Silicon Photoelectrode Thermodynamics and Hydrogen Evolution Kinetics Measured by Intensity-Modulated High-Frequency Resistivity Impedance Spectroscopy

Anderson, Nicholas C.; Carroll, Gerard M.; Pekarek, Ryan T.; Christensen, Steven T.; van de Lagemaat, Jao; Neale, Nathan R.

doi:10.1021/acs.jpclett.7b01311

Title: Silicon Photoelectrode Thermodynamics and Hydrogen Evolution Kinetics Measured by Intensity-Modulated High-Frequency Resistivity Impedance Spectroscopy

Journal Article · Thu Oct 05 00:00:00 EDT 2017 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.7b01311· OSTI ID:1402562

Anderson, Nicholas C. ^[1]; Carroll, Gerard M. ^[1]; Pekarek, Ryan T. ^[2]; Christensen, Steven T. ^[1]; van de Lagemaat, Jao ^[1];

^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); The Univ. of Texas at Austin, Austin, TX (United States)

Here, we present an impedance technique based on light intensity-modulated high-frequency resistivity (IMHFR) that provides a new way to elucidate both the thermodynamics and kinetics in complex semiconductor photoelectrodes. We apply IMHFR to probe electrode interfacial energetics on oxide-modified semiconductor surfaces frequently used to improve the stability and efficiency of photoelectrochemical water splitting systems. Combined with current density-voltage measurements, the technique quantifies the overpotential for proton reduction relative to its thermodynamic potential in Si photocathodes coated with three oxides (SiO_x, TiO₂, and Al₂O₃) and a Pt catalyst. In pH 7 electrolyte, the flatband potentials of TiO_2^- and Al₂O₃-coated Si electrodes are negative relative to samples with native SiO_x, indicating that SiO_x is a better protective layer against oxidative electrochemical corrosion than ALD-deposited crystalline TiO₂ or Al₂O₃. Adding a Pt catalyst to SiO_x/Si minimizes proton reduction overpotential losses but at the expense of a reduction in available energy characterized by a more negative flatband potential relative to catalyst-free SiO_x/Si.

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Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

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

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1402562

Report Number(s):: NREL/JA-5900-68410

Journal Information:: Journal of Physical Chemistry Letters, Vol. 8, Issue 21; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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References (37)

