纳米针尖状质子化聚苯胺负载的单原子铂催化剂实现高效酸性电解水制氢  

Atomically dispersed platinum supported onto nanoneedle-shaped protonated polyaniline for efficient hydrogen production in acidic water electrolysis

作　　者：吴振中 白京 赖飞立 郑慧 张亦喆 张楠 王传洗 王震宇 张龙生 刘天西 Zhenzhong Wu;Jing Bai;Feili Lai;Hui Zheng;Yizhe Zhang;Nan Zhang;Chuanxi Wang;Zhenyu Wang;Longsheng Zhang;Tianxi Liu(Key Laboratory of Synthetic and Biological Colloids,Ministry of Education,School of Chemical and Material Engineering,International Joint Research Laboratory for Nano Energy Composites,Jiangnan University,Wuxi 214122,China;Department of Chemistry,KU Leuven,Celestijnenlaan 200F,Leuven 3001,Belgium;Institute of Environmental Processes and Pollution control,School of Environment and Civil Engineering,Jiangnan University,Wuxi 214122,China)

机构地区：[1]Key Laboratory of Synthetic and Biological Colloids,Ministry of Education,School of Chemical and Material Engineering,International Joint Research Laboratory for Nano Energy Composites,Jiangnan University,Wuxi 214122,China [2]Department of Chemistry,KU Leuven,Celestijnenlaan 200F,Leuven 3001,Belgium [3]Institute of Environmental Processes and Pollution control,School of Environment and Civil Engineering,Jiangnan University,Wuxi 214122,China

出　　处：《Science China Materials》2023年第7期2680-2688,共9页中国科学（材料科学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(52103260,52161135302,and 52211530489);the Research Foundation Flanders(G0F2322N);the Natural Science Foundation of Jiangsu Province(BK20210482);China Postdoctoral Science Foundation(2021M690067);Jiangsu Province Postdoctoral Science Foundation(2021K053A)。

摘　　要：开发高性能单原子铂催化剂对酸性电解水制氢领域具有重要意义.在酸性电解液中,氢离子(H^(+))会被水分子包围并形成水合氢离子,这会导致单原子铂活性位点的局部H^(+)浓度降低,从而使其析氢反应动力学受到限制.本研究通过将单原子铂负载在纳米针尖状质子化聚苯胺上,它既能捕获水合氢离子中的H^(+),又能通过促进电荷积累以加快H^(+)的电化学还原,从而提高单原子铂的析氢反应动力学.结果表明,相比于扁平状质子化聚苯胺负载的单原子铂,针尖状质子化聚苯胺负载的单原子铂的析氢反应转换频率得到显著提高.结合X射线光电子能谱、有限元模拟和电化学行为研究,我们发现局部H^(+)富集促使的氢溢流现象对提升纳米针尖状质子化聚苯胺负载的单原子铂催化剂的析氢活性具有重要贡献.Developing high-performance single-atom platinum(Pt)catalysts for acidic hydrogen evolution reaction(HER)is of significance.However,their HER kinetics are limited due to the low concentration of hydrogen ions(H^(+))near the Pt sites in acidic electrolytes,where hydronium ions are undesirably formed with H^(+)surrounded by water molecules.Here,we seek to improve the HER kinetics by anchoring single-atom Pt catalyst on nanoneedle-shaped protonated polyaniline supports,which can not only capture H^(+)from the hydronium ions but also facilitate the electroreduction of H^(+)by promoting the electron accumulation.As a result,the turnover frequency of single-atom Pt supported on the nanoneedle-shaped protonated polyaniline is appreciably enhanced,compared with that of the single-atom Pt supported on the flat-shaped protonated polyaniline.By combining the X-ray photoelectron spectroscopy,finite-element simulation and electrochemical studies,we find that the enhanced HER activity of single-atom Pt on nanoneedle-shaped protonated polyaniline support may arise from a hydrogen spillover pathway induced by the increased local concentration of H^(+)near the Pt sites.

关 键 词：electrocatalytic hydrogen evolution reaction kinetics single-atom platinum catalysts protonated polyaniline 

分 类 号：TQ426[化学工程] TQ116.2