Atomic NbOx overlayers on palladium nanoparticles enhance selective hydrodehydroxylation

Ye Liu; Bin Zhang; Jing Xia; Mark Douthwaite; Minghua Dong; Haiyang Yuan; Xiaomeng Cheng; Sen Luan; Yuxuan Wu; Zhijuan Zhao; Jing Tai; Lihua Chen; Bao Lian Su; Buxing Han; Huizhen Liu

doi:10.1016/j.cej.2023.147687

Atomic NbOx overlayers on palladium nanoparticles enhance selective hydrodehydroxylation

Ye Liu, Bin Zhang, Jing Xia, Mark Douthwaite, Minghua Dong, Haiyang Yuan, Xiaomeng Cheng, Sen Luan, Yuxuan Wu, Zhijuan Zhao, Jing Tai, Lihua Chen, Bao Lian Su, Buxing Han, Huizhen Liu

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

Résumé

The implementation of strong metal–support interactions (SMSI) is an effective design strategy that can be used to control reaction selectivity. In this study, we present evidence for the existence of SMSI between Nb2O5 and Pd, which results in the formation of an atomic thick layer of NbOx that coats the surface of Pd nanoparticles. The NbOx layer was found to profoundly affect the catalytic hydrodehydroxylation of 5-(hydroxymethyl)furfural (HMF) to 5-methylfurfural (MF). Under optimal reaction conditions, it significantly increased MF selectivity (from 6.4% to 81.0%) compared to an analogous control sample at iso-conversion. Through probing these two materials, the origin of this enhancement was attributed to the blocking of active sites responsible for the (undesirable) hydrogenation of C = O moieties. Importantly, however, the NbOx overlayer did not appear to influence the ability of the material to activate H2 and preferentially dissociate C – OH on Nb2O5, which are key steps in the hydrodehydroxylation mechanism.

langue originale	Anglais
Numéro d'article	147687
journal	Chemical Engineering Journal
Volume	479
Les DOIs	https://doi.org/10.1016/j.cej.2023.147687
Etat de la publication	Publié - 1 janv. 2024

Financement

This work received financial support from the National Key Research and Development Program of China ( 2022YFA1504901 ), the National Natural Science Foundation of China (22293020, 22293022, 22179132, 22121002, 22293012, 22302209), and the Junior Fellowship of Beijing National Laboratory of Molecular Science (2021BMS20059).

Bailleurs de fonds	Numéro du bailleur de fonds
National Natural Science Foundation of China	22302209, 22121002, 22293012, 22293022, 22179132, 22293020
National Natural Science Foundation of China
National Key Research and Development Program of China	2022YFA1504901
National Key Research and Development Program of China
Beijing national laboratory for molecular sciences	2021BMS20059
Beijing national laboratory for molecular sciences

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@article{fe49e9cd277e41f49b0e3746678880fb,

title = "Atomic NbOx overlayers on palladium nanoparticles enhance selective hydrodehydroxylation",

abstract = "The implementation of strong metal–support interactions (SMSI) is an effective design strategy that can be used to control reaction selectivity. In this study, we present evidence for the existence of SMSI between Nb2O5 and Pd, which results in the formation of an atomic thick layer of NbOx that coats the surface of Pd nanoparticles. The NbOx layer was found to profoundly affect the catalytic hydrodehydroxylation of 5-(hydroxymethyl)furfural (HMF) to 5-methylfurfural (MF). Under optimal reaction conditions, it significantly increased MF selectivity (from 6.4% to 81.0%) compared to an analogous control sample at iso-conversion. Through probing these two materials, the origin of this enhancement was attributed to the blocking of active sites responsible for the (undesirable) hydrogenation of C = O moieties. Importantly, however, the NbOx overlayer did not appear to influence the ability of the material to activate H2 and preferentially dissociate C – OH on Nb2O5, which are key steps in the hydrodehydroxylation mechanism.",

keywords = "Biomass conversion, Metal encapsulation, Nb O catalysts 2 5, Selective hydrogenolysis, Strong metal–support interaction (SMSI), Nb O catalysts",

author = "Ye Liu and Bin Zhang and Jing Xia and Mark Douthwaite and Minghua Dong and Haiyang Yuan and Xiaomeng Cheng and Sen Luan and Yuxuan Wu and Zhijuan Zhao and Jing Tai and Lihua Chen and Su, {Bao Lian} and Buxing Han and Huizhen Liu",

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year = "2024",

month = jan,

day = "1",

doi = "10.1016/j.cej.2023.147687",

language = "English",

volume = "479",

journal = "Chemical Engineering Journal",

issn = "1385-8947",

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TY - JOUR

T1 - Atomic NbOx overlayers on palladium nanoparticles enhance selective hydrodehydroxylation

AU - Liu, Ye

AU - Zhang, Bin

AU - Xia, Jing

AU - Douthwaite, Mark

AU - Dong, Minghua

AU - Yuan, Haiyang

AU - Cheng, Xiaomeng

AU - Luan, Sen

AU - Wu, Yuxuan

AU - Zhao, Zhijuan

AU - Tai, Jing

AU - Chen, Lihua

AU - Su, Bao Lian

AU - Han, Buxing

AU - Liu, Huizhen

PY - 2024/1/1

Y1 - 2024/1/1

N2 - The implementation of strong metal–support interactions (SMSI) is an effective design strategy that can be used to control reaction selectivity. In this study, we present evidence for the existence of SMSI between Nb2O5 and Pd, which results in the formation of an atomic thick layer of NbOx that coats the surface of Pd nanoparticles. The NbOx layer was found to profoundly affect the catalytic hydrodehydroxylation of 5-(hydroxymethyl)furfural (HMF) to 5-methylfurfural (MF). Under optimal reaction conditions, it significantly increased MF selectivity (from 6.4% to 81.0%) compared to an analogous control sample at iso-conversion. Through probing these two materials, the origin of this enhancement was attributed to the blocking of active sites responsible for the (undesirable) hydrogenation of C = O moieties. Importantly, however, the NbOx overlayer did not appear to influence the ability of the material to activate H2 and preferentially dissociate C – OH on Nb2O5, which are key steps in the hydrodehydroxylation mechanism.

AB - The implementation of strong metal–support interactions (SMSI) is an effective design strategy that can be used to control reaction selectivity. In this study, we present evidence for the existence of SMSI between Nb2O5 and Pd, which results in the formation of an atomic thick layer of NbOx that coats the surface of Pd nanoparticles. The NbOx layer was found to profoundly affect the catalytic hydrodehydroxylation of 5-(hydroxymethyl)furfural (HMF) to 5-methylfurfural (MF). Under optimal reaction conditions, it significantly increased MF selectivity (from 6.4% to 81.0%) compared to an analogous control sample at iso-conversion. Through probing these two materials, the origin of this enhancement was attributed to the blocking of active sites responsible for the (undesirable) hydrogenation of C = O moieties. Importantly, however, the NbOx overlayer did not appear to influence the ability of the material to activate H2 and preferentially dissociate C – OH on Nb2O5, which are key steps in the hydrodehydroxylation mechanism.

KW - Biomass conversion

KW - Metal encapsulation

KW - Nb O catalysts 2 5

KW - Selective hydrogenolysis

KW - Strong metal–support interaction (SMSI)

KW - Nb O catalysts

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Atomic NbOx overlayers on palladium nanoparticles enhance selective hydrodehydroxylation

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