Honeysuckles-derived porous nitrogen, sulfur, dual-doped carbon as high-performance metal-free oxygen electroreduction catalyst

Gao, Shuyan; Liu, Haiying; Geng, Keran; Wei, Xianjun

doi:10.1016/j.nanoen.2015.02.004

Cited by 172 publications

(86 citation statements)

References 57 publications

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“…[6] In recent decades, considerable efforts have committed to exploiting catalysts based on Fe-N-C and N-doped carbons with remarkable ORR activity, which are comparable with commercial Pt/C. [7,8] For instance, Wang et al reported the high-density Fe@N-C material with a positive E 1/2 (0.83 V vs reversible hydrogen electrode (RHE)) than Pt/C (0.82 V vs RHE) and relatively high limiting current density. [2] Su et al developed FeCo nanoparticles encapsulated by N-doped graphitic carbon nanotubes (CNTs) with predominant catalytic activity and stability, preferable to that of noble metal benchmarks.…”

Section: Introductionmentioning

confidence: 99%

Single Fe Atom on Hierarchically Porous S, N‐Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn‐Air Batteries

Zhang

Zeng

et al. 2019

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Iron–nitrogen–carbon materials (Fe–N–C) are known for their excellent oxygen reduction reaction (ORR) performance. Unfortunately, they generally show a laggard oxygen evolution reaction (OER) activity, which results in a lethargic charging performance in rechargeable Zn–air batteries. Here porous S‐doped Fe–N–C nanosheets are innovatively synthesized utilizing a scalable FeCl3‐encapsulated‐porphyra precursor pyrolysis strategy. The obtained electrocatalyst exhibits ultrahigh ORR activity (E1/2 = 0.84 V vs reversible hydrogen electrode) and impressive OER performance (Ej = 10 = 1.64 V). The potential gap (ΔE = Ej = 10 − E1/2) is 0.80 V, outperforming that of most highly active bifunctional electrocatalysts reported to date. Furthermore, the key role of S involved in the atomically dispersed Fe–Nx species on the enhanced ORR and OER activities is expounded for the first time by ultrasound‐assisted extraction of the exclusive S source (taurine) from porphyra. Moreover, the assembled rechargeable Zn–air battery comprising this bifunctional electrocatalyst exhibits higher power density (225.1 mW cm−2) and lower charging–discharging overpotential (1.00 V, 100 mA cm−2 compared to Pt/C + RuO2 catalyst). The design strategy can expand the utilization of earth‐abundant biomaterial‐derived catalysts, and the mechanism investigations of S doping on the structure–activity relationship can inspire the progress of other functional electrocatalysts.

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Section: Introductionmentioning

confidence: 99%

Single Fe Atom on Hierarchically Porous S, N‐Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn‐Air Batteries

Zhang

Zeng

et al. 2019

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“…Thus, instead of decomposing biomass into molecular precursors and then reconstituting them into doped carbon powder, a more energy efficient and simpler process would be to make use of the natural porosity of wood to create channels and fabricate “breathable” carbon plates. This would also allow the mechanical strength of wood and the natural microchannels present in it to be exploited, which would be a distinct advantage over the significantly weaker carbonized powder reconstituted from molecular precursors . Although wood‐derived materials have been used as cathodes for Li–O 2 batteries, on their own, these materials do not display sufficiently high catalytic activities and Ru or RuO 2 have to be loaded on these materials as catalysts .…”

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confidence: 99%

Hierarchically Porous Carbon Plates Derived from Wood as Bifunctional ORR/OER Electrodes

