ACS Energy Letters 最新文献_第9页

Valorization of Nitrate and Carbon Dioxide into Ammonia and Urea under Visible Light 硝酸盐和二氧化碳在可见光下转化为氨和尿素的研究

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.6c01894

Eve K Stegner, Nadeeka Lakshani, Madison R Kuns, Alba Ruiz-Aguirre, Ilaria Berruti, Sixto Malato, Gonzalo Guirado, Javier Vela

{"title":"Valorization of Nitrate and Carbon Dioxide into Ammonia and Urea under Visible Light","authors":"Eve K Stegner, Nadeeka Lakshani, Madison R Kuns, Alba Ruiz-Aguirre, Ilaria Berruti, Sixto Malato, Gonzalo Guirado, Javier Vela","doi":"10.1021/acsenergylett.6c01894","DOIUrl":"10.1021/acsenergylett.6c01894","url":null,"abstract":"The energy-intensive manufacture of nitrogen-based fertilizers such as ammonia (NH3) and urea consumes a significant fraction of the global energy supply. At the same time, widespread accumulation of excess nitrate (NO3–) from agricultural runoff poses serious risks to ecological and human health. These escalating environmental and economic costs highlight a pressing need for more sustainable fertilizer production. Photocatalytic conversion of waste NO3– into NH3 underscores a growing interest in circular low-energy alternatives to the traditional Haber–Bosch process. For example, as the most widely applied nitrogen fertilizer, analogous routes to urea remain critically underdeveloped. We demonstrate the valorization of two abundant and harmful pollutants, nitrate and carbon dioxide (CO2) into urea over a mixture of commercially available TiO2 and CuO photocatalysts. The ability to drive this complex transformation under ambient temperature and pressure using solar energy highlights its potential to lower the energy demand of conventional fertilizer production. These results provide a fundamental platform from which to envision a more sustainable, visible light-driven ammonia/urea synthesis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6651–6656"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148908740","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

Tailoring Guest Symmetry for Efficient Charge Transport via Pre-structuring in Ternary Organic Solar Cells 利用三元有机太阳能电池的预结构裁剪客体对称以实现高效电荷输运

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-04 DOI: 10.1021/acsenergylett.6c01944

Zhichao Mao, Haotian Hu, Jing Li, Jingyu Shi, Yaqin Gong, Mengmeng Yang, Jiahan Xie, Changming Han, Wei Song, Ziyi Ge

{"title":"Tailoring Guest Symmetry for Efficient Charge Transport via Pre-structuring in Ternary Organic Solar Cells","authors":"Zhichao Mao, Haotian Hu, Jing Li, Jingyu Shi, Yaqin Gong, Mengmeng Yang, Jiahan Xie, Changming Han, Wei Song, Ziyi Ge","doi":"10.1021/acsenergylett.6c01944","DOIUrl":"10.1021/acsenergylett.6c01944","url":null,"abstract":"Achieving an ideal bi-continuous network in organic solar cells requires balancing molecular self-assembly and film-formation kinetics. For strong-interaction polymers like D18, intense backbone interactions often lead to kinetically trapped, disordered states. Here, we present a molecular symmetry-breaking strategy using an asymmetric small-molecule donor, BC-A2O, as a guest regulator. Compared with its symmetric counterpart BC-A4O, BC-A2O features a rigid rhodanine hook and higher liquid-crystal Gibbs free energy difference. This strong thermodynamic drive enables BC-A2O to preferentially anchor onto D18 chains, establishing solution-phase interfacial pre-structuring that seeds a highly ordered fibrillar host network with optimized charge transport channels. Consequently, BC-A2O-based ternary devices achieve a benchmark efficiency of 20.53% (versus 19.46% for the binary baseline) with a fill factor of 81.16%. This work demonstrates the power of small-molecule donors in orchestrating hierarchical assembly for advanced photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6707–6718"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148895431","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

Dual-Side Engineered Bilayer Molybdenum for Flexible Monolithic Perovskite/ Cu(In,Ga)Se2 Tandem Solar Cells on Polyimide 基于聚酰亚胺的柔性单片钙钛矿/ Cu(In,Ga)Se2串联太阳能电池的双侧工程钼

