Biocatalytic and Bioelectrocatalytic Approaches for the Reduction of Carbon Dioxide using Enzymes

Schlager, Stefanie; Dibenedetto, Angela; Aresta, Michele; Apaydın, Doğukan Hazar; Dumitru, Liviu Mihai; Neugebauer, Helmut; Sariciftci, Niyazi Serdar

doi:10.1002/ente.201600610

Cited by 71 publications

(51 citation statements)

References 85 publications

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“…Organic electro‐catalysts made their appearance as potentially viable CO 2 reduction catalysts in the early 1990s, with Bocarsly and co‐workers pioneering the use of pyridine molecules in a homogenous media to reduce CO 2 to methanol with FE toward CH 3 OH of 30%. However, at the time and until recently, pyridine catalysts have not been very stable upon electrolysis and are prone to degradation . Additionally, only until late, there had not been viable recycling methods for the catalyst as its reduction mechanism had been under heavy debate …”

Section: Metal‐free Organic Catalystsmentioning

confidence: 99%

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Elouarzaki

Kannan

Jose

et al. 2019

Advanced Energy Materials

161

102

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provides a promising alternative to hydrocarbon sources for petrochemical feedstock. Thanks to the electrochemical nature of the CO 2 conversion to fuels and chemicals, the electrical energy invested to convert CO 2 in the form of a chemical fuel can be stored and redistributed using established supply chains for future use. Additionally, the integration of renewable energy systems (green electricity) into the grid can potentially create a carbon neutral energy cycle, and when driven by solar energy, offers a completely renewable energy cycle or negative carbon technology. Converting CO 2 electrochemically into compounds with high energy densities, such as alcohols (methanol, ethanol), formates, and CO, represents a form of energy storage and is also adaptable to demand response or energy arbitrage technologies. [3][4][5][6][7] The recoverable energy density of the chemicals that can be converted from CO 2 is substantially higher than most battery technologies.Given CO 2 electroreduction's immense economic and environmental potential, it has been the subject of much research activity over the past decades. [8][9][10][11] One of the greatest challenges of reducing CO 2 in an electrochemical cell is overcoming the immense energy barrier required to do so; the single electron reduction of CO 2 to CO 2 −˙, a common step in many CO 2 reduction mechanisms, requires an applied potential of −1.97 V measured versus standard hydrogen electrode (SHE). To alleviate this problem, many catalytic cathodes have been developed to avoid this intermediate and to reroute the reduction mechanism through alternate pathways requiring much lower applied potentials (a necessity if CO 2 electroreduction is to be implemented at industrial scale). [12][13][14] However, despite the low potentials offered by catalytic electrodes, the cost of electrodes is not always viable when upscaled to industrial levels. [15,16] Therefore, recent research trends in electrocatalytic reduction of CO 2 have been shifting toward the development of molecular catalysts that can exist as either solutes in electrolytes or can be surface-confined on electrodes. [13,16] The tunable nature and electronic characteristics of molecular catalysts give access to a large variety of catalysts with high activity, selectivity, and durability, as well as their ability to be integrated into sophisticated nanoassemblies. [17][18][19] Thanks to the aforementioned proprieties, performing CO 2 reduction using molecularly defined compounds offer several advantages compared to classical solid-state counterparts. Molecular catalysts usually exhibit well-defined homogeneous and/or CO 2 reduction using molecular catalysts is a key area of study for achieving electrical-to-chemical energy storage and feedstock chemical synthesis. Compared to classical metallic solid-state catalysts, these molecular catalysts often result in high performance and selectivity, even under unfavorable aqueous environments. This review considers the recent state-of-the-art molecular catalysts for CO 2 electro...

