Heteroatom-doped carbon-based oxygen reduction electrocatalysts with tailored four-electron and two-electron selectivity

Woo, Jinwoo; Lim, June Sung; Kim, Jae Hyung; Joo, Sang Hoon

doi:10.1039/d1cc02667d

Cited by 53 publications

(53 citation statements)

References 93 publications

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“…The selection of electrocatalysts is vital to efficient H 2 O 2 electrochemical synthesis. Heteroatom‐doped carbon materials are one type of promising electrocatalysts for the two‐electron ORR [6] . Their ORR activity and selectivity can be tailored through control of the active sites [7] .…”

Section: Introductionmentioning

confidence: 99%

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Impact of Pore Structure on Two‐Electron Oxygen Reduction Reaction in Nitrogen‐Doped Carbon Materials: Rotating Ring‐Disk Electrode vs. Flow Cell

Wang

et al. 2022

ChemSusChem

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The impact of pore structure on the two‐electron oxygen reduction reaction (ORR) in nitrogen‐doped carbon materials is currently under debate, and previous studies are mainly limited to the rotating ring‐disk electrode (RRDE) rather than the practical flow cell (FC) system. In this study, assisted by a group of reliable pore models, the impact of two pore structure parameters, that is, Brunauer–Emmett–Teller surface area (SBET) and micropore surface fraction (fmicro), on ORR activity and selectivity are investigated in both RRDE and FC. The ORR mass activity correlates positively to the SBET in the RRDE and FC because a higher SBET can host more active sites. The H2O2 selectivity is independent of fmicro in the RRDE but correlates negatively to fmicro in the FC. The inconsistency results from different states of the electrode in the RRDE and the FC. These insights will guide the design of carbon materials for H2O2 synthesis.

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Section: Introductionmentioning

confidence: 99%

“…Heteroatom-doped carbon materials are one type of promising electrocatalysts for the two-electron ORR. [6] Their ORR activity and selectivity can be tailored through control of the active sites. [7] Another efficient strategy is to tailor the pore structure to host active sites on their surface.…”

Section: Introductionmentioning

confidence: 99%

Impact of Pore Structure on Two‐Electron Oxygen Reduction Reaction in Nitrogen‐Doped Carbon Materials: Rotating Ring‐Disk Electrode vs. Flow Cell

Wang

et al. 2022

ChemSusChem

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“…Carbon-based electrocatalysts are considered promising alternatives to platinum electrocatalysts to promote ORR on the cathode of Zn–air batteries. In particular, heteroatom-doped carbon electrocatalysts were found to exhibit enhanced electrocatalytic activity for ORR through modification of their local electronic structure [ 8 – 11 ]. Furthermore, coupling transition metals onto N -doped carbon skeletons was suggested as an effective way to design the active sites of carbon electrocatalysts for ORR [ 12 , 13 ].…”

Section: Introductionmentioning

confidence: 99%

Modulating the electrocatalytic activity of N-doped carbon frameworks via coupling with dual metals for Zn–air batteries

Park

Shin

et al. 2022

Nano Convergence

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N-Doped carbon electrocatalysts are a promising alternative to precious metal catalysts to promote oxygen reduction reaction (ORR). However, it remains a challenge to design the desired active sites on carbon skeletons in a controllable manner for ORR. Herein, we developed a facile approach based on oxygen-mediated solvothermal radical reaction (OSRR) for preparation of N-doped carbon electrocatalysts with a pre-designed active site and modulated catalytic activity for ORR. In the OSRR, 2-methylimidazole reacted with Co and Mn salts to form an active site precursor (MnCo-MIm) in N-methyl-2-pyrrolidone (NMP) at room temperature. Then, the reaction temperature increased to 140 °C under an oxygen atmosphere to generate NMP radicals, followed by their polymerization with the pre-formed MnCo-MIm to produce Mn-coupled Co nanoparticle-embedded N-doped carbon framework (MnCo-NCF). The MnCo-NCF showed uniform dispersion of nitrogen atoms and Mn-doped Co nanoparticles on the carbon skeleton with micropores and mesopores. The MnCo-NCF exhibited higher electrocatalytic activity for ORR than did a Co nanoparticle only-incorporated carbon framework due to the improved charge transfer from the Mn-doped Co nanoparticles to the carbon skeleton. In addition, the Zn–air battery assembled with MnCo-NCF had superior performance and durability to the battery using commercial Pt/C. This facile approach can be extended for designing carbon electrocatalysts with desired active sites to promote specific reactions. Graphical Abstract

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“…1 The identification of the active sites and detailed catalytic mechanisms is always controversial, although tremendous progress in metal-free carbon-based catalysts has been made. 2,3 The argument is firstly focused on whether the ORR activity comes from transition-metal impurities or the metal-free species. 4 Through a strict metal-free synthesis of N-CNTs reported by Dai's group 5 and the deactivation experiment of N-doped graphene by selective passivation of the active sites, 6 N-doped sites have been proven to exhibit ORR activity, but their activity is generally lower than the typical values of metal-involved catalysts.…”

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confidence: 99%

Identification of a pyrone-type species as the active site for the oxygen reduction reaction

et al. 2022

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Heteroatom-doped carbon-based oxygen reduction electrocatalysts with tailored four-electron and two-electron selectivity

Abstract: Oxygen reduction reaction (ORR) plays a pivotal role in electrochemical energy conversion and commodity chemical production. Oxygen reduction involving a complete four-electron (4e−) transfer is important for the efficient operation...

Cited by 53 publications

References 93 publications

Impact of Pore Structure on Two‐Electron Oxygen Reduction Reaction in Nitrogen‐Doped Carbon Materials: Rotating Ring‐Disk Electrode vs. Flow Cell

Impact of Pore Structure on Two‐Electron Oxygen Reduction Reaction in Nitrogen‐Doped Carbon Materials: Rotating Ring‐Disk Electrode vs. Flow Cell

Modulating the electrocatalytic activity of N-doped carbon frameworks via coupling with dual metals for Zn–air batteries

Identification of a pyrone-type species as the active site for the oxygen reduction reaction

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