of charge. Spatially resolved TXM reveals that this divergence originates from size-dependent accessibility constraints—large particles develop persistent intra-particle state-of-charge gradients, while small particles exhibit pronounced inter-particle disparity. This work establishes a quantitative framework linking bulk Li-content population dynamics to particle-level degradation mechanisms in high-nickel cathodes.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6537–6547"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148908743","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}
引用次数: 0
Stabilizing Grain Boundaries by Flexible Bidirectional Multisite Hydrazide Cations toward High-Performance Inverted Perovskite Solar Cells 柔性双向多位点肼离子稳定晶界用于高性能倒钙钛矿太阳能电池
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-03 DOI: 10.1021/acsenergylett.6c01861
Linlin Lu, Zuolin Zhang, Dongmei He, Meirong Fu, Xuxia Shai, Yue Yu, Xinxing Liu, Xingyu Gao, Jiajia Zhang, Cong Chen, Jianhong Yi, Jiangzhao Chen
{"title":"Stabilizing Grain Boundaries by Flexible Bidirectional Multisite Hydrazide Cations toward High-Performance Inverted Perovskite Solar Cells","authors":"Linlin Lu,&nbsp;Zuolin Zhang,&nbsp;Dongmei He,&nbsp;Meirong Fu,&nbsp;Xuxia Shai,&nbsp;Yue Yu,&nbsp;Xinxing Liu,&nbsp;Xingyu Gao,&nbsp;Jiajia Zhang,&nbsp;Cong Chen,&nbsp;Jianhong Yi,&nbsp;Jiangzhao Chen","doi":"10.1021/acsenergylett.6c01861","DOIUrl":"10.1021/acsenergylett.6c01861","url":null,"abstract":"<p>The grain boundary instability induced by defects and tensible strain impedes the realization of high-performance inverted perovskite solar cells (PSCs). Here, we propose a flexible bidirectional multisite additive strategy to stabilize perovskite. (6-(2,5-Dioxo-2,5-dihydro-1H-pyrror-1-yl) hexanehydrazide hydrochloride (PHHCl) with a hydrazide cation, three carbonyl groups, and a flexible alkyl chain is leveraged to manipulate the GBs of perovskite. The multiple functional groups in PHH<sup>+</sup> synergistically participate in passivating various charged defects via rich chemical bonding modes. The bidirectional distribution of functional groups and molecular flexibility can not only enhance the defect passivation capability of PHH<sup>+</sup> but also realize chemical bridging between neighboring perovskite grains. The PHHCl-modulated 1.55 eV inverted PSC accomplishes a certified power conversion efficiency (PCE) of 27.0%, accompanied by exceptional operational stability with a <em>T</em><sub>90</sub> lifetime of 1084 h under continuous maximum power point tracking. Moreover, the PHHCl-modified 1.78 eV and 1.68 eV PSCs yield PCEs of 20.3% and 23.5%, respectively.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6618–6628"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148885529","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}
引用次数: 0
Regulating Asynchronous Crystallization via Additive Coordination Enables Efficient Perovskite/Silicon Tandems 通过添加剂配位调节异步结晶实现高效的钙钛矿/硅串联
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-07 DOI: 10.1021/acsenergylett.6c02301
Taomiao Wang, Fei Wang, Shuangbiao Xia, Yutao Wang, Yumeng Shi, Haoran Lin, Yonghua Chen, Mingjian Yuan, Liping Zhang, Haizhe Zhong, Hanlin Hu
{"title":"Regulating Asynchronous Crystallization via Additive Coordination Enables Efficient Perovskite/Silicon Tandems","authors":"Taomiao Wang,&nbsp;Fei Wang,&nbsp;Shuangbiao Xia,&nbsp;Yutao Wang,&nbsp;Yumeng Shi,&nbsp;Haoran Lin,&nbsp;Yonghua Chen,&nbsp;Mingjian Yuan,&nbsp;Liping Zhang,&nbsp;Haizhe Zhong,&nbsp;Hanlin Hu","doi":"10.1021/acsenergylett.6c02301","DOIUrl":"10.1021/acsenergylett.6c02301","url":null,"abstract":"<p>Wide-bandgap perovskites are essential for high-efficiency perovskite/silicon tandem solar cells but are limited by halide segregation and a narrow crystallization temperature window. Although temperature is known to influence perovskite film formation, its role in driving asynchronous crystallization between I-rich and Br-rich domains—and thus the extent of phase segregation—remains insufficiently understood. Here, we reveal that substrate temperature critically regulates these asynchronous crystallization pathways and propose an additive-engineering strategy to overcome this bottleneck. By introducing 2-mercapto-4-(trifluoromethyl) pyrimidine (2-MTP), the strong PbX<sub>2</sub> coordination regulates DMSO–PbX<sub>2</sub> intermediates, substantially broadening the processing temperature window. This controlled coordination modulates precursor conversion kinetics, mitigates asynchronous halide-rich domains crystallization, and effectively suppresses phase segregation in wide-bandgap perovskite films. As a result, 2-MTP-modified wide-bandgap devices achieve PCEs of 23.79% (1.67 eV; certified 23.02%) and 19.81% (1.84 eV). When implemented in perovskite/silicon tandem architectures, additive-regulated crystallization delivers 32.48% PCE (certified 31.60%) and markedly improved operational stability.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6909–6918"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973160","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}
