Isolation of Cu Atoms in Pd Lattice: Forming Highly Selective Sites for Photocatalytic Conversion of CO 2 to CH 4
Abstract
Photocatalytic conversion of CO 2 to CH 4, a carbon-neutral fuel, represents an appealing approach to remedy the current energy and environmental crisis; however, it suffers from the large production of CO and H 2 by side reactions. The design of catalytic sites for CO 2 adsorption and activation holds the key to address this grand challenge. In this Article, we develop highly selective sites for photocatalytic conversion of CO 2 to CH 4 by isolating Cu atoms in Pd lattice. According to our synchrotron-radiation characterizations and theoretical simulations, the isolation of Cu atoms in Pd lattice can play dual roles in the enhancement of CO 2 -to-CH 4 conversion: (1) providing the paired Cu–Pd sites for the enhanced CO 2 adsorption and the suppressed H 2 evolution; and (2) elevating the d -band center of Cu sites for the improved CO 2 activation. As a result, the Pd 7 Cu 1 –TiO 2 photocatalyst achieves the high selectivity of 96% for CH 4 production with a rate of 19.6 μmol g cat –1 h –1 . This work provides fresh insights into the catalytic site design for selective photocatalytic CO 2 conversion, and highlights the importance of catalyst lattice engineering at atomic precision to catalytic performance.
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Valuable fuels such as CO, CH4, CH3OH, HCOOH, and C2+ products have been generated through proton-assisted multiple electron-transfer processes.
“Many valuable fuels, such as CO, CH4, CH3OH, HCOOH, and C2+ products have been generated through proton-assisted multiple electron-transfer processes.306, 307, 308, 309, 310”
From Technologies and perspectives for achieving carbon neutrality (2021) · cites this paper as [307]
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- Authors
- Long, R., Li, Y., Liu, Y., Chen, S., Zheng, X., Gao, C., He, C., Chen, N., Qi, Z., Song, L., Jiang, J., Zhu, J., & Xiong, Y.
- Affiliations
- University of Science and Technology of China (CN)
- Corresponding author
- Xiong, Yujie
- ORCID
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-03-16
- Volume
- 139
- Issue
- 12
- Pages
- 4486-4492
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2593644763
- Cited by
- 571
- References
- 37
- Citations by year
- 2026: 28 · 2025: 47 · 2024: 62 · 2023: 61 · 2022: 94 · 2021: 79 · 2020: 63 · 2019: 50 · 2018: 71 · 2017: 16
- FWCI
- 14.62
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Journal of the American Chemical Society (publishedVersion)
- PubMed (publishedVersion)
- Funders
- Ministry of Science and Technology of the People's Republic of China (2014CB848900)
- China Postdoctoral Science Foundation (2015T80660)
- National Natural Science Foundation of China (21471141, 21601173, U1532135)
- Natural Science Foundation of Anhui Province (1608085QB24)
- Chinese Academy of Sciences (QYZDB-SSW-SLH018)
- Topics
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
- Physical Sciences › Chemical Engineering › Catalysis › Catalysts for Methane Reforming
- Keywords
- photocatalytic CO2 reduction, CO2 to CH4 conversion, TiO2 photocatalyst, CO2 adsorption, d-band center, lattice engineering, methane selectivity
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