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-02 DOI: 10.1021/acsenergylett.6c01967

Liting Tang, Huachuan Zhou, Hui Yan, Li Zeng, Jun Luo, Wuji Wang, Haofei Xia, Yujie Chen, Zhipeng Zhao, Xiaomin Wang, Xudong Xiao, Jianmin Li

{"title":"Dual-Side Engineered Bilayer Molybdenum for Flexible Monolithic Perovskite/ Cu(In,Ga)Se2 Tandem Solar Cells on Polyimide","authors":"Liting Tang, Huachuan Zhou, Hui Yan, Li Zeng, Jun Luo, Wuji Wang, Haofei Xia, Yujie Chen, Zhipeng Zhao, Xiaomin Wang, Xudong Xiao, Jianmin Li","doi":"10.1021/acsenergylett.6c01967","DOIUrl":"10.1021/acsenergylett.6c01967","url":null,"abstract":"Flexible monolithic perovskite/Cu(In,Ga)Se2 (CIGS) tandem solar cells (TSCs) on polyimide (PI) substrates suffer from severe interfacial delamination and compromised CIGS crystallization induced by back-contact thermal limitations. Herein, we introduce a dual-side engineered bilayer molybdenum (DEBM) architecture to mitigate these challenges. The loose surface layer of DEBM enhances selenium diffusion to secure robust adhesion, while the backside Mo microstructure modulates infrared reflectivity for efficient thermal management. This synergistic regulation improves CIGS crystallization and suppresses defects. Consequently, single-junction flexible CIGS cells eliminate cracking and delamination, achieving a > 20.0% certified efficiency. The integrated monolithic TSCs deliver a champion efficiency of 27.03% (certified 26.30%), the highest efficiency reported to date for PI-based TSCs. The device also exhibits outstanding bending durability, retaining over 96% of initial performance after 20,000 bending cycles at a 5 mm radius. This architecture provides a viable pathway for highly reliable, flexible tandem photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6719–6726"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148885266","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

Enhanced Operational Stability in Tin-Based Perovskite Solar Cells via a Natural Antioxidant 天然抗氧化剂增强锡基钙钛矿太阳能电池的运行稳定性

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-27 DOI: 10.1021/acsenergylett.6c01792

Shengnan Zuo, Kazuki Morita, Yuan Zhang, Arman Mahboubi Soufiani, Thomas W. Gries, Mailis Lounasvuori, Fan Hu, Andrea Cabrera-Espinoza, Pedro B. Groszewicz, Yeonghun Yun, Wentao Liu, Chiara Frasca, Yuxin Liu, Siddha Hill, Alwani Imanah Rafieh, Fengshuo Zu, Martin D. Hager, Ulrich S. Schubert, Steve Albrecht, Norbert Koch, Klaus Lips, Meng Li, Artem Musiienko, Eva Unger, Antonio Abate

{"title":"Enhanced Operational Stability in Tin-Based Perovskite Solar Cells via a Natural Antioxidant","authors":"Shengnan Zuo, Kazuki Morita, Yuan Zhang, Arman Mahboubi Soufiani, Thomas W. Gries, Mailis Lounasvuori, Fan Hu, Andrea Cabrera-Espinoza, Pedro B. Groszewicz, Yeonghun Yun, Wentao Liu, Chiara Frasca, Yuxin Liu, Siddha Hill, Alwani Imanah Rafieh, Fengshuo Zu, Martin D. Hager, Ulrich S. Schubert, Steve Albrecht, Norbert Koch, Klaus Lips, Meng Li, Artem Musiienko, Eva Unger, Antonio Abate","doi":"10.1021/acsenergylett.6c01792","DOIUrl":"10.1021/acsenergylett.6c01792","url":null,"abstract":"In tin-based perovskite solar cells (TPSCs), Sn(II) oxidation and illumination-induced lattice instability are primary drivers of device degradation. In this study, we introduce ellagic acid (EA), a natural antioxidant, into DMSO-free fabricated tin perovskites. Computational simulations show that EA stabilizes formamidinium sites within the perovskite lattice and effectively inhibits Sn(II) oxidation. Besides, this incorporation greatly improves film homogeneity and passivates defect traps, increasing the champion power conversion efficiency from 9.3 to 10.2%. Consequently, unencapsulated EA-incorporated devices exhibit a sixfold increase in T80 lifetime (in a nitrogen atmosphere) and a threefold increase in T60 lifetime (in dry air) at the maximum power point tracking under continuous illumination. Moreover, an EA-incorporated device achieves a 16% increment over 1000 h of day/night cycling, significantly outperforming the 7% rise of the control. These results demonstrate that natural antioxidants are a highly effective and sustainable strategy for enhancing the operational stability of lead-free TPSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6590–6597"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049805","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

