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Laser assisted embedding of Pd10Cu bimetals in ZIF-8 enabling highly selective hydrogenation of C = C in π-bond conjugation

•The first synthesis of laser-assisted ultrafine bimetallic catalysts embedded in a porous MOF matrix.•Bimetallic PdCu catalyst induces the formation of an arch structure for CAL, improving selective hydrogenation of C = C within the π-bond conjugation.•Embedding Pd10Cu in MOFs leads to 98.03 % conv...

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Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2024-09, Vol.495, p.153334, Article 153334
Main Authors: Wang, Jiulong, Jian, Jie, Jing, Xixiang, Shuang, Yazhou, Wang, Shiyuan, Wang, Fang, Ma, Zelin, Guo, Pengfei, Shchukin, Dmitry, Vinokurov, Vladimir A., Novikov, Andrei A., Glotov, Aleksandr P., Xue, Junmin, Cao, Tengfei, Fan, Xiaoli, Wang, Hongqiang
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Language:English
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Summary:•The first synthesis of laser-assisted ultrafine bimetallic catalysts embedded in a porous MOF matrix.•Bimetallic PdCu catalyst induces the formation of an arch structure for CAL, improving selective hydrogenation of C = C within the π-bond conjugation.•Embedding Pd10Cu in MOFs leads to 98.03 % conversion of cinnamaldehyde with 100 % selectivity of the C = C bond is achieved. Selective hydrogenation of vinyl groups (C = C) and carbonyl groups (C = O) is of significance to effectively convert low-value organic compounds into high-value target chemicals, while a challenge remains on the hydrogenation of C = C bond that is in π-bond conjugation with the C = O bond. Herein, we address this challenge based on a synergetic modulation strategy on electronic structure and adsorption configurations to achieve a highly selective hydrogenation of the C = C bond, achieved by laser-assisted embedding of PdxCu bimetals in the ZIF-8 bulk phase (x represents the Pd/Cu molar ratio in PdCu nanoparticles). It is revealed that laser assisted synthesis of PdxCu bimetals not only inhibits the hydrogenation of C = O and promotes the hydrogenation of C = C, but also results in an arched absorption configuration for substrate molecules that facilitates the selective hydrogenation of vinyl groups. Exemplified by cinnamaldehyde (CAL), the present work achieves 98.03 % conversion of CAL and 100 % selectivity of the hydrocinnamaldehyde (HCAL) (70 °C, 1 MPa H2, 1 h), indicating the potential of laser-matter interaction to tackle the trade-off between conversion efficiency and selectivity in thermal catalysis.
ISSN:1385-8947
DOI:10.1016/j.cej.2024.153334