{"title":"An n‐type Polymer with High‐Performance Thermoelectric Properties by Solvent‐Mediated Oxidation","authors":"Zhijun Chen, Yue Wen, Yuzhi Hu, Chunlin Wu, Cheng Xu, Tongwei Zhang, Qingyang Ni, Sunmi Shin, Kuan Sun, Jianyong Ouyang","doi":"10.1002/aenm.202502996","DOIUrl":"https://doi.org/10.1002/aenm.202502996","url":null,"abstract":"Organic thermoelectric (OTE) materials are interesting because they can have the merits of high mechanical flexibility, lightweight, and low or no toxicity over inorganic thermoelectric (TE) materials. Both <jats:italic>p</jats:italic>‐ and <jats:italic>n</jats:italic>‐type OTE materials are required for efficient TE conversion. But the performance of <jats:italic>n</jats:italic>‐type OTE materials lags well behind their <jats:italic>p</jats:italic>‐type counterparts. Herein, the great enhancement in the TE properties of poly(benzodifurandione) (PBFDO) films through a treatment with a solution of FeCl<jats:sub>3</jats:sub> with dimethyl sulfoxide (DMSO) as the solvent is reported. This can greatly enhance the Seebeck coefficient and thus the power factor of PBFDO. The optimal power factor is 306.1 ± 8.7 µW m<jats:sup>−1</jats:sup> K<jats:sup>−2</jats:sup>, and the corresponding electrical conductivity and Seebeck coefficient are 970 ± 26 S cm<jats:sup>−1</jats:sup> and −56.2 ± 1.6 µV K<jats:sup>−1</jats:sup>, respectively. This is the highest power factor for <jats:italic>n</jats:italic>‐type OTEs. The corresponding <jats:italic>ZT</jats:italic> value is 0.27 ± 0.01 at room temperature. The TE properties depend on the solvent of the FeCl<jats:sub>3</jats:sub> solution. A solvent with a high donor number, like DMSO, can share its electrons with PBFDO. It can hinder the dedoping of PBFDO by Fe<jats:sup>3+</jats:sup> and thus greatly enhance the Seebeck coefficient while not lowering the electrical conductivity too much.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"122 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145260614","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Optimizing Lithium Nucleation Overpotential in Anode-Free Garnet-Based Hybrid Solid-State Batteries","authors":"Subhajit Sarkar, Joshua Budde, Ingo Bardenhagen, Julian Schwenzel, Todd Sutherland, Venkataraman Thangadurai","doi":"10.1002/aenm.202503537","DOIUrl":"https://doi.org/10.1002/aenm.202503537","url":null,"abstract":"Anode-free solid-state lithium batteries promise high-energy-density storage but remain limited by unstable interfaces between the solid electrolyte and in situ-formed lithium. In this work, a hybrid solid–liquid electrolyte strategy is developed using a localized high-concentration electrolyte containing AlCl<sub>3</sub> and LiPO<sub>2</sub>F<sub>2</sub>, a trilayer garnet-type Li<sub>6.4</sub>Ga<sub>0.1</sub>La<sub>2.9</sub>Ba<sub>0.1</sub>Zr<sub>1.6</sub>Ta<sub>0.4</sub>O<sub>12</sub> solid electrolyte. This configuration forms a mechanically stable and ionically conductive solid-liquid electrolyte interphase, enabling 81% Coulombic efficiency after 300 cycles at 2 mA cm<sup>−2</sup> and 1 mAh cm<sup>−2</sup> in Cu/Li half-cells. A single-layer anode-free hybrid solid-state pouch cell demonstrated excellent long-term cycling performance, retaining 75% of its initial capacity after 400 cycles at 1C (1.25 mA cm<sup>−2</sup>), with a Coulombic efficiency of 99% without external pressure and at room temperature. At the lab scale, this hybrid electrolyte approach shows both scalability and performance, providing a potential practical pathway to next-generation anode-free hybrid solid-state lithium batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"31 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255432","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}
Trong Huy Pham, Hung D. T. Lai, Ngoc Kim Dang, Tu N. Nguyen, Viktoria Golovanova, Eduardo Henrique Dias, Anh-Dao Ho, Lu Xia, Jackson Crane, F. Pelayo García de Arquer, Edward H. Sargent, David Sinton, Cao-Thang Dinh
