Beyond ionic conduction and solid-electrolyte interphase formation, the fundamental roles of lithium salt anions in batteries remain unexplored. Herein, an anion-induced competitive solvation mechanism that governs lithium polysulfide (LiPS) behaviors in high-energy-density lithium–sulfur batteries is pioneeringly unveiled. Specifically, anions contend against weakly solvating solvents to occupy the LiPS inner solvation shell. Enhancing anion coordination while diminishing weakly solvating solvent coordination overcomes the rate-determining LiPS charge-transfer barriers. As a proof of concept, bis(fluorosulfonyl)imide anion coordination reduces activation polarization and boosts cycling stability at high current densities. Ah-level pouch cells achieve stable operation at high rates of 0.35 C and deliver a record-setting energy density of 622 Wh kg−1 (based on total weight) with stable cycling. By elucidating the anion-induced competitive solvation mechanism, our work transcends conventional views of anion roles and establishes a new paradigm for advancing practical Li–S batteries.
{"title":"Competitive anion coordination overcomes charge-transfer barriers for lithium–sulfur batteries","authors":"Xi-Yao Li, Bo-Quan Li, Tian Jin, Shuai Feng, Yu-Chen Gao, Meng Zhao, Xiang Chen, Jia-Qi Huang, Qiang Zhang","doi":"10.1016/j.joule.2025.102259","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102259","url":null,"abstract":"Beyond ionic conduction and solid-electrolyte interphase formation, the fundamental roles of lithium salt anions in batteries remain unexplored. Herein, an anion-induced competitive solvation mechanism that governs lithium polysulfide (LiPS) behaviors in high-energy-density lithium–sulfur batteries is pioneeringly unveiled. Specifically, anions contend against weakly solvating solvents to occupy the LiPS inner solvation shell. Enhancing anion coordination while diminishing weakly solvating solvent coordination overcomes the rate-determining LiPS charge-transfer barriers. As a proof of concept, bis(fluorosulfonyl)imide anion coordination reduces activation polarization and boosts cycling stability at high current densities. Ah-level pouch cells achieve stable operation at high rates of 0.35 C and deliver a record-setting energy density of 622 Wh kg<sup>−1</sup> (based on total weight) with stable cycling. By elucidating the anion-induced competitive solvation mechanism, our work transcends conventional views of anion roles and establishes a new paradigm for advancing practical Li–S batteries.","PeriodicalId":343,"journal":{"name":"Joule","volume":"30 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146021979","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102233
Huaimin Jin , Xingyu Wang , Simeng Zhang , Xiangzhen Zhu , Chong Liu , Junyi Yue , Jie Qu , Bei Wu , Xu Han , Yueyue Wang , Yang Xu , Han Wu , Liyu Zhou , Mingying Zhang , Hao Lai , Shuo Wang , Jiangwen Liang , Xueliang Sun , Xiaona Li
Fluoride solid-state electrolytes (SSEs) offer superior electrochemical stability, making them theoretically ideal for high-voltage all-solid-state batteries (ASSBs), but their low Li+ conductivity hinders practical application. Here, we exploit the polyanion coordination strategy to develop a class of fluoride SSEs, LixTi(PO4)x/3F4, which exhibits high ionic conductivity and ultrahigh-voltage stability. Especially, Li1.3Ti(PO4)1.3/3F4 (1.16 × 10−5 S cm−1) demonstrates a two-order-of-magnitude enhancement in Li+ conductivity compared to analogous Li2TiF6. Combined experimental and theoretical analyses reveal that the high ionic conductivity of LixTi(PO4)x/3F4 arises from weakened Li+-surrounding interactions and flexible network structures. Attractively, the exceptional ionic conductivity and ultrahigh-voltage stability of Li1.3Ti(PO4)1.3/3F4 enable a low-resistance and highly stable electrolyte-electrode interface, contributing to 91.6% capacity retention after 200 cycles for 5 V-class LiNi0.5Mn1.5O4-based ASSBs at 1 C and 30°C. The discoveries in this work open a new avenue for designing high-conductivity fluoride SSEs, paving the way for the application of high-voltage cathodes in high-energy-density ASSBs.
