Multivariate Machine Learning Models of Nanoscale Porosity from Ultrafast NMR Relaxometry

• Published in: Angewandte Chemie International Edition 2024-03, Vol.63 (13), p.e202316664-n/a
• Main Authors: Fricke, Sophia N., Salgado, Mia, Menezes, Tamires, Costa Santos, Kátilla M., Gallagher, Neal B., Song, Ah‐Young, Wang, Jieyu, Engler, Kaitlyn, Wang, Yang, Mao, Haiyan, Reimer, Jeffrey A.
• Format: Article
• Language: English
• Subjects: Catalysis; Catalysts; Energy storage; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Learning algorithms; Machine learning; Magnetic resonance; Metal-organic frameworks; Metals; NMR; NMR relaxometry; Nuclear magnetic resonance; Pore size; Porosity; porous materials; Principal components analysis; Surface area; Time domain analysis
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202316664

Nanoporous materials are of great interest in many applications, such as catalysis, separation, and energy storage. The performance of these materials is closely related to their pore sizes, which are inefficient to determine through the conventional measurement of gas adsorption isotherms. Nuclear magnetic resonance (NMR) relaxometry has emerged as a technique highly sensitive to porosity in such materials. Nonetheless, streamlined methods to estimate pore size from NMR relaxometry remain elusive. Previous attempts have been hindered by inverting a time domain signal to relaxation rate distribution, and dealing with resulting parameters that vary in number, location, and magnitude. Here we invoke well‐established machine learning techniques to directly correlate time domain signals to BET surface areas for a set of metal‐organic frameworks (MOFs) imbibed with solvent at varied concentrations. We employ this series of MOFs to establish a correlation between NMR signal and surface area via partial least squares (PLS), following screening with principal component analysis, and apply the PLS model to predict surface area of various nanoporous materials. This approach offers a high‐throughput, non‐destructive way to assess porosity in c.a. one minute. We anticipate this work will contribute to the development of new materials with optimized pore sizes for various applications. Machine learning allows rapid classification and prediction of the surface area (SA) of nanoporous materials through NMR relaxometry measurements of solvent imbibed in the porous network. Here, principal component analysis (PCA) screens “high” and “low” SA materials, and partial least squares (PLS) provides numerical estimates of SA. This non‐destructive technique can be used to help develop new materials with optimized porosity.