et al. 2019

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oxygen evolution reaction or OER) processes. [1][2][3][4][5] To avoid the use of costly noble metal catalysts, nitrogen-doped porous carbon materials are proposed as the electrode materials in these batteries since they can be derived from naturally abundant biomass. The performance of these porous carbon materials as electrodes depends on the chemistry that results in the generation of OER-active pyridinic N and ORR-active quaternary N groups in a high density as well as the porosity of the materials. [6] This is because these factors determine the extent of exposure of the active sites to the relevant chemical species such as O 2 , OH − , and H 2 O and help prevent the rapid clogging of the planar electrode surface. [7][8][9][10] SiO 2 [8,11,12] and Al 2 O 3[13] microbeads have been employed widely as templates for generating nanopores in carbon-based catalysts. However, this requires multiple steps such as the bottom-up synthesis of the catalysts from carbon precursors as well as etching and purification processes to remove the templates, which increases the cost for mass production. [14][15][16][17][18] In addition, porous carbon materials synthesized by bottom-up methods are generally in the powder form and are thus not self-supporting. Thus, the fabrication of air electrodes requires an additional process, wherein the powder carbon materials are electrosprayed onto carbon cloth/paper, which then lead to the inevitable decreases Porous carbon electrodes have emerged as important cathode materials for metal-air battery systems. However, most approaches for fabricating porous carbon electrodes from biomass are highly energy inefficient as they require the breaking down of the biomass and its subsequent reconstitution into powder-like carbon. Here, enzymes are explored to effectively hydrolyze the partial cellulose in bulk raw wood to form a large number of nanopores, which helps to maximally expose the inner parts of the raw wood to sufficiently dope nitrogen onto the carbon skeletons during the subsequent pyrolysis process. The resulting carbons exhibit excellent catalytic activity with respect to the oxygen reduction and oxygen evolution reactions. As-fabricated cellulosedigested, carbonized wood plates are mechanically strong, have high conductivity, and contain a crosslinked network and natural ion-transport channels and can be employed directly as metal-free electrodes without carbon paper, polymer binders, or carbon black. When used as metal-free cathodes in zincair batteries, they result in a specific capacity of 801 mA h g −1 and an energy density of 955 W h kg −1 with the long-term stability of the batteries being as high as 110 h. This work paves the way for the ready conversion of abundant biomass into high-value engineering products for energy-related applications.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201900341.Rechargeable Zn-air batteries have emerged as a promising technology for coping with future energy demands owin...

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“…S2a, b (online), the highresolution C 1s peak of NDPC-X can be deconvoluted into three peaks at 284.77, 285.89 and 288.84 eV, corresponding to C@C bond, CAN or C@N bond, and CAO or C@O bond, respectively. The C 1s peak at 285.89 eV for CAN or C@N bond confirmed the nitrogen doping [40,41]. According to the XPS survey spectra, the percentage of nitrogen atoms in materials was 2.10 at.% for NDPC-800, 2.07 at.% for NDPC-900 and 2.0 at.% for NDPC-1000, respectively.…”

Section: Results and Conclusionmentioning

confidence: 69%

Bifunctional 3D n-doped porous carbon materials derived from paper towel for oxygen reduction reaction and supercapacitor

Gao

Kong

et al. 2018

Science Bulletin

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a b s t r a c tDesigning and fabricating cheap and active bifunctional materials is crucial for the development of renewable energy technologies. In this article, three-dimensional nitrogen-doped porous carbon materials (NDPC-X, in which X represents the pyrolysis temperature) were fabricated by simultaneous carbonization and activation of polypyrrole-coated paper towel protected by a silica layer followed by acid etching. The material had a high specific surface area (1,123.40 m 2 /g). The as-obtained NDPC-900 displayed outstanding activity as a catalyst for the oxygen reduction reaction (ORR) as well as an electrode with a high specific capacitance in a supercapacitor in an alkaline medium. The NDPC-900 catalyst for the ORR exhibited a more positive reduction peak potential of À0.068 V (vs. Hg|HgCl 2 ) than that of Pt/ C (À0.121 V), as well as better cycling stability and stronger methanol tolerance. Moreover, the NDPC-900 had a high specific capacitance of 379.50 F/g at a current density of 1 A/g, with a retention rate of 94.5% after 10,000 cycles in 6 mol/L KOH electrolyte when used as an electrode in a supercapacitor. All these results were attributed to the effect of a large surface area, which provided electrochemically active sites. This work introduces an effective way to use biomass-derived materials for the synthesis of promising bifunctional carbon material for electrochemical energy conversion and storage devices.

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Honeysuckles-derived porous nitrogen, sulfur, dual-doped carbon as high-performance metal-free oxygen electroreduction catalyst

Cited by 172 publications

References 57 publications

Single Fe Atom on Hierarchically Porous S, N‐Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn‐Air Batteries

Single Fe Atom on Hierarchically Porous S, N‐Codoped Nanocarbon Derived from Porphyra Enable Boosted Oxygen Catalysis for Rechargeable Zn‐Air Batteries

Hierarchically Porous Carbon Plates Derived from Wood as Bifunctional ORR/OER Electrodes

Bifunctional 3D n-doped porous carbon materials derived from paper towel for oxygen reduction reaction and supercapacitor

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