氟化物固态电解质（sse）具有优异的电化学稳定性，理论上是高压全固态电池（assb）的理想选择，但其低Li+导电性阻碍了实际应用。本研究利用聚阴离子配位策略，制备了一类具有高离子电导率和超高电压稳定性的氟化物ssi， LixTi(PO4)x/3F4。特别是，Li1.3Ti(PO4)1.3/3F4 （1.16 × 10−5 S cm−1）与类似的Li2TiF6相比，Li+电导率提高了两个数量级。实验和理论分析表明，LixTi(PO4)x/3F4的高离子电导率源于Li+周围相互作用的减弱和网络结构的柔性。引人注目的是，Li1.3Ti(PO4)1.3/3F4优异的离子电导率和超高电压稳定性使其具有低电阻和高度稳定的电解质-电极界面，在1℃和30℃下，5个v级lini0.5 mn1.5 o4基assb在200次循环后的容量保持率为91.6%。本工作的发现为设计高导电性氟化sbs开辟了新的途径，为高压阴极在高能量密度assb中的应用铺平了道路。
{"title":"Boosting ionic conductivity of fluoride electrolytes by polyanion coordination chemistry enabling 5 V-Class all-solid-state batteries","authors":"Huaimin Jin , Xingyu Wang , Simeng Zhang , Xiangzhen Zhu , Chong Liu , Junyi Yue , Jie Qu , Bei Wu , Xu Han , Yueyue Wang , Yang Xu , Han Wu , Liyu Zhou , Mingying Zhang , Hao Lai , Shuo Wang , Jiangwen Liang , Xueliang Sun , Xiaona Li","doi":"10.1016/j.joule.2025.102233","DOIUrl":"10.1016/j.joule.2025.102233","url":null,"abstract":"<div><div>Fluoride solid-state electrolytes (SSEs) offer superior electrochemical stability, making them theoretically ideal for high-voltage all-solid-state batteries (ASSBs), but their low Li<sup>+</sup> conductivity hinders practical application. Here, we exploit the polyanion coordination strategy to develop a class of fluoride SSEs, Li<sub><em>x</em></sub>Ti(PO<sub>4</sub>)<sub><em>x</em>/3</sub>F<sub>4</sub>, which exhibits high ionic conductivity and ultrahigh-voltage stability. Especially, Li<sub>1.3</sub>Ti(PO<sub>4</sub>)<sub>1.3/3</sub>F<sub>4</sub> (1.16 × 10<sup>−5</sup> S cm<sup>−1</sup>) demonstrates a two-order-of-magnitude enhancement in Li<sup>+</sup> conductivity compared to analogous Li<sub>2</sub>TiF<sub>6</sub>. Combined experimental and theoretical analyses reveal that the high ionic conductivity of Li<sub><em>x</em></sub>Ti(PO<sub>4</sub>)<sub><em>x</em>/3</sub>F<sub>4</sub> arises from weakened Li<sup>+</sup>-surrounding interactions and flexible network structures. Attractively, the exceptional ionic conductivity and ultrahigh-voltage stability of Li<sub>1.3</sub>Ti(PO<sub>4</sub>)<sub>1.3/3</sub>F<sub>4</sub> enable a low-resistance and highly stable electrolyte-electrode interface, contributing to 91.6% capacity retention after 200 cycles for 5 V-class LiNi<sub>0.5</sub>Mn<sub>1.5</sub>O<sub>4</sub>-based ASSBs at 1 C and 30°C. The discoveries in this work open a new avenue for designing high-conductivity fluoride SSEs, paving the way for the application of high-voltage cathodes in high-energy-density ASSBs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102233"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145785913","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102238
Christine Heume, Violeta Karyofylli, Ali Javed, Krzysztof Dzieciol, Shibabrata Basak, Jean-Pierre Poc, Yasemin Tasdemir, Yannik Rutsch, Lukas Rein, Niklas Wolf, Sebastian Speer, Sven Jovanovic, Leander Treutlein, Julian Borowec, Florian Hausen, Ladislaus Dobrenizki, Stephan Malmberg, Josef Granwehr, Hans Kungl, Eva Jodat, Rüdiger-A. Eichel
Proton exchange membrane electrolysis cells (PEMECs) are key to producing green hydrogen. The success of the green hydrogen economy depends on the technical maturity and scalability of water electrolysis systems. However, achieving energy-efficient and long-term operation requires a thorough understanding of aging mechanisms. While PEMECs have been extensively studied under laboratory conditions, data derived from industrial-scale operations are scarce.Our study addresses aging in an industry-oriented PEMEC operated under realistic conditions for 5,000 h, revealing systematic parasitic current pathways from cross-plane iridium filaments within the membrane, correlated with the anode/porous transport layer (PTL) interface. Experiments and computational models confirm that these parasitic currents do not impede system operation but do reduce system efficiency. This filament formation associated with the anode/PTL interface represents a hitherto unreported source of aging within PEMECs. Our findings will help optimize PEMEC design, effectively improving system performance and lifetime on an industrial scale, thus advancing the green hydrogen economy.
