Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

Chen, Yechuan; Gokhale, Rohan; Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen

doi:10.1016/j.nanoen.2017.05.059

Cited by 86 publications

(47 citation statements)

References 54 publications

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“…[11,12] In spite of the controversial identifications of active sites for Fe-N x -based carbon catalysts in scientific community, there comes a consensus in catalysis that the reactivity would be remarkably improved by downsizing the catalyst to increase the number of active sites. [17][18][19][20] Nevertheless, the fabrication of ISA catalysts remains a grand challenge due to the very high surface energy, easy migration, and serious aggregation of ISAs during catalytic reaction. [17][18][19][20] Nevertheless, the fabrication of ISA catalysts remains a grand challenge due to the very high surface energy, easy migration, and serious aggregation of ISAs during catalytic reaction.…”

Section: Introductionmentioning

confidence: 99%

Isolated Fe Single Atomic Sites Anchored on Highly Steady Hollow Graphene Nanospheres as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

et al. 2018

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The rational design of economical and high‐performance nanocatalysts to substitute Pt for the oxygen reduction reaction (ORR) is extremely desirable for the advancement of sustainable energy‐conversion devices. Isolated single atom (ISA) catalysts have sparked tremendous interests in electrocatalysis due to their maximized atom utilization efficiency. Nevertheless, the fabrication of ISA catalysts remains a grand challenge. Here, a template‐assisted approach is demonstrated to synthesize isolated Fe single atomic sites anchoring on graphene hollow nanospheres (denoted as Fe ISAs/GHSs) by using Fe phthalocyanine (FePc) as Fe precursor. The rigid planar macrocycle structure of FePc molecules and the steric‐hindrance effect of graphene nanospheres are responsible for the dispersion of Fe–Nx species at an atomic level. The combination of atomically dispersed Fe active sites and highly steady hollow substrate affords the Fe ISAs/GHSs outstanding ORR performance with enhanced activity, long‐term stability, and better tolerance to methanol, SO2, and NOx in alkaline medium, outperforming the state‐of‐the‐art commercial Pt/C catalyst. This work highlights the great promises of cost‐effective Fe‐based ISA catalysts in electrocatalysis and provides a versatile strategy for the synthesis of other single metal atom catalysts with superior performance for diverse applications.

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Section: Introductionmentioning

confidence: 99%

Isolated Fe Single Atomic Sites Anchored on Highly Steady Hollow Graphene Nanospