Pub Date : 2026-02-18Epub Date: 2025-12-31DOI: 10.1016/j.joule.2025.102236
Xiao Li , Rebecca R. Hernandez , Alona Armstrong , Pan Liu , Sarah M. Jordaan
Global energy transitions with high growth in solar photovoltaics must consider land consequences and economics to align with sustainability goals. We quantify a capacity-weighted average value of land-use efficiency (LUE) as 57 (37–62, 25th–75th percentile) W/m2, and lifetime land transformation (LTL) as 409 (300–537) m2/GWh for all large, ground-mounted photovoltaic (G-PV) plants globally. Asia Pacific had a 15% higher LUE (and a 21% lower LT) compared with other regions. High growth in solar is anticipated to impact only 0.1%–0.2% of the global land mass by 2050. Results inform comparisons of levelized costs and capital expenditures of rooftop (land-sparing) vs. large, ground-mounted (land-intensive) PV solar energy buildouts by country and region. Substituting land-intensive with land-sparing PV buildouts is most expensive in the United States ($950–1,030/kW by 2050) and cheapest in Brazil ($−70 – −60/kW, by 2050). Results point to the need to determine economic implications of global land-sparing opportunities and enact policies to support local implementation.
{"title":"Global land and solar energy relationships for sustainability","authors":"Xiao Li , Rebecca R. Hernandez , Alona Armstrong , Pan Liu , Sarah M. Jordaan","doi":"10.1016/j.joule.2025.102236","DOIUrl":"10.1016/j.joule.2025.102236","url":null,"abstract":"<div><div>Global energy transitions with high growth in solar photovoltaics must consider land consequences and economics to align with sustainability goals. We quantify a capacity-weighted average value of land-use efficiency (LUE) as 57 (37–62, 25<sup>th</sup>–75<sup>th</sup> percentile) W/m<sup>2</sup>, and lifetime land transformation (LT<sub>L</sub>) as 409 (300–537) m<sup>2</sup>/GWh for all large, ground-mounted photovoltaic (G-PV) plants globally. Asia Pacific had a 15% higher LUE (and a 21% lower LT) compared with other regions. High growth in solar is anticipated to impact only 0.1%–0.2% of the global land mass by 2050. Results inform comparisons of levelized costs and capital expenditures of rooftop (land-sparing) vs. large, ground-mounted (land-intensive) PV solar energy buildouts by country and region. Substituting land-intensive with land-sparing PV buildouts is most expensive in the United States ($950–1,030/kW by 2050) and cheapest in Brazil ($−70 – −60/kW, by 2050). Results point to the need to determine economic implications of global land-sparing opportunities and enact policies to support local implementation.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102236"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895734","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 : 2026-02-18Epub Date: 2026-01-21DOI: 10.1016/j.joule.2025.102265
Elizabeth Dach , Juliana Marston , Sara Abu-Obaid , Allison Peng , Ngai Yin Yip
This study presents a proof-of-concept for switchable solvent selective extraction (S3E) for direct lithium extraction from brines. S3E utilizes an amine solvent with thermally switchable hydrophilicity to extract Li+ and water from the brine, and a modest temperature swing toggles the solvent to its hydrophobic state, releasing a purified lithium product stream and regenerating the solvent. S3E demonstrated a consistent preference for lithium across amines with different chemical structures, achieving Li+/Na+ selectivities as high as ≈10. The selectivity for lithium was maintained even when challenged with Li+ concentrations 1,000× lower than Na+ or K+, whereas Li+/Na+ and Li+/K+ selectivities for a simulated Salton Sea geothermal brine are ≈13 and ≈24, respectively, with magnesium completely removed as Mg(OH)2 precipitates due to the basicity of the amine solvent. Furthermore, repeated semibatch extraction cycles reusing the solvent demonstrated practical Li+ recovery yields (40% after four cycles) and solvent regenerability while preserving selectivity.
