Shaping the Water-Harvesting Behavior of Metal–Organic Frameworks Aided by Fine-Tuned GPT Models

Zheng, Zhiling; Alawadhi, Ali H.; Chheda, Saumil; Neumann, S. Ephraim; Rampal, Nakul; Liu, Shengchao; Nguyen, Ha L.; Lin, Yen-hsu; Rong, Zichao; Siepmann, J. Ilja; Gagliardi, Laura; Anandkumar, Anima; Borgs, Christian; Chayes, Jennifer T.; Yaghi, Omar M.

doi:10.1021/jacs.3c12086

Shaping the Water-Harvesting Behavior of Metal–Organic Frameworks Aided by Fine-Tuned GPT Models

Journal Article · Wed Dec 13 00:00:00 EST 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c12086· OSTI ID:2510855

^[1]; ^[1]; ^[2]; ^[1]; Rampal, Nakul ^[1]; Liu, Shengchao ^[1]; ^[1]; Lin, Yen-hsu ^[1]; ^[1]; ^[3]; ^[4]; Anandkumar, Anima ^[5]; Borgs, Christian ^[1]; Chayes, Jennifer T. ^[1]; ^[6]

University of California, Berkeley, CA (United States)
University of California, Berkeley, CA (United States); University of Minnesota─Twin Cities, Minneapolis, MN (United States)
University of Minnesota─Twin Cities, Minneapolis, MN (United States)
University of Chicago, IL (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States); NVIDIA Corporation, Santa Clara, CA (United States)
University of California, Berkeley, CA (United States); King Abdulaziz City for Science and Technology, Riyadh (Saudi Arabia)

Here, we construct a data set of metal–organic framework (MOF) linkers and employ a fine-tuned GPT assistant to propose MOF linker designs by mutating and modifying the existing linker structures. This strategy allows the GPT model to learn the intricate language of chemistry in molecular representations, thereby achieving an enhanced accuracy in generating linker structures compared with its base models. Aiming to highlight the significance of linker design strategies in advancing the discovery of water-harvesting MOFs, we conducted a systematic MOF variant expansion upon state-of-the-art MOF-303 utilizing a multidimensional approach that integrates linker extension with multivariate tuning strategies. We synthesized a series of isoreticular aluminum MOFs, termed Long-Arm MOFs (LAMOF-1 to LAMOF-10), featuring linkers that bear various combinations of heteroatoms in their five-membered ring moiety, replacing pyrazole with either thiophene, furan, or thiazole rings or a combination of two. Beyond their consistent and robust architecture, as demonstrated by permanent porosity and thermal stability, the LAMOF series offers a generalizable synthesis strategy. Importantly, these 10 LAMOFs establish new benchmarks for water uptake (up to 0.64 g g^–1) and operational humidity ranges (between 13 and 53%), thereby expanding the diversity of water-harvesting MOFs.

View Accepted Manuscript (DOE)

Research Organization:: University of Minnesota, Minneapolis, MN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0023454

OSTI ID:: 2510855

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 51 Vol. 145; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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