微流控-核磁-微区光谱方法研究耗散分子组装体系相分离过程的物理化学机制

Dissipative molecular assembly system far away from thermodynamic equilibrium is one of the frontiers in the molecular assembly area, and study of their physical-chemical mechanisms are challenging, especially in the construction of dissipative systems and in-situ high-resolution characterization. This project will take the liquid-liquid phase separation (LLPS) process of the dissipative chemical reaction networks as a model system, and apply micro-fluidic NMR and microscopic spectrometer to characterize the LLPS process and systematically study its physical-chemical mechanism. The dissipative molecular assembly system will be constructed on microfluidic chips and maintain its dissipative state by injecting chemical fuel into the system through the tubes in microfluidic chips. High-resolution NMR spectra will be taken in-situ to reveal the structure, concentration and kinetic process of each component during the phase separation process. Finally, by applying the theory of non-equilibrium, non-linear thermodynamics and kinetics, we'll establish the physical-chemical model and mechanisms of the LLPS process. The project will provide a novel approach towards constructing and characterizing artificial dissipative molecular assembly systems and their physical-chemical study and will contribute to the study of LLPS process in biology.

远离平衡态的耗散态分子组装体系是分子组装领域前沿，其物理化学机制研究难度极大，难点在于耗散分子组装体系的构建及其原位、高分辨表征。本课题拟采用耗散态化学反应网络中的液-液相分离作为模型体系，采用微流控-核磁和微区光谱技术表征相分离过程，系统研究其物理化学机制。在微流控芯片上原位构建耗散分子组装体系，通过注入能量（燃料分子或光）维持体系在耗散态，并采集高分辨核磁共振谱获得相分离过程中组分的种类、含量及动力学过程等关键信息。此外，耗散体系与溶液中传质过程、浓度梯度等因素密切相关，采用微区光谱技术可获得相分离过程中不同空间位点的反应信息。最终结合非平衡态非线性热力学和动力学理论建立相分离过程的物理化学模型，阐明相分离机制。本课题为构建和表征人工耗散态体系及其物理化学研究提供新思路，对阐明生物相分离机理具重要意义。

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