A graded catalytic–protective layer for an efficient and stable water-splitting photocathode
Abstract
Achieving solar-to-hydrogen efficiencies above 15% is key for the commercial success of photoelectrochemical water splitting devices. While tandem cells can reach those efficiencies, increasing the catalytic activity and long-term stability remains a significant challenge. We show that annealing a bilayer of amorphous titanium dioxide (TiOx) and molybdenum sulfide (MoSx) deposited onto GaInP2 results in a photocathode with high catalytic activity (current density of 11 mA/cm-2 at 0 V vs. the reversible hydrogen electrode under 1 sun illumination) and stability (retention of 80% of initial photocurrent density over a 20 h durability test) for the hydrogen evolution reaction. Microscopy and spectroscopy reveal that annealing results in a graded MoSx/MoOx/TiO2 layer that retains much of the high catalytic activity of amorphous MoSx but with stability similar to crystalline MoS2. These findings demonstrate the potential of utilizing a hybridized, heterogeneous surface layer as a cost-effective catalytic and protective interface for solar hydrogen production.
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1339236
- Report Number(s):
- NREL/JA-5900-67483
Journal ID: ISSN 2058-7546
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Energy
- Additional Journal Information:
- Journal Volume: 2; Journal ID: ISSN 2058-7546
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 14 SOLAR ENERGY; 36 MATERIALS SCIENCE; water-splitting; photocathodes; protective interface; graded MoSx/MoOx/TiO2 layer; catalytic activity
Citation Formats
Gu, Jing, Aguiar, Jeffery A., Ferrere, Suzanne, Steirer, K. Xerxes, Yan, Yong, Xiao, Chuanxiao, Young, James L., Al-Jassim, Mowafak, Neale, Nathan R., and Turner, John A. A graded catalytic–protective layer for an efficient and stable water-splitting photocathode. United States: N. p., 2017.
Web. doi:10.1038/nenergy.2016.192.
Gu, Jing, Aguiar, Jeffery A., Ferrere, Suzanne, Steirer, K. Xerxes, Yan, Yong, Xiao, Chuanxiao, Young, James L., Al-Jassim, Mowafak, Neale, Nathan R., & Turner, John A. A graded catalytic–protective layer for an efficient and stable water-splitting photocathode. United States. https://doi.org/10.1038/nenergy.2016.192
Gu, Jing, Aguiar, Jeffery A., Ferrere, Suzanne, Steirer, K. Xerxes, Yan, Yong, Xiao, Chuanxiao, Young, James L., Al-Jassim, Mowafak, Neale, Nathan R., and Turner, John A. Mon .
"A graded catalytic–protective layer for an efficient and stable water-splitting photocathode". United States. https://doi.org/10.1038/nenergy.2016.192. https://www.osti.gov/servlets/purl/1339236.
@article{osti_1339236,
title = {A graded catalytic–protective layer for an efficient and stable water-splitting photocathode},
author = {Gu, Jing and Aguiar, Jeffery A. and Ferrere, Suzanne and Steirer, K. Xerxes and Yan, Yong and Xiao, Chuanxiao and Young, James L. and Al-Jassim, Mowafak and Neale, Nathan R. and Turner, John A.},
abstractNote = {Achieving solar-to-hydrogen efficiencies above 15% is key for the commercial success of photoelectrochemical water splitting devices. While tandem cells can reach those efficiencies, increasing the catalytic activity and long-term stability remains a significant challenge. We show that annealing a bilayer of amorphous titanium dioxide (TiOx) and molybdenum sulfide (MoSx) deposited onto GaInP2 results in a photocathode with high catalytic activity (current density of 11 mA/cm-2 at 0 V vs. the reversible hydrogen electrode under 1 sun illumination) and stability (retention of 80% of initial photocurrent density over a 20 h durability test) for the hydrogen evolution reaction. Microscopy and spectroscopy reveal that annealing results in a graded MoSx/MoOx/TiO2 layer that retains much of the high catalytic activity of amorphous MoSx but with stability similar to crystalline MoS2. These findings demonstrate the potential of utilizing a hybridized, heterogeneous surface layer as a cost-effective catalytic and protective interface for solar hydrogen production.},
doi = {10.1038/nenergy.2016.192},
journal = {Nature Energy},
number = ,
volume = 2,
place = {United States},
year = {Mon Jan 09 00:00:00 EST 2017},
month = {Mon Jan 09 00:00:00 EST 2017}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 110 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Nonstoichiometric rutile TiO2 photoelectrodes for improved photoelectrochemical water splitting
journal, January 2013
- Zhen, Chao; Wang, Lianzhou; Liu, Li
- Chemical Communications, Vol. 49, Issue 55
Photoelectrochemical decomposition of water utilizing monolithic tandem cells
journal, April 1998
- Kocha, S.
