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Title: Facet-Selective Deposition of Ultrathin Al2 O3 on Copper Nanocrystals for Highly Stable CO2 Electroreduction to Ethylene.

Abstract

Abstract Catalysts based on Cu nanocrystals (NCs) for electrochemical CO 2 ‐to‐C 2+ conversion with high activity have been a subject of considerable interest, but poor stability and low selectivity for a single C 2+ product remain obstacles for realizing sustainable carbon‐neutral cycles. Here, we used the facet‐selective atomic layer deposition (FS‐ALD) technique to selectively cover the (111) surface of Cu NCs with ultrathin Al 2 O 3 to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C 2 H 4 /CH 4 for overcoated Cu NCs 22 times higher than that for pure Cu NCs. Peak performance of the overcoated catalyst (Cu NCs/Al 2 O 3 ‐10C) reaches a C 2 H 4 faradaic efficiency of 60.4 % at a current density of 300 mA cm −2 in 5 M KOH electrolyte, when using a gas diffusion electrode flow cell. Moreover, the Al 2 O 3 overcoating effectively suppresses the dynamic mobility and the aggregation of Cu NCs, which explains the negligible activity loss and selectivity degradations of Cu NCs/Al 2 O 3 ‐10C shown in stability tests.

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [4];  [5];  [1];  [1];  [1];  [4];  [5];  [3]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Soochow University, Suzhou (China)
  3. Peking Univ., Beijing (China)
  4. Harbin Institute of Technology (China)
  5. Wake Forest Univ., Winston-Salem, NC (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); Natural Science Foundation of Jiangsu Higher Education Institutions; Guangdong Basic and Applied Basic Research Foundation
OSTI Identifier:
1834366
Alternate Identifier(s):
OSTI ID: 1826213
Grant/Contract Number:  
AC02-05CH11231; AC02- 76SF00515; SC0004993; 21903058; 51961165105; SBK20190810; 2020B1515120039
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 60; Journal Issue: 47; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Li, Hui, Yu, Peiping, Lei, Renbo, Yang, Feipeng, Wen, Peng, Ma, Xiao, Zeng, Guosong, Guo, Jinghua, Toma, Francesca M., Qiu, Yejun, Geyer, Scott M., Wang, Xinwei, Cheng, Tao, and Drisdell, Walter S. Facet-Selective Deposition of Ultrathin Al2 O3 on Copper Nanocrystals for Highly Stable CO2 Electroreduction to Ethylene.. United States: N. p., 2021. Web. doi:10.1002/anie.202109600.
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Li, Hui, Yu, Peiping, Lei, Renbo, Yang, Feipeng, Wen, Peng, Ma, Xiao, Zeng, Guosong, Guo, Jinghua, Toma, Francesca M., Qiu, Yejun, Geyer, Scott M., Wang, Xinwei, Cheng, Tao, & Drisdell, Walter S. Facet-Selective Deposition of Ultrathin Al2 O3 on Copper Nanocrystals for Highly Stable CO2 Electroreduction to Ethylene.. United States. https://doi.org/10.1002/anie.202109600
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Li, Hui, Yu, Peiping, Lei, Renbo, Yang, Feipeng, Wen, Peng, Ma, Xiao, Zeng, Guosong, Guo, Jinghua, Toma, Francesca M., Qiu, Yejun, Geyer, Scott M., Wang, Xinwei, Cheng, Tao, and Drisdell, Walter S. Mon . "Facet-Selective Deposition of Ultrathin Al2 O3 on Copper Nanocrystals for Highly Stable CO2 Electroreduction to Ethylene.". United States. https://doi.org/10.1002/anie.202109600. https://www.osti.gov/servlets/purl/1834366.
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@article{osti_1834366,
title = {Facet-Selective Deposition of Ultrathin Al2 O3 on Copper Nanocrystals for Highly Stable CO2 Electroreduction to Ethylene.},
author = {Li, Hui and Yu, Peiping and Lei, Renbo and Yang, Feipeng and Wen, Peng and Ma, Xiao and Zeng, Guosong and Guo, Jinghua and Toma, Francesca M. and Qiu, Yejun and Geyer, Scott M. and Wang, Xinwei and Cheng, Tao and Drisdell, Walter S.},
abstractNote = {Abstract Catalysts based on Cu nanocrystals (NCs) for electrochemical CO 2 ‐to‐C 2+ conversion with high activity have been a subject of considerable interest, but poor stability and low selectivity for a single C 2+ product remain obstacles for realizing sustainable carbon‐neutral cycles. Here, we used the facet‐selective atomic layer deposition (FS‐ALD) technique to selectively cover the (111) surface of Cu NCs with ultrathin Al 2 O 3 to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C 2 H 4 /CH 4 for overcoated Cu NCs 22 times higher than that for pure Cu NCs. Peak performance of the overcoated catalyst (Cu NCs/Al 2 O 3 ‐10C) reaches a C 2 H 4 faradaic efficiency of 60.4 % at a current density of 300 mA cm −2 in 5 M KOH electrolyte, when using a gas diffusion electrode flow cell. Moreover, the Al 2 O 3 overcoating effectively suppresses the dynamic mobility and the aggregation of Cu NCs, which explains the negligible activity loss and selectivity degradations of Cu NCs/Al 2 O 3 ‐10C shown in stability tests.},
doi = {10.1002/anie.202109600},
journal = {Angewandte Chemie (International Edition)},
number = 47,
volume = 60,
place = {United States},
year = {Mon Sep 20 00:00:00 EDT 2021},
month = {Mon Sep 20 00:00:00 EDT 2021}
}
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https://doi.org/10.1002/anie.202109600
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