Computer-aided discovery of a metal–organic framework with superior oxygen uptake

Abstract

Current advances in materials science have resulted in the rapid emergence of thousands of functional adsorbent materials in recent years. This clearly creates multiple opportunities for their potential application, but it also creates the following challenge: how does one identify the most promising structures, among the thousands of possibilities, for a particular application? Here, we present a case of computer-aided material discovery, in which we complete the full cycle from computational screening of metal–organic framework materials for oxygen storage, to identification, synthesis and measurement of oxygen adsorption in the top-ranked structure. We introduce an interactive visualization concept to analyze over 1000 unique structure–property plots in five dimensions and delimit the relationships between structural properties and oxygen adsorption performance at different pressures for 2932 already-synthesized structures. We also report a world-record holding material for oxygen storage, UMCM-152, which delivers 22.5% more oxygen than the best known material to date, to the best of our knowledge.

Modeling the Structural and Thermal Properties of Loaded Metal–Organic Frameworks. An Interplay of Quantum and Anharmonic Fluctuations

“…The harmonic approximation could therefore serve as an efficient procedure to accurately estimate the heat capacity of the empty framework in the increasing number of high-throughput MOF screenings. 9,11,[96][97][98] In order to study the effect of adsorbates, we start by considering the case of a loading x of high-level PIMD strategy might not be required to estimate the heat capacity of the empty MOF host, PIMD proves to be crucial to capture the correct temperature dependence of the loaded system, as can be seen in the left panel of Figure 6. Here, anharmonic effects become important as we observe differences between the PIMD results and the harmonic approximation.…”

Identifying promising metal–organic frameworks for heterogeneous catalysis via high‐throughput periodic density functional theory

“…One of the main goals of HT screening of MOF crystal structure databases is to reduce the time‐to‐discovery of MOFs with desired chemical and physical properties. In the area of gas storage and separations, HT grand canonical Monte Carlo simulations using classical force fields have been successfully used to identify top‐performing MOFs with respect to CH 4 storage capacity, CO 2 capture, H 2 storage, and O 2 uptake . However, extending HT screening of MOFs to applications requiring quantum chemical calculations, such as catalysis, remains a challenge.…”

Pillared-layered metal–organic frameworks for mechanical energy storage applications

“…ref. [18][19][20], but most computational studies on exible materials still tend to focus only on understanding the exibility of specic case studies (e.g. ref.…”