Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers

Yingzhang Shi, Peng Li, Huiling Chen, Zhiwen Wang, Yujie Song, Yu Tang, Sen Lin (), Zhiyang Yu (), Ling Wu (), Jimmy C. Yu and Xianzhi Fu
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Yingzhang Shi: Fuzhou University
Peng Li: Fuzhou University
Huiling Chen: Fuzhou University
Zhiwen Wang: Fuzhou University
Yujie Song: Fuzhou University
Yu Tang: Fuzhou University
Sen Lin: Fuzhou University
Zhiyang Yu: Fuzhou University
Ling Wu: Fuzhou University
Jimmy C. Yu: Fuzhou University
Xianzhi Fu: Fuzhou University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Adsorption and activation of C–H bonds by photocatalysts are crucial for the efficient conversion of C–H bonds to produce high-value chemicals. Nevertheless, the delivery of surface-active oxygen species for C–H bond oxygenation inevitably needs to overcome obstacles due to the separated active centers, which suppresses the catalytic efficiency. Herein, Ni dopants are introduced into a monolayer Bi2WO6 to create cascaded active units consisting of unsaturated W atoms and Bi/O frustrated Lewis pairs. Experimental characterizations and density functional theory calculations reveal that these special sites can establish an efficient and controllable C–H bond oxidation process. The activated oxygen species on unsaturated W are readily transferred to the Bi/O sites for C–H bond oxygenation. The catalyst with a Ni mass fraction of 1.8% exhibits excellent toluene conversion rates and high selectivity towards benzaldehyde. This study presents a fascinating strategy for toluene oxidation through the design of efficient cascaded active units.

Date: 2024
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DOI: 10.1038/s41467-024-49005-6

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