Before You Submit Another Perovskite Additive Paper 在您提交另一份钙钛矿添加剂论文之前

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-27 DOI: 10.1021/acsenergylett.6c02887

Filippo De Angelis

引用次数: 0

Impact of Solvent Impurities from Upscaled Synthesis and Their Purification in Lithium Metal Batteries 锂金属电池规模化合成中溶剂杂质的影响及其净化

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-29 DOI: 10.1021/acsenergylett.6c02137

Hao Lyu, Tianyang Chen, Zehao Cui, Chen Liu, Jonathan Miller, Hui Zhou, Fenghua Guo, Elizabeth Zhang, Yangju Lin, Gan Chen, Yuelang Chen, Il Rok Choi, Trevor L. Dzwiniel, Arumugam Manthiram, M. Stanley Whittingham, Zhenan Bao

{"title":"Impact of Solvent Impurities from Upscaled Synthesis and Their Purification in Lithium Metal Batteries","authors":"Hao Lyu, Tianyang Chen, Zehao Cui, Chen Liu, Jonathan Miller, Hui Zhou, Fenghua Guo, Elizabeth Zhang, Yangju Lin, Gan Chen, Yuelang Chen, Il Rok Choi, Trevor L. Dzwiniel, Arumugam Manthiram, M. Stanley Whittingham, Zhenan Bao","doi":"10.1021/acsenergylett.6c02137","DOIUrl":"10.1021/acsenergylett.6c02137","url":null,"abstract":"Fluorinated ether electrolytes are promising for high-energy-density lithium metal batteries, yet their translation to larger-scale production requires systematic control of solvent impurities generated during synthesis and purification. Using 2-(2-(2,2-difluoroethoxy)ethoxy)–1,1,1-trifluoroethane (F5DEE) as a high-performance model solvent, we compare gram- and kilogram-scale batches to correlate impurity origin, purification, and electrochemistry. Although upscaled F5DEE shows >99% purity by standard techniques, ppm-level moisture and organic impurities reduce Li Coulombic efficiency and increase cell variability. We classify impurities by generation pathway into retained intermediates, starting-material-derived analogues, side-reaction products, and purification-introduced residues. Distillation, adsorption, and reactive purification implicate water, alkoxide-derived byproducts, and amines as key performance-limiting species. However, excessive purification generates secondary impurities that degrade performance, revealing a removal–generation trade-off. Thermal, electrochemical, operando microcalorimetry, and online mass spectrometry analyses reveal impurity-dependent current-collector corrosion, heat release, gas evolution, and full-cell degradation. This route-resolved, source-to-consequence workflow provides a transferable qualification framework for electrolyte solvent scale-up.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6822–6831"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091008","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

Mapping Solid Electrolyte Interphase Evolution and Lithium Deposition at Solid-State Interfaces by Operando Nano-focus WAXS 利用Operando纳米焦点WAXS在固态界面上映射固体电解质界面演化和锂沉积

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-04 DOI: 10.1021/acsenergylett.6c01817

Yingying Yan, Liangzhen Liu, Yuxin Liang, Fabian A.C. Apfelbeck, Lyuyang Cheng, Guangjiu Pan, Da Lei, Lixing Li, Tianle Zheng, Zhuijun Xu, Lan Xia, Cheng Yuan, Liang Zhang, Ya-Jun Cheng, Anton Davydok, Christina Krywka, Roland A. Fischer, Peter Müller-Buschbaum

