Controlling Carbodiimide-Driven Reaction Networks Through the Reversible Formation of Pyridine Adducts DOI
William S. Salvia, Georgia Mantel, Nirob K. Saha

и другие.

Chemical Communications, Год журнала: 2024, Номер 60(88), С. 12876 - 12879

Опубликована: Янв. 1, 2024

The reversible formation of adducts between a carbodiimide and pyridine allows the slow release fuels for transient anhydride bond formation.

Язык: Английский

Positioning dynamic polymeric materials within the modern polymer economy: From application to recycling and circularity DOI Creative Commons
Meng Jiang,

Nadim Mahmud,

Christopher Koelbl

и другие.

Journal of Polymer Science, Год журнала: 2024, Номер 62(15), С. 3562 - 3583

Опубликована: Май 22, 2024

Abstract Innovations in dynamic polymeric materials offer prospects to improve the circularity and lower environmental impact of modern polymer economy. These are also beginning blur distinction between re‐use recycling methods since bulk material properties may be rationally changed after applying a stimulus or performing controlled chemical reaction. In this Perspective, we propose that polymers denote unique class versatile post‐consumer waste, which shares similarities emergent upcycling approaches while offering additional opportunities within more classical schemes. A brief overview stimuli‐responsive is presented where illustrative examples discussed context developing practical materials. Dynamic covalent then highlighted, along with emerging techniques such as editing, focus on recent reports demonstrating rational manipulation properties. Finally, discuss these alongside explore how could perform sphere.

Язык: Английский

Процитировано

3

Photoresponsive Polymers for Carbodiimide-Fueled Transient Hydrogels DOI Creative Commons
Ibrahim O. Raji,

Torin C. Wilcox,

C. Scott Hartley

и другие.

Polymer Chemistry, Год журнала: 2025, Номер 16(8), С. 947 - 953

Опубликована: Янв. 1, 2025

Light and fuel responsive polymers were developed. Transient hydrogels could be formed only after exposure to both photochemical stimuli.

Язык: Английский

Процитировано

0

Transient Stiffness Patterning in Hydrogels Driven by Dissipative Mechanochemical Coupling DOI Creative Commons
Roberto Baretta, Maria F. Pantano, Marco Frasconi

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Май 9, 2025

Abstract Living systems adapt to mechanical forces through a series of biochemical feedback loops and dissipative signal transduction mechanisms across multiple length scales. By contrast, synthetic materials are static, closed with minimal interaction their surroundings lack the ability deformations. Here, strategy that enables hydrogel temporal modulation its stiffness properties is reported. It demonstrated force‐induced bond rupture at disulfide linkages hydrogel, coupled chemical reoxidation leads dissipative, transient functions. The electrochemical generation oxidant as output loop triggered by an externally applied force provides high spatiotemporal control over process, enabling engineering hydrogels out‐of‐equilibrium patterns. Additionally, dose‐controlled, release model protein payloads from demonstrated. proposed concept has potential enhance autonomous interactive functionalities hydrogels, advancing applications in biomedical field soft robotics.

Язык: Английский

Процитировано

0

Cyclic Macroscopic Assembly and Disassembly Driven by Ionic Strength Fuel: A Waste-Free Approach DOI
Ting Zhao, Zhongrui Wang, Yang Yang

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2023, Номер 15(27), С. 33169 - 33179

Опубликована: Июль 4, 2023

Nonequilibrium assembling systems developed so far have relied on chemical fuels to drive the programmable pH cycles, redox reactions, and metastable bond formations. However, these methods often result in unwanted accumulation of waste. Herein, we present a novel strategy for achieving cyclic waste-free nonequilibrium assembly disassembly macroscopic hydrogels, utilizing an ionic strength-mediated approach. Our involves using ammonium carbonate as fuel temporally regulate attractions between oppositely charged hydrogels via strength-controlled charge screening hydrogel elasticity changes. This effectively mediates assembly/disassembly processes prevents waste accumulation, can completely decompose into volatile The reversible process be achieved without significant damping due self-clearance mechanism, long is repeatedly supplied. concept holds promise creating microscopic self-adaptive materials.

Язык: Английский

Процитировано

5

Bio‐Inspired Far‐From‐Equilibrium Hydrogels: Design Principles and Applications DOI
Jiadong Tang,

Yibo Cheng,

Muhua Ding

и другие.

ChemPlusChem, Год журнала: 2023, Номер 88(12)

Опубликована: Окт. 3, 2023

Abstract Inspired from dynamic living systems that operate under out‐of‐equilibrium conditions in biology, developing supramolecular hydrogels with self‐regulating and autonomously properties to further advance adaptive life‐like behavior is important. This review presents recent progress of bio‐inspired out‐of‐equilibrium. The principle self‐assembly for creating discussed. Various design strategies have been identified, such as chemical‐driven reaction cycles feedback control physically oscillatory systems. These can be coupled achieve temporal spatial over structural mechanical well programmable lifetime. studies open up huge opportunities potential applications, fluidic guidance, information storage, drug delivery, actuators more. Finally, we address the challenges ahead us coming years, future possibilities prospects are identified.

