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

拟议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。人们感兴趣的反应是甲烷燃烧和二氧化碳加氢。拟议的创新工艺和催化剂设计将消除对高温和压力的需求，并为二氧化碳加氢生成C2和C3产品带来更高的转化率和所需的产品选择性。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，将有助于推动这一项目的进展。EPOC也被称为非法拉第电催化活性修饰(NEMCA)，是一种很有前途的改进催化过程和推进催化前沿的概念。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使用固体电解质(离子导电陶瓷)作为催化剂载体。来自固体电解质(O2-、H、Na、K、OH-等)的离子它们以电化学方式提供给催化剂表面，并作为促进物种来改变催化剂的电子性质，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膜的电位，在反应条件下改变催化剂表面的助剂水平。此外，O2-或H等促进剂不能通过气体吸附形成，也不容易通过化学方法投加。EPOC已经被观察到在各种催化剂-载体系统促进的大量化学反应中。其中包括在化学合成的各个领域中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尾气排放。有鉴于此，电化学促进通过原位提供离子促进剂而不需要高温和压力，为选择性二氧化碳加氢和甲烷燃烧反应开辟了一个全新的视角。 本项目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助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，从更一般的角度来看，将有助于更好地了解使用促进剂的所有催化解决方案。

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.