- Solar Energy Materials and Solar Cells, Vol. 52, Issue 3-4
Novel Assembly of an MoS 2 Electrocatalyst onto a Silicon Nanowire Array Electrode to Construct a Photocathode Composed of Elements Abundant on the Earth for Hydrogen Generation
journal, September 2012
- Tran, Phong D.; Pramana, Stevin S.; Kale, Vinayak S.
- Chemistry - A European Journal, Vol. 18, Issue 44
Electrochemical Stability of p-GaInP[sub 2] in Aqueous Electrolytes Toward Photoelectrochemical Water Splitting
journal, January 1998
- Khaselev, Oscar
- Journal of The Electrochemical Society, Vol. 145, Issue 10
X-ray photoelectron spectroscopy characterization of amorphous molybdenum oxysulfide thin films
journal, March 1995
- Benoist, L.; Gonbeau, D.; Pfister-Guillouzo, G.
- Thin Solid Films, Vol. 258, Issue 1-2
MoS2-wrapped silicon nanowires for photoelectrochemical water reduction
journal, December 2014
- Zhang, Liming; Liu, Chong; Wong, Andrew Barnabas
- Nano Research, Vol. 8, Issue 1
Displacement of the Bandedges of GaInP[sub 2] in Aqueous Electrolytes Induced by Surface Modification
journal, January 1995
- Kocha, Shyam S.
- Journal of The Electrochemical Society, Vol. 142, Issue 8
Hydrogen production through sorption-enhanced steam methane reforming and membrane technology: A review
journal, April 2008
- Barelli, L.; Bidini, G.; Gallorini, F.
- Energy, Vol. 33, Issue 4
Pt–Ru Alloyed Fuel Cell Catalysts Sputtered from a Single Alloyed Target
journal, August 2011
- Dameron, Arrelaine A.; Olson, Tim S.; Christensen, Steven T.
- ACS Catalysis, Vol. 1, Issue 10
Growth and Activation of an Amorphous Molybdenum Sulfide Hydrogen Evolving Catalyst
journal, August 2013
- Vrubel, Heron; Hu, Xile
- ACS Catalysis, Vol. 3, Issue 9
Hydrogen Evolution from Pt/Ru-Coated p-Type WSe 2 Photocathodes
journal, December 2012
- McKone, James R.; Pieterick, Adam P.; Gray, Harry B.
- Journal of the American Chemical Society, Vol. 135, Issue 1
Electrochemistry and photochemistry of MoS2 layer crystals. I
journal, August 1977
- Tributsch, H.; Bennett, J. C.
- Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 81, Issue 1
Core–shell MoO3–MoS2 Nanowires for Hydrogen Evolution A Functional Design for Electrocatalytic Materials
journal, October 2011
- Chen, Zhebo; Cummins, Dustin; Reinecke, Benjamin N.
- Nano Letters, Vol. 11, Issue 10, p. 4168-4175
Universal and Versatile MoO 3 -Based Hole Transport Layers for Efficient and Stable Polymer Solar Cells
journal, May 2014
- Hu, Xiaotian; Chen, Lie; Chen, Yiwang
- The Journal of Physical Chemistry C, Vol. 118, Issue 19
The stability of illuminated p-GaInP2 semiconductor photoelectrode
journal, October 2012
- Wang, Heli; Deutsch, Todd; Welch, Adam
- International Journal of Hydrogen Energy, Vol. 37, Issue 19
Enhancing Water Splitting Activity and Chemical Stability of Zinc Oxide Nanowire Photoanodes with Ultrathin Titania Shells
journal, June 2013
- Liu, Mingzhao; Nam, Chang-Yong; Black, Charles T.
