Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material

Mohana Shivanna; Ken ichi Otake; Bai Qiao Song; Lisa M. van Wyk; Qing Yuan Yang; Naveen Kumar; Wesley K. Feldmann; Tony Pham; Shanelle Suepaul; Brian Space; Leonard J. Barbour; Susumu Kitagawa; Michael J. Zaworotko

doi:10.1002/anie.202106263

Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material

Mohana Shivanna, Ken ichi Otake, Bai Qiao Song, Lisa M. van Wyk, Qing Yuan Yang, Naveen Kumar, Wesley K. Feldmann, Tony Pham, Shanelle Suepaul, Brian Space, Leonard J. Barbour, Susumu Kitagawa, Michael J. Zaworotko

Department of Chemical Sciences

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

Abstract

Structural changes at the active site of an enzyme induced by binding to a substrate molecule can result in enhanced activity in biological systems. Herein, we report that the new hybrid ultramicroporous material sql-SIFSIX-bpe-Zn exhibits an induced fit binding mechanism when exposed to acetylene, C₂H₂. The resulting phase change affords exceptionally strong C₂H₂ binding that in turn enables highly selective C₂H₂/C₂H₄ and C₂H₂/CO₂ separation demonstrated by dynamic breakthrough experiments. sql-SIFSIX-bpe-Zn was observed to exhibit at least four phases: as-synthesised (α); activated (β); and C₂H₂ induced phases (β′ and γ). sql-SIFSIX-bpe-Zn-β exhibited strong affinity for C₂H₂ at ambient conditions as demonstrated by benchmark isosteric heat of adsorption (Q_st) of 67.5 kJ mol⁻¹ validated through in situ pressure gradient differential scanning calorimetry (PG-DSC). Further, in situ characterisation and DFT calculations provide insight into the mechanism of the C₂H₂ induced fit transformation, binding positions and the nature of host-guest and guest-guest interactions.

Original language	English
Pages (from-to)	20383-20390
Number of pages	8
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	37
DOIs	https://doi.org/10.1002/anie.202106263
Publication status	Published - 6 Sep 2021

Keywords

CH/CH and CH/CO separation
coordination polymers
induced fit mechanism
physisorption
ultramicroporous materials

UN SDGs

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

Access to Document

10.1002/anie.202106263

Cite this

Shivanna, M., Otake, K. I., Song, B. Q., van Wyk, L. M., Yang, Q. Y., Kumar, N., Feldmann, W. K., Pham, T., Suepaul, S., Space, B., Barbour, L. J., Kitagawa, S., & Zaworotko, M. J. (2021). Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material. Angewandte Chemie - International Edition, 60(37), 20383-20390. https://doi.org/10.1002/anie.202106263

@article{43321b660db54135a0c2b98400fb3dc2,

title = "Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material",

abstract = "Structural changes at the active site of an enzyme induced by binding to a substrate molecule can result in enhanced activity in biological systems. Herein, we report that the new hybrid ultramicroporous material sql-SIFSIX-bpe-Zn exhibits an induced fit binding mechanism when exposed to acetylene, C2H2. The resulting phase change affords exceptionally strong C2H2 binding that in turn enables highly selective C2H2/C2H4 and C2H2/CO2 separation demonstrated by dynamic breakthrough experiments. sql-SIFSIX-bpe-Zn was observed to exhibit at least four phases: as-synthesised (α); activated (β); and C2H2 induced phases (β′ and γ). sql-SIFSIX-bpe-Zn-β exhibited strong affinity for C2H2 at ambient conditions as demonstrated by benchmark isosteric heat of adsorption (Qst) of 67.5 kJ mol−1 validated through in situ pressure gradient differential scanning calorimetry (PG-DSC). Further, in situ characterisation and DFT calculations provide insight into the mechanism of the C2H2 induced fit transformation, binding positions and the nature of host-guest and guest-guest interactions.",

keywords = "CH/CH and CH/CO separation, coordination polymers, induced fit mechanism, physisorption, ultramicroporous materials",

author = "Mohana Shivanna and Otake, {Ken ichi} and Song, {Bai Qiao} and {van Wyk}, {Lisa M.} and Yang, {Qing Yuan} and Naveen Kumar and Feldmann, {Wesley K.} and Tony Pham and Shanelle Suepaul and Brian Space and Barbour, {Leonard J.} and Susumu Kitagawa and Zaworotko, {Michael J.}",

