溶剂-溶质间协同竞争的物理化学耦合作用机制、调控及天然气脱硫溶剂分子组成智能化设计

加快天然气资源安全、优质、高效开发是构建“清洁低碳、安全高效”能源体系的重要途径。传统基于组分实验筛选及调配的脱硫溶剂研发已不能适应天然气开发需求，亟需发展智能化的溶剂组成设计方法。本课题拟通过计算模拟与多技术实验表征相结合研究并阐明溶剂与天然气组分间协同竞争的物理化学耦合作用机制，探索溶剂-溶质间交互作用的定向调控方法；采用COSMO-RS计算与实验相结合的方法获取溶解度参数，并建立溶解度参数与溶剂分子结构向量间QSAR模型；同时构建基于结构向量的溶剂溶质分子矩阵，利用Ab initio计算与实验相结合获取反应速率常数，并建立基于结构向量的溶剂-溶质分子间反应网络和动力学模型；进一步将反应网络与QSAR模型耦合，构建响应原料硫化物分布特征的智能化溶剂分子组成设计策略。为高效选择性脱硫溶剂设计开发发展新的研究思路和高效方法，同时拓展溶剂-溶质分子间复杂交互作用及硫化物选择性吸收的基础理论。

Expediting the exploration of natural gas resource on a high safety, quality and efficiency level is a very important approach to building a Clean, Low-Carbon, Safe and Effective energy system. Traditionally, desulfurization solvents were developed by means of experimental screening as well as blending of components. However, such strategy cannot meet the requirement of natural gas exploration. There is an urgent need to explore an intelligent method for molecular composition design of solvent. This project is focused on mechanism of cooperative-competitive physical and chemical interplay between solvent and natural gas components by using simulation method coupled with multiple characterization techniques. The solvent-solute interplay is also expected to be regulated in present research proposal. By means of modeling calculation using COSMO-RS model coupled with experimental measurement, solubility parameters will be observed and a QSAR model can be established between solubility parameters and structural vectors of solvent molecules. In addition, applying Ab initio calculation assisted with experimental investigation, rate constants with respect to various reactions between solute and solvent molecules can be derived. Then a reaction network as well as its kinetics model can be obtained. Furthermore, the reaction network and the QSAR model will be combined to build an intelligent molecular composition design strategy for solvent development, which responds to the composition changes of the sulfides in raw materials. Such research not only provides a new and efficient approach to the molecular design and development of desulfurization solvent but also enriches the basic theory behind the complex interplay involved in solvent-solute systems.