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Methods of photoelectrode characterization with high spatial and temporal resolution

Esposito, Daniel V. and Baxter, Jason B. and John, Jimmy and Lewis, Nathan S. and Moffat, Thomas P. and Ogitsu, Tadashi and O'Neil, Glen D. and Pham, Tuan Anh and Talin, A. Alec and Velazquez, Jesus M. and Wood, Brandon C. (2015) Methods of photoelectrode characterization with high spatial and temporal resolution. Energy and Environmental Science, 8 (10). pp. 2863-2885. ISSN 1754-5692. doi:10.1039/c5ee00835b.

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Materials and photoelectrode architectures that are highly efficient, extremely stable, and made from low cost materials are required for commercially viable photoelectrochemical (PEC) water-splitting technology. A key challenge is the heterogeneous nature of real-world materials, which often possess spatial variation in their crystal structure, morphology, and/or composition at the nano-, micro-, or macro-scale. Different structures and compositions can have vastly different properties and can therefore strongly influence the overall performance of the photoelectrode through complex structure–property relationships. A complete understanding of photoelectrode materials would also involve elucidation of processes such as carrier collection and electrochemical charge transfer that occur at very fast time scales. We present herein an overview of a broad suite of experimental and computational tools that can be used to define the structure–property relationships of photoelectrode materials at small dimensions and on fast time scales. A major focus is on in situ scanning-probe measurement (SPM) techniques that possess the ability to measure differences in optical, electronic, catalytic, and physical properties with nano- or micro-scale spatial resolution. In situ ultrafast spectroscopic techniques, used to probe carrier dynamics involved with processes such as carrier generation, recombination, and interfacial charge transport, are also discussed. Complementing all of these experimental techniques are computational atomistic modeling tools, which can be invaluable for interpreting experimental results, aiding in materials discovery, and interrogating PEC processes at length and time scales not currently accessible by experiment. In addition to reviewing the basic capabilities of these experimental and computational techniques, we highlight key opportunities and limitations of applying these tools for the development of PEC materials.

Item Type:Article
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URLURL TypeDescription!divAbstractPublisherArticle
Esposito, Daniel V.0000-0002-0550-801X
Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2015 The Royal Society of Chemistry. Received 13 Mar 2015, Accepted 18 Jun 2015; First published online 19 Jun 2015. The authors thank Dr. Eric Miller for the inspiration to compile this review, and the members of the U.S. Department of Energy’s Photoelectrochemical Working Group and Task 35 (Renewable Hydrogen) of the International Energy Agency’s Hydrogen Implementing Agreement for helpful comments, suggestions, and discussions. DVE acknowledges support from the NIST National Research Council postdoctoral Fellowship Program. JMV and NSL would like to acknowledge 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 and the National Science Foundation Grant CHE-1214152. JMV acknowledges support through a NRC Ford Foundation Postdoctoral Fellowship. JJ thanks the Camille and Henry Dreyfus Foundation for financial support through its postdoctoral fellowship program in environmental chemistry. JBB acknowledges support from NSF ECCS-1201957 and NSF CBET-1333649. BW and TO acknowledge support from the Fuel Cell Technologies Program within the DOE Office of Energy Efficiency and Renewable Energy. T.A.P acknowledges support from the Lawrence Fellowship. A portion of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the U.S. DOE National Nuclear Security Administration under Contract DE-AC04-94AL85000. AAT was supported by Science of Precision Multifunctional Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences under award DESC0001160. A summary version of this review paper (DOI: 10.2172/1209497), and associated summary tables that will be updated as the field progresses, will be available on the working group website (
Funding AgencyGrant Number
NIST National Research CouncilUNSPECIFIED
Department of Energy (DOE)DE-SC0004993
NRC Ford Foundation Postdoctoral FellowshipUNSPECIFIED
Camille and Henry Dreyfus FoundationUNSPECIFIED
Camille and Henry Dreyfus FoundationUNSPECIFIED
Lawrence FellowshipUNSPECIFIED
Department of Energy (DOE)DE-AC52-07NA27344
Department of Energy (DOE)DE-AC04-94AL85000
Department of Energy (DOE)DESC0001160
Issue or Number:10
Record Number:CaltechAUTHORS:20151029-140911122
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:61716
Deposited By: Tony Diaz
Deposited On:29 Oct 2015 23:49
Last Modified:10 Nov 2021 22:53

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