{"title":"Cross-plane iridium-based filaments sap efficiency in proton exchange membrane electrolyzers","authors":"Christine Heume, Violeta Karyofylli, Ali Javed, Krzysztof Dzieciol, Shibabrata Basak, Jean-Pierre Poc, Yasemin Tasdemir, Yannik Rutsch, Lukas Rein, Niklas Wolf, Sebastian Speer, Sven Jovanovic, Leander Treutlein, Julian Borowec, Florian Hausen, Ladislaus Dobrenizki, Stephan Malmberg, Josef Granwehr, Hans Kungl, Eva Jodat, Rüdiger-A. Eichel","doi":"10.1016/j.joule.2025.102238","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102238","url":null,"abstract":"Proton exchange membrane electrolysis cells (PEMECs) are key to producing green hydrogen. The success of the green hydrogen economy depends on the technical maturity and scalability of water electrolysis systems. However, achieving energy-efficient and long-term operation requires a thorough understanding of aging mechanisms. While PEMECs have been extensively studied under laboratory conditions, data derived from industrial-scale operations are scarce.Our study addresses aging in an industry-oriented PEMEC operated under realistic conditions for 5,000 h, revealing systematic parasitic current pathways from cross-plane iridium filaments within the membrane, correlated with the anode/porous transport layer (PTL) interface. Experiments and computational models confirm that these parasitic currents do not impede system operation but do reduce system efficiency. This filament formation associated with the anode/PTL interface represents a hitherto unreported source of aging within PEMECs. Our findings will help optimize PEMEC design, effectively improving system performance and lifetime on an industrial scale, thus advancing the green hydrogen economy.","PeriodicalId":343,"journal":{"name":"Joule","volume":"31 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005591","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102224
Tian Du , Hakan U. Dag , Zijian Peng , Jonas Englhard , Anastasia Barabash , Handan Zhang , Jiyun Zhang , Jiayi Tan , Shudi Qiu , Lirong Dong , Michael Wagner , Jens A. Hauch , Fei Guo , Olga Kasian , Julien Bachmann , Christoph J. Brabec
Printable rear electrodes represent a key enabling technology for the upscaling of perovskite solar cells (PSCs). Carbon electrodes are appealing candidates widely employed in n-i-p (so-called “conventional”) architectures, but their integration into p-i-n (so-called “inverted”) architectures is prohibited by interfacial energetic mismatch. We address this challenge by introducing a tin oxide (SnOx) interlayer with desirable mechanical durability and n-doping level. We show in detail how the tailored interlayer converts carbon from a hole-collecting anode to an electron-collecting cathode and how the electron-extraction barrier is minimized, narrowing the efficiency gap between carbon (21.8%) and silver (24.0%) electrodes. The advancement results in a remarkably improved viability of the PSCs: a modest drop in efficiency is outweighed by a 3-fold improvement in projected operational lifetime (>8,000 h) and a 60% reduction in the bill of materials. These results underscore the potential of carbon as a cost-effective alternative to silver in the industrialization of p-i-n PSCs.