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Section: Metal‐free Organic Catalystsmentioning

confidence: 99%

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Elouarzaki

Kannan

Jose

et al. 2019

Advanced Energy Materials

161

102

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“…In the enzymatic approach, dehydrogenase enzymes have been reported as efficient catalysts for the CO 2 conversion to alcohols, aldehydes and other hydrocarbons . Generally, these dehydrogenase enzymes only catalyze specific reactions with the requirement of a sacrificial cofactor . For example, formate dehydrogenase (FDH) is known to catalyze the reduction of CO 2 to formate with the aid of nicotinamide adenine dinucleotide (NADH) as a cofactor .…”

Section: Introductionmentioning

confidence: 99%

Enhanced Bio‐Electrochemical Reduction of Carbon Dioxide by Using Neutral Red as a Redox Mediator

et al. 2019

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Microbial electrosynthetic cells containing Methylobacterium extorquens were studied for the reduction of CO2 to formate by direct electron injection and redox mediator‐assisted approaches, with CO2 as the sole carbon source. The formation of a biofilm on a carbon felt (CF) electrode was achieved while applying a constant potential of −0.75 V versus Ag/AgCl under CO2‐saturated conditions. During the biofilm growth period, continuous H2 evolution was observed. The long‐term performance for CO2 reduction of the biofilm with and without neutral red as a redox mediator was studied by an applied potential of −0.75 V versus Ag/AgCl. The neutral red was introduced into the systems in two different ways: homogeneous (dissolved in solution) and heterogeneous (electropolymerized onto the working electrode). The heterogeneous approach was investigated in the microbial system, for the first time, where the CF working electrode was coated with poly(neutral red) by the oxidative electropolymerization thereof. The formation of poly(neutral red) was characterized by spectroscopic techniques. During long‐term electrolysis up to 17 weeks, the formation of formate was observed continuously with an average Faradaic efficiency of 4 %. With the contribution of neutral red, higher formate accumulation was observed. Moreover, the microbial electrosynthetic cell was characterized by means of electrochemical impedance spectroscopy to obtain more information on the CO2 reduction mechanism.

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“…The combination of enzymes and photocatalysts for CO 2 conversion has attracted increasing attention because it makes full use of the abundant energy supply of solar light and high specificity of enzyme catalysis [ 108 , 109 , 110 ]. These reactions can be conducted at mild conditions similar to the photosynthesis that occurs in plants or certain bacteria.…”

Section: Catalytic Reduction Of Comentioning

confidence: 99%

Research Progress in Conversion of CO2 to Valuable Fuels

Xiu

Liu

et al. 2020

Molecules

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Rapid growth in the world’s economy depends on a significant increase in energy consumption. As is known, most of the present energy supply comes from coal, oil, and natural gas. The overreliance on fossil energy brings serious environmental problems in addition to the scarcity of energy. One of the most concerning environmental problems is the large contribution to global warming because of the massive discharge of CO2 in the burning of fossil fuels. Therefore, many efforts have been made to resolve such issues. Among them, the preparation of valuable fuels or chemicals from greenhouse gas (CO2) has attracted great attention because it has made a promising step toward simultaneously resolving the environment and energy problems. This article reviews the current progress in CO2 conversion via different strategies, including thermal catalysis, electrocatalysis, photocatalysis, and photoelectrocatalysis. Inspired by natural photosynthesis, light-capturing agents including macrocycles with conjugated structures similar to chlorophyll have attracted increasing attention. Using such macrocycles as photosensitizers, photocatalysis, photoelectrocatalysis, or coupling with enzymatic reactions were conducted to fulfill the conversion of CO2 with high efficiency and specificity. Recent progress in enzyme coupled to photocatalysis and enzyme coupled to photoelectrocatalysis were specially reviewed in this review. Additionally, the characteristics, advantages, and disadvantages of different conversion methods were also presented. We wish to provide certain constructive ideas for new investigators and deep insights into the research of CO2 conversion.

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Biocatalytic and Bioelectrocatalytic Approaches for the Reduction of Carbon Dioxide using Enzymes

Cited by 71 publications

References 85 publications

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Enhanced Bio‐Electrochemical Reduction of Carbon Dioxide by Using Neutral Red as a Redox Mediator

Research Progress in Conversion of CO2 to Valuable Fuels

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Biocatalytic and Bioelectrocatalytic Approaches for the Reduction of Carbon Dioxide using Enzymes

Cited by 71 publications

References 85 publications

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO2 by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO2 by Molecular Catalysts

Enhanced Bio‐Electrochemical Reduction of Carbon Dioxide by Using Neutral Red as a Redox Mediator

Research Progress in Conversion of CO2 to Valuable Fuels

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Product

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Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts