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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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container_title Chemical engineering journal (Lausanne, Switzerland : 1996)
container_volume 495
creator 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
description •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.
doi_str_mv 10.1016/j.cej.2024.153334
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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.</description><identifier>ISSN: 1385-8947</identifier><identifier>DOI: 10.1016/j.cej.2024.153334</identifier><language>eng</language><publisher>Elsevier B.V</publisher><subject>Bimetallic metals ; Component regulation ; Laser synthesis ; MOF ; Selective hydrogenation</subject><ispartof>Chemical engineering journal (Lausanne, Switzerland : 1996), 2024-09, Vol.495, p.153334, Article 153334</ispartof><rights>2024 Elsevier B.V.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c944-761c9eadd54bd7567bef970fc2b15988b12657cd85f1879bd6d0ce5bbb1b33973</cites><orcidid>0000-0002-2877-0395 ; 0000-0003-1262-1958</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Wang, Jiulong</creatorcontrib><creatorcontrib>Jian, Jie</creatorcontrib><creatorcontrib>Jing, Xixiang</creatorcontrib><creatorcontrib>Shuang, Yazhou</creatorcontrib><creatorcontrib>Wang, Shiyuan</creatorcontrib><creatorcontrib>Wang, Fang</creatorcontrib><creatorcontrib>Ma, Zelin</creatorcontrib><creatorcontrib>Guo, Pengfei</creatorcontrib><creatorcontrib>Shchukin, Dmitry</creatorcontrib><creatorcontrib>Vinokurov, Vladimir A.</creatorcontrib><creatorcontrib>Novikov, Andrei A.</creatorcontrib><creatorcontrib>Glotov, Aleksandr P.</creatorcontrib><creatorcontrib>Xue, Junmin</creatorcontrib><creatorcontrib>Cao, Tengfei</creatorcontrib><creatorcontrib>Fan, Xiaoli</creatorcontrib><creatorcontrib>Wang, Hongqiang</creatorcontrib><title>Laser assisted embedding of Pd10Cu bimetals in ZIF-8 enabling highly selective hydrogenation of C = C in π-bond conjugation</title><title>Chemical engineering journal (Lausanne, Switzerland : 1996)</title><description>•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. 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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.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.cej.2024.153334</doi><orcidid>https://orcid.org/0000-0002-2877-0395</orcidid><orcidid>https://orcid.org/0000-0003-1262-1958</orcidid></addata></record>
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ispartof Chemical engineering journal (Lausanne, Switzerland : 1996), 2024-09, Vol.495, p.153334, Article 153334
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source ScienceDirect Freedom Collection 2022-2024
subjects Bimetallic metals
Component regulation
Laser synthesis
MOF
Selective hydrogenation
title Laser assisted embedding of Pd10Cu bimetals in ZIF-8 enabling highly selective hydrogenation of C = C in π-bond conjugation
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