Pd-Catalyzed Dehydrogenation Enhanced by Charge Transfer from MoOx Promoter

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-01-13 DOI:10.1021/acscatal.4c04684

Byung Gwan Park, Jihyeon Lee, Yoojin Lee, Hyeongeon Lee, Jueun Kim, Eonu Nam, Jong-Seong Bae, Jeong Woo Han, Kwangjin An

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Abstract

Incorporating metal oxides is a sensible strategy for enhancing the efficiency of precious metals. Upon the introduction of molybdenum oxide, diverse coordination structures were formed on the support surface depending on the concentration used. This modified surface architecture orchestrates consequential alterations in the electronic and geometric configurations of the active metal, concurrently influencing the catalytic performance. In this study, MoO_x species were introduced into Pd in a controlled manner to substantially enhance the dehydrogenation activity of the N-heterocyclic liquid organic hydrogen carrier system. Pd−MoO_x/Al₂O₃ catalyst─featuring an optimal 0.18 wt % Mo loading─demonstrated noteworthy improvement in activity, surpassing Pd/Al₂O₃ by factors of 1.57 and 1.24, accompanied by enhanced recyclability in two distinct LOHC systems. Integrated characterization and theoretical calculations elucidated the modification of the electronic properties of both Pd and Al₂O₃ upon MoO_x introduction and the corresponding adsorption behavior of the reactants, highlighting the charge transfer phenomenon from Pd to MoO_x.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.