Язык: Английский

Процитировано

4

Transient Covalent Polymers through Carbodiimide‐driven Assembly DOI Creative Commons
Nirob K. Saha, William S. Salvia, Dominik Konkolewicz

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(31)

Опубликована: Май 21, 2024

Abstract Biochemical systems make use of out‐of‐equilibrium polymers generated under kinetic control. Inspired by these systems, many abiotic supramolecular driven chemical fuel reactions have been reported. Conversely, based on transient covalent bonds received little attention, even though they the potential to complement generating structures stronger and offering a straightforward tuning reaction kinetics. In this study, we show that simple aqueous dicarboxylic acids give poly(anhydrides) when treated with carbodiimide EDC. Transient molecular weights exceeding 15,000 are which then decompose over course hours weeks. Disassembly kinetics can be controlled using substituent effects in monomer design. The impact solvent polarity, concentration, temperature, pyridine concentration polymer properties lifetimes has investigated. results reveal substantial control assembly disassembly kinetics, highlighting for fine‐tuned nonequilibrium polymerization systems.

Язык: Английский

Процитировано

1

Transient Covalent Polymers through Carbodiimide‐driven Assembly DOI Creative Commons
Nirob K. Saha, William S. Salvia, Dominik Konkolewicz

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(31)

Опубликована: Май 21, 2024

Abstract Biochemical systems make use of out‐of‐equilibrium polymers generated under kinetic control. Inspired by these systems, many abiotic supramolecular driven chemical fuel reactions have been reported. Conversely, based on transient covalent bonds received little attention, even though they the potential to complement generating structures stronger and offering a straightforward tuning reaction kinetics. In this study, we show that simple aqueous dicarboxylic acids give poly(anhydrides) when treated with carbodiimide EDC. Transient molecular weights exceeding 15,000 are which then decompose over course hours weeks. Disassembly kinetics can be controlled using substituent effects in monomer design. The impact solvent polarity, concentration, temperature, pyridine concentration polymer properties lifetimes has investigated. results reveal substantial control assembly disassembly kinetics, highlighting for fine‐tuned nonequilibrium polymerization systems.

Язык: Английский

Процитировано

1

Fuel‐driven π‐conjugated Superstructures to Form Transient Conductive Hydrogels DOI
Ifigeneia Tsironi, Jarek A. Maleszka,

Brigitte A. K. Kriebish

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 21, 2024

Abstract Despite advances in creating dissipative materials with transient properties, such as hydrogels and active droplets, their application remains confined to temporal changes structural properties. Developing out‐of‐equilibrium whose electronic functions are parameterized by a chemical reaction cycle is challenging. Yet, this class of required construct biomimetic materials. In contrast traditional cycles that exploit molecularly dissolved building blocks at thermodynamic equilibrium, we show fiber structures derived from reactive naphthalene diimide (NDI) can be used resting states form far‐from‐equilibrium conductive after the addition fuels. Upon fueling NDI‐derived fibers, dual‐component activation deactivation pathway deduced kinetic analysis absent when using state. Investigating solid‐state morphologies formed throughout fuel‐driven cryo‐EM reveals fibers evolve thicker fibrils layered superstructures. We redox‐active exhibit nearly threefold increase electrical conductivity upon fuel consumption before reverting original value over hours. These potential candidates applications programmable biorobotics computing.

Язык: Английский

Процитировано

1

Photochemical Patterning and Characterization of Mechanical Properties on Soft Materials DOI Creative Commons
Jun Hyeong Park, Patrick J. Grimes, Henry E. Symons

и другие.

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 2, 2024

Abstract Although different chemistries for the spatio‐temporal localization of molecules and gradients chemical signals within soft materials are now available, achievement patterns mechanical properties in such their characterization remain considerable challenges. This study presents syntheses two novel photo‐sensitive thermoresponsive hydrogel systems, a photo‐stiffening photo‐softening hydrogel. Their potential fabricating with patterned is then demonstrated by an actuator whose higher‐order bending can be switched on light, encoding digital information encryption storage. Microindentation custom‐made data analysis software essential all materials. From general perspective, this work opens route to fabrication properties, addressing important emerging challenge science applications robotics

Язык: Английский

Процитировано

1

Dynamic surface chemistry and interparticle interactions mediating chemically fueled dissipative assembly of colloids DOI

Thilini Umesha Dissanayake,

Justin Hughes,

Taylor J. Woehl

и другие.

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 650, С. 972 - 982

Опубликована: Июль 1, 2023

Язык: Английский

Процитировано

3