Maximizing hydrogen evolution via Co-Ni dual atoms and nanoclusters on hierarchically ordered porous carbon framework  

有序多级孔碳框架负载的Co–Ni双原子与纳米团簇高效析氢

作　　者：Qian Li Pan Zhang Huaiguang Li Yuan Wang Dongsheng Tang Qun Li Jiabin Wu 李谦;张盼;李怀光;王苑;唐东升;李群;吴佳宾(Synergetic Innovation Center for Quantum Effects and Application,Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education,College of Physics and Information Science,Hunan Normal University,Changsha 410081,China;National Key Laboratory of Advanced Micro and Nano Manufacture Technology,School of Integrated Circuits,Peking University,Beijing 100871,China;The Chinese University of Hong Kong,Shenzhen,Shenzhen 518172,China;CAS Key Laboratory of Nanosystem and Hierarchical Fabrication&CAS Center for Excellence in Nanoscience,National Center for Nanoscience and Technology,Beijing 100190,China;Department of Chemistry,Tsinghua University,Beijing 100084,China;Insititute of Microelectronics,State Key Laboratory of Analog and Mixed-Signal VLSI,University of Macao,Macao 519000,China)

机构地区：[1]Synergetic Innovation Center for Quantum Effects and Application,Key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education,College of Physics and Information Science,Hunan Normal University,Changsha 410081,China [2]National Key Laboratory of Advanced Micro and Nano Manufacture Technology,School of Integrated Circuits,Peking University,Beijing 100871,China [3]The Chinese University of Hong Kong,Shenzhen,Shenzhen 518172,China [4]CAS Key Laboratory of Nanosystem and Hierarchical Fabrication&CAS Center for Excellence in Nanoscience,National Center for Nanoscience and Technology,Beijing 100190,China [5]Department of Chemistry,Tsinghua University,Beijing 100084,China [6]Insititute of Microelectronics,State Key Laboratory of Analog and Mixed-Signal VLSI,University of Macao,Macao 519000,China

出　　处：《Science China Materials》2024年第10期3197-3205,共9页中国科学（材料科学）（英文版）

基　　金：financially supported by the National Key R&D Program of China(2022YFC2603901);the Scientific Research Project of Hunan Provincial Department of Education(23B0066);the National Natural Science Foundation of China(62304012,12074116,22201309);the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(2019ZT08L101);the University Stability Support Program of Shenzhen(2023SC0027);the Shenzhen Science and Technology Innovation Commission(JSGGKQTD20221101115701006);the Beijing Natural Science Foundation(2224103);the China Postdoctoral Science Foundation(2021M691759,2021M700981,2021TQ0169)。

摘　　要：Efficient hydrogen production through water splitting relies on the development of high-performance catalysts for the hydrogen evolution reaction(HER).In this study,we synthesized the CoNi SAs@NPs-NC catalyst using multi-metal single-crystal ordered macroporous metal-organic frameworks(MOFs)as precursors.This catalyst features a hierarchical porous structure with ordered macropores and micropores,which not only provides a high specific surface area but also promotes efficient mass diffusion.Furthermore,the incorporation of bimetallic components,coupled with synergistic interactions between single atoms(SAs)and nanoparticles(NPs),significantly enhances its catalytic activity.The CoNi SAs@NPs-NC nanocatalysts demonstrated exceptional activity in the HER,recording overpotentials of 90 mV in 1 M KOH and 61 mV in 0.5 M H_(2)SO_(4),both at a current density of 10 mA cm^(−2).In addition,density functional theory(DFT)analysis was employed to investigate the synergistic interactions among CoNi NPs,SAs,and nitrogen dopants.Our finding highlights the promising potential of the CoNi SAs@NPs-NC catalyst for efficient hydrogen evolution,making it a valuable candidate for advancing the field of water splitting.本研究中,我们使用多金属单晶有序大孔金属-有机框架(MOFs)作为前体,合成了CoNi SAs@NPs-NC催化剂.该催化剂具有大孔和微孔的多级孔结构,该结构不仅提供了高比表面积,还提供了快速的物质扩散通道.此外,该催化剂具有的双金属组分,以及单原子(SAs)和纳米颗粒(NPs)之间的协同作用显著增强了其催化活性.CoNi SAs@NPs-NC纳米催化剂在析氢反应中展示了卓越的活性,在1 M的KOH和0.5 M的H_(2)SO_(4)中分别具有90和61 mV的过电势(电流密度10 mA cm^(−2)).此外,我们还使用密度泛函理论(DFT)分析研究了CoNi NPs与SAs之间的协同作用.本工作展示了CoNi SAs@NPs-NC催化剂在高效析氢中的潜力.

关 键 词：three dimensional ordered macroporous Co-Ni dual atoms Co-Ni nanoclusters HER synergistic effect 

分 类 号：TQ116.2[化学工程—无机化工] TQ426