Journal
SMALL
Volume 14, Issue 15, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201704319
Keywords
electrocatalysis; media dependence; metal-adsorbate interactions; selectivity; single-atom dispersed catalysts
Categories
Funding
- National Key Basic Research Program of China [2013CB933200]
- Shanghai International Cooperation project [16520710200]
- China National Funds for Distinguished Young Scientists [51225202]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- UCAS Joint PhD Training Program
- Northern Illinois University
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The development of cost-effective catalysts to replace noble metal is attracting increasing interests in many fields of catalysis and energy, and intensive efforts are focused on the integration of transition-metal sites in carbon as noble-metal-free candidates. Recently, the discovery of single-atom dispersed catalyst (SAC) provides a new frontier in heterogeneous catalysis. However, the electrocatalytic application of SAC is still subject to several theoretical and experimental limitations. Further advances depend on a better design of SAC through optimizing its interaction with adsorbates during catalysis. Here, distinctive from previous studies, favorable 3d electronic occupation and enhanced metal-adsorbates interactions in single-atom centers via the construction of nonplanar coordination is achieved, which is confirmed by advanced X-ray spectroscopic and electrochemical studies. The as-designed atomically dispersed cobalt sites within nonplanar coordination show significantly improved catalytic activity and selectivity toward the oxygen reduction reaction, approaching the benchmark Pt-based catalysts. More importantly, the illustration of the active sites in SAC indicates metal-natured catalytic sites and a media-dependent catalytic pathway. Achieving structural and electronic engineering on SAC that promotes its catalytic performances provides a paradigm to bridge the gap between single-atom catalysts design and electrocatalytic applications.
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