{"title":"A novel approach for direct lithium extraction from alkali metal cations in brine mixtures using thermally switchable solvents","authors":"Elizabeth Dach , Juliana Marston , Sara Abu-Obaid , Allison Peng , Ngai Yin Yip","doi":"10.1016/j.joule.2025.102265","DOIUrl":"10.1016/j.joule.2025.102265","url":null,"abstract":"<div><div>This study presents a proof-of-concept for switchable solvent selective extraction (S<sup>3</sup>E) for direct lithium extraction from brines. S<sup>3</sup>E utilizes an amine solvent with thermally switchable hydrophilicity to extract Li<sup>+</sup> and water from the brine, and a modest temperature swing toggles the solvent to its hydrophobic state, releasing a purified lithium product stream and regenerating the solvent. S<sup>3</sup>E demonstrated a consistent preference for lithium across amines with different chemical structures, achieving Li<sup>+</sup>/Na<sup>+</sup> selectivities as high as ≈10. The selectivity for lithium was maintained even when challenged with Li<sup>+</sup> concentrations 1,000× lower than Na<sup>+</sup> or K<sup>+</sup>, whereas Li<sup>+</sup>/Na<sup>+</sup> and Li<sup>+</sup>/K<sup>+</sup> selectivities for a simulated Salton Sea geothermal brine are ≈13 and ≈24, respectively, with magnesium completely removed as Mg(OH)<sub>2</sub> precipitates due to the basicity of the amine solvent. Furthermore, repeated semibatch extraction cycles reusing the solvent demonstrated practical Li<sup>+</sup> recovery yields (40% after four cycles) and solvent regenerability while preserving selectivity.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102265"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146014742","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 : 2026-02-18DOI: 10.1016/j.joule.2026.102321
Eleonora Isotta , Alexandra Zevalkink
In a recent Advanced Energy Materials article, authors Wang et al. describe a new concept for optimizing the performance of skutterudites by combining electronegative fillers and compensation doping, leading to extremely low thermal conductivity for this class of materials and high thermoelectric performance.
{"title":"Chemical compensation meets bond engineering in skutterudites","authors":"Eleonora Isotta , Alexandra Zevalkink","doi":"10.1016/j.joule.2026.102321","DOIUrl":"10.1016/j.joule.2026.102321","url":null,"abstract":"<div><div>In a recent <em>Advanced Energy Materials</em> article, authors Wang et al. describe a new concept for optimizing the performance of skutterudites by combining electronegative fillers and compensation doping, leading to extremely low thermal conductivity for this class of materials and high thermoelectric performance.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102321"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146778038","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}
Lithium-sulfur all-solid-state batteries (Li-S ASSBs) offer ultrahigh specific capacity and enhanced safety but are hindered by low cathode-level energy density. Simulations reveal that intra-agglomerate mass-transport limitations in bulk sulfur represent the primary challenge. To address this, we propose an “active material (AM)-free” design using a cathode composed solely of Li6PS5Cl (LPSCl) and carbon, where AMs form in situ via electrolyte decomposition. The resulting submicron-scale AMs overcome mass-transport limitations through shortened diffusion paths. By expanding LPSCl-carbon interfaces, this cathode exhibits high cathode-level energy density. The self-limiting AM growth prevents excessive degradation, ensuring cycling stability (95% retention after 500 cycles at 50°C). Subsequent optimization with LiI additive further elevates cathode-level energy density to 1,277.8 Wh kg−1 (9.25 mAh cm−2) and extends cycle life to 767 cycles at room temperature (RT). This work provides a promising approach to designing high-performance cathodes by exploiting the redox activity of the solid electrolyte.
