Article
Chemistry, Multidisciplinary
Josefine Meurer, Julian Hniopek, Thomas Baetz, Stefan Zechel, Marcel Enke, Juergen Vitz, Michael Schmitt, Juergen Popp, Martin D. Hager, Ulrich S. Schubert
Summary: A new shape-memory polymer is presented, utilizing two different metal complexes to achieve high strain fixity rates and strain recovery rates, with the mechanism revealed through various techniques such as Raman spectroscopy.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Xiao Li, Minghao Li, Lisa Tang, Diwei Shi, Emily Lam, Jinhye Bae
Summary: This review explores the potential of stimuli-responsive hydrogels in mimicking the morphing behavior of living tissues or organisms, and discusses how functional additives can be combined with hydrogels to extend their functionalities. It also highlights the potential applications of stimuli-responsive composite hydrogels in various fields including soft robotics, information encryption/decryption, biomedical research, flexible electronics, and engineering living materials.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Multidisciplinary
Jia-Qi Zhu, Han Wu, Zhen-Li Li, Xin-Fei Xu, Hao Xing, Ming-Da Wang, Hang-Dong Jia, Lei Liang, Chao Li, Li-Yang Sun, Yu-Guang Wang, Feng Shen, Dong-Sheng Huang, Tian Yang
Summary: This article summarizes the synthesis methods and applications of nanocomposite responsive hydrogels, which can respond to external or internal physiological stimuli and be used for responsive drug delivery.
ADVANCED MATERIALS
(2022)
Article
Polymer Science
Xiaozhuang Zhou, Shruthi Kandalai, Farzana Hossain, Nan Zhang, Huapeng Li, Qingfei Zheng
Summary: A new class of pH-responsive and recyclable hydrogels with versatile gas-releasing and scavenging properties is reported in this study. The hydrogels can be reversibly controlled through pH changes, allowing for disassembly and reassembly of the gel network. The disassembled copolymer chains can reform hydrogels, and the mineral salts used in the process can function as gas donors or scavengers. This research provides a facile and environmentally friendly method to recycle hydrogels with gas-releasing and gas-scavenging properties, with potential applications in wound healing, wastewater management, and gas therapy for diseases.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Lingcong Huang, Yang Liu, Hongxiang Chen, Jun Wu, Xiongzhi Zhang, Simin Liu
Summary: In this study, a supramolecular photonic crystal hydrogel (SPCH) with responsive and self-healing properties was developed. The SPCH exhibited a bright structural color that could be tuned by water content, ethanol, and competitive guest concentration. The SPCH also showed self-healing properties at room temperature.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)
Review
Chemistry, Multidisciplinary
Pedro Lavrador, Marco R. Esteves, Vitor M. Gaspar, Joao F. Mano
Summary: Recent advances in the design of stimuli-responsive nanocomposite hydrogels have expanded their potential for operating as advanced systems in various biomedical applications, benefitting from tailored single or multi-responsiveness. The combination of hydrogels and nanoparticles showcases an intrinsic ability to react to external or internal/physiological stimuli, developing intelligent systems with application-oriented features.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Zheng Li, Zhiqiang Yang, Yinan Zhang, Bing Yang, Ying-Wei Yang
Summary: A macrocycle-to-framework strategy was used to construct functional organic polymers with bright yellowish-green luminescence and unique solvatochromism behaviors. The materials showed amplified sensitivity to acidic conditions with luminescent and colorimetric dual-modal patterns, as well as rapid luminescence quenching and high selectivity to nitrobenzene compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Organic
Fabian Hoffmann, Anna-Lena Leistner, Susanne Kirchner, Burkhard Luy, Claudia Muhle-Goll, Zbigniew Pianowski
Summary: This study presents a structural analysis of peptide-derived photochromic supramolecular hydrogels using advanced techniques of nuclear magnetic resonance. The hydrogels were physically loaded with a selection of biologically related compounds. The results provide detailed and correct understanding of the loading process and will guide the correct design of phototriggered drug delivery systems.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Review
Polymer Science
Tyus J. Yeingst, Julien H. Arrizabalaga, Daniel J. Hayes
Summary: Stimuli-responsive hydrogel drug delivery systems that release drugs under external stimuli, such as ultrasound, have gained importance in the field of drug delivery. This review summarizes the current understanding of ultrasound-responsive hydrogels, including mechanisms of drug release, innovative formulations, and applications in cancer treatment and tissue engineering.
