Journal
ADVANCED MATERIALS
Volume 31, Issue 28, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201807576
Keywords
charge separation; defect engineering; electronic structure; photocatalytic nitrogen fixation; single-unit-cell Bi3O4Br
Categories
Funding
- National Natural Science Foundation of China [21676128, 21576123]
- Singapore National Research Foundation under NRF RF [NRF-RF201308, MOE2016-T2-1-131, MOE2018-T3-1-002, Tier 1 2017-T1-001-075]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division
- ORNL's Center for Nanophase Materials Sciences - Scientific User Facilities Division of U.S. Department of Energy
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Science Foundation [ACI-1053575, DMR160118]
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Solar photocatalysis is a potential solution to satisfying energy demand and its resulting environmental impact. However, the low electron-hole separation efficiency in semiconductors has slowed the development of this technology. The effect of defects on electron-hole separation is not always clear. A model atomically thin structure of single-unit-cell Bi3O4Br nanosheets with surface defects is proposed to boost photocatalytic efficiency by simultaneously promoting bulk- and surface-charge separation. Defect-rich single-unit-cell Bi3O4Br displays 4.9 and 30.9 times enhanced photocatalytic hydrogen evolution and nitrogen fixation activity, respectively, than bulk Bi3O4Br. After the preparation of single-unit-cell structure, the bismuth defects are controlled to tune the oxygen defects. Benefiting from the unique single-unit-cell architecture and defects, the local atomic arrangement and electronic structure are tuned so as to greatly increase the charge separation efficiency and subsequently boost photocatalytic activity. This strategy provides an accessible pathway for next-generation photocatalysts.
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