Pub Date : 2026-02-03DOI: 10.1021/acsenergylett.6c00053
Myeongjun Choi,Jeongwoo Seo,Min-Ho Kim,Hojoon Kim,Euna Kim,Jinyeong Choe,Haeseong Jang,Jeeho Ha,Nyung Joo Kong,Seok Ju Kang,Dong-Hwa Seo,Young Hwa Jung,Hyun-Wook Lee
Anionic redox in lithium-rich layered oxides (LRLOs) offers a breakthrough to higher energy density but is limited by voltage hysteresis arising from irreversible structural disorder. While enhancing transition metal–oxygen (TM-O) covalency through π-type interaction improves the reversibility of anionic processes, inevitable structural disorder during the first cycle still deteriorates TM-O hybridization. Here, we propose a counterintuitive strategy that embraces pre-synthetic cation disorder to preserve TM-O π-redox. The in-plane disordered arrangement modulates the first-cycle phase evolution, suppressing O3–O1 slab gliding and relaxing localized cationic oxidation at high voltage. This structural control maintains robust TM-O coordination and stabilized oxygen states even under high-voltage operation, yielding markedly reduced voltage hysteresis (0.31 vs 0.62 V) and exceptional long-term stability with minimal voltage decay (−0.04 mV cycle–1) and 98.0% energy retention after 160 cycles. This work establishes structural-disorder-driven phase evolution control as a practical design principle for stabilizing π-redox chemistry, achieving high-energy, structurally resilient LRLOs.
富锂层状氧化物（LRLOs）的阴离子氧化还原为实现更高的能量密度提供了突破口，但由于不可逆结构紊乱引起的电压滞后限制了离子氧化还原技术的发展。虽然通过π型相互作用增强过渡金属-氧（TM-O）共价提高了阴离子过程的可逆性，但在第一个循环中不可避免的结构紊乱仍然会使TM-O杂化恶化。在这里，我们提出了一种反直觉的策略，采用预合成阳离子紊乱来保护TM-O π-氧化还原。平面内无序排列调节了第一循环相演化，抑制了O3-O1板的滑动，并在高压下放松了局域阳离子氧化。这种结构控制保持了强大的TM-O协调和稳定的氧态，即使在高压下也能产生显著降低的电压滞后（0.31 vs 0.62 V）和卓越的长期稳定性，具有最小的电压衰减（- 0.04 mV cycle-1）和160次循环后98.0%的能量保留。本工作建立了结构无序驱动的相演化控制作为稳定π-氧化还原化学的实用设计原则，实现了高能量、结构弹性的LRLOs。
{"title":"Pre-Disordering for Preserving Transition Metal–Oxygen Covalency in Lithium-Rich Layered Oxide Cathodes","authors":"Myeongjun Choi,Jeongwoo Seo,Min-Ho Kim,Hojoon Kim,Euna Kim,Jinyeong Choe,Haeseong Jang,Jeeho Ha,Nyung Joo Kong,Seok Ju Kang,Dong-Hwa Seo,Young Hwa Jung,Hyun-Wook Lee","doi":"10.1021/acsenergylett.6c00053","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00053","url":null,"abstract":"Anionic redox in lithium-rich layered oxides (LRLOs) offers a breakthrough to higher energy density but is limited by voltage hysteresis arising from irreversible structural disorder. While enhancing transition metal–oxygen (TM-O) covalency through π-type interaction improves the reversibility of anionic processes, inevitable structural disorder during the first cycle still deteriorates TM-O hybridization. Here, we propose a counterintuitive strategy that embraces pre-synthetic cation disorder to preserve TM-O π-redox. The in-plane disordered arrangement modulates the first-cycle phase evolution, suppressing O3–O1 slab gliding and relaxing localized cationic oxidation at high voltage. This structural control maintains robust TM-O coordination and stabilized oxygen states even under high-voltage operation, yielding markedly reduced voltage hysteresis (0.31 vs 0.62 V) and exceptional long-term stability with minimal voltage decay (−0.04 mV cycle–1) and 98.0% energy retention after 160 cycles. This work establishes structural-disorder-driven phase evolution control as a practical design principle for stabilizing π-redox chemistry, achieving high-energy, structurally resilient LRLOs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"91 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111132","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 : 2026-02-02DOI: 10.1021/acsenergylett.5c03921
Haoliang Chen, Min Cheng, Mengjie Li, Wenjie Huang, Weiwei Han, Xuerong Zheng, Yida Deng
