4.8 Article

Hydrogen Evolution Electrocatalyst Design: Turning Inert Gold into Active Catalyst by Atomically Precise Nanochemistry

期刊

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 29, 页码 11102-11108

出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c04606

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资金

  1. National Science Foundation (NSF) [DMR-1808675]
  2. U.S. Department of Energy, National Energy Technology Laboratory through NETL-Penn State University Coalition for Fossil Energy Research (UCFER) [DE-FE0026825]
  3. U.S. Department of Energy Office of Science User Facility [DE-AC02-05CH11231]

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In this study, a thiolate (SR)-protected Au-36 Ag-2 (SR)(18) nanocluster with low ligand coverage and a core composed of three icosahedral (I-h) units is reported for efficient catalyzing hydrogen evolution reaction (HER). The Au-36 Ag-2 (SR)(18) exhibits high catalytic activity at lower overpotentials due to its low ligand-to-metal ratio, low-coordinated Au atoms and unfilled superatomic orbitals. This study provides a new strategy for constructing highly active catalysts from inert metals by pursuing atomically precise nanoclusters and controlling their geometrical and electronic structures.
Electrocatalytic hydrogen evolution reaction (HER) holds promise in the renewable clean energy scheme. Crystalline Au and Ag are, however, poor in catalyzing HER, and the ligands on colloidal nanoparticles are generally another disadvantage. Herein, we report a thiolate (SR)-protected Au-36 Ag-2 (SR)(18) nanocluster with low coverage of ligands and a core composed of three icosahedral (I-h) units for catalyzing HER efficiently. This trimeric structure, together with the monomeric I-h Au-25 (SR)(18) - and dimeric I-h Au-38 (SR)(24), constitutes a unique series, providing an opportunity for revealing the correlation between the catalytic properties and the catalyst's structure. The Au-36 Ag-2 (SR)(18) surprisingly exhibits high catalytic activity at lower overpotentials for HER due to its low ligand-to-metal ratio, low-coordinated Au atoms and unfilled superatomic orbitals. The current density of Au-36 Ag-2 (SR)(18) at -0.3 V vs RHE is 3.8 and 5.1 times that of Au-25 (SR)(18) - and Au-38 (SR)(24), respectively. Density functional theory (DFT) calculations reveal lower hydrogen binding energy and higher electron affinity of Au-36 Ag-2 (SR)(18) for an energetically feasible HER pathway. Our findings provide a new strategy for constructing highly active catalysts from inert metals by pursuing atomically precise nanoclusters and controlling their geometrical and electronic structures.

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