Hierarchically porous metal organic framework immobilized formate dehydrogenase for enzyme electrocatalytic CO2 reduction

Yan, Lihang; Liu, Guanhua; Liu, Jianqiao; Bai, Jing; Li, Yaoxuan; Chen, Huaxun; Zhou, Liya; Gao, Jing; Jiang, Yanjun

doi:10.1016/j.cej.2022.138164

Cited by 20 publications

(7 citation statements)

References 62 publications

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“…As shown in Figure a, the CVs of the Rh complex were recorded in the potential range from −2.0 to 0 V ( vs Ag/AgCl). The reductive current peak of the Rh complex significantly increased from −1.72 to −2.32 mA cm –2 when NAD + was added to the system, implying the occurrence of NAD + reduction . In addition, no reduction peak or oxidation peaks were detected, and the current density was extremely low on the bare amino-group-functionalized electrode.…”

Section: Resultsmentioning

confidence: 96%

“…The reductive current peak of the Rh complex significantly increased from −1.72 to −2.32 mA cm −2 when NAD + was added to the system, implying the occurrence of NAD + reduction. 52 In addition, no reduction peak or oxidation peaks were detected, and the current density was extremely low on the bare amino-groupfunctionalized electrode. The aforementioned phenomena indicated that NADH regeneration was a two-step process.…”

Section: Molecular Docking Simulationsmentioning

confidence: 98%

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Electroenzymatic Reduction of Furfural to Furfuryl Alcohol by an Electron Mediator and Enzyme Orderly Assembled Biocathode

Zhan

Liu

Zhang

et al. 2023

ACS Appl. Mater. Interfaces

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The electroenzymatic valorization of biomass derivatives into valuable biochemicals has a promising outlook. However, bottlenecks including poor electron transfer between the electrode surface and oxidoreductase, inefficient regeneration of cofactors, and high cost of enzymes and electron mediators hindered the realistic applications of the technique. Herein, to address the above technical barriers, a novel bio-electrocatalytic system that integrates the electrochemical NADH regeneration and enzymatic reaction was constructed, using an orderly assembled composite bioelectrode consisting of an outer immobilized enzyme layer and a sandwiched redox mediator rhodium complex layer. The as-prepared composite bioelectrode was further applied for the highly selective hydrogenation of furfural into furfural alcohol. Results indicated that the enzyme activity was significantly improved, while the furfural valorization was promoted by effective interfacial electron transition and co-factor regeneration on the composite bioelectrode. Considerable high furfural conversion (96.4%) can be achieved accompanied by a furfural alcohol selectivity of 90.0% at −1.2 V (vs Ag/AgCl). The novel composite bioelectrode also showed good stability and reusability. Up to 85.1% of the original furfural alcohol selectivity can be preserved after 10 times of recycling. This work presents a promising green alternative for the valorization of furfural, which also shows great potential extending to the valorization of other biomass compounds.

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Section: Resultsmentioning

confidence: 96%

Section: Molecular Docking Simulationsmentioning

confidence: 98%

Electroenzymatic Reduction of Furfural to Furfuryl Alcohol by an Electron Mediator and Enzyme Orderly Assembled Biocathode

Zhan

Liu

Zhang

et al. 2023

ACS Appl. Mater. Interfaces

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“…Even the thermal stability of CL@HMSS-SP is comparable to that of commercial Novozym 435. The hydroxyl group of silica spheres forms a hydrogen bond with the protein to further stabilize the structure of the lipase and prevent conformational changes caused by thermal denaturation. , All of these features lay a good foundation for the construction of subsequent interfacial biocatalysis.…”

Section: Resultsmentioning

confidence: 99%

Ultraviolet/Visible Light-Responsive Pickering Interfacial Biocatalysis: Efficient and Robust Platform for Bioconversions

Zhong,

Zhang,

Gong

et al. 2023

ACS Sustainable Chem. Eng.

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Stimuli-responsive Pickering interfacial biocatalysis (PIB) platforms are highly desirable due to their convenient product extraction and catalyst recovery. Light-responsive PIB stabilized by immobilized biocatalyst particles, which serve as both emulsifiers and catalysts, have not attracted enough attention. Herein, a novel and effective ultraviolet/visible light-responsive PIB system is proposed to facilitate reversible emulsification/demulsification. The modified hollow mesoporous silica nanospheres (HMSS-N) with photochromic spiropyran (SP-COOH) were utilized as a light-responsive emulsifier and carrier of lipase CL (CL@HMSS-SP). The light-responsive performance and catalytic performance of the PIB system were also studied in detail. As a result, the O/W emulsion demulsification or emulsification could be easily accomplished by inducing ultraviolet or visible light to change the surface wettability of the smart emulsifiers. The system exhibited the highest catalytic activity in the model esterification reaction between n-hexanol acid and 1-hexanol that has been reported so far (a catalytic efficiency value of 80.9 mmol g −1 h −1 ), which is a 12.6-fold enhancement compared with the conventional free enzyme one-phase system. The robust system maintained high catalytic activity even after 10 cycles, averaging 148.2 g of product g −1 biocatalyst. Thus, the ultraviolet/visible light-responsive PIB gives insights into the biocatalytic synthesis of flavor esters with high efficiency and stable reusability and shows great potential for cleaner production in the future.

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“…[7] As a result, the decomposition of CO 2 is an arduous and energy-intensive task when conventional methods are employed. Currently, numerous methods such as biocatalysis, [8,9] thermocatalysis, [10][11][12] photocatalysis, [13][14][15] and electrocatalysis [16][17][18] have been investigated with promising outcomes for CO 2 reduction. The process of biocatalysis involves the use of enzymes that are less stable and prone to deactivation.…”

Section: Introductionmentioning

confidence: 99%

Recent advances in novel materials for photocatalytic carbon dioxide reduction

Lu,

Zhang,

Liu

et al. 2024

Carbon Neutralization

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The conversion of CO2 into chemical fuels, which can be stored and utilized through photocatalysis, represents an effective, environmentally friendly, and sustainable means to address both environmental concerns and energy shortages. CO2, as a stable oxidation product, poses challenges for reduction through light energy alone, necessitating the use of catalysts. Thus, a crucial aspect of CO2 photocatalytic reduction technology lies in the development of effective photocatalysts. Based on the basic principle of PCRR (photocatalytic CO2 reduction reaction), the review provides a detailed introduction to the core issues in PCRR process, including the relationship between band gap and catalyst reduction performance, effective utilization of photogenerated carriers, product selectivity, and methods for product analysis. Then, the recent research progresses of various photocatalysts are reviewed in the form of research examples combined with the above basic principles. Finally, this review summarizes and provides insights into the effective techniques for enhancing the photocatalytic activity of CO2, while also offering future prospects in this field.

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Hierarchically porous metal organic framework immobilized formate dehydrogenase for enzyme electrocatalytic CO2 reduction

Cited by 20 publications

References 62 publications

Electroenzymatic Reduction of Furfural to Furfuryl Alcohol by an Electron Mediator and Enzyme Orderly Assembled Biocathode

Electroenzymatic Reduction of Furfural to Furfuryl Alcohol by an Electron Mediator and Enzyme Orderly Assembled Biocathode

Ultraviolet/Visible Light-Responsive Pickering Interfacial Biocatalysis: Efficient and Robust Platform for Bioconversions

Recent advances in novel materials for photocatalytic carbon dioxide reduction

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