Aqueous zinc metal batteries (AZMBs) are limited by water-driven parasitic reactions and unstable Zn deposition. We report a hydrogen-bond-mediated interfacial water-masking strategy using isosorbide dimethyl ether (IDE), a symmetric molecule with electron-rich sites and multiple hydrogen-bond acceptors, to regulate Zn interfacial chemistry at the molecular level. Here, IDE reconstructs the outer hydrogen-bonding network to reduce water activity without occupying the primary Zn2+ solvation sheath. Density-functional analysis further reveals facet-selective adsorption of IDE on Zn(100)/(101), guiding deposition toward the low-energy (002) orientation. IDE-related complexes also promote the formation of an inorganic SEI layer, yielding a compact, low-reactivity interface. With this cooperative regulation, the optimized ZSE–IDE10 electrolyte enables Zn||Zn cells to cycle for over 5400 h at 1 mA cm–2 and 1200 h at 10 mA cm–2, while Zn||NH4V4O10 full cells exhibit improved cycling stability and rate capability. This work establishes a molecular-level design principle for regulating interfacial chemistry in AZMBs.
水性锌金属电池（azmb）受水驱动的寄生反应和不稳定的锌沉积的限制。我们报道了一种氢键介导的界面水掩膜策略，使用异山梨酯二甲醚（IDE），一种具有富电子位点和多个氢键受体的对称分子，在分子水平上调节Zn界面化学。在这里，IDE重建了外部氢键网络，以降低水活性，而不占用原生Zn2+溶剂化鞘层。密度功能分析进一步揭示了IDE在Zn(100)/(101)上的面选择性吸附，引导沉积向低能（002）方向发展。ide相关的配合物也促进了无机SEI层的形成，从而产生致密、低反应性的界面。通过这种协同调节，优化后的ZSE-IDE10电解质使Zn||锌电池在1 mA cm-2下循环超过5400 h，在10 mA cm-2下循环超过1200 h，而Zn||NH4V4O10全电池表现出更好的循环稳定性和速率能力。本工作建立了调节azmb界面化学的分子水平设计原则。
{"title":"Hydrogen-Bond-Mediated Interfacial Water-Masking Strategy for Facet-Controlled Zn Deposition in Aqueous Zn Metal Batteries","authors":"Haoliang Chen, Min Cheng, Mengjie Li, Wenjie Huang, Weiwei Han, Xuerong Zheng, Yida Deng","doi":"10.1021/acsenergylett.5c03921","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03921","url":null,"abstract":"Aqueous zinc metal batteries (AZMBs) are limited by water-driven parasitic reactions and unstable Zn deposition. We report a hydrogen-bond-mediated interfacial water-masking strategy using isosorbide dimethyl ether (IDE), a symmetric molecule with electron-rich sites and multiple hydrogen-bond acceptors, to regulate Zn interfacial chemistry at the molecular level. Here, IDE reconstructs the outer hydrogen-bonding network to reduce water activity without occupying the primary Zn<sup>2+</sup> solvation sheath. Density-functional analysis further reveals facet-selective adsorption of IDE on Zn(100)/(101), guiding deposition toward the low-energy (002) orientation. IDE-related complexes also promote the formation of an inorganic SEI layer, yielding a compact, low-reactivity interface. With this cooperative regulation, the optimized ZSE–IDE10 electrolyte enables Zn||Zn cells to cycle for over 5400 h at 1 mA cm<sup>–2</sup> and 1200 h at 10 mA cm<sup>–2</sup>, while Zn||NH<sub>4</sub>V<sub>4</sub>O<sub>10</sub> full cells exhibit improved cycling stability and rate capability. This work establishes a molecular-level design principle for regulating interfacial chemistry in AZMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097848","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 : 2026-02-02DOI: 10.1021/acsenergylett.5c04101
Paul Byaruhanga, Yu Wang, Richard Tran, Kai Shen Choong, Hong Zhong, Vidhi Joshi, Shaowei Song, Dezhi Wang, Mingchu Zou, Viktor G Hadjiev, Hua Guo, Jiming Bao, Lars C. Grabow, Zhenxing Feng, Zhifeng Ren, Shuo Chen
Hydrogen production in aqueous alkaline media is constrained by both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Here, we report an anion-environment-regulated synthesis strategy that enables uniform Ce incorporation into NiFe layered double hydroxides (LDHs) by replacing NH4F with NH4Cl during hydrothermal growth. The chloride precursor provides a milder coordination environment, enabling homogeneous Ce doping and improved charge transfer. The optimized NiFe0.95Ce0.05 LDH requires only a 307 mV overpotential to reach 1000 mA cm–2 in 1 M KOH. Raman spectroscopy, X-ray absorption spectroscopy, and density functional theory analyses indicate that Ce doping accelerates Ni oxidation and stabilizes β-NiOOH active species. When paired with a Ni&Ni0.2Mo0.8N cathode, the resulting anion exchange membrane electrolyzer (AEMWE) delivers 1 A cm–2 at 1.616 V and 8 A cm–2 at 2.185 V in 1 M KOH at 80 °C without iR compensation for high-current-density alkaline water electrolysis.
