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<p>In biological systems, cells engage in intricate multilevel feedback communication through complex signaling pathway networks, which is a core mechanism for maintaining physiological functions and dynamic balance. However, replicating these complex signaling pathways in artificial systems, particularly achieving intercellular communication across multiple levels and time scales, remains a significant challenge. To address this, we have designed a non-equilibrium polymer nanoreactor system composed of two enzyme-containing polymersomes with distinct functions, aiming to achieve light-controlled multiple feedback chemical communication and self-oscillation. The community comprises photosensitive polymersomes functionalized with photo-responsive donor-acceptor Stenhouse adducts (DASA) containing horseradish peroxidase (HRP) and thioacetylcholine (ATCh), and light-insensitive semipermeable polymersomes loaded with acetylcholinesterase (AChE). Under red light irradiation, the permeability of DASA-polymersomes membrane increases, allowing the 3,3′,5,5′-tetramethylbenzidine (TMB) substrate to interact with the encapsulated enzyme, leading to the generation of the oxidized substrate oxTMB. Meanwhile, the release of the encapsulated ATCh activates the second polymersomes containing AChE, resulting in the production of thiocholine. At this stage, oxTMB with red light absorption capability deactivates the DASA-polymersomes, reducing the concentration of oxTMB. Concurrently, the formation of thiocholine reduces oxTMB back to the colorless TMB, reopening the DASA-polymersomes membrane and reactivating the HRP activity. This multi-feedback mechanism mimics the positive and negative feedback regulation processes commonly observed in cellular signaling, reflecting the complexity and temporal nature of intercellular information exchange. Through temporal and spatial feedback control, our system dynamically regulates catalytic activity at different stages of the reaction, simulating the complex signaling networks and interactions within cells. This approach provides new avenues for the development of more complex artificial cells and nonequilibrium systems, with broad application potential in fields such as biological modeling, primitive cell simulation, and biomimetic medicine.</p>

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Biomimetic vesicle-to-vesicle communication in feedback-controlled polymer nanoreactor system

  • 期刊论文

  • 发表日期：

    2026年5月7日

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  • Xin Liang,
  • Yulian Zhang,
  • Yicun Wang,
  • Jun Xiang,
  • Qiang Yan

摘要

In biological systems, cells engage in intricate multilevel feedback communication through complex signaling pathway networks, which is a core mechanism for maintaining physiological functions and dynamic balance. However, replicating these complex signaling pathways in artificial systems, particularly achieving intercellular communication across multiple levels and time scales, remains a significant challenge. To address this, we have designed a non-equilibrium polymer nanoreactor system composed of two enzyme-containing polymersomes with distinct functions, aiming to achieve light-controlled multiple feedback chemical communication and self-oscillation. The community comprises photosensitive polymersomes functionalized with photo-responsive donor-acceptor Stenhouse adducts (DASA) containing horseradish peroxidase (HRP) and thioacetylcholine (ATCh), and light-insensitive semipermeable polymersomes loaded with acetylcholinesterase (AChE). Under red light irradiation, the permeability of DASA-polymersomes membrane increases, allowing the 3,3′,5,5′-tetramethylbenzidine (TMB) substrate to interact with the encapsulated enzyme, leading to the generation of the oxidized substrate oxTMB. Meanwhile, the release of the encapsulated ATCh activates the second polymersomes containing AChE, resulting in the production of thiocholine. At this stage, oxTMB with red light absorption capability deactivates the DASA-polymersomes, reducing the concentration of oxTMB. Concurrently, the formation of thiocholine reduces oxTMB back to the colorless TMB, reopening the DASA-polymersomes membrane and reactivating the HRP activity. This multi-feedback mechanism mimics the positive and negative feedback regulation processes commonly observed in cellular signaling, reflecting the complexity and temporal nature of intercellular information exchange. Through temporal and spatial feedback control, our system dynamically regulates catalytic activity at different stages of the reaction, simulating the complex signaling networks and interactions within cells. This approach provides new avenues for the development of more complex artificial cells and nonequilibrium systems, with broad application potential in fields such as biological modeling, primitive cell simulation, and biomimetic medicine.