Efficient ionic liquid-based platform for multi-enzymatic conversion of carbon dioxide to methanol

Zhibo Zhang, Jan Muschiol, Yuhong Huang, Sigyn Björk Sigurdardóttir, Nicolas von Solms, Anders E. Daugaard, Jiang Wei, Jianquan Luo, Bao-Hua Xu, Suojiang Zhang, Manuel Pinelo*

*Corresponding author for this work

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Abstract

Low yields commonly obtained during enzymatic conversion of CO2 to methanol are attributed to low CO2 solubility in water. In this study, four selected ionic liquids with high CO2 solubility were separately added to the multi-enzyme reaction mixture and the yields were compared to the pure aqueous system (control). In an aqueous 20% [CH][Glu] system, yield increased ca. 3.5-fold compared to the control (ca. 5-fold if NADH regeneration was incorporated). Molecular dynamics simulation revealed that CO2 remains for longer in a productive conformation in the enzyme in the presence of [CH][Glu], which explains the marked increase of yield that was also confirmed by isothermal titration calorimetry – lower energy (ΔG) binding of CO2 to FDH. The results suggest that the accessibility of CO2 to the enzyme active site depends on the absence/presence and nature of the ionic liquid, and that the enzyme conformation determines CO2 retention and hence final conversion.
Original languageEnglish
JournalGreen Chemistry
Volume20
Issue number18
Pages (from-to)4339-4348
ISSN1463-9262
DOIs
Publication statusPublished - 2018

Bibliographical note

Electronic supplementary information (ESI) available. See DOI: 10.1039/c8gc02230e

Cite this

@article{dd9a5b4fa6444b8b85967f447b206209,
title = "Efficient ionic liquid-based platform for multi-enzymatic conversion of carbon dioxide to methanol",
abstract = "Low yields commonly obtained during enzymatic conversion of CO2 to methanol are attributed to low CO2 solubility in water. In this study, four selected ionic liquids with high CO2 solubility were separately added to the multi-enzyme reaction mixture and the yields were compared to the pure aqueous system (control). In an aqueous 20{\%} [CH][Glu] system, yield increased ca. 3.5-fold compared to the control (ca. 5-fold if NADH regeneration was incorporated). Molecular dynamics simulation revealed that CO2 remains for longer in a productive conformation in the enzyme in the presence of [CH][Glu], which explains the marked increase of yield that was also confirmed by isothermal titration calorimetry – lower energy (ΔG) binding of CO2 to FDH. The results suggest that the accessibility of CO2 to the enzyme active site depends on the absence/presence and nature of the ionic liquid, and that the enzyme conformation determines CO2 retention and hence final conversion.",
author = "Zhibo Zhang and Jan Muschiol and Yuhong Huang and Sigurdard{\'o}ttir, {Sigyn Bj{\"o}rk} and {von Solms}, Nicolas and Daugaard, {Anders E.} and Jiang Wei and Jianquan Luo and Bao-Hua Xu and Suojiang Zhang and Manuel Pinelo",
note = "Electronic supplementary information (ESI) available. See DOI: 10.1039/c8gc02230e",
year = "2018",
doi = "10.1039/c8gc02230e",
language = "English",
volume = "20",
pages = "4339--4348",
journal = "Green Chemistry",
issn = "1463-9262",
publisher = "Royal Society of Chemistry",
number = "18",

}

Efficient ionic liquid-based platform for multi-enzymatic conversion of carbon dioxide to methanol. / Zhang, Zhibo; Muschiol, Jan; Huang, Yuhong; Sigurdardóttir, Sigyn Björk; von Solms, Nicolas; Daugaard, Anders E.; Wei, Jiang; Luo, Jianquan; Xu, Bao-Hua; Zhang, Suojiang; Pinelo, Manuel.

In: Green Chemistry, Vol. 20, No. 18, 2018, p. 4339-4348.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Efficient ionic liquid-based platform for multi-enzymatic conversion of carbon dioxide to methanol

AU - Zhang, Zhibo

AU - Muschiol, Jan

AU - Huang, Yuhong

AU - Sigurdardóttir, Sigyn Björk

AU - von Solms, Nicolas

AU - Daugaard, Anders E.

AU - Wei, Jiang

AU - Luo, Jianquan

AU - Xu, Bao-Hua

AU - Zhang, Suojiang

AU - Pinelo, Manuel

N1 - Electronic supplementary information (ESI) available. See DOI: 10.1039/c8gc02230e

PY - 2018

Y1 - 2018

N2 - Low yields commonly obtained during enzymatic conversion of CO2 to methanol are attributed to low CO2 solubility in water. In this study, four selected ionic liquids with high CO2 solubility were separately added to the multi-enzyme reaction mixture and the yields were compared to the pure aqueous system (control). In an aqueous 20% [CH][Glu] system, yield increased ca. 3.5-fold compared to the control (ca. 5-fold if NADH regeneration was incorporated). Molecular dynamics simulation revealed that CO2 remains for longer in a productive conformation in the enzyme in the presence of [CH][Glu], which explains the marked increase of yield that was also confirmed by isothermal titration calorimetry – lower energy (ΔG) binding of CO2 to FDH. The results suggest that the accessibility of CO2 to the enzyme active site depends on the absence/presence and nature of the ionic liquid, and that the enzyme conformation determines CO2 retention and hence final conversion.

AB - Low yields commonly obtained during enzymatic conversion of CO2 to methanol are attributed to low CO2 solubility in water. In this study, four selected ionic liquids with high CO2 solubility were separately added to the multi-enzyme reaction mixture and the yields were compared to the pure aqueous system (control). In an aqueous 20% [CH][Glu] system, yield increased ca. 3.5-fold compared to the control (ca. 5-fold if NADH regeneration was incorporated). Molecular dynamics simulation revealed that CO2 remains for longer in a productive conformation in the enzyme in the presence of [CH][Glu], which explains the marked increase of yield that was also confirmed by isothermal titration calorimetry – lower energy (ΔG) binding of CO2 to FDH. The results suggest that the accessibility of CO2 to the enzyme active site depends on the absence/presence and nature of the ionic liquid, and that the enzyme conformation determines CO2 retention and hence final conversion.

U2 - 10.1039/c8gc02230e

DO - 10.1039/c8gc02230e

M3 - Journal article

VL - 20

SP - 4339

EP - 4348

JO - Green Chemistry

JF - Green Chemistry

SN - 1463-9262

IS - 18

ER -