Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce ...Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce their prospects as industrial catalyst.Herein, a novel hybrid material HPW@Zr-BTC,composed of 12-tungstophoric acid(HPW) and Zr^(Ⅳ)-benzene tri-carboxylate(Zr-BTC) metal-organic framework(MOF), was prepared via one-pot solvothermal method. Excellent HPW loading up to 32.3 wt% was achieved, and HPW@Zr-BTC composite proved to be highly stable, besides the crystalline morphology of Zr-BTC was intact. The catalytic activity of the hybrid composite was explored via Friedel-Crafts acylation of anisole with benzoyl chloride.The 28.2 wt% HPW@Zr-BTC showed excellent catalytic performance, with 99.4% anisole conversion and 97.6% yield(pmethoxybenzophenone) under solvent free conditions. Excellent retention of catalytic activity was achieved after at least five consecutive runs due to non-observable HPW leaching. The promising activity and stability of the catalyst forecasted its potential industrial applications.展开更多
基金supported by the National Key Research and Development Program of China(2016YFB0601303)the National Natural Science Foundation of China(51374193,21676278)+1 种基金Key Program of National Natural Science Foundation of China(9143420)Chinese Academy of Sciences,State Administration of Foreign Experts Affairs(CAS/SAFEA)International Partnership Program for Creative Research Teams(20140491518)
文摘Heteropoly acids(HPA) are well known for their versatile solid acid catalysis in diverse chemical reactions, however they suffer from low surface area(<10 m^2/g) and leaching into the reactions media, which reduce their prospects as industrial catalyst.Herein, a novel hybrid material HPW@Zr-BTC,composed of 12-tungstophoric acid(HPW) and Zr^(Ⅳ)-benzene tri-carboxylate(Zr-BTC) metal-organic framework(MOF), was prepared via one-pot solvothermal method. Excellent HPW loading up to 32.3 wt% was achieved, and HPW@Zr-BTC composite proved to be highly stable, besides the crystalline morphology of Zr-BTC was intact. The catalytic activity of the hybrid composite was explored via Friedel-Crafts acylation of anisole with benzoyl chloride.The 28.2 wt% HPW@Zr-BTC showed excellent catalytic performance, with 99.4% anisole conversion and 97.6% yield(pmethoxybenzophenone) under solvent free conditions. Excellent retention of catalytic activity was achieved after at least five consecutive runs due to non-observable HPW leaching. The promising activity and stability of the catalyst forecasted its potential industrial applications.