The DOI matches its Crossref record; 9 of the 9 references it cites were found in a registry or an index.
Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts
Open accessAbstract
Atomic-level coordination engineering is an efficient strategy for tuning the catalytic performance of single-atom catalysts (SACs). However, their rational design has so far been plagued by the lack of a universal correlation between the coordination symmetry and catalytic properties. Herein, we synthesised planar-symmetry-broken CuN 3 (PSB-CuN 3) SACs through microwave heating for electrocatalytic CO 2 reduction. Remarkably, the as-prepared catalysts exhibited a selectivity of 94.3% towards formate at −0.73 V vs. RHE, surpassing the symmetrical CuN 4 catalyst (72.4% at −0.93 V vs. RHE). In a flow cell equipped with a PSB-CuN 3 electrode, over 90% formate selectivity was maintained at an average current density of 94.4 mA cm−2 during 100 h operation. By combining definitive structural identification with operando X-ray spectroscopy and theoretical calculations, we revealed that the intrinsic local symmetry breaking from planar D4 h configuration induces an unconventional dsp hybridisation, and thus a strong correlation between the catalytic activity and microenvironment of metal centre (i.e., coordination number and distortion), with high preference for formate production in CuN 3 moiety. The finding opens an avenue for designing efficient SACs with specific local symmetries for selective electrocatalysis.
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Cites
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Yang, H. B., Hung, S.-F., Liu, S., Yuan, K., Miao, S., Zhang, L., Huang, X., Wang, H.-Y., Cai, W., Chen, R., et al. (2018) · Nature Energy · doi:10.1038/s41560-017-0078-8 · Cited by 2,239
Self-citationLi, C. W., & Kanan, M. W. (2012) · Journal of the American Chemical Society · doi:10.1021/ja3010978 · Cited by 2,000
Self-citationFei, H., Dong, J., Feng, Y., Allen, C. S., Wan, C., Volosskiy, B., Li, M., Zhao, Z., Wang, Y., Sun, H., et al. (2018) · Nature Catalysis · doi:10.1038/s41929-017-0008-y · Cited by 1,973
Self-citationPartially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel
Gao, S., Lin, Y., Jiao, X., Sun, Y., Luo, Q., Zhang, W., Li, D., Yang, J., & Xie, Y. (2016) · Nature · doi:10.1038/nature16455 · Cited by 1,865
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Single-atom Rh/N-doped carbon electrocatalyst for formic acid oxidation
Xiong, Y., Dong, J., Huang, Z.-Q., Xin, P., Chen, W., Wang, Y., Li, Z., Jin, Z., Xing, W., Zhuang, Z., et al. (2020) · Nature Nanotechnology · doi:10.1038/s41565-020-0665-x · Cited by 610
Self-citationHighly Dense Cu Nanowires for Low-Overpotential CO 2 Reduction
Raciti, D., Livi, K. J., & Wang, C. (2015) · Nano Letters · doi:10.1021/acs.nanolett.5b03298 · Cited by 395
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Analysis of the limitations in the oxygen reduction activity of transition metal oxide surfaces
Li, H., Kelly, S., Guevarra, D., Wang, Z., Wang, Y., Haber, J. A., Anand, M., Gunasooriya, G. T. K. K., Abraham, C. S., Vijay, S., et al. (2021) · Nature Catalysis · doi:10.1038/s41929-021-00618-w · Cited by 341
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Jiang, M., Wang, H., Zhu, M., Luo, X., He, Y., Wang, M., Wu, C., Zhang, L., Li, X., Liao, X., et al. (2024) · Chemical Society Reviews · doi:10.1039/d3cs00857f · Cited by 299
Atomic Dispersed Co on NC@Cu Core‐Shells for Solar Seawater Splitting
Sun, Z., Cheng, S., Jing, X., Liu, K., Chen, Y., Wibowo, A. A., Yin, H., Usman, M., MacDonald, D., Cheong, S., et al. (2024) · Advanced Materials · doi:10.1002/adma.202406088 · Cited by 45
Metadata
- Authors
- Dong, J., Liu, Y., Pei, J., Li, H., Ji, S., Shi, L., Zhang, Y., Li, C., Tang, C., Liao, J., Xu, S., Zhang, H., Li, Q., & Zhao, S.
- Venue
- Nature Communications
- Published
- 2023-10-27
- Volume
- 14
- Issue
- 1
- Pages
- 6849-6849
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W4387972786
- Cited by
- 233
- References
- 9
- FWCI
- 10.91
- Type
- journal article
- Language
- en
- Open access
- gold
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- Dong, J., Liu, Y., Pei, J., Li, H., Ji, S., Shi, L., Zhang, Y., Li, C., Tang, C., Liao, J., Xu, S., Zhang, H., Li, Q., & Zhao, S. (2023). Continuous electroproduction of formate via CO2 reduction on local symmetry-broken single-atom catalysts. Nature Communications. https://doi.org/10.1038/s41467-023-42539-1
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