Fe is not only the most abundant metal on the planet, but also the key component of many enzymes in organisms that are capable to catalyze many chemical conversions. Mono-dispersed Fe atoms on carbonaceous materials are a kind of single atom catalysts (SACs) that function like enzymes. To tackle the outstanding catalytic performance of Fe based SACs, we extended CO oxidation reaction network over mono-dispersed Fe atoms on graphene (FeGR) by first-principles based calculations. FeGR catalyzed CO oxidation initiates with revised Langmuir–Hinshelwood pathway through CO assisted scission of O-O bond in peroxide species (OCOO). We showed that carbonate species (CO3) that was generally considered as a persistence species blocking reaction sites before may form from CO2 and negatively charge O species. This pathway competes with desorption of CO2 and reduction of Fe center with gaseous CO, and is exothermic and inevitable, especially at low temperatures and with high CO2 content. Though direct dissociation of CO3 is demanding on FeGR, further adsorption of CO on Fe in CO3 is plausible and takes place spontaneously. We then showed that adsorbed CO may react with CO3, forming a cyclic-carbonate-like species that dissociates easily to CO2. The finding highlights the reaction condition-dependent formation and evolution of CO3, as well as its contribution to CO conversion, and may extend the understanding to performance of SACs in low temperature CO oxidation.

以聚酰亚胺为基底的柔性钙钛矿太阳电池因其出色的热稳定性和高功质比可应用于航天飞行器。然而，聚酰亚胺的金属电极会造成钙钛矿太阳电池非辐射复合增大，降低钙钛矿太阳电池的转换效率。因此，本文介绍了一种采用ITO修饰策略来提升柔性钙钛矿太阳电池转换效率的新方法。通过在金属电极上沉积一层ITO，不仅提高了空穴传输层中Ni³⁺/Ni²⁺的比例，提高了空穴传输层的电导率，还改善了钙钛矿薄膜成膜质量，抑制了钙钛矿薄膜与氧化镍界面之间的非辐射复合。基于ITO修饰策略制备的聚酰亚胺基底柔性钙钛矿太阳电池转换效率达17.91%。本文为提升聚酰亚胺基底的柔性钙钛矿太阳电池的转换效率提供了一种有效途径。