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A Closed-Loop Chemical Reaction Network for Autonomous, Dual-Window Temporal Programming From a Single Fuel Pulse.

Yingshuai Zhao1,2, Yuanfeng Zhao1,2, Peng Zhao1,2

  • 1School of Physical Science and Technology & State Key Laboratory of Advanced Medical Materials and Devices, ShanghaiTech University, Shanghai, China.

Angewandte Chemie (International Ed. in English)
|February 25, 2026
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Summary
This summary is machine-generated.

This study presents a chemically fueled reaction network that mimics living systems by converting a single fuel pulse into two distinct gel phases, enabling autonomous, repeatable cycles. This programmable system offers a durable platform for life-like functions.

Keywords:
closed‐loop chemical reactiondisulfidefuel‐driven chemical reaction networksol‐gel transitionsupramolecular self‐assembly

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Area of Science:

  • Chemical Engineering
  • Materials Science
  • Biomimetic Systems

Background:

  • Living systems exhibit complex, multi-phase responses to single stimuli.
  • Existing synthetic systems often lack autonomous, resettable, and programmable temporal control.

Purpose of the Study:

  • To develop a closed-loop chemically fueled reaction network (CRN) that emulates life-like temporal programming.
  • To achieve autonomous, multi-phase responses from a single fuel input with programmable control.

Main Methods:

  • Utilized a CRN based on N-benzoyl-l-cysteine methyl ester-N-methylpiperazine dithiocarbamate (DTC).
  • Employed dithiothreitol (DTT) as the fuel to trigger a sequence of chemical and physical transformations (Sol1 → Gel1 → Sol2 → Gel2 → Sol1).
  • Investigated the role of pH and fuel reducing strength in controlling temporal gating and phase transitions.
  • Combined experimental validation with kinetic modeling to confirm system behavior.

Main Results:

  • Demonstrated a single fuel pulse (DTT) generating two temporally separated gel phases.
  • Achieved autonomous cycling with molecular-level reset over >7 iterations.
  • Showcased programmable temporal windows controlled by pH and fuel properties.
  • Confirmed the hierarchical kinetic landscape's role in temporal gating and loop closure.

Conclusions:

  • Developed a durable, resettable, and programmable platform for life-like dissipative functions.
  • Successfully transitioned fuel-driven materials beyond single-event responses.
  • Established a novel approach coupling closed-loop chemistry with temporal gating for advanced material functions.