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Title: Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi2O4 Employing a High-Throughput Methodology

Abstract

Metal oxide semiconductors are promising for solar photochemistry if the issues of excessive charge carrier recombination and material degradation can be resolved, which are both influenced by surface quality and interface chemistry. Coating the semiconductor with an overlayer to passivate surface states is a common remedial strategy but is less desirable than application of a functional coating that can improve carrier extraction and reduce recombination while mitigating corrosion. Here, a data-driven materials science approach utilizing high-throughput methodologies, including inkjet printing and scanning droplet electrochemical cell measurements, is used to create and evaluate multi-element coating libraries to discover new classes of candidate passivation and electron-selective contact materials for p-type CuBi2O4. The optimized overlayer (Cu1.5TiOz) improves the onset potential by 110 mV, the photocurrent by 2.8×, and the absorbed photon-to-current efficiency by 15.5% compared to non-coated photoelectrodes. It is shown that these enhancements are related to reduced surface recombination through passivation of surface defect states as well as improved carrier extraction efficiency through Fermi level engineering. This work presents a generalizable, high-throughput method to design and optimize passivation materials for a variety of semiconductors, providing a powerful platform for development of high-performance photoelectrodes for incorporation into solar-fuel generation systems.

Authors:
 [1];  [2];  [3];  [3];  [3];  [3];  [4];  [4];  [3]; ORCiD logo [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lanzhou Univ. (China)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. California Institute of Technology (CalTech), Pasadena, CA (United States)
  4. Lanzhou Univ. (China)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Chinese Scholarship Council (CSC)
OSTI Identifier:
1642689
Alternate Identifier(s):
OSTI ID: 1617068
Grant/Contract Number:  
AC02-05CH11231; SC0004993; AC02‐05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 24; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; fermi level engineering; high-throughput methodology; passivation layer; p-type semiconductor; solar photochemistry

Citation Formats

Zhang, Zemin, Lindley, Sarah A., Guevarra, Dan, Kan, Kevin, Shinde, Aniketa, Gregoire, John M., Han, Weihua, Xie, Erqing, Haber, Joel A., and Cooper, Jason K. Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi2O4 Employing a High-Throughput Methodology. United States: N. p., 2020. Web. doi:10.1002/adfm.202000948.
Zhang, Zemin, Lindley, Sarah A., Guevarra, Dan, Kan, Kevin, Shinde, Aniketa, Gregoire, John M., Han, Weihua, Xie, Erqing, Haber, Joel A., & Cooper, Jason K. Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi2O4 Employing a High-Throughput Methodology. United States. https://doi.org/10.1002/adfm.202000948
Zhang, Zemin, Lindley, Sarah A., Guevarra, Dan, Kan, Kevin, Shinde, Aniketa, Gregoire, John M., Han, Weihua, Xie, Erqing, Haber, Joel A., and Cooper, Jason K. Mon . "Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi2O4 Employing a High-Throughput Methodology". United States. https://doi.org/10.1002/adfm.202000948. https://www.osti.gov/servlets/purl/1642689.
@article{osti_1642689,
title = {Fermi Level Engineering of Passivation and Electron Transport Materials for p-Type CuBi2O4 Employing a High-Throughput Methodology},
author = {Zhang, Zemin and Lindley, Sarah A. and Guevarra, Dan and Kan, Kevin and Shinde, Aniketa and Gregoire, John M. and Han, Weihua and Xie, Erqing and Haber, Joel A. and Cooper, Jason K.},
abstractNote = {Metal oxide semiconductors are promising for solar photochemistry if the issues of excessive charge carrier recombination and material degradation can be resolved, which are both influenced by surface quality and interface chemistry. Coating the semiconductor with an overlayer to passivate surface states is a common remedial strategy but is less desirable than application of a functional coating that can improve carrier extraction and reduce recombination while mitigating corrosion. Here, a data-driven materials science approach utilizing high-throughput methodologies, including inkjet printing and scanning droplet electrochemical cell measurements, is used to create and evaluate multi-element coating libraries to discover new classes of candidate passivation and electron-selective contact materials for p-type CuBi2O4. The optimized overlayer (Cu1.5TiOz) improves the onset potential by 110 mV, the photocurrent by 2.8×, and the absorbed photon-to-current efficiency by 15.5% compared to non-coated photoelectrodes. It is shown that these enhancements are related to reduced surface recombination through passivation of surface defect states as well as improved carrier extraction efficiency through Fermi level engineering. This work presents a generalizable, high-throughput method to design and optimize passivation materials for a variety of semiconductors, providing a powerful platform for development of high-performance photoelectrodes for incorporation into solar-fuel generation systems.},
doi = {10.1002/adfm.202000948},
journal = {Advanced Functional Materials},
number = 24,
volume = 30,
place = {United States},
year = {Mon May 04 00:00:00 EDT 2020},
month = {Mon May 04 00:00:00 EDT 2020}
}

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