Pub 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":"https://doi.org/10.1016/j.joule.2025.102306","url":null,"abstract":"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.","PeriodicalId":343,"journal":{"name":"Joule","volume":"275 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-02-03","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}
Conventional lithium-sulfur (Li-S) batteries, which rely on alkali metal ions (Li⁺/Na⁺/K⁺) as charge carriers, suffer from polysulfide dissolution, poor Li2S conductivity, and low redox potential (−0.5 V vs. the standard hydrogen electrode [SHE]). Here, we report a copper-ion-mediated sulfur battery chemistry that fundamentally circumvents these limitations by leveraging the intrinsically low solubility of CuxS in non-aqueous electrolytes. By replacing alkali metal ions with copper ions as the charge carrier in a 1,3-dioxolane/1,2-dimethoxyethane (DOL/DME)-based electrolyte, we achieve an insoluble CuxS discharge intermediate, which elevates the sulfur redox potential to 0.5 V vs. SHE, more than a 1.2 V increase over conventional Li-S systems, enabling a discharge voltage of 3.3 V in a hybrid Li-S full cell. Simultaneously, the formation of conductive CuₓS species ensures efficient reaction kinetics while eliminating polysulfide shuttling. The copper-ion-mediated sulfur electrochemistry unlocks high energy density and fast kinetics, paving the way for practical sulfur-based batteries.
{"title":"High-voltage sulfur electrochemistry enabled by copper-ion mediation in non-aqueous batteries","authors":"Yu Ding, Chunlong Dai, Fei Wang, Zhaohui Li, Haichuan Zhou, Zongbin Luo, Maowen Xu, Linyu Hu, Zifeng Lin","doi":"10.1016/j.joule.2025.102268","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102268","url":null,"abstract":"Conventional lithium-sulfur (Li-S) batteries, which rely on alkali metal ions (Li⁺/Na⁺/K⁺) as charge carriers, suffer from polysulfide dissolution, poor Li<sub>2</sub>S conductivity, and low redox potential (−0.5 V vs. the standard hydrogen electrode [SHE]). Here, we report a copper-ion-mediated sulfur battery chemistry that fundamentally circumvents these limitations by leveraging the intrinsically low solubility of Cu<sub><em>x</em></sub>S in non-aqueous electrolytes. By replacing alkali metal ions with copper ions as the charge carrier in a 1,3-dioxolane/1,2-dimethoxyethane (DOL/DME)-based electrolyte, we achieve an insoluble Cu<sub><em>x</em></sub>S discharge intermediate, which elevates the sulfur redox potential to 0.5 V vs. SHE, more than a 1.2 V increase over conventional Li-S systems, enabling a discharge voltage of 3.3 V in a hybrid Li-S full cell. Simultaneously, the formation of conductive Cu<em>ₓ</em>S species ensures efficient reaction kinetics while eliminating polysulfide shuttling. The copper-ion-mediated sulfur electrochemistry unlocks high energy density and fast kinetics, paving the way for practical sulfur-based batteries.","PeriodicalId":343,"journal":{"name":"Joule","volume":"263 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146070615","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 : 2026-01-27DOI: 10.1016/j.joule.2025.102266
Yupei Han, Adam Lovett, Nuebi Xavier, Matthew Blunt, Pan He, Ajay Piriya Vijaya Kumar Saroja, Wanjun Ren, Yi Lu, Yudong Luo, Thomas S. Miller, Qiong Cai, Yang Xu
{"title":"Work of adhesion guided nucleation control for energy-dense potassium metal batteries","authors":"Yupei Han, Adam Lovett, Nuebi Xavier, Matthew Blunt, Pan He, Ajay Piriya Vijaya Kumar Saroja, Wanjun Ren, Yi Lu, Yudong Luo, Thomas S. Miller, Qiong Cai, Yang Xu","doi":"10.1016/j.joule.2025.102266","DOIUrl":"https://doi.org/10.1016/j.joule.2025.102266","url":null,"abstract":"","PeriodicalId":343,"journal":{"name":"Joule","volume":"43 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072533","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 : 2026-01-26DOI: 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
{"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":"https://doi.org/10.1016/j.joule.2025.102262","url":null,"abstract":"","PeriodicalId":343,"journal":{"name":"Joule","volume":"85 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2026-01-26","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}
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}