在碱性水介质中，析氢反应（HER）和析氧反应（OER）对氢气的生成有一定的限制。在这里，我们报告了阴离子环境调节的合成策略，通过在水热生长过程中用NH4Cl取代NH4F，使Ce均匀地掺入NiFe层状双氢氧化物（LDHs）中。氯化物前驱体提供了一个温和的配位环境，使Ce掺杂均匀，并改善了电荷转移。优化后的NiFe0.95Ce0.05 LDH仅需307 mV过电位即可在1 M KOH条件下达到1000 mA cm-2。拉曼光谱、x射线吸收光谱和密度泛函理论分析表明，Ce掺杂加速了Ni氧化，稳定了β-NiOOH活性物质。当与Ni0.2Mo0.8N阴极配对时，得到的阴离子交换膜电解槽（AEMWE）在1.616 V和2.185 V下，在1 M KOH， 80°C下，无iR补偿，可用于高电流密度碱性电解。
{"title":"Anion-Environment-Controlled Synthesis of Ce-Doped NiFe LDH for Enhanced Activity and Stability in High-Current-Density Alkaline Oxygen Evolution","authors":"Paul Byaruhanga, Yu Wang, Richard Tran, Kai Shen Choong, Hong Zhong, Vidhi Joshi, Shaowei Song, Dezhi Wang, Mingchu Zou, Viktor G Hadjiev, Hua Guo, Jiming Bao, Lars C. Grabow, Zhenxing Feng, Zhifeng Ren, Shuo Chen","doi":"10.1021/acsenergylett.5c04101","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04101","url":null,"abstract":"Hydrogen production in aqueous alkaline media is constrained by both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Here, we report an anion-environment-regulated synthesis strategy that enables uniform Ce incorporation into NiFe layered double hydroxides (LDHs) by replacing NH<sub>4</sub>F with NH<sub>4</sub>Cl during hydrothermal growth. The chloride precursor provides a milder coordination environment, enabling homogeneous Ce doping and improved charge transfer. The optimized NiFe<sub>0.95</sub>Ce<sub>0.05</sub> LDH requires only a 307 mV overpotential to reach 1000 mA cm<sup>–2</sup> in 1 M KOH. Raman spectroscopy, X-ray absorption spectroscopy, and density functional theory analyses indicate that Ce doping accelerates Ni oxidation and stabilizes β-NiOOH active species. When paired with a Ni&Ni<sub>0.2</sub>Mo<sub>0.8</sub>N cathode, the resulting anion exchange membrane electrolyzer (AEMWE) delivers 1 A cm<sup>–2</sup> at 1.616 V and 8 A cm<sup>–2</sup> at 2.185 V in 1 M KOH at 80 °C without <i>iR</i> compensation for high-current-density alkaline water electrolysis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097849","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}
The rapid increase of lithium-ion batteries (LIBs) faces severe challenges. Due to the environmental effects from numerous spent LIBs and the imbalanced supply demand of raw materials, recycling of spent LIBs is urgently needed. However, at present recycling techniques face significant hindrances, such as inefficient metal separation, high energy consumption, and secondary pollution. This review demonstrates a detailed analysis of commercial LIB cathode materials that refers to both merits and limitations from technological and industrial aspects. Moreover, the entire recycling chain is systematically investigated, including pretreatment and mainstream recycling methods, such as pyrometallurgy, hydrometallurgy, bioleaching, and direct regeneration. Meanwhile, optimization pathways for separation techniques are discussed. Finally, a multicriteria framework for evaluating cathode material recycling technologies is developed, which comprises energy consumption, environmental impact, cost, recycling efficiency, and closed-loop duration. It provides insights for optimizing sustainable processes. This review discusses the technology for recycling cathode materials in LIBs and proposes strategies for renewable energy.
