期刊
ACS CATALYSIS
卷 10, 期 3, 页码 2026-2032出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b03814
关键词
twin boundary; CO2 reduction; one-dimensional catalyst; intrinsic activity; copper; methane
资金
- National Natural Science Foundation of China [21771040]
- National Key Research and Development Program of China [2017YFA0207303, 2016YFA0203900]
- 1000 Plan Program for Young Talents
- National Science Foundation [1900039]
- Welch Foundation [F-1959-20180324]
- DOE's Office of EERE
- Extreme Science and Engineering Discovery Environment (XSEDE) [TG-CHE190065]
- Center for Nanoscale Materials (a DOE Office of Science user facility) at Argonne National Lab [DE-AC02-06CH113.57]
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [1900039] Funding Source: National Science Foundation
Electrocatalysts are evolving toward chemically tunable atomic structures, among which the catalyst engineering from a defect perspective represents one of the mainstream technical genres. However, most defects cannot be purified or their numbers gauged, making them too complex to explore the hidden catalytic mechanism. A twin boundary, with well-defined symmetric structure and high electrocatalytic activity, is an elegant one-dimensional model catalyst in pursuing such studies. Here on polished Cu electrodes, we successfully synthesized a series of copper twin boundaries, whose density ranges from 0 to 10(5) cm(-1). The CH4 turnover frequency on the twin boundary atoms is 3 orders higher than that on the plane atoms, and the local partial current density reaches 1294 mA cm(-2), with an intrinsic Faradaic efficiency of 92%. An intermediate experiment and density functional theory studies confirm the twin boundary's advantage in converting the absorbed CO* into CH4.
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