Breaking the trade-off between selectivity and adsorption capacity for gas separation

Naveen Kumar; Soumya Mukherjee; Nathan C. Harvey-Reid; Andrey A. Bezrukov; Kui Tan; Vinicius Martins; Matthias Vandichel; Tony Pham; Lisa M. van Wyk; Kolade Oyekan; Amrit Kumar; Katherine A. Forrest; Komal M. Patil; Leonard J. Barbour; Brian Space; Yining Huang; Paul E. Kruger; Michael J. Zaworotko

doi:10.1016/j.chempr.2021.07.007

Breaking the trade-off between selectivity and adsorption capacity for gas separation

Naveen Kumar, Soumya Mukherjee, Nathan C. Harvey-Reid, Andrey A. Bezrukov, Kui Tan, Vinicius Martins, Matthias Vandichel, Tony Pham, Lisa M. van Wyk, Kolade Oyekan, Amrit Kumar, Katherine A. Forrest, Komal M. Patil, Leonard J. Barbour, Brian Space, Yining Huang, Paul E. Kruger, Michael J. Zaworotko

Department of Chemical Sciences

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

Abstract

The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C₂H₂ removal from CO₂ in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C₂H₂ and weaker affinity for CO₂. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C₂H₂/CO₂ separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C₂H₂/CO₂ binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C₂H₂ selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g⁻¹).

Original language	English
Pages (from-to)	3085-3098
Number of pages	14
Journal	Chem
Volume	7
Issue number	11
DOIs	https://doi.org/10.1016/j.chempr.2021.07.007
Publication status	Published - 11 Nov 2021

Keywords

acetylene
carbon dioxide
crystal engineering
gas purification
gas separation
hybrid ultramicroporous material
physisorbent
porous materials
SDG7: Affordable and clean energy
selectivity

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.chempr.2021.07.007

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Kumar, N., Mukherjee, S., Harvey-Reid, N. C., Bezrukov, A. A., Tan, K., Martins, V., Vandichel, M., Pham, T., van Wyk, L. M., Oyekan, K., Kumar, A., Forrest, K. A., Patil, K. M., Barbour, L. J., Space, B., Huang, Y., Kruger, P. E., & Zaworotko, M. J. (2021). Breaking the trade-off between selectivity and adsorption capacity for gas separation. Chem, 7(11), 3085-3098. https://doi.org/10.1016/j.chempr.2021.07.007

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title = "Breaking the trade-off between selectivity and adsorption capacity for gas separation",

abstract = "The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C2H2 and weaker affinity for CO2. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C2H2/CO2 separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C2H2/CO2 binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C2H2 selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g−1).",

keywords = "acetylene, carbon dioxide, crystal engineering, gas purification, gas separation, hybrid ultramicroporous material, physisorbent, porous materials, SDG7: Affordable and clean energy, selectivity",

author = "Naveen Kumar and Soumya Mukherjee and Harvey-Reid, {Nathan C.} and Bezrukov, {Andrey A.} and Kui Tan and Vinicius Martins and Matthias Vandichel and Tony Pham and {van Wyk}, {Lisa M.} and Kolade Oyekan and Amrit Kumar and Forrest, {Katherine A.} and Patil, {Komal M.} and Barbour, {Leonard J.} and Brian Space and Yining Huang and Kruger, {Paul E.} and Zaworotko, {Michael J.}",

note = "Publisher Copyright: {\textcopyright} 2021 The Authors",

year = "2021",

month = nov,

day = "11",

doi = "10.1016/j.chempr.2021.07.007",

language = "English",

volume = "7",

pages = "3085--3098",

journal = "Chem",

issn = "2451-9308",

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Kumar, N, Mukherjee, S, Harvey-Reid, NC, Bezrukov, AA, Tan, K, Martins, V, Vandichel, M, Pham, T, van Wyk, LM, Oyekan, K, Kumar, A, Forrest, KA, Patil, KM, Barbour, LJ, Space, B, Huang, Y, Kruger, PE & Zaworotko, MJ 2021, 'Breaking the trade-off between selectivity and adsorption capacity for gas separation', Chem, vol. 7, no. 11, pp. 3085-3098. https://doi.org/10.1016/j.chempr.2021.07.007

TY - JOUR

T1 - Breaking the trade-off between selectivity and adsorption capacity for gas separation

AU - Kumar, Naveen

AU - Mukherjee, Soumya

AU - Harvey-Reid, Nathan C.

AU - Bezrukov, Andrey A.

AU - Tan, Kui

AU - Martins, Vinicius

AU - Vandichel, Matthias

AU - Pham, Tony

AU - van Wyk, Lisa M.

AU - Oyekan, Kolade

AU - Kumar, Amrit

AU - Forrest, Katherine A.

AU - Patil, Komal M.

AU - Barbour, Leonard J.

AU - Space, Brian

AU - Huang, Yining

AU - Kruger, Paul E.

AU - Zaworotko, Michael J.

PY - 2021/11/11

Y1 - 2021/11/11

N2 - The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C2H2 and weaker affinity for CO2. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C2H2/CO2 separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C2H2/CO2 binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C2H2 selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g−1).

AB - The trade-off between selectivity and adsorption capacity with porous materials is a major roadblock to reducing the energy footprint of gas separation technologies. To address this matter, we report herein a systematic crystal engineering study of C2H2 removal from CO2 in a family of hybrid ultramicroporous materials (HUMs). The HUMs are composed of the same organic linker ligand, 4-(3,5-dimethyl-1H-pyrazol-4-yl)pyridine, pypz, three inorganic pillar ligands, and two metal cations, thereby affording six isostructural pcu topology HUMs. All six HUMs exhibited strong binding sites for C2H2 and weaker affinity for CO2. The tuning of pore size and chemistry enabled by crystal engineering resulted in benchmark C2H2/CO2 separation performance. Fixed-bed dynamic column breakthrough experiments for an equimolar (v/v = 1:1) C2H2/CO2 binary gas mixture revealed that one sorbent, SIFSIX-21-Ni, was the first C2H2 selective sorbent that combines exceptional separation selectivity (27.7) with high adsorption capacity (4 mmol·g−1).

KW - acetylene

KW - carbon dioxide

KW - crystal engineering

KW - gas purification

KW - gas separation

KW - hybrid ultramicroporous material

KW - physisorbent

KW - porous materials

KW - SDG7: Affordable and clean energy

KW - selectivity

UR - http://www.scopus.com/inward/record.url?scp=85113731461&partnerID=8YFLogxK

U2 - 10.1016/j.chempr.2021.07.007

DO - 10.1016/j.chempr.2021.07.007

M3 - Article

AN - SCOPUS:85113731461

SN - 2451-9308

VL - 7

SP - 3085

EP - 3098

JO - Chem

JF - Chem

IS - 11

ER -

Breaking the trade-off between selectivity and adsorption capacity for gas separation

Abstract

Keywords

UN SDGs

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