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Photocatalytic nonoxidative coupling of methane to ethylene over carbon-doped ZnO/Au catalysts

Science china chemistry 2023年第11期66卷 3252-3261页

作者： Jing Wang Yuhao Peng Wei Xiao college of chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072China

A photocatalytic nonoxidative coupling of methane to multi-carbon compounds remains a huge challenge due to its high dissociation energy of c–h bonds and sluggish charge carrier dynamics.Au-modified carbon-doped ZnO(c-ZnO/Au)photocatalyst is constructed by an interfacial modification-assisted self-assembly approach for efficient photocatalytic nonoxidative coupling of methane to ethylene and hydrogen(2ch_4=c_2h_4+2h_2).Benefitting from the presence of c-ZnO/Au interfaces,the catalyst not only weakens the excitonic confinement to improve the photogenerated charge carrier separation,but also enhances the stability of lattice oxygen to suppress c_2h_4 overoxidation.Moreover,this hybrid catalyst also accelerates the generation of Zn~+–O~–pairs to activate c–h bonds,stabilizes the important reaction intermediate(*Och_3)to achieve the c–c coupling,and promotes the generation of low-valence Zn to accelerate the dehydrogenation of the*Oc_2h_5 into c_2h_4.Therefore,a stable photocatalytic methane conversion performance can be achieved over c-ZnO/Au heterojunctions with a stoichiometric generation of the oxidation product(c_2h_4,45.85μmol g~(-1)h~(-1))and reduction product(h_2,88.07μmol g~(-1)h~(-1)).This work provides deep insights into the elemental doping and oxide/Au interfaces for the enhanced photocatalytic activity and product selectivity under mild conditions in the absence of extra oxidants.

关键词： carbon-doped ZnO charge separation c–h bond activation photocatalytic nonoxidative coupling of methane

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Theoretical investigation toward the organophosphine-catalyzed [3+3]annulation reaction of carbonates with azomethine imines: mechanism,stereoselectivity, and role of catalyst

Theoretical investigation toward the organophosphine-catalyz...

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河南省化学会2016年学术年会

作者： Yang Wang Xue Li Donghui Wei Mingsheng Tang The college of chemistry and Molecular Engineering Center of Computational Chemistry Zhengzhou University

The detailed mechanisms and stereoselectivity of the chiral phosphine-catalyzed c(sp)-h activation/[3+3] cycloaddition cascade reaction between Morita-Baylis-hillman(MBh) carbonates and c,N-cyclic azomethine imines have been investigated. The calculated results indicate the c(sp)-h activation is rate-determining, and the stereoselectivity is controlled by the [3 + 3] cycloaddition step.The special roles of the Lewis base organocatalyst(i.e. activation of c(sp)-h and c-O bonds and"umpolung") were also identified by NBO charge and GRI analyses. The mechanistic insights obtained in the present study should be useful for understanding the novel organocatalytic c(sp)-h activation,and thus provide valuable clues on rational design of efficient organocatalysts for the c(sp)-h activation/cycloaddition reactions.

关键词： c–h bond activation [3 + 3] cycloaddition organophosphine DFT

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construction of Organic Optoelectronic Molecules Based on highly Efficient and Selective c–h bond Transformations

Construction of Organic Optoelectronic Molecules Based on Hi...

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中国化学会第十三届全国有机合成化学学术研讨会

作者： Jingsong You Key Laboratory of Green chemistry and Technology of Ministry of Education College of ChemistrySichuan University

The design and synthesis of π-conjugated organic molecules are one of the most important research contents of organic chemistry and are also a source of innovation for molecular materials and devices.The development of straightforward accesses to organic functional materials through c–h activation is a revolutionary trend in organic synthesis.Our research aims to offer the chemical basis for the construction of organic photoelectric molecules through the development of highly efficient and selective transformations of c–h bonds.In recent years,we have successfully developed a number of synthetically challenging π-conjugated structures,especially the frameworks that are difficult to access by common synthetic disconnections without c–h activation tactics.Furthermore,we have also explored their applications in organic photoelectric materials such as organic photovoltaic,electroluminescence,field effect transistor,biosensing and piezochromism.The highly efficient routes to diverse organic photoelectric molecules have exemplified the great charm of c–h activation and would finally boost the development of the organic optoelectronic materials.

关键词： c–h bond activation conjugated Frameworks Organic Optoelectronic Molecules

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