One-pot synthesis of nitrogen and sulfur co-doped graphene as efficient metal-free electrocatalysts for the oxygen reduction reaction

Wang, Xin; Wang, Jie; Wang, Deli; Dou, Shuo; Ma, Zhaoling; Wu, Jianghong; Li, Tao; Shen, Anli; Ouyang, Canbin; Liu, Qiuhong; Wang, Shuangyin

doi:10.1039/c4cc00440j

Cited by 308 publications

(180 citation statements)

References 15 publications

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“…6b), close to that of the reported metal-free electrocatalysts such as NSG700. 19 With the disc and ring currents in the LSV curve, the electron transfer number (n) per oxygen molecule involved in the ORR was calculated from the following equation:…”

Section: Electrochemical Properties Analysismentioning

confidence: 99%

Templated synthesis of nitrogen-doped graphene-like carbon materials using spent montmorillonite

Chen

Wang

et al. 2015

RSC Adv.

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Montmorillonite (Mt) as an environmentally-friendly, low-cost, and highly-efficient adsorbent for cationic dyes has a promising application in dye wastewater treatment. However, proper disposal of the spent Mt is still a challenge holding back the wide application of Mt. This article reports a simple method which can synthesize N-doped graphene-like carbon materials using the spent Mt after the adsorption of crystal violet (CV). The spent Mt was pyrolyzed under the protection of N 2 to carbonize the adsorbed CV within the interlayer space of Mt, and the interlayer spacing of Mt decreased from 11.0Å to approximately 3.6Å, close to the thickness of a single graphene layer (3.4Å). After demineralization (i.e., washing with a mixture of HF and HCl), the carbon material was released from the interlayer space of Mt. Raman spectra showed the presence of both the D-band and G-band on the obtained carbon materials, and transmission electron microscopy observed the thin layers of carbon material. X-ray photoelectron spectroscopy results indicated the simultaneous presence of pyridinic, pyrrolic, and quaternary N on the carbon materials. In addition, the percentage of pyridinic N increases with increasing pyrolysis temperature; whereas that of quaternary N decreases and of pyrrolic N remains relatively constant. The above results suggested the successful synthesis of N-doped graphene-like carbon material. Finally, the obtained materials show interesting electrocatalytic activity for the oxygen reduction reaction and show potential to be used as efficient metal-free electrocatalysts in fuel cells.

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Section: Electrochemical Properties Analysismentioning

confidence: 99%

Templated synthesis of nitrogen-doped graphene-like carbon materials using spent montmorillonite

Chen

Wang

et al. 2015

RSC Adv.

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“…S6) before and after acid leaching showed that the -C-S-C-covalent bond can be stable in the acid solution. According to previous studies, -C-S-C-is beneficial for enhancing the catalytic activity of ORR [60,61]. The high-resolution Fe 2p spectrum of PmPDA-GR-Fe (Fig.…”

Section: Science China Materialsmentioning

confidence: 99%

Graphene-templated synthesis of sandwich-like porous carbon nanosheets for efficient oxygen reduction reaction in both alkaline and acidic media

Wang

et al. 2018

Sci. China Mater.

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Developing low-cost, high-performance electrocatalysts for the oxygen reduction reaction (ORR) is crucial for implementation of fuel cells and metal-air batteries into practical applications. Graphene-based catalysts have been extensively investigated for ORR in alkaline electrolytes. However, their performance in acidic electrolytes still requires further improvement compared to the Pt/C catalyst. Here we report a self-templating approach to prepare graphene-based sandwich-like porous carbon nanosheets for efficient ORR in both alkaline and acidic electrolytes. Graphene oxides were first used to adsorb m-phenylenediamine molecules which can form a nitrogen-rich polymer network after oxidative polymerization. Then iron (Fe) salt was introduced into the polymer network and transformed into ORR active Fe-N-C sites along with Fe, FeS, and FeN 0.05 nanoparticles after pyrolysis, generating ORR active sandwich-like carbon nanosheets. Due to the presence of multiple ORR active sites. The as-obtained catalyst exhibited prominent ORR activity with a half-wave potential~30 mV more positive than Pt/C in 0.1 mol L −1 KOH, while the half-wave potential of the catalyst was only~40 mV lower than that of commercial Pt/C in 0.1 mol L −1 HClO 4 . The unique planar sandwich-like structure could expose abundant active sites for ORR. Meanwhile, the graphene layer and porous structure could simultaneously enhance electrical conductivity and facilitate mass transport. The prominent electrocatalytic activity and durability in both alkaline and acidic electrolytes indicate that these carbon nanosheets hold great potential as alternatives to precious metalbased catalysts, as demonstrated in zinc-air batteries and proton exchange membrane fuel cells.

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“…However, the dual doping could bring out high asymmetric spin density of C atoms, which plays a much more important role than the atomic charge density in determining the catalytic active sites. or thermal reaction of graphene oxide and solid/gaseous N/S-containing precursors 21,63 (e. g., thiourea or NH 3 /H 2 S gas). The synergistic effect between heteroatoms was also reported for N and S dual-doped graphene, which is eneficial for improving the RR or example, Qiao"s group displayed a very high ORR onset potential of NSG (−0.06 V vs. Ag/AgCl), very close to that of commercial Pt/C (−0.03 V vs.…”

Section: N B-doped Graphenementioning

confidence: 99%

Recent Advances in Heteroatom-Doped Graphene Materials as Efficient Electrocatalysts towards the Oxygen Reduction Reaction

Ma¹,

Ma²,

Yang³

et al. 2016

Nano Adv

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The development of cost-effective, efficient and stable electrocatalysts towards oxygen reduction reaction (ORR) has been an aim to overcome the bottleneck of widespread application of fuel cells and rechargeable metal-air batteries. Unique physicochemical properties of heteroatom-doped graphene open up a brand-new avenue for design and application of metal-free electrocatalysts in these electrochemical devices. Given the flourishing research of graphene and electrochemical energy storage, we critically summarize recent progress in the design, synthesis and application of various heteroatom (N, S, P, B, etc)-doped graphene materials as the electrocatalysts towards ORR. The distinctive properties resulting from various dopants and the resultant electrocatalytic activity are highlighted to gain insights into the mechanism of heteroatom-doped graphene for ORR. We conclude this article with some future trends and opportunities of developing heteroatom-doped-graphene-based electrocatalysts in the application of the ORR-related devices.

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One-pot synthesis of nitrogen and sulfur co-doped graphene as efficient metal-free electrocatalysts for the oxygen reduction reaction

Cited by 308 publications

References 15 publications

Templated synthesis of nitrogen-doped graphene-like carbon materials using spent montmorillonite

Templated synthesis of nitrogen-doped graphene-like carbon materials using spent montmorillonite

Graphene-templated synthesis of sandwich-like porous carbon nanosheets for efficient oxygen reduction reaction in both alkaline and acidic media

Recent Advances in Heteroatom-Doped Graphene Materials as Efficient Electrocatalysts towards the Oxygen Reduction Reaction

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