Rational design of palladium single-atoms and clusters supported on silicoaluminophosphate-31 by a photochemical route for chemoselective hydrodeoxygenation of vanillin  

作　　者：Xiaowen Lu Chunmu Guo Mingyang Zhang Leipeng Leng J.Hugh Horton Wei Wu Zhijun Li 

机构地区：[1]Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science,College of Chemistry and Chemical Engineering,Northeast Petroleum University,Daqing,163318,China [2]National Center for International Research on Catalytic Technology,School of Chemistry and Material Science,Heilongjiang University,Harbin,150080,China [3]Department of Chemistry,Queen’s University,Kingston,K7L 3N6,Canada

出　　处：《Nano Research》2021年第11期4347-4355,共9页纳米研究（英文版）

基　　金：The authors greatly acknowledge the financial support from the China Postdoctoral Science Foundation(Nos.2019M661247 and 2020T130091);Postdoctoral Science Foundation of Heilongjiang Province(LBH-Z19047);Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China(719900091);Key Laboratory of Functional Inorganic Material Chemistry(Heilongjiang University),Ministry of Education.

摘　　要：Chemoselective hydrodeoxygenation of vanillin is of great importance in converting biomass into high value-added chemicals.Herein,we describe a facile photochemical route to access palladium single atoms and clusters supported on silicoaluminophosphate-31(SAPO-31)as a highly active,chemoselective,and reusable catalyst for hydrodeoxygenation of vanillin.Characterizations by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy,extended X-ray absorption fine structure measurement,and CO-absorbed diffuse reflectance infrared Fourier transform spectroscopy reveal the atomically dispersed palladium single atoms and clusters are loosely bonded and randomly dispersed,without forming strong palladium-palladium metallic bonding,over the SAPO-31 support.This catalyst,with a full metal availability to the reactants,exhibits exceptional catalytic activity(TOF:3,000 h^(−1),Yield:>99%)in the hydrodeoxygenation of vanillin toward 2-methoxy-4-methylphenol(MMP)under mild conditions(1 atm,80°C,30 min),along with excellent stability,scalability(up to 100-fold),and wide substrate scope.The superior catalytic performance can be attributed to the synergistic effect of the positively charged palladium single atoms and fully exposed clusters,as well as the strong metal-support interactions.This work may offer a new avenue for the design and synthesis of fully exposed metal catalysts with targeted functionalities.

关 键 词：heterogeneous catalysis photochemical reduction palladium single atoms and clusters atomic dispersion HYDRODEOXYGENATION VANILLIN 

分 类 号：O64[理学—物理化学]