Article
Materials Science, Multidisciplinary
Supissra Boon-in, Man Theerasilp, Daniel Crespy
Summary: Skin inflammation can cause an increase in skin temperature, and cooling inflamed skin can relieve pain and dissipate heat. Evaporative cooling hydrogels with high latent heat are promising materials for flexible dressings. A double-network hydrogel formed with PAMPS and PNIPAM can release water above the skin temperature and delay the release of water, resulting in prolonged cooling performance and enhanced mechanical properties. Our material demonstrates superior cooling power with lower temperature compared to other reported hydrogels for passive cooling, and it can be applied to cool other structures such as photovoltaic panels or roofs of buildings.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yoshimitsu Sagara, Hanna Traeger, Jie Li, Yuji Okado, Stephen Schrettl, Nobuyuki Tamaoki, Christoph Weder
Summary: A new approach to cyclophane-based supramolecular mechanophores is introduced in this study. The mechanically responsive cyclic motif shows a noticeable change in emission color upon deformation, indicating a suppression of excimer-promoting interactions between luminophores. The research suggests that cyclophanes have the potential for developing various supramolecular mechanophores for detecting and visualizing weak forces in polymeric materials or living tissues.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Review
Automation & Control Systems
Yusen Zhao, Mutian Hua, Yichen Yan, Shuwang Wu, Yousif Alsaid, Ximin He
Summary: This article reviews recent progress in the use of stimuli-responsive polymers for soft robotics. Different types of representative stimuli-responsive polymers are introduced, and their actuation mechanisms and performance evaluation are discussed. Examples of soft robotic applications based on stimuli-responsive polymers are presented. Current opportunities and challenges of stimuli-responsive soft robots for future study are discussed.
ANNUAL REVIEW OF CONTROL ROBOTICS AND AUTONOMOUS SYSTEMS
(2022)
Article
Mechanics
Matthew D. Butler, Thomas D. Montenegro-Johnson
Summary: Thermo-responsive hydrogels exhibit significant expansion and contraction in response to temperature changes, making them promising materials for controllable actuators in micro-scale devices. By studying these systems using a poro-elastic model, we can better understand the dynamic properties and different swelling and shrinking behaviors of thermo-responsive hydrogels.
JOURNAL OF FLUID MECHANICS
(2022)
Review
Chemistry, Physical
Xinxing Lin, Xiaolin Wang, Liangpeng Zeng, Zi Liang Wu, Hui Guo, Dominique Hourdet
Summary: This article provides a detailed review of hydrogels with stimuli-responsive toughness, discussing characteristic reinforcement mechanisms and demonstrating smart hydrogels that respond to various stimuli. Special attention is paid to thermal, light, pH, and salt triggers due to their broad applications and easy implementation. In addition, the applications and future development challenges of these smart hydrogels are summarized.
CHEMISTRY OF MATERIALS
(2021)
Article
Polymer Science
Matthew Mulvee, Natasa Vasiljevic, Stephen Mann, Avinash J. Patil
Summary: This study demonstrates the formation of hybrid nucleotide-amino acid supramolecular hydrogels using silver ion-triggered silver-guanosine monophosphate dimers. The assembly kinetics, supramolecular organization, and mechanical properties of the hydrogels are affected by the molar ratio of Ag:GMP:FY. pH can be used as an external stimulus to selectively disassemble nanofilaments from the hybrid hydrogels.
Article
Multidisciplinary Sciences
Xin Li, Laura Hetjens, Nadja Wolter, Helin Li, Xiangyang Shi, Andrij Pich
Summary: In this study, lysozyme-responsive microgels were developed for the treatment of inflammatory bowel disease. Compared to other pH-responsive carriers, lysozyme-responsive microgels can better identify healthy and inflamed intestines, achieving effective treatment with fewer side effects.
