Journal
CHEMICAL REVIEWS
Volume 120, Issue 16, Pages 8641-8715Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemrev.0c00148
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Funding
- National Science Foundation through the Division of Materials Research [DMR-1956403]
- National Science Foundation [ACI-1548562]
- PICS Coeus High Performance Computer - National Science Foundation [1624776]
- University of Oregon High Performance Computer, Talapas
- Division Of Mathematical Sciences
- Direct For Mathematical & Physical Scien [1624776] Funding Source: National Science Foundation
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Owing to their molecular building blocks, yet highly crystalline nature, metal-organic frameworks (MOFs) sit at the interface between molecule and material. Their diverse structures and compositions enable them to be useful materials as catalysts in heterogeneous reactions, electrical conductors in energy storage and transfer applications, chromophores in photoenabled chemical transformations, and beyond. In all cases, density functional theory (DFT) and higher-level methods for electronic structure determination provide valuable quantitative information about the electronic properties that underpin the functions of these frameworks. However, there are only two general modeling approaches in conventional electronic structure software packages: those that treat materials as extended, periodic solids, and those that treat materials as discrete molecules. Each approach has features and benefits; both have been widely employed to understand the emergent chemistry that arises from the formation of the metal-organic interface. This Review canvases these approaches to date, with emphasis placed on the application of electronic structure theory to explore reactivity and electron transfer using periodic, molecular, and embedded models. This includes (i) computational chemistry considerations such as how functional, k-grid, and other model variables are selected to enable insights into MOF properties, (ii) extended solid models that treat MOFs as materials rather than molecules, (iii) the mechanics of cluster extraction and subsequent chemistry enabled by these molecular models, (iv) catalytic studies using both solids and clusters thereof, and (v) embedded, mixed-method approaches, which simulate a fraction of the material using one level of theory and the remainder of the material using another dissimilar theoretical implementation.
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