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Fan, B. (author), Torres García, Diana (author), Salehi, Marziye (author), Webber, Matthew J. (author), van Kasteren, S.I. (author), Eelkema, R. (author)Dextran-based hydrogels are promising therapeutic materials for drug delivery, tissue regeneration devices, and cell therapy vectors, due to their high biocompatibility, along with their ability to protect and release active therapeutic agents. This report describes the synthesis, characterization, and application of a new dynamic covalent...journal article 2023
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Spitzbarth, B. (author), Eelkema, R. (author)Dynamic covalent (DCv) ureas have been used abundantly to design self-healing materials. We demonstrate that apart from self-healing materials, the species present in the equilibrium of DCv ureas can be employed as responsive organocatalysts. Easily controllable stimuli like heat or addition of water shift the equilibrium towards isocyanate...journal article 2023
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Li, G. (author), Wan, Yucheng (author), Lewis, R.W. (author), Fan, B. (author), Eelkema, R. (author)Living systems can respond to their environment through signal transduction cascades. In these cascades, original stimuli are amplified and translated into reaction or assembly events. In an effort to instill synthetic materials with biomimetic responsivity, we report an aggregation process forming a supramolecular network held together by...journal article 2023
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Lewis, R.W. (author), Muralidharan, A. (author), Klemm, B. (author), Boukany, P. (author), Eelkema, R. (author)Polycationic carriers promise low cost and scalable gene therapy treatments, however inefficient intracellular unpacking of the genetic cargo has limited transfection efficiency. Charge-reversing polycations, which transition from cationic to neutral or negative charge, can offer targeted intracellular DNA release. We describe a new class of...journal article 2023
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Li, G. (author), Lewis, R.W. (author), Eelkema, R. (author)The field of supramolecular chemistry is rapidly progressing, transitioning from the creation of thermodynamically stable systems found in local or global minima on the free energy landscape to the development of out-of-equilibrium systems that rely on chemical reactions to establish and maintain their structures. Over the past decade,...review 2023
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Sharko, Anastasiia (author), Spitzbarth, B. (author), Hermans, Thomas M. (author), Eelkema, R. (author)Shunts, alternative pathways in chemical reaction networks (CRNs), are ubiquitous in nature, enabling adaptability to external and internal stimuli. We introduce a CRN in which the recovery of Michael-accepting species is driven by oxidation chemistry. Using weak oxidants can enable access to two shunts within this CRN with different kinetics...journal article 2023
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Piergentili, I. (author), Hilberath, T. (author), Klemm, B. (author), Hollmann, F. (author), Eelkema, R. (author)Hydrogels that can disintegrate upon exposure to reactive oxygen species (ROS) have the potential for targeted drug delivery to tumor cells. In this study, we developed a diphenylalanine (FF) derivative with a thioether phenyl moiety attached to the N-terminus that can form supramolecular hydrogels at neutral and mildly acidic pH. The...journal article 2023
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Lantos, Emese (author), Mótyán, Gergő (author), Frank, Éva (author), Eelkema, R. (author), van Esch, J.H. (author), Horváth, Dezső (author), Tóth, Ágota (author)In living systems adaptive regulation requires the presence of nonlinear responses in the underlying chemical networks. Positive feedbacks, for example, can lead to autocatalytic bursts that provide switches between two stable states or to oscillatory dynamics. The stereostructure stabilized by hydrogen bonds provides an enzyme its...journal article 2023
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Spitzbarth, B. (author), Eelkema, R. (author)Over the last few decades, the study of more complex, chemical systems closer to those found in nature, and the interactions within those systems, has grown immensely. Despite great efforts, the need for new, versatile, and robust chemistry to apply in CRNs remains. In this Feature Article, we give a brief overview over previous developments...journal article 2023
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Wang, Hucheng (author), Fu, Xiaoming (author), Gu, Guanyao (author), Bai, Shengyu (author), Li, Runlai (author), Zhong, Weimin (author), Guo, Xuhong (author), Eelkema, R. (author), van Esch, J.H. (author), Cao, Zhixing (author), Wang, Yiming (author)Living organisms are capable of dynamically changing their structures for adaptive functions through sophisticated reaction-diffusion processes. Here we show how active supramolecular hydrogels with programmable lifetimes and macroscopic structures can be created by relying on a simple reaction-diffusion strategy. Two hydrogel precursors ...journal article 2023
