A mechanistic study of 4-aminoantipyrine and iron derived non-platinum group metal catalyst on the oxygen reduction reaction

Robson, Michael H.; Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen

doi:10.1016/j.electacta.2012.11.025

Cited by 108 publications

(111 citation statements)

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“…where j D is the reductive current density measured at the disk and j R is the current measured at the ring, corrected by the collection efficiency for the used rotating ring disk electrode which, for our experiments, was 0.37, measured from the redox process of iron ferrocyanide, as it has been mentioned in our previous studies [52]. The number of electrons transferred by AC is always higher than CB at both pH levels investigated indicating that AC has higher electrocatalytic activity towards the ORR compared to CB ( Figure 2).…”

Section: Rrde Resultsmentioning

confidence: 99%

“…This is an important parameter, as the oxygen reduction to water or hydroxyls is a four e − transfer process, whereas the reduction to hydrogen peroxide yields only two e − . The formula that correlates the current measured at the disk and the current measured at the ring to estimate the amount of transferred electrons during the reduction reactions is (Equation (5)): (5) where jD is the reductive current density measured at the disk and jR is the current measured at the ring, corrected by the collection efficiency for the used rotating ring disk electrode which, for our experiments, was 0.37, measured from the redox process of iron ferrocyanide, as it has been mentioned in our previous studies [52]. The number of electrons transferred by AC is always higher than CB at both pH levels investigated indicating that AC has higher electrocatalytic activity towards In the RRDE setup, it is also possible to measure the amount of hydrogen peroxide produced during the ORR, as this peroxide is further reduced to water in the platinum ring that the probe possesses.…”

Section: Rrde Resultsmentioning

confidence: 99%

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Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

et al. 2016

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Abstract:A comparison between different carbon-based gas-diffusion air-breathing cathodes for microbial fuel cells (MFCs) is presented in this work. A micro-porous layer (MPL) based on carbon black (CB) and an activated carbon (AC) layer were used as catalysts and applied on different supporting materials, including carbon cloth (CC), carbon felt (CF), and stainless steel (SS) forming cathode electrodes for MFCs treating urine. Rotating ring disk electrode (RRDE) analyses were done on CB and AC to: (i) understand the kinetics of the carbonaceous catalysts; (ii) evaluate the hydrogen peroxide production; and (iii) estimate the electron transfer. CB and AC were then used to fabricate electrodes. Half-cell electrochemical analysis, as well as MFCs continuous power performance, have been monitored. Generally, the current generated was higher from the MFCs with AC electrodes compared to the MPL electrodes, showing an increase between 34% and 61% in power with the AC layer comparing to the MPL. When the MPL was used, the supporting material showed a slight effect in the power performance, being that the CF is more powerful than the CC and the SS. These differences also agree with the electrochemical analysis performed. However, the different supporting materials showed a bigger effect in the power density when the AC layer was used, being the SS the most efficient, with a power generation of 65.6 mW·m −2 , followed by the CC (54 mW·m −2 ) and the CF (44 mW·m −2 ).

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Section: Rrde Resultsmentioning

confidence: 99%

Section: Rrde Resultsmentioning

confidence: 99%

Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

et al. 2016

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“…As it has been shown from our group, the sacrificial support method (SSM) is a powerful tool for the preparation of cathode materials, anode materials and CNTs. [17][18][19][20][21][22][23][24][25][26][27] High surface areas of the final catalyst are a result of removing the sacrificial support, which can be controlled by the selection of silica with different particle sizes and surface areas.XRD analyses of the four samples show that the CuCo 2 O 4 made by SSM was a phase-pure spinel (∼96 wt%), despite the usage of a significantly lower temperature and calcination duration during synthesis (Figure 1, bottom). This can be explained by homogeneous coverage of the precursors on the surface of mono-dispersed silica particles.…”

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confidence: 99%

“…Four synthetic methods were selected: pore-forming, sol-gel, spray pyrolysis and the sacrificial support method. [17][18][19][20][21][22][23][24][25][26][27] As-prepared materials were tested in ORR/OER reactions and show promising performance, which allows for using them as highly active bi-functional catalysts.…”

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confidence: 99%

CuCo₂O₄ORR/OER Bi-Functional Catalyst: Influence of Synthetic Approach on Performance

