Fe,N‐Codoped Graphdiyne Displaying Efficient Oxygen Reduction Reaction Activity

Si, Wenyan; Yang, Ze; Wang, Xin; Lv, Qing; Zhao, Fuhua; Li, Xiaodong; He, Jianjiang; Long, Yun‐Ze; Gao, Juan

doi:10.1002/cssc.201802170

Cited by 80 publications

(49 citation statements)

References 38 publications

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“…For a 4e ORR, I lim should be a fixed value in a particular concentration solution at 1600 rpm on a 5 mm working electrode, such as 5.277 mA cm −2 for 0.5 M H 2 SO 4 , 6.332 mA cm −2 for 0.1 M HClO 4 , and 5.968 mA cm −2 for 0.1 M KOH (The parameters were listed in support information). However, the experimentally measured I lim for 4e ORR are quite different among various literatures under the same experimental conditions, no matter on Pt/C catalysts or non‐noble metal catalysts, as shown in Figure . It is noteworthy that most measured I lim are lower than the theoretical value, and some are even only half of the theoretical value.…”

Section: Introductionmentioning

confidence: 68%

Effect of Experimental Operations on the Limiting Current Density of Oxygen Reduction Reaction Evaluated by Rotating‐Disk Electrode

Zhong

Liu

et al. 2020

ChemElectroChem

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The universal linear scan voltammogram measurement on the rotating disk electrode (RDE) has been identified as a simple method to investigate the oxygen reduction activity of electrocatalysts. The steady‐state limiting current density Ilim indicates the maximum diffusion current density in the oxygen reduction reaction (ORR) during RDE measurement, which should be a fixed value in theory for a 4e ORR in a particular concentration solution and at a certain rotate speed. However, in experiments, Ilim is always variable and smaller than theoretical value even though with the same the catalyst, electrode, and rotator. So the impact of various experimental operating parameters on Ilim is highly necessary to be investigated. In this paper, factors, such as catalyst loading, O2 inlet condition, O2 flow rate, gas tightness, solution concentration, and purity, have been investigated for their effects on the Ilim of ORR on three typical catalysts (20 % commercial Pt/C, Iron/Nitrogen/Carbon‐catalyst and N‐doped carbon nanotubes). The results indicate that the catalyst loading and O2 inlet condition are the key factors influencing the Ilim of ORR. While, the O2 flow rate, gas tightness, solution concentration, and purity have little influence on the Ilim of ORR. The correct Ilim could be obtained under the optimized catalyst loading and the O2 inlet with an extended sand core tube.

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Section: Introductionmentioning

confidence: 68%

Effect of Experimental Operations on the Limiting Current Density of Oxygen Reduction Reaction Evaluated by Rotating‐Disk Electrode

Zhong

Liu

et al. 2020

ChemElectroChem

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“…An analogue of graphene is graphdiyne: a semiconductor that consists of carbon hexagonal rings (sp 2 ‐hybridized C) and diacetylenic linkages (CCCC, sp‐hybridized C) . Recently, N‐doped graphdiynes emerged as promising ORR metal‐free catalysts, with low overpotential, small crossover effect, and long‐term stability . For example, Liu et al prepared N‐doped graphdiyne by heating graphdiyne under high‐purity ammonia mixed with argon.…”

Section: Introductionmentioning

confidence: 99%

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

et al. 2019

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Nitrogen‐doped graphdiynes recently emerged as promising metal‐free oxygen reduction reaction (ORR) electrocatalysts. However, which type of N‐dopants contributing to the enhanced catalytic performance and the catalytic performances of other heteroatom‐doped graphdiynes has not been explored systematically. Herein, ORR and oxygen evolution reaction (OER) catalytic performances of X‐doped graphdiynes are examined by means of DFT computations (X = B, N, P, and S). It is revealed that the graphitic S‐doped graphdiyne (Model S1), the sp‐N‐doped graphdiyne (Model N3) and the graphitic P‐doped graphdiyne (Model P1) exhibit comparable or even better ORR/OER activities than Pt/C or RuO2, with ORR activity trend as Model S1 > Pt/C > Model N3 and OER trend as Model P1 > RuO2 > Model N3. The carbon atoms near N‐ and S‐dopants and featuring large positive charge are the ORR active sites in Models N3 and S1, whereas the carbon atoms near N‐ and P‐dopants and possessing high spin are the OER active sites in Models N3 and P1. Overall, this study not only gains deep insights into the catalytic activity of N‐doped graphdiyne for ORR, but also guides developing of graphdiyne‐based ORR/OER catalysts beyond N‐doping.

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“…The newly developed 2D sp‐ and sp 2 ‐cohybridized carbon allotrope of GDY has aroused great interest in scientific research owing to its unique physicochemical properties. [ 61,62 ] The theoretical arithmetic reveals that the presence of sp‐hybridized carbon atoms and triangular cavities in 2D GDY conjugated network are beneficial for forming tight interfacial contact with active constituents, which has not been detected in preceding developed sp 2 ‐ and sp 3 ‐hybridized carbon allotropes. [ 23 ] This strong interactivity is attributed to the sp‐hybridized‐carbon‐rich structure, which accelerates the electron transfer process and strengthens the stability of metal oxides in electrochemical energy conversion.…”

Section: Gdy Supported Electrocatalysts For Energy Conversionmentioning

confidence: 99%

“…In consideration of the superior optical and electrical features of GDY, more GDY‐based materials will be developed for ORR. [ 62,135 ]…”

Section: Gdy Supported Electrocatalysts For Energy Conversionmentioning

confidence: 99%

Graphdiyne: A Rising Star of Electrocatalyst Support for Energy Conversion

Lai

Zhang

et al. 2020

Advanced Energy Materials

119

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Graphdiyne (GDY), a rising star of 2D carbon allotropes with one‐atom‐thick planar layers, has achieved the coexistence of sp‐ and sp2‐hybridized carbon atoms in a 2D planar structure. In contrast to the prevailing carbon allotropes, GDY possesses Dirac cone structures, which endow it with unique chemical and physical properties, including an adjustable inherent bandgap, high‐speed charge carrier transfer efficiency, and excellent conductivity. Additionally, GDY also displays great potential in photocatalysis, rechargeable batteries, solar cells, detectors, and especially electrocatalysis. In this work, various GDY‐supported electrocatalysts are described and the reasons why GDY can act as a novel support are analyzed from the perspective of molecular structure, electronic properties, mechanical properties, and stability. The various electrochemical applications of GDY‐supported electrocatalysts in energy conversion such as hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, overall water splitting, and nitrogen reduction reaction are reviewed. The challenges facing GDY and GDY‐based materials in future research are also outlined. This review aims at providing an in‐depth understanding of GDY and promoting the development and application of this novel carbon material.

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Fe,N‐Codoped Graphdiyne Displaying Efficient Oxygen Reduction Reaction Activity

Cited by 80 publications

References 38 publications

Effect of Experimental Operations on the Limiting Current Density of Oxygen Reduction Reaction Evaluated by Rotating‐Disk Electrode

Effect of Experimental Operations on the Limiting Current Density of Oxygen Reduction Reaction Evaluated by Rotating‐Disk Electrode

Boosting ORR/OER Activity of Graphdiyne by Simple Heteroatom Doping

Graphdiyne: A Rising Star of Electrocatalyst Support for Energy Conversion

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