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

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.

doi:10.1039/c7cp04155a

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

Journal Article · Thu Dec 14 00:00:00 EST 2017 · Physical Chemistry Chemical Physics. PCCP (Print)

DOI:https://doi.org/10.1039/c7cp04155a· OSTI ID:1421970

Luo, Si ^[1];

^[2];

^[1]; Waluyo, Iradwikanari ^[3];

^[2]; Gamalski, Andrew D. ^[4]; Barrio, Laura ^[5];

^[6]; Polyansky, Dmitry E. ^[2];

^[1];

^[2]

Chemistry Department, Brookhaven National Laboratory; Upton; USA; Department of Chemistry, Stony Brook University, Stony Brook; USA
Chemistry Department, Brookhaven National Laboratory; Upton; USA
Photon Sciences Division, National Synchrotron Light Source II, Brookhaven National Laboratory; Upton; USA
Center for Functional Nanomaterials, Brookhaven National Laboratory; Upton; USA
CSIC – Instituto de Catalisis y Petroleoquimica Cantoblanco; E-28049 Madrid; Spain
X-ray Science Division, Advanced Photon Source, Argonne National Laboratory; Argonne; USA

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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States); Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-06CH11357

OSTI ID:: 1421970

Alternate ID(s):: OSTI ID: 1425095; OSTI ID: 1426455

Report Number(s):: BNL-203311-2018-JAAM; BNL-203344-2018-JAAM; PPCPFQ; 141343

Journal Information:: Physical Chemistry Chemical Physics. PCCP (Print), Vol. 20, Issue 3; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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