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Title: Enhanced, robust light-driven H2 generation by gallium-doped titania nanoparticles

Abstract

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 H2 evolution performance of gallium doped TiO2 photocatalysts with varying degrees of Ga dopant. The gallium(III) ions induced significant changes in the structural, textural and electronic properties of TiO2 nanoparticles, resulting in remarkably enhanced photocatalytic activity and good stability for H2 production. Ga3+ ions can act as hole traps that enable a large number of excited electrons to migrate towards the TiO2 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 H2 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-TiO2, thus improving the interfacial electron transfer process. Finally, thesemore » 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 [2];  [4];  [5]; ORCiD logo [6];  [2]; ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Chemistry Department, Brookhaven National Laboratory; Upton; USA; Department of Chemistry, Stony Brook University, Stony Brook; USA
  2. Chemistry Department, Brookhaven National Laboratory; Upton; USA
  3. Photon Sciences Division, National Synchrotron Light Source II, Brookhaven National Laboratory; Upton; USA
  4. Center for Functional Nanomaterials, Brookhaven National Laboratory; Upton; USA
  5. CSIC – Instituto de Catalisis y Petroleoquimica Cantoblanco; E-28049 Madrid; Spain
  6. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory; Argonne; USA
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1421970
Alternate Identifier(s):
OSTI ID: 1425095; OSTI ID: 1426455
Report Number(s):
BNL-203311-2018-JAAM; BNL-203344-2018-JAAM
Journal ID: ISSN 1463-9076; PPCPFQ; 141343
Grant/Contract Number:  
SC0012704; AC02-06CH11357
Resource 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
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 14 SOLAR ENERGY; 77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Luo, Si, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Waluyo, Iradwikanari, Palomino, Robert M., Gamalski, Andrew D., Barrio, Laura, Xu, Wenqian, Polyansky, Dmitry E., Rodriguez, José A., and Senanayake, Sanjaya D. Enhanced, robust light-driven H2 generation by gallium-doped titania nanoparticles. United States: N. p., 2017. Web. doi:10.1039/c7cp04155a.
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Luo, Si, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Waluyo, Iradwikanari, Palomino, Robert M., Gamalski, Andrew D., Barrio, Laura, Xu, Wenqian, Polyansky, Dmitry E., Rodriguez, José A., & Senanayake, Sanjaya D. Enhanced, robust light-driven H2 generation by gallium-doped titania nanoparticles. United States. https://doi.org/10.1039/c7cp04155a
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Luo, Si, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Waluyo, Iradwikanari, Palomino, Robert M., Gamalski, Andrew D., Barrio, Laura, Xu, Wenqian, Polyansky, Dmitry E., Rodriguez, José A., and Senanayake, Sanjaya D. Thu . "Enhanced, robust light-driven H2 generation by gallium-doped titania nanoparticles". United States. https://doi.org/10.1039/c7cp04155a. https://www.osti.gov/servlets/purl/1421970.
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@article{osti_1421970,
title = {Enhanced, robust light-driven H2 generation by gallium-doped titania nanoparticles},
author = {Luo, Si and Nguyen-Phan, Thuy-Duong and Vovchok, Dimitriy and Waluyo, Iradwikanari and Palomino, Robert M. and Gamalski, Andrew D. and Barrio, Laura and Xu, Wenqian and Polyansky, Dmitry E. and Rodriguez, José A. and Senanayake, Sanjaya D.},
abstractNote = {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 H2 evolution performance of gallium doped TiO2 photocatalysts with varying degrees of Ga dopant. The gallium(III) ions induced significant changes in the structural, textural and electronic properties of TiO2 nanoparticles, resulting in remarkably enhanced photocatalytic activity and good stability for H2 production. Ga3+ ions can act as hole traps that enable a large number of excited electrons to migrate towards the TiO2 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 H2 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-TiO2, 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.},
doi = {10.1039/c7cp04155a},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 3,
volume = 20,
place = {United States},
year = {Thu Dec 14 00:00:00 EST 2017},
month = {Thu Dec 14 00:00:00 EST 2017}
}
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https://doi.org/10.1039/c7cp04155a
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