{"title":"Enhancing the viability of p-i-n perovskite solar cells with printable carbon cathode: Origin of polarity inversion","authors":"Tian Du , Hakan U. Dag , Zijian Peng , Jonas Englhard , Anastasia Barabash , Handan Zhang , Jiyun Zhang , Jiayi Tan , Shudi Qiu , Lirong Dong , Michael Wagner , Jens A. Hauch , Fei Guo , Olga Kasian , Julien Bachmann , Christoph J. Brabec","doi":"10.1016/j.joule.2025.102224","DOIUrl":"10.1016/j.joule.2025.102224","url":null,"abstract":"<div><div>Printable rear electrodes represent a key enabling technology for the upscaling of perovskite solar cells (PSCs). Carbon electrodes are appealing candidates widely employed in n-i-p (so-called “conventional”) architectures, but their integration into p-i-n (so-called “inverted”) architectures is prohibited by interfacial energetic mismatch. We address this challenge by introducing a tin oxide (SnO<sub>x</sub>) interlayer with desirable mechanical durability and n-doping level. We show in detail how the tailored interlayer converts carbon from a hole-collecting anode to an electron-collecting cathode and how the electron-extraction barrier is minimized, narrowing the efficiency gap between carbon (21.8%) and silver (24.0%) electrodes. The advancement results in a remarkably improved viability of the PSCs: a modest drop in efficiency is outweighed by a 3-fold improvement in projected operational lifetime (>8,000 h) and a 60% reduction in the bill of materials. These results underscore the potential of carbon as a cost-effective alternative to silver in the industrialization of p-i-n PSCs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102224"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145689031","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102226
Juhyun Lee , Jinuk Kim , Wontae Jang , Dong Gyu Lee , Hongsin Kim , Yuha An , Junsu Son , Minjeong Kang , Gyuwon Lee , Jungyoon Lee , Donghyeok Son , Cheol-Young Park , Keonwoo Choi , Dongseok Shin , Tae Kyung Lee , Joonhee Moon , Sung Gap Im , Jinwoo Lee
Although anode-free lithium metal batteries (AFLMBs) offer exceptional energy density, they suffer from rapid capacity fading attributable to interfacial instability and the absence of a lithium reservoir. An interfacial solvation tuning strategy using ultrathin (∼15 nm) polymer coatings on Cu current collectors via initiated chemical vapor deposition is presented in this study. The designed polymer poly(heptadecafluorodecyl methacrylate) (pPFDMA) exhibits strong electrolyte- and solvent-phobicity, suppressing parasitic reactions and inducing local salt enrichment within the polymer. This solvation environment promotes a thin, inorganic-rich solid-electrolyte interphase layer and ensures high bulk ionic conductivity, enhancing both the cycling stability and rate capability. Consequently, pPFDMA-coated Cu enables a threefold improvement in the cycle life of half-cells and achieves 413 Wh kg−1 and 826 W kg−1 in LiNi0.8Co0.1Mn0.1O2 (NCM811)-based anode-free pouch cells. This work provides a practical and generalizable approach for interfacial engineering in AFLMBs, focusing on current collector-electrolyte interactions.
