Defect-Tailoring Mediated Electron–Hole Separation in Single-Unit-Cell Bi3O4Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation

Jun Di; Jiexiang Xia; Matthew F. Chisholm; Jun Zhong; Chao Chen; Xingzhong Cao; Fan Dong; Zhen Chi; Hailong Chen; Yu Xiang Weng; Jun Xiong; Shi Ze Yang; Huaming Li; Zheng Liu; Sheng Dai

doi:10.1002/adma.201807576

Defect-Tailoring Mediated Electron–Hole Separation in Single-Unit-Cell Bi₃O₄Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation

Jun Di, Jiexiang Xia, Matthew F. Chisholm, Jun Zhong, Chao Chen, Xingzhong Cao, Fan Dong, Zhen Chi, Hailong Chen, Yu Xiang Weng, Jun Xiong, Shi Ze Yang, Huaming Li, Zheng Liu, Sheng Dai

Chemical Sciences Division

Research output: Contribution to journal › Article › peer-review

373 Scopus citations

Abstract

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.

Original language	English
Article number	1807576
Journal	Advanced Materials
Volume	31
Issue number	28
DOIs	https://doi.org/10.1002/adma.201807576
State	Published - Jul 12 2019

Funding

This work was financially supported by the National Natural Science Foundation of China (Nos. 21676128 and 21576123) and Singapore National Research Foundation under NRF RF Award No. NRF-RF2013-08, MOE2016-T2-1-131, MOE2018-T3-1-002, Tier 1 2017-T1-001-075. The electron microscopy done at ORNL (S.-Z.Y. and M.F.C.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user project supported by ORNL's Center for Nanophase Materials Sciences, which was sponsored by the Scientific User Facilities Division of U.S. Department of Energy. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation under Grant Nos. ACI-1053575 and DMR160118. This work was financially supported by the National Natural Science Foundation of China (Nos. 21676128 and 21576123) and Singapore National Research Foundation under NRF RF Award No. NRF-RF2013-08, MOE2016-T2-1-131, MOE2018-T3-1-002, Tier 1 2017-T1-001-075. The electron microscopy done at ORNL (S.-Z.Y. and M.F.C.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user project supported by ORNL’s Center for Nanophase Materials Sciences, which was sponsored by the Scientific User Facilities Division of U.S. Department of Energy. This research used resources of the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. This work used the Extreme Science and Engineering Discovery Environment (XSEDE), which was supported by National Science Foundation under Grant Nos. ACI-1053575 and DMR160118.

Keywords

charge separation
defect engineering
electronic structure
photocatalytic nitrogen fixation
single-unit-cell BiOBr

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1002/adma.201807576

Cite this

Di, J., Xia, J., Chisholm, M. F., Zhong, J., Chen, C., Cao, X., Dong, F., Chi, Z., Chen, H., Weng, Y. X., Xiong, J., Yang, S. Z., Li, H., Liu, Z., & Dai, S. (2019). Defect-Tailoring Mediated Electron–Hole Separation in Single-Unit-Cell Bi₃O₄Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation. Advanced Materials, 31(28), Article 1807576. https://doi.org/10.1002/adma.201807576

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title = "Defect-Tailoring Mediated Electron–Hole Separation in Single-Unit-Cell Bi3O4Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation",

abstract = "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.",

keywords = "charge separation, defect engineering, electronic structure, photocatalytic nitrogen fixation, single-unit-cell BiOBr",

author = "Jun Di and Jiexiang Xia and Chisholm, {Matthew F.} and Jun Zhong and Chao Chen and Xingzhong Cao and Fan Dong and Zhen Chi and Hailong Chen and Weng, {Yu Xiang} and Jun Xiong and Yang, {Shi Ze} and Huaming Li and Zheng Liu and Sheng Dai",

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Di, J, Xia, J, Chisholm, MF, Zhong, J, Chen, C, Cao, X, Dong, F, Chi, Z, Chen, H, Weng, YX, Xiong, J, Yang, SZ, Li, H, Liu, Z & Dai, S 2019, 'Defect-Tailoring Mediated Electron–Hole Separation in Single-Unit-Cell Bi₃O₄Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation', Advanced Materials, vol. 31, no. 28, 1807576. https://doi.org/10.1002/adma.201807576

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