Computation-informed optimization of Ni(PyC)2 functionalization for noble gas separations

Nickolas Gantzler; Min Bum Kim; Alexander Robinson; Maxwell W. Terban; Sanjit Ghose; Robert E. Dinnebier; Arthur Henry York; Davide Tiana; Cory M. Simon; Praveen K. Thallapally

doi:10.1016/j.xcrp.2022.101025

Computation-informed optimization of Ni(PyC)₂ functionalization for noble gas separations

Nickolas Gantzler
, Min Bum Kim
, Alexander Robinson
, Maxwell W. Terban
, Sanjit Ghose
, Robert E. Dinnebier
, Arthur Henry York
, Davide Tiana
, Cory M. Simon
, Praveen K. Thallapally

School of Chemistry

Oregon State University
Pacific Northwest National Laboratory
Max Planck Institute for Solid State Research
Brookhaven National Laboratory

Research output: Contribution to journal › Article › peer-review

Abstract

Our objective is to tune a “lead” metal-organic framework, Ni(PyC)₂ (pyridine-4-carboxylate [PyC]), by functionalizing its PyC ligands to maximize its adsorptive selectivity for xenon over krypton at room temperature. To guide experiments, we (1) construct a library of Ni(PyC-X)₂ (X = functional group) crystal structure models then (2) use molecular simulations to predict their noble gas adsorption and selectivity at room temperature. Motivated by our virtual screening, we synthesize Ni(PyC-m-NH₂)₂, determine its crystal structure by X-ray powder diffraction, measure its Xe, Kr, and Ar adsorption isotherms (298 K), and indeed find that its dilute Xe/Kr selectivity at 298 K (20) exceeds that of its parent Ni(PyC)₂ (17). Corroborated by molecular models, in situ X-ray diffraction shows that Ni(PyC-m-NH₂)₂ organizes well-defined, Xe-tailored binding pockets along its one-dimensional channels. Our study illustrates the computation-informed optimization of a “lead” metal-organic framework.

Original language	English
Article number	101025
Journal	Cell Reports Physical Science
Volume	3
Issue number	9
DOIs	https://doi.org/10.1016/j.xcrp.2022.101025
Publication status	Published - 21 Sept 2022

Keywords

computational screening
gas adsorption
gas separations
metal-organic frameworks
MOFs
molecular simulations
noble gas adsorption
Xe/Kr separations

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10.1016/j.xcrp.2022.101025

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title = "Computation-informed optimization of Ni(PyC)2 functionalization for noble gas separations",

abstract = "Our objective is to tune a “lead” metal-organic framework, Ni(PyC)2 (pyridine-4-carboxylate [PyC]), by functionalizing its PyC ligands to maximize its adsorptive selectivity for xenon over krypton at room temperature. To guide experiments, we (1) construct a library of Ni(PyC-X)2 (X = functional group) crystal structure models then (2) use molecular simulations to predict their noble gas adsorption and selectivity at room temperature. Motivated by our virtual screening, we synthesize Ni(PyC-m-NH2)2, determine its crystal structure by X-ray powder diffraction, measure its Xe, Kr, and Ar adsorption isotherms (298 K), and indeed find that its dilute Xe/Kr selectivity at 298 K (20) exceeds that of its parent Ni(PyC)2 (17). Corroborated by molecular models, in situ X-ray diffraction shows that Ni(PyC-m-NH2)2 organizes well-defined, Xe-tailored binding pockets along its one-dimensional channels. Our study illustrates the computation-informed optimization of a “lead” metal-organic framework.",

keywords = "computational screening, gas adsorption, gas separations, metal-organic frameworks, MOFs, molecular simulations, noble gas adsorption, Xe/Kr separations",

author = "Nickolas Gantzler and Kim, \{Min Bum\} and Alexander Robinson and Terban, \{Maxwell W.\} and Sanjit Ghose and Dinnebier, \{Robert E.\} and York, \{Arthur Henry\} and Davide Tiana and Simon, \{Cory M.\} and Thallapally, \{Praveen K.\}",

note = "Publisher Copyright: {\textcopyright} 2022 The Author(s)",

year = "2022",

month = sep,

day = "21",

doi = "10.1016/j.xcrp.2022.101025",

language = "English",

volume = "3",

journal = "Cell Reports Physical Science",

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TY - JOUR

T1 - Computation-informed optimization of Ni(PyC)2 functionalization for noble gas separations

AU - Gantzler, Nickolas

AU - Kim, Min Bum

AU - Robinson, Alexander

AU - Terban, Maxwell W.

AU - Ghose, Sanjit

AU - Dinnebier, Robert E.

AU - York, Arthur Henry

AU - Tiana, Davide

AU - Simon, Cory M.

AU - Thallapally, Praveen K.

PY - 2022/9/21

Y1 - 2022/9/21

N2 - Our objective is to tune a “lead” metal-organic framework, Ni(PyC)2 (pyridine-4-carboxylate [PyC]), by functionalizing its PyC ligands to maximize its adsorptive selectivity for xenon over krypton at room temperature. To guide experiments, we (1) construct a library of Ni(PyC-X)2 (X = functional group) crystal structure models then (2) use molecular simulations to predict their noble gas adsorption and selectivity at room temperature. Motivated by our virtual screening, we synthesize Ni(PyC-m-NH2)2, determine its crystal structure by X-ray powder diffraction, measure its Xe, Kr, and Ar adsorption isotherms (298 K), and indeed find that its dilute Xe/Kr selectivity at 298 K (20) exceeds that of its parent Ni(PyC)2 (17). Corroborated by molecular models, in situ X-ray diffraction shows that Ni(PyC-m-NH2)2 organizes well-defined, Xe-tailored binding pockets along its one-dimensional channels. Our study illustrates the computation-informed optimization of a “lead” metal-organic framework.

AB - Our objective is to tune a “lead” metal-organic framework, Ni(PyC)2 (pyridine-4-carboxylate [PyC]), by functionalizing its PyC ligands to maximize its adsorptive selectivity for xenon over krypton at room temperature. To guide experiments, we (1) construct a library of Ni(PyC-X)2 (X = functional group) crystal structure models then (2) use molecular simulations to predict their noble gas adsorption and selectivity at room temperature. Motivated by our virtual screening, we synthesize Ni(PyC-m-NH2)2, determine its crystal structure by X-ray powder diffraction, measure its Xe, Kr, and Ar adsorption isotherms (298 K), and indeed find that its dilute Xe/Kr selectivity at 298 K (20) exceeds that of its parent Ni(PyC)2 (17). Corroborated by molecular models, in situ X-ray diffraction shows that Ni(PyC-m-NH2)2 organizes well-defined, Xe-tailored binding pockets along its one-dimensional channels. Our study illustrates the computation-informed optimization of a “lead” metal-organic framework.

KW - computational screening

KW - gas adsorption

KW - gas separations

KW - metal-organic frameworks

KW - MOFs

KW - molecular simulations

KW - noble gas adsorption

KW - Xe/Kr separations

UR - https://www.scopus.com/pages/publications/85138191028

U2 - 10.1016/j.xcrp.2022.101025

DO - 10.1016/j.xcrp.2022.101025

M3 - Article

AN - SCOPUS:85138191028

SN - 2666-3864

VL - 3

JO - Cell Reports Physical Science

JF - Cell Reports Physical Science

IS - 9

M1 - 101025

ER -

Computation-informed optimization of Ni(PyC)₂ functionalization for noble gas separations

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