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Polymer Mechanochemistry pp 37–96Cite as

Theoretical Approaches for Understanding the Interplay Between Stress and Chemical Reactivity

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Part of the book series: Topics in Current Chemistry ((TOPCURRCHEM,volume 369))

Abstract

The use of mechanical stresses to induce chemical reactions has attracted significant interest in recent years. Computational modeling can play a significant role in developing a comprehensive understanding of the interplay between stresses and chemical reactivity. In this review, we discuss techniques for simulating chemical reactions occurring under mechanochemical conditions. The methods described are broadly divided into techniques that are appropriate for studying molecular mechanochemistry and those suited to modeling bulk mechanochemistry. In both cases, several different approaches are described and compared. Methods for examining molecular mechanochemistry are based on exploring the force-modified potential energy surface on which a molecule subjected to an external force moves. Meanwhile, it is suggested that condensed phase simulation methods typically used to study tribochemical reactions, i.e., those occurring in sliding contacts, can be adapted to study bulk mechanochemistry.

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Abbreviations

AFM:

Atomic force microscopy

AP:

Attachment point

CASMP2:

Complete active space Møller–Plesset 2nd order perturbation theory

CASSCF:

Complete active space self-consistent field

CPMD:

Car–Parrinello molecular dynamics

DFT:

Density functional theory

EFEI:

External force is explicitly included

FF:

Force field

FMPES:

Force-modified potential energy surface

GSSNEB:

Generalized solid-state nudged elastic band

IRC:

Intrinsic reaction coordinate

MD:

Molecular dynamics

MEP:

Minimum energy path

NEB:

Nudged elastic band

PES:

Potential energy surface

PP:

Pulling point

QC:

Quantum chemical

QM/MM:

Quantum mechanics/molecular mechanics

RI:

Registry index

SMD:

Steered molecular dynamics

TS:

Transition state

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Acknowledgements

Financial support from the Natural Sciences and Engineering Research Council of Canada’s Discovery Grant Program is acknowledged. GSK is grateful for support from the Ontario Graduate Scholarship program.

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  1. Department of Chemistry, Queen’s University, 90 Bader Lane, Kingston, ON, Canada, K7L 3N6

    Gurpaul S. Kochhar, Gavin S. Heverly-Coulson & Nicholas J. Mosey

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    Roman Boulatov

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Kochhar, G.S., Heverly-Coulson, G.S., Mosey, N.J. (2015). Theoretical Approaches for Understanding the Interplay Between Stress and Chemical Reactivity. In: Boulatov, R. (eds) Polymer Mechanochemistry. Topics in Current Chemistry, vol 369. Springer, Cham. https://doi.org/10.1007/128_2015_648

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