期刊
ADVANCED MATERIALS
卷 31, 期 52, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201903491
关键词
photocatalysis; single-metal-atom-oxides; single-site mechanism
类别
资金
- Key Project of National Natural Science Foundation of China [91860202]
- National Natural Science Foundation of China [11404014, 51471008, 11327901, 51872008]
- 111 project [DB18015]
- Natural Science Foundation of Beijing Municipality [Z180014, 2192008]
- Beijing Outstanding Young Scientists Projects [BJJWZYJH01201910005018]
- U.S. National Science Foundation [DMREF-1627028]
Metal oxides, as one of the mostly abundant and widely utilized materials, are extensively investigated and applied in environmental remediation and protection, and in energy conversion and storage. Most of these diverse applications are the result of a large diversity of the electronic states of metal oxides. Noticeably, however, many metal oxides present obstacles for applications in catalysis, mainly due to the lack of efficient active sites with desired electronic states. Here, the fabrication of single-tungsten-atom-oxide (STAO) is demonstrated, in which the metal oxide's volume reaches its minimum as a unit cell. The catalytic mechanism in the STAO is determined by a new single-site physics mechanism, named as quasi-atom physics. The photogenerated electron transfer process is enabled by an electron in the spin-up channel excited from the highest occupied molecular orbital to the lowest unoccupied molecular orbital +1 state, which can only occur in STAO with W5+. STAO results in a record-high and stable sunlight photocatalytic degradation rate of 0.24 s(-1), which exceeds the rates of available photocatalysts by two orders of magnitude. The fabrication of STAO and its unique quasi-atom photocatalytic mechanism lays new ground for achieving novel physical and chemical properties using single-metal-atom oxides (SMAO).
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