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Polymer mechanochemistry: from single molecule to bulk material

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

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Article Chemistry, Multidisciplinary

Mechanically gated formation of donor-acceptor Stenhouse adducts enabling mechanochemical multicolour soft lithography

Anna C. Overholts et al.

Summary: Mechanophores are stress-sensitive molecules that undergo productive chemical transformations under mechanical force. A new platform has been introduced to achieve mechanically gated multicolour chromogenic reactivity. This platform is based on an activated furan precursor, which, when mechanochemically activated, generates a diverse range of color variations. This system has been applied to create a complex multicolour composite image through localized compression and reaction with different secondary amines.

NATURE CHEMISTRY (2023)

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Article Chemistry, Multidisciplinary

Intrinsic Anti-Freezing and Unique Phosphorescence of Glassy Hydrogels with Ultrahigh Stiffness and Toughness at Low Temperatures

Li Xin Hou et al.

Summary: This study presents a glassy hydrogel with intrinsic anti-freezing capacity and excellent optical and mechanical properties at ultra-low temperatures. The hydrogel has a moderate water content and dense hydrogen-bond associations, and becomes stronger and stiffer, yet still ductile, as the temperature decreases. It retains high transparency even in liquid nitrogen and exhibits unique phosphorescence at subzero temperatures.

ADVANCED MATERIALS (2023)

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Article Multidisciplinary Sciences

Facile mechanochemical cycloreversion of polymer cross-linkers enhances tear resistance

Shu Wang et al.

SCIENCE (2023)

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Article Multidisciplinary Sciences

Mechanical nonreciprocity in a uniform composite material

Xiang Wang et al.

Summary: We report a uniform composite hydrogel that displays substantial mechanical nonreciprocity, owing to direction-dependent buckling of embedded nanofillers. This material exhibits an asymmetric deformation when subjected to local interactions, which can induce directional motion of various objects. This material could promote the development of nonreciprocal systems for practical applications such as energy conversion and biological manipulation.

SCIENCE (2023)

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Article Polymer Science

Origin of Surface Charge of Double Network Hydrogels Prepared by Sequential Polymerization

Martin Frauenlob et al.

Summary: Understanding the molecular origin of surface charges in double network hydrogels is crucial for their applications. This paper investigates the incorporation of unreacted monomers from the first network into the second network, which results in an increase in surface charge and affects the repulsive/adhesive properties. The authors propose a method to remove unreacted monomers and modulate the surface charge density of double network hydrogels.

ACS MACRO LETTERS (2023)

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Article Chemistry, Multidisciplinary

Azo-Crosslinked Double-Network Hydrogels Enabling Highly Efficient Mechanoradical Generation

Zhi Jian Wang et al.

Summary: Double-network hydrogels with increased mechanoradical concentration achieved by incorporating azoalkane crosslinker exhibit improved mechanical properties and functionality. This finding broadens the application range of force-responsive DN gels to biomedical devices and soft robots.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Ratiometric Flapping Force Probe That Works in Polymer Gels

Takuya Yamakado et al.

Summary: A new ratiometric force probe has been developed that functions in common organogels, showing excellent responsiveness and reversibility. It displays a dual-fluorescence response under compression, facilitating observation and quantification of stress concentration in polymer chains.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Physical

Tough and stretchable ionogels by in situ phase separation

Meixiang Wang et al.

Summary: Ultra-tough and stretchable ionogels can be achieved by randomly copolymerizing two monomers with distinct solubility in an ionic liquid. These ionogels have high fracture strength, fracture energy, and Young's modulus, while being highly stretchable and possessing self-healing and shape-memory properties.

NATURE MATERIALS (2022)

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Article Multidisciplinary Sciences

Bridging pico-to-nanonewtons with a ratiometric force probe for monitoring nanoscale polymer physics before damage

Ryota Kotani et al.

Summary: Understanding the transmission of nanoscale forces is crucial in polymer physics. Physical approaches have limitations in analyzing the local force distribution in condensed environments. This study presents a conformationally flexible dual-fluorescence force probe, enabling ratiometric analysis of the distribution of local forces in a stretched polymer chain network. Chemical control of the probe location reveals a higher local stress concentration at crosslinkers than at main chains, especially in a strain-hardening region.

NATURE COMMUNICATIONS (2022)

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Article Chemistry, Multidisciplinary

Mechanochemical Lithography

Yuehai Mei et al.