尽管无阳极锂金属电池（aflmb）具有优异的能量密度，但由于界面不稳定和缺乏锂储层，它们的容量会迅速衰减。本研究提出了一种通过化学气相沉积在Cu集热器上使用超薄（~ 15 nm）聚合物涂层的界面溶剂化调谐策略。所设计的聚合物聚甲基丙烯酸十六氟癸酯（pPFDMA）具有很强的电解质和溶剂疏水性，可以抑制寄生反应并诱导聚合物内部的局部盐富集。这种溶剂化环境促进了薄的、无机丰富的固体电解质间相层，并确保了高体积离子电导率，增强了循环稳定性和速率能力。因此，ppfdma涂层Cu使半电池的循环寿命提高了三倍，在LiNi0.8Co0.1Mn0.1O2 （NCM811）基无阳极袋状电池中达到413 Wh kg - 1和826 W kg - 1。这项工作为aflmb的界面工程提供了一种实用和可推广的方法，重点是电流集电极-电解质相互作用。
{"title":"A strategic tuning of interfacial Li+ solvation with ultrathin polymer layers for anode-free lithium metal batteries","authors":"Juhyun Lee , Jinuk Kim , Wontae Jang , Dong Gyu Lee , Hongsin Kim , Yuha An , Junsu Son , Minjeong Kang , Gyuwon Lee , Jungyoon Lee , Donghyeok Son , Cheol-Young Park , Keonwoo Choi , Dongseok Shin , Tae Kyung Lee , Joonhee Moon , Sung Gap Im , Jinwoo Lee","doi":"10.1016/j.joule.2025.102226","DOIUrl":"10.1016/j.joule.2025.102226","url":null,"abstract":"<div><div>Although anode-free lithium metal batteries (AFLMBs) offer exceptional energy density, they suffer from rapid capacity fading attributable to interfacial instability and the absence of a lithium reservoir. An interfacial solvation tuning strategy using ultrathin (∼15 nm) polymer coatings on Cu current collectors via initiated chemical vapor deposition is presented in this study. The designed polymer poly(heptadecafluorodecyl methacrylate) (pPFDMA) exhibits strong electrolyte- and solvent-phobicity, suppressing parasitic reactions and inducing local salt enrichment within the polymer. This solvation environment promotes a thin, inorganic-rich solid-electrolyte interphase layer and ensures high bulk ionic conductivity, enhancing both the cycling stability and rate capability. Consequently, pPFDMA-coated Cu enables a threefold improvement in the cycle life of half-cells and achieves 413 Wh kg<sup>−1</sup> and 826 W kg<sup>−1</sup> in LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811)-based anode-free pouch cells. This work provides a practical and generalizable approach for interfacial engineering in AFLMBs, focusing on current collector-electrolyte interactions.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102226"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145711427","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102235
B. Edward Sartor , Samantha B. Reese , Lorelle M. Mansfield , Ryan Muzzio , Chun-Sheng Jiang , Eric Colegrove , John S. Mangum , Camden L. Kasik , Daniel Z. Shaw , James R. Sites , Ramesh G. Dhere , Alex B. Goldstone , Michael S. Moats , Lana Alagha , Chungho Lee , Dingyuan Lu , Gang Xiong , Rouin Farshchi , Jialiu Ma , Timothy Nagle , Michael J. Heben
This roadmap highlights pathways to expand the CdTe module manufacturing capacity per year to 100 GWDC by 2030 by improving Te extraction from existing supply chains, minimizing Te usage in modules by leveraging thinner absorbers, and focusing research efforts in key areas to improve module efficiencies. Both scientific and supply chain innovations will be necessary to maintain the high compound annual growth rate of the CdTe photovoltaic (PV) industry and cement its role as a key technology for multi-TW-scale PV deployment.