JOURNAL OF ADVANCED RESEARCH
(2023)
Article
Polymer Science
Catalina Molano-Lopez, Susanne Braun, Michael Kather, Alexander Toepel, Gil van Wissen, Andrij Pich
Summary: This work focuses on the pH-triggered disassembly of supramacromolecular microgels. The properties of the microgels can be easily tuned by varying the ratio between the temperature-responsive poly(N-vinylcaprolactam) and the natural polyphenol tannic acid. The pH and temperature can precisely control the degradation profile of the microgels.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Article
Biochemistry & Molecular Biology
Willem E. M. Noteborn, Sandeepa K. Vittala, Maria Broto Torredemer, Chandan Maity, Frank Versluis, Rienk Eelkema, Roxanne E. Kieltyka
Summary: Low-molecular-weight hydrogels are modular and easy to prepare scaffolds for drug delivery applications. A reaction-coupled gelator is used to tune drug release by altering the reaction pathway. The release mode changes from Fickian to semi-Fickian with a decreased rate when covalent ligation is increased. The reaction-coupled approach allows the preparation of drug-loaded hydrogels in situ with tunable mechanics and drug release profiles.
Article
Chemistry, Multidisciplinary
Benjamin Spitzbarth, Rienk Eelkema
Summary: Dynamic covalent (DCv) ureas are widely used in the design of self-healing materials. In addition to self-healing, the species in the equilibrium of DCv ureas can serve as responsive organocatalysts. By controlling stimuli such as heat or water addition, the equilibrium can be shifted towards isocyanate and free base, which can function as in situ released reagents. We demonstrate the application of DCv ureas as organocatalysts in two examples, including the catalytic activation of a latent organocatalyst and the triggering of nitrile-N-oxide release for the formation of an isoxazoline polymer gel.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Bohang Wu, Reece W. W. Lewis, Guotai Li, Yifan Gao, Bowen Fan, Benjamin Klemm, Jianan Huang, Junyou Wang, Martien A. A. Cohen Stuart, Rienk Eelkema
Summary: By constructing a coacervate hydrogel with a Michael addition-based chemical reaction network (CRN) as a platform, the state of the coacervate materials can be easily controlled by specific chemical signals. The designed pyridine-based ABA triblock copolymer can undergo regulation through quaternization by an allyl acetate electrophile and an amine nucleophile, resulting in gel construction and collapse in the presence of polyanions. The coacervate gels exhibit highly tunable stiffness and gelation times, as well as excellent self-healing ability and injectability with different sized needles, and accelerated degradation induced by chemical signal-induced coacervation disruption. This work represents a first step towards the development of a new class of signal-responsive injectable materials.
Article
Biochemistry & Molecular Biology
Bowen Fan, Diana Torres Garcia, Marziye Salehi, Matthew J. Webber, Sander I. van Kasteren, Rienk Eelkema
Summary: This report describes the synthesis, characterization, and application of a new dynamic covalent dextran hydrogel as an injectable depot for peptide vaccines. The hydrogel shows shear-thinning and self-healing capabilities, enabling hydrogel injection. The hydrogels deliver peptides without modifying their immunogenicity and demonstrate potential as a sustained-release material for the delivery of peptide vaccines.
ACS CHEMICAL BIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Chaolei Hu, Pit van Bonn, Dan E. E. Demco, Carsten Bolm, Andrij Pich
Summary: This article demonstrates for the first time that mechanochemically triggered free-radical polymerization allows solvent- and initiator-free syntheses of complex functional macro molecular architectures, namely stimuliresponsive microgels. The developed mechanochemical polymerization approach is applicable to a variety of monomers and allows synthesizing microgels with tunable chemical structure, variable size, controlled number of crosslinks and reactive functional end-groups.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Irene Piergentili, Thomas Hilberath, Benjamin Klemm, Frank Hollmann, Rienk Eelkema
Summary: In this study, a diphenylalanine (FF) derivative with a thioether phenyl moiety was developed to form supramolecular hydrogels at neutral and mildly acidic pH. The thioether can be oxidized by reactive oxygen species (ROS) to form the corresponding sulfoxide, resulting in hydrogel disintegration. Peroxidases were incorporated to enhance ROS sensitivity, enabling the hydrogels to collapse with lower concentrations of hydrogen peroxide.
