Light-Driven Water Splitting Mediated by Photogenerated Bromine

Sheridan, Matthew V.; Wang, Ying; Wang, Degao; Troian-Gautier, Ludovic; Dares, Christopher J.; Sherman, Benjamin D.; Meyer, Thomas J.

doi:10.1002/anie.201708879

Light-Driven Water Splitting Mediated by Photogenerated Bromine

Journal Article · Wed Jan 31 04:00:00 EST 2018 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201708879· OSTI ID:1470106

^[1]; Wang, Ying ^[2]; Wang, Degao ^[2]; ^[2]; ^[1]; ^[3]; ^[2]

Florida International Univ., Miami, FL (United States)
Univ. of North Carolina, Chapel Hill, NC (United States)
Texas Christian Univ. (TCU), Fort Worth, TX (United States)

Light-driven water splitting was attained using a dye-sensitized mesoporous oxide film and the oxidation of bromide (Br–) to bromine (Br₂) or tribromide (Br₃–). The chemical oxidant (Br₂ or Br₃–) is formed during illumination at the photoanode and used as a sacrificial oxidant to drive a water oxidation catalyst (WOC), here shown using [Ru(bda)(pic)₂], (1; pic=picoline, bda=2,2'-bipyridine-6,6'-dicarboxylate). The photochemical oxidation of bromide produces a chemical oxidant with a possibility of 1.09 V vs. NHE for the Br₂/Br– couple or 1.05 V vs. NHE for the Br₃–/Br– couple, which is sufficient to drive water oxidation at 1 (Ru^V/IV≈1.0 V vs. NHE at pH 5.6). At pH 5.6, using a 0.2 _M acetate buffer containing 40 mm LiBr and the [Ru(4,4'-PO3H2-bpy)(bpy)₂]²⁺ (RuP²⁺, bpy=2,2'-bipyridine) chromophore dye on a SnO₂/TiO₂ core–shell electrode resulted in a photocurrent density of around 1.2 mA cm^–2 under approximately 1 Sun illumination and a Faradaic efficiency upon addition of 1 of 77 % for oxygen evolution.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of North Carolina, Chapel Hill, NC (United States). Energy Frontier Research Center (EFRC) Center for Solar Fuels (UNC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0001011

OSTI ID:: 1470106

Alternate ID(s):: OSTI ID: 1423382

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 13 Vol. 57; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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