Artificial Photosynthesis: Solar Splitting of Water to Hydrogen and Oxygen Bard, Allen J.; Fox, Marye Anne Accounts of Chemical Research, Vol. 28, Issue 3 https://doi.org/10.1021/ar00051a007	journal	March 1995
Powering the planet: Chemical challenges in solar energy utilization Lewis, N. S.; Nocera, D. G. Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735 https://doi.org/10.1073/pnas.0603395103	journal	October 2006
Solar Water Splitting Cells Walter, Michael G.; Warren, Emily L.; McKone, James R. Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473 https://doi.org/10.1021/cr1002326	journal	November 2010
Enabling Silicon for Solar-Fuel Production Sun, Ke; Shen, Shaohua; Liang, Yongqi Chemical Reviews, Vol. 114, Issue 17 https://doi.org/10.1021/cr300459q	journal	January 2014
Solar-to-hydrogen efficiency: shining light on photoelectrochemical device performance Döscher, H.; Young, J. L.; Geisz, J. F. Energy & Environmental Science, Vol. 9, Issue 1 https://doi.org/10.1039/C5EE03206G	journal	January 2016
A graded catalytic–protective layer for an efficient and stable water-splitting photocathode Gu, Jing; Aguiar, Jeffery A.; Ferrere, Suzanne Nature Energy, Vol. 2, Issue 2 https://doi.org/10.1038/nenergy.2016.192	journal	January 2017
Direct solar-to-hydrogen conversion via inverted metamorphic multi-junction semiconductor architectures Young, James L.; Steiner, Myles A.; Döscher, Henning Nature Energy, Vol. 2, Issue 4 https://doi.org/10.1038/nenergy.2017.28	journal	March 2017
Remarkable stability of unmodified GaAs photocathodes during hydrogen evolution in acidic electrolyte Young, J. L.; Steirer, K. X.; Dzara, M. J. Journal of Materials Chemistry A, Vol. 4, Issue 8 https://doi.org/10.1039/C5TA07648J	journal	January 2016
Highly active oxide photocathode for photoelectrochemical water reduction Paracchino, Adriana; Laporte, Vincent; Sivula, Kevin Nature Materials, Vol. 10, Issue 6 https://doi.org/10.1038/nmat3017	journal	May 2011
Electrochemical Synthesis of p-Type CuFeO ₂ Electrodes for Use in a Photoelectrochemical Cell Read, Carrie G.; Park, Yiseul; Choi, Kyoung-Shin The Journal of Physical Chemistry Letters, Vol. 3, Issue 14 https://doi.org/10.1021/jz300709t	journal	July 2012
All First Row Transition Metal Oxide Photoanode for Water Splitting Based on Cu ₃ V ₂ O ₈ Seabold, Jason A.; Neale, Nathan R. Chemistry of Materials, Vol. 27, Issue 3 https://doi.org/10.1021/cm504327f	journal	January 2015
Synthesis and Characterization of CuV ₂ O ₆ and Cu ₂ V ₂ O ₇ : Two Photoanode Candidates for Photoelectrochemical Water Oxidation Guo, Wenlong; Chemelewski, William D.; Mabayoje, Oluwaniyi The Journal of Physical Chemistry C, Vol. 119, Issue 49 https://doi.org/10.1021/acs.jpcc.5b07219	journal	November 2015
Solar fuel photoanodes prepared by inkjet printing of copper vanadates Newhouse, P. F.; Boyd, D. A.; Shinde, A. Journal of Materials Chemistry A, Vol. 4, Issue 19 https://doi.org/10.1039/C6TA01252C	journal	January 2016
Chromium doped copper vanadate photoanodes for water splitting Cardenas-Morcoso, Drialys; Peiro-Franch, Anna; Herraiz-Cardona, Isaac Catalysis Today, Vol. 290 https://doi.org/10.1016/j.cattod.2016.11.002	journal	July 2017
Solar Water Oxidation by Composite Catalyst/α-Fe ₂ O ₃ Photoanodes Zhong, Diane K.; Sun, Jianwei; Inumaru, Hiroki Journal of the American Chemical Society, Vol. 131, Issue 17 https://doi.org/10.1021/ja9016478	journal	May 2009
Solar Water Splitting: Progress Using Hematite (α-Fe2O3) Photoelectrodes Sivula, Kevin; Le Formal, Florian; Grätzel, Michael ChemSusChem, Vol. 4, Issue 4 https://doi.org/10.1002/cssc.201000416	journal	March 2011
Splitting water with rust: hematite photoelectrochemistry Hamann, Thomas W. Dalton Transactions, Vol. 41, Issue 26 https://doi.org/10.1039/c2dt30340j	journal	January 2012
Efficient solar water splitting by enhanced charge separation in a bismuth vanadate-silicon tandem photoelectrode Abdi, Fatwa F.; Han, Lihao; Smets, Arno H. M. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3195	journal	July 2013
Efficient solar photoelectrolysis by nanoporous Mo:BiVO ₄ through controlled electron transport Seabold, Jason A.; Zhu, Kai; Neale, Nathan R. Phys. Chem. Chem. Phys., Vol. 16, Issue 3 https://doi.org/10.1039/C3CP54356K	journal	January 2014
Nanoporous BiVO₄ Photoanodes with Dual-Layer Oxygen Evolution Catalysts for Solar Water Splitting Kim, Tae Woo; Choi, Kyoung-Shin Science, Vol. 343, Issue 6174, p. 990-994 https://doi.org/10.1126/science.1246913	journal	February 2014
