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Title: Enhanced, robust light-driven H 2 generation by gallium-doped titania nanoparticles

The splitting of water into molecular hydrogen and oxygen with the use of renewable solar energy is considered one of the most promising routes to yield sustainable fuel. In this paper, we report the H 2 evolution performance of gallium doped TiO 2 photocatalysts with varying degrees of Ga dopant. The gallium(III) ions induced significant changes in the structural, textural and electronic properties of TiO 2 nanoparticles, resulting in remarkably enhanced photocatalytic activity and good stability for H 2 production. Ga 3+ ions can act as hole traps that enable a large number of excited electrons to migrate towards the TiO 2 surface, thereby facilitating electron transfer and charge separation. Additionally, the cationic dopant and its induced defects might introduce a mid-gap state, promoting electron migration and prolonging the lifetime of charge carrier pairs. We have discovered that the optimal Ga dopant concentration was 3.125 at% and that the incorporation of platinum (0.5 wt%) as a co-catalyst further improved the H 2 evolution rate up to 5722 μmol g -1 h -1. Pt not only acts as an electron sink, drastically increasing the electron/hole pair lifetime, but it also creates an intimate contact at the heterojunction between Pt and Ga-TiOmore » 2, thus improving the interfacial electron transfer process. Finally, these catalyst design strategies provide new ways of designing transition metal photocatalysts that improve green fuel production from renewable solar energy and water.« less
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [1] ;  [3] ; ORCiD logo [4] ;  [5] ;  [6] ; ORCiD logo [7] ;  [4] ; ORCiD logo [1] ; ORCiD logo [4]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; Stony Brook Univ., NY (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.; National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Photon Sciences Division. National Synchrotron Light Source II
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  6. Spanish National Research Council (CSIC), Madrid (Spain). Inst. of Catalysis and Petroleum Chemistry
  7. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division. Advanced Photon Source
Publication Date:
Report Number(s):
BNL-203311-2018-JAAM; BNL-203344-2018-JAAM
Journal ID: ISSN 1463-9076
Grant/Contract Number:
SC0012704; AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 3; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Research Org:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
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; 14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY
OSTI Identifier:
1425095
Alternate Identifier(s):
OSTI ID: 1426455