skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Employing overlayers to improve the performance of Cu2BaSnS4 thin film based photoelectrochemical water reduction devices

Abstract

Earth-abundant copper-barium-thiostannate Cu2BaSnS4 (CBTS)-based thin films have recently been reported to exhibit the optoelectronic and defect properties suitable as absorbers for photoelectrochemical (PEC) water splitting and the top cell of tandem photovoltaic solar cells. However, the photocurrents of CBTS-based PEC devices are still much lower than the theoretical value, partially due to ineffective charge collection at CBTS/water interface and instability of CBTS in electrolytes. Here, we report on overcoming these issues by employing overlayer engineering. We find that CdS/ZnO/TiO2 overlayers can significant-ly improve the PEC performance, achieving saturated cathodic photocurrents up to 7.8 mA cm-2 at the potential of -0.10 V versus reversible hydrogen electrode (RHE) in a neutral electrolyte solution, which is much higher than the best bare CBTS film attaining a photocurrent of 4.8 mA cm-2 at the potential of -0.2 V versus RHE. Finally, our results suggest a viable approach for improving the performance of CBTS-based PEC cells.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [2];  [2];  [2];  [1];  [1]; ORCiD logo [1]
  1. The Univ. of Toledo, Toledo, OH (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); National Science Foundation (NSF)
OSTI Identifier:
1346536
Report Number(s):
NREL/JA-5900-67785
Journal ID: ISSN 0897-4756
Grant/Contract Number:  
AC36-08GO28308; AC02-05CH11231; CHE-1230246; DMR-1534686
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 3; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; optoelectronics; absorbers; photoelectrochemical water splitting; overlayer engineering

Citation Formats

Ge, Jie, Roland, Paul J., Koirala, Prakash, Meng, Weiwei, Young, James L., Petersen, Reese, Deutsch, Todd G., Teeter, Glenn, Ellingson, Randy J., Collins, Robert W., and Yan, Yanfa. Employing overlayers to improve the performance of Cu2BaSnS4 thin film based photoelectrochemical water reduction devices. United States: N. p., 2017. Web. https://doi.org/10.1021/acs.chemmater.6b03347.
Ge, Jie, Roland, Paul J., Koirala, Prakash, Meng, Weiwei, Young, James L., Petersen, Reese, Deutsch, Todd G., Teeter, Glenn, Ellingson, Randy J., Collins, Robert W., & Yan, Yanfa. Employing overlayers to improve the performance of Cu2BaSnS4 thin film based photoelectrochemical water reduction devices. United States. https://doi.org/10.1021/acs.chemmater.6b03347
Ge, Jie, Roland, Paul J., Koirala, Prakash, Meng, Weiwei, Young, James L., Petersen, Reese, Deutsch, Todd G., Teeter, Glenn, Ellingson, Randy J., Collins, Robert W., and Yan, Yanfa. Thu . "Employing overlayers to improve the performance of Cu2BaSnS4 thin film based photoelectrochemical water reduction devices". United States. https://doi.org/10.1021/acs.chemmater.6b03347. https://www.osti.gov/servlets/purl/1346536.
@article{osti_1346536,
title = {Employing overlayers to improve the performance of Cu2BaSnS4 thin film based photoelectrochemical water reduction devices},
author = {Ge, Jie and Roland, Paul J. and Koirala, Prakash and Meng, Weiwei and Young, James L. and Petersen, Reese and Deutsch, Todd G. and Teeter, Glenn and Ellingson, Randy J. and Collins, Robert W. and Yan, Yanfa},
abstractNote = {Earth-abundant copper-barium-thiostannate Cu2BaSnS4 (CBTS)-based thin films have recently been reported to exhibit the optoelectronic and defect properties suitable as absorbers for photoelectrochemical (PEC) water splitting and the top cell of tandem photovoltaic solar cells. However, the photocurrents of CBTS-based PEC devices are still much lower than the theoretical value, partially due to ineffective charge collection at CBTS/water interface and instability of CBTS in electrolytes. Here, we report on overcoming these issues by employing overlayer engineering. We find that CdS/ZnO/TiO2 overlayers can significant-ly improve the PEC performance, achieving saturated cathodic photocurrents up to 7.8 mA cm-2 at the potential of -0.10 V versus reversible hydrogen electrode (RHE) in a neutral electrolyte solution, which is much higher than the best bare CBTS film attaining a photocurrent of 4.8 mA cm-2 at the potential of -0.2 V versus RHE. Finally, our results suggest a viable approach for improving the performance of CBTS-based PEC cells.},
doi = {10.1021/acs.chemmater.6b03347},
journal = {Chemistry of Materials},
number = 3,
volume = 29,
place = {United States},
year = {2017},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Efficient direct solar-to-hydrogen conversion by in situ interface transformation of a tandem structure
journal, September 2015

  • May, Matthias M.; Lewerenz, Hans-Joachim; Lackner, David
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9286

