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New process of low-temperature methanol synthesis from CO/CO_2/H_2 based on dual-catalysis

Science China Chemistry 2002年第1期45卷 106-112页

作者：曾健青 TSUBAKINoritatsu FUJIMOTOKaoru Guangzhou Institute of Chemistry Chinese Academy of Sciences Guangzhou China University of Tokyo Tokyo Japan

A new process of low-temperature methanol synthesis from CO/CO2/H2 based on dual-catalysis has been developed. Some alcohols, especially 2-alcohol, were found to have high catalytic promoting effect on the synthesis of methanol from CO hydrogenation. At 443 K and 5 MPa, the synthesis of methanol could process high effectively, resulting from the synergic catalysis of Cu/ZnO solid catalyst and 2-alcohol solvent catalyst. The primary results showed that when 2-butanol was used as reaction solvent, the one-pass average yield and the selectivity of methanol, in 40 h continuous reaction at temperature as low as 443 K and 5 MPa, were high up to 46.51% and 98.94% respectively. The catalytic activity was stable and the reaction temperature was 80 K or so lower than that in current industry synthesis process. This new process hopefully will become a practical method for methanol synthesis at low temperature.

关键词： dual-catalysis methanol low-temperature synthesis new process.

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Decarboxylative Acylation of Carboxylic Acids:Reaction Investigation and Mechanistic Study

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CCS Chemistry 2022年第7期4卷 2469-2480页

作者： Xiaopeng Wu Jie Han Siyu Xia Weipeng Li Chengjian Zhu Jin Xie State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023 State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryShanghai 200032 Advanced Catalytic Engineering Research Center of the Ministry of Education Hunan UniversityChangsha 410082

Ketones serve as one of the most critical building blocks in organic synthesis,involving numerous functional group ***,we rep ort an unprecedented photoredox-nickel metallap hotoredox-catalyzed decarboxylative acylation of common aliphatic acids with readily available aromatic and aliphatic thioesters.A wide range of structurally diverse asymmetrical aryl alkyl and dialkyl ketones have been constructed in yields of up to 98% with this *** protocol has excellent reaction selectivity and functional group compatibility,representing a significant step forward in ketone *** one-pot decarboxylative acylation at the gram scale from two different carboxylic acids and the late-stage application for the synthesis of complex ketones shows its synthetic *** mechanistic experiments and density functional theory(DFT)calculations suggest that the decarboxylative acylation reaction operates via an underdeveloped Ni(Ⅰ)-Ni(Ⅱ)-Ni(Ⅰ)-Ni(Ⅲ)-Ni(Ⅰ)catalytic cycle.

关键词： metallaphotoredox decarboxylative acylation ketones synthesis dual-catalysis carboxylic acid

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