Enhancement of visible-light-driven oxidative amine coupling under aerobic and anaerobic conditions by photocatalyst with spatial separation of photoinduced charge carriers  

作　　者：Shasha Wang Kuan Gao Yang Cui Shuwen Li Heyao Zhang Bin Zhang Jie Wu Hongwei Hou Shuangquan Zang 

机构地区：[1]Green Catalysis Center,College of Chemistry,Zhengzhou University,Zhengzhou 450001,China [2]School of Chemical Engineering,Zhengzhou University,Zhengzhou 450001,China [3]School of Science,Xuchang University,Xuchang 461000,China

出　　处：《Nano Research》2023年第4期4715-4722,共8页纳米研究（英文版）

基　　金：supported by the National Natural Science Foundation of China(Nos.21771163 and 22171247);Zhongyuan thousand talents project.

摘　　要：Spatial separation of oxidation/reduction cocatalyst is an effective means to improve the efficiency of charge separation in photocatalytic reaction systems.Herein,a yolk-shell Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction was designed and synthesized by integration of electron collector Pd and hole collector Cu_(2)O inside and outside of a photoactive metal-organic framework(MOF)NH_(2)-UiO-66,respectively.The obtained Pd@NH_(2)-UiO-66@Cu_(2)O heterojunction effectively inhibits the electron and hole recombination through the photo-induced electrons and holes flow inward and outward of the composite,and promotes the reduction and oxidation abilities for the oxidative coupling of benzylamine to imines.Compared with Pd/NH_(2)-UiO-66@Cu_(2)O,Pd@NH_(2)-UiO-66,and Pd/NH_(2)-UiO-66,Pd@NH_(2)-UiO-66@Cu_(2)O exhibits the highest photocatalytic activity.More importantly,Pd@NH_(2)-UiO-66@Cu_(2)O shows a conversion rate of benzylamine up to 99%either by oxidation under aerobic conditions or by strong adsorption of H atom(Hads)under anaerobic conditions.In addition,the catalyst shows good stability and can be recycled at least ten times.This work provides useful guidance on construction of MOFs-based composites with spatially separated photoinduced charge carriers to realize efficient oxidation coupling of benzylamine in both aerobic and anaerobic conditions.

关 键 词：metal-organic frameworks palladium nanoparticle photocatalysis cuprous oxide oxidative coupling of amines 

分 类 号：O64[理学—物理化学]