锂硫全固态电池（li -硫全固态电池）具有超高的比容量和更高的安全性，但受到低阴极能级能量密度的阻碍。模拟表明，块状硫的团块内部质量传输限制是主要的挑战。为了解决这个问题，我们提出了一种“无活性材料（AM）”设计，使用仅由Li6PS5Cl （LPSCl）和碳组成的阴极，其中AMs通过电解质分解在原位形成。由此产生的亚微米级AMs通过缩短扩散路径克服了质量输运的限制。通过扩展lpscl -碳界面，该阴极具有较高的阴极能级能量密度。自限制AM生长防止过度降解，确保循环稳定性（在50°C下500次循环后保持95%）。随后使用LiI添加剂进行优化，进一步将阴极能级能量密度提高到1,277.8 Wh kg - 1 (9.25 mAh cm - 2)，并将室温下的循环寿命延长到767次。这项工作为利用固体电解质的氧化还原活性来设计高性能阴极提供了一种有前途的方法。
{"title":"“Active material-free” design to overcome mass-transport limitations for high-energy-density all-solid-state Li-S batteries","authors":"Zhengcheng Gu , Shengfu Wei , Xing Zhang , Weigang Ma","doi":"10.1016/j.joule.2025.102239","DOIUrl":"10.1016/j.joule.2025.102239","url":null,"abstract":"<div><div>Lithium-sulfur all-solid-state batteries (Li-S ASSBs) offer ultrahigh specific capacity and enhanced safety but are hindered by low cathode-level energy density. Simulations reveal that intra-agglomerate mass-transport limitations in bulk sulfur represent the primary challenge. To address this, we propose an “active material (AM)-free” design using a cathode composed solely of Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) and carbon, where AMs form <em>in situ</em> via electrolyte decomposition. The resulting submicron-scale AMs overcome mass-transport limitations through shortened diffusion paths. By expanding LPSCl-carbon interfaces, this cathode exhibits high cathode-level energy density. The self-limiting AM growth prevents excessive degradation, ensuring cycling stability (95% retention after 500 cycles at 50°C). Subsequent optimization with LiI additive further elevates cathode-level energy density to 1,277.8 Wh kg<sup>−1</sup> (9.25 mAh cm<sup>−2</sup>) and extends cycle life to 767 cycles at room temperature (RT). This work provides a promising approach to designing high-performance cathodes by exploiting the redox activity of the solid electrolyte.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102239"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995965","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 : 2026-02-18Epub Date: 2026-01-26DOI: 10.1016/j.joule.2025.102262
Jung Hwan Lee , Yu Jin Lee , Hyungju Ahn , Jeong Eun Park , Ryan Rhee , Yonghyun Albert Kwon , Taehee Kim , Jeong Ho Cho , Ji-Sang Park , Dongho Kim , Jong Hyeok Park
Being placed near the perovskite grain boundaries, pyrene molecules reduce PbI6 octahedral tilting by controlling the orientations of the formamidinium (FA) cations within the lattice. Pyrene treatment immobilizes FA cations, reduces octahedral tilting, prevents their uncontrolled loss during film formation, and promotes the formation of pure α-formamidinium lead triiodide (FAPbI3). Using confocal fluorescence lifetime imaging microscopy (FLIM), we observed reduced electron-phonon coupling and a uniform spatioenergetic landscape, indicating enhanced structural rigidity of FAPbI3. Additionally, direct visualization of the exciton transport process revealed the significance of the stabilized octahedral cage for the carrier transport process. Consequently, we achieved a remarkable power conversion efficiency of 25.7% (certified 25.64%). The devices exhibited outstanding intrinsic stability, retaining over 94% of their initial current with encapsulation for over 3,400 h, while the unencapsulated devices also maintained over 90% for 2,000 h.
