多酸-金属铜纳米复合电催化剂的设计合成及其在二氧化碳还原中的应用

Carbon dioxide conversion into higher value-added products products provides a fantastic strategy to mitigate global warming and to simultaneously store renewable energy as chemical bonds. Electroreduction of CO2 working with catalysts which possess high activity, unique selectivity and long-term stability plays important role in this domain. However, the design and synthesis of required electro-catalysts or even multiple devices remain huge challenge. The search of new materials that can convert CO2 into value-added multicarbon products thus addressing the problem of carbon dioxide that accumulates into atmosphere is proposed in this project. CO2 conversion will be achieved via the electrochemical reduction of CO2 and original catalysts containing copper nanoparticles (NPs) and polyoxometalates (POMs). Copper as electrocatalysts, its catalysis selectivity will be tuned by polyoxometalates. POMs are green chemicals composed of polyanion clusters with oxometal polyhedra as basic construction units. In this project, several POMs will be used to modify the local electronic and protonic environment of Cu NPs to obtain a catalyst that converts completely CO2 into hydrocarbons. A cutting-edge technology (i.e. Differential Electrochemical Mass Spectrometry) will be exploited for the real-time analysis of reaction intermediates and products, hence giving insights about the reaction mechanism. In conclusion, the project is based on the philosophy of converting a pollutant gas into a form of energy (hydrocarbons) by using novel green chemicals and being supported by a high-standard technology. It will promote the application of polyoxometalate in the field of electrocatalysis and promote the development of controlled carbon dioxide reduction chemistry.

二氧化碳转化为高附加值产品可以减轻温室效应并同时实现可再生能源的化学储存，具有重要的环境和能源意义。借助于催化剂的电催化二氧化碳还原具有高反应活性，独特的产品选择性和长时间稳定性的优点在该领域起到了至关重要的作用。然而，设计和合成所需要的电化学催化剂或器件设备仍存在很大的挑战。本项目通过组装一种多酸-铜金属纳米复合材料作为催化剂，将二氧化碳转化成多碳产物，从而提出一种解决温室气体在大气中积累的策略。铜作为催化剂其催化选择性将通过多酸材料进行调节。多金属氧酸盐是由聚阴离子簇和可作为碱性结构单位的金属氧化物聚多面体中心构成的一种绿色化学品，结构多样和性能优越。本项目中，多种类型的多金属氧酸盐将被应用于合成和改变金属铜纳米材料的局域电子和质子环境，以组建二氧化碳转化为碳氢化合物的催化剂。本项目将促进多酸在电催化领域的应用，推动二氧化碳可控还原化学的发展。