Highly efficient water splitting by a dual-absorber tandem cell
journal, November 2012


Efficient solar water splitting by enhanced charge separation in a bismuth vanadate-silicon tandem photoelectrode
journal, July 2013

  • Abdi, Fatwa F.; Han, Lihao; Smets, Arno H. M.
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3195

Visible-light driven heterojunction photocatalysts for water splitting – a critical review
journal, January 2015

  • Moniz, Savio J. A.; Shevlin, Stephen A.; Martin, David James
  • Energy & Environmental Science, Vol. 8, Issue 3
  • DOI: 10.1039/C4EE03271C

Highly active oxide photocathode for photoelectrochemical water reduction
journal, May 2011

  • Paracchino, Adriana; Laporte, Vincent; Sivula, Kevin
  • Nature Materials, Vol. 10, Issue 6
  • DOI: 10.1038/nmat3017

Positive onset potential and stability of Cu 2 O-based photocathodes in water splitting by atomic layer deposition of a Ga 2 O 3 buffer layer
journal, January 2015

  • Li, Changli; Hisatomi, Takashi; Watanabe, Osamu
  • Energy & Environmental Science, Vol. 8, Issue 5
  • DOI: 10.1039/C5EE00250H

Atomic Layer Deposited Gallium Oxide Buffer Layer Enables 1.2 V Open-Circuit Voltage in Cuprous Oxide Solar Cells
journal, May 2014

  • Lee, Yun Seog; Chua, Danny; Brandt, Riley E.
  • Advanced Materials, Vol. 26, Issue 27
  • DOI: 10.1002/adma.201401054

A Bismuth Vanadate–Cuprous Oxide Tandem Cell for Overall Solar Water Splitting
journal, April 2014

  • Bornoz, Pauline; Abdi, Fatwa F.; Tilley, S. David
  • The Journal of Physical Chemistry C, Vol. 118, Issue 30
  • DOI: 10.1021/jp500441h

Transparent Cuprous Oxide Photocathode Enabling a Stacked Tandem Cell for Unbiased Water Splitting
journal, October 2015

  • Dias, Paula; Schreier, Marcel; Tilley, S. David
  • Advanced Energy Materials, Vol. 5, Issue 24
  • DOI: 10.1002/aenm.201501537

Trigonal Cu 2 -II-Sn-VI 4 (II = Ba, Sr and VI = S, Se) quaternary compounds for earth-abundant photovoltaics
journal, January 2016

  • Hong, Feng; Lin, Wenjun; Meng, Weiwei
  • Physical Chemistry Chemical Physics, Vol. 18, Issue 6
  • DOI: 10.1039/C5CP06977G

Distant-Atom Mutation for Better Earth-Abundant Light Absorbers: A Case Study of Cu 2 BaSnSe 4
journal, December 2016


Is the Cu/Zn Disorder the Main Culprit for the Voltage Deficit in Kesterite Solar Cells?
journal, March 2016

  • Bourdais, Stéphane; Choné, Christophe; Delatouche, Bruno
  • Advanced Energy Materials, Vol. 6, Issue 12
  • DOI: 10.1002/aenm.201502276

Pr�parative und r�ntgenographische Untersuchung am System Cu2?xAgxBaSnS4
journal, October 1976

  • Teske, Chr. L.; Vetter, O.
  • Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 426, Issue 3
  • DOI: 10.1002/zaac.19764260308

2-Photon tandem device for water splitting: comparing photocathode first versus photoanode first designs
journal, January 2014

  • Seger, Brian; Castelli, Ivano E.; Vesborg, Peter C. K.
  • Energy Environ. Sci., Vol. 7, Issue 8
  • DOI: 10.1039/C4EE01335B

BaCu 2 Sn(S,Se) 4 : Earth-Abundant Chalcogenides for Thin-Film Photovoltaics
journal, June 2016


Cu-based quaternary chalcogenide Cu 2 BaSnS 4 thin films acting as hole transport layers in inverted perovskite CH 3 NH 3 PbI 3 solar cells
journal, January 2017

  • Ge, Jie; Grice, Corey R.; Yan, Yanfa
  • Journal of Materials Chemistry A, Vol. 5, Issue 6
  • DOI: 10.1039/C6TA08426E

Earth-abundant trigonal BaCu 2 Sn(Se x S 1−x ) 4 (x = 0–0.55) thin films with tunable band gaps for solar water splitting
journal, January 2016

  • Ge, Jie; Yu, Yue; Yan, Yanfa
  • J. Mater. Chem. A, Vol. 4, Issue 48
  • DOI: 10.1039/C6TA06702F

Oxygenated CdS Buffer Layers Enabling High Open‐Circuit Voltages in Earth‐Abundant Cu 2 BaSnS 4 Thin‐Film Solar Cells
journal, December 2016

  • Ge, Jie; Koirala, Prakash; Grice, Corey R.
  • Advanced Energy Materials, Vol. 7, Issue 6
  • DOI: 10.1002/aenm.201601803

