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Photoelectron Imaging Spectroscopy of ZrO-Diatomic Anion

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Chinese Journal of Chemical Physics 2015年第4期28卷 -页

作者： Qing-yu Liu Lian-rui Hu Hui Chen sheng-gui he Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190China Beijing National Laboratory for Molecular Sciences Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

The diatomic ZrO? anion has been prepared by laser ablation and studied by photoelectron imaging spectroscopy combined with quantum chemistry calculations. The observed photoelectron spectra can be well assigned on the basis of reported optical spectroscopy and high-level ab initio calculations. The ground state of ZrO? is a 2Δ state with spin-orbit splitting of 578±12 cm?1. The electron affinity of ZrO is 1.249±0.005 eV. For the first time, the c3∑? state of ZrO has been experimentally observed at 13316±24 cm?1 with respect to the X1∑+ground state. A comparison between ZrO and the isoelectronic molecule NbN has been made.

关键词： Diatomic molecules Electronic structure Spin-orbit splitting Photoelectron imaging spectroscopy ab initio calculations

Experimental and Theoretical Study of Reactions between Manganese Oxide Cluster Cations and Hydrogen Sulfide

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Chinese Journal of Chemical Physics 2013年第6期26卷 679-686,I0003,I0004页

作者： Mei-ye Jia sheng-gui he Mao-fa Ge Beijing National Laboratory for Molecular Sciences (BNLMS) State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China University of Chinese Academy of Sciences Beijing 100049 China

Manganese oxide cluster cations Mnm180n＋ were prepared by laser ablation and reacted with hydrogen sulfide （H2S） in a fast flow reactor under thermal collision conditions. A time-of-flight mass spectrometer was used to detect the cluster distributions before and after the interactions with H2S. The experiments suggest that oxygen-for-sulfur （O/S） ex- change reaction to release water took place in the reactor for most of the manganese oxide cluster cations： MnmlSOn＋＋H2S→Mnm18On-1S＋＋H218O. Density functional theory cal- culations were performed for reaction mechanisms of Mn202＋＋H2S, Mn203＋＋H2S, and Mn204＋＋H2S. The computational results indicate these O/S exchange reactions are both thermodynamically and kinetically favorable, thus in good agreement with the experimental observations. The O/S exchange reactions identified in this gas-phase cluster study parallel similar behavior of related condensed phase reaction systems.

关键词： Cluster Oxygen-for-sulfur exchange Reaction mechanism Mass spectrometry Density functional theory

Metal-mediated catalysis in the gas phase: A review

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Chinese Journal of Catalysis 2017年第9期38卷 1515-1527页

作者： Xiao‐Na Li Xiu‐Ping Zou sheng‐gui he Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China School of Chemistry and Chemical Engineering South China University of Technology Guangzhou 510641 Guangdong China

This review summarizes a variety of experimentally identified gas‐phase catalytic cycles,all of which are mediated by atomic metal ions,bare metal clusters,metal oxide clusters or metal *** is placed on the latest advances in the unique catalytic reactivity of cluster‐confined single noble metal *** cycles discussed in this paper cover a wide range of inorganic and organic *** use of start‐of‐the‐art mass spectrometric instrumentation in conjunction with quantum chemistry calculations is also reported,as these techniques have determined the mechanistic details of the elementary steps of such catalytic *** important role of gas‐phase data in guiding the rational design of better‐performing catalysts in related condensed phase reactions is also *** particular,this review focuses on the following three topics:(1)the catalytic oxidation of carbon monoxide,(2)the catalytic functionalization of methane,and(3)catalytic decarboxylation.

关键词： Metal catalysis Clusters Single atom catalysts Carbon monoxide Methane

Activation of Dinitrogen by Gas-Phase Species

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Chinese Journal of Chemical Physics 2020年第5期33卷 507-520,I0078页

作者： Li-hui Mou gui-duo Jiang Zi-yu Li sheng-gui he State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular Sciences Beijing 100190China

Reactions of gas-phase species with small molecules are being actively studied to understand the elementary steps and mechanistic details of related condensed-phase *** of the very inert N≡N triple bond of dinitrogen molecule by isolated gas-phase species has attracted considerable interest in the past few *** from molecular adsorption and dissociative adsorption,interesting processes such as C-N coupling and degenerate ligand exchange were *** present review focuses on the recent progress on adsorption,activation,and functionalization of N2 by gas-phase species(particularly metal cluster ions)using mass spectrometry,infrared photo-dissociation spectroscopy,anion photoelectron spectroscopy,and quantum chemical calculations including density functional theory and high-level ab initio *** advances including characterization of adsorption products,dependence of clusters’reactivity on their sizes and structures,and mechanisms of N≡N weakening and splitting have been emphasized and prospects have been discussed.