{"title":"Ambipolar Ion Transport Membranes Enable Stable Noble-Metal-Free CO2 Electrolysis in Neutral Media","authors":"Trong Huy Pham, Hung D. T. Lai, Ngoc Kim Dang, Tu N. Nguyen, Viktoria Golovanova, Eduardo Henrique Dias, Anh-Dao Ho, Lu Xia, Jackson Crane, F. Pelayo García de Arquer, Edward H. Sargent, David Sinton, Cao-Thang Dinh","doi":"10.1002/aenm.202504286","DOIUrl":"https://doi.org/10.1002/aenm.202504286","url":null,"abstract":"Carbon dioxide (CO<sub>2</sub>) electrolysis traditionally relies on monopolar ion-exchange membranes, including anion exchange membranes (AEM), cation exchange membranes (CEM), and a layered juxtaposition of two such monopolar membranes (bipolar membrane, BPM). The monopolar approach has worked well in water electrolysis in alkaline and acidic environments; however, in CO<sub>2</sub> electrolysis, alkaline conditions promote carbonate formation, reducing stability, while acidic media favor competing hydrogen evolution reaction. Here, ambipolar ion transport membranes (AITMs) are reported in CO<sub>2</sub> electrolysis. AITMs facilitate the free movement of ions and water between the cathode and anode, enabling stable CO<sub>2</sub> electrolysis with highly concentrated electrolytes. This results in low operating cell voltages and compatibility with Earth-abundant anodes in pH-neutral electrolytes. Using a membrane electrode assembly cell, the electrochemical CO<sub>2</sub> reduction is demonstrated in neutral media with a benchmark copper-sputtered polytetrafluoroethylene cathode and a nickel anode, achieving a high Faradaic efficiency of 75% for C<sub>2</sub> products. This system operates at a current density of 110 mA cm<sup>−2</sup> and a cell voltage of 3.15 V, maintaining a stable performance with a total operation exceeding 950 h. This work provides a pathway for stable CO<sub>2</sub> conversion at relatively high current densities using Earth-abundant materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"24 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255427","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}
Ashutosh Rana, Md. Arif Faisal, James H. Nguyen, Saptarshi Paul, John F. Koons, Jeremy H. Lawrence, Kingshuk Roy, Jeffrey E. Dick
{"title":"An Electroanalytical Perspective on the Competitive Interplay between Zinc Deposition and Hydrogen Evolution in Aqueous Zinc Metal Batteries","authors":"Ashutosh Rana, Md. Arif Faisal, James H. Nguyen, Saptarshi Paul, John F. Koons, Jeremy H. Lawrence, Kingshuk Roy, Jeffrey E. Dick","doi":"10.1002/aenm.202503630","DOIUrl":"https://doi.org/10.1002/aenm.202503630","url":null,"abstract":"This perspective highlights the consequences of the intricate interplay between the hydrogen evolution reaction (HER) and zinc electrodeposition on anode stability in aqueous zinc metal batteries (AZMBs), considering both cycling and resting conditions. Recent advances in the precise quantification of HER kinetics and its mechanistic origin are discussed, alongside accurately probing the kinetics of zinc plating using fast-scan voltammetry. From an electroanalytical standpoint, we emphasize on how measurement science has informed electrolyte and additive design, SEI engineering, charge–discharge protocols, and interfacial pH effects. The findings discussed help rationalize observed phenomena, such as paradoxically high Coulombic efficiencies at high current densities. Importantly, challenges during resting states are highlighted, where spontaneous HER and corrosion lead to active loss of zinc inventory (12–37%). Taken together, this work underscores the need for standardized kinetic evaluation and comprehensive stability metrics to guide the rational design of next-generation AZMB anodes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"18 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255422","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}
