Kinetic Approach to Investigate the Mechanistic Pathways of Oxygen Reduction Reaction on Fe-Containing N-Doped Carbon Catalysts

Muthukrishnan, Azhagumuthu; Nabae, Yuta; Okajima, Takaharu; Ohsaka, Takeo

doi:10.1021/acscatal.5b00397

Cited by 108 publications

(85 citation statements)

References 51 publications

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“…To the best of our knowledge, our CNT@Fe-N-PC catalyst showed the best ORR performance in an acidic medium compared with all previously reported Fe-N-C and other non-noble-metal catalysts (Supplementary Table 2). 11,12,13,20,22,27,28,31,[37][38][39][40] In addition to the high activity, we further studied the durability of the CNT@Fe-N-PC catalyst. Figure 3c shows that the current density decay is 12% after 40 000 s of testing, much smaller than that (57%) of commercial Pt/C.…”

Section: Resultsmentioning

confidence: 99%

N-doped carbon nanotubes containing a high concentration of single iron atoms for efficient oxygen reduction

et al. 2018

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Fe-N-C has emerged as a promising noble-metal-free catalyst for the oxygen reduction reaction (ORR). However, achieving a catalytic activity comparable to that of Pt in acidic medium remains a great challenge. Here we report a N-doped carbon nanotube (CNT) catalyst in which a high concentration of single Fe atoms has been dispersed (CNT@Fe-N-PC). The catalyst was prepared by a simple and scalable atomic isolation method, in which a metal isolation agent was introduced to isolate Fe atoms and was then evaporated to produce abundant micropores that host single Fe atom active sites. The CNT@Fe-N-PC catalyst contained a high concentration of single Fe atom active sites and exhibited ultrahigh ORR activity with a half-wave potential of 0.82 V, comparable to that of Pt/C in an acidic medium. A high concentration of Fe-N x active sites was created on a flexible single-wall CNT film and carbon cloth using this technique, and these materials showed even better ORR performance, that is, 40-60 mV more positive onset potentials than those of a commercial Pt/C catalyst. These catalysts exhibit excellent catalytic activity, good durability and low cost, and show great potential for commercial use as substitutes for current Pt-based catalysts.

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Section: Resultsmentioning

confidence: 99%

N-doped carbon nanotubes containing a high concentration of single iron atoms for efficient oxygen reduction

et al. 2018

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“…Indeed, Olson et al proposed a bi-functional ORR mechanism over Fe/N/C catalysts in 2010 [25], but quantitative discussion to resolve the quasi-four-electron reduction reaction proved difficult. While Ohsaka and co-workers tried to apply the Damjanovic-Hsueh approach [21,26], which involves detailed RRDE analysis by plotting of the obtained parameters against the rotation speeds, such analysis relying on rotation speeds suffered from huge noise [27,28]. To address these concerns, Nabae and co-workers recently developed a new model (Figure 2b) and method for RRDE analysis [29].…”

Section: Orr Reaction Scheme and Active Sites Over Npm Catalystsmentioning

confidence: 99%

“…In this context, as shown in Figure 3, a hybrid mechanism is worth considering for the ORR conducted over Fe/N/C catalysts, where the first two-electron reduction to form H 2 O 2 is catalyzed by metal-free N/C catalytic centers and the following two-electron reduction of H 2 O 2 and/or the direct four-electron reduction of O 2 to form H 2 O are catalyzed by Fe/N/C-based catalytic centers. from huge noise [27,28]. To address these concerns, Nabae and co-workers recently developed a new model ( Figure 2b) and method for RRDE analysis [29].…”

Section: Orr Reaction Scheme and Active Sites Over Npm Catalystsmentioning

confidence: 99%

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Morphology-Controlled Nitrogen-Containing Polymers as Synthetic Precursors for Electrochemical Oxygen Reduction Fe/N/C Cathode Catalysts

Nabae

2018

Catalysts

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Nitrogen-containing aromatic polymers such as polyimide are known for their high thermal stability. While they have been widely used in industry, their relevance to catalysis is still quite limited. In recent years, nitrogen-containing polymers have been explored as precursors of nitrogen-doped carbonaceous materials, which are particularly attractive as non-precious metal catalysts for oxygen reduction in fuel cells. The high thermal stability of nitrogen-containing polymers contributes to an effective control over the morphology of the resulting carbonaceous catalysts. This review article provides an overview of the recent progress on the research and development of Fe/N/C oxygen reduction catalysts prepared from morphology-controlled nitrogen-containing polymers.

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“…This result can be attributed to the facile conversion of active nitrogen species [12,13]. This result can be attributed to the facile conversion of active nitrogen species into inactive ones, or the domination of less efficient two-electron process involved with intermediates during the ORR process of n-doped graphene in an acidic environment [14,15].…”

Section: Introductionmentioning

confidence: 99%

Terpyridine-Containing Imine-Rich Graphene for the Oxygen Reduction Reaction

et al. 2017

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Abstract:We report a facile synthetic method for the preparation of a terpyridine-containing imine-rich graphene (IrGO-Tpy) using an acid-catalyzed dehydration reaction between graphene oxide (GO) and 4 -(aminophenyl)-2,2 :6 2"-terpyridine. Owing to the presence of terpyridine ligands, cobalt ions (Co 2+ ) were readily incorporated into the IrGO-Tpy structures, affording a metal complex, denoted IrGo-Tpy-Co. Cyclic voltammetry and linear sweep voltammetry measurements confirm the noticeable oxygen reduction reaction (ORR) activities of the IrGo-Tpy and IrGo-Tpy-Co electroacatalysts in alkaline electrolytes, along with the additional merits of high selectivity, excellent long-term durability, and good resistance to methanol crossover. In addition, a remarkable improvement in the ORR performance was observed for IrGO-Tpy-Co compared with that of IrGo-Tpy, arising from the significant contribution of the cobalt-terpyridine complex in facilitating the ORR process.

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Kinetic Approach to Investigate the Mechanistic Pathways of Oxygen Reduction Reaction on Fe-Containing N-Doped Carbon Catalysts

Cited by 108 publications

References 51 publications

N-doped carbon nanotubes containing a high concentration of single iron atoms for efficient oxygen reduction

N-doped carbon nanotubes containing a high concentration of single iron atoms for efficient oxygen reduction

Morphology-Controlled Nitrogen-Containing Polymers as Synthetic Precursors for Electrochemical Oxygen Reduction Fe/N/C Cathode Catalysts

Terpyridine-Containing Imine-Rich Graphene for the Oxygen Reduction Reaction

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