Serov

Andersen

Matanović

et al. 2015

J. Electrochem. Soc.

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A series of CuCo 2 O 4 catalysts were synthesized by pore forming, sol-gel, spray pyrolysis and sacrificial support methods. Catalysts were characterized by XRD, SEM, XPS and BET techniques. The electrochemical activity for the oxygen reduction and oxygen evolution reactions (ORR and OER) was evaluated in alkaline media by RRDE. Density Functional Theory was used to identify two different types of active sites responsible for ORR/OER activity of CuCo 2 O 4 and it was found that CuCo 2 O 4 can activate the O-O bond by binding molecular oxygen in bridging positions between Co or Co and Cu atoms. It was found that the sacrificial support method (SSM) catalyst has the highest performance in both ORR and OER and has the highest content of phase-pure CuCo 2 O 4 . It was shown that the presence of CuO significantly decreases the activity in oxygen reduction and oxygen evolution reactions. The half-wave potential (E 1/2 ) of CuCo 2 O 4 -SSM was found as 0.8 V, making this material a state-of-the-art, unsupported oxide catalyst. © The Author(s) 2015. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. [DOI: 10.1149/2.0921504jes] All rights reserved.Manuscript submitted December 3, 2014; revised manuscript received January 28, 2015. Published February 7, 2015 Development of highly active bi-functional catalysts, in reactions of oxygen reduction/oxygen evolution (ORR/OER), attracts the attention of not only researchers in academia, but also from industrial R&D centers. The industrial interest is apparent by the growing market for supplying pure hydrogen and oxygen for fuel cell back-up power systems in India and Africa. Presently, both fuel cells and electrolyzers utilize a substantial amount of platinum-group metals (PGM), mainly platinum for ORR and IrO 2 for OER. Despite the fact that platinum is the most active catalyst for oxygen reduction, it has a high price; the discovered resources are scarce and major mining facilities are located in politically unstable countries. On the other side, iridium is one of the least abundant elements in the Earth's crust, making its application commercially unviable. The combination of these factors leads to the problem of the incredibly high price of fuel cell stacks and electrolyzers. There is substantial progress in substituting platinum from the cathode side of fuel cell MEAs, 1 while there has been no such breakthrough for electrolyzers reported in open literature.Secondly, there is a promising application for bi-functional catalysts in metal-air batteries, especially Lithium-air batteries. Li-air batteries should effectively reduce oxygen during the discharge cycle and evolve oxygen during the charge cycle. Highly efficient catalysts for those cycles are precious metal-based materials: Pt, Au, Ag, Pd. 2,3Li-air batteries and electrolyzers will be bro...

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“…This behavior has been reported before for other non-PGM catalysts. 28,29 Even for the thinnest layer used here, there might still be significant two-step reduction in the catalyst layer.…”

Section: Resultsmentioning

confidence: 99%

Pyrolyzed Copper-Based Catalyst with High Oxygen Reduction Activity for PEM Fuel Cell Applications

Goenaga

Foister

Belapure

et al. 2014

ECS Electrochemistry Letters

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We have synthesized a copper-based catalyst for the oxygen reduction reaction in low temperature fuel cells. Catalysts were prepared by covalently attaching a phthalocyanine-type ligand to a carbon black surface, and adding Cu(OAc) 2 . The phthalocyanine-type ligand provides the nitrogen to form the presumed catalytic centers with the Cu metal. Rotating ring disk electrode experiments revealed that the catalytic activity of the as-synthesized material is greatly enhanced after one-step pyrolysis under inert atmosphere, reaching an onset potential of 0.82 V vs. RHE in acidic environment after thermal treatment at 950 • C, making this the best copper-based ORR catalyst in acid reported to date. State of the art proton exchange membrane fuel cells (PEMFCs) use Pt as the catalyst for oxygen reduction reaction (ORR) at the cathode. Due to the high cost of Pt, minimizing the Pt content of the PEMFC has become a major endeavor to make feasible the mass commercialization of PEMFC.1 While a number of efforts seek to achieve this by improving the activity and utilization of Pt-based catalysts, the most direct approach is replacing Pt with non-precious metal catalysts (NPMC). Synthesis of NPMCs is often inspired by natural systems:2 enzymes, such as laccase, are very efficient ORR catalysts. Such Cu oxidases are known to reduce oxygen at approximately 1.2 V vs. the reversible hydrogen electrode (RHE) under mild pH conditions.2-4 The ORR in these enzymes is known to occur in a three or four Cu-atom active site. 4 Since Jasinski first reported the use of Co-phthalocyanine as a catalyst for ORR, 5 a prolonged effort has been devoted to developing ORR catalyst materials based on transition metal complexes. The best NPMCs to date are based on Fe and Co, and can be unsupported 6 or supported on carbon. 7,8 In general their synthesis requires a nitrogen source (nitrogen containing molecule and/or reactive gas) and heat-treatment at high temperatures to form the presumed Me-N 2 and Me-N 4 ORR catalytic centers. After pyrolysis, the precise nature and loading of the catalytic centers are unknown. Though seemingly critical to rational development of new catalysts, the actual active structure is still the subject of speculation, uncertainty and debate.7-14 However, some significant correlative information providing insight into the most favorable nitrogen arrangement has been achieved through the systematic application of XPS methods. From this, it is suggested that the eventual formation of pyridinic nitrogen centers is associated with many successful pyrolysis attempts.Compared to Fe and Co based materials, few studies have been done on ORR using Cu-based catalysts in acidic environments. At low pH values, previous reported Cu-based catalysts exhibit overpotentials for ORR in excess of 600 mV.13,15-21 However, in alkaline media Cubased catalysts show higher catalytic activity, making them suitable for a wide range of applications as ORR catalysts.3,14,20-22 Gewirth's group has adsorbed Cu-based catalysts onto a carbon support and s...

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A mechanistic study of 4-aminoantipyrine and iron derived non-platinum group metal catalyst on the oxygen reduction reaction

Cited by 108 publications

References 74 publications

Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

CuCo₂O₄ORR/OER Bi-Functional Catalyst: Influence of Synthetic Approach on Performance

Pyrolyzed Copper-Based Catalyst with High Oxygen Reduction Activity for PEM Fuel Cell Applications

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A mechanistic study of 4-aminoantipyrine and iron derived non-platinum group metal catalyst on the oxygen reduction reaction

Cited by 108 publications

References 74 publications

Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

Carbon-Based Air-Breathing Cathodes for Microbial Fuel Cells

CuCo2O4ORR/OER Bi-Functional Catalyst: Influence of Synthetic Approach on Performance

Pyrolyzed Copper-Based Catalyst with High Oxygen Reduction Activity for PEM Fuel Cell Applications

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CuCo₂O₄ORR/OER Bi-Functional Catalyst: Influence of Synthetic Approach on Performance