本课题组2016级本科生-陈爽以第一作者在能源、催化材料知名期刊ACS Applied Materials & Interfaces杂志上发表了题为《Ultrasmall Silver Clusters Stabilized on MgO for Robust Oxygen-Promoted Hydrogen Production from Formaldehyde Reforming》的学术论文。该期刊2018年的影响因子达到了8.456。
论文摘要：
Efficient molecular hydrogen generation from renewable biomassderived 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 H2 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 O2 molecules, leading to the implementation of low-temperature O2 adsorption and activation. The catalytically active species, •OOH, is thus selectively generated via a preferential two-electron reduction of O2 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 H2 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.