Operando-reconstructed polyatomic ion layers boost the activity and stability of industrial current–density water splitting  

原位重构的多原子离子层打破活性-稳定平衡提升大电流下工业电解水

作　　者：Yingxia Zhao Ying Wu Qunlei Wen Danji Huang Ruoou Yang Haozhi Wang Yingying Xu Ming Sun Youwen Liu Jiakun Fang Tianyou Zhai Lin Yu 赵英霞;吴颖;温群磊;黄丹极;杨若欧;王浩志;许盈盈;孙明;刘友文;方家琨;翟天佑;余林

机构地区：[1]Guangdong Engineering Technology Research Center of Modern Fine Chemical Engineering,School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou 510006,China [2]State Key Laboratory of Materials Processing and Die&Mould Technology,and School of Materials Science and Engineering,Huazhong University of Science and Technology,Wuhan 430074,China [3]State Key Laboratory of Advanced Electromagnetic Engineering and Technology,and School of Electrical and Electronic Engineering,Huazhong University of Science and Technology,Wuhan 430074,China [4]Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory),Jieyang 515200,China [5]School of Chemistry and Chemical Engineering,South China University of Technology,Guangzhou 510641,China [6]Analysis and Test Center Guangdong University of Technology,Guangdong University of Technology,Guangzhou 510006,China [7]State Key Laboratory of Marine Resource Utilization in South China Se1,School of Materials Science and Engineering,Hainan University,Haikou 570228,China

出　　处：《Science Bulletin》2024年第21期3384-3394,共11页科学通报（英文版）

基　　金：supported by the Foundation of Basic and Applied Basic Research of Guangdong Province(2023B1515120043);the National Natural Science Foundation of China(22071069 and 22275060);the Yangfan Project of Maoming City(MMGCIRI2022YFJH-Y-014);Guangdong Basic and Applied Basic Research Foundation(2019A1515011512,2021A1515010172,and 2023A1515030274);the Foundation of the Smart Medical Innovation Technology Center in Guangdong University of Technology(ZYZX24-031);support from Analysis and Testing Center of Guangdong University of Technology。

摘　　要：Metal–organic frameworks have garnered attention as highly efficient pre-electrocatalysts for the oxygen evolution reaction(OER).Current structure–activity relationships primarily rely on the assumption that the complete dissolution of organic ligands occurs during electrocatalysis.Herein,modeling based on NiFe Prussian blue analogs(NiFe-PBAs)show that cyanide ligands leach from the matrix and subsequently oxidize to corresponding inorganic ions(ammonium and carbonate)that re-adsorb onto the surface of NiFe OOH during the OER process.Interestingly,the surface-adsorbed inorganic ions induce the OER reaction of NiFe OOH to switch from the adsorbate evolution to the lattice-oxygen–mediated mechanism,thus contributing to the high activity.In addition,this reconstructed inorganic ion layer acting as a versatile protective layer can prevent the dissolution of metal sites to maintain contact between catalytic sites and reactive ions,thus breaking the activity–stability trade-off.Consequently,our constructed NiFePBAs exhibit excellent durability for 1250 h with an ultralow overpotential of 253 mV at 100 mA cm2.The scale-up NiFe-PBAs operated with a low energy consumption of4.18 kWh m3 H2 in industrial water electrolysis equipment.The economic analysis of the entire life cycle demonstrates that this green hydrogen production is priced at US$2.59 kg^(-1)H_(2),meeting global targets(<US$2.5 kg^(-1)H_(2)).

关 键 词：Chemical recognition Oxygen evolution mechanism Industrial water electrolysis 

分 类 号：TQ116.21[化学工程—无机化工] TQ426