引用次数: 0
Phosphoric Acid Cross-linking Regulates Closed Pores for Scalable Hard Carbon Anodes 磷酸交联调节可扩展硬碳阳极的封闭孔
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-26 DOI: 10.1021/acsenergylett.6c01963
Peng Shi, Xiaobing Zhao, Qingshi Meng, Zhenyu Guo, Xinlun Song, Ying Xiong, Xingguo Qi, Fei Xie, Junmei Zhao, Yong-Sheng Hu
{"title":"Phosphoric Acid Cross-linking Regulates Closed Pores for Scalable Hard Carbon Anodes","authors":"Peng Shi,&nbsp;Xiaobing Zhao,&nbsp;Qingshi Meng,&nbsp;Zhenyu Guo,&nbsp;Xinlun Song,&nbsp;Ying Xiong,&nbsp;Xingguo Qi,&nbsp;Fei Xie,&nbsp;Junmei Zhao,&nbsp;Yong-Sheng Hu","doi":"10.1021/acsenergylett.6c01963","DOIUrl":"10.1021/acsenergylett.6c01963","url":null,"abstract":"<p>The low-voltage capacity of hard carbon anodes, governed by closed-pore structures, directly determines the energy density of Na-ion batteries (NIBs), yet rational regulation of closed pores remains challenging. Herein, we report a phosphoric acid-induced cross-linking strategy to precisely tailor the closed pores of starch-derived hard carbon. H<sub>3</sub>PO<sub>4</sub> promotes cross-linking with starch at low temperatures (150−400 °C), enhancing carbon conversion, while its removal by washing generates micropores through a templating effect that evolve into closed pores after high-temperature carbonization. Consequently, the carbon yield increases from 14.0% to 31.7%, and the resulting hard carbon delivers a reversible capacity of 395.8 mAh g<sup>−1</sup> with an initial Coulombic efficiency of 89.4%. Additionally, the 3.5 Ah-level 26700 cylindrical cell based on the resulting anode demonstrates a high capacity retention of 96.5% after 500 cycles at the 1 C rate. This work provides a scalable and cost-effective pathway toward high-performance hard carbon anodes for practical NIB applications.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6727–6736"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049809","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}
引用次数: 0
Molecular Topological Anchoring Enables Thermodynamic–Kinetic Synergy in Hard-Carbon Anodes 分子拓扑锚定实现硬碳阳极的热力学-动力学协同作用
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-23 DOI: 10.1021/acsenergylett.6c02316
Zhiyong Xiong, Yi Zhang, Yiran Zhu, Xinrui Yang, Xi Peng, Zheng Yi, Yuansen Xie, Yuhao Lu, Maowen Xu, Yuruo Qi
{"title":"Molecular Topological Anchoring Enables Thermodynamic–Kinetic Synergy in Hard-Carbon Anodes","authors":"Zhiyong Xiong,&nbsp;Yi Zhang,&nbsp;Yiran Zhu,&nbsp;Xinrui Yang,&nbsp;Xi Peng,&nbsp;Zheng Yi,&nbsp;Yuansen Xie,&nbsp;Yuhao Lu,&nbsp;Maowen Xu,&nbsp;Yuruo Qi","doi":"10.1021/acsenergylett.6c02316","DOIUrl":"10.1021/acsenergylett.6c02316","url":null,"abstract":"<p>The practical deployment of hard carbon anodes in sodium-ion batteries is severely constrained by inferior sodium insertion thermodynamics and sluggish ion diffusion kinetics. We report a molecular topological anchoring strategy that simultaneously optimizes both aspects by cross-linking sucrose and zinc gluconate. The furan ring of sucrose acts as topological anchors, stabilizing Zn<sup>2+</sup> in the atomically dispersed form via C–Zn–O bonds, unlike conventional ZnO templating. This chemistry-driven pathway obviates hydrothermal pretreatment, precalcination and acid-washing, retarding graphitization and promoting expanded interlayers, high defect density, abundant closed pores, and redox-active oxygen groups. These features simultaneously enhance capacity through favorable sodium storage sites and accelerate kinetics via expanded interlayers and low-barrier hopping pathways. The optimized anode delivers 375.9 mA h g<sup>–1</sup> with 91.2% initial Coulombic efficiency, outstanding rate capability, and 91% capacity retention over 3000 cycles. This work demonstrates molecular topological engineering as an effective strategy to tune both thermodynamics and kinetics of carbon materials.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6928–6939"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049852","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}