Emma van der Minne, Priscila Vensaus, Vadim Ratovskii, Seenivasan Hariharan, Jan Behrends, Cesare Franchini, Jonas Fransson, Sarnjeet S. Dhesi, Felix Gunkel, Florian Gossing, Georgios Katsoukis, Ulrike I. Kramm, Magalí Lingenfelder, Qianqian Lan, Yury V. Kolen'ko, Yang Li, Ramsundar Rani Mohan, Jeffrey McCord, Lingmei Ni, Eva Pavarini, Rossitza Pentcheva, David H. Waldeck, Michael Verhage, Anke Yu, Zhichuan J. Xu, Piero Torelli, Silvia Mauri, Narcis Avarvari, Anja Bieberle-Hütter, Christoph Baeumer
{"title":"Spin Matters: A Multidisciplinary Roadmap to Understanding Spin Effects in Oxygen Evolution Reaction During Water Electrolysis","authors":"Emma van der Minne, Priscila Vensaus, Vadim Ratovskii, Seenivasan Hariharan, Jan Behrends, Cesare Franchini, Jonas Fransson, Sarnjeet S. Dhesi, Felix Gunkel, Florian Gossing, Georgios Katsoukis, Ulrike I. Kramm, Magalí Lingenfelder, Qianqian Lan, Yury V. Kolen'ko, Yang Li, Ramsundar Rani Mohan, Jeffrey McCord, Lingmei Ni, Eva Pavarini, Rossitza Pentcheva, David H. Waldeck, Michael Verhage, Anke Yu, Zhichuan J. Xu, Piero Torelli, Silvia Mauri, Narcis Avarvari, Anja Bieberle-Hütter, Christoph Baeumer","doi":"10.1002/aenm.202503556","DOIUrl":"https://doi.org/10.1002/aenm.202503556","url":null,"abstract":"A central challenge in water electrolysis lies with the oxygen evolution reaction (OER) where the formation of molecular oxygen (O<sub>2</sub>) is hindered by the constraint of angular momentum conservation. While the reactants OH<sup>−</sup> or H<sub>2</sub>O are diamagnetic (DM), the O<sub>2</sub> product has a paramagnetic (PM) triplet ground state, requiring a change in spin configuration when being formed. This constraint has prompted interest in spin-selective catalysts as a means to facilitate OER. In this context, the roles of magnetism and chirality-induced spin selectivity (CISS) in promoting the OER reaction have recently been investigated through both theoretical and experimental studies. However, pinpointing the key principles and their relative contribution in mediating spin-enhancement remains a significant challenge. This roadmap offers a forward-looking perspective on current experimental trends and theoretical developments in spin-enhanced OER electrocatalysis and outlines strategic directions for integrating incisive experiments and operando approaches with computational modeling to disentangle key mechanisms. By providing a conceptual framework and identifying critical knowledge gaps, this perspective aims to guide researchers toward dedicated experimental and computational studies that will deepen the understanding of spin-induced OER enhancement and accelerate the development of next-generation catalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"20 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145255426","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}
Steffen Weinmann, Hana Gobena, Lucie Quincke, Jesse J. Hinricher, Samuel Merk, Hyunwon Chu, Thorben Prein, Jennifer L.M. Rupp, Kun Joong Kim
{"title":"Stabilizing Interfaces of All-Ceramic Composite Cathodes for Li-Garnet Batteries (Adv. Energy Mater. 37/2025)","authors":"Steffen Weinmann, Hana Gobena, Lucie Quincke, Jesse J. Hinricher, Samuel Merk, Hyunwon Chu, Thorben Prein, Jennifer L.M. Rupp, Kun Joong Kim","doi":"10.1002/aenm.70184","DOIUrl":"https://doi.org/10.1002/aenm.70184","url":null,"abstract":"<p><b>Lithium Metal Batteries</b></p><p>A novel co-firing approach enables dense, secondary-phase-free LiCoO<sub>2</sub>–Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> composite cathodes under high lithium and oxygen partial pressures. This strategy reduces interfacial resistance by orders of magnitude and delivers a record areal capacity of 3.48 mAh cm<sup>−2</sup>, advancing the development of oxide-based all-solid-state lithium metal batteries. More in article number 2502280, Kun Joong Kim and co-workers.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 37","pages":""},"PeriodicalIF":26.0,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://advanced.onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.70184","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145243075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Eswaran Jayaraman, Michela Prete, Abhinav Chandel, Fathimath Faseela, Kun Wang, Chun Yuen Ho, Jani Lamminaho, Morten Madsen
