Water-assisted hydrogen spillover in Pt nanoparticle-based metal–organic framework composites

Zhida Gu, Mengke Li, Cheng Chen, Xinglong Zhang, Chengyang Luo, Yutao Yin, Ruifa Su, Suoying Zhang, Yu Shen, Yu Fu (), Weina Zhang () and Fengwei Huo ()
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Zhida Gu: Northeastern University
Mengke Li: Nanjing Tech University (NanjingTech)
Cheng Chen: Nanjing Tech University (NanjingTech)
Xinglong Zhang: Nanjing Tech University (NanjingTech)
Chengyang Luo: Nanjing Tech University (NanjingTech)
Yutao Yin: Nanjing Tech University (NanjingTech)
Ruifa Su: Nanjing Tech University (NanjingTech)
Suoying Zhang: Nanjing Tech University (NanjingTech)
Yu Shen: Nanjing University of Posts & Telecommunications
Yu Fu: Northeastern University
Weina Zhang: Nanjing Tech University (NanjingTech)
Fengwei Huo: Nanjing Tech University (NanjingTech)

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Hydrogen spillover is the migration of activated hydrogen atoms from a metal particle onto the surface of catalyst support, which has made significant progress in heterogeneous catalysis. The phenomenon has been well researched on oxide supports, yet its occurrence, detection method and mechanism on non-oxide supports such as metal–organic frameworks (MOFs) remain controversial. Herein, we develop a facile strategy for efficiency enhancement of hydrogen spillover on various MOFs with the aid of water molecules. By encapsulating platinum (Pt) nanoparticles in MOF-801 for activating hydrogen and hydrogenation of C=C in the MOF ligand as activated hydrogen detector, a research platform is built with Pt@MOF-801 to measure the hydrogenation region for quantifying the efficiency and spatial extent of hydrogen spillover. A water-assisted hydrogen spillover path is found with lower migration energy barrier than the traditional spillover path via ligand. The synergy of the two paths explains a significant boost of hydrogen spillover in MOF-801 from imperceptible existence to spanning at least 100-nm-diameter region. Moreover, such strategy shows universality in different MOF and covalent organic framework materials for efficiency promotion of hydrogen spillover and improvement of catalytic activity and antitoxicity, opening up new horizons for catalyst design in porous crystalline materials.

Date: 2023
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DOI: 10.1038/s41467-023-40697-w

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