Understanding the CO2 reduction mechanism over CoCu-based catalyst by combined theoretical and experimental studies

大气中CO2浓度的增加导致了包括全球气候变化和海洋酸化在内的严重问题，这两个问题都被认为是对人类社会的严重威胁。因此，如何有效利用二氧化碳成为研究的热点。本研究的重点是CO2加氢合成低碳醇合成催化剂的开发。该提案将采用一个渐进的研究计划，从研究反应机理，到计算辅助催化剂筛选，以及实验合成和催化行为的评价。通过系统地发展和部署密度泛函理论计算、从头算热力学分析、全局结构优化策略、表面科学技术、各种线性标度关系，将确定CoCu合金的结构、合金/氧化物界面和相应的活性中心，指导理论预测的潜在催化剂的合成。该项目的成功实施将加深对CO2加氢反应的认识，为催化剂的设计和改进提供新的指导和依据。

The increasing CO2 concentration in atmosphere has led to serious problems including the global climate change and ocean acidification, both of which are believed to be serious threats to human societies. Therefore, how to effectively utilize CO2 becomes a hot research topic. This proposal focuses on the development of higher alcohol synthesis catalyst from CO2 hydrogenation. A progressive research plan, from a study of the reaction mechanism, to computational aided catalyst screening as well as experimental synthesis and evaluation of the catalytic behavior, will be adapted in the proposal. By systematically developing and deploying density functional theory calculations, ab-initio thermodynamic analysis, global structural optimization strategies, surface science techniques, various linear scaling relationships, the structure of CoCu alloy, alloy/oxide interface and the corresponding active site will be identified, guiding the synthesis of theoretical predicted potential catalysts. The successful execution of this project will provide deep understanding of CO2 hydrogenation reactions and offer new guideline and foundation for catalyst design and improvement.