{"title":"Roadmap to 100 GWDC: Scientific and supply chain challenges for CdTe photovoltaics","authors":"B. Edward Sartor , Samantha B. Reese , Lorelle M. Mansfield , Ryan Muzzio , Chun-Sheng Jiang , Eric Colegrove , John S. Mangum , Camden L. Kasik , Daniel Z. Shaw , James R. Sites , Ramesh G. Dhere , Alex B. Goldstone , Michael S. Moats , Lana Alagha , Chungho Lee , Dingyuan Lu , Gang Xiong , Rouin Farshchi , Jialiu Ma , Timothy Nagle , Michael J. Heben","doi":"10.1016/j.joule.2025.102235","DOIUrl":"10.1016/j.joule.2025.102235","url":null,"abstract":"<div><div>This roadmap highlights pathways to expand the CdTe module manufacturing capacity per year to 100 GW<sub>DC</sub> by 2030 by improving Te extraction from existing supply chains, minimizing Te usage in modules by leveraging thinner absorbers, and focusing research efforts in key areas to improve module efficiencies. Both scientific and supply chain innovations will be necessary to maintain the high compound annual growth rate of the CdTe photovoltaic (PV) industry and cement its role as a key technology for multi-TW-scale PV deployment.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102235"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145785912","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102234
Jinhui Li , Lanbin Wang , Beikai Zhang , Duanmei Song , Jiadong Yu
Conventional mixing-then-separating recycling processes struggle with emerging urban minerals containing chemically akin metals because the resulting high-entropy mixtures become kinetically trapped against separation. This work introduces an atomic-scale low-entropy-increasing strategy for selective gallium (Ga) recovery from end-of-life Cu(In,Ga)Se2 (CIGS) photovoltaics. The process integrates mechanochemical molten-salt extraction with water leaching, delivering 96.08% Ga recovery with a Ga/indium (In) separation factor of 88.89, which is ∼35 times higher than existing metallurgical benchmarks. Mechanistic investigations reveal that mechanochemical polarization selectively cleaves Ga–selenium (Se) bonds (3.01 eV) over copper (Cu)–Se (4.33 eV) and In–Se (4.47 eV), dissolving Ga as Ga(OH)4− complexes while retaining CuInSe2 solids with intact CIGS configuration. Compared with other CIGS recycling methods, this entropy-minimizing lattice-topology-conversion strategy slashes carbon emissions, water consumption, and fossil fuel demand by 70.32%–86.94%, 87.72%–92.00%, and 62.91%–81.45%, respectively. Overall, we establish a scalable metallurgical design for critical metal recovery in urban mining, advancing the circular economy.
{"title":"Mechanochemical extraction of gallium from chemically akin metal mixtures via an atomic-scale low-entropy-increasing strategy","authors":"Jinhui Li , Lanbin Wang , Beikai Zhang , Duanmei Song , Jiadong Yu","doi":"10.1016/j.joule.2025.102234","DOIUrl":"10.1016/j.joule.2025.102234","url":null,"abstract":"<div><div>Conventional mixing-then-separating recycling processes struggle with emerging urban minerals containing chemically akin metals because the resulting high-entropy mixtures become kinetically trapped against separation. This work introduces an atomic-scale low-entropy-increasing strategy for selective gallium (Ga) recovery from end-of-life Cu(In,Ga)Se<sub>2</sub> (CIGS) photovoltaics. The process integrates mechanochemical molten-salt extraction with water leaching, delivering 96.08% Ga recovery with a Ga/indium (In) separation factor of 88.89, which is ∼35 times higher than existing metallurgical benchmarks. Mechanistic investigations reveal that mechanochemical polarization selectively cleaves Ga–selenium (Se) bonds (3.01 eV) over copper (Cu)–Se (4.33 eV) and In–Se (4.47 eV), dissolving Ga as Ga(OH)<sub>4</sub><sup>−</sup> complexes while retaining CuInSe<sub>2</sub> solids with intact CIGS configuration. Compared with other CIGS recycling methods, this entropy-minimizing lattice-topology-conversion strategy slashes carbon emissions, water consumption, and fossil fuel demand by 70.32%–86.94%, 87.72%–92.00%, and 62.91%–81.45%, respectively. Overall, we establish a scalable metallurgical design for critical metal recovery in urban mining, advancing the circular economy.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102234"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145785923","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102308
Lei Shi , Huiyuan Zhu
In a recent issue of Nature Materials, Ma et al. introduce a ligand-constrained strategy for synthesizing highly paired dual-atom catalysts. By coordinating metal centers with diamine ligands of tunable lengths, they achieved a pairing ratio exceeding 80%, precisely controlled interatomic distance, and enhanced catalytic activity for electrochemical nitrate reduction reaction.
