Organically doped palladium: a highly efficient catalyst for electroreduction of CO<sub>2</sub>to methanol

Yang, Hengpan; Qin, Sen; Wang, Huan; Lu, Jia‐Xing

doi:10.1039/c5gc01504a

Cited by 64 publications

(41 citation statements)

References 33 publications

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“…These biomolecules are usually entrapped within a metal matrix and immobilized onto the electrode to improve the electrical connection. [122] To do so, metallic doping was adopted to create an enlarged derivative of pyridine catalyst (by attaching three benzene rings to it) (PYD), to trap it inside porous palladium cages (Figure 46); in this way the pyridine catalyst remains immobilized while smaller molecules can diffuse in and out of the cage. However, at the time and until recently, pyridine catalysts have not been very stable upon electrolysis and are prone to degradation.…”

Section: Metal-free Organic Catalystsmentioning

confidence: 99%

“…[122] Based on pH testing, they proposed that PYD combines with a hydrogen cation and is then reduced to the PYD radical, which upon reacting with CO 2 forms intermediate products like formic acid (a trace product in the above CPE) eventually leading up to methanol similar to the Py/Pt homogenous system created by Bocarsly and co-workers. [122] Based on pH testing, they proposed that PYD combines with a hydrogen cation and is then reduced to the PYD radical, which upon reacting with CO 2 forms intermediate products like formic acid (a trace product in the above CPE) eventually leading up to methanol similar to the Py/Pt homogenous system created by Bocarsly and co-workers.…”

Section: Metal-free Organic Catalystsmentioning

confidence: 99%

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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%

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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“…[25][26][27][28] Thev arying composition in Pd x Cu y aerogels resulted in different Pd 0 /Pd II and Cu I + Cu 0 /Cu II radios,w hich was found to be correlated with the CO 2 electrocatalytic activity and CH 3 OH selectivity.M oreover, the special nanochain structure of aerogels also contributed to the enhancement of Pd/Cu grain boundaries and CH 3 OH production. We prepared as erious of Pd x Cu y bimetallic aerogels with controlled composition via at emplate-free self-assembly process.B y using Pd 83 Cu 17 bimetallic aerogels on carbon paper (CP) as electrode and 1-butyl-3-methylimidazoliumtetrafluoroborate ([Bmim]BF 4 )a queous solution as electrolyte,t he Faradaic efficiency for CH 3 OH production could reach 80.0 %w ith acurrent density of 31.8 mA cm À2 ,which is higher than those reported previously.…”

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confidence: 99%

Highly Efficient Electroreduction of CO₂ to Methanol on Palladium–Copper Bimetallic Aerogels

et al. 2018

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Electrochemical reduction of CO to CH OH is of great interest. Aerogels have fine inorganic superstructure with high porosity and are known to be exceptional materials. Now a Pd-Cu bimetallic aerogel electrocatalyst has been developed for conversion of CO into CH OH. The current density and Faradaic efficiency of CH OH can be as high as 31.8 mA cm and 80.0 % over the Pd Cu aerogel at a very low overpotential (0.24 V). The superior performance of the electrocatalyst results from efficient adsorption and stabilization of the CO radical anion, high Pd /Pd and Cu +Cu /Cu ratios, and sufficient Pd/Cu grain boundaries of aerogel nanochains.

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“…Therefore, in our experimental electrolysis conditions either methanol is not formed or its concentration too low to be detected by 1 H NMR spectroscopy. Note that in all cases the charges passed during electrolysis (Table ) are in the same order as those reported in the literature (between 4 and 64 C cm −2 ) but without methanol formation in our conditions . Control experiments by injection of methanol (2 m m ) into a solution containing pyridine at the beginning of electrolysis revealed that the methanol concentration remained unchanged over a 25 h electrolysis (Figure S4).…”

Section: Resultsmentioning

confidence: 99%

Electrochemical Behavior of Pyridinium and N‐Methyl Pyridinium Cations in Aqueous Electrolytes for CO₂ Reduction

2017

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The electrochemical reduction of aqueous pyridinium and N‐methyl pyridinium ions is investigated in the absence and presence of CO2 and electrolysis reaction products on glassy carbon, Au, and Pt electrodes are studied. Unlike pyridinium, N‐methyl pyridinium is not electroactive at the Pt electrode. The electrochemical reduction of the two pyridine derivatives was found to be irreversible on glassy carbon. These results confirmed the essential role of the N−H bond of the pyridinium cation. In contrast, the electrochemical response of N‐methyl pyridinium ion at the glassy carbon electrode suggests that a specific interaction occurs between the glassy carbon surface and the aromatic ring of the pyridinium derivative. For all electrodes, an enhancement of current was observed in the presence of CO2. However, NMR spectroscopy of the solutions following electrolysis showed no formation of methanol or other possible byproducts of the reduction of CO2 in the presence of either pyridinium derivative ion.

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Organically doped palladium: a highly efficient catalyst for electroreduction of CO₂to methanol

Abstract: Electrochemical reduction of CO2to methanol with 35% Faradaic efficiency on organically doped palladium cathode in aqueous solution.

Cited by 64 publications

References 33 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

Highly Efficient Electroreduction of CO₂ to Methanol on Palladium–Copper Bimetallic Aerogels

Electrochemical Behavior of Pyridinium and N‐Methyl Pyridinium Cations in Aqueous Electrolytes for CO₂ Reduction

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Organically doped palladium: a highly efficient catalyst for electroreduction of CO2to methanol

Abstract: Electrochemical reduction of CO2to methanol with 35% Faradaic efficiency on organically doped palladium cathode in aqueous solution.

Cited by 64 publications

References 33 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

Highly Efficient Electroreduction of CO2 to Methanol on Palladium–Copper Bimetallic Aerogels

Electrochemical Behavior of Pyridinium and N‐Methyl Pyridinium Cations in Aqueous Electrolytes for CO2 Reduction

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Resources

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Organically doped palladium: a highly efficient catalyst for electroreduction of CO₂to methanol

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

Highly Efficient Electroreduction of CO₂ to Methanol on Palladium–Copper Bimetallic Aerogels

Electrochemical Behavior of Pyridinium and N‐Methyl Pyridinium Cations in Aqueous Electrolytes for CO₂ Reduction