{"title":"Recycling Critical Metals from Spent Lithium-Ion Battery Cathodes: Technologies, Challenges, and Perspectives to Sustainable Closed-Loop Systems","authors":"Qi Zhang,Hui-Ling Deng,Rui Huang,Cai-Yun Zhang,Chen-Zhe Zhang,Chen-Yang Wang,Yang Liu,Xiang Gao,Min Yan,Zhitian Liu","doi":"10.1021/acsenergylett.5c03663","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03663","url":null,"abstract":"The rapid increase of lithium-ion batteries (LIBs) faces severe challenges. Due to the environmental effects from numerous spent LIBs and the imbalanced supply demand of raw materials, recycling of spent LIBs is urgently needed. However, at present recycling techniques face significant hindrances, such as inefficient metal separation, high energy consumption, and secondary pollution. This review demonstrates a detailed analysis of commercial LIB cathode materials that refers to both merits and limitations from technological and industrial aspects. Moreover, the entire recycling chain is systematically investigated, including pretreatment and mainstream recycling methods, such as pyrometallurgy, hydrometallurgy, bioleaching, and direct regeneration. Meanwhile, optimization pathways for separation techniques are discussed. Finally, a multicriteria framework for evaluating cathode material recycling technologies is developed, which comprises energy consumption, environmental impact, cost, recycling efficiency, and closed-loop duration. It provides insights for optimizing sustainable processes. This review discusses the technology for recycling cathode materials in LIBs and proposes strategies for renewable energy.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097861","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}
We demonstrated perovskite–Cu(In,Ga)Se2 (CIGS) tandem solar cells in which the perovskite top absorber is deposited by coevaporation, enabling highly uniform film formation on rough CIGS bottom cells. In addition, we introduced a compact tin oxide buffer layer on the zinc oxide surface, effectively preventing the detrimental Lewis acid–base reaction with the perovskite. A certified power conversion efficiency of 24.5% (1 cm2 aperture area) is achieved from the resulting monolithic perovskite–CIGS tandems. This work establishes a scalable vacuum-based route for delivering high-efficiency perovskite–CIGS tandem photovoltaics.
我们展示了钙钛矿- cu (In,Ga)Se2 （CIGS）串联太阳能电池，其中钙钛矿顶部吸收剂通过共蒸发沉积，使粗糙的CIGS底部电池形成高度均匀的薄膜。此外，我们在氧化锌表面引入了致密的氧化锡缓冲层，有效地防止了与钙钛矿的有害刘易斯酸碱反应。由此产生的单片钙钛矿- cigs串联实现了24.5% （1 cm2孔径面积）的认证功率转换效率。这项工作建立了一种可扩展的真空路线，用于输送高效钙钛矿- cigs串联光伏电池。
{"title":"Efficient Perovskite–Cu(In,Ga)Se2 Tandem Solar Cells Enabled by Coevaporation","authors":"Nengxu Li,Shuping Lin,Xiuxiu Niu,Zhenrong Jia,Ming Zhao,Ying Zhao,Yao Sun,Dalong Zhong,Yi Hou","doi":"10.1021/acsenergylett.5c04203","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04203","url":null,"abstract":"We demonstrated perovskite–Cu(In,Ga)Se2 (CIGS) tandem solar cells in which the perovskite top absorber is deposited by coevaporation, enabling highly uniform film formation on rough CIGS bottom cells. In addition, we introduced a compact tin oxide buffer layer on the zinc oxide surface, effectively preventing the detrimental Lewis acid–base reaction with the perovskite. A certified power conversion efficiency of 24.5% (1 cm2 aperture area) is achieved from the resulting monolithic perovskite–CIGS tandems. This work establishes a scalable vacuum-based route for delivering high-efficiency perovskite–CIGS tandem photovoltaics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097860","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}