- The Journal of Physical Chemistry C, Vol. 117, Issue 26
Electrochemical deposition of MoS2 thin films by reduction of tetrathiomolybdate
journal, July 1996
- Ponomarev, E. A.; Neumann-Spallart, M.; Hodes, G.
- Thin Solid Films, Vol. 280, Issue 1-2
Water reduction by a p-GaInP2 photoelectrode stabilized by an amorphous TiO2 coating and a molecular cobalt catalyst
journal, December 2015
- Gu, Jing; Yan, Yong; Young, James L.
- Nature Materials, Vol. 15, Issue 4
Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation
journal, May 2014
- Hu, S.; Shaner, M. R.; Beardslee, J. A.
- Science, Vol. 344, Issue 6187
Recent Development of Molybdenum Sulfides as Advanced Electrocatalysts for Hydrogen Evolution Reaction
journal, April 2014
- Yan, Ya; Xia, BaoYu; Xu, Zhichuan
- ACS Catalysis, Vol. 4, Issue 6
Current Status of Hydrogen Production Techniques by Steam Reforming of Ethanol: A Review
journal, September 2005
- Haryanto, Agus; Fernando, Sandun; Murali, Naveen
- Energy & Fuels, Vol. 19, Issue 5
Solar Water Splitting Cells
journal, November 2010
- Walter, Michael G.; Warren, Emily L.; McKone, James R.
- Chemical Reviews, Vol. 110, Issue 11, p. 6446-6473
A Monolithic Photovoltaic-Photoelectrochemical Device for Hydrogen Production via Water Splitting
journal, April 1998
- Khaselev, O.
- Science, Vol. 280, Issue 5362
Catalyzing the Hydrogen Evolution Reaction (HER) with Molybdenum Sulfide Nanomaterials
journal, October 2014
- Benck, Jesse D.; Hellstern, Thomas R.; Kibsgaard, Jakob
- ACS Catalysis, Vol. 4, Issue 11
Electrodeposition of Ni–Mo alloy coatings and their characterization as cathodes for hydrogen evolution in sodium hydroxide solution
journal, July 2008
- Krstajic, N.; Jovic, V.; Gajickrstajic, L.
- International Journal of Hydrogen Energy, Vol. 33, Issue 14
Rh-Doped SrTiO 3 Photocatalyst Electrode Showing Cathodic Photocurrent for Water Splitting under Visible-Light Irradiation
journal, August 2011
- Iwashina, Katsuya; Kudo, Akihiko
- Journal of the American Chemical Society, Vol. 133, Issue 34
Hydrogen evolution from a copper(I) oxide photocathode coated with an amorphous molybdenum sulphide catalyst
journal, January 2014
- Morales-Guio, Carlos G.; Tilley, S. David; Vrubel, Heron
- Nature Communications, Vol. 5, Issue 1
Effect of ceria-doped titania on the structure and acidic properties of MoO3/TiO2 catalysts
journal, July 2004
- Mohamed, Mohamed Mokhtar
- Applied Catalysis A: General, Vol. 267, Issue 1-2
Amorphous Molybdenum Sulfide Catalysts for Electrochemical Hydrogen Production: Insights into the Origin of their Catalytic Activity
journal, August 2012
- Benck, Jesse D.; Chen, Zhebo; Kuritzky, Leah Y.
- ACS Catalysis, Vol. 2, Issue 9, p. 1916-1923
p-Type InP Nanopillar Photocathodes for Efficient Solar-Driven Hydrogen Production
journal, September 2012
- Lee, Min Hyung; Takei, Kuniharu; Zhang, Junjun
- Angewandte Chemie, Vol. 124, Issue 43
Single-Crystal Semiconductors with Narrow Band Gaps for Solar Water Splitting
journal, July 2015
- Wang, Tuo; Gong, Jinlong
- Angewandte Chemie International Edition, Vol. 54, Issue 37
Post-1989 calibration energies for X-ray photoelectron spectrometers and the 1990 Josephson constant
journal, August 1989
- Seah, M. P.
