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Title: Facet‐Selective Deposition of Ultrathin Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 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];  [4];  [5];  [6];  [1];  [4];  [1];  [5];  [6];  [3]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Joint Center for Artificial Photosynthesis Chemical Sciences Division Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley California 94720 USA
  2. Institute of Functional Nano and Soft Materials Soochow University Suzhou 215123 China
  3. School of Advanced Materials Shenzhen Graduate School Peking University Shenzhen 518055 China
  4. Advanced Light Source Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley California 94720 USA
  5. Shenzhen Engineering Lab of Flexible Transparent Conductive Films Department of Materials Science and Engineering Harbin Institute of Technology Shenzhen 518055 China
  6. Department of Chemistry Wake Forest University Winston-Salem North Carolina 27109 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1826397
Grant/Contract Number:  
SC0004993
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Angewandte Chemie
Additional Journal Information:
Journal Name: Angewandte Chemie Journal Volume: 133 Journal Issue: 47; Journal ID: ISSN 0044-8249
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

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 Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 Electroreduction to Ethylene. Germany: N. p., 2021. Web. doi:10.1002/ange.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 Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 Electroreduction to Ethylene. Germany. https://doi.org/10.1002/ange.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. Wed . "Facet‐Selective Deposition of Ultrathin Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 Electroreduction to Ethylene". Germany. https://doi.org/10.1002/ange.202109600.
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@article{osti_1826397,
title = {Facet‐Selective Deposition of Ultrathin Al 2 O 3 on Copper Nanocrystals for Highly Stable CO 2 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/ange.202109600},
journal = {Angewandte Chemie},
number = 47,
volume = 133,
place = {Germany},
year = {Wed Oct 13 00:00:00 EDT 2021},
month = {Wed Oct 13 00:00:00 EDT 2021}
}
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Publisher's Version of Record
https://doi.org/10.1002/ange.202109600
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