Acidic flow cells and solid-state electrolyte (SSE) cells represent two promising electrolyzer configurations for a practical CO2 reduction reaction (CO2RR), yet their comparative technical metrics remain underexplored. This study systematically investigates the electrolyzer performance, local reaction environment, and technical economic feasibility of acidic flow cells and SSE cells using precise HCOOH electrosynthesis from high-rate CO2RR as a model system. High CO2 utilization efficiency (74.7%) and HCOOH selectivity (96.1%) are achieved in an acidic flow cell aided by a K+-enhanced local electric field that facilitates the *OCHO pathway, as verified by in situ spectroelectrochemistry and numerical simulations. Impedance analysis reveals better CO2 mass transport kinetics in the acidic flow cell, whereas improved reaction dynamics is observed in the SSE cell. Techno-economic analysis demonstrates a 14.4% lower HCOOH production cost within the SSE system, primarily due to reduced product separation expenses and enhanced energy efficiency. These findings advance the understanding of the CO2 electrolyzer design and optimization for efficient electrosynthesis.
{"title":"Electrified CO2-to-HCOOH Valorization: A Comparative Technical Analysis on Acidic Flow Cell and Solid-State Electrolyte Cell Reactors","authors":"Yanbo Hua,Daokun Kang,Jiaao Huang,Baoxin Ni,Wen-Bin Cai,Kun Jiang","doi":"10.1021/acsenergylett.5c03557","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03557","url":null,"abstract":"Acidic flow cells and solid-state electrolyte (SSE) cells represent two promising electrolyzer configurations for a practical CO2 reduction reaction (CO2RR), yet their comparative technical metrics remain underexplored. This study systematically investigates the electrolyzer performance, local reaction environment, and technical economic feasibility of acidic flow cells and SSE cells using precise HCOOH electrosynthesis from high-rate CO2RR as a model system. High CO2 utilization efficiency (74.7%) and HCOOH selectivity (96.1%) are achieved in an acidic flow cell aided by a K+-enhanced local electric field that facilitates the *OCHO pathway, as verified by in situ spectroelectrochemistry and numerical simulations. Impedance analysis reveals better CO2 mass transport kinetics in the acidic flow cell, whereas improved reaction dynamics is observed in the SSE cell. Techno-economic analysis demonstrates a 14.4% lower HCOOH production cost within the SSE system, primarily due to reduced product separation expenses and enhanced energy efficiency. These findings advance the understanding of the CO2 electrolyzer design and optimization for efficient electrosynthesis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"275 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097862","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 : 2026-02-02DOI: 10.1021/acsenergylett.5c03985
Boyeong Jang, Jongyoung Lee, Yoon Seok Jung
Sulfide solid electrolytes uniquely combine high ionic conductivity, mechanical compliance, and solvent-mediated processability, positioning them at the forefront of all-solid-state battery (ASSB) development. This perspective provides a comprehensive view of liquid-phase routes across the entire life cycle─from synthesis and electrode fabrication to regeneration and potential recycling. We discuss how solvent-based processes facilitate particle uniformity, densification, and interfacial contact while imparting distinctive morphological and mechanical characteristics that are unattainable through solid-state methods. We then highlight the often-overlooked solvent footprint, whereby solvent exposure introduces persistent organic species in the form of coordinated adducts, surface-adsorbed molecules, or chemically transformed byproducts. These residues markedly alter interfacial chemistry, interparticle contact mechanics, electronic conductivity, and overall electrochemical performance, thereby necessitating residue-aware processing strategies. Finally, we outline the key challenges and future research directions for solvent-compatible and residue-conscious design, underscoring its importance in scalable manufacturing, electrochemical reliability, and sustainable ASSB technologies.