{"title":"Mapping Solid Electrolyte Interphase Evolution and Lithium Deposition at Solid-State Interfaces by Operando Nano-focus WAXS","authors":"Yingying Yan, Liangzhen Liu, Yuxin Liang, Fabian A.C. Apfelbeck, Lyuyang Cheng, Guangjiu Pan, Da Lei, Lixing Li, Tianle Zheng, Zhuijun Xu, Lan Xia, Cheng Yuan, Liang Zhang, Ya-Jun Cheng, Anton Davydok, Christina Krywka, Roland A. Fischer, Peter Müller-Buschbaum","doi":"10.1021/acsenergylett.6c01817","DOIUrl":"10.1021/acsenergylett.6c01817","url":null,"abstract":"Composite solid polymer electrolytes (CSPEs) have emerged as promising candidates for next-generation lithium metal batteries. However, the spatial evolution of the solid electrolyte interphase (SEI) at solid-state interfaces remains poorly understood despite its critical role in lithium metal stability. Herein, the anion-trapping layered double hydroxide (LDH) is introduced to poly(ethylene oxide)-based CSPEs to regulate Li+ transport and stabilize the lithium/electrolyte interface. The LDH-enhanced electrolyte achieves exceptional cycling stability over 950 h with a lithium electrode and 90.1% capacity retention after 250 cycles in LiFePO4||Li full cells. Operando nano-focus wide-angle X-ray scattering maps the spatial distributions of both the SEI and lithium dendrites at the lithium/electrolyte interface across micron-scale lateral and vertical dimensions. The regulated Li+ flux promotes homogeneous lithium deposition and the formation of a robust, multifunctional SEI, thereby suppressing lithium dendrite growth and stabilizing the interface. This study provides direct visualization of SEI evolution in CSPEs and clarifies its role in dendrite-free all-solid-state lithium metal batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6607–6617"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148895430","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

Chemo-electrochemical Tandem Reduction Enables Eupolymer-Inorganic Solid-Electrolyte Interphases for Silicon-Based Anodes 化学-电化学串联还原使欧洲聚合物-无机固体-电解质界面用于硅基阳极

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-02 DOI: 10.1021/acsenergylett.6c02291

Hao Zhang, Lu Wang, Long Chen, Xin He, Ruifan Lin, Huipeng Zeng, Jijian Xu

{"title":"Chemo-electrochemical Tandem Reduction Enables Eupolymer-Inorganic Solid-Electrolyte Interphases for Silicon-Based Anodes","authors":"Hao Zhang, Lu Wang, Long Chen, Xin He, Ruifan Lin, Huipeng Zeng, Jijian Xu","doi":"10.1021/acsenergylett.6c02291","DOIUrl":"10.1021/acsenergylett.6c02291","url":null,"abstract":"Silicon-based anodes offer substantial potential for increasing batteries’ energy density but are limited by unstable solid-electrolyte interphases (SEIs). Here, we report a chemo-electrochemical tandem reduction strategy to construct an integrated eupolymer-inorganic SEI with both favorable mechanical robustness and fast Li+ transport. This strategy couples a selective ester–amine exchange reaction in the bulk electrolyte with a subsequent electrochemical reduction at the anode surface. The identified chemical intermediate exhibits facilitated de-fluorination kinetics, enriching the SEI with nanoscale inorganic species while triggering a free-radical polymerization of unsaturated additives. Benefiting from the integrated eupolymer-inorganic SEI, SiOx anodes demonstrate 80.1% capacity retention after 800 cycles and retain 551.9 mAh g–1 at 5 A g–1. Practical Ah-level Si/C∥NCM811 pouch cells operating under a cut-off voltage of 4.4 V achieve 90.9% capacity retention over 300 cycles, with an average Coulombic efficiency of 99.91%. This work provides profound insights into SEI tailoring, offering pathway toward long-life, fast-charging silicon-based batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6897–6908"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148885311","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

Thermally Robust Organic Photodetectors Enabled by Polymer Acceptors with Tunable Rigidity 刚性可调聚合物受体实现的热鲁棒有机光电探测器