Photoelectrocatalytic Water Splitting: Significance of Cocatalysts, Electrolyte, and Interfaces Ding, Chunmei; Shi, Jingying; Wang, Zhiliang ACS Catalysis, Vol. 7, Issue 1 https://doi.org/10.1021/acscatal.6b03107	journal	December 2016
Catalyst or spectator? Gamelin, Daniel R. Nature Chemistry, Vol. 4, Issue 12 https://doi.org/10.1038/nchem.1514	journal	November 2012
Dynamics of photogenerated holes in surface modified -Fe2O3 photoanodes for solar water splitting Barroso, M.; Mesa, C. A.; Pendlebury, S. R. Proceedings of the National Academy of Sciences, Vol. 109, Issue 39 https://doi.org/10.1073/pnas.1118326109	journal	July 2012
Kinetics and mechanism of light-driven oxygen evolution at thin film α-Fe2O3 electrodes Cummings, Charles Y.; Marken, Frank; Peter, Laurence M. Chemical Communications, Vol. 48, Issue 14 https://doi.org/10.1039/c2cc16382a	journal	January 2012
Water Oxidation at Hematite Photoelectrodes: The Role of Surface States Klahr, Benjamin; Gimenez, Sixto; Fabregat-Santiago, Francisco Journal of the American Chemical Society, Vol. 134, Issue 9 https://doi.org/10.1021/ja210755h	journal	February 2012
Electrochemical and photoelectrochemical investigation of water oxidation with hematite electrodes Klahr, Benjamin; Gimenez, Sixto; Fabregat-Santiago, Francisco Energy & Environmental Science, Vol. 5, Issue 6 https://doi.org/10.1039/c2ee21414h	journal	January 2012
Photoelectrochemical and Impedance Spectroscopic Investigation of Water Oxidation with “Co–Pi”-Coated Hematite Electrodes Klahr, Benjamin; Gimenez, Sixto; Fabregat-Santiago, Francisco Journal of the American Chemical Society, Vol. 134, Issue 40 https://doi.org/10.1021/ja306427f	journal	September 2012
Kinetic analysis of photoelectrochemical water oxidation by mesostructured Co-Pi/α-Fe ₂ O ₃ photoanodes Carroll, Gerard M.; Gamelin, Daniel R. Journal of Materials Chemistry A, Vol. 4, Issue 8 https://doi.org/10.1039/C5TA06978E	journal	January 2016
Photocurrent of BiVO ₄ is limited by surface recombination, not surface catalysis Zachäus, Carolin; Abdi, Fatwa F.; Peter, Laurence M. Chemical Science, Vol. 8, Issue 5 https://doi.org/10.1039/C7SC00363C	journal	January 2017
Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation Hu, S.; Shaner, M. R.; Beardslee, J. A. Science, Vol. 344, Issue 6187 https://doi.org/10.1126/science.1251428	journal	May 2014
Semiconductor interfacial carrier dynamics via photoinduced electric fields Yang, Y.; Gu, J.; Young, J. L. Science, Vol. 350, Issue 6264 https://doi.org/10.1126/science.aad3459	journal	November 2015
Semiconductor electrodes. IV. Electrochemical behavior of n- and p-type silicon electrodes in acetonitrile solutions Laser, Daniel; Bard, Allen J. The Journal of Physical Chemistry, Vol. 80, Issue 5 https://doi.org/10.1021/j100546a008	journal	February 1976
Determination of flat-band potentials of silicon electrodes in HF by means of ac resistance measurements Ottow, S.; Popkirov, G. S.; Föll, H. Journal of Electroanalytical Chemistry, Vol. 455, Issue 1-2 https://doi.org/10.1016/S0022-0728(98)00189-2	journal	September 1998
Oxidatively Stable Nanoporous Silicon Photocathodes with Enhanced Onset Voltage for Photoelectrochemical Proton Reduction Zhao, Y.; Anderson, N. C.; Zhu, K. Nano Letters, Vol. 15, Issue 4 https://doi.org/10.1021/acs.nanolett.5b00086	journal	March 2015
Enhanced Photoelectrochemical Water Oxidation on Bismuth Vanadate by Electrodeposition of Amorphous Titanium Dioxide Eisenberg, David; Ahn, Hyun S.; Bard, Allen J. Journal of the American Chemical Society, Vol. 136, Issue 40 https://doi.org/10.1021/ja5082475	journal	August 2014
Role of TiO ₂ Surface Passivation on Improving the Performance of p-InP Photocathodes Lin, Yongjing; Kapadia, Rehan; Yang, Jinhui The Journal of Physical Chemistry C, Vol. 119, Issue 5 https://doi.org/10.1021/jp5107313	journal	February 2015
Charge-Transfer through Ultrathin Film TiO ₂ on n -Si(111) Photoelectrodes: Experimental and Theoretical Investigation of Electric Field-Enhanced Transport with a Nonaqueous Redox Couple Kim, Hark Jin; Kearney, Kara L.; Le, Luc H. The Journal of Physical Chemistry C, Vol. 120, Issue 45 https://doi.org/10.1021/acs.jpcc.6b08096	journal	November 2016

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Title: Silicon Photoelectrode Thermodynamics and Hydrogen Evolution Kinetics Measured by Intensity-Modulated High-Frequency Resistivity Impedance Spectroscopy

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