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MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2
Abstract
A central topic in single-atom catalysis is building strong interactions between single atoms and the support for stabilization. Herein we report the preparation of stabilized single-atom catalysts via a simultaneous self-reduction stabilization process at room temperature using ultrathin two-dimensional Ti 3– x C 2 T y MXene nanosheets characterized by abundant Ti-deficit vacancy defects and a high reducing capability. The single atoms therein form strong metal–carbon bonds with the Ti 3– x C 2 T y support and are therefore stabilized onto the sites previously occupied by Ti. Pt-based single-atom catalyst (SAC) Pt 1 /Ti 3– x C 2 T y offers a green route to utilizing greenhouse gas CO 2, via the formylation of amines, as a C 1 source in organic synthesis. DFT calculations reveal that, compared to Pt nanoparticles, the single Pt atoms on Ti 3– x C 2 T y support feature partial positive charges and atomic dispersion, which helps to significantly decrease the adsorption energy and activation energy of silane, CO 2, and aniline, thereby boosting catalytic performance. We believe that these results would open up new opportunities for the fabrication of SACs and the applications of MXenes in organic synthesis.
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Cited by
Lim, K. R. G., Handoko, A. D., Nemani, S. K., Wyatt, B., Jiang, H.-Y., Tang, J., Anasori, B., & Seh, Z. W. (2020) · ACS Nano · doi:10.1021/acsnano.0c05482 · Cited by 585
Two-dimensional MXene-based and MXene-derived photocatalysts: Recent developments and perspectives
Zhong, Q., Li, Y., & Zhang, G. (2021) · Chemical Engineering Journal · doi:10.1016/j.cej.2020.128099 · Cited by 466
Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications
Song, Z., Zhang, L., Doyle‐Davis, K., Fu, X., Luo, J., & Sun, X. (2020) · Advanced Energy Materials · doi:10.1002/aenm.202001561 · Cited by 412
Rational Design of Flexible Two-Dimensional MXenes with Multiple Functionalities
Fu, Z., Wang, N., Legut, D., Si, C., Zhang, Q., Du, S., Germann, T. C., Francisco, J. S., & Zhang, R. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.9b00348 · Cited by 396
Zhu, J., Xia, L., Yu, R., Lu, R., Li, J., He, R., Wu, Y., Zhang, W., Hong, X., Chen, W., et al. (2022) · Journal of the American Chemical Society · doi:10.1021/jacs.2c03982 · Cited by 384
Metadata
- Authors
- Zhao, D., Chen, Z., Yang, W., Liu, S., Zhang, X., Yu, Y., Cheong, W.-C., Zheng, L., Ren, F., Ying, G., Cao, X., Wang, D., Peng, Q., Wang, G., & Chen, C.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-01-30
- Volume
- 141
- Issue
- 9
- Pages
- 4086-4093
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2913075899
- Cited by
- 767
- References
- 0
- FWCI
- 26.53
- Type
- journal article
- Language
- en
- Open access
- closed
- Licence
- Funders
- Ministry of Science and Technology of the People's Republic of China (2016YFA0202801, 2017YFA0700101)
- Natural Science Foundation of Beijing Municipality (JQ18007)
- China Postdoctoral Science Foundation (2018M631445, 2018M631486, 2018M631444)
- Ministry of Human Resources and Social Security (BX201700131)
- National Natural Science Foundation of China (21590792, 21866032, 51651201, 21872076, 21805184, 21573119)
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- Zhao, D., Chen, Z., Yang, W., Liu, S., Zhang, X., Yu, Y., Cheong, W.-C., Zheng, L., Ren, F., Ying, G., Cao, X., Wang, D., Peng, Q., Wang, G., & Chen, C. (2019). MXene (Ti3C2) Vacancy-Confined Single-Atom Catalyst for Efficient Functionalization of CO2. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.8b13579
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