Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl
Abstract
Introducing defects into semiconductor photocatalysts has been identified as an effective approach to extend the visible-light absorption and achieve high-efficiency solar energy conversion. However, the band gap model system of defect states may not truly describe the evolutions in real materials as the narrower band gap would limit the photocatalytic activity via suppressing the charge separation. We report that reorganizing the surface termination in a defective semiconductor plays a key role in determining the photocatalytic performance. We directly observed that the surface reorganizations are accompanied by the formation of defects in layered structured bismuth oxychloride (BiOCl). Both experimental and theoretical results demonstrate that varying terminations have strong effects on the electronic structure and electron–hole pair recombination, which is shown to be the driving force of the promotion of visible-light photocatalytic activity in BiOCl. We also reveal that the surface reorganization induces a novel transfer path and high-dielectric surface to prevent the trapping of charge carriers, highlighting an efficient way of improving the photocatalytic activity by surface reorganization.
- Authors:
-
[1];
[2];
[3];
[4];
[5];
[3];
[6];
- Chongqing Univ. (China). Electron Microscopy Center. College of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
- Chongqing Univ. (China). Electron Microscopy Center. College of Materials Science and Engineering
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences; Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences. Computational Sciences and Engineering Division
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Georgia Institute of Technology, Atlanta, GA (United States); Chongqing Univ. (China)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NSFC); Chongqing Research Program of Basic Research and Frontier Technology (China); Fundamental Research Funds for the Central Universities (China); China Scholarship Council
- OSTI Identifier:
- 1511920
- Grant/Contract Number:
- AC05-00OR22725; AC02-05CH11231; DGE-1650044; 51302329; 51501024; cstc2018jcyjAX0408; cstc2015jcyjA90004; 2018CDQYCL0027; 201606055013
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 15; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE
Citation Formats
Wu, Sujuan, Sun, Weiwei, Sun, Jianguo, Hood, Zachary D., Yang, Shi-Ze, Sun, Lidong, Kent, Paul R. C., and Chisholm, Matthew F. Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b01629.
Wu, Sujuan, Sun, Weiwei, Sun, Jianguo, Hood, Zachary D., Yang, Shi-Ze, Sun, Lidong, Kent, Paul R. C., & Chisholm, Matthew F. Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl. United States. https://doi.org/10.1021/acs.chemmater.8b01629
Wu, Sujuan, Sun, Weiwei, Sun, Jianguo, Hood, Zachary D., Yang, Shi-Ze, Sun, Lidong, Kent, Paul R. C., and Chisholm, Matthew F. Tue .
"Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl". United States. https://doi.org/10.1021/acs.chemmater.8b01629. https://www.osti.gov/servlets/purl/1511920.
@article{osti_1511920,
title = {Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl},
author = {Wu, Sujuan and Sun, Weiwei and Sun, Jianguo and Hood, Zachary D. and Yang, Shi-Ze and Sun, Lidong and Kent, Paul R. C. and Chisholm, Matthew F.},
abstractNote = {Introducing defects into semiconductor photocatalysts has been identified as an effective approach to extend the visible-light absorption and achieve high-efficiency solar energy conversion. However, the band gap model system of defect states may not truly describe the evolutions in real materials as the narrower band gap would limit the photocatalytic activity via suppressing the charge separation. We report that reorganizing the surface termination in a defective semiconductor plays a key role in determining the photocatalytic performance. We directly observed that the surface reorganizations are accompanied by the formation of defects in layered structured bismuth oxychloride (BiOCl). Both experimental and theoretical results demonstrate that varying terminations have strong effects on the electronic structure and electron–hole pair recombination, which is shown to be the driving force of the promotion of visible-light photocatalytic activity in BiOCl. We also reveal that the surface reorganization induces a novel transfer path and high-dielectric surface to prevent the trapping of charge carriers, highlighting an efficient way of improving the photocatalytic activity by surface reorganization.},
doi = {10.1021/acs.chemmater.8b01629},
journal = {Chemistry of Materials},
number = 15,
volume = 30,
place = {United States},
year = {Tue Jul 17 00:00:00 EDT 2018},
month = {Tue Jul 17 00:00:00 EDT 2018}
}
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