电化学还原CO2合成碳酸二甲酯所用关键电极材料及反应机理的研究

Dimethyl carbonate (DMC) has been paid much attention, because DMC is an environmentally benign chemical production. In recently years, the direct synthesis of DMC from CO2 by electrochemistry is the more preferred route as it matches the view of the ―Sustainable Society‖ and ―Green Chemistry‖. But the activation of the CO2 is the key problem, and thus there is an urgent need to identify new materials for CO2 reduction. Our initial is to explore modification of the new materials and some work will be studied, as follows: 1. The solid solutions will be prepared by complex-decomposition method using organic acids as precursors. The solid solutions will be used in CO2 electrochemical reduction synthesis of DMC. Combined with the characterization results by means of XRD, Raman, SEM, the relationships between the catalytic activities and DMC yields will be discussed. 2. In order to enhance the catalytic activity, the solid solutions will be modified by adding graphene, the relationships between the catalytic activities and DMC yields will be also studied.3. The mechanism for the electrochemical reduction of CO2 synthesis of DMC will be investigated.

碳酸二甲酯(DMC)作为一种绿色化学品，近年来受到广泛的关注。目前DMC的合成路线正朝着简单化、无毒化和无污染化的方向发展，电化学还原CO2合成DMC的路线越来越受到关注。但是该合成路线的关键问题是CO2不易活化,寻找新的高活性电极材料刻不容缓。本项目以化学反应中高效催化剂为先导，拟重点进行下列研究：1.以有机酸为配位剂，硝酸盐为前躯体，采用配位-分解法制备催化剂固溶体。通过XRD、Raman、SEM等方法对固溶体的孔型结构、比表面积以及对CO2的化学吸附性能和电化学还原催化性能等进行考察，并还原CO2直接合成DMC，将固溶体的性能与其结构的关系进行关联和解析。2.为了提高电极材料的催化活性，对制备的催化剂进行了改性，加入导电性能好、比表面积大的石墨烯，并对其催化合成DMC的性能进行探讨。3.推测电极材料催化还原CO2合成DMC的反应机理

近几年来，CO2的固定转化一直是一个研究的热点问题。CO2作为一种可以循环使用的碳资源，可以用多种方法进行固定转化，其中电化学方法是一种比较有应用前景的方法。电极是电化学固定CO2的关键材料，对CO2的催化转化起着至关重要的作用。因此本项目制备了在温和条件下对CO2的电化学还原有良好催化活性的铜，银系列的阴极材料；结合新型材料的表征方法和电催化CO2合成碳酸二甲酯的结果，获得高效稳定的纳米铜、银催化材料；阐明材料微观形貌与电催化CO2还原性能之间的相关性；从微观层面上认识表面效应、界面效应等对电催化CO2还原的作用。为拓展CO2的资源化利用体系和新型高效电催化材料的设计制备奠定理论基础。