- Surface and Interface Analysis, Vol. 14, Issue 8
Magnetically Separable, Carbon-Supported Nanocatalysts for the Manufacture of Fine Chemicals
journal, October 2004
- Tsang, Shik Chi; Caps, Val�rie; Paraskevas, Ioannis
- Angewandte Chemie, Vol. 116, Issue 42
Using TiO 2 as a Conductive Protective Layer for Photocathodic H 2 Evolution
journal, January 2013
- Seger, Brian; Pedersen, Thomas; Laursen, Anders B.
- Journal of the American Chemical Society, Vol. 135, Issue 3
Amorphous molybdenum sulfide films as catalysts for electrochemical hydrogen production in water
journal, January 2011
- Merki, Daniel; Fierro, Stéphane; Vrubel, Heron
- Chem. Sci., Vol. 2, Issue 7, p. 1262-1267
Works referencing / citing this record:
Three Birds, One-Stone Strategy for Hybrid Microwave Synthesis of Ta and Sn Codoped Fe 2 O 3 @FeTaO 4 Nanorods for Photo-Electrochemical Water Oxidation
journal, January 2019
- Zhang, Hemin; Noh, Woo Yeong; Li, Feng
- Advanced Functional Materials, Vol. 29, Issue 11
Fine Tuning Electronic Structure of Catalysts through Atomic Engineering for Enhanced Hydrogen Evolution
journal, June 2018
- Huang, Yichao; Hu, Jun; Xu, Haoxiang
- Advanced Energy Materials, Vol. 8, Issue 24
Tuning Internal Strain in Metal–Organic Frameworks via Vapor Phase Infiltration for CO 2 Reduction
journal, January 2020
- Yang, Fan; Hu, Wenhui; Yang, Chongqing
- Angewandte Chemie International Edition, Vol. 59, Issue 11
Building a Thermostable Metabolon for Facilitating Coenzyme Transport and In Vitro Hydrogen Production at Elevated Temperature
journal, August 2018
- Chen, Hui; Huang, Rui; Kim, Eui-Jin
- ChemSusChem, Vol. 11, Issue 18
Stable p‐type Cu:CdS 1− x Se x /Pt Thin‐Film Photocathodes with Fully Tunable Bandgap for Scavenger‐Free Photoelectrochemical Water Splitting
journal, January 2020
- Ye, Zi; Hu, Zhuofeng; Yang, Lixia
- Solar RRL, Vol. 4, Issue 3
Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%
journal, April 2017
- Yan, Yong; Crisp, Ryan W.; Gu, Jing
- Nature Energy, Vol. 2, Issue 5
Crystalline TiO2 protective layer with graded oxygen defects for efficient and stable silicon-based photocathode
journal, September 2018
- Zheng, Jianyun; Lyu, Yanhong; Wang, Ruilun
- Nature Communications, Vol. 9, Issue 1
Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution
journal, February 2019
- Huang, Yichao; Sun, Yuanhui; Zheng, Xueli
- Nature Communications, Vol. 10, Issue 1
High performance III-V photoelectrodes for solar water splitting via synergistically tailored structure and stoichiometry
journal, July 2019
- Lim, Haneol; Young, James L.; Geisz, John F.
- Nature Communications, Vol. 10, Issue 1
An efficient and stable photoelectrochemical system with 9% solar-to-hydrogen conversion efficiency via InGaP/GaAs double junction
journal, November 2019
- Varadhan, Purushothaman; Fu, Hui-Chun; Kao, Yu-Cheng
- Nature Communications, Vol. 10, Issue 1
Spatial control of cocatalysts and elimination of interfacial defects towards efficient and robust CIGS photocathodes for solar water splitting
journal, January 2018
- Chen, Mengxin; Liu, Yang; Li, Chengcheng
- Energy & Environmental Science, Vol. 11, Issue 8
Photocorrosion-resistant Sb 2 Se 3 photocathodes with earth abundant MoS x hydrogen evolution catalyst
journal, January 2017
- Prabhakar, Rajiv Ramanujam; Septina, Wilman; Siol, Sebastian
- Journal of Materials Chemistry A, Vol. 5, Issue 44
Strategies for enhancing the photocurrent, photovoltage, and stability of photoelectrodes for photoelectrochemical water splitting
journal, January 2019
- Yang, Wooseok; Prabhakar, Rajiv Ramanujam; Tan, Jeiwan
- Chemical Society Reviews, Vol. 48, Issue 19
Ultra-rapid rates of water splitting for biohydrogen gas production through in vitro artificial enzymatic pathways
journal, January 2018
- Kim, Eui-Jin; Kim, Jae-Eung; Zhang, Yi-Heng P. Job
- Energy & Environmental Science, Vol. 11, Issue 8
Two-dimensional materials in semiconductor photoelectrocatalytic systems for water splitting
journal, January 2019
- Faraji, Monireh; Yousefi, Mahdieh; Yousefzadeh, Samira
- Energy & Environmental Science, Vol. 12, Issue 1
Unbiased solar H 2 production with current density up to 23 mA cm −2 by Swiss-cheese black Si coupled with wastewater bioanode
journal, January 2019
- Lu, Lu; Vakki, Waltteri; Aguiar, Jeffery A.
- Energy & Environmental Science, Vol. 12, Issue 3
Aluminum-incorporated p-CuO/n-ZnO photocathode coated with nanocrystal-engineered TiO 2 protective layer for photoelectrochemical water splitting and hydrogen generation
journal, January 2018
- Masudy-Panah, Saeid; Eugene, Y. -J. Kong; Khiavi, Negar Dasineh
- Journal of Materials Chemistry A, Vol. 6, Issue 25
A heterojunction strategy to improve the visible light sensitive water splitting performance of photocatalytic materials
journal, January 2018
- Afroz, Khurshida; Moniruddin, Md; Bakranov, Nurlan
- Journal of Materials Chemistry A, Vol. 6, Issue 44
Efficiency and stability of narrow-gap semiconductor-based photoelectrodes
journal, January 2019
- Zheng, Jianyun; Zhou, Huaijuan; Zou, Yuqin
- Energy & Environmental Science, Vol. 12, Issue 8
Spontaneous full photocatalytic water splitting on 2D MoSe 2 /SnSe 2 and WSe 2 /SnSe 2 vdW heterostructures
journal, January 2019
- Fan, Yingcai; Wang, Junru; Zhao, Mingwen
- Nanoscale, Vol. 11, Issue 31
Two-dimensional FeS 2 -encapsulated Au: a quasi-epitaxial heterojunction for synergistic catalytic activity under photoelectrocatalytic water reduction
journal, January 2019
- Mondal, Indranil; Moon, Song Yi; Lee, Hyunhwa
- Journal of Materials Chemistry A, Vol. 7, Issue 33
Surface chemistry and photoelectrochemistry—Case study on tantalum nitride
journal, October 2019
- He, Yumin; Chen, Rong; Fa, Wenjun
- The Journal of Chemical Physics, Vol. 151, Issue 13
NiFeP nanoflakes composite with CoP on carbon cloth as flexible and durable electrocatalyst for efficient overall water splitting
journal, September 2019
- Li, Mai; Li, Sa; Wang, Jiale
- Nanotechnology, Vol. 30, Issue 48
Strategies for enhancing the photocurrent, photovoltage, and stability of photoelectrodes for photoelectrochemical water splitting
text, January 2019
- Wooseok, Yang,; Ramanujam, Prabhakar, Rajiv; Jeiwan, Tan,
- Royal Society of Chemistry
Crystalline TiO2 protective layer with graded oxygen defects for efficient and stable silicon-based photocathode
journal, September 2018
- Zheng, Jianyun; Lyu, Yanhong; Wang, Ruilun
- Nature Communications, Vol. 9, Issue 1
Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution
journal, February 2019
- Huang, Yichao; Sun, Yuanhui; Zheng, Xueli
- Nature Communications, Vol. 10, Issue 1
High performance III-V photoelectrodes for solar water splitting via synergistically tailored structure and stoichiometry
journal, July 2019
- Lim, Haneol; Young, James L.; Geisz, John F.
- Nature Communications, Vol. 10, Issue 1
An efficient and stable photoelectrochemical system with 9% solar-to-hydrogen conversion efficiency via InGaP/GaAs double junction
journal, November 2019
- Varadhan, Purushothaman; Fu, Hui-Chun; Kao, Yu-Cheng
- Nature Communications, Vol. 10, Issue 1