Ultrasmall Silver Clusters Stabilized on MgO for Robust Oxygen-Promoted Hydrogen Production from Formaldehyde Reforming.

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ID: 57601
2019
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Abstract
Efficient molecular hydrogen generation from renewable biomass-derived resources and water is of great importance to the sustainable development of the future society. Herein, ultrasmall Ag nanoclusters supported on a defect-rich MgO matrix (AgUCs/MgO) are synthesized by a facile impregnation/calcination method and are applied to robust oxygen-promoted formaldehyde reforming into H at room temperature. Density functional theory calculations and experimental observations show that the catalyst spatially builds up a channel for directional electron transfer from electron-rich Ag sites to the anti-bonding π orbital of chemisorbed bridged O molecules, leading to the implementation of low-temperature O adsorption and activation. The catalytically active species, OOH, is thus selectively generated via a preferential two-electron reduction of O with a low energy barrier on Ag sites, involving an unusual long-range proton-coupled electron transfer process. The OOH-AgUCs/MgO active center is efficient for the subsequent C-H activation and H generation, leading to a 3-fold improvement of the turnover frequency as compared with its analogous AgNPs/MgO catalyst. Our atomic-level design and synthetic strategy provide a platform that facilitates the construction of an electron-proton transfer channel for catalysis, altered adsorption configurations of activated reactants, and enhancement of catalytic hydrogen generation activity, extending a promising direction for the development of next-generation energy catalysts.
Reference Key
chen2019ultrasmallacs Use this key to autocite in the manuscript while using SciMatic Manuscript Manager or Thesis Manager
Authors Chen, Shuang;Liang, Shipan;Wu, Biling;Lan, Zhuohuang;Guo, Ziwei;Kobayashi, Hisayoshi;Yan, Xiaoqing;Li, Renhong;
Journal ACS applied materials & interfaces
Year 2019
DOI
10.1021/acsami.9b11023
URL
Keywords
formaldehyde hydrogen production cluster proton-coupled electron transfer reforming

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