{"title":"Solvent Footprint in Wet-Chemical Processing of Sulfide Solid Electrolytes for All-Solid-State Batteries","authors":"Boyeong Jang, Jongyoung Lee, Yoon Seok Jung","doi":"10.1021/acsenergylett.5c03985","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03985","url":null,"abstract":"Sulfide solid electrolytes uniquely combine high ionic conductivity, mechanical compliance, and solvent-mediated processability, positioning them at the forefront of all-solid-state battery (ASSB) development. This perspective provides a comprehensive view of liquid-phase routes across the entire life cycle─from synthesis and electrode fabrication to regeneration and potential recycling. We discuss how solvent-based processes facilitate particle uniformity, densification, and interfacial contact while imparting distinctive morphological and mechanical characteristics that are unattainable through solid-state methods. We then highlight the often-overlooked solvent footprint, whereby solvent exposure introduces persistent organic species in the form of coordinated adducts, surface-adsorbed molecules, or chemically transformed byproducts. These residues markedly alter interfacial chemistry, interparticle contact mechanics, electronic conductivity, and overall electrochemical performance, thereby necessitating residue-aware processing strategies. Finally, we outline the key challenges and future research directions for solvent-compatible and residue-conscious design, underscoring its importance in scalable manufacturing, electrochemical reliability, and sustainable ASSB technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"295 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146111004","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}
Protonic ceramic electrochemical cells (PCECs) show promise for efficient hydrogen production and power generation, yet surface degradation of perovskite air electrodes caused by A-site cation segregation poses a challenge. Rather than suppressing surface segregation, this work leverages the opportunity, unlocking the latent potential of the catalytically active, B-site-enriched subsurface beneath the segregated surface layers. Using PrBa0.5Sr0.5Co1.5Fe0.5O5+δ (PBSCF) as a model electrode, we expose a subsurface enriched with oxygen vacancies through an alkaline treatment. As a result, the electrolysis current density increases by 28% at 1.3 V and the peak power density improves by 24% at 650 °C in reversible PCEC operation, while maintaining stability. These improvements arise from enhanced H2O/O2 adsorption and dissociation, and facilitated charge transfer, supported by experimental and theoretical analysis. This surface activation strategy is further validated across multiple perovskite air electrodes, demonstrating a general approach to revive segregated electrodes by harnessing the self-reconstructed subsurface.
{"title":"Reviving Air Electrodes in Protonic Ceramic Cells by Unlocking Subsurface","authors":"Haoqing Lin, Bing Li, Shunrui Luo, Yong Ding, Tongtong Li, Tenghui Yuan, Chaoxia Peng, Kai Pei, Yucun Zhou, Simin Jiang, Shasha Luo, Jordi Arbiol, Yu Chen, Wei Yuan, Enzuo Liu, Meilin Liu, Bote Zhao","doi":"10.1021/acsenergylett.5c03995","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03995","url":null,"abstract":"Protonic ceramic electrochemical cells (PCECs) show promise for efficient hydrogen production and power generation, yet surface degradation of perovskite air electrodes caused by A-site cation segregation poses a challenge. Rather than suppressing surface segregation, this work leverages the opportunity, unlocking the latent potential of the catalytically active, B-site-enriched subsurface beneath the segregated surface layers. Using PrBa<sub>0.5</sub>Sr<sub>0.5</sub>Co<sub>1.5</sub>Fe<sub>0.5</sub>O<sub>5+δ</sub> (PBSCF) as a model electrode, we expose a subsurface enriched with oxygen vacancies through an alkaline treatment. As a result, the electrolysis current density increases by 28% at 1.3 V and the peak power density improves by 24% at 650 °C in reversible PCEC operation, while maintaining stability. These improvements arise from enhanced H<sub>2</sub>O/O<sub>2</sub> adsorption and dissociation, and facilitated charge transfer, supported by experimental and theoretical analysis. This surface activation strategy is further validated across multiple perovskite air electrodes, demonstrating a general approach to revive segregated electrodes by harnessing the self-reconstructed subsurface.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"79 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101524","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 : 2026-02-01DOI: 10.1021/acsenergylett.5c03792
Boling Liu, Chengcheng Fang
Sulfide and halide solid-state electrolytes (SSEs) are promising for next-generation battery systems, yet their poor moisture stability remains a critical challenge. Despite extensive research on materials design and protection strategies, the lack of standardized, quantitative methods for evaluating moisture stability is a fundamental barrier to translating SSEs into practical technologies. In this Perspective, we survey the literature on moisture stability of sulfide and halide SSEs and critically examine testing practices, including humidity levels, exposure duration, sample form, and postexposure heat treatment─which all vary widely and impede cross-study comparison. We highlight that postexposure heat treatment, often underreported, can strongly influence the apparent recovery of ionic conductivity and structure. We call for standardized protocols and reporting metrics to enable fair benchmarking, reproducibility, and clearer identification of truly effective stabilization strategies for reliable, manufacturable solid-state batteries.
