Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation
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...
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sg-ntu-dr.10356-1516022021-07-13T03:54:01Z Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation Di, Jun Xia, Jiexiang Chisholm, Matthew F. Zhong, Jun Chen, Chao Cao, Xingzhong Dong, Fan Chi, Zhen Chen, Hailong Weng, Yu-Xiang Xiong, Jun Yang, Shi-Ze Li, Huaming Liu, Zheng Dai, Sheng School of Materials Science and Engineering Centre for Programmable Materials Engineering::Materials Charge Separation Defect Engineering 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 Bi3 O4 Br nanosheets with surface defects is proposed to boost photocatalytic efficiency by simultaneously promoting bulk- and surface-charge separation. Defect-rich single-unit-cell Bi3 O4 Br displays 4.9 and 30.9 times enhanced photocatalytic hydrogen evolution and nitrogen fixation activity, respectively, than bulk Bi3 O4 Br. 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. Ministry of Education (MOE) National Research Foundation (NRF) 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. 2021-07-13T03:54:01Z 2021-07-13T03:54:01Z 2019 Journal Article Di, J., Xia, J., Chisholm, M. F., Zhong, J., Chen, C., Cao, X., Dong, F., Chi, Z., Chen, H., Weng, Y., Xiong, J., Yang, S., 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), e1807576-. https://dx.doi.org/10.1002/adma.201807576 0935-9648 0000-0002-8825-7198 https://hdl.handle.net/10356/151602 10.1002/adma.201807576 31081183 2-s2.0-85065736297 28 31 e1807576 en NRF-RF2013-08 MOE2016-T2-1-131 MOE2018-T3-1-002 2017-T1-001-075 Advanced Materials © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. All rights reserved. |
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Engineering::Materials Charge Separation Defect Engineering Di, Jun Xia, Jiexiang Chisholm, Matthew F. Zhong, Jun Chen, Chao Cao, Xingzhong Dong, Fan Chi, Zhen Chen, Hailong Weng, Yu-Xiang Xiong, Jun Yang, Shi-Ze Li, Huaming Liu, Zheng Dai, Sheng Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
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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 Bi3 O4 Br nanosheets with surface defects is proposed to boost photocatalytic efficiency by simultaneously promoting bulk- and surface-charge separation. Defect-rich single-unit-cell Bi3 O4 Br displays 4.9 and 30.9 times enhanced photocatalytic hydrogen evolution and nitrogen fixation activity, respectively, than bulk Bi3 O4 Br. 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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School of Materials Science and Engineering |
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School of Materials Science and Engineering Di, Jun Xia, Jiexiang Chisholm, Matthew F. Zhong, Jun Chen, Chao Cao, Xingzhong Dong, Fan Chi, Zhen Chen, Hailong Weng, Yu-Xiang Xiong, Jun Yang, Shi-Ze Li, Huaming Liu, Zheng Dai, Sheng |
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Article |
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Di, Jun Xia, Jiexiang Chisholm, Matthew F. Zhong, Jun Chen, Chao Cao, Xingzhong Dong, Fan Chi, Zhen Chen, Hailong Weng, Yu-Xiang Xiong, Jun Yang, Shi-Ze Li, Huaming Liu, Zheng Dai, Sheng |
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Di, Jun |
title |
Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
title_short |
Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
title_full |
Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
title_fullStr |
Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
title_full_unstemmed |
Defect-tailoring mediated electron–hole separation in single-unit-cell Bi₃O₄Br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
title_sort |
defect-tailoring mediated electron–hole separation in single-unit-cell bi₃o₄br nanosheets for boosting photocatalytic hydrogen evolution and nitrogen fixation |
publishDate |
2021 |
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https://hdl.handle.net/10356/151602 |
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1707050390748397568 |