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

Zhang, Zhibo; Muschiol, Jan; Huang, Yuhong; Sigurdardóttir, Sigyn Björk; Solms, Nicolas von; Daugaard, Anders Egede; Wei, Jiang; Luo, Jianquan; Xu, Bao‐Hua; Zhang, Suojiang; Pinelo, Manuel

doi:10.1039/c8gc02230e

Cited by 69 publications

(56 citation statements)

References 48 publications

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“…et al, 2012; Fixen et al, 2016; Shah and Imae, 2017; Cai et al, 2018; Liu et al, 2018), or photocatalyst/biocatalyst integrated systems (Yadav et al, 2014). Compared with other methods, the transformation of CO 2 to methanol by enzymatic catalysis is preferable due to the significant advantages of high selectivity and specificity, high efficiency, and mild operational conditions (Obert and Dave, 1999; Wang X. et al, 2014; Ji et al, 2015; Kuk et al, 2017; Nabavi Zadeh et al, 2018; Zhang Z. et al, 2018).…”

Section: Introductionmentioning

confidence: 99%

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Wen

Tan

et al. 2019

Front. Bioeng. Biotechnol.

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The main challenges in multienzymatic cascade reactions for CO2 reduction are the low CO2 solubility in water, the adjustment of substrate channeling, and the regeneration of co-factor. In this study, metal-organic frameworks (MOFs) were prepared as adsorbents for the storage of CO2 and at the same time as solid supports for the sequential co-immobilization of multienzymes via a layer-by-layer self-assembly approach. Amine-functionalized MIL-101(Cr) was synthesized for the adsorption of CO2. Using amine-MIL-101(Cr) as the core, two HKUST-1 layers were then fabricated for the immobilization of three enzymes chosen for the reduction of CO2 to formate. Carbonic anhydrase was encapsulated in the inner HKUST-1 layer and hydrated the released CO2 to HCO3-. Bicarbonate ions then migrated directly to the outer HKUST-1 shell containing formate dehydrogenase and were converted to formate. Glutamate dehydrogenase on the outer MOF layer achieved the regeneration of co-factor. Compared with free enzymes in solution using the bubbled CO2 as substrate, the immobilized enzymes using stored CO2 as substrate exhibited 13.1-times higher of formate production due to the enhanced substrate concentration. The sequential immobilization of enzymes also facilitated the channeling of substrate and eventually enabled higher catalytic efficiency with a co-factor-based formate yield of 179.8%. The immobilized enzymes showed good operational stability and reusability with a cofactor cumulative formate yield of 1077.7% after 10 cycles of reusing.

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Section: Introductionmentioning

confidence: 99%

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Wen

Tan

et al. 2019

Front. Bioeng. Biotechnol.

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“…A sustainable solution to cope with the emission of CO 2 to the atmosphere has been recently proposed by means of the enzymatic conversion of CO 2 into methanol in the presence of ILs (Figure ) . Previously the analogue enzymatic process in aqueous medium had rendered low production of methanol (44 %) due to unfavorable kinetics in the starting reduction of CO 2 into formic acid mediated by formate dehydrogenase (FDH).…”

Section: Enzymatic Cascades For the Valorization Of Bioresourcesmentioning

confidence: 99%

Non‐Conventional Media as Strategy to Overcome the Solvent Dilemma in Chemoenzymatic Tandem Catalysis

Kourist

González‐Sabín

2020

ChemCatChem

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The amazing potential of multi‐catalytic cascade reactions to reduce the number of reaction steps and to solve synthetic problems brings the challenge of an increasing complexity that must be controlled. Particularly chemo‐enzymatic reactions are prone to conflicts regarding different optimal reaction conditions for chemical and biological catalysts. The preference of many chemical catalysts for hydrophobic (and often water‐free) solvent and of many enzymes for water poses a solvent dilemma. Recently, non‐conventional solvents have been very successful to provide suitable reaction media for catalysts that otherwise require very different solvents, and to alleviate fundamental problems such as the low solubility of many substrates in aqueous solvents. In the last few years, several examples underlined the considerable potential of ionic liquids and deep eutectic solvents for the engineering of cascade reactions. This mini‐review showcases the recent developments on the implementation of the so‐called non‐conventional media in such processes.

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“…firstly coimmobilized formate dehydrogenase, formaldehyde dehydrogenase, and alcohol dehydrogenase in a polymeric membrane by reverse filtration, and the resultant biocatalytic membrane achieved the bioconversion of CO 2 to methanol (0.5 mM) [8]. Using a suitable ionic liquid as buffer solution, methanol yield increased by 3.5‐fold due to higher CO 2 solubility in the biocatalytic membrane system [37]. Zhu et al.…”

Section: Applications Of Biocatalytic Membranementioning

confidence: 99%

Biocatalytic membrane: Go far beyond enzyme immobilization

Luo

Song

Zhang

et al. 2020

Engineering in Life Sciences

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Biocatalytic membrane takes advantages of reaction–separation integration as well as enzyme immobilization, which has attracted increasing attentions in online detection and biomanufacturing. However, the high preparation cost, inferior comprehensive performance, and low stability limit its applications. Thus, besides enzyme immobilization, more efforts should be made in biocatalytic membrane configuration design for a specific application to enhance the synergistic effect of reaction and separation and improve its operating stability. This review summarized the recent progress on biocatalytic membrane preparation, discussed different membrane configurations for various applications, finally proposed several challenges and possible solutions, which provided directions and guides for the development and industrialization of biocatalytic membrane.

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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.

Cited by 69 publications

References 48 publications

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Non‐Conventional Media as Strategy to Overcome the Solvent Dilemma in Chemoenzymatic Tandem Catalysis

Biocatalytic membrane: Go far beyond enzyme immobilization

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