Mode Specificity Dynamics of Prototypical Multi-Channel H+CH3OH Reaction on Globally Accurate Potential Energy Surface

被引：2

作者：

Lu, Dandan

Li, Jun ^{[1
]}

机构：

[1] Chongqing Univ, Sch Chem & Chem Engn, Chongqing 401331, Peoples R China

来源：

CHINESE JOURNAL OF CHEMICAL PHYSICS | 2022年 / 35卷 / 03期

基金：

中国国家自然科学基金;

关键词：

Mode specific dynamics; Quasi-classical trajectory; Branching ratio; Reaction kinetics; AB-INITIO; HYDROGEN ABSTRACTION; VIBRATIONAL EXCITATIONS; RATE CONSTANTS; H-ATOMS; METHANOL; CH3OH; SCATTERING; MECHANISM; CHANNEL;

D O I：

10.1063/1674-0068/cjcp2201018

中图分类号：

O64 [物理化学（理论化学）、化学物理学]; O56 [分子物理学、原子物理学];

学科分类号：

070203 ; 070304 ; 081704 ; 1406 ;

摘要：

The H+CH3OH reaction, which plays an important role in combustion and the interstellar medium, presents a prototypical system with multiple channels. In this work, mode specific dynamics of different product channels is investigated theoretically on a recently developed reliable potential energy surface based on a large number of data points calculated at the level of UCCSD(T)-F12a/AVTZ. It has been demonstrated that vibrational excitations of the O-H stretching motion, the torsional motion, the C-H stretching vibrations, show different influences on the four product channels, H-2+CH3O, H-2+CH2OH, H2O+CH3, and H+CH3OH. This work is helpful for understanding the mode-specific dynamics and controlling the competition for complicated reactions with multiple product channels.

引用

收藏

页码：481 / 487

页数：7

相关论文

共 52 条

[1] REACTION OF HYDROGEN ATOMS WITH METHANOL [J].

ADERS, WK ;

WAGNER, HG .

ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-FRANKFURT, 1971, 74 (3-6) :224-&

[2] Four Generations of High-Dimensional Neural Network Potentials [J].

Behler, Joerg .

CHEMICAL REVIEWS, 2021, 121 (16) :10037-10072

[3] Ab initio calculations of the reactions of hydrogen with methanol: A comparison of the role of bond distortions and Pauli repulsions on the intrinsic barriers for chemical reactions [J].

Blowers, P ;

Ford, L ;

Masel, R .

JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (46) :9267-9277

[4] Theoretical calculations of energetics, structures, and rate constants for the H+CH3OHhydrogen abstraction reactions [J].

Carvalho, E. F. V. ;

Barauna, Alessandra N. ;

Machado, Francisco B. C. ;

Roberto-Neto, Orlando .

CHEMICAL PHYSICS LETTERS, 2008, 463 (1-3) :33-37

[5] DFT study for the reactions of H atoms with CH3OH and C2H5OH [J].

Carvalho, Edson F. V. ;

Barauna, Alessandra N. ;

Machado, Francisco B. C. ;

Roberto-Neto, Orlando .

INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 2008, 108 (13) :2476-2485

[6] Direct dynamics for free radical kinetics in solution: Solvent effect on the rate constant for the reaction of methanol with atomic hydrogen [J].

Chuang, YY ;

Radhakrishnan, ML ;

Fast, PL ;

Cramer, CJ ;

Truhlar, DG .

JOURNAL OF PHYSICAL CHEMISTRY A, 1999, 103 (25) :4893-4909

[7] Low-Temperature Kinetic Isotope Effects in CH3OH + H → CH2OH + H2 Shed Light on the Deuteration of Methanol in Space [J].

Cooper, April M. ;

Kastner, Johannes .

JOURNAL OF PHYSICAL CHEMISTRY A, 2019, 123 (42) :9061-9068

[8] State-to-state dynamics of the Cl(2P)+C2H6(5,1=0,1)HCl(v, j)+C2H5 hydrogen abstraction reactions [J].

Corchado, Jose C. ;

Chamorro, Moises G. ;

Rangel, Cipriano ;

Espinosa-Garcia, Joaquin .

THEORETICAL CHEMISTRY ACCOUNTS, 2019, 138 (02)

[9] Chemical dynamics of vibrationally excited molecules: Controlling reactions in gases and on surfaces [J].

Crim, F. Fleming .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (35) :12654-12661

[10] Dynamics of the Reaction of Methane with Chlorine Atom on an Accurate Potential Energy Surface [J].

Czako, Gabor ;

Bowman, Joel M. .

SCIENCE, 2011, 334 (6054) :343-346

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