{"title":"From Mechanism to Metrics: Quantitative Insights into Moisture Stability of Solid-State Electrolytes","authors":"Boling Liu, Chengcheng Fang","doi":"10.1021/acsenergylett.5c03792","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03792","url":null,"abstract":"Sulfide and halide solid-state electrolytes (SSEs) are promising for next-generation battery systems, yet their poor moisture stability remains a critical challenge. Despite extensive research on materials design and protection strategies, the lack of standardized, quantitative methods for evaluating moisture stability is a fundamental barrier to translating SSEs into practical technologies. In this Perspective, we survey the literature on moisture stability of sulfide and halide SSEs and critically examine testing practices, including humidity levels, exposure duration, sample form, and postexposure heat treatment─which all vary widely and impede cross-study comparison. We highlight that postexposure heat treatment, often underreported, can strongly influence the apparent recovery of ionic conductivity and structure. We call for standardized protocols and reporting metrics to enable fair benchmarking, reproducibility, and clearer identification of truly effective stabilization strategies for reliable, manufacturable solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"20 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097851","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 : 2026-02-01DOI: 10.1021/acsenergylett.5c03478
Zhehan Yi, Da-Qian Cai, Hong Jin Fan
Four-electron Zn–I2 batteries (FEZIBs) have garnered increasing research interest due to their potential in grid-scale energy storage. Compared with the energy density (<300 Wh kg–1) of conventional two-electron iodine cathodes, the I–/I0/I+ redox pair endows four-electron iodine cathodes with an energy density of >600 Wh kg–1. However, the formation of I+ species is hindered by the high energy barrier of I0/I+ oxidation and their intrinsic chemical instability. In this Perspective, we elucidate the SN2-type nucleophilic mechanism as a fundamental principle for activating the I0/I+ conversion and propose that the instability of I+ species originates from shuttling effects and hydrolysis reactions. Based on these insights, feasible strategies for I0/I+ activation and I+ species stabilization are proposed. Moreover, we outline the key targets, opportunities, and challenges for the future development of FEZIBs. This Perspective may provide insights into further advancement of Zn–I2 batteries.
{"title":"Rethinking the Four-Electron Iodine Redox Mechanism in Zn–I2 Batteries","authors":"Zhehan Yi, Da-Qian Cai, Hong Jin Fan","doi":"10.1021/acsenergylett.5c03478","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03478","url":null,"abstract":"Four-electron Zn–I<sub>2</sub> batteries (FEZIBs) have garnered increasing research interest due to their potential in grid-scale energy storage. Compared with the energy density (<300 Wh kg<sup>–1</sup>) of conventional two-electron iodine cathodes, the I<sup>–</sup>/I<sup>0</sup>/I<sup>+</sup> redox pair endows four-electron iodine cathodes with an energy density of >600 Wh kg<sup>–1</sup>. However, the formation of I<sup>+</sup> species is hindered by the high energy barrier of I<sup>0</sup>/I<sup>+</sup> oxidation and their intrinsic chemical instability. In this Perspective, we elucidate the S<sub>N</sub>2-type nucleophilic mechanism as a fundamental principle for activating the I<sup>0</sup>/I<sup>+</sup> conversion and propose that the instability of I<sup>+</sup> species originates from shuttling effects and hydrolysis reactions. Based on these insights, feasible strategies for I<sup>0</sup>/I<sup>+</sup> activation and I<sup>+</sup> species stabilization are proposed. Moreover, we outline the key targets, opportunities, and challenges for the future development of FEZIBs. This Perspective may provide insights into further advancement of Zn–I<sub>2</sub> batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"42 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097850","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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