Single catalyst electrocatalytic reduction of CO2in water to H2+CO syngas mixtures with water oxidation to O2

Kang, Peng; Chen, Zuofeng; Nayak, Animesh; Zhang, Sheng; Meyer, Thomas J.

doi:10.1039/c4ee01904k

Cited by 122 publications

(109 citation statements)

References 47 publications

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“…Cu-ZnO/GaN/n +− p Si was recently reported as a highly efficient PEC catalyst to produce syngas with a tunable H 2 /CO ratio (between 1:2 and 4:1) 5 . Metal or metal-based composites, including Ag 9 , Cu 10 , Ru(II) polypyridyl complex 11 , Ag/C 3 N 4 12 , and Re-functionalized graphene oxide 13 , have been investigated for EC reduction of CO 2 and H + /H 2 O to syngas. The different methods used to tune the ratio of H 2 /CO include altering the CO 2 flow rate 14 and pressure 15 , the reaction temperature 16 , and the applied potential 9 .…”

Section: Introductionmentioning

confidence: 99%

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

et al. 2017

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Syngas, a CO and H2 mixture mostly generated from non-renewable fossil fuels, is an essential feedstock for production of liquid fuels. Electrochemical reduction of CO2 and H+/H2O is an alternative renewable route to produce syngas. Here we introduce the concept of coupling a hydrogen evolution reaction (HER) catalyst with a CDots/C3N4 composite (a CO2 reduction catalyst) to achieve a cheap, stable, selective and efficient route for tunable syngas production. Co3O4, MoS2, Au and Pt serve as the HER component. The Co3O4-CDots-C3N4 electrocatalyst is found to be the most efficient among the combinations studied. The H2/CO ratio of the produced syngas is tunable from 0.07:1 to 4:1 by controlling the potential. This catalyst is highly stable for syngas generation (over 100 h) with no other products besides CO and H2. Insight into the mechanisms balancing between CO2 reduction and H2 evolution when applying the HER-CDots-C3N4 catalyst concept is provided.

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Section: Introductionmentioning

confidence: 99%

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

et al. 2017

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“…Previous reports have focused on monometallic molecular and heterogeneous catalytic systems, which have been used for simultaneous production of CO and H 2 . However, single catalytic sites offer limited possibilities for selective tuning of the catalyst.…”

Section: Introductionmentioning

confidence: 99%

Zn–Cu Alloy Nanofoams as Efficient Catalysts for the Reduction of CO₂ to Syngas Mixtures with a Potential‐Independent H₂/CO Ratio

Lamaison

Wakerley

Montero³

et al. 2019

ChemSusChem

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Alloying strategies are commonly used to design electrocatalysts that take on properties of their constituent elements. Herein, such a strategy is used to develop Zn–Cu alloyed electrodes with unique hierarchical porosity and tunable selectivity for CO2 versus H+ reduction. By varying the Zn/Cu ratio, tailored syngas mixtures are obtained without the production of other gaseous products, which is attributed to preferential CO‐ and H2‐forming pathways on the alloys. The syngas ratios are also significantly less sensitive to the applied potential in the alloys relative to pure metal equivalents; an essential quality when coupling electrocatalysis with renewable power sources that have fluctuating intensity. As such, industrially relevant syngas ratios are achieved at large currents (−60 mA) for extensive operating times (>9 h), demonstrating the potential of this strategy for fossil‐free fuel production.

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“…Indeed, a previous attempt showed poor CO 2 /H 2 selectivity and practically no catalytic effect in cyclic voltammetry (37). In the same vein, Ni cyclam seems to be a selective and efficient catalyst of the CO 2 -to-CO conversion in water under the condition of being operated with a mercury electrode, pointing to favorable specific interactions of the catalytic species with the mercury surface (38,39), whereas the use of a carbon electrode leads to much less efficiency in terms of rate (maximal turnover frequency of 90 s −1…”

mentioning

confidence: 99%

Efficient and selective molecular catalyst for the CO ₂ -to-CO electrochemical conversion in water

