Boosting Catalysis of Pd Nanoparticles in MOFs by Pore Wall Engineering: The Roles of Electron Transfer and Adsorption Energy

Advanced Materials
Dongxiao ChenHai-Long Jiang

Abstract

The chemical environment of metal nanoparticles (NPs) possesses significant influence on their catalytic performance yet is far from being well understood. Herein, tiny Pd NPs are encapsulated into the pore space of metal-organic frameworks (MOFs), UiO-66-X (X = H, OMe, NH2 , 2OH, 2OH(Hf)), affording Pd@UiO-66-X composites. The surface microenvironment of the Pd NPs is readily modulated by pore wall engineering, via the functional group and metal substitution in the MOFs. Consequently, the catalytic activity of Pd@UiO-66-X follows the order of Pd@UiO-66-OH > Pd@UiO-66-2OH(Hf) > Pd@UiO-66-NH2 > Pd@UiO-66-OMe > Pd@UiO-66-H toward the hydrogenation of benzoic acid. It is found that the activity difference is not only ascribed to the distinct charge transfer between Pd and the MOF, but is also explained by the discriminated substrate adsorption energy of Pd@UiO-66-X (-OH < -2OH(Hf) < -NH2 < -OMe < -H), based on CO-diffuse reflectance infrared Fourier transform spectra and density-functional theory (DFT) calculations. The Pd@UiO-66-OH, featuring a high Pd electronic state and moderate adsorption energy, displays the highest activity. This work highlights the influence of the surface microenvironment of guest metal NPs, the catalytic...Continue Reading

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Citations

Aug 26, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Qiu-Ting FuZhi-Guo Gu
Dec 8, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Yohei TakashimaKensuke Akamatsu
Apr 25, 2021·Advanced Materials·Weiqing XuChengzhou Zhu
May 14, 2021·The Journal of Physical Chemistry Letters·Suhwan KimKwanghyo Son
Jun 3, 2021·Membranes·Po-Hsiang TangChia-Her Lin
Jul 10, 2021·Journal of the American Chemical Society·Shenjie WuJing Li
Aug 10, 2021·ACS Applied Materials & Interfaces·Peishan QinFengwei Huo
Nov 11, 2020·ACS Applied Materials & Interfaces·Wenlei ZhangFengwei Huo
May 30, 2021·Advanced Materials·Yu ShenFengwei Huo
Sep 29, 2021·ACS Applied Materials & Interfaces·Shan ZhongQiang Xu

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