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Methane activation by[LnO]^(+):the 4f orbital matters

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Science China Chemistry 2024年第1期67卷 330-335页

作者： Bowei Yuan Jingxiang Zou Mincheng Yu Shaodong Zhou College of Chemical and Biological Engineering Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture TechnologyZhejiang UniversityHangzhou 310027China Zhejiang Provincial Innovation Center of Advanced Chemicals Technology Institute of Zhejiang University–QuzhouQuzhou 324000China Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China

Gas-phase reactions of[LnO]^(+)with methane have been studied by using inductively coupled plasma-mass spectrometer(ICP-MS)combined with quantum chemical *** indicate that the[LnO]^(+)(Ln=Sm-Lu)ions are able to activate methane to generate methyl *** particular,[EuO]^(+)and[YbO]^(+)exhibit the highest ***,ab initio computations reveal a novel HAT process operating in the absence of a terminal oxygen radical,as mediated by[EuO]^(+)and[YbO]^(+).Such a process diverges from previous findings on the methane activation by metal oxide clusters,not only on the electronic pattern during the course of hydrogen transfer,but also on the important role that 4f electrons *** associated electronic origins have been discussed,and the well-designed 4f electron occupation may turn to be a promising approach in constructing lanthanide involved catalysts.

关键词： lanthanide oxides methane activation 4f orbitals quantum chemical calculation ion-molecule reaction

Investigation of the Structures of the Product ions Produced via self-CI of Acetone

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Chinese Chemical Letters 1998年第7期9卷 675-678页

作者： Zhi Li LI Shu Ying LIU(Changchun Institute of Applied Chendstry, Chinese Academy of Sciences,Changchun 130022) Chinese Acad Sci Changchun Inst Appl Chem Changchun 130022 Peoples R China

The ion-molecule reactions in acetone were investigated which were induced under the chemical ionization. The structural information of the reaction products were obtained by using collision-induced dissociation (CID)... 详细信息

关键词： ion-molecule reaction acetone ion structure collision-induced dissociation

ion-Velocity Imaging Study of Dissociative Charge Exchange reactions between Ar^(+)and trans-/cis-Dichloroethylene

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Chinese Journal of Chemical Physics 2023年第5期36卷 509-516,I0001页

作者： Zi-Xin Chen Jie Hu Yaya Zhi Chun-Xiao Wu Shan Xi Tian Hefei National Research Center for Physical Sciences at the Microscale Department of Chemical PhysicsUniversity of Science and Technology of ChinaHefei 230026China

Dissociative charge exchange re-actions between Ar^(+)ion and trans-/cis-dichloroethylene(trans-/cis-C_(2)H_(2)Cl_(2))are investi-gated with the ion-velocity imag-ing *** dechlorinated product C_(2)H_(2)Cl^(+)is the predomi-nant,and most of this product show the spatial distribution around the target,implying that the dissociation occurs in the large impact-parameter collision and via the energy resonant charge ***,a few C_(2)H_(2)Cl^(+)locate around the center-of-mass,which is at-tributed to the fragmentation of intimate association between C_(2)H_(2)Cl_(2)and Ar^(+)or in the small impact-parameter *** product C_(2)HCl_(+)exhibits the velocity distribution fea-tures similar to those of C_(2)H_(2)Cl_(+).The rarest product C_(2)HCl_(2)+shows the distributions around the molecular target,due to the quick dehydrogenation after the energy-resonant charge transfer in the large impact-parameter collision.

关键词： ion-molecule reaction Dissociative charge exchange Velocity map imaging