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Klemm, B. (author), Roshanasan, A. (author), Piergentili, I. (author), van Esch, J.H. (author), Eelkema, R. (author)We present an approach for detecting thiol analytes through a self-propagating amplification cycle that triggers the macroscopic degradation of a hydrogel scaffold. The amplification system consists of an allylic phosphonium salt that upon reaction with the thiol analyte releases a phosphine, which reduces a disulfide to form two thiols,...journal article 2023
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Piergentili, I. (author), Cai, Mao (author), Klemm, B. (author), Xu, B. (author), Luo, Sanzhong (author), Eelkema, R. (author)The redox balance in tumor and diseased cells often leads to the production of reactive oxygen species (ROS). Many ROS-responsive materials based on sulfur oxidation have been reported with the goal of achieving controlled delivery at the tumor. However, these materials often lack responsiveness to low ROS concentrations present in the tumor...journal article 2023
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Wu, B. (author), Lewis, R.W. (author), Li, G. (author), Gao, Yifan (author), Fan, B. (author), Klemm, B. (author), Huang, J. (author), Wang, Junyou (author), Cohen Stuart, Martien A. (author), Eelkema, R. (author)In the quest for stimuli-responsive materials with specific, controllable functions, coacervate hydrogels have become a promising candidate, featuring sensitive responsiveness to environmental signals enabling control over sol-gel transitions. However, conventional coacervation-based materials are regulated by relatively non-specific signals,...journal article 2023
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Noteborn, Willem E.M. (author), Vittala, Sandeepa K. (author), Torredemer, Maria Broto (author), Maity, C. (author), Versluis, F. (author), Eelkema, R. (author), Kieltyka, Roxanne E. (author)Low-molecular-weight hydrogels are attractive scaffolds for drug delivery applications because of their modular and facile preparation starting from inexpensive molecular components. The molecular design of the hydrogelator results in a commitment to a particular release strategy, where either noncovalent or covalent bonding of the drug...journal article 2023
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Liu, H. (author), Nadar, R.A. (author), Fauzia, R.P. (author), Laan, A.C. (author), Wang, R. (author), van Cooten, Quenteijn (author), Carroll, E.C.M. (author), Eelkema, R. (author), Denkova, A.G. (author)Combination of therapies is a common strategy in cancer treatment. Such combined therapies only have merit provided that there is superior therapeutic outcome with fewer side effects, compared to single therapies. Here, this work explores the possibility to combine chemotherapy with radionuclide therapy using polymeric micelles as a delivery...journal article 2023
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Klemm, B. (author), Lewis, R.W. (author), Piergentili, I. (author), Eelkema, R. (author)Out of equilibrium operation of chemical reaction networks (CRNs) enables artificial materials to autonomously respond to their environment by activation and deactivation of intermolecular interactions. Generally, their activation can be driven by various chemical conversions, yet their deactivation to non-interacting building blocks remains...journal article 2022
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Liu, H. (author), de Kruijff, R.M. (author), Laan, A.C. (author), Beekman, F.J. (author), van den Heuvel, E.J. (author), Ramakers, R.M. (author), Eelkema, R. (author), Denkova, A.G. (author)A variety of polymer micelles are designed for the delivery of chemotherapeutic drugs to tumors. Although the promise of these nanocarriers is very high, in the clinic the effectivity is rather limited. Determining the in vivo fate of the micelles can greatly help to improve this treatment. Here, a simple and fast chelator-free method for...journal article 2022
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Lewis, R.W. (author), Klemm, B. (author), Macchione, M. (author), Eelkema, R. (author)Fuel-driven macromolecular coacervation is an entry into the transient formation of highly charged, responsive material phases. In this work, we used a chemical reaction network (CRN) to drive the coacervation of macromolecular species readily produced using radical polymerisation methods. The CRN enables transient quaternization of tertiary...journal article 2022
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Piergentili, I. (author), Bouwmans, Pepijn R. (author), Reinalda, L. (author), Lewis, R.W. (author), Klemm, Benjamin (author), Liu, H. (author), de Kruijff, R.M. (author), Denkova, A.G. (author), Eelkema, R. (author)In certain tumor and diseased tissues, reactive oxygen species (ROS), such as H<sub>2</sub>O<sub>2</sub>, are produced in higher concentrations than in healthy cells. Drug delivery and release systems that respond selectively to the presence of ROS, while maintaining their stability in “healthy” biological conditions, have great potential as...journal article 2022
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Eren, H. (author), Bednarz, Roland Jan Reiner (author), Alimoradi Jazi, M. (author), Donk, Laura (author), Gudjónsdóttir, S. (author), Bohländer, P.R. (author), Eelkema, R. (author), Houtepen, A.J. (author)Quantum dots (QDs) are considered for devices like light-emitting diodes (LEDs) and photodetectors as a result of their tunable optoelectronic properties. To utilize the full potential of QDs for optoelectronic applications, control over the charge carrier density is vital. However, controlled electronic doping of these materials has remained...journal article 2022