{"title":"Flexible ITO‐Free Organic Solar Modules Using Fully Roll‐to‐Roll Processable Top Illumination Design","authors":"Eswaran Jayaraman, Michela Prete, Abhinav Chandel, Fathimath Faseela, Kun Wang, Chun Yuen Ho, Jani Lamminaho, Morten Madsen","doi":"10.1002/aenm.202504465","DOIUrl":"https://doi.org/10.1002/aenm.202504465","url":null,"abstract":"Organic photovoltaics (OPVs) have reached above 20% Power Conversion Efficiency (<jats:italic>PCE</jats:italic>) in recent years. However, all state‐of‐the‐art devices are fabricated using techniques that are largely unsuitable for industry‐compatible Roll‐to‐Roll (R2R) coating methods. In this study, a hybrid approach that combines the advantages of R2R vacuum and solution coating methods for fabricating organic solar modules on glass and flexible polyethylene terephthalate (PET) in a top‐illumination configuration is adopted. The opaque bottom electrodes are developed using R2R sputtering to achieve low sheet resistance and reduced surface roughness. The remaining layers in the devices, including top transparent Silver nanowire (AgNWs) anodes, are optimized using the R2R‐compatible slot‐die coating method at ambient conditions using greener solvents. The best devices on glass substrates achieved a <jats:italic>PCE</jats:italic> of 13.5%, using this ITO‐free scalable OPV architecture. An equally impressive <jats:italic>PCE</jats:italic> of 12.5% is attained when the devices are scaled up to mini‐modules with an active area of 12.8 cm<jats:sup>2</jats:sup>. Furthermore, six mini‐modules on a PET substrate measuring 24 cm x 17 cm are developed, reaching <jats:italic>PCE</jats:italic> up to 11.5%, the highest reported in this category. This research highlights the potential for developing high‐performance, cost‐efficient, and mechanically adaptable ITO‐free devices using industry‐compatible methods.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"158 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241193","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}
Sourav Chaule, Doniyor Khudoyarov, Sungdo Kim, Yeju Yoon, Ji-Hyun Jang
{"title":"Inverse-L Shaped Evaporator Based on La1−xSrxMnO3 Perovskite with Efficient Salt Collection via Localized Salt Gradient (Adv. Energy Mater. 37/2025)","authors":"Sourav Chaule, Doniyor Khudoyarov, Sungdo Kim, Yeju Yoon, Ji-Hyun Jang","doi":"10.1002/aenm.70183","DOIUrl":"10.1002/aenm.70183","url":null,"abstract":"<p><b>Solar Desalination</b></p><p>Solar desalination offers a sustainable route to freshwater but is often hindered by low evaporation rates and salt fouling. In article number 2501360, Ji-Hyun Jang and co-workers demonstrated that La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub> enables efficient photothermal conversion via intra-band trap states, achieving a high evaporation rate of 3.40 kg m<sup>−2</sup> h under one sun. Additionally, its edge-directed salt management effectively prevents surface fouling.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 37","pages":""},"PeriodicalIF":26.0,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://advanced.onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.70183","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241194","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"MXene-Scaffolded Planner Mesoporous Carbon with Homogeneous Electric Field Enabling Uniform and Robust SEI for Ultra-Stable Sodium Storage","authors":"Mengjia Yu, Zhongting Wang, Lei Zhao, Yumei Wang, Suparada Kamchompo, Kexin Liu, Jianming Wang, Jintara Padchasri, Shuai Yuan, Yin Fang, Siriporn Jungsuttiwong, Phornphimon Maitarad, Pinit Kidkhunthod, Liyi Shi, Dongyuan Zhao, Yingying Lv","doi":"10.1002/aenm.202503682","DOIUrl":"https://doi.org/10.1002/aenm.202503682","url":null,"abstract":"For