Summary: The study proposes a mechanochemical lithography (MCL) method based on compressive force-triggered reactions for creating surfaces with patterned biomolecules. The method allows printing in physiological conditions and enables the creation of complex structures. The researchers discovered that amino groups in biomolecules can react with maleimide through a force-triggered reaction, resulting in mechanically and chemically stable covalent linkages.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2022)

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Article Chemistry, Multidisciplinary

Diselenide as a Dual Functional Mechanophore Capable of Stress Self-Reporting and Self-Strengthening in Polyurethane Elastomers

Xiaopei Li et al.

Summary: In this study, a new type of elastomer material is reported, which converts destructive forces into productive reactions by using diselenide as a mechanophore. By incorporating labile Se-Se bonds into polyurethane, radical transfer and cross-linking reactions can be activated under mechanical compression, leading to enhanced mechanical and fluorescence properties of the material.

CCS CHEMISTRY (2022)

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Article Multidisciplinary Sciences

Force-reversible chemical reaction at ambient temperature for designing toughened dynamic covalent polymer networks

Mengqi Du et al.

Summary: The click chemistry reaction between triazolinedione (TAD) and indole derivatives was used to create force-reversible C-N bonds, which enable materials to display reversible stress-responsiveness in real time. This method provides a general strategy to enhance mechanical strength and ductility in covalently crosslinked polymer materials.

NATURE COMMUNICATIONS (2022)

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Article Multidisciplinary Sciences

Force-triggered rapid microstructure growth on hydrogel surface for on-demand functions

Qifeng Mu et al.

Summary: The authors report on a force-triggered polymerisation mechanism of double-network hydrogels, which allows for the growth of structures on polymer surfaces within seconds and demonstrates the creation of different functionalities. This force stamp method enables fast spatial modulation of the hydrogel surface, allowing for on-demand functions.

NATURE COMMUNICATIONS (2022)

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Review Nanoscience & Nanotechnology

The role of polymer mechanochemistry in responsive materials and additive manufacturing

Maroun Abi Ghanem et al.

Summary: Polymer mechanochemistry involves converting mechanical forces in materials to chemical reactions through the response of functional groups known as mechanophores. This technology has applications in materials science, polymer physics, and additive manufacturing. The historical development of using mechanical force to chemically transform polymers spans decades, leading to a range of engineered molecular responses that impact optical, mechanical, electronic, and thermal properties.

NATURE REVIEWS MATERIALS (2021)

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Article Chemistry, Multidisciplinary

Segmented Polyurethane Elastomers with Mechanochromic and Self-Strengthening Functions

Kota Seshimo et al.

Summary: Mechanochromic elastomers with force-induced cross-linking reactions and fluorescence properties have been successfully synthesized, demonstrating for the first time damage detection and changes in the mechanical properties of bulk elastomers induced by simple compression or extension.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2021)

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Article Chemistry, Physical

Bio-inspired mechanically adaptive materials through vibration-induced crosslinking

Zhao Wang et al.

Summary: The polymer gel composite material self-strengthens in response to mechanical vibrations similar to observed bone remodelling in animals. It adapts to the mechanical environment by varying its modulus based on force, time, and frequency of agitation, with a 66-fold increase in modulus driven by mechanically responsive ZnO. This material design could have a wide range of applications, from adhesives to materials interfacing with biological systems.

NATURE MATERIALS (2021)

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Article Multidisciplinary Sciences

Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links

Junsoo Kim et al.

Summary: By synthesizing polymers with a large number of entanglements and sparse cross-links, high toughness, strength, and fatigue resistance can be achieved, resulting in hydrogels with low hysteresis, low friction, and high wear resistance after swelling in water.

SCIENCE (2021)

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Article Multidisciplinary Sciences

Toughening hydrogels through force-triggered chemical reactions that lengthen polymer strands

Zi Wang et al.

Summary: This study introduces polymer networks with reactive strand extensions, which significantly improve the stretchability and tear energy of hydrogels. The enhancements synergize with double-network architectures and complement existing toughening strategies.

SCIENCE (2021)

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Article Multidisciplinary Sciences

Flyby reaction trajectories: Chemical dynamics under extrinsic force

Yun Liu et al.

Summary: External force exerted on cyclobutanes can dramatically influence product selectivity through nonstatistical dynamic effects, as demonstrated by experiments and computational modeling. This effect critically depends on external force, reactant stereochemistry, and intermediate stability.

SCIENCE (2021)

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Article Polymer Science

Sensitized Mechanoluminescence Design toward Mechanically Induced Intense Red Emission from Transparent Polymer Films

Fan Yang et al.

MACROMOLECULES (2020)

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Article Nanoscience & Nanotechnology

Robust Multiscale-Oriented Thermoresponsive Fibrous Hydrogels with Rapid Self-Recovery and Ultrafast Response Underwater

Qifeng Mu et al.

