Transient Substrate‐Induced Catalyst Formation in a Dynamic Molecular Network

Fanlo-Virgós, Hugo; Alba, Andrea‐Nekane R.; Hamieh, Saleh; Colomb-Delsuc, Mathieu; Otto, Sijbren

doi:10.1002/ange.201403480

Cited by 28 publications

(4 citation statements)

References 99 publications

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“…Such systems have properties that are more similar to living systems and are expected to offer new applications in the field of materials and nanotechnology 12 . Examples of dissipative self-assembled systems 13 14 15 , transient catalysts 16 , molecular transport systems 17 and molecular motors 18 19 20 are emerging.…”

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confidence: 99%

Transient signal generation in a self-assembled nanosystem fueled by ATP

2015

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A fundamental difference exists in the way signal generation is dealt with in natural and synthetic systems. While nature uses the transient activation of signalling pathways to regulate all cellular functions, chemists rely on sensory devices that convert the presence of an analyte into a steady output signal. The development of chemical systems that bear a closer analogy to living ones (that is, require energy for functioning, are transient in nature and operate out-of-equilibrium) requires a paradigm shift in the design of such systems. Here we report a straightforward strategy that enables transient signal generation in a self-assembled system and show that it can be used to mimic key features of natural signalling pathways, which are control over the output signal intensity and decay rate, the concentration-dependent activation of different signalling pathways and the transient downregulation of catalytic activity. Overall, the reported methodology provides temporal control over supramolecular processes.

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confidence: 99%

Transient signal generation in a self-assembled nanosystem fueled by ATP

2015

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“…Otto's group has discovered that the transition state of a reaction can be associated with and stabilized by a dynamic molecular network. Interestingly after the reaction was completed, the catalyst was disassembled, opening up new opportunities for controlling catalysis in synthetic chemical systems [104]. Tiefenbacher et al successfully used a supramolecular pocket to mimic cyclase enzymes and achieved a catalytic non-stop tail-to-head terpene with geranyl acetate as the substrate.…”

Section: Enzyme-like Materials Supramolecular Catalysismentioning

confidence: 99%

Emerging functional materials based on chemically designed molecular recognition

Chen

Tian

et al. 2020

BMC Mat

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The specific interactions responsible for molecular recognition play a crucial role in the fundamental functions of biological systems. Mimicking these interactions remains one of the overriding challenges for advances in both fundamental research in biochemistry and applications in material science. However, current molecular recognition systems based on host-guest supramolecular chemistry rely on familiar platforms (e.g., cyclodextrins, crown ethers, cucurbiturils, calixarenes, etc.) for orienting functionality. These platforms limit the opportunity for diversification of function, especially considering the vast demands in modern material science. Rational design of novel receptor-like systems for both biological and chemical recognition is important for the development of diverse functional materials. In this review, we focus on recent progress in chemically designed molecular recognition and their applications in material science. After a brief introduction to representative strategies, we describe selected advances in these emerging fields. The developed functional materials with dynamic properties including molecular assembly, enzymelike and bio-recognition abilities are highlighted. We have also selected materials with dynamic properties in contract to traditional supramolecular host-guest systems. Finally, the current limitations and some future trends of these systems are discussed.

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“…[29,32] Besides molecular machines, [28,[33][34][35][36][37] examples in this area are essentially limited to few deracemizations [38][39][40] and mostly individual cases of dynamic-covalent reactions. [18,[41][42][43][44][45] Usually, such systems exploit a templating agent that is removed to afford a metastable distribution. [42][43][44] In a recent example of this type, a hydrazone with catalytic properties could be over-accumulated (from 47% to 83%).…”

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confidence: 99%

Endergonic synthesis of Diels-Alder adducts enables non-equilibrium adaptive behaviors in chemical reaction networks

Al Shehimy,

Le,

Di Noja

et al. 2024

Preprint

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The overwhelming majority of artificial chemical reaction networks respond to stimuli relaxing towards an equilibrium state. The opposite response – moving away from equilibrium – can afford the endergonic synthesis of molecules, of which only rare examples have been reported. Here, we report six examples of Diels-Alder adducts accumulated in an endergonic process and use this strategy to realize adaptive phenomena. Indeed, systems respond to repeated occurrences of the same stimulus by increasing the amount of adduct formed, with the final network distribution depending on the number and frequency of stimuli received. Our findings indicate how endergonic processes can contribute to the transition from responsive to adaptive systems.

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Transient Substrate‐Induced Catalyst Formation in a Dynamic Molecular Network

Cited by 28 publications

References 99 publications

Transient signal generation in a self-assembled nanosystem fueled by ATP

Transient signal generation in a self-assembled nanosystem fueled by ATP

Emerging functional materials based on chemically designed molecular recognition

Endergonic synthesis of Diels-Alder adducts enables non-equilibrium adaptive behaviors in chemical reaction networks

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