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-02 DOI: 10.1021/acsenergylett.6c01868

Zhong-Ze Qu, Qiaonan Chen, Hoang Mai Luong, Subhrangsu Mukherjee, Qunping Fan, Jordan Fishburn, Yunyan Lai, Harald Ade, Ergang Wang, Thuc-Quyen Nguyen

{"title":"Thermally Robust Organic Photodetectors Enabled by Polymer Acceptors with Tunable Rigidity","authors":"Zhong-Ze Qu, Qiaonan Chen, Hoang Mai Luong, Subhrangsu Mukherjee, Qunping Fan, Jordan Fishburn, Yunyan Lai, Harald Ade, Ergang Wang, Thuc-Quyen Nguyen","doi":"10.1021/acsenergylett.6c01868","DOIUrl":"10.1021/acsenergylett.6c01868","url":null,"abstract":"Organic photodetectors (OPDs) have emerged as promising candidates for next-generation optoelectronic applications. However, their widespread adoption is hindered by the low thermal stability. This study addresses this issue by investigating the performance of OPDs employing three polymer acceptors: PF5-Y5, PYTS-C2, and PY2TS-C2 paired with the PBDB-T polymer donor. These devices demonstrate significantly improved resistance to thermal stress. After annealing at 150 °C for 1 h, the PF5-Y5-based OPDs can maintain a dark current density (Jd) below 1 × 10–6 A/cm2 and an external quantum efficiency (EQE) above 50%, leading to a specific detectivity of 1.7 × 1011 Jones. Detailed analysis reveals that the EQE drop in the PF5-Y5-based OPDs is due to decreased electron mobility, and Jd increases in the PY2TS-C2 and Y6 systems are attributed to enhanced aggregation and phase separation and C60 and electrode diffusion. These results highlight the advantages of polymer acceptors in enhancing thermal robustness and provide design strategies for developing thermally stable OPDs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6629–6640"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148885322","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

Lattice Distortion Regulates Na-Ion Percolation in High-Entropy Cation-Disordered Rocksalt Cathodes 晶格畸变调节na离子在高熵阳离子无序岩盐阴极中的渗透

IF 17.5 1区材料科学

ACS Energy Letters Pub Date : 2026-10-09 Epub Date: 2026-09-24 DOI: 10.1021/acsenergylett.6c02544

Zichang Zhang, Jiewei Cheng, Qiang Sun, Ram B. Gupta, Puru Jena

{"title":"Lattice Distortion Regulates Na-Ion Percolation in High-Entropy Cation-Disordered Rocksalt Cathodes","authors":"Zichang Zhang, Jiewei Cheng, Qiang Sun, Ram B. Gupta, Puru Jena","doi":"10.1021/acsenergylett.6c02544","DOIUrl":"10.1021/acsenergylett.6c02544","url":null,"abstract":"Ion percolation in cation-disordered rocksalt (DRX) Na-ion cathodes is conventionally viewed as a topological problem governed by the connectivity of zero-transition-metal (0-TM) channels. Here, we show that configurational-entropy-induced lattice distortion extends this paradigm by rendering nominally unfavorable 1-TM pathways kinetically accessible in high-entropy DRX cathodes. Guided by a mixing-temperature-based design strategy, we identify a synthetically accessible Na-rich high-entropy DRX cathode, Na1.2Ti0.133Mn0.133Nb0.133V0.133Fe0.133Mo0.133O2, with a percolation-limited accessible capacity of 260.0 mAh g–1 and a corresponding theoretical gravimetric energy density of 718.8 Wh kg–1. First-principles calculations and machine-learning-accelerated hybrid Monte Carlo–molecular dynamics simulations reveal two coupled effects governing Na+ transport: suppressed short-range order enhances 0-TM connectivity, while lattice distortion lowers migration barriers along 1-TM pathways, expanding the effective percolation network beyond the conventional 0-TM limit. These findings recast ion percolation as a topology–kinetics-coupled phenomenon and establish lattice adaptability as a design variable for engineering fast ion transport in high-entropy cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 10","pages":"6981–6989"},"PeriodicalIF":17.5,"publicationDate":"2026-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049813","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