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Title: Scanning Electrochemical Flow Cell with Online Mass Spectroscopy for Accelerated Screening of Carbon Dioxide Reduction Electrocatalysts

Abstract

Electrochemical conversion of carbon dioxide into valuable chemicals or fuels is an increasingly important strategy for achieving carbon neutral technologies. The lack of a sufficiently active and selective electrocatalyst, particularly for synthesizing highly reduced products, motivates accelerated screening to evaluate new catalyst spaces. Traditional techniques, which couple electrocatalyst operation with analytical techniques to measure product distributions, enable screening throughput at 1–10 catalysts per day. In this paper, a combinatorial screening instrument is designed for MS detection of hydrogen, methane, and ethylene in quasi-real-time during catalyst operation experiments in an electrochemical flow cell. Coupled with experiment modeling, product detection during cyclic voltammetry (CV) enables modeling of the voltage-dependent partial current density for each detected product. Here, we demonstrate the technique by using the well-established thin film Cu catalysts and by screening a Pd–Zn composition library in carbonate-buffered aqueous electrolyte. The rapid product distribution characterization over a large range of overpotential makes the instrument uniquely suited for accelerating screening of electrocatalysts for the carbon dioxide reduction reaction.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [2]
  1. California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP)
  2. California Institute of Technology (CalTech), Pasadena, CA (United States). Joint Center for Artificial Photosynthesis (JCAP), and Division of Engineering and Applied Science
Publication Date:
Research Org.:
California Institute of Technology (CalTech), Pasadena, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1606293
Grant/Contract Number:  
SC0004993; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
ACS Combinatorial Science
Additional Journal Information:
Journal Volume: 21; Journal Issue: 10; Journal ID: ISSN 2156-8952
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; carbon dioxide reduction; catalyst discovery; electrocatalysis; high throughput experimentation; product detection

Citation Formats

Lai, Yungchieh, Jones, Ryan J. R., Wang, Yu, Zhou, Lan, and Gregoire, John M. Scanning Electrochemical Flow Cell with Online Mass Spectroscopy for Accelerated Screening of Carbon Dioxide Reduction Electrocatalysts. United States: N. p., 2019. Web. doi:10.1021/acscombsci.9b00130.
Lai, Yungchieh, Jones, Ryan J. R., Wang, Yu, Zhou, Lan, & Gregoire, John M. Scanning Electrochemical Flow Cell with Online Mass Spectroscopy for Accelerated Screening of Carbon Dioxide Reduction Electrocatalysts. United States. https://doi.org/10.1021/acscombsci.9b00130
Lai, Yungchieh, Jones, Ryan J. R., Wang, Yu, Zhou, Lan, and Gregoire, John M. Tue . "Scanning Electrochemical Flow Cell with Online Mass Spectroscopy for Accelerated Screening of Carbon Dioxide Reduction Electrocatalysts". United States. https://doi.org/10.1021/acscombsci.9b00130. https://www.osti.gov/servlets/purl/1606293.
@article{osti_1606293,
title = {Scanning Electrochemical Flow Cell with Online Mass Spectroscopy for Accelerated Screening of Carbon Dioxide Reduction Electrocatalysts},
author = {Lai, Yungchieh and Jones, Ryan J. R. and Wang, Yu and Zhou, Lan and Gregoire, John M.},
abstractNote = {Electrochemical conversion of carbon dioxide into valuable chemicals or fuels is an increasingly important strategy for achieving carbon neutral technologies. The lack of a sufficiently active and selective electrocatalyst, particularly for synthesizing highly reduced products, motivates accelerated screening to evaluate new catalyst spaces. Traditional techniques, which couple electrocatalyst operation with analytical techniques to measure product distributions, enable screening throughput at 1–10 catalysts per day. In this paper, a combinatorial screening instrument is designed for MS detection of hydrogen, methane, and ethylene in quasi-real-time during catalyst operation experiments in an electrochemical flow cell. Coupled with experiment modeling, product detection during cyclic voltammetry (CV) enables modeling of the voltage-dependent partial current density for each detected product. Here, we demonstrate the technique by using the well-established thin film Cu catalysts and by screening a Pd–Zn composition library in carbonate-buffered aqueous electrolyte. The rapid product distribution characterization over a large range of overpotential makes the instrument uniquely suited for accelerating screening of electrocatalysts for the carbon dioxide reduction reaction.},
doi = {10.1021/acscombsci.9b00130},
journal = {ACS Combinatorial Science},
number = 10,
volume = 21,
place = {United States},
year = {2019},
month = {8}
}

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Works referencing / citing this record:

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