期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 9, 页码 5020-5028出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.0c09289
关键词
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资金
- Austrian Academy of Sciences at the Institute of Physical Chemistry
- China Scholarship Council
- German Research Foundation (DFG) [Strategy-EXC 2089/1-390776260]
- Austrian Science Fund (FWF) [I-4114-N37]
Copper (Cu) exhibits structural dynamics and atomic density decrease at its potential of zero free charge (pzfc) in alkaline electrolyte, with a shift towards more positive potentials per decreasing pH unit. At higher potentials, full reconstruction and electric field dependent OH adsorption occurs, leading to a decrease in the atomic density of the first Cu layer.
Copper (Cu) is a unique electrocatalyst, which is able to efficiently oxidize CO at very low overpotentials and reduce CO2 to valuable fuels with reasonable Faradaic efficiencies. Yet, knowledge of its electro-chemical properties at the solid/liquid interface is still scarce. Here, we present the first two-stranded correlation of the potential of zero free charge (pzfc) of Cu(111) in alkaline electrolyte at different pH values through application of nanosecond laser pulses and the corresponding interfacial structure changes by in situ electrochemical scanning tunneling microscopy imaging. The pzfc of Cu(111) at pH 13 is identified at -0.73 V-SHE in the apparent double layer region, prior to the onset of hydroxide adsorption. It shifts by (88 +/- 4) mV to more positive potentials per decreasing pH unit. At the pzfc, Cu(111) shows structural dynamics at both pH 13 and pH 11, which can be understood as the onset of surface restructuring. At higher potentials, full reconstruction and electric field dependent OH adsorption occurs, which causes a remarkable decrease in the atomic density of the first Cu layer. The expansion of the Cu-Cu distance to 0.3 nm generates a hexagonal Moire pattern, on which the adsorbed OH forms a commensurate (1 x 2) adlayer structure with a steady state coverage of 0.5 monolayers at pH 13. Our experimental findings shed light on the true charge distribution and its interrelation with the atomic structure of the electrochemical interface of Cu.
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