{"title":"Ligand rulers dictate atomic pairing and geometry of dual-atom catalysts","authors":"Lei Shi , Huiyuan Zhu","doi":"10.1016/j.joule.2025.102308","DOIUrl":"10.1016/j.joule.2025.102308","url":null,"abstract":"<div><div>In a recent issue of <em>Nature Materials</em>, Ma et al. introduce a ligand-constrained strategy for synthesizing highly paired dual-atom catalysts. By coordinating metal centers with diamine ligands of tunable lengths, they achieved a pairing ratio exceeding 80%, precisely controlled interatomic distance, and enhanced catalytic activity for electrochemical nitrate reduction reaction.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102308"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146006713","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}
Pub Date : 2026-01-21DOI: 10.1016/j.joule.2025.102269
Seongjae Ko , Makoto Ue , Atsuo Yamada
Seongjae Ko worked as a senior researcher at Samsung SDI in South Korea from 2012 to 2015. He joined Professor Yamada’s group as an academic support specialist in 2015. From 2017 to 2020, he worked as a DC1 research fellow at the Japan Society for the Promotion of Science. He received his PhD from the University of Tokyo in 2020. Since 2021, he has served as an assistant professor at the University of Tokyo and was later promoted to lecturer. Further details are available at https://orcid.org/0000-0001-6163-7687.
Makoto Ue obtained his MS and PhD from The University of Tokyo in 1981 and 1995, respectively, and studied at the University of Pittsburgh and Lawrence Berkeley National Laboratory from 1988 to 1990. He worked for Mitsubishi Chemical from 1981 to 2012 (fellow), Samsung SDI as a vice president from 2012 to 2018, National Institute for Materials Science as a special researcher from 2019 to 2020, and Waseda University as a guest professor since 2022. He was awarded eight awards including the Achievement Award from ECSJ (2022), the Battery Division Technology Award from ECS (2004), and the Research Award from IBA (1997).
Atsuo Yamada has had a unique career in both academic and industrial research. After serving as the laboratory head of the Sony Research Center, he was appointed as associate professor at the Tokyo Institute of Technology in 2002, and as full professor at the University of Tokyo in 2009. He has been awarded the Spriggs Award (2010) and the Purdy Award (2016) by ACerS, the Scientific Achievement Award (2016) by ECSJ, Research Award (2016) from IBA, the Battery Division Research Award (2022) from ECS, Science & Technology Award (2023) from MEXT minister, and Clarivate Highly Cited Researcher (2019, 2025).
{"title":"A critical outlook for large-scale all-solid-state batteries","authors":"Seongjae Ko , Makoto Ue , Atsuo Yamada","doi":"10.1016/j.joule.2025.102269","DOIUrl":"10.1016/j.joule.2025.102269","url":null,"abstract":"<div><div>Seongjae Ko worked as a senior researcher at Samsung SDI in South Korea from 2012 to 2015. He joined Professor Yamada’s group as an academic support specialist in 2015. From 2017 to 2020, he worked as a DC1 research fellow at the Japan Society for the Promotion of Science. He received his PhD from the University of Tokyo in 2020. Since 2021, he has served as an assistant professor at the University of Tokyo and was later promoted to lecturer. Further details are available at <span><span>https://orcid.org/0000-0001-6163-7687</span><svg><path></path></svg></span>.</div><div>Makoto Ue obtained his MS and PhD from The University of Tokyo in 1981 and 1995, respectively, and studied at the University of Pittsburgh and Lawrence Berkeley National Laboratory from 1988 to 1990. He worked for Mitsubishi Chemical from 1981 to 2012 (fellow), Samsung SDI as a vice president from 2012 to 2018, National Institute for Materials Science as a special researcher from 2019 to 2020, and Waseda University as a guest professor since 2022. He was awarded eight awards including the Achievement Award from ECSJ (2022), the Battery Division Technology Award from ECS (2004), and the Research Award from IBA (1997).</div><div>Atsuo Yamada has had a unique career in both academic and industrial research. After serving as the laboratory head of the Sony Research Center, he was appointed as associate professor at the Tokyo Institute of Technology in 2002, and as full professor at the University of Tokyo in 2009. He has been awarded the Spriggs Award (2010) and the Purdy Award (2016) by ACerS, the Scientific Achievement Award (2016) by ECSJ, Research Award (2016) from IBA, the Battery Division Research Award (2022) from ECS, Science & Technology Award (2023) from MEXT minister, and Clarivate Highly Cited Researcher (2019, 2025).</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 1","pages":"Article 102269"},"PeriodicalIF":35.4,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145938137","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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