Electrochemical conversion of carbon dioxide to methanol with the assistance of formate dehydrogenase and methanol dehydrogenase as biocatalysts

Kuwabata, Susumu; Tsuda, Ryo; Yoneyama, Hiroshi

doi:10.1021/ja00091a056

Cited by 134 publications

(83 citation statements)

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“…Notably, there have also been reports on the use of enzymes as catalysts toward the electrolytic conversion of CO 2 . However, the reaction conditions for the enzymatic conversion of CO 2 should be restricted to neutral pH and mild temperatures, as otherwise, the enzymes would easily become unstable and inactive [22][23][24].…”

Section: Introductionmentioning

confidence: 99%

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Choi

Jung

Yoo

et al. 2017

Journal of Electrochemical Science and Technology

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Electrochemical conversion of CO 2 and production of H 2 were attempted on a three-dimensionally ordered, porous metal organic framework (MOF-74) in which transition metals (Co, Ni, and Zn) were impregnated. A lab-scale proton exchange membrane-based electrolyzer was fabricated and used for the reduction of CO 2 . Real-time gas chromatography enabled the instantaneous measurement of the amount of carbon monoxide and hydrogen produced. Comprehensive calculations, based on electrochemical measurements and gaseous product analysis, presented a time-dependent selectivity of the produced gases. M-MOF-74 samples with different central metals were successfully obtained because of the simple synthetic process. It was revealed that Co-and Ni-MOF-74 selectively produce hydrogen gas, while Zn-MOF-74 successfully generates a mixture of carbon monoxide and hydrogen. The results indicated that M-MOF-74 can be used as an electrocatalyst to selectively convert CO 2 into useful chemicals.

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Section: Introductionmentioning

confidence: 99%

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Choi

Jung

Yoo

et al. 2017

Journal of Electrochemical Science and Technology

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“…However, when the authors attempted to use NAD + immobilization, the conversion dropped drastically to 5%, indicating some diffusional limitation of the redox process in the system Therefore, since the immobilized FDH, FalDH and ADH species exhibit outstanding stability and activity, the NAD + /NADH regeneration systems become a critical issue for improving the methanol synthesis. For this reason, several groups (Kuwabata et al 1994, Schlager et al 2016, Singh et al 2017, Dibenedetto et al 2012) have been focusing their research at this front, using different strategies, such as a phosphite dehydrogenase (PTDH) system, a glycerol dehydrogenase system or a natural photosystem from spinach leaves (chloroplasts). The phosphite dehydrogenase system was the most efficient one, working at pH 7 and yielding 4.3 mmol (g commercial enzymatic powder ) −1 after 3 h reaction (Cazelles et al 2013).…”

Section: Merging the Immobilized Enzymes In Catalysismentioning

confidence: 99%

Carbon dioxide/methanol conversion cycle based on cascade enzymatic reactions supported on superparamagnetic nanoparticles

Netto

Andrade

Toma

2017

An. Acad. Bras. Ciênc.

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The conversion of carbon dioxide into important industrial feedstock is a subject of growing interest in modern society. A possible way to achieve this goal is by carrying out the CO 2 /methanol cascade reaction, allowing the recycle of CO 2 using either chemical catalysts or enzymes. Efficient and selective reactions can be performed by enzymes; however, due to their low stability, immobilization protocols are required to improve their performance. The cascade reaction to reduce carbon dioxide into methanol has been explored by the authors, using, sequentially, alcohol dehydrogenase (ADH), formaldehyde dehydrogenase (FalDH), and formate dehydrogenase (FDH), powered by NAD + /NADH and glutamate dehydrogenase (GDH) as the co-enzyme regenerating system. All the enzymes have been immobilized on functionalized magnetite nanoparticles, and their reactions investigated separately in order to establish the best performance conditions. Although the stepwise scheme led to only 2.3% yield of methanol per NADH; in a batch system under CO 2 pressure, the combination of the four immobilized enzymes increased the methanol yield by 64 fold. The studies indicated a successful regeneration of NADH in situ, envisaging a real possibility of using immobilized enzymes to perform the cascade CO 2 -methanol reaction.