ACS APPLIED MATERIALS & INTERFACES (2020)

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Article Multidisciplinary Sciences

Stretchable hydrogels with low hysteresis and anti-fatigue fracture based on polyprotein cross-linkers

Hai Lei et al.

NATURE COMMUNICATIONS (2020)

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Article Chemistry, Multidisciplinary

Validation of the CoGEF Method as a Predictive Tool for Polymer Mechanochemistry

Isabel M. Klein et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2020)

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Article Polymer Science

Crack Tip Field of a Double-Network Gel: Visualization of Covalent Bond Scission through Mechanoradical Polymerization

Takahiro Matsuda et al.

MACROMOLECULES (2020)

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Article Polymer Science

Diselenide-Linked Polymers under Sonication

Qin Wu et al.

ACS MACRO LETTERS (2020)

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Review Chemistry, Multidisciplinary

Reaction Cascades in Polymer Mechanochemistry

Huan Hu et al.

MATERIALS CHEMISTRY FRONTIERS (2020)

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Article Chemistry, Multidisciplinary

Maleimide-thiol adducts stabilized through stretching

Wenmao Huang et al.

NATURE CHEMISTRY (2019)

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Article Multidisciplinary Sciences

Mechanoresponsive self-growing hydrogels inspired by muscle training

Takahiro Matsuda et al.

SCIENCE (2019)

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Article Polymer Science

Modulation and Characterization of the Double Network Hydrogel Surface-Bulk Transition

Martin Frauenlob et al.

MACROMOLECULES (2019)

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Article Polymer Science

Phase-Locked Dynamic and Mechanoresponsive Bonds Design toward Robust and Mechanoluminescent Self-Healing Polyurethanes: A Microscopic View of Self-Healing Behaviors

Chunmei Yan et al.

MACROMOLECULES (2019)

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Article Chemistry, Multidisciplinary

Rotaxanes as Mechanochromic Fluorescent Force Transducers in Polymers

Yoshimitsu Sagara et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

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Review Polymer Science

Empowering mechanochemistry with multi-mechanophore polymer architectures

Brandon H. Bowser et al.

POLYMER CHEMISTRY (2018)

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Article Chemistry, Multidisciplinary

Mechanochemical Regulation of a Photochemical Reaction

Xiaoran Hu et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2018)

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Article Polymer Science

Improving Mechanoluminescent Sensitivity of 1,2-Dioxetane-Containing Thermoplastic Polyurethanes by Controlling Energy Transfer across Polymer Chains

Wei Yuan et al.

MACROMOLECULES (2018)

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Article Polymer Science

Thermally Stable Radical-Type Mechanochromic Polymers Based on Difluorenylsuccinonitrile

Hio Sakai et al.

ACS MACRO LETTERS (2018)

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Article Chemistry, Multidisciplinary

Structural Evolution and Formation Mechanism of the Soft Colloidal Arrays in the Core of PAAm Nanofibers by Electrospun Packing

Qifeng Mu et al.

LANGMUIR (2017)

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Review Polymer Science

Visualized bond scission in mechanically activated polymers

Yuan Yuan et al.

CHINESE JOURNAL OF POLYMER SCIENCE (2017)

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Article Nanoscience & Nanotechnology

Novel Reversible Mechanochromic Elastomer with High Sensitivity: Bond Scission and Bending-Induced Multicolor Switching

Taisheng Wang et al.

ACS APPLIED MATERIALS & INTERFACES (2017)

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Editorial Material Polymer Science

Dynamic Chemistry of Selenium: Se-N and Se-Se Dynamic Covalent Bonds in Polymeric Systems

Shaobo Ji et al.

ACS MACRO LETTERS (2016)

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Article Chemistry, Multidisciplinary

Mechanochromism and Mechanical-Force-Triggered Cross-Linking from a Single Reactive Moiety Incorporated into Polymer Chains

Huan Zhang et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2016)

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Article Chemistry, Multidisciplinary

Stress-induced colouration and crosslinking of polymeric materials by mechanochemical formation of triphenylimidazolyl radicals

F. Verstraeten et al.

CHEMICAL COMMUNICATIONS (2016)

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Article Chemistry, Multidisciplinary

π-extended anthracenes as sensitive probes for mechanical stress

R. Gostl et al.

CHEMICAL SCIENCE (2016)

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Article Multidisciplinary Sciences

Mechanical gating of a mechanochemical reaction cascade

Junpeng Wang et al.

NATURE COMMUNICATIONS (2016)

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Article Chemistry, Multidisciplinary

A Novel Mechanochromic and Photochromic Polymer Film: When Rhodamine Joins Polyurethane

Zhijian Wang et al.

