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

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

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Keywords

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

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10.1002/anie.202106263

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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",

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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 - https://www.scopus.com/pages/publications/85112642380

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

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Keywords

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