This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the...This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the research field of one-carbon(C1)chemistry,including catalytic conversion of C1 molecules to valuable chemicals and superclean fuels,innovative catalyst and reactor development,and the design of new catalytic reactions and processes.Organized chronologically,this review highlights Prof.Tsubaki’s academic contributions from 1990,when he studied and worked at The University of Tokyo,to his current role as a full professor at the University of Toyama.The academic section of this review is divided into three main parts,focusing on Prof.Tsubaki’s pioneering work in C1 chemistry.We believe that this review will serve as a highly valuable reference for colleagues in the fields of C1 chemistry and catalysis,and inspire the development of more original and groundbreaking research.展开更多
Methanol synthesis via CO_(2)conversion is a“green carbon”route for mitigating the greenhouse effect and recycling carbon resources.However,despite the widespread use of copper-based systems for methanol synthesis i...Methanol synthesis via CO_(2)conversion is a“green carbon”route for mitigating the greenhouse effect and recycling carbon resources.However,despite the widespread use of copper-based systems for methanol synthesis in recent decades,the chemical state of the active Cu species remains controversial.In this study,various Cu/ZnO/SBA-15 catalysts possessing different interfacial structures were engineered by atomic layer deposition(ALD).The optimized Cu/50c-ZnO/SBA-15 afforded the highest mass-specific methanol formation rate of 211.7 gMeOH·kgcat^(-1)·h^(-1)under the conditions of 250℃ and 3.0 MPa.In-depth characterizations indicated that the electronic state of Cu could be modulated by engineering the interfacial structures of the Cu/ZnO series catalysts,and the Cu cation sites(Cu^(δ+)and Cu^(+))are the active centers for methanol synthesis reaction rather than the Cu^(0)sites.Mechanistic analysis demonstrated that HCO_(3)^(*)and CO_(3)^(*)were slowly transformed to HCOO*and further hydrogenated to methanol following the formate-methoxy intermediate route.This work provides an improved understanding of the origin of the methanol synthesis active centers and emphasizes the potential for fabricating next-generation Cu-based catalysts via ALD.展开更多
基金All thanks go to the contributions from all students,postdoctoral fellows,and visiting scholars.Special thanks are extended to the contributions from Prof.Jong Wook Bae(Sungkyunkwan University),Prof.Ruiqin Yang(Zhejiang University of Science and Technology),Prof.Yisheng Tan(Institute of Coal Chemistry,Chinese Academy of Sciences),Prof.Minbo Wu(China University of Petroleum),Prof.Xingang Li(Tianjin University),et al.Jie Yao appreciates the Grant-in-Aid for JSPS Fellows(JSPS KAKENHI 22J11458 and 22KJ1456).
文摘This review provides a comprehensive overview of the distinguished academic career and scientific accomplishments of Prof.Noritatsu Tsubaki at the University of Toyama.For over 35 years,he has dedicated himself to the research field of one-carbon(C1)chemistry,including catalytic conversion of C1 molecules to valuable chemicals and superclean fuels,innovative catalyst and reactor development,and the design of new catalytic reactions and processes.Organized chronologically,this review highlights Prof.Tsubaki’s academic contributions from 1990,when he studied and worked at The University of Tokyo,to his current role as a full professor at the University of Toyama.The academic section of this review is divided into three main parts,focusing on Prof.Tsubaki’s pioneering work in C1 chemistry.We believe that this review will serve as a highly valuable reference for colleagues in the fields of C1 chemistry and catalysis,and inspire the development of more original and groundbreaking research.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)the National Natural Science Foundation of China(22172032 and U22A20431).
文摘Methanol synthesis via CO_(2)conversion is a“green carbon”route for mitigating the greenhouse effect and recycling carbon resources.However,despite the widespread use of copper-based systems for methanol synthesis in recent decades,the chemical state of the active Cu species remains controversial.In this study,various Cu/ZnO/SBA-15 catalysts possessing different interfacial structures were engineered by atomic layer deposition(ALD).The optimized Cu/50c-ZnO/SBA-15 afforded the highest mass-specific methanol formation rate of 211.7 gMeOH·kgcat^(-1)·h^(-1)under the conditions of 250℃ and 3.0 MPa.In-depth characterizations indicated that the electronic state of Cu could be modulated by engineering the interfacial structures of the Cu/ZnO series catalysts,and the Cu cation sites(Cu^(δ+)and Cu^(+))are the active centers for methanol synthesis reaction rather than the Cu^(0)sites.Mechanistic analysis demonstrated that HCO_(3)^(*)and CO_(3)^(*)were slowly transformed to HCOO*and further hydrogenated to methanol following the formate-methoxy intermediate route.This work provides an improved understanding of the origin of the methanol synthesis active centers and emphasizes the potential for fabricating next-generation Cu-based catalysts via ALD.