Costentin

Robert

Savéant

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

307

288

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Substitution of the four paraphenyl hydrogens of iron tetraphenylporphyrin by trimethylammonio groups provides a watersoluble molecule able to catalyze the electrochemical conversion of carbon dioxide into carbon monoxide. The reaction, performed in pH-neutral water, forms quasi-exclusively carbon monoxide with very little production of hydrogen, despite partial equilibration of CO 2 with carbonic acid-a low pK a acid. This selective molecular catalyst is endowed with a good stability and a high turnover frequency. On this basis, prescribed composition of CO-H 2 mixtures can be obtained by adjusting the pH of the solution, optionally adding an electroinactive buffer. The development of these strategies will be greatly facilitated by the fact that one operates in water. The same applies for the association of the cathode compartment with a proton-producing anode by means of a suitable separator.CO 2 -to-CO conversion | contemporary energy challenges | electrochemistry | catalysis | solar fuels O ne of the most important issues of contemporary energy and environmental challenges consists of reducing carbon dioxide into fuels by means of sunlight (1-3). One route toward this ultimate goal is to first convert solar energy into electricity, which will then be used to reduce CO 2 electrochemically. Direct electrochemical injection of an electron into the CO 2 molecule, forming the corresponding anion radical CO 2 .− requires a very high energy [the standard potential of the CO 2 / CO 2 .− couple is indeed −1.97 V vs. normal hydrogen electrode (NHE) in N,N′dimethylformamide (DMF)] (4, 5). Electrochemical conversion of CO 2 to any reaction product thus requires catalytic schemes that preferably avoid this intermediate. Carbon monoxide may be an interesting step en route to the desired fuels because it can be used as feedstock for the synthesis of alkanes through the classic Fischer-Tropsch process. A number of molecular catalysts for the homogeneous electrochemical CO 2 -to-CO conversion have been proposed. They mainly derive from transition metal complexes by electrochemical generation of an appropriately reduced state, which is restored by the catalytic reaction. So far, nonaqueous aprotic solvents (mostly DMF and acetonitrile) have been used for this purpose (5-16). Brönsted acids have been shown to boost catalysis. However, they should not be too strong, at the risk of leading to H 2 formation at the expense of the CO. Trifluoroethanol and water (possibly in large amounts) have typically played the role of a weak acid in the purpose of boosting catalysis while avoiding hydrogen evolution.One of the most thoroughly investigated families of transitionmetal complex catalysts of CO 2 -to-CO conversion is that of iron porphyrins brought electrochemically to the oxidation degree 0. The importance of coupling electron transfer and introduction of CO 2 into the coordination sphere of iron with proton transfers required by the formation of CO, CO 2 + 2e − + 2AH ↔ CO + H 2 O + 2A − , appeared from the very beginning of these ...

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Single catalyst electrocatalytic reduction of CO₂in water to H₂+CO syngas mixtures with water oxidation to O₂

Cited by 122 publications

References 47 publications

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

Zn–Cu Alloy Nanofoams as Efficient Catalysts for the Reduction of CO₂ to Syngas Mixtures with a Potential‐Independent H₂/CO Ratio

Efficient and selective molecular catalyst for the CO ₂ -to-CO electrochemical conversion in water

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Single catalyst electrocatalytic reduction of CO2in water to H2+CO syngas mixtures with water oxidation to O2

Cited by 122 publications

References 47 publications

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

A Co3O4-CDots-C3N4 three component electrocatalyst design concept for efficient and tunable CO2 reduction to syngas

Zn–Cu Alloy Nanofoams as Efficient Catalysts for the Reduction of CO2 to Syngas Mixtures with a Potential‐Independent H2/CO Ratio

Efficient and selective molecular catalyst for the CO 2 -to-CO electrochemical conversion in water

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Single catalyst electrocatalytic reduction of CO₂in water to H₂+CO syngas mixtures with water oxidation to O₂

Zn–Cu Alloy Nanofoams as Efficient Catalysts for the Reduction of CO₂ to Syngas Mixtures with a Potential‐Independent H₂/CO Ratio

Efficient and selective molecular catalyst for the CO ₂ -to-CO electrochemical conversion in water