Article
Chemistry, Physical
Jacek J. Walkowiak, Casper van Duijnhoven, Pia Boeschen, Nadja A. Wolter, Joanna Michalska-Walkowiak, Martin Dulle, Andrij Pich
Summary: Raspberry-like poly(oligoethylene methacrylate-b-N-vinylcaprolactam)/polystyrene (POEGMA-b-PVCL/PS) patchy particles (PPs) and complex colloidal particle clusters (CCPCs) were successfully fabricated using a two-step or one-step cascade flow process. The internal structure and surface morphology of the particles were studied under different polymerization conditions. The use of a tubular flow reactor for photo-initiated reversible addition-fragmentation transfer precipitation polymerization (Photo-RPP) provided advantages over heat dissipation and homogeneous light distribution.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Anastasiia Sharko, Benjamin Spitzbarth, Thomas M. Hermans, Rienk Eelkema
Summary: This article introduces shunts in chemical reaction networks (CRNs), which are widely distributed in nature, allowing adaptability to both external and internal stimuli. By using weak oxidants, access to two shunts with different kinetics and fewer side reactions compared to the main cycle driven by strong oxidants can be achieved in this CRN. Additionally, a strategy is proposed to recycle one of the main products under flow conditions to partially reverse the CRN and control product speciation over time. These findings provide new levels of control in artificial CRNs driven by redox chemistry, bridging the gap between synthetic and natural systems.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Pharmacology & Pharmacy
Huanhuan Liu, Robin A. Nadar, Retna Putri Fauzia, Adrianus C. Laan, Britt Doeswijk, Runze Wang, Astrid van de Meer, Quenteijn van Cooten, Elizabeth C. M. Carroll, Rienk Eelkema, Antonia G. Denkova
Summary: This study explores the combination of chemotherapy and radionuclide therapy using polymeric micelles as a delivery vehicle. The results show that the micelles can penetrate deep into the tumor spheroid and mainly accumulate around or in the lysosomes. Furthermore, the combined therapy achieves a superior therapeutic outcome compared to single treatments.
ADVANCED THERAPEUTICS
(2023)
Article
Chemistry, Multidisciplinary
Guotai Li, Yucheng Wan, Reece W. Lewis, Bowen Fan, Rienk Eelkema
Summary: Living systems can respond to environmental stimuli through signal transduction cascades. Researchers have developed a synthetic material that forms a supramolecular network responsive to nucleophilic chemical signals through a reaction-assembly cascade. This work opens up new possibilities for signal-responsive synthetic materials and interactions with biological systems.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Jules Stouten, Huixing Cao, Andrij Pich, Katrien V. Bernaerts
Summary: Renewable and functional cross-linkable latexes synthesized by polymerization-induced self-assembly (PISA) exhibit small particle size, good colloidal stability, and are free of volatile organic compounds. After UV curing, the latex can form flexible to rigid cross-linked films, which show promise as oil and water barriers in paper coating applications.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Hannah F. Mathews, Maria I. Pieper, Se-Hyeong Jung, Andrij Pich
Summary: In this study, pH-responsive drug carriers were successfully fabricated and it was demonstrated that the distribution of charges has an impact on delivery efficiency. By synthesizing polyampholyte nanogel-in-microgel colloids, the arrangement of nanogels could be easily manipulated by adjusting synthesis conditions. The obtained nanogels, with positive and negative charges, were incorporated into microgel networks. Confocal laser scanning microscopy confirmed the formation of colloids with different nanogel arrangements depending on nanogel concentration, pH value, and ionic strength. This research is a significant advancement in the uptake and release of oppositely charged drug molecules.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Susanne Braun, Guilherme Dilarri, Leticia C. de Lencastre Novaes, Philipp Huth, Alexander Toepel, Larissa Hussmann, Alexander Boes, Miguel Divino da Rocha, Felix Jakob, Luis Octavio Regasini, Ulrich Schwaneberg, Henrique Ferreira, Andrij Pich
Summary: The development of efficient and environmentally friendly plant protection systems is crucial for sustainable agriculture. Citrus canker caused by Xanthomonas citri is a major problem worldwide, with current copper-based formulations causing contamination and environmental damage. A copper-free microgel-based system is designed to combat citrus canker effectively, providing long-term protection and reducing environmental pollution.
ADVANCED FUNCTIONAL MATERIALS
(2023)