{"title":"Stabilizing α-FAPbI3 perovskite via centered formamidinium cation immobilization","authors":"Jung Hwan Lee , Yu Jin Lee , Hyungju Ahn , Jeong Eun Park , Ryan Rhee , Yonghyun Albert Kwon , Taehee Kim , Jeong Ho Cho , Ji-Sang Park , Dongho Kim , Jong Hyeok Park","doi":"10.1016/j.joule.2025.102262","DOIUrl":"10.1016/j.joule.2025.102262","url":null,"abstract":"<div><div>Being placed near the perovskite grain boundaries, pyrene molecules reduce PbI<sub>6</sub> octahedral tilting by controlling the orientations of the formamidinium (FA) cations within the lattice. Pyrene treatment immobilizes FA cations, reduces octahedral tilting, prevents their uncontrolled loss during film formation, and promotes the formation of pure α-formamidinium lead triiodide (FAPbI<sub>3</sub>). Using confocal fluorescence lifetime imaging microscopy (FLIM), we observed reduced electron-phonon coupling and a uniform spatioenergetic landscape, indicating enhanced structural rigidity of FAPbI<sub>3</sub>. Additionally, direct visualization of the exciton transport process revealed the significance of the stabilized octahedral cage for the carrier transport process. Consequently, we achieved a remarkable power conversion efficiency of 25.7% (certified 25.64%). The devices exhibited outstanding intrinsic stability, retaining over 94% of their initial current with encapsulation for over 3,400 h, while the unencapsulated devices also maintained over 90% for 2,000 h.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102262"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048637","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 : 2026-02-18Epub Date: 2026-01-29DOI: 10.1016/j.joule.2025.102267
Yufeng Liu , Kai Wan , Zhipeng Xiang , Zhiyong Fu , Yuan Li , Mingbao Huang , Yi-Chun Lu , Shang-Da Jiang , Zhenxing Liang
Aqueous organic redox flow batteries (AORFBs) are promising for safe and sustainable long-duration energy storage but suffer from the oxygen sensitivity of reduced-state negolyte species, which limits coulombic efficiency and cycling stability. Here, we develop a kinetic strategy to achieve full-cycle oxygen tolerance through the construction of folda-dimer. The folded conformation weakens the electronic coupling between the reduced-state molecule and oxygen, lowering the observed rate constant by two orders of magnitude compared with monomeric analogues. Moreover, this folded structure endows the system with concentration-independent characteristics, yielding full-cycle oxygen tolerance. As demonstrated, the AORFB with the bis-viologen negolyte shows a high capacity of 46.5 Ah L−1, high coulombic efficiency of 99.9%, and superior cyclability (capacity retention rate of 99.96% per day in the configuration with 30% excess posolyte and 99.46% per day in the charge-balanced configuration) under air. This study establishes a kinetic stabilization paradigm for developing oxygen-tolerant electroactive organics of AORFBs.
{"title":"Full-cycle oxygen-tolerant organic flow batteries","authors":"Yufeng Liu , Kai Wan , Zhipeng Xiang , Zhiyong Fu , Yuan Li , Mingbao Huang , Yi-Chun Lu , Shang-Da Jiang , Zhenxing Liang","doi":"10.1016/j.joule.2025.102267","DOIUrl":"10.1016/j.joule.2025.102267","url":null,"abstract":"<div><div>Aqueous organic redox flow batteries (AORFBs) are promising for safe and sustainable long-duration energy storage but suffer from the oxygen sensitivity of reduced-state negolyte species, which limits coulombic efficiency and cycling stability. Here, we develop a kinetic strategy to achieve full-cycle oxygen tolerance through the construction of folda-dimer. The folded conformation weakens the electronic coupling between the reduced-state molecule and oxygen, lowering the observed rate constant by two orders of magnitude compared with monomeric analogues. Moreover, this folded structure endows the system with concentration-independent characteristics, yielding full-cycle oxygen tolerance. As demonstrated, the AORFB with the bis-viologen negolyte shows a high capacity of 46.5 Ah L<sup>−1</sup>, high coulombic efficiency of 99.9%, and superior cyclability (capacity retention rate of 99.96% per day in the configuration with 30% excess posolyte and 99.46% per day in the charge-balanced configuration) under air. This study establishes a kinetic stabilization paradigm for developing oxygen-tolerant electroactive organics of AORFBs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102267"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146071897","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 : 2026-02-18Epub Date: 2026-02-03DOI: 10.1016/j.joule.2025.102306
Wenyu An , Yu Zhong , Liang Luo , Daojin Zhou , Xiaoming Sun
Green hydrogen production and utilization represent a promising carbon-neutral energy strategy, basically being categorized into alkaline, anion-exchange membrane, and proton exchange membrane electrolysis according to the types of electrolytes. Apart from the optimization of intrinsic activity of catalysts, electrolyte engineering has become an emerging and effective approach. Aiming to get deeper insights into the electrode-electrolyte interface, this perspective highlights two primary mechanisms: restructuring of hydrogen-bond networks that govern reactant transport and modulation of intermediate adsorption through hydration layers or electrostatic interactions. Electrolyte effects are systematically discussed across key reactions involved in hydrogen energy production and utilization, including the two half-reactions of water electrolysis, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), as well as the two half-reactions in fuel cells (FCs), hydrogen oxidation reaction (HOR) and oxygen reduction reaction (ORR). We conclude by outlining strategic opportunities to leverage ion-mediated effects through electrolyte engineering, offering guidance toward more efficient, selective, and durable electrocatalytic systems for future energy conversion.