关键词： Dinitrogen activation Atomic cluster Reaction mechanisms

Coupling of Methane and Carbon Dioxide by Gas-Phase Ions

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Coupling of Methane and Carbon Dioxide by Gas-Phase Ions

Reactivity of Atomic Oxygen Radical Anions over Metal Oxide Nano-Particles in the Gas Phase: C-H Bond Activation and CO Oxidation

第十六届全国化学动力学会议

作者： sheng-gui he Institute of Chemistry Chinese Academy of Sciences

Methane (CH) and Carbon dioxide (CO) are two abundantly available carbon-based *** of CHwith CO to form value-added products such as HCHO,CHOH,and C compounds are very important research ***,both CH and CO molecules are thermodynamically very stable and kinetically *** is difficult to activate either of the *** using mass spectrometry based techniques and state-of-the-art quantum chemistry calculations,the reactions of gas-phase ions with CH and CO have been extensively studied to understand the mechanisms of CH activation[1]and CO activation[2]separately,while the ions to mediate the coupling reaction have been rarely identified[3].This talk will discuss a few oxide and boride species (see one example in Fig.1) that have been very recently characterized to be able to mediate the coupling of CH and CO in the gas phase.

关键词： ion-molecule reactions C-C coupling mass spectrometry quantum chemistry calculations boride species

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Reactivity of Atomic Oxygen Radical Anions over Metal Oxide ...

Recent research progress in the study of catalytic CO oxidation by gas phase atomic clusters

第十三届全国化学动力学会议

作者： sheng-gui he Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences

＜正＞Atomic oxygen radical anions （O-） are important reactive intermediates involved in oxidation reactions over widely used transition metal oxide catalysts.1,2 Due to short life-times and low concentrations, the ... 详细信息

关键词： Oxygen-centred radical Atomic cluster Nano size Mass spectrometry Density functional theory

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Science China Materials 2020年第6期63卷 892-902页

作者： Li-Na Wang Xiao-Na Li sheng-gui he State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular Sciences Beijing 100190China

Oxidation of CO into CO2 is a major solution to reduce CO emission into the atmosphere and to remove CO in fuel gas ***,CO oxidation serves as a prototypical reaction for heterogeneous *** review provides an overview and an update on how to study catalytic CO oxidation at a strictly molecular level by performing wellcontrolled gas-phase experiments in combination with quantum chemistry *** advances in the unique catalytic reactivity of single-atom cluster catalysts are *** catalytically active sites and various mechanistic aspects in the redox couples N2O/CO and O2/CO for the seemingly simple oxidation reaction are described.

关键词： CO oxidation single-atom catalysts atomic clusters mass spectrometry density functional theory calculations

Experimental and Theoretical Study of Hydrogen Atom Abstraction from Ethylene by Stoichiometric Zirconium Oxide Clusters

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Chinese Journal of Chemical Physics 2009年第6期22卷 635-641,J0002页

作者： Xiao-nan Wu Yan-xia Zhao sheng-gui he Xun-lei Ding Beijing National Laboratory for Molecular Sciences State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China Graduate University of the Chinese Academy of Sciences Beijing 200049 China

The reactions of cationic zirconium oxide clusters （ZrxOy^＋） with ethylene （C2H4） were investigated by using a time-of-flight mass spectrometer coupled with a laser ablation/supersonic expansion cluster source. Some hydrogen containing products （ZrO2）xH^＋（x=-1-4） were observed after the reaction. The density functional theory calculations indicate that apart from the common oxygen transfer reaction channel, the hydrogen abstraction channel can also occur in （ZrO2）x^＋＋C2H4, which supports that the observed （ZrO2）xH^＋ may be due to （ZrO2）x^＋＋C2H4→（ZrO2）xH^＋＋C2H3. The rate constants of different reaction channels were also calculated by Rice-Rarnsberger-Kassel-Marcus theory.

关键词： Time-of-flight mass spectrometer Zirconium oxide clusters Fast flow reactor Density functional theory Rice-Ramsberger-Kassel-Marcus theory

^(15)N/^(14)N Isotopic Exchange in the Dissociative Adsorption of N_(2) on Tantalum Nitride Cluster Anions Ta_(3)N_(3)

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Chinese Journal of Chemical Physics 2022年第1期35卷 77-85,I0062,I0063页

作者： Zi-Yu Li Li-Hui Mou gui-Duo Jiang Qing-Yu Liu sheng-gui he State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular Sciences Beijing 100190China

Adsorption and activation of dinitrogen(N_(2)) is an indispensable process in nitrogen *** nitride species continue to attract attention as a promsing catalyst for ammonia ***,the detailed mechanisms at a molecular level between reactive nitride species and N_(2) remain unclear at elevated temperature,which is important to understand the temperature effect and narrow the gap between the gas phase system and condensed phase ***,the ^(15)N/^(14)N isotopic exchange in the reaction between tantalum nitride cluster anions Ta_(3)^(14)N_(3)^(-) and ^(15)N_(2) leading to the regeneration of ^(14)N_(2)/^(14)N^(15)N was observed at elevated temperature(393-593 K)using mass *** the aid of theoretical calculations,the exchange mechanism and the effect of temperature to promote the dissociation of N_(2) on Ta_(3)N_(3)^(-) were elucidated.A comparison experiment for Ta_(3)^(14)N_(4)^(-)/^(15)N_(2) couple indicated that only desorption of ^(15)N_(2) from Ta_(3)^(14)N_(4)^(15)N_(2)^(-) took place at elevated *** different exchange behavior can be well understood by the fact that nitrogen vacancy is a requisite for the dinitrogen activation over metal nitride *** study may shed light on understanding the role of nitrogen vacancy in nitride species for ammonia synthesis and provide clues in designing effective catalysts for nitrogen fixation.

关键词： Temperature effect Dinitrogen activation Transition metal nitrides Nitrogen vacancy Isotopic exchange