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Cited by 393CO2 Reduction Techniques and CatalystsCatalysts for Methane ReformingAdvanced Photocatalysis Techniques

The DOI matches its Crossref record; 48 of the 48 references it cites were found in a registry or an index.

Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2

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Liang, Zhi-Qin, Zhuang, Tao-Tao, Seifitokaldani, Ali, Li, Jun, Huang, Chun-Wei, Tan, Chih-Shan, Li, Yi, De Luna, Phil, Dinh, Cao Thang, Hu, Yongfeng, Xiao, Qunfeng, Hsieh, Pei-Lun, Wang, Yuhang, Li, Fengwang, Quintero-Bermudez, Rafael, Zhou, Yansong, Chen, Peining, Pang, Yuanjie, Lo, Shen-Chuan, Chen, Lih-Juann, Tan, Hairen, Xu, Zheng, Zhao, Suling, Sinton, David, Sargent, Edward H.·2018·Nature Communications
DOI 10.1038/s41467-018-06311-0PMC PMC6148248
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Abstract

Copper-based materials are promising electrocatalysts for CO 2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO 2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO 2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C 2+ products. We achieve a 40-fold enhancement in the ratio of C 2+ to the competing CH 4 compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO 2 reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier—a rate-limiting step in CO 2 reduction to multi-carbon products.

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Figures

Fig. 1 Electrocatalyst design and the corresponding XPS characterization. a Schematic of preparing the Cu-on-Cu3N catalyst. b XPS spectra of Cu 2p, N 1 s, and Auger Cu LMM of the Cu3N nanocrystals with long organic ODA (i), the Cu3N nanocrystals with an oxide layer after N3- ligand exchange (ii), and the Cu-on-Cu3N composite after initial electroreduction (iii)
Fig. 1 Electrocatalyst design and the corresponding XPS characterization. a Schematic of preparing the Cu-on-Cu3N catalyst. b XPS spectra of Cu 2p, N 1 s, and Auger Cu LMM of the Cu3N nanocrystals with long organic ODA (i), the Cu3N nanocrystals with an oxide layer after N3- ligand exchange (ii), and the Cu-on-Cu3N composite after initial electroreduction (iii)CC BY · PubMed Central
Fig. 2 TEM characterization of the Cu-on-Cu3N catalyst. a, b HADDF-STEM images. c STEM-EELS Cu and N Element mapping of one individual particle in b, d, EEL spectra of element N K-edge circled as point A and point B in b. The scale bars are 50 nm in a, and 10 nm in b and c
Fig. 2 TEM characterization of the Cu-on-Cu3N catalyst. a, b HADDF-STEM images. c STEM-EELS Cu and N Element mapping of one individual particle in b, d, EEL spectra of element N K-edge circled as point A and point B in b. The scale bars are 50 nm in a, and 10 nm in b and cCC BY · PubMed Central
Fig. 3 In situ characterization of the structure and chemical state for the catalysts during CO2 reduction. a Cu K-edge XAS spectra of the Cu-on-Cu3N catalyst as function of reaction time at −0.95 V vs RHE. b The first derivatives of the spectra in a. c In situ Cu K-edge spectra during the initial 30 min on the catalysts: Cu-on-Cu3N (green) and Cu-on-Cu2O (orange). Spectra of Cu (red) and Cu3N (yellow) are also listed as references. d Ratio of Cu+ relative to the reaction time at −0.95 V vs RHE
Fig. 3 In situ characterization of the structure and chemical state for the catalysts during CO2 reduction. a Cu K-edge XAS spectra of the Cu-on-Cu3N catalyst as function of reaction time at −0.95 V vs RHE. b The first derivatives of the spectra in a. c In situ Cu K-edge spectra during the initial 30 min on the catalysts: Cu-on-Cu3N (green) and Cu-on-Cu2O (orange). Spectra of Cu (red) and Cu3N (yellow) are also listed as references. d Ratio of Cu+ relative to the reaction time at −0.95 V vs RHECC BY · PubMed Central
Fig. 4 CO2 electroreduction performance of the designed catalysts. a Faradaic efficiency of the C2+ distribution on Cu-on-Cu3N at different potentials. b Comparison of faradaic efficiency for C2+ and the ratio of C2+/CH4 at −0.95 V vs RHE on Cu, Cu-on-Cu2O, and Cu-on-Cu3N. c C2+ partial current density at different potentials on the three catalysts. d Stability test of C2+ selectivity on the three catalysts. Experiments from a to d were performed in triplicates and the results are shown as mean ± standard deviation
Fig. 4 CO2 electroreduction performance of the designed catalysts. a Faradaic efficiency of the C2+ distribution on Cu-on-Cu3N at different potentials. b Comparison of faradaic efficiency for C2+ and the ratio of C2+/CH4 at −0.95 V vs RHE on Cu, Cu-on-Cu2O, and Cu-on-Cu3N. c C2+ partial current density at different potentials on the three catalysts. d Stability test of C2+ selectivity on the three catalysts. Experiments from a to d were performed in triplicates and the results are shown as mean ± standard deviationCC BY · PubMed Central

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  1. Papa, A. J. in Ullmann’s Encyclopedia of Industrial Chemistry (Wiley-VCH Verlag GmbH & Co. KGaA, South Charleston, 2000).

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Metadata

Authors
Liang, Z.-Q., Zhuang, T.-T., Seifitokaldani, A., Li, J., Huang, C.-W., Tan, C.-S., Li, Y., De Luna, P., Dinh, C. T., Hu, Y., Xiao, Q., Hsieh, P.-L., Wang, Y., Li, F., Quintero-Bermudez, R., Zhou, Y., Chen, P., Pang, Y., Lo, S.-C., Chen, L.-J., Tan, H., Xu, Z., Zhao, S., Sinton, D., & Sargent, E. H.
Affiliations
  • University of Toronto (CA)
  • Industrial Technology Research Institute (TW)
  • University of Science and Technology of China (CN)
  • Canadian Light Source (Canada) (CA)
  • National Tsing Hua University (TW)
  • Beijing Jiaotong University (CN)
Corresponding author
Sargent, Edward H.
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2018-09-20
Volume
9
Issue
1
Pages
3828-3828
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-018-06311-0
PMC
PMC6148248
OpenAlex
W2889577864
Cited by
393
References
48
Citations by year
2026: 22 · 2025: 48 · 2024: 62 · 2023: 64 · 2022: 58 · 2021: 59 · 2020: 54 · 2019: 25 · 2018: 1
FWCI
8.03
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • Europe PMC (PubMed Central) (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
Funders
  • Canadian Institute for Advanced Research
  • Canadian Light Source
  • University of Saskatchewan
  • Ontario Centres of Excellence
  • Nederlandse Organisatie voor Wetenschappelijk Onderzoek (680-50-1511, 680-50-151)
  • University of Toronto
  • Mitacs
  • China Scholarship Council
  • Beijing Jiaotong University
  • Canadian Institutes of Health Research
  • Natural Sciences and Engineering Research Council of Canada
  • Western Economic Diversification Canada
  • National Research Council Canada
  • Fonds de recherche du Québec – Nature et technologies
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
  • Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
Keywords
CO2 reduction, copper electrocatalysts, copper nitride, multi-carbon products, Faradaic efficiency, CO dimerization, reaction mechanism, catalyst stability, methane selectivity

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