Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2

Yan Shen, Chunjin Ren, Lirong Zheng, Xiaoyong Xu, Ran Long, Wenqing Zhang, Yong Yang, Yongcai Zhang, Yingfang Yao, Haoqiang Chi, Jinlan Wang (), Qing Shen, Yujie Xiong (), Zhigang Zou and Yong Zhou ()
Additional contact information
Yan Shen: Nanjing University
Chunjin Ren: Southeast University
Lirong Zheng: Chinese Academy of Sciences
Xiaoyong Xu: Yangzhou University
Ran Long: University of Science and Technology of China
Wenqing Zhang: University of Science and Technology of China
Yong Yang: Nanjing University of Science and Technology
Yongcai Zhang: Yangzhou University
Yingfang Yao: Nanjing University
Haoqiang Chi: Nanjing University
Jinlan Wang: Southeast University
Qing Shen: Graduate School of Informatics and Engineering
Yujie Xiong: University of Science and Technology of China
Zhigang Zou: Nanjing University
Yong Zhou: Nanjing University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Photochemical conversion of CO2 into high-value C2+ 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 CO2 into C3H8 is prepared by implanting Cu single atoms on Ti0.91O2 atomically-thin single layers. Cu single atoms promote the formation of neighbouring oxygen vacancies (VOs) in Ti0.91O2 matrix. These oxygen vacancies modulate the electronic coupling interaction between Cu atoms and adjacent Ti atoms to form a unique Cu-Ti-VO unit in Ti0.91O2 matrix. A high electron-based selectivity of 64.8% for C3H8 (product-based selectivity of 32.4%), and 86.2% for total C2+ hydrocarbons (product-based selectivity of 50.2%) are achieved. Theoretical calculations suggest that Cu-Ti-VO unit may stabilize the key *CHOCO and *CH2OCOCO intermediates and reduce their energy levels, tuning both C1-C1 and C1-C2 couplings into thermodynamically-favourable exothermal processes. Tandem catalysis mechanism and potential reaction pathway are tentatively proposed for C3H8 formation, involving an overall (20e− – 20H+) reduction and coupling of three CO2 molecules at room temperature.

Date: 2023
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DOI: 10.1038/s41467-023-36778-5

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