Highly performed platinum nanosheets synthesized under in situ reaction conditions for hydrogen generation
Highly performed platinum nanosheets synthesized under in situ reaction conditions for hydrogen generation
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原位反应条件下合成的高性能铂纳米片用于制氢
DOI：
10.1016/j.jechem.2020.03.064
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发表时间：
2020-12-01
影响因子：
13.1
通讯作者：
Wang, Yong
中科院分区：
文献类型：
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作者：
Bao, Xiaobing;Gong, Yutong;Wang, Yong
催化剂的表面性质，特别是暴露的晶面和配位态，直接影响催化剂的性能。在此，我们说明了反应条件如何指导在析氢反应（HER）的情况下制备具有所需结构的性能良好的催化剂。在HER过程中，稳定吸附在CNTs上的PtClx离子被原位电化学还原成由高指数（311）、低指数（200）和（111）面包围的独特的Pt纳米片结构。实验结果和密度泛函理论（DFT）计算揭示了这些独特结构与反应物之间的作用机理。吸附的H2O和活性物质作为封盖剂保护（311）面，促进水分子的解离，产生的H *中间体在附近的低指数Pt位点上有利地结合和释放。这些活性位点的共同作用使Pt纳米片的活性与20% Pt/C相当，是质量活性的12.7倍。这些发现为合成具有高特异性的多相催化剂提供了新的见解。(c) 2020年由Elsevier B.V.和科学出版社代表科学出版社和中国科学院大连化学物理研究所出版
Surface properties of a catalyst, especially exposed crystal facets and coordination states, directly affect the catalyst's performance. Herein, we illustrate how reaction conditions direct the fabrication of a wellbehaved catalyst with desired structures in the case of hydrogen evolution reaction (HER). Stable adsorbed PtClx ions on CNTs are in situ electrochemically reduced into a unique Pt nanosheet structure enclosed by high-index (311) and low-index (200) and (111) facets during HER process. Experimental results and density functional theory (DFT) calculation disclose the function mechanism between these unique structures and reactants. The adsorbed H2O and reactive species act as capping agents protecting the (311) facet where the dissociation of water molecule is promoted, and the produced H * intermediates favorably combine and release on the nearby low-index Pt sites. The joint collaborations of these active sites afford Pt nanosheets comparable activity to 20 wt% Pt/C and a 12.7-fold over mass activity. These findings provide novel insight into the synthesis of heterogeneous catalysts with high specificity. (c) 2020 Published by Elsevier B.V. and Science Press on behalf of Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences