Light-Driven Water Oxidation Using Polyelectrolyte Layer-by-Layer Chromophore–Catalyst Assemblies

Leem, Gyu; Sherman, Benjamin D.; Burnett, Alex J.; Morseth, Zachary A.; Wee, Kyung-Ryang; Papanikolas, John M.; Meyer, Thomas J.; Schanze, Kirk S.

doi:10.1021/acsenergylett.6b00171

Title: Light-Driven Water Oxidation Using Polyelectrolyte Layer-by-Layer Chromophore–Catalyst Assemblies

Journal Article · Tue Jun 21 00:00:00 EDT 2016 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.6b00171· OSTI ID:1387883

Leem, Gyu ^[1]; Sherman, Benjamin D. ^[2]; Burnett, Alex J. ^[1]; Morseth, Zachary A. ^[2]; Wee, Kyung-Ryang ^[2]; Papanikolas, John M. ^[2]; Meyer, Thomas J. ^[2]; Schanze, Kirk S. ^[1]

Univ. of Florida, Gainesville, FL (United States)
Univ. of North Carolina, Chapel Hill, NC (United States)

Layer-by-Layer (LbL) polyelectrolyte self-assembly occurs by the alternate exposure of a substrate to solutions of oppositely charged polyelectrolytes or polyions. Here, we report the application of LbL to construct chromophore–catalyst assemblies consisting of a cationic polystyrene-based Ru polychromophore (PS-Ru) and a [Ru(tpy)(2-pyridyl-N-methylbenzimidazole) (OH₂)]²⁺ water oxidation catalyst (RuC), codeposited with poly(acrylic acid) (PAA) as an inert polyanion. These assemblies are deposited onto planar indium tin oxide (ITO, Sn:In₂O₃) substrates for electrochemical characterization and onto mesoporous substrates consisting of a SnO₂/TiO₂ core/shell structure atop fluorine doped tin oxide (FTO) for application to light-driven water oxidation in a dye-sensitized photoelectrosynthesis cell. Cyclic voltammetry and ultraviolet–visible absorption spectroscopy reveal that multilayer deposition progressively increases the film thickness on ITO glass substrates. Under an applied bias, photocurrent measurements of the (PAA/PS-Ru)₅/(PAA/RuC)₅ LbL films formed on FTO//SnO₂/TiO₂ mesoporous core–shell electrodes demonstrate a clear anodic photocurrent response. Prolonged photoelectrolysis experiments, with the use of a dual working electrode collector–generator cell, reveal production of O₂ from the illuminated photoanode with a Faradaic efficiency of 22%. Finally, this is the first report to demonstrate the use of polyelectrolyte LbL to construct chromophore–catalyst assemblies for water oxidation.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

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

Grant/Contract Number:: SC0001011

OSTI ID:: 1387883

Journal Information:: ACS Energy Letters, Vol. 1, Issue 2; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 35 works

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Cited By (3)

Layer-by-layer assembly for photoelectrochemical nanoarchitectonics Kim, Dongseok; Gu, Minsu; Park, Minju Molecular Systems Design & Engineering, Vol. 4, Issue 1 https://doi.org/10.1039/c8me00067k	journal	January 2019
Inorganic Photochemistry and Solar Energy Harvesting: Current Developments and Challenges to Solar Fuel Production Sousa, Sinval F.; Souza, Breno L.; Barros, Cristiane L. International Journal of Photoenergy, Vol. 2019 https://doi.org/10.1155/2019/9624092	journal	January 2019
Polymer-based chromophore–catalyst assemblies for solar energy conversion Leem, Gyu; Sherman, Benjamin D.; Schanze, Kirk S. Nano Convergence, Vol. 4, Issue 1 https://doi.org/10.1186/s40580-017-0132-z	journal	December 2017

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Title: Light-Driven Water Oxidation Using Polyelectrolyte Layer-by-Layer Chromophore–Catalyst Assemblies

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