Evaluation and screening of multivariate metal-organic frameworks for hydrogen storage

Multivariate metal-organic frameworks (MTV-MOFs) are characterized by their unique structural feature of incorporating multiple organic linkers and metal ions into a unified framework. This composite construction bestows MTV-MOFs with a broader spectrum of diverse and intricate properties compared to traditional single-component MOFs. In this study, the performance of 560 MTV-MOFs as hydrogen storage adsorbents has been thoroughly investigated. Firstly, the key structural parameters of materials, including density, pore occupied accessible volume, accessible surface area, and porosity were computed. Then, high-throughput Grand Canonical Monte Carlo (GCMC) simulations were employed to calculate hydrogen adsorption capacity of MTV-MOFs under hydrogen pressures of 100 bar at both 77 K and 298 K. Based on simulated results, the deliverable hydrogen capacity of these MTV-MOFs were deduced under both room temperature conditions (298 K, 97.2 bar → 298 K, 5 bar) and low-temperature conditions (77 K, 100 bar → 160 K, 5 bar). Through high-throughput screening, we identified top ten promising MTV-MOFs with the highest hydrogen storage capacity and conducted in-depth studies on their hydrogen adsorption properties. Furthermore, we developed a multivariate linear regression model to quantitatively predict the relationship between hydrogen adsorption capacity and their structural parameters for these MTV-MOFs. The predictions of this model align closely with the outcomes derived from GCMC simulations. The present study highlights the potential of MTV-MOFs as promising candidates for hydrogen storage applications, thereby providing valuable theoretical insights into the exploration of high-capacity hydrogen storage materials. © 2024