{"title":"Electrolyte engineering for hydrogen energy","authors":"Wenyu An , Yu Zhong , Liang Luo , Daojin Zhou , Xiaoming Sun","doi":"10.1016/j.joule.2025.102306","DOIUrl":"10.1016/j.joule.2025.102306","url":null,"abstract":"<div><div>Green hydrogen production and utilization represent a promising carbon-neutral energy strategy, basically being categorized into alkaline, anion-exchange membrane, and proton exchange membrane electrolysis according to the types of electrolytes. Apart from the optimization of intrinsic activity of catalysts, electrolyte engineering has become an emerging and effective approach. Aiming to get deeper insights into the electrode-electrolyte interface, this perspective highlights two primary mechanisms: restructuring of hydrogen-bond networks that govern reactant transport and modulation of intermediate adsorption through hydration layers or electrostatic interactions. Electrolyte effects are systematically discussed across key reactions involved in hydrogen energy production and utilization, including the two half-reactions of water electrolysis, hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), as well as the two half-reactions in fuel cells (FCs), hydrogen oxidation reaction (HOR) and oxygen reduction reaction (ORR). We conclude by outlining strategic opportunities to leverage ion-mediated effects through electrolyte engineering, offering guidance toward more efficient, selective, and durable electrocatalytic systems for future energy conversion.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102306"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101522","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 : 2026-02-18Epub Date: 2026-01-20DOI: 10.1016/j.joule.2025.102237
Jiajia Hong , Xuntian Zheng , Haowen Luo , Bowen Yang , Jiajia Suo , Xinrui Han , Zijing Chu , Lu Zhao , Hongfei Sun , Shuncheng Yang , Yijia Guo , Jinyan Guo , Wennan Ou , Enzuo Wang , Anh Dinh Bui , Khoa Nguyen , Daniel MacDonald , Renxing Lin , Wenchi Kong , Hairen Tan
Scalable fabrication of wide-band-gap perovskite sub-cells under ambient conditions is essential for commercial perovskite/silicon tandem photovoltaics. However, uncontrolled ambient moisture renders crystallization unmanageable and triggers irreversible surface decomposition. To address this, we innovate a wet-film intervention strategy using bifunctional n-butylammonium thiocyanate (nBASCN) to regulate perovskite crystallization and mitigate the adverse impact of moisture. The strategic incorporation of SCN− into wet films enables homogeneous secondary grain growth with enhanced crystallinity and grain size by decoupling the crystallization process from environmental humidity. Optimally tailored nBA+ cations balance hydrophobicity with SCN−-assisted crystallization, constructing a self-volatile 2D hydrophobic barrier that effectively suppresses moisture-induced surface degradation without compromising charge transport. As a result, we achieved a remarkable efficiency of 30.71% (certified 30.51%) for perovskite/silicon tandem devices (1.1664 cm2) and 29.09% for large-area tandem devices (16 cm2), representing the highest efficiency of perovskite/silicon tandem solar cells via scalable fabrication in ambient air.