next-generation sodium-ion batteries, nanostructured porous carbons with high surface areas exhibit enhanced rate performance, yet their commercialization is constrained by insufficient cycling stability. Herein, an insight from electrode architecture by using planar 2D MXene@mesoporous carbon (MXene@mesoC) nanosheets are developed to address this challenge. By precisely modulating, the engineered electrode achieves an ultra-smooth surface, which ensures uniform current density and effectively suppresses localized charge accumulation and result a homogeneous electric field. Combined with the mesopore-induced enrichment of PF<sub>6</sub><sup>−</sup> anions in the Inner Helmholtz layer and a significantly reduced decomposition energy barrier catalyzed by MXene, a uniform, robust, and NaF-rich solid electrolyte interphase (SEI) is formed. The resulting anode demonstrates exceptional electrochemical performance, including ultra-stable cycling (98.4% capacity retention after 10 000 cycles at 5.0 A g<sup>−1</sup>), high average Coulombic efficiency (99.98%), and remarkable low-temperature operation (down to −40 °C). Furthermore, the feasibility of inkjet printing these materials into customizable microstructures highlights their potential for flexible and high-loading electrodes. This electrode architecture strategy bridges nanoscale interfacial regulation with macroscopic electrode design, offering a general approach for advanced sodium-ion storage in the future.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"128 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247652","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}
Meilian Cao, Menglu Feng, Jun Hu, Yue Xu, Chun Fang, Jian Peng, Jiantao Han, Yunhui Huang
{"title":"Dual Regulation of Stability and Kinetics in Iron-Based Mixed Phosphate Cathode for All-Climate Sodium-Ion Batteries","authors":"Meilian Cao, Menglu Feng, Jun Hu, Yue Xu, Chun Fang, Jian Peng, Jiantao Han, Yunhui Huang","doi":"10.1002/aenm.202504854","DOIUrl":"https://doi.org/10.1002/aenm.202504854","url":null,"abstract":"Iron-based mixed-phosphate Na<sub>4</sub>Fe<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>P<sub>2</sub>O<sub>7</sub> (NFPP) is a representative cathode for sodium-ion batteries owing to its low cost and environmental compatibility. The behavior of sodium ions in NFPP is governed by four crystallographically distinguishable sodium sites, yet the underlying mechanism for occupation sites and diffusion kinetics remains not fully understood. Herein, a scalable synthesis strategy for NFPP materials with tunable local structures is proposed by controlling the iron valence during preparation. The nonstoichiometric Na<sub>4.024</sub>Fe<sub>2.921</sub>(PO<sub>4</sub>)<sub>2</sub>P<sub>2</sub>O<sub>7</sub> strikes an optimal balance between the ordering and proportion of inert sodium ions. These ordered inert sodium ions act as structural pillars, providing markedly enhanced stability compared to disordered counterparts. The optimized sodium environment leads to a synergistic enhancement of both thermal stability and sodium ionic kinetics. The cathode delivers a remarkable rate performance and cycling stability (90.7% capacity retention after 10,000 cycles). This exceptional stability is corroborated by a small lattice volume variation of 4.18% upon desodiation. Moreover, cylindrical full cells assembled with kilogram-scale Na<sub>4.024</sub>Fe<sub>2.921</sub>(PO<sub>4</sub>)<sub>2</sub>P<sub>2</sub>O<sub>7</sub> cathode and a hard carbon anode demonstrate excellent performance across a wide temperature range from −40 to 45 °C. This work establishes the critical interplay between local environment and electrochemical properties, offering valuable insights for the design of advanced cathode materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"9 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247653","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}