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
Two-dimensional （2D） MoS2 is used as a catalyst or support and has received increased research interest because of its superior structural and electronic properties compared with those of bulk structures. In this ar...Two-dimensional （2D） MoS2 is used as a catalyst or support and has received increased research interest because of its superior structural and electronic properties compared with those of bulk structures. In this article, we illustrate the active sites of 2D MoS2 and various strategies for enhancing its intrinsic catalytic activity. The recent advances in the use of 2D MoS2-based materials for applications such as thermocatalysis, electrocatalysis, and photocatalysis are discussed. We also discuss the future opportunities and challenges for 2D MoS2-based materials, in both fundamental research and industrial applications.展开更多
High costs and low catalytic efficiency of metalloporphyrins, which are an analogue of cytochrome P450 enzyme, are the bot-tlenecks in the industrialization of biomimetic hydrocarbon oxidation reactions. The basic pri...High costs and low catalytic efficiency of metalloporphyrins, which are an analogue of cytochrome P450 enzyme, are the bot-tlenecks in the industrialization of biomimetic hydrocarbon oxidation reactions. The basic principle and research technique of physical organic chemistry were applied to the process of biomimetic oxidation of hydrocarbon catalyzed by metalloporphyrins. This biomimetic technology could be adapted to bulk chemicals production by developing the new methods for efficient scale-up synthesis of metalloporphyrins, new pathways for molecular oxygen activation on an industrial scale and new approaches to elevate the catalytic efficiency of metalloporphyrins. This review mainly focuses on research carried out in our group.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.
基金We gratefully acknowledge the financial support from the Ministry of Science and Technology of China （Grant Nos. 2016YFA0204100 and 2016YFA0200200）, the Na- tional Natural Science Foundation of China （Grant Nos. 21573220 and 21621063）, the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences （Grant No. QYZDB-SSW- JSC020）, and the Strategic Priority Research Program of the Chi- nese Academy of Sciences （Grant No. XDA09030100）.
文摘Two-dimensional （2D） MoS2 is used as a catalyst or support and has received increased research interest because of its superior structural and electronic properties compared with those of bulk structures. In this article, we illustrate the active sites of 2D MoS2 and various strategies for enhancing its intrinsic catalytic activity. The recent advances in the use of 2D MoS2-based materials for applications such as thermocatalysis, electrocatalysis, and photocatalysis are discussed. We also discuss the future opportunities and challenges for 2D MoS2-based materials, in both fundamental research and industrial applications.
基金supported by the National Natural Science Foundation of China (0142003, 20376018, 2890047, 29372047 , 2950041)National High-Tech Research & Development Program of China (863 Program, 2002AA321070 and 2006AA32Z467)National Key Technologies R & D Program of China (2004BA322B)
文摘High costs and low catalytic efficiency of metalloporphyrins, which are an analogue of cytochrome P450 enzyme, are the bot-tlenecks in the industrialization of biomimetic hydrocarbon oxidation reactions. The basic principle and research technique of physical organic chemistry were applied to the process of biomimetic oxidation of hydrocarbon catalyzed by metalloporphyrins. This biomimetic technology could be adapted to bulk chemicals production by developing the new methods for efficient scale-up synthesis of metalloporphyrins, new pathways for molecular oxygen activation on an industrial scale and new approaches to elevate the catalytic efficiency of metalloporphyrins. This review mainly focuses on research carried out in our group.