{"title":"Scalable ambient fabrication of perovskite/silicon tandem solar cells via wet-film intervention","authors":"Jiajia Hong , Xuntian Zheng , Haowen Luo , Bowen Yang , Jiajia Suo , Xinrui Han , Zijing Chu , Lu Zhao , Hongfei Sun , Shuncheng Yang , Yijia Guo , Jinyan Guo , Wennan Ou , Enzuo Wang , Anh Dinh Bui , Khoa Nguyen , Daniel MacDonald , Renxing Lin , Wenchi Kong , Hairen Tan","doi":"10.1016/j.joule.2025.102237","DOIUrl":"10.1016/j.joule.2025.102237","url":null,"abstract":"<div><div>Scalable fabrication of wide-band-gap perovskite sub-cells under ambient conditions is essential for commercial perovskite/silicon tandem photovoltaics. However, uncontrolled ambient moisture renders crystallization unmanageable and triggers irreversible surface decomposition. To address this, we innovate a wet-film intervention strategy using bifunctional n-butylammonium thiocyanate (nBASCN) to regulate perovskite crystallization and mitigate the adverse impact of moisture. The strategic incorporation of SCN<sup>−</sup> into wet films enables homogeneous secondary grain growth with enhanced crystallinity and grain size by decoupling the crystallization process from environmental humidity. Optimally tailored nBA<sup>+</sup> cations balance hydrophobicity with SCN<sup>−</sup>-assisted crystallization, constructing a self-volatile 2D hydrophobic barrier that effectively suppresses moisture-induced surface degradation without compromising charge transport. As a result, we achieved a remarkable efficiency of 30.71% (certified 30.51%) for perovskite/silicon tandem devices (1.1664 cm<sup>2</sup>) and 29.09% for large-area tandem devices (16 cm<sup>2</sup>), representing the highest efficiency of perovskite/silicon tandem solar cells via scalable fabrication in ambient air.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"10 2","pages":"Article 102237"},"PeriodicalIF":35.4,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005762","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 : 2026-02-18DOI: 10.1016/j.joule.2025.102278
Ao Jia, Wanjie Gao, Jie Wang, Xinying Wang, Xi Liu, Guangyu Pan, Yang Liu, Xinghao Zhang, Tianhan Huang, Yuping Wu, Jiarui He
Lithium plating in graphite anodes, caused by surface lithium congestion, hampers lithium-ion battery performance. Here, we introduce a concentration-gradient-driven force to improve lithium solid diffusion in graphite. Sulfurized polyacrylonitrile (SPAN) is selected as a modulator to tailor the interfacial lithium concentration via the in situ formation of SPAN over graphite (Gr@SPAN). SPAN induces a pronounced concentration gradient between the surface and the interior, initiating an accelerated solid diffusion process inside graphite. Such an accelerated solid diffusion process results in suppressed lithium plating and superior lithium storage of graphite itself with an ultrahigh capacity of ∼392 mAh g−1 of Gr@SPAN, exceeding the theoretical capacity of graphite (372 mAh g−1). Furthermore, the Gr@SPAN anode achieves a specific capacity of ∼357 mAh g−1 after 700 cycles, with a remarkable capacity retention of 91.3% at 1 C. This multifunctional interface based on the concentration-gradient-driven force paves a new way to fabricate advanced graphite anodes.
