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Title: Revealing structural evolution of PbS nanocrystal catalysts in electrochemical CO2 reduction using in situ synchrotron radiation X-ray diffraction

Abstract

We investigated the structural evolution of PbS catalysts under electrochemical CO2 reduction reaction (eCO2RR) conditions using an in situ synchrotron radiation X-ray diffraction (SR-XRD) technique. The PbS catalyst with an initial form of size-tunable nanocrystals (NCs) performed efficiently in the electrochemical conversion of CO2 to formate with a record-high mass activity (MA) of 52.2 ± 5.2 mA mgPb-1 at -1.2 V and 74.9 ± 4.7 mA mgPb-1 at -1.4 V vs. the reversible hydrogen electrode (RHE). In situ SR-XRD analyses revealed that PbS NCs underwent rapid structural transformation to Pb thin films during the eCO2RR, providing the real catalytic surface for the eCO2RR. Such a structural change is complex, with PbS first being converted to PbCO3 and the latter species being further reduced to Pb. This work highlights the importance of understanding environmental impacts on the instability of nanocatalysts under eCO2RR conditions and the need for designing more robust electrocatalysts.

Authors:
ORCiD logo [1];  [1];  [1];  [2];  [2]; ORCiD logo [1]
  1. Univ. of Virginia, Charlottesville, VA (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
4-VA Collaborative Research Grant Program; USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1630295
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 41; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Zhang, Zhiyong, Liu, Chang, Brosnahan, John T., Zhou, Hua, Xu, Wenqian, and Zhang, Sen. Revealing structural evolution of PbS nanocrystal catalysts in electrochemical CO2 reduction using in situ synchrotron radiation X-ray diffraction. United States: N. p., 2019. Web. doi:10.1039/c9ta06750g.
Zhang, Zhiyong, Liu, Chang, Brosnahan, John T., Zhou, Hua, Xu, Wenqian, & Zhang, Sen. Revealing structural evolution of PbS nanocrystal catalysts in electrochemical CO2 reduction using in situ synchrotron radiation X-ray diffraction. United States. https://doi.org/10.1039/c9ta06750g
Zhang, Zhiyong, Liu, Chang, Brosnahan, John T., Zhou, Hua, Xu, Wenqian, and Zhang, Sen. Mon . "Revealing structural evolution of PbS nanocrystal catalysts in electrochemical CO2 reduction using in situ synchrotron radiation X-ray diffraction". United States. https://doi.org/10.1039/c9ta06750g. https://www.osti.gov/servlets/purl/1630295.
@article{osti_1630295,
title = {Revealing structural evolution of PbS nanocrystal catalysts in electrochemical CO2 reduction using in situ synchrotron radiation X-ray diffraction},
author = {Zhang, Zhiyong and Liu, Chang and Brosnahan, John T. and Zhou, Hua and Xu, Wenqian and Zhang, Sen},
abstractNote = {We investigated the structural evolution of PbS catalysts under electrochemical CO2 reduction reaction (eCO2RR) conditions using an in situ synchrotron radiation X-ray diffraction (SR-XRD) technique. The PbS catalyst with an initial form of size-tunable nanocrystals (NCs) performed efficiently in the electrochemical conversion of CO2 to formate with a record-high mass activity (MA) of 52.2 ± 5.2 mA mgPb-1 at -1.2 V and 74.9 ± 4.7 mA mgPb-1 at -1.4 V vs. the reversible hydrogen electrode (RHE). In situ SR-XRD analyses revealed that PbS NCs underwent rapid structural transformation to Pb thin films during the eCO2RR, providing the real catalytic surface for the eCO2RR. Such a structural change is complex, with PbS first being converted to PbCO3 and the latter species being further reduced to Pb. This work highlights the importance of understanding environmental impacts on the instability of nanocatalysts under eCO2RR conditions and the need for designing more robust electrocatalysts.},
doi = {10.1039/c9ta06750g},
journal = {Journal of Materials Chemistry. A},
number = 41,
volume = 7,
place = {United States},
year = {Mon Sep 16 00:00:00 EDT 2019},
month = {Mon Sep 16 00:00:00 EDT 2019}
}

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Cited by: 15 works
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