M. Fumanal, A. Ortega-Guerrero, K. M. Jablonka, B. Smit, and I. Tavernelli, Charge Separation and Charge Carrier Mobility in Photocatalytic Metal-Organic Frameworks Adv. Funct. Mater. (2020) http://dx.doi.org/10.1002/adfm.202003792
Abstract Metalâorganic frameworks (MOFs) are highly versatile materials owing to their vast structural and chemical tunability. These hybrid inorganicâorganic crystalline materials offer an ideal platform to incorporate lightâharvesting and catalytic centers and thus, exhibit a great potential to be exploited in solarâdriven photocatalytic processes such as H2Â production and CO2Â reduction. To be photocatalytically active, UVâvisible optical absorption and appropriate band alignment with respect to the target redox potential is required. Despite fulfilling these criteria, the photocatalytic performance of MOFs is still limited by their ability to produce longâlived electronâhole pairs and longârange charge transport. Here, a computational strategy is presented to address these two descriptors in MOFs and to translate them into charge transfer numbers and effective mass values. The approach is applied to 15 MOFs from the literature that encompass the main strategies used in the design of efficient photocatalysts including different metals, ligands, and topologies. The results capture the main characteristics previously reported for these MOFs and enable to identify promising candidates. In the quest of novel photocatalytic systems, highâthroughput screening based on charge separation and charge mobility features are envisioned to be applied in large databases of both experimentally and in silico generated MOFs.