Статья

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

Yan ShenCollege of Engineering and Applied Sciences, Nanjing University, Nanjing, ChinaChunjin RenSchool of Physics, Southeast University, Nanjing, ChinaLirong ZhengInstitute of High Energy Physics, Chinese Academy of Sciences, Beijing, ChinaXiaoyong XuChemistry Interdisciplinary Research Center, School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, ChinaRan LongHefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, ChinaWenqing ZhangHefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, ChinaYong YangKey Laboratory of Soft Chemistry and Functional Materials (MOE), Nanjing University of Science and Technology, Nanjing, ChinaYongcai ZhangChemistry Interdisciplinary Research Center, School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, ChinaYingfang YaoCollege of Engineering and Applied Sciences, Nanjing University, Nanjing, ChinaHaoqiang ChiKey Laboratory of Modern Acoustics (MOE), Institute of Acoustics, School of Physics, Jiangsu Key Laboratory of Nanotechnology, Eco-materials and Renewable Energy Research Center (ERERC), National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, ChinaJinlan WangSchool of Physics, Southeast University, Nanjing, China. [email protected]Qing ShenUniversity of Electrocommunication, Graduate School of Informatics and Engineering, Chofu, Tokyo, JapanYujie XiongHefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, China. [email protected]Zhigang ZouCollege of Engineering and Applied Sciences, Nanjing University, Nanjing, ChinaYong ZhouKey Laboratory of Modern Acoustics (MOE), Institute of Acoustics, School of Physics, Jiangsu Key Laboratory of Nanotechnology, Eco-materials and Renewable Energy Research Center (ERERC), National Laboratory of Solid State Microstructures, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, China. [email protected]

2023en

ABI

Аннотация

Abstract 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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Идентификаторы

DOI: 10.1038/s41467-023-36778-5

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