双原子催化剂中金属原子协同作用的理论研究

To reduce the metal usage in catalysis and enhance the catalytic efficiency, the single-atom catalysts (SACs) have become a hot topic in recent years. The single-atom catalyst contains only isolated individual atoms dispersed on, and/or coordinated with, the surface atoms of an appropriate support, which maximizes the metal atom efficiency. So far, various SACs have been successfully fabricated, and are highly active for a variety of catalytic reactions. It is also notable that metal-metal bonds play a very important role in catalysis. In this project, by employing density functional theory we will search highly effective, low-cost, and environmental beginning bi-atom catalysts with high-throughput calculations. We first find the suitable two-dimensional nanomaterials to anchor the metal dimer, and explore the stability and electronic properties of the heterogeneous catalysts. Next we study the catalytic mechanism of these bi-atom catalysts for a few reactions. Then by comparing the catalytic performance of the bi-atom catalysts with their monometallic counterparts, we discuss the cooperative effects of the metal dimers on the activity and selectivity of a catalytic reaction. Finally, we examine the catalytic activity of the bi-atom catalysts by tuning the organic groups of the two-dimensional supports. This project not only spans the single-atom catalysts, but also provides insights and guidelines to experimentalists and promotes the design and production in novel nanocatalysts.

近年来，为降低金属在催化领域中的使用量、提高催化效率，单原子催化剂逐渐成为研究的热点。在单原子催化中，负载的每个孤立的金属原子作为催化剂的活性位点，可以使得金属的利用率最大化。目前已有多种单原子催化剂被合成出来，它们在多种反应中表现出很高的催化活性。需要注意的是，除了金属原子本身，金属-金属键在催化反应中也起到重要的作用。基于此，本项目拟将双金属原子团簇稳定地负载在合适的二维材料上，采用密度泛函理论方法通过高通量计算筛选高效催化剂，对比双金属原子和单金属原子的催化活性，考察金属原子 (同核和异核) 间的协同作用 (电子耦合、电负性差、金属键极性等) 及载体有机官能团对双原子催化剂反应活性和选择性的影响。该研究扩展了单原子催化的设计理念，将为实验上寻找高效、低廉、清洁的双原子催化剂提供重要的借鉴和指导。

近年来，为降低金属在催化领域中的使用量、提高催化效率，单原子催化剂逐渐成为研究的热点。在单原子催化中，负载的每个孤立的金属原子作为催化剂的活性位点，可以使得金属的利用率最大化。目前已有多种单原子催化剂被合成出来，并且这类催化剂在多种反应中具有很高的催化活性。另一方面，金属-金属键在催化反应中起着重要的作用。本项目采用密度泛函理论方法将双金属原子团簇稳定地负载在具有合适孔洞的二维材料上，通过高通量计算筛选高效催化剂，对比双金属原子和单金属原子的催化活性，考察了金属原子(同核和异核)间的协同作用对反应活性的影响。上述研究成果一定程度上扩展了单原子催化的设计理念，探索了金属原子间的协同效应与反应活性的关联，为实验工作者寻找高效、低廉、清洁的双原子金属团簇催化剂提供借鉴和指导。通过本项目的研究，发表SCI论文8篇，其中发表在Small Methods、ACS Applied Materials & Interfaces、Nanoscale和Applied Surface Science各一篇，发表论文最高影响因子12.13，单篇最高引用67次，被科学媒介报道两次。项目组举办线上会议1次，参加各相关领域国内外学术会议16次和学术访问1次，并作邀请/口头报告8次、墙报展示2次。

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