在石墨阳极上镀锂，由于表面锂堵塞，会影响锂离子电池的性能。在这里，我们引入了浓度梯度驱动力来改善锂固体在石墨中的扩散。选择硫化聚丙烯腈（SPAN）作为调制剂，通过在石墨上原位形成SPAN来调整界面锂浓度（Gr@SPAN）。SPAN在石墨表面和内部之间产生了明显的浓度梯度，加速了石墨内部的固体扩散过程。这种加速的固体扩散过程抑制了锂的电镀，石墨本身具有优异的锂存储能力，其容量高达Gr@SPAN的~ 392 mAh g−1，超过了石墨的理论容量（372 mAh g−1）。此外，Gr@SPAN阳极在700次循环后达到了~ 357 mAh g−1的比容量，在1℃下具有91.3%的显着容量保持率。这种基于浓度梯度驱动力的多功能界面为制造先进的石墨阳极铺平了新途径。
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Pub Date : 2026-02-18DOI: 10.1016/j.joule.2025.102297
Qihang Yu, Yang Hu, Sixu Deng, Mohsen Shakouri, Graham King, Lo-Yueh Chang, Karim Zaghib, Tsun-Kong Sham, Xia Li
All-solid-state batteries (ASSBs) can prevent the dissolution of sustainable organic electrode materials (OEMs) in liquid electrolytes, but their practical implementation is limited by the low energy density arising from interfacial reactions between OEMs and solid electrolytes (SEs). Here, we show that controlled interfacial chemistry between OEMs and sulfide SEs can instead activate reversible S2− anionic redox, enabling an electrode-level energy density of 477 Wh kg−1 and stable cycling for over 2,000 cycles at room temperature. Mechanistic analysis identifies two key criteria for effective OEM-catalyzed S2− anionic redox: (1) a moderate OEM electrode potential sufficient to oxidize S2− without over-oxidation and (2) low cation–S2− bond covalency, localizing electron density on S atoms to enhance redox activity. Our findings challenge the prevailing notion that a chemically inert cathode-electrolyte interface is essential for excellent electrochemical performance and offer a pathway for next-generation sustainable ASSBs with high energy density.
全固态电池（assb）可以防止可持续有机电极材料（oem）在液体电解质中的溶解，但其实际应用受到oem与固体电解质（SEs）之间界面反应产生的低能量密度的限制。在这里，我们发现oem和硫化物se之间的界面化学控制可以激活可逆的S2 -阴离子氧化还原，使电极级能量密度达到477 Wh kg - 1，并在室温下稳定循环超过2000次。机理分析确定了有效的OEM催化S2 -阴离子氧化还原的两个关键标准：(1)适度的OEM电极电位足以氧化S2 -而不会过度氧化；(2)低阳离子- S2 -键共价，在S原子上定位电子密度以增强氧化还原活性。我们的研究结果挑战了化学惰性阴极-电解质界面对于优异的电化学性能至关重要的普遍观点，并为下一代高能量密度可持续的assb提供了途径。
{"title":"Catalyzed anionic redox in sulfide electrolytes for high-energy all-solid-state organic batteries","authors":"Qihang Yu, Yang Hu, Sixu Deng, Mohsen Shakouri, Graham King, Lo-Yueh Chang, Karim Zaghib, Tsun-Kong Sham, Xia Li","doi":"10.1016/j.joule.2025.102297","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102297","url":null,"abstract":"All-solid-state batteries (ASSBs) can prevent the dissolution of sustainable organic electrode materials (OEMs) in liquid electrolytes, but their practical implementation is limited by the low energy density arising from interfacial reactions between OEMs and solid electrolytes (SEs). Here, we show that controlled interfacial chemistry between OEMs and sulfide SEs can instead activate reversible S<sup>2−</sup> anionic redox, enabling an electrode-level energy density of 477 Wh kg<sup>−1</sup> and stable cycling for over 2,000 cycles at room temperature. Mechanistic analysis identifies two key criteria for effective OEM-catalyzed S<sup>2−</sup> anionic redox: (1) a moderate OEM electrode potential sufficient to oxidize S<sup>2−</sup> without over-oxidation and (2) low cation–S<sup>2−</sup> bond covalency, localizing electron density on S atoms to enhance redox activity. Our findings challenge the prevailing notion that a chemically inert cathode-electrolyte interface is essential for excellent electrochemical performance and offer a pathway for next-generation sustainable ASSBs with high energy density.","PeriodicalId":343,"journal":{"name":"Joule","volume":"46 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146231350","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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