基于界面溶剂微结构的限域气体溶解扩散机制的研究

由氢氧直接合成双氧水的绿色技术有望取代传统会分解生成有毒副产物的蒽醌法合成工艺，对实现绿色化工过程具有重要意义。利用多孔膜作为气体分布器，精确调控气体的增溶与传质，建立溶解扩散-反应动态平衡，有望解决双氧水直接合成过程中副反应与安全性等问题。然而限域溶剂环境中气体溶解扩散机制尚不清楚，严重制约了该技术在工业应用方面的发展。本项目拟在申请者对界面流体微结构丰富研究经验的基础上，创新地提出以界面溶剂特征微结构为切入点，以分子模拟为主结合微观实验，分析限域溶剂环境中气体溶解扩散性能的影响因素。项目预期将揭示限域溶剂环境中气体促溶性能对膜孔道尺寸、界面性质、溶剂种类等的响应规律，从分子层面深化对界面溶剂微结构与气体溶解扩散机制内在联系的理解，构建具有预测功能的气体限域传质模型，为双氧水高效安全制备的颠覆性技术的开发提供基础数据和理论依据。

The green technology of direct synthesis of hydrogen peroxide from hydrogen and oxygen is expected to replace the traditional anthraquinone synthesis process which can decompose into toxic by-products. It is of great significance to the realization of green chemical engineering. Using porous membrane as gas distributor can accurately control the solubilization and mass transfer of gas, and establish the dynamic balance between solution-diffusion and reaction, which is expected to solve the problems of side reaction and safety in the process of hydrogen peroxide direct synthesis. However, the mechanism of gas solution and diffusion in confined solvent environment is still unclear, which seriously restricts the development of this technology in industrial application. On the basis of our previous systematical investigations of the interfacial fluid microstructure, the innovation of this project is to focus on the interfacial fluid microstructure and treat it as an essential cutting-in point to understand the nanoconfined gas solution-diffusion mechanism in confined solvent. With the combination of molecular simulation and micro-experiment techniques, this study aims to shed light on the responses of gas solution and diffusion in confined solvent to membrane pore size, interfacial properties and solvent types, and deepen the understanding of the internal relationship between interfacial solvent microstructure and gas solution-diffusion mechanism from the molecular level. Moreover, a prediction gas confined mass transfer model will be constructed to provide basic data and theoretical basis for the development of subversive technology for the efficient and safe preparation of hydrogen peroxide.