Incorporating Flexibility Effects into Metal–Organic Framework Adsorption Simulations Using Different Models

Yu, Zhenzi; Anstine, Dylan M.; Boulfelfel, Salah Eddine; Gu, Chenkai; Colina, Coray M.; Sholl, David S.

doi:10.1021/acsami.1c20583

Title: Incorporating Flexibility Effects into Metal–Organic Framework Adsorption Simulations Using Different Models

Journal Article · Mon Dec 20 00:00:00 EST 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c20583· OSTI ID:1847524

Yu, Zhenzi ^[1]; Anstine, Dylan M. ^[2]; Boulfelfel, Salah Eddine ^[1]; Gu, Chenkai ^[3];

^[2];

^[4]

Georgia Inst. of Technology, Atlanta, GA (United States)
Univ. of Florida, Gainesville, FL (United States)
Georgia Inst. of Technology, Atlanta, GA (United States); Huazhong Univ. of Science and Technology, Wuhan (China)
Georgia Inst. of Technology, Atlanta, GA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

High-throughput calculations based on molecular simulations to predict the adsorption of molecules inside metal–organic frameworks (MOFs) have become a useful complement to experimental efforts to identify promising adsorbents for chemical separations and storage. For computational convenience, all existing efforts of this kind have relied on simulations in which the MOF is approximated as rigid. In this paper, we use extensive adsorption–relaxation simulations that fully include MOF flexibility effects to explore the validity of the rigid framework approximation. We also examine the accuracy of several approximate methods to incorporate framework flexibility that are more computationally efficient than adsorption–relaxation calculations. We first benchmark various models of MOF flexibility for four MOFs with well-established CO₂ experimental consensus isotherms. We then consider a range of adsorption properties, including Henry’s constants, nondilute loadings, and adsorption selectivity, for seven adsorbates in 15 MOFs randomly selected from the CoRE MOF database. Our results indicate that in many MOFs adsorption–relaxation simulations are necessary to make quantitative predictions of adsorption, particularly for adsorption at dilute concentrations, although more standard calculations based on rigid structures can provide useful information. Finally, we investigate whether a correlation exists between the elastic properties of empty MOFs and the importance of including framework flexibility in making accurate predictions of molecular adsorption. Our results did not identify a simple correlation of this type.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME)

Sponsoring Organization:: Fundamental Research Funds for the Central Universities; China Scholarship Council (CSC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC05-00OR22725; SC0012577; FG02-17ER16362

OSTI ID:: 1847524

Journal Information:: ACS Applied Materials and Interfaces, Vol. 13, Issue 51; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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