Earth-Abundant Orthorhombic BaCu 2 Sn(Se x S 1– x ) 4 ( x ≈ 0.83) Thin Film for Solar Energy Conversion
journal, August 2016


Addressing the terawatt challenge: scalability in the supply of chemical elements for renewable energy
journal, January 2012

  • Vesborg, Peter C. K.; Jaramillo, Thomas F.
  • RSC Advances, Vol. 2, Issue 21
  • DOI: 10.1039/c2ra20839c

A road towards 25% efficiency and beyond: perovskite tandem solar cells
journal, January 2016

  • Todorov, T.; Gunawan, O.; Guha, S.
  • Molecular Systems Design & Engineering, Vol. 1, Issue 4
  • DOI: 10.1039/C6ME00041J

A Bottom-Up Approach toward All-Solution-Processed High-Efficiency Cu(In,Ga)S 2 Photocathodes for Solar Water Splitting
journal, January 2016

  • Guijarro, Néstor; Prévot, Mathieu S.; Yu, Xiaoyun
  • Advanced Energy Materials, Vol. 6, Issue 7
  • DOI: 10.1002/aenm.201501949

Molecular Chemistry-Controlled Hybrid Ink-Derived Efficient Cu 2 ZnSnS 4 Photocathodes for Photoelectrochemical Water Splitting
journal, November 2016


Targeting Ideal Dual-Absorber Tandem Water Splitting Using Perovskite Photovoltaics and CuIn x Ga 1- x Se 2 Photocathodes
journal, October 2015

  • Luo, Jingshan; Li, Zhen; Nishiwaki, Shiro
  • Advanced Energy Materials, Vol. 5, Issue 24
  • DOI: 10.1002/aenm.201501520

Buffer layers and transparent conducting oxides for chalcopyrite Cu(In,Ga)(S,Se)2 based thin film photovoltaics: present status and current developments
journal, August 2010

  • Naghavi, N.; Abou-Ras, D.; Allsop, N.
  • Progress in Photovoltaics: Research and Applications, Vol. 18, Issue 6, p. 411-433
  • DOI: 10.1002/pip.955

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
  • DOI: 10.1038/nmat4511

A thin-film silicon based photocathode with a hydrogen doped TiO 2 protection layer for solar hydrogen evolution
journal, January 2016

  • Liang, Junhui; Tan, Hairen; Liu, Min
  • Journal of Materials Chemistry A, Vol. 4, Issue 43
  • DOI: 10.1039/C6TA07701C

Excitation-power dependence of the near-band-edge photoluminescence of semiconductors
journal, April 1992


Luminescence of CuInS2
journal, June 1982


Luminescence of CuInS2
journal, June 1982


Free-to-bound recombination in near stoichiometric Cu 2 ZnSnS 4 single crystals
journal, July 2012


Radiative transitions in highly doped and compensated chalcopyrites and kesterites: The case of Cu 2 ZnSnS 4
journal, December 2014


Characteristics of In-Substituted CZTS Thin Film and Bifacial Solar Cell
journal, November 2014

  • Ge, Jie; Chu, Junhao; Jiang, Jinchun
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 23
  • DOI: 10.1021/am505980n

Preparation, transport properties, and electronic structure of quaternary sulfides based on tetrahedral [MS4]4− units: SrCu2MS4 (M=Ge, Sn)
journal, March 2001


    Works referencing / citing this record:

    Modelling of novel-structured copper barium tin sulphide thin film solar cells
    journal, July 2019


    Three‐Dimensional GeSe Microstructured Air Brick Photocathode for Advanced Solar Water Splitting
    journal, February 2020


    Solar light harvesting with multinary metal chalcogenide nanocrystals
    journal, January 2018

    • Stroyuk, Oleksandr; Raevskaya, Alexandra; Gaponik, Nikolai
    • Chemical Society Reviews, Vol. 47, Issue 14
    • DOI: 10.1039/c8cs00029h

    Efficiency enhancement of Cu2BaSnS4 experimental thin-film solar cell by device modeling
    journal, August 2019

    • Khattak, Yousaf Hameed; Baig, Faisal; Toura, Hanae
    • Journal of Materials Science, Vol. 54, Issue 24
    • DOI: 10.1007/s10853-019-03942-6

    Cation Substitution in Earth-Abundant Kesterite Photovoltaic Materials
    journal, January 2018


    Recent Advances in Earth‐Abundant Photocathodes for Photoelectrochemical Water Splitting
    journal, August 2018


    Resistance-based analysis of limiting interfaces in multilayer water splitting photocathodes by impedance spectroscopy
    journal, January 2019

    • Moehl, Thomas; Cui, Wei; Wick-Joliat, René
    • Sustainable Energy & Fuels, Vol. 3, Issue 8
    • DOI: 10.1039/c9se00248k

    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
    • DOI: 10.1039/c8cs00997j