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Title: Anatomy of a Visible Light Activated Photocatalyst for Water Splitting

The supported mixed oxide (Rh 2-yCr yO 3)/(Ga 1-xZn x)(N 1-xO x) photocatalyst, highly active for splitting of H 2O, was extensively characterized for its bulk and surface properties with the objective of developing fundamental structure-photoactivity relationships. Raman and UV-vis spectroscopy revealed that the molecular and electronic structures, respectively, of the oxynitride (Ga 1-xZn x)(N 1-xO x) support are not perturbed by the deposition of the (Rh 2-yCr yO 3) NPs. Photoluminescence (PL) spectroscopy, however, showed that the oxynitride (Ga 1-xZn x)(N 1-xO x) support is the source of excited electrons/holes and the (Rh 2-yCr yO 3) NPs greatly reduce the undesirable recombination of photoexcited electron/holes by acting as efficient electron traps as well as increase the lifetimes of the excitons. High Resolution-XPS and High Sensitivity-LEIS surface analyses reveal that the surfaces of the (Rh 2-yCr yO 3) NPs consist of Rh +3 and Cr +3 mixed oxide species. In Situ AP-XPS help to reveal that the Rh+3 and surface N atoms are involved in water splitting. Dispersed RhOx species on the (Ga 1-xZn x)(N 1-xO x) support and on CrO x NPs were found to be the photocatalytic active sites for H 2 generation and N and Zn sitesmore » from the (Ga 1-xZn x)(N 1-xO x) support are the photocatalytic active site for O 2 generation. In conclusion, the current investigation establishes the fundamental structure-photoactivity relationships of these visible light activated photocatalysts.« less
Authors:
 [1] ;  [1] ;  [2] ;  [2] ;  [3] ;  [3] ;  [3] ;  [4] ;  [5] ;  [6] ;  [4] ;  [1]
  1. Lehigh Univ., Bethlehem, PA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. of Kansas, Lawrence, KS (United States)
  4. Univ. of Tokyo (Japan)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). BioEnergy Science Center (BESC)
  6. (Feng) [Univ. of Kansas, Lawrence, KS (United States)
Publication Date:
Grant/Contract Number:
FG02-93ER14350; AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 7; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Research Org:
Lehigh Univ., Bethlehem, PA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; AP-XPS; HS-LEIS; photocatalysis; photocatalyst; spectroscopy; water splitting
OSTI Identifier:
1440775
Alternate Identifier(s):
OSTI ID: 1461067

Phivilay, Somphonh Peter, Roberts, Charles, Gamalski, Andrew, Stach, Eric A., Zhang, Shiran, Nguyen, Luan, Tang, Yu, Xiong, Anke, Puretzky, Alexander, Tao, Franklin, Domen, Kazunari, and Wachs, Israel E.. Anatomy of a Visible Light Activated Photocatalyst for Water Splitting. United States: N. p., Web. doi:10.1021/acscatal.8b01388.
Phivilay, Somphonh Peter, Roberts, Charles, Gamalski, Andrew, Stach, Eric A., Zhang, Shiran, Nguyen, Luan, Tang, Yu, Xiong, Anke, Puretzky, Alexander, Tao, Franklin, Domen, Kazunari, & Wachs, Israel E.. Anatomy of a Visible Light Activated Photocatalyst for Water Splitting. United States. doi:10.1021/acscatal.8b01388.
Phivilay, Somphonh Peter, Roberts, Charles, Gamalski, Andrew, Stach, Eric A., Zhang, Shiran, Nguyen, Luan, Tang, Yu, Xiong, Anke, Puretzky, Alexander, Tao, Franklin, Domen, Kazunari, and Wachs, Israel E.. 2018. "Anatomy of a Visible Light Activated Photocatalyst for Water Splitting". United States. doi:10.1021/acscatal.8b01388.
@article{osti_1440775,
title = {Anatomy of a Visible Light Activated Photocatalyst for Water Splitting},
author = {Phivilay, Somphonh Peter and Roberts, Charles and Gamalski, Andrew and Stach, Eric A. and Zhang, Shiran and Nguyen, Luan and Tang, Yu and Xiong, Anke and Puretzky, Alexander and Tao, Franklin and Domen, Kazunari and Wachs, Israel E.},
abstractNote = {The supported mixed oxide (Rh2-yCryO3)/(Ga1-xZnx)(N1-xOx) photocatalyst, highly active for splitting of H2O, was extensively characterized for its bulk and surface properties with the objective of developing fundamental structure-photoactivity relationships. Raman and UV-vis spectroscopy revealed that the molecular and electronic structures, respectively, of the oxynitride (Ga1-xZnx)(N1-xOx) support are not perturbed by the deposition of the (Rh2-yCryO3) NPs. Photoluminescence (PL) spectroscopy, however, showed that the oxynitride (Ga1-xZnx)(N1-xOx) support is the source of excited electrons/holes and the (Rh2-yCryO3) NPs greatly reduce the undesirable recombination of photoexcited electron/holes by acting as efficient electron traps as well as increase the lifetimes of the excitons. High Resolution-XPS and High Sensitivity-LEIS surface analyses reveal that the surfaces of the (Rh2-yCryO3) NPs consist of Rh+3 and Cr+3 mixed oxide species. In Situ AP-XPS help to reveal that the Rh+3 and surface N atoms are involved in water splitting. Dispersed RhOx species on the (Ga1-xZnx)(N1-xOx) support and on CrOx NPs were found to be the photocatalytic active sites for H2 generation and N and Zn sites from the (Ga1-xZnx)(N1-xOx) support are the photocatalytic active site for O2 generation. In conclusion, the current investigation establishes the fundamental structure-photoactivity relationships of these visible light activated photocatalysts.},
doi = {10.1021/acscatal.8b01388},
journal = {ACS Catalysis},
number = 7,
volume = 8,
place = {United States},
year = {2018},
month = {6}
}