Sterically controlled mechanochemistry under hydrostatic pressure

Nature
Hao YanNicholas A Melosh

Abstract

Mechanical stimuli can modify the energy landscape of chemical reactions and enable reaction pathways, offering a synthetic strategy that complements conventional chemistry. These mechanochemical mechanisms have been studied extensively in one-dimensional polymers under tensile stress using ring-opening and reorganization, polymer unzipping and disulfide reduction as model reactions. In these systems, the pulling force stretches chemical bonds, initiating the reaction. Additionally, it has been shown that forces orthogonal to the chemical bonds can alter the rate of bond dissociation. However, these bond activation mechanisms have not been possible under isotropic, compressive stress (that is, hydrostatic pressure). Here we show that mechanochemistry through isotropic compression is possible by molecularly engineering structures that can translate macroscopic isotropic stress into molecular-level anisotropic strain. We engineer molecules with mechanically heterogeneous components-a compressible ('soft') mechanophore and incompressible ('hard') ligands. In these 'molecular anvils', isotropic stress leads to relative motions of the rigid ligands, anisotropically deforming the compressible mechanophore and activating bonds. Conver...Continue Reading

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Citations

Oct 20, 2018·Angewandte Chemie·Joseph L HowardDuncan L Browne
Nov 13, 2018·Angewandte Chemie·Carsten Bolm, José G Hernández
Dec 21, 2019·Science·Hesheng Xia, Zhenhua Wang
Feb 23, 2018·Nature·Stuart L James
Jun 10, 2020·Angewandte Chemie·Christian SchumacherCarsten Bolm
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Feb 1, 2018·Nature·Stuart L James
Nov 25, 2020·Nature Communications·Fangrui ZhengZuowei Xie
Mar 6, 2021·Physical Review Letters·Zhuohan Li, Izabela Szlufarska
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Aug 12, 2021·Chemical Communications : Chem Comm·Feng KeManzhou Zhu
Oct 30, 2018·Langmuir : the ACS Journal of Surfaces and Colloids·Derek C PoppleJ Nathan Hohman
Dec 1, 2020·Journal of the American Chemical Society·Anna Kataki-AnastasakouEllen M Sletten
Sep 29, 2018·Journal of the American Chemical Society·Brittany TrangJ Nathan Hohman
May 12, 2018·Journal of the American Chemical Society·Takuya YamakadoShohei Saito

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