Reactivity oscillation in the heavy-light-heavy Cl + CH4 reaction

Chen, Zhen1,2; Chen, Jun1,3; Chen, Rongjun1; Xie, Ting4; Wang, Xingan4; Liu, Shu1; Wu, Guorong1; Dai, Dongxu1; Yang, Xueming1,5; Zhang, Dong H.1

2020-04-28

10.1073/pnas.1917618117

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA   影响因子和分区

0027-8424

It has long been predicted that oscillatory behavior exists in reactivity as a function of collision energy for heavy-light-heavy (HLH) chemical reactions in which a light atom is transferred between two heavy atoms or groups of atoms, but direct observation of such a behavior in bimolecular reactions remains a challenge. Here we report a joint theoretical and crossed-molecular-beam study on the Cl + CH4 -> HCl + CH3 reaction. A distinctive peak at a collision energy of 0.15 eV for the CH3(v = 0) product was experimentally detected in the backward scattering direction. Detailed quantum-dynamics calculations on a highly accurate potential energy surface revealed that this feature originates from the reactivity oscillation in this HLH polyatomic reaction. We anticipate that such reactivity oscillations exist in many HLH reactions involving polyatomic reagents.

heavy-light-heavy quantum differential cross-sections reactivity oscillations polyatomic reaction

SCI

英语

NI论文

通讯

National Natural Science Foundation of China[21773235][21590804][21688102][21433009][21673234] ; Chinese Academy of Sciences[XDB17010200] ; International Partnership Program of Chinese Academy of Sciences[121421KYSB20170012] ; Dalian Institute of Chemical Physics[DICP ZZBS201611]

Science & Technology - Other Topics

Multidisciplinary Sciences

WOS:000530099500018

NATL ACAD SCIENCES

BIOLOGY & BIOCHEMISTRY;CLINICAL MEDICINE;MULTIDISCIPLINARY;PLANT & ANIMAL SCIENCE;ENVIRONMENT/ECOLOGY;SOCIAL SCIENCES, GENERAL;MICROBIOLOGY;ECONOMICS BUSINESS;IMMUNOLOGY;MATERIALS SCIENCE;MATHEMATICS;SPACE SCIENCE;MOLECULAR BIOLOGY & GENETICS;PHARMACOLOGY & TOXICOLOGY;CHEMISTRY;PSYCHIATRY/PSYCHOLOGY;NEUROSCIENCE & BEHAVIOR;PHYSICS;GEOSCIENCES;AGRICULTURAL SCIENCES;ENGINEERING

Web of Science

1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Xiamen Univ, Coll Chem & Chem Engn, Xiamen 361005, Fujian, Peoples R China
4.Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China
5.Southern Univ Sci & Technol, Sch Sci, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China

Chen, Zhen,Chen, Jun,Chen, Rongjun,et al. Reactivity oscillation in the heavy-light-heavy Cl + CH4 reaction[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2020,117(17):9202-9207.

Chen, Zhen.,Chen, Jun.,Chen, Rongjun.,Xie, Ting.,Wang, Xingan.,...&Zhang, Dong H..(2020).Reactivity oscillation in the heavy-light-heavy Cl + CH4 reaction.PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,117(17),9202-9207.

Chen, Zhen,et al."Reactivity oscillation in the heavy-light-heavy Cl + CH4 reaction".PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 117.17(2020):9202-9207.