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Xing Ma, Hang Liu, Weijie Yang, Guangyang Mao, Lirong Zheng, Hai‐Long Jiang
Well-organized photosensitive units and catalytic sites in proximity are crucial for improving charge separation efficiency and boosting photocatalysis. Herein, a general and facile strategy for the construction of high-loading (>4 wt %) single-atom catalysts (SACs) with a tunable coordination microenvironment has been developed on the basis of metal–organic frameworks (MOFs). The neighboring −O/OH x groups from a Zr 6 -oxo cluster in the MOFs provide lone-pair electrons and charge balance to immobilize the extraneous single metal atoms. The well-accessible and atomically dispersed metal sites possess close proximity to the photosensitive units (i.e., linkers), which greatly accelerates charge transfer and thereby promotes the redox reaction. The coordination environment of the representative single-atom Ni sites significantly modulates the electronic state and the proton activation barrier toward hydrogen production. As a result, the optimized Ni 1 –S/MOF with a unique Ni(I) microenvironment presents excellent photocatalytic H 2 production activity, up to 270 fold of the pristine MOF and far surpassing the other Ni 1 –X/MOF counterparts. This work unambiguously demonstrates the great advantage of MOFs in the fabrication of high-content SACs with variable microenvironments that are in close proximity to photosensitive linkers, thereby facilitating the electron transfer and promoting photocatalysis.
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Ma, X., Liu, H., Yang, W., Mao, G., Zheng, L., & Jiang, H. (2021). Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis. Journal of the American Chemical Society, 143(31), 12220–12229. https://doi.org/10.1021/jacs.1c05032
Ma, Xing, et al. "Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis." Journal of the American Chemical Society, vol. 143, no. 31, 2021, pp. 12220–12229, https://doi.org/10.1021/jacs.1c05032.
Ma, Xing, Hang Liu, Weijie Yang, Guangyang Mao, Lirong Zheng, and Hai‐Long Jiang. "Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis." Journal of the American Chemical Society 143, no. 31 (2021): 12220–12229. https://doi.org/10.1021/jacs.1c05032.
Ma X., Liu H., Yang W. [и др.] Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis // Journal of the American Chemical Society. — 2021. — Vol. 143, № 31. — P. 12220–12229. — URL: https://doi.org/10.1021/jacs.1c05032
@article{ma2021modulating,
title = {{Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis}},
author = {Xing Ma and Hang Liu and Weijie Yang and Guangyang Mao and Lirong Zheng and Hai‐Long Jiang},
journal = {Journal of the American Chemical Society},
year = {2021},
volume = {143},
number = {31},
pages = {12220--12229},
doi = {10.1021/jacs.1c05032},
url = {https://doi.org/10.1021/jacs.1c05032}
}TY - JOUR AU - Ma, Xing AU - Liu, Hang AU - Yang, Weijie AU - Mao, Guangyang AU - Zheng, Lirong AU - Jiang, Hai‐Long TI - Modulating Coordination Environment of Single-Atom Catalysts and Their Proximity to Photosensitive Units for Boosting MOF Photocatalysis JO - Journal of the American Chemical Society VL - 143 IS - 31 SP - 12220 EP - 12229 PY - 2021 DA - 2021/07/29 DO - 10.1021/jacs.1c05032 UR - https://doi.org/10.1021/jacs.1c05032 ER -
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