Mechanochemistry: targeted delivery of single molecules

Duwez, Anne‐Sophie; Cuenot, Stéphane; Jérôme, Christine; Gabriel, Sabine; Jérôme, Robert; Rapino, Stefania; Zerbetto, Francesco

doi:10.1038/nnano.2006.92

Cited by 102 publications

(81 citation statements)

References 30 publications

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“…However, as Duwez and coworkers showed, the electrografting of NHSA from an AFM tip could be used to deliver and immobilize individual molecules on a surface. 91,92 In this remarkable study, they electrografted the polymeric activated ester PNHSA from a gold coated AFM tip, which was then brought in contact with an amino functionalized surface. The formation of a covalent amide bond linked the polymer chain to the surface.…”

Section: Electrochemical Polymerizationmentioning

confidence: 99%

Synthesis of well‐defined polymeric activated esters

Théato

2008

J. Polym. Sci. A Polym. Chem.

277

260

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Monomers bearing an activated ester group can be polymerized under various controlled polymerization techniques, such as ATRP, NMP, RAFT polymerization, or ROMP. Combining the functionalization of polymers via polymeric activated esters with these controlled polymerization techniques generate possibilities to realize highly functionalized polymer architectures. Within this highlight two different research areas of activated esters in polymer science will be discussed: (i) the preparation of defined reactive polymer architectures by controlled polymerization techniques and (ii) the preparation of defined reactive thin films. © 2008 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 46: 6677–6687, 2008

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Section: Electrochemical Polymerizationmentioning

confidence: 99%

Synthesis of well‐defined polymeric activated esters

Théato

2008

J. Polym. Sci. A Polym. Chem.

277

260

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“…Macroscale mechanochemical processes such as ball milling and ultrasonic cavitation are often used to drive such reactions 3,4 ; however, in situ characterization is difficult and the delivery of precise stresses is not possible. Pulling on individual molecules with atomic force microscope (AFM) 5 tips can rupture bonds with pN resolution, but the technique is limited to molecules long enough to detect rupture and systems where the bonds between tip and sample are stronger than the bond under investigation [6][7][8][9] . There is a need for an experimental system capable of measuring mechanochemical bond scission that can be applied universally to a wide variety of material systems and that produces quantitative information about the chemical reaction occurring.…”

mentioning

confidence: 99%

Direct mechanochemical cleavage of functional groups from graphene

et al. 2015

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Mechanical stress can drive chemical reactions and is unique in that the reaction product can depend on both the magnitude and the direction of the applied force. Indeed, this directionality can drive chemical reactions impossible through conventional means. However, unlike heat-or pressure-driven reactions, mechanical stress is rarely applied isometrically, obscuring how mechanical inputs relate to the force applied to the bond. Here we report an atomic force microscope technique that can measure mechanically induced bond scission on graphene in real time with sensitivity to atomic-scale interactions. Quantitative measurements of the stress-driven reaction dynamics show that the reaction rate depends both on the bond being broken and on the tip material. Oxygen cleaves from graphene more readily than fluorine, which in turn cleaves more readily than hydrogen. The technique may be extended to study the mechanochemistry of any arbitrary combination of tip material, chemical group and substrate.

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“…In the sub-field of diamondoid mechanosynthesis (DMS), 1 2 initial experimental feasibility studies have begun but are difficult due to the current inability to positionally control and deposit carbon (C) atoms or reactive organic fragments, although prior experimental studies demonstrate the feasibility of mechanical bond manipulation [3][4][5] and the first US patent on DMS was issued in 2010. 6 The positional-control feature of DMS defines its many differences from (and possible advantages over) traditional chemosynthetic approaches for the fabrication of complex nanostructures.…”

Section: Introductionmentioning

confidence: 99%

Analysis of Diamondoid Mechanosynthesis Tooltip Pathologies Generated via a Distributed Computing Approach

Allis¹,

Helfrich²,

Freitas³

et al. 2011

Jnl of Comp & Theo Nano

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The results of a combined molecular dynamics/quantum chemistry pathology study of previously reported organic (diamondoid) tooltips for diamondoid mechanosynthesis (DMS) are presented. This study, employing the NanoHive@Home (NH@H) distributed computing project, produced 80,000 tooltip geometries used in 200,000 calculations optimized at either the RHF/3-21G or RHF/STO-3G levels of theory based on geometries obtained from high-energy molecular dynamics simulations to produce highly deformed starting geometries. These 200,000 calculations have been catalogued, grouped according to energies and geometries, and analyzed to consider potentially accessible defect structures (pathologies) for tooltip geometries either binding a carbon dimer (C 2 feedstock or not containing the transported dimer feedstock. The transport and deposition of feedstock and the stability of the tooltip between dimer "loading" cycles are important geometries that must be considered as part of a tooltip stability analysis. The NH@H framework is found to be a useful method both for the study of highly deforming covalent geometries and, using lower-temperature MD simulations, for generating and optimizing molecular conformations (demonstrated using biotin, n-heptane, and n-octane in this study). The results of the pathology survey are discussed and general considerations for the exploration of DMS tooltip usability are explored.

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Mechanochemistry: targeted delivery of single molecules

Cited by 102 publications

References 30 publications

Synthesis of well‐defined polymeric activated esters

Synthesis of well‐defined polymeric activated esters

Direct mechanochemical cleavage of functional groups from graphene

Analysis of Diamondoid Mechanosynthesis Tooltip Pathologies Generated via a Distributed Computing Approach

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