Signaling in Systems Chemistry: Programing Gold Nanoparticles Formation and Assembly Using a Dynamic Bistable Network

Maity, Indrajit; Dev, Dharm; Basu, Kingshuk; Wagner, Nathaniel; Ashkenasy, Gonen

doi:10.1002/ange.202012837

Cited by 5 publications

(1 citation statement)

References 67 publications

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“…These networks rely on autocatalytic chemical reaction systems, which, in turn, rely on highly evolved enzymes. Non-enzymatic reaction networks that display bistability also exist but rely on autocatalytic reactions, which are rare and hard to design [12][13][14][15][16][17][18][19][20][21][22] . Thus, designing more generalizable methods of creating bistability would be a milestone towards autonomous, evolving systems that can store memory of past events.…”

Section: Introductionmentioning

confidence: 99%

Memory, switches, and logic gates through bistability in chemically fueled crystals

Schnitter¹,

Rieß²,

Boekhoven³

2021

Preprint

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The ability to store information in chemical reaction networks is essential for evolution, calculations, and, more generally, for the complex behavior, we associate with life. In biology, cellular memory is regulated through transcriptional states that are bistable, i.e., a state that can either be on or off and can be flipped from one to another through a transient signal. Such memory circuits have been realized synthetically through the rewiring of genetic systems in vivo or through the rational design of reaction networks based on DNA and highly evolved enzymes in vitro. Completely bottom-up analogs based on small molecules are rare and hard to design and thus represent a challenge for systems chemistry. In this work, we show that bistability can be designed from an extremely simple non-equilibrium reaction cycle that is coupled to crystallization. The crystals exert the necessary feedback on the reaction cycle required for the bistability resulting in an on-state with assemblies and an off-state without. We can switch the state on and off, such that each state represents volatile memory that can be stored in continuously stirred tank reactors indefinitely despite the fact that molecules are turned over on a minute-timescale. We showcase the system’s abilities by creating a matrix display that can store images and by performing Boolean logic by coupling several switches together.

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Section: Introductionmentioning

confidence: 99%

Memory, switches, and logic gates through bistability in chemically fueled crystals

Schnitter¹,

Rieß²,

Boekhoven³

2021

Preprint

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Feedback and Communication in Active Hydrogel Spheres with pH Fronts: Facile Approaches to Grow Soft Hydrogel Structures

et al. 2021

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Compartmentalized reaction networks regulating signal processing, communication and pattern formation are central to living systems. Towards achieving life‐like materials, we compartmentalized urea‐urease and more complex urea‐urease/ester‐esterase pH‐feedback reaction networks into hydrogel spheres and investigate how fuel‐driven pH fronts can be sent out from these spheres and regulated by internal reaction networks. Membrane characteristics are installed by covering urease spheres with responsive hydrogel shells. We then encapsulate the two networks (urea‐urease and ester‐esterase) separately into different hydrogel spheres to devise communication, pattern formation and attraction. Moreover, these pH fronts and patterns can be used for self‐growing hydrogels, and for developing complex geometries from non‐injectable hydrogels without 3D printing tools. This study opens possibilities for compartmentalized feedback reactions and their use in next generation materials fabrication.

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Fluorescent Microswimmers Based on Cross‐β Amyloid Nanotubes and Divergent Cascade Networks

Chatterjee

Ghosh

et al. 2022

Angewandte Chemie

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Shaped through millions of years of evolution, the spatial localization of multiple enzymes in living cells employs extensive cascade reactions to enable highly coordinated multimodal functions. Herein, by utilizing a complex divergent cascade, we exploit the catalytic potential as well as templating abilities of streamlined cross‐β amyloid nanotubes to yield two orthogonal roles simultaneously. The short peptide based paracrystalline nanotube surfaces demonstrated the generation of fluorescence signals within entangled networks loaded with alcohol dehydrogenase (ADH). The nanotubular morphologies were further used to generate cascade‐driven microscopic motility through surface entrapment of sarcosine oxidase (SOX) and catalase (Cat). Moreover, a divergent cascade network was initiated by upstream catalysis of the substrate molecules through the surface mutation of catalytic moieties. Notably, the resultant downstream products led to the generation of motile fluorescent microswimmers by utilizing the two sets of orthogonal properties and, thus, mimicked the complex cascade‐mediated functionalities of extant biology.

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Signaling in Systems Chemistry: Programing Gold Nanoparticles Formation and Assembly Using a Dynamic Bistable Network

Cited by 5 publications

References 67 publications

Memory, switches, and logic gates through bistability in chemically fueled crystals

Memory, switches, and logic gates through bistability in chemically fueled crystals

Feedback and Communication in Active Hydrogel Spheres with pH Fronts: Facile Approaches to Grow Soft Hydrogel Structures

Fluorescent Microswimmers Based on Cross‐β Amyloid Nanotubes and Divergent Cascade Networks

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