<i>De novo</i>Design of Chemical Reaction Networks and Oscillators and Their Relation to Emergent Properties

Semenov, Sergey N.

doi:10.1002/9783527821990.ch4

Out‐of‐Equilibrium (Supra)molecular Systems and Materials 2021

DOI: 10.1002/9783527821990.ch4

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De novoDesign of Chemical Reaction Networks and Oscillators and Their Relation to Emergent Properties

Sergey N. Semenov

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2024

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Cited by 5 publications

(1 citation statement)

References 175 publications

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“…The design of our system follows an established principle for chemical oscillators: a combination of a positive and negative feedback loop(s) leads to alternating growth and decay phases, giving rise to oscillations 6,31,32 . We chose to base our system on autocatalytic Fmoc deprotection (Fig.…”

mentioning

confidence: 99%

A catalytically active oscillator made from small organic molecules

ter Harmsel,

Maguire,

Runikhina

et al. 2023

Nature

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Oscillatory systems regulate many biological processes, including key cellular functions such as metabolism and cell division, as well as larger-scale processes such as circadian rhythm and heartbeat1–4. Abiotic chemical oscillations, discovered originally in inorganic systems5,6, inspired the development of various synthetic oscillators for application as autonomous time-keeping systems in analytical chemistry, materials chemistry and the biomedical field7–17. Expanding their role beyond that of a pacemaker by having synthetic chemical oscillators periodically drive a secondary function would turn them into significantly more powerful tools. However, this is not trivial because the participation of components of the oscillator in the secondary function might jeopardize its time-keeping ability. We now report a small molecule oscillator that can catalyse an independent chemical reaction in situ without impairing its oscillating properties. In a flow system, the concentration of the catalytically active product of the oscillator shows sustained oscillations and the catalysed reaction is accelerated only during concentration peaks. Augmentation of synthetic oscillators with periodic catalytic action allows the construction of complex systems that, in the future, may benefit applications in automated synthesis, systems and polymerization chemistry and periodic drug delivery.

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confidence: 99%

A catalytically active oscillator made from small organic molecules

ter Harmsel,

Maguire,

Runikhina

et al. 2023

Nature

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Reduction‐Induced Self‐Propelled Oscillatory Motion of Perylenediimides on Water

Holstein,

Suematsu,

Takeuchi

et al. 2024

Angewandte Chemie

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The emergence of macroscopic self‐propelled oscillatory motion based on molecular design has attracted continual attention in relation to autonomous systems in living organisms. Herein, a series of perylenediimides (PDIs) with various imide side chains was prepared to explore the impact of molecular design and alignment on the self‐propelled motion at the air–water interface. When placed on an aqueous solution containing a reductant, a solid disk of neutral PDI was reduced to form the water soluble, surface‐active PDI dianion species, which induces a surface tension gradient in the vicinity of the disk for self‐propelled motion. We found that centimeter‐scale oscillatory motion could be elicited by controlling the supply rate of PDI dianion species through the reductant concentration and the structure of imide side chains. Furthermore, we found that the onset and speed of the self‐propelled motion could be changed by the crystallinity of PDI at the water surface. This design principle using π‐conjugated molecules and their self‐assemblies could advance self‐propelled, non‐equilibrium systems powered by chemical energy.

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Reduction‐Induced Self‐Propelled Oscillatory Motion of Perylenediimides on Water

Holstein,

Suematsu,

Takeuchi

et al. 2024

Angew Chem Int Ed

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De novoDesign of Chemical Reaction Networks and Oscillators and Their Relation to Emergent Properties

Cited by 5 publications

References 175 publications

A catalytically active oscillator made from small organic molecules

A catalytically active oscillator made from small organic molecules

Reduction‐Induced Self‐Propelled Oscillatory Motion of Perylenediimides on Water

Reduction‐Induced Self‐Propelled Oscillatory Motion of Perylenediimides on Water

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