期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 116, 期 24, 页码 11618-11623出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1821091116
关键词
scanning electrochemistry; oxygen evolution reaction; electron tomography
资金
- National Science Foundation [CHE-1900463, CHE-1900401]
- National Natural Science Foundation of China [51661135011]
- Xiamen University Malaysia Research Fund [XMUMRF/2019-C3/IORI/0001]
- US Department of Energy Office of Science Facility, at Brookhaven National Laboratory [DE-SC0012704]
The catalytic activity of low-dimensional electrocatalysts is highly dependent on their local atomic structures, particularly those less-coordinated sites found at edges and corners; therefore, a direct probe of the electrocatalytic current at specified local sites with true nanoscopic resolution has become critically important. Despite the growing availability of operando imaging tools, to date it has not been possible to measure the electrocatalytic activities from individual material edges and directly correlate those with the local structural defects. Herein, we show the possibility of using feedback and generation/collection modes of operation of the scanning electro-chemical microscope (SECM) to independently image the topography and local electrocatalytic activity with 15-nm spatial resolution. We employed this operando microscopy technique to map out the oxygen evolution activity of a semi-2D nickel oxide nanosheet. The improved resolution and sensitivity enables us to distinguish the higher activities of the materials' edges from that of the fully coordinated surfaces in operando. The combination of spatially resolved electro-chemical information with state-of-the-art electron tomography, that unravels the 3D complexity of the edges, and ab initio calculations allows us to reveal the intricate coordination dependent activity along individual edges of the semi-2D material that is not achievable by other methods. The comparison of the simulated line scans to the experimental data suggests that the catalytic current density at the nanosheet edge is similar to 200 times higher than that at the NiO basal plane.
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