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Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2
Open accessAbstract
Photochemical conversion of CO 2 into high-value C 2+ products is difficult to achieve due to the energetic and mechanistic challenges in forming multiple C-C bonds. Herein, an efficient photocatalyst for the conversion of CO 2 into C 3 H 8 is prepared by implanting Cu single atoms on Ti 0.91 O 2 atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (V O s) in Ti 0.91 O 2 matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-V O unit in Ti 0.91 O 2 matrix. A high electron-based selectivity of 64.8% for C 3 H 8 (product-based selectivity of 32.4%), and 86.2% for total C 2+ hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-V O unit may stabilize the key *CHOCO and *CH 2 OCOCO intermediates and reduce their energy levels, tuning both C 1-C 1 and C 1-C 2 couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are tentatively proposed for C 3 H 8 formation, involving an overall (20 e− – 20 H+) reduction and coupling of three CO 2 molecules at room temperature.
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Cited by
Chai, Y., Kong, Y., Lin, M., Lin, W., Shen, J., Long, J., Yuan, R., Dai, W., Wang, X., & Zhang, Z. (2023) · Nature Communications · doi:10.1038/s41467-023-41943-x · Cited by 267
Yang, K., Huang, Y., Wang, T., Li, Y., Du, Y., Ling, J., Fan, Z., Zhang, C., & Ma, C. (2024) · Advanced Materials · doi:10.1002/adma.202409832 · Cited by 86
Metadata
- Authors
- Shen, Y., Ren, C., Zheng, L., Xu, X., Long, R., Zhang, W., Yang, Y., Zhang, Y., Yao, Y., Chi, H., Wang, J., Shen, Q., Xiong, Y., Zou, Z., & Zhou, Y.
- Venue
- Nature Communications
- Published
- 2023-02-27
- Volume
- 14
- Issue
- 1
- Pages
- 1117-1117
- ISSN
- 2041-1723 (ISSN-L)
- OpenAlex
- W4322494161
- Cited by
- 355
- References
- 63
- FWCI
- 16.62
- Type
- journal article
- Language
- en
- Open access
- gold
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- Shen, Y., Ren, C., Zheng, L., Xu, X., Long, R., Zhang, W., Yang, Y., Zhang, Y., Yao, Y., Chi, H., Wang, J., Shen, Q., Xiong, Y., Zou, Z., & Zhou, Y. (2023). Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2. Nature Communications. https://doi.org/10.1038/s41467-023-36778-5
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