Synergistic Effects between Atomically Dispersed Fe−N−C and C−S−C for the Oxygen Reduction Reaction in Acidic Media

Shen, Hong; Gracia‐Espino, Eduardo; Ma, Jingyuan; Zang, Ketao; Luo, Jun; Wang, Le; Gao, Sanshuang; Mamat, Xamxikamar; Hu, Guangzhi; Wågberg, Thomas; Guo, Shaojun

doi:10.1002/ange.201706602

Cited by 110 publications

(52 citation statements)

References 43 publications

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“…The two peaks at 164.0 and 165.2 eV can be described to S 2p 3/2 and S 2p 1/2 of thiophene-like C-S-C structure, respectively [32,33], while the third peak at 167.3 eV corresponds to sulfate species. The synergetic effects of N, S co-doping would significantly improve the ORR activity by reducing the electron localization around the Fe centers, and improve the interaction with oxygen, facilitating the four-electron pathway [34]. The high-resolution Fe 2p spectrum of Fe/NS/C-g-C 3 N 4 /TPTZ-1000 presents two major peaks at around 711 and 724 eV, corresponding to Fe 2p 1/2 and Fe 2p 3/2 , respectively (Figure 6f) [15,35].…”

Section: Resultsmentioning

confidence: 99%

Binary Nitrogen Precursor-Derived Porous Fe-N-S/C Catalyst for Efficient Oxygen Reduction Reaction in a Zn-Air Battery

et al. 2018

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Abstract:It is still a challenge to synthesize non-precious-metal catalysts with high activity and stability for the oxygen reduction reaction (ORR) to replace the state-of-the art Pt/C catalyst. Herein, a Fe, N, S co-doped porous carbon (Fe-NS/PC) is developed by using g-C 3 N 4 and 2,4,6-tri(2-pyridyl)-1,3,5-triazine (TPTZ) as binary nitrogen precursors. The interaction of binary nitrogen precursors not only leads to the formation of more micropores, but also increases the doping amount of both iron and nitrogen dispersed in the carbon matrix. After a second heat-treatment, the best Fe/NS/C-g-C 3 N 4 /TPTZ-1000 catalyst exhibits excellent ORR performance with an onset potential of 1.0 V vs. reversible hydrogen electrode (RHE) and a half-wave potential of 0.868 V (RHE) in alkaline medium. The long-term durability is even superior to the commercial Pt/C catalyst. In the meantime, an assembled Zn-air battery with Fe/NS/C-g-C 3 N 4 /TPTZ-1000 as the cathode shows a maximal power density of 225 mW·cm −2 and excellent durability, demonstrating the great potential of practical applications in energy conversion devices.

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Section: Resultsmentioning

confidence: 99%

Binary Nitrogen Precursor-Derived Porous Fe-N-S/C Catalyst for Efficient Oxygen Reduction Reaction in a Zn-Air Battery

et al. 2018

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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: 70%

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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“…The peaks at 168.2 eV and 169.4 eV can be ascribed to SOx species. The previous work has demonstrated that S‐doping can increase the ORR catalytic activity of Fe/N/C materials because of the electronegativity, polarizability and large atomic radius of S atom . Moreover, Figure F shows the high‐resolution spectrum of Fe2p, which can be separated into two pairs of peaks for Fe 3+ (725.2 and 713.5 eV) and Fe 2+ (722.4 and 710.8 eV), corresponding to the Fe 3 O 4 and doped‐Fe in the NCMs.…”

Section: Resultsmentioning

confidence: 88%

Self‐Assembly Synthesis of Mulberry‐Like Fe/N/S‐Doped Highly Porous Carbon Materials: Efficient and Stable Catalysts for Oxygen Reduction Reaction

Liu

2018

ChemNanoMat

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In this work, unique structures of mulberry‐like Fe/N/S‐doped nanoporous carbon materials (NCMs) are synthesized via a simple self‐assembly assisted process. The Fe2+‐mediated polymerization of dopamine (DA) and further interaction with triblock copolymer F127 micelles induce the formation of mulberry‐like Fe/PDA/F127 structures. After carbonization, the Fe/N/S‐doped NCMs are obtained with a highly porous structure and large Brunauer‐Emmett‐Teller (BET) surface area of 913.2 m2 g−1. Moreover, DA and iron salt introduce active sites, such as Sp2 C, graphitic N, pyridinic N, Fe−Nx, C−S−C, etc. Benefiting from these unique structural features and chemical compositions, the optimized Fe/N/S‐doped NCMs exhibit enhanced electrocatalytic activity and excellent durability for oxygen reduction reaction (ORR) compared with commercial Pt/C catalyst. These studies provide not only a new synthesis method for heteroatom‐doped NCMs, but also a platform for various applications.

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Synergistic Effects between Atomically Dispersed Fe−N−C and C−S−C for the Oxygen Reduction Reaction in Acidic Media

Cited by 110 publications

References 43 publications

Binary Nitrogen Precursor-Derived Porous Fe-N-S/C Catalyst for Efficient Oxygen Reduction Reaction in a Zn-Air Battery

Binary Nitrogen Precursor-Derived Porous Fe-N-S/C Catalyst for Efficient Oxygen Reduction Reaction in a Zn-Air Battery

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

Self‐Assembly Synthesis of Mulberry‐Like Fe/N/S‐Doped Highly Porous Carbon Materials: Efficient and Stable Catalysts for Oxygen Reduction Reaction

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