CO2调控生物来源酸碱参与构筑的酸碱功能化低共熔溶剂研究

The project intends to synthesis biocompatible acid/base functional deep eutectic solvents (DESs) by bio-originated acids and alkaloids as structural units, then prepare of environmental benign CO2 switchable DESs by interactions between ambient CO2 and DESs, and further fine regulate properties of DESs by introducing high pressure CO2. Moreover, systematic and thorough investigations on the system will be carried out to clarify the relationship between the molecular structure and physiochemical properties of DESs, the effect of CO2 temperature and pressure, and further to reveal the intrinsic molecular mechanism of DESs systems. Last but not the least, the interactions between CO2 and DESs with tailorable properties will be used for irreversible sequestration, activation and catalytic transformation of CO2 into energy and chemicals..This project will expand the scope of DESs, deepen the insights into the relationship between the structure and the properties of DESs and provide scientific base for preparation of cheap, environmental benign, biocompatible DESs with regulated properties and specific functions. Based on the above researches, the potential applications of DESs on sequestration, activation and catalytic transformation of CO2 will be explored, which can provide new ideas to solve the energy and environmental issues, promote the sustainable development of human society.

本项目拟采用生物来源的酸和生物碱作为结构单元，构筑生物相容的酸碱功能化低共熔溶剂（DESs）；然后利用常压CO2与DESs相互作用，获得环境友好、性质可调控的CO2开关型DESs；并进一步利用高压CO2的压力和温度精确调控DESs体系的性质。此外，系统深入的研究所构筑体系，阐明构筑单元、DESs物化性质、CO2温度压力之间关系的规律性，揭示产生规律性的内在分子作用机制。最后，探索基于性质可调控的DESs与CO2之间的作用可逆分离CO2和CO2的相关能源化学品的催化转化。.本项目的研究工作将拓展DESs的研究范围，加深人们对DESs结构和性质之间规律性认识，为构筑便宜、环境友好、生物相容、性质可调控的具有特定功能的DESs提供科学依据，探索DESs在CO2捕集分离和活化转化中的应用，为解决能源和环境方面问题提供新思路，推动人类社会的可持续发展。

2003年，Abbott等人命名低共熔溶剂（简称DESs）。DESs便宜易得和绿色，被称为“21世纪的溶剂”。用具有酸碱性的生物质参与构筑具备生物相容、环境友好、便宜易得、性质可控的酸碱功能化DESs，能加深对于DESs的科学认识，为更有效的设计和应用功能化DESs提供科学依据，促进人类社会的可持续发展。.主要研究内容、重要结果、关键数据如下：.形成了基于有机碱和硫脲的准DESs，通用溶剂，可以用于溶解金属，金属硫化物和金属氧化物，包括CoO，NiO，CuS，Fe，W，Cu和V2VI3硫属元素化物（Green Chem., 2018, 20, 5266-5270）。形成了Brønsted酸性DESs，用于溶解稀土氧化物（Green Chem., 2019, 21, 4748-4756）。扩大了绿色溶剂的范围，并对低温电解和溶液加工进行了改进。用二维相关红外光谱技术系统研究了DESs的吸水性（PCCP, 2019, 21, 2601-2610.），揭示了超碱衍生的DESs用于二氧化碳捕集的高度挥发性（PCCP, 2021, 23, 2193-2210；研究了DESs的传输性质，并用Walden plot方法以及脉冲场核磁共振技术研究了DESs的离子度（PCCP, 2020, 22, 25760-25768）。受邀在Chem Soc Rev（2021, 50, 8596-8638）上发表了题为Eutectics: formation, properties, and applications的综述。在Green Chem（2021, 23, 4228–4254）上发表关于5羟甲基糠醛电化学转化的综述。