二氧化碳电催化还原与矿化发电高效耦合研究

One of the major environmental concerns is how to decrease the content of carbon dioxide (CO2) in the atmosphere because of its greenhouse effect. Meanwhile, CO2, the most abundant carbon source on earth may be utilized and recycled into useful carbon-containing fuels, such as methane, formic acid, methanol and so on via the reduction reaction of CO2 (CO2RR). It is meaningful to recycle and utilize the CO2 for the mitigation of environmental problems, alleviating energy crisis and recycling of carbon resources. By selecting and modifying of catalysts, we have improved the catalyst performance for CO2RR to small fuel molecules and in the meantime carried out the reaction mechanism by some preliminary researches earlier. However, CO2RR is not the net emission reduction of CO2 because it needs the external energy to drive the overall reaction. On this basis, this project aims to effectively couple CO2 mineralization power generation with electrocatalytic CO2RR. On the one hand, as a resource, CO2 can be transformed into high-value-added sodium bicarbonate solid through the mineralization power generation process. On the other hand, CO2 can act as a kind of green energy. The low-phase energy generated by CO2 mineralization power generation can be used into the process of CO2RR, which makes it effective to obtain carbon-containing fuels, thus storing it at a high energy level. Finally, the high-efficiency coupling technology of recycling and utilization of CO2 can be obtained. The implementation of this project is expected to realize the integration of recycling and utilization of CO2, treat wastes with processes of wastes against one another and turn wastes into treasures, lay a theoretical and practical foundation for the subsequent researches on emission reduction and reuse of CO2 .

作为主要的温室气体，CO2排放量的快速增加带来了严重的环境问题。CO2减排和再利用对减轻环境问题、缓解能源危机以及碳资源的循环利用具有重要的意义。前期，我们通过对催化剂的筛选和改性，提升了催化剂催化CO2还原到小分子燃料的性能，并对其反应机理进行了初步的研究，但将CO2还原成含碳小分子燃料需从外部获取能量，无法单纯地实现CO2的净减排。在此基础上，本项目拟将CO2矿化发电与电催化CO2还原高效耦合，将CO2同时作为一种资源和能源。一方面通过矿化发电过程将其转变为高附加值的碳酸氢钠固体；另一方面将矿化发电产生的低位电能用于电催化CO2还原，有效地将CO2转化为高能位、可储存的含碳化学燃料，最终形成CO2资源化、能源化利用的高效耦合方法与技术。本项目的实施，可将CO2资源化和能源化整合，实现以废治废、变废为宝，为后续CO2的减排和再利用提供技术支持和经验借鉴。

二氧化碳（CO2）是主要的温室气体，同时也是地球上最丰富的碳资源，将CO2催化还原成含碳小分子燃料，如甲烷、甲酸和甲醇等，对CO2的回收和循环利用具有重要的意义。本项目的工作以电催化CO2还原（CO2RR）为研究目标，以电化学、原位表面增强红外光谱为主要手段，结合材料的制备与表征、反应产物分析，以及DFT计算等，研究电催化材料的组成与结构对CO2RR的反应活性与产物选择性的影响，并探讨相关的CO2RR反应可能的机制和吸附中间体。具体的工作有：成功研究和开发了铂（Pt）类新型电催化剂；构建金属-氧化物界面能够有效提升催化剂的催化性和选择性，成功设计合成了银（Ag）基-氧化物异质结构催化剂，将其应用在电化学二氧化碳还原的体系中；建立了电化学催化CO2还原与原位红外谱学的联用技术，用以研究CO2RR过程中的反应机理。以第一/通讯作者发表标注了该项目的SCI论文4篇，其中ACS Catal.一篇，ACS Appl. Mater. Interfaces一篇，Nano Res.一篇，Chem. Asian J一篇，参加学术会议三次。