ABSTRACT

Formic acid is a liquid organic hydrogen carrier. Metal and metal-complex catalysts are known to catalyze the hydrogen production from formic acid and hydrogen transfer reactions with formic acid as a hydrogen donor. In this review, we will show that heterogeneous catalysts with single metal atoms are promising for these reactions. The main emphasis is done to the catalysts with single atoms stabilized by pyridinic nitrogen atoms on the edge or vacancy sites of graphene sheets. The activity of the catalysts containing these sites often exceeds that of the catalysts with nanoparticles. We consider application of different physical methods and density functional theory calculations to establish the nature of single-atom active sites and reaction mechanism. Coordination of these sites significantly affects their performance in the mentioned reactions. This review could be useful for development of novel efficient catalysts.

摘要

甲酸是一种液态有机氢载体。已知金属和金属络合物催化剂可催化甲酸制氢和以甲酸作为氢供体的氢转移反应。在这篇综述中，我们将展示具有单金属原子的非均相催化剂对这些反应很有前景。主要重点是单原子由石墨烯片边缘或空位上的吡啶氮原子稳定的催化剂。包含这些位点的催化剂的活性通常超过具有纳米颗粒的催化剂的活性。我们考虑应用不同的物理方法和密度泛函理论计算来确定单原子活性位点的性质和反应机理。这些位点的协调显着影响它们在上述反应中的表现。