Theoretical studies of metal-organic frameworks: Calculation methods and applications in catalysis, gas separation, and energy storage

Metal-organic frameworks (MOFs), a functional material with a large specific surface area and high porosity have attracted increasing attention for their great potential in various applications. As a relatively time-saving, cost-effective, high-efficient and results-predictable method, theoretical calculation has gradually become a trend to guide MOFs material design and development. In this review, the most recent advances in theoretical studies of MOFs were systemically summarized, introducing the development of calculation methods and models with their merits and drawbacks, and emphasizing the employment of theoretical calculations in practical applications of MOFs. First, we briefly introduced the development of MOFs’ database construction, including hypothetical and experimental databases. The calculation methods and models to predict structures and properties of MOFs were thoroughly reviewed in the next part, and the merits and possible limitations are also discussed in detail. Additionally, we summarized the various promising applications of theoretical calculations in catalysis (including electrocatalysis and photocatalysis), selective gas separation and energy storage (including batteries and supercapacitor). The existing challenges of theoretical calculation in MOFs were also pointed out in the outlook. This review will provide a helpful guideline for the rational structure and function design of MOFs, and contribute to the material optimizations in applications of catalysis and energy storage.