Surface Reorganization Leads to Enhanced Photocatalytic Activity in Defective BiOCl

Sujuan Wu, Weiwei Sun, Jianguo Sun, Zachary D. Hood, Shi Ze Yang, Lidong Sun, Paul R.C. Kent, Matthew F. Chisholm

Research output: Contribution to journalArticlepeer-review

59 Scopus citations

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. Here, 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.

Original languageEnglish
Pages (from-to)5128-5136
Number of pages9
JournalChemistry of Materials
Volume30
Issue number15
DOIs
StatePublished - Aug 14 2018

Funding

This research was financially supported by the National Natural Science Foundation of China (51302329 and 51501024), the Chongqing Research Program of Basic Research and Frontier Technology (cstc2018jcyjAX0408 and cstc2015jcyjA90004), the Fundamental Research Funds for the Central Universities (2018CDQYCL0027), and the China Scholarship Council (201606055013). The authors gratefully acknowledge the valuable experimental support from Mr. Yuqi Zhang and Dr. Yuan Yuan and helpful editing form Mr. Arashdeep Singh Thind. Theoretical calculations (W.S. and P.R.C.K.) were supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. This research used resources of the National Energy Research Scientific Computing Center, a U.S. Department of Energy (DOE) Office of Science User Facility supported by the Office of Science of the DOE under Contract DE-AC02-05CH11231. Z.D.H. gratefully acknowledges support from the National Science Foundation Graduate Research Fellowship under Grant DGE-1650044 and the Georgia Tech-ORNL Fellowship. A portion of this research was completed at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User facility. S.-Z.Y. and M.F.C. gratefully acknowledge support from the DOE, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division.

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