引用次数: 0
Substrate-Enhanced Atomic Layer Deposition of Lithium Niobate on NMC Cathodes for Sulfide-Based All-Solid-State Batteries 硫化基全固态电池NMC阴极上衬底增强铌酸锂原子层沉积研究
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-28 DOI: 10.1021/acsenergylett.6c01988
Jaka Šivavec, Léo Lapeyre, Daniele Casari, Mariia Svyrydenko, Matthias Klimpel, Roland Widmer, Patrice Raynaud, Johann Michler, Ivo Utke, Kostiantyn V. Kravchyk, Maksym V. Kovalenko
{"title":"Substrate-Enhanced Atomic Layer Deposition of Lithium Niobate on NMC Cathodes for Sulfide-Based All-Solid-State Batteries","authors":"Jaka Šivavec,&nbsp;Léo Lapeyre,&nbsp;Daniele Casari,&nbsp;Mariia Svyrydenko,&nbsp;Matthias Klimpel,&nbsp;Roland Widmer,&nbsp;Patrice Raynaud,&nbsp;Johann Michler,&nbsp;Ivo Utke,&nbsp;Kostiantyn V. Kravchyk,&nbsp;Maksym V. Kovalenko","doi":"10.1021/acsenergylett.6c01988","DOIUrl":"10.1021/acsenergylett.6c01988","url":null,"abstract":"<p>Maintaining a stable interface between sulfide solid-state electrolytes and layered oxide cathodes remains a major challenge limiting the performance of all-solid-state batteries. Atomic layer deposition (ALD) of lithium niobate (LNO) on layered oxide cathodes is widely used to stabilize these interfaces, yet the early-stage growth of LNO remains poorly understood and strongly influenced by precursor chemistry. Here, we demonstrate substrate-enhanced ALD growth of LNO on single-crystal LiNi<sub>0.82</sub>Mn<sub>0.07</sub>Co<sub>0.11</sub>O<sub>2</sub> (NMC) achieved using commercial lithium–niobium precursor chemistry, enabling complete surface encapsulation with conformal LNO coatings thinner than 8 nm. The resulting ultrathin LNO coatings increase the discharge capacity of Li<sub>6</sub>PS<sub>5</sub>Cl-NMC all-solid-state batteries by up to 20% while maintaining good rate capability. The improved electrochemical performance is attributed to the suppressed electrochemical decomposition of the Li<sub>6</sub>PS<sub>5</sub>Cl solid-state electrolyte during cycling, as evidenced by X-ray photoelectron spectroscopy, highlighting the importance of controlling the early-stage ALD growth of LNO.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6737–6744"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090808","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}
引用次数: 0
Defect-Targeted Passivation Enabling Capacity Compensation of Hard Carbon Anodes for Sodium-Ion Batteries 钠离子电池硬碳阳极缺陷钝化实现容量补偿
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-15 DOI: 10.1021/acsenergylett.6c01903
Hang Li, Yutian Yang, Jiajun Wu, Jinghan Meng, Weihang Li, Ziyi Zhu, Shuang Zhou, Anqiang Pan
{"title":"Defect-Targeted Passivation Enabling Capacity Compensation of Hard Carbon Anodes for Sodium-Ion Batteries","authors":"Hang Li,&nbsp;Yutian Yang,&nbsp;Jiajun Wu,&nbsp;Jinghan Meng,&nbsp;Weihang Li,&nbsp;Ziyi Zhu,&nbsp;Shuang Zhou,&nbsp;Anqiang Pan","doi":"10.1021/acsenergylett.6c01903","DOIUrl":"10.1021/acsenergylett.6c01903","url":null,"abstract":"<p>Hard carbon is an anode material for sodium-ion batteries, yet its performance is hindered by rapid capacity decay and insufficient rate capability. The challenges arise from uncontrolled defects, pore distribution, and interlayer spacing within the carbon framework. Herein, a defect-targeted passivation strategy is originally proposed that compensates the capacity of hard carbon anodes through precise control of defect types and distribution. Specifically, selective passivation of reactive edge defects suppresses parasitic reactions and irreversible Na<sup>+</sup> consumption, while topological and compound defects provide reversible Na<sup>+</sup> storage to boost diffusion kinetics. Benefiting from this strategy, the optimized hard carbon anodes deliver an operational temperature range (–50 to 60 °C), a reversible capacity of 405.7 mAh g<sup>–1</sup>, an initial Coulombic efficiency of 90.50%, a stabilized rate capability (up to 10 A g<sup>–1</sup>), and cycling stability. This work establishes a directional defect-engineering for concurrently boosting the rate capability and stability of hard carbon anodes.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6657–6668"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148973919","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}
