Electrochemical promotion of nano-structured catalysis for green house gas mitigation

提出的研究计划的主要目标是利用电化学促进催化（EPOC）的概念为温室气体减排提供高效和节能的途径。感兴趣的反应是甲烷燃烧和CO2加氢。提出的创新工艺和催化剂设计将消除对高温和高压的需求，并导致更高的转化率和所需的产品选择性，将CO2加氢为C2和C3产品。电促进科学的最新进展，特别是高度分散的纳米结构催化剂的开发和应用，将有助于推进这一项目。EPOC又称非法拉第电化学修饰催化活性（NEMCA），是改善催化过程和推进催化前沿的一个很有前途的概念。这一创新的催化领域旨在以可逆和可控的方式改变催化剂的活性和选择性。EPOC利用固体电解质（离子导电陶瓷）作为催化剂载体。固体电解质中的离子（O2-、H+、Na+、K+、OH-等）以电化学方式供给到催化剂表面，作为促进物质修饰催化剂的电子性质，以达到最佳的催化性能。EPOC提供了一种独特的方法，通过简单地改变催化剂膜的电位，在反应条件下改变催化剂表面的促进剂水平。此外，O2-或H+等促进物质不能通过气体吸附形成，也不容易通过化学方法给药。在各种催化剂-载体体系促进的大量化学反应中已经观察到EPOC。其中包括在各种化学合成领域至关重要的反应系统，包括生产商品和精细化学品以及减少汽车排放。综上所述，电化学促进通过原位提供离子促进剂，消除了对高温高压的需要，为选择性CO2加氢和甲烷燃烧反应开辟了一个全新的视角。本课题将解决电促进科学的主要问题：纳米级分散催化剂与电化学活化的耦合。这一突破将为系统研究促进剂在其他重要技术体系中的作用开辟新的视角，从而为设计高效的催化配方提供一条途径。此外，该项目将有助于更好地了解EPOC过程，并从更一般的角度了解使用助剂的所有催化溶液。

The main objective of the proposed research program is to use the concept of Electrochemical Promotion of Catalysis (EPOC) for efficient and energy-saving routes for green house gas mitigation. The reactions of interests are methane combustion and CO2 hydrogenation. The proposed innovative processes and catalyst design will eliminate the need for high temperature and pressure, as well as lead to higher conversions and desired product selectivity for CO2 hydrogenation to C2 and C3 products. Recent advances in electropromotion science in particular development and application of highly-dispersed nano-structured catalysts will contribute towards advancement of this project. EPOC also known as non-faradaic electrochemical modification of catalytic activity (NEMCA) is a promising concept for improving catalytic processes and advancing the frontiers of catalysis. This innovative area of catalysis aims to modify in-operando both the activity and the selectivity of catalysts, in a reversible and controlled manner. EPOC utilizes solid electrolytes (ionically conducting ceramics) as catalyst support. Ions from solid electrolytes (O2-, H+, Na+, K+, OH-, etc.) are electrochemically supplied to the catalyst surface and act as promoting species to modify the catalyst electronic properties in order to achieve optimal catalytic performance. EPOC provides a unique means of varying promoter levels at the catalyst surface under reaction conditions by simply changing the potential of the catalyst film. Moreover, promoting species such as O2- or H+ cannot be formed via gaseous adsorption and cannot be easily dosed by chemical ways. EPOC has been observed for a large number of chemical reactions promoted by a variety of catalyst-support systems. Those include reaction systems of critical importance in diverse fields of chemical synthesis including the production of commodity and fine chemicals and in the abatement of automotive emissions. In view of the above, Electrochemical Promotion opens an entire new perspective in the selective CO2 hydrogenation and methane combustion reactions by in-situ providing ionic promoters eliminating the need for high temperatures and pressures. The current project will solve the main issue of the electropromotion science: coupling dispersed catalysts at the nanometric scale with electrochemical activation. This breakthrough will open new perspectives for the systematic investigation of the role of promoters in other technological important systems, hence offering a route to design efficient catalytic formulations. In addition, the project will contribute to a better understanding of the EPOC process and, from a more general point of view, of all catalytic solutions using a promoter.