ADVANCED MATERIALS (2015)

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Article Chemistry, Multidisciplinary

Mechanophores with a Reversible Radical System and Freezing-Induced Mechanochemistry in Polymer Solutions and Gels

Keiichi Imato et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2015)

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Article Chemistry, Multidisciplinary

A Mechanochemically Triggered Click Catalyst

Philipp Michael et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2015)

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Article Polymer Science

Mechanochemical Strengthening of a Multi-mechanophore Benzocyclobutene Polymer

Junpeng Wang et al.

ACS MACRO LETTERS (2015)

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3D-Printed Mechanochromic Materials

Gregory I. Peterson et al.

ACS APPLIED MATERIALS & INTERFACES (2015)

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Successive Mechanochemical Activation and Small Molecule Release in an Elastomeric Material

Michael B. Larsen et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2014)

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Direct correlation of single-molecule properties with bulk mechanical performance for the biomimetic design of polymers

Jaeyoon Chung et al.

NATURE MATERIALS (2014)

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Ultrasound-triggered disruption and self-healing of reversibly cross-linked hydrogels for drug delivery and enhanced chemotherapy

Nathaniel Huebsch et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2014)

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Cephalopod-inspired design of electro-mechano-chemically responsive elastomers for on-demand fluorescent patterning

Qiming Wang et al.

NATURE COMMUNICATIONS (2014)

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γ-Ray-Responsive Supramolecular Hydrogel Based on a Diselenide-Containing Polymer and a Peptide

Wei Cao et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2013)

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Flex-Activated Mechanophores: Using Polymer Mechanochemistry To Direct Bond Bending Activation

Michael B. Larsen et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2013)

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Mechanochemical strengthening of a synthetic polymer in response to typically destructive shear forces

Ashley L. Black Ramirez et al.

NATURE CHEMISTRY (2013)

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Review Chemistry, Multidisciplinary

Covalent Mechanochemistry: Theoretical Concepts and Computational Tools with Applications to Molecular Nanomechanics

Jordi Ribas-Arino et al.

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Proton-Coupled Mechanochemical Transduction: A Mechanogenerated Add

Charles E. Diesendruck et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2012)

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Mechanically induced chemiluminescence from polymers incorporating a 1,2-dioxetane unit in the main chain

Yulan Chen et al.

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Force-Transformed Free-Energy Surfaces and Trajectory-Shooting Simulations Reveal the Mechano-Stereochemistry of Cyclopropane Ring-Opening Reactions

Przemyslaw Dopieralski et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2011)

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Structure-Mechanochemical Activity Relationships for Cyclobutane Mechanophores

Matthew J. Kryger et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2011)

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Article Chemistry, Multidisciplinary

Molecular Stress Relief through a Force-Induced Irreversible Extension in Polymer Contour Length

Dong Wu et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2010)

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Article Chemistry, Multidisciplinary

Dual Redox Responsive Assemblies Formed from Diselenide Block Copolymers

Ning Ma et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2010)

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Article Chemistry, Multidisciplinary

Force-Induced Redistribution of a Chemical Equilibrium

Corissa K. Lee et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2010)

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Article Chemistry, Multidisciplinary

Understanding Covalent Mechanochemistry

Jordi Ribas-Arino et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2009)

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Review Chemistry, Multidisciplinary

Mechanically-Induced Chemical Changes in Polymeric Materials

Mary M. Caruso et al.

CHEMICAL REVIEWS (2009)

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Article Multidisciplinary Sciences

Force-induced activation of covalent bonds in mechanoresponsive polymeric materials

Douglas A. Davis et al.

NATURE (2009)

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Article Chemistry, Multidisciplinary

Activating catalysts with mechanical force

Alessio Piermattei et al.

NATURE CHEMISTRY (2009)

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Article Multidisciplinary Sciences

Biasing reaction pathways with mechanical force

Charles R. Hickenboth et al.

NATURE (2007)

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Article Polymer Science

Ultrasound-induced site-specific cleavage of azo-functionalized poly(ethylene glycol)

KL Berkowski et al.

MACROMOLECULES (2005)

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Review Chemistry, Multidisciplinary

Mechanochemistry: The mechanical activation of covalent bonds

MK Beyer et al.

CHEMICAL REVIEWS (2005)

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Article Chemistry, Multidisciplinary

Reversible mechanochemistry of a Pd-II coordination polymer

JMJ Paulusse et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2004)

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Review Biochemistry & Molecular Biology

Force spectroscopy with single bio-molecules

H Clausen-Schaumann et al.

CURRENT OPINION IN CHEMICAL BIOLOGY (2000)

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Article Chemistry, Physical

The mechanical strength of a covalent bond calculated by density functional theory

MK Beyer

JOURNAL OF CHEMICAL PHYSICS (2000)

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