引用次数: 0
Configurational-Entropy-Engineered Prussian Blue Analogue Cathodes for Low-Temperature Semi-solid-state H2 Batteries 低温半固态H2电池的配置熵工程普鲁士蓝模拟阴极
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-18 DOI: 10.1021/acsenergylett.6c01803
Xiuquan Chen, Yuhua Zhao, Simin Hong, Xiaodong Rang, Xiang Cui, Kostya S. Novoselov, Yajing Liu
{"title":"Configurational-Entropy-Engineered Prussian Blue Analogue Cathodes for Low-Temperature Semi-solid-state H2 Batteries","authors":"Xiuquan Chen,&nbsp;Yuhua Zhao,&nbsp;Simin Hong,&nbsp;Xiaodong Rang,&nbsp;Xiang Cui,&nbsp;Kostya S. Novoselov,&nbsp;Yajing Liu","doi":"10.1021/acsenergylett.6c01803","DOIUrl":"10.1021/acsenergylett.6c01803","url":null,"abstract":"<p>Low-temperature proton transport kinetics remains a key limitation for rechargeable H<sub>2</sub> batteries. Herein, we report a configurational-entropy-engineered K<sub>1.36</sub>Mn<sub>0.6</sub>Fe<sub>0.1</sub>Co<sub>0.1</sub>Ni<sub>0.1</sub>Cu<sub>0.1</sub>[Fe(CN)<sub>6</sub>]<sub>0.61</sub>·□<sub>0.39</sub>·1.2H<sub>2</sub>O (CEM<sub>0.6</sub>-PBA) cathode for semi-solid-state H<sub>2</sub> batteries. Density functional theory calculations reveal that configurational entropy tailors the electronic structure, optimizes proton adsorption energetics, and lowers the proton migration barrier, thereby improving both the thermodynamics and kinetics of proton storage. In addition, an interconnected hydrogen-bonding network facilitates rapid proton transport under subzero conditions. As a result, the full cell delivers 155.9 mA h g<sup>–</sup><sup>1</sup> and 125.2 W h kg<sup>–</sup><sup>1</sup>, with 71.9% capacity retention after 10,000 cycles. Notably, it exhibits outstanding low-temperature performance, delivering 157.9, 128.3, and 80.0 mA h g<sup>–1</sup> at –10, –30, and –40 °C, respectively, operating down to –60 °C, and retaining 85.7 mA h g<sup>–</sup><sup>1</sup> after 2900 cycles at 0.3 A g<sup>–</sup><sup>1</sup> under –30 °C. This work establishes configurational-entropy engineering as an effective strategy for regulating proton-storage thermodynamics and kinetics in H<sub>2</sub> batteries under extreme conditions.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6598–6606"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149003385","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}
引用次数: 0
Pressure-Driven Performance and Thermal Safety Tradeoff in Solid-State Batteries 固态电池的压力驱动性能和热安全权衡
IF 17.5 1区 材料科学
ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-18 DOI: 10.1021/acsenergylett.6c02060
Arpan K. Sharma, Alvaro J. Miguel, Bairav S. Vishnugopi, Alex M. Bates, Nathan B. Johnson, John Hewson, Loraine Torres-Castro, Partha P. Mukherjee
{"title":"Pressure-Driven Performance and Thermal Safety Tradeoff in Solid-State Batteries","authors":"Arpan K. Sharma,&nbsp;Alvaro J. Miguel,&nbsp;Bairav S. Vishnugopi,&nbsp;Alex M. Bates,&nbsp;Nathan B. Johnson,&nbsp;John Hewson,&nbsp;Loraine Torres-Castro,&nbsp;Partha P. Mukherjee","doi":"10.1021/acsenergylett.6c02060","DOIUrl":"10.1021/acsenergylett.6c02060","url":null,"abstract":"<p>Solid-state batteries (SSBs) offer high energy density and improved safety, but their performance is limited by poor particle contact and sluggish ion transport across solid–solid interfaces. External pressure improves electrochemical performance by enhancing interfacial contact and reducing resistance; however, its impact on thermal behavior and safety remains unclear. Here, we investigate how pressure influences the thermal response of composite solid-state cathodes and its implications for cell-level safety. Over 0–70 MPa, increasing pressure enhances capacity but induces a nonmonotonic thermal response governed by the balance between reduced heat generation and extended discharge duration. Pressure consistently improves thermal efficiency by lowering the heat-to-capacity ratio. Incorporating a self-heating onset criterion, we quantify thermal runaway risk and identify performance-safety trade-offs that evolve with pressure, C-rate, and cathode thickness. These results provide design guidelines for pressure-optimized, thermally stable SSBs for high-power and high-energy applications.</p>","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6755–6763"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149003386","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}
引用次数: 0
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