note = "Publisher Copyright: {\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH",

year = "2021",

month = sep,

day = "6",

doi = "10.1002/anie.202106263",

language = "English",

volume = "60",

pages = "20383--20390",

journal = "Angewandte Chemie - International Edition",

issn = "1433-7851",

number = "37",

}

Shivanna, M, Otake, KI, Song, BQ, van Wyk, LM, Yang, QY, Kumar, N, Feldmann, WK, Pham, T, Suepaul, S, Space, B, Barbour, LJ, Kitagawa, S & Zaworotko, MJ 2021, 'Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material', Angewandte Chemie - International Edition, vol. 60, no. 37, pp. 20383-20390. https://doi.org/10.1002/anie.202106263

TY - JOUR

T1 - Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material

AU - Shivanna, Mohana

AU - Otake, Ken ichi

AU - Song, Bai Qiao

AU - van Wyk, Lisa M.

AU - Yang, Qing Yuan

AU - Kumar, Naveen

AU - Feldmann, Wesley K.

AU - Pham, Tony

AU - Suepaul, Shanelle

AU - Space, Brian

AU - Barbour, Leonard J.

AU - Kitagawa, Susumu

AU - Zaworotko, Michael J.

PY - 2021/9/6

Y1 - 2021/9/6

N2 - Structural changes at the active site of an enzyme induced by binding to a substrate molecule can result in enhanced activity in biological systems. Herein, we report that the new hybrid ultramicroporous material sql-SIFSIX-bpe-Zn exhibits an induced fit binding mechanism when exposed to acetylene, C2H2. The resulting phase change affords exceptionally strong C2H2 binding that in turn enables highly selective C2H2/C2H4 and C2H2/CO2 separation demonstrated by dynamic breakthrough experiments. sql-SIFSIX-bpe-Zn was observed to exhibit at least four phases: as-synthesised (α); activated (β); and C2H2 induced phases (β′ and γ). sql-SIFSIX-bpe-Zn-β exhibited strong affinity for C2H2 at ambient conditions as demonstrated by benchmark isosteric heat of adsorption (Qst) of 67.5 kJ mol−1 validated through in situ pressure gradient differential scanning calorimetry (PG-DSC). Further, in situ characterisation and DFT calculations provide insight into the mechanism of the C2H2 induced fit transformation, binding positions and the nature of host-guest and guest-guest interactions.

AB - Structural changes at the active site of an enzyme induced by binding to a substrate molecule can result in enhanced activity in biological systems. Herein, we report that the new hybrid ultramicroporous material sql-SIFSIX-bpe-Zn exhibits an induced fit binding mechanism when exposed to acetylene, C2H2. The resulting phase change affords exceptionally strong C2H2 binding that in turn enables highly selective C2H2/C2H4 and C2H2/CO2 separation demonstrated by dynamic breakthrough experiments. sql-SIFSIX-bpe-Zn was observed to exhibit at least four phases: as-synthesised (α); activated (β); and C2H2 induced phases (β′ and γ). sql-SIFSIX-bpe-Zn-β exhibited strong affinity for C2H2 at ambient conditions as demonstrated by benchmark isosteric heat of adsorption (Qst) of 67.5 kJ mol−1 validated through in situ pressure gradient differential scanning calorimetry (PG-DSC). Further, in situ characterisation and DFT calculations provide insight into the mechanism of the C2H2 induced fit transformation, binding positions and the nature of host-guest and guest-guest interactions.

KW - CH/CH and CH/CO separation

KW - coordination polymers

KW - induced fit mechanism

KW - physisorption

KW - ultramicroporous materials

UR - http://www.scopus.com/inward/record.url?scp=85112642380&partnerID=8YFLogxK

U2 - 10.1002/anie.202106263

DO - 10.1002/anie.202106263

M3 - Article

C2 - 34250717

AN - SCOPUS:85112642380

SN - 1433-7851

VL - 60

SP - 20383

EP - 20390

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 37

ER -

Benchmark Acetylene Binding Affinity and Separation through Induced Fit in a Flexible Hybrid Ultramicroporous Material

Abstract

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this