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A comparison of the chemical, optical and electrocatalytic properties of water-oxidation catalysts for use in integrated solar-fuel generators

Sun, Ke and Moreno-Hernandez, Ivan A. and Schmidt, William C. and Zhou, Xinghao and Crompton, J. Chance and Liu, Rui and Saadi, Fadl H. and Chen, Yikai and Papadantonakis, Kimberly M. and Lewis, Nathan S. (2017) A comparison of the chemical, optical and electrocatalytic properties of water-oxidation catalysts for use in integrated solar-fuel generators. Energy and Environmental Science, 10 (4). pp. 987-1002. ISSN 1754-5692. doi:10.1039/C6EE03563A.

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The in situ optical properties and electrocatalytic performance of representative catalysts for the oxygen-evolution reaction (OER) have been considered together to evaluate system-level effects that accompany the integration of OER catalysts into a solar-fuel device driven by a tandem-junction light absorber with a photoanode top cell, i.e., a design that requires incident light to be transmitted through the OER catalyst before reaching a semiconducting light absorber. The relationship between the overpotential and optical transmission of the catalysts determined the attainable efficiencies for integrated solar-fuel devices as well as the optimal band gaps for the photoanode in such devices. The systems investigated generally showed: (1) the OER catalysts dissolved in acid, and were less stable in buffered near-neutral pH electrolytes than in strongly alkaline electrolytes; (2) higher overpotentials were required to drive the OER at a specified current density when the catalysts were operated in contact with near-neutral pH electrolytes than strong alkaline electrolytes; (3) for some of the OER catalysts, the electrocatalytic activity and in situ absorption spectra depended strongly on the preparation method; (4) increasing the loading of the electrocatalyst reduced the overpotential and the optical transmission; (5) for the catalysts studied, the optical transmission and overpotential were generally correlated, and the trend lines did not cross, indicating that based on these factors alone, the optimal approach is to use lower loadings of highly active catalysts, rather than to use a less active but more transparent catalysts; (6) for a solar-fuel device driven by semiconductors operating at the Shockley–Queisser limit and using a continuous film of a given OER catalyst in the path of incident light, the efficiency decrease due to the reduced optical transmittance that accompanies increased OER catalyst loading can be substantially greater than any efficiency increase that might be gained through the reduction in catalytic overpotential by increasing the catalyst loading; and (7) HER catalysts possessed the same performance trade-off when the light is incident through the HER catalysts as is observed for OER catalysts when the light is incident from the OER side.

Item Type:Article
Related URLs:
URLURL TypeDescription Information
Sun, Ke0000-0001-8209-364X
Moreno-Hernandez, Ivan A.0000-0001-6461-9214
Zhou, Xinghao0000-0001-9229-7670
Saadi, Fadl H.0000-0003-3941-0464
Papadantonakis, Kimberly M.0000-0002-9900-5500
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2017 Royal Society of Chemistry. Received 7th December 2016 , Accepted 9th March 2017. First published on the web 9th March 2017. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award No. DE-SC0004993. This work was also supported by the Gordon and Betty Moore Foundation under Award No. GBMF1225. This material is also based upon work supported by the National Science Foundation Graduate Research Fellowship under Grant No. DGE-1144469 (IAM).
Group:JCAP, Kavli Nanoscience Institute
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Gordon and Betty Moore FoundationGBMF1225
NSF Graduate Research FellowshipDGE-1144469
Issue or Number:4
Record Number:CaltechAUTHORS:20170331-105139021
Persistent URL:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:75584
Deposited By: George Porter
Deposited On:31 Mar 2017 18:16
Last Modified:15 Nov 2021 16:34

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