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“…The feasibility of using isolated enzymes to convert CO 2 to malic, aspartic, isocitric, and formic acids has been demonstrated over two decades ago (Parkinson and Weaver, 1984;Ruschig et al, 1976). As a result of the growing concerns of the environment's well-being, the formate dehydrogenase (FDH)-catalyzed CO 2 reduction has been examined more extensively in recent years as a promising approach to greenhouse gas fixation and the production of renewable fuels and chemicals (Dave, 2000;Kuwabata et al, 1994;Neuhauser et al, 1998;Obert and Dave, 1999). The production of methanol from CO 2 through the use of multienzyme systems (without cofactor regeneration) has also been demonstrated (Kuwabata et al, 1994).…”

Section: Introductionmentioning

confidence: 99%

“…As a result of the growing concerns of the environment's well-being, the formate dehydrogenase (FDH)-catalyzed CO 2 reduction has been examined more extensively in recent years as a promising approach to greenhouse gas fixation and the production of renewable fuels and chemicals (Dave, 2000;Kuwabata et al, 1994;Neuhauser et al, 1998;Obert and Dave, 1999). The production of methanol from CO 2 through the use of multienzyme systems (without cofactor regeneration) has also been demonstrated (Kuwabata et al, 1994). Similar to many other enzymatic redox reactions, the enzymatic reduction of CO 2 requires cofactors such as NADH, pyrroloquinolinequinone, and methyl viologen to function as electron donors (Neuhauser et al, 1998).…”

Section: Introductionmentioning

confidence: 99%

Particle‐tethered NADH for production of methanol from CO₂ catalyzed by coimmobilized enzymes

El‐Zahab¹,

Donnelly²,

Wang³

2007

Biotech & Bioengineering

172

120

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Efficient cofactor regeneration and reuse are highly desired for many important biotransformation applications. Here we show for the first time that cofactor NAD(H) covalently attached to micro particles, which can be easily recovered and reused, effectively mediated multistep reactions catalyzed by enzymes that were also immobilized with the micro particles. Such an immobilized enzyme-cofactor catalytic system was examined for the production of methanol from CO(2) with in situ cofactor regeneration. Four enzymes including formate, formaldehyde, alcohol, and glutamate dehydrogenases were coimmobilized using the same particles as that used for cofactor immobilization (enzymes and cofactor were immobilized separately). Reactions were performed by bubbling CO(2) in a suspension solution of the particle-attached enzymes and cofactor. It appeared that the collision among the particles afforded sufficient interactions between the cofactor and enzymes, and thus enabled the sequential transformation of CO(2) to methanol along with cofactor regeneration. For a 30-min batch reaction, a productivity of 0.02 micromol methanol/h/g-enzyme was achieved. That was lower than but comparable to the 0.04 micromol methanol/h/g-enzyme observed for free enzymes and cofactor at the same reaction conditions. The immobilized system showed fairly good stabilities in reusing. Over 80% of their original productivity was retained after 11 reusing cycles, with a cumulative methanol yield based on the amount of cofactor reached 127%. That was a promising enhancement in cofactor utilization as compared to the single-batch yield of 12% observed with free enzymes and free cofactor.

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Electrochemical conversion of carbon dioxide to methanol with the assistance of formate dehydrogenase and methanol dehydrogenase as biocatalysts

Cited by 134 publications

References 0 publications

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Carbon dioxide/methanol conversion cycle based on cascade enzymatic reactions supported on superparamagnetic nanoparticles

Particle‐tethered NADH for production of methanol from CO₂ catalyzed by coimmobilized enzymes

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Electrochemical conversion of carbon dioxide to methanol with the assistance of formate dehydrogenase and methanol dehydrogenase as biocatalysts

Cited by 134 publications

References 0 publications

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO2 Conversion and H2 Production

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO2 Conversion and H2 Production

Carbon dioxide/methanol conversion cycle based on cascade enzymatic reactions supported on superparamagnetic nanoparticles

Particle‐tethered NADH for production of methanol from CO2 catalyzed by coimmobilized enzymes

Contact Info

Product

Resources

About

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Facile Synthesis of M-MOF-74 (M=Co, Ni, Zn) and its Application as an ElectroCatalyst for Electrochemical CO₂ Conversion and H₂ Production

Particle‐tethered NADH for production of methanol from CO₂ catalyzed by coimmobilized enzymes