Clean and sustainable energy technologies, such as fuel cells, metal-air batteries, water-splitting and solar cells, are currently under intensive research and development because of their high efficiency, promising large-scale applications, and virtually no pollution or greenhouse gas emission. At the heart of these energy devices, there are three critical chemical reactions: oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and CO2 reduction to fuel(CO2RR) that determine the efficiencies of energy conversion and storage. These reactions, however, are sluggish and require noble metals (e.g., platinum) or their oxides as catalysts. The limited resources and high cost of platinum have hampered the commercialization of these technologies. Therefore, it is necessary to search for alternative materials to replace Pt. Covalent organic frameworks (COF) are appealing as an alternative for catalytic applications because of their structures and excellent properties. Although the superior catalytic capabilities of COFs for ORR have been demonstrated, trial-and-error approaches are still used to date for the development of highly-efficient catalysts. To rationally design a catalyst, it is critical to understand which intrinsic material characteristics, or descriptors that control catalysis. Through first-principles calculations, we have identified a material property that serves as the activity descriptor for predicating ORR and OER activities, and established a volcano relationship between the descriptor and the bifunctional activities of the COF materials. Such descriptor enables us to design new catalysts with enhanced ORR and OER activities, even better than those reported for platinum-based metal catalysts. The design principles can be used as a guidance to develop various new COF materials for clean energy conversion and storage. This approach has been extended to the COF materials for CO2RR.

Computational screening and design principles of COF materials as high-performance catalysts for clean energy conversion

2019 Fall National Meeting

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