The DOI matches its Crossref record; 12 of the 12 references it cites were found in a registry or an index.
Efficient and Robust Carbon Dioxide Electroreduction Enabled by Atomically Dispersed Snδ+ Sites
Abstract
Electrocatalytic CO 2 reduction at considerably low overpotentials still remains a great challenge. Here, a positively charged single‐atom metal electrocatalyst to largely reduce the overpotentials is designed and hence CO 2 electroreduction performance is accelerated. Taking the metal Sn as an example, kilogram‐scale single‐atom Snδ+ on N‐doped graphene is first fabricated by a quick freeze–vacuum drying–calcination method. Synchrotron‐radiation X‐ray absorption fine structure and high‐angle annular dark‐field scanning transmission electron microscopy demonstrate the atomically dispersed Sn atoms are positively charged, which enables CO 2 activation and protonation to proceed spontaneously through stabilizing CO 2•−* and HCOO−*, affirmed by in situ Fourier transform infrared spectra and Gibbs free energy calculations. Furthermore, N‐doping facilitates the rate‐limiting formate desorption step, verified by the decreased desorption energy from 2.16 to 1.01 eV and the elongated SnHCOO− bond length. As an result, single‐atom Snδ+ on N‐doped graphene exhibits a very low onset overpotential down to 60 mV for formate production and shows a very large turnover frequency up to 11930 h−1, while its electroreduction activity proceeds without deactivation even after 200 h. This work offers a new pathway for manipulating electrocatalytic performance.
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Cites
Atomically dispersed Ni(i) as the active site for electrochemical CO2 reduction
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Self-citationElectroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper
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Atomic cobalt on nitrogen-doped graphene for hydrogen generation
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Ionic Liquid–Mediated Selective Conversion of CO 2 to CO at Low Overpotentials
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Sulfur-Modulated Tin Sites Enable Highly Selective Electrochemical Reduction of CO2 to Formate
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Wang, G., Chen, J., Ding, Y., Cai, P., Yi, L., Li, Y., Tu, C., Hou, Y., Wen, Z., & Dai, L. (2021) · Chemical Society Reviews · doi:10.1039/d0cs00071j · Cited by 1,295
In Situ/Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy
Timoshenko, J., & Roldan Cuenya, B. (2021) · Chemical Reviews · doi:10.1021/acs.chemrev.0c00396 · Cited by 931
Shi, Y., Ma, Z.-R., Xiao, Y.-Y., Yin, Y.-C., Huang, W.-M., Huang, Z.-C., Zheng, Y.-Z., Mu, F.-Y., Huang, R., Shi, G.-Y., et al. (2021) · Nature Communications · doi:10.1038/s41467-021-23306-6 · Cited by 894
Self-citationSingle atom electrocatalysts supported on graphene or graphene-like carbons
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Stable and Efficient Single-Atom Zn Catalyst for CO2 Reduction to CH4
Han, L., Song, S., Liu, M., Yao, S., Liang, Z., Cheng, H., Ren, Z., Liu, W., Lin, R., Qi, G., et al. (2020) · Journal of the American Chemical Society · doi:10.1021/jacs.9b12111 · Cited by 538
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Metadata
- Authors
- Zu, X., Li, X., Liu, W., Sun, Y., Xu, J., Yao, T., Yan, W., Gao, S., Wang, C., Wei, S., & Xie, Y.
- Venue
- Advanced Materials
- Publisher
- Wiley
- Published
- 2019-02-21
- Volume
- 31
- Issue
- 15
- Pages
- e1808135-e1808135
- ISSN
- 0935-9648 (ISSN-L)
- 1521-4095
- OpenAlex
- W2916946178
- Cited by
- 457
- References
- 12
- FWCI
- 12.32
- Type
- journal article
- Language
- en
- Open access
- closed
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- Zu, X., Li, X., Liu, W., Sun, Y., Xu, J., Yao, T., Yan, W., Gao, S., Wang, C., Wei, S., & Xie, Y. (2019). Efficient and Robust Carbon Dioxide Electroreduction Enabled by Atomically Dispersed Snδ+ Sites. Advanced Materials. https://doi.org/10.1002/adma.201808135
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