Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 137, Issue 12, Pages 4223-4229Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.5b01006
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Funding
- University of Delaware Research Foundation Strategic Initiatives (UDRF-SI) grant
- National Natural Science Foundation of China [21006024]
- Fundamental Research Funds for the Central Universities [WB 1213004-1]
- New Century Excellent Talents in University [NCET-11-0644]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-98CH10886]
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Oxygen evolution from water poses a significant challenge in solar fuel production because it requires an efficient catalyst to bridge the one-electron photon capture process with the four-electron oxygen evolution reaction (OER). Here, a new strategy was developed to synthesize nonsupported ultrasmall cobalt oxide nanocubanes through an in situ phase transformation mechanism using a layered Co(OH)(OCH3) precursor. Under sonication, the precursor was exfoliated and transformed into cobalt oxide nanocubanes in the presence of NaHCO3-Na2SiF6 buffer solution. The resulting cobalt catalyst with an average particle size less than 2 nm exhibited a turnover frequency of 0.023 per second per cobalt in photocatalytic water oxidation. X-ray absorption results suggested a unique nanocubane structure, where 13 cobalt atoms fully coordinated with oxygen in an octahedral arrangement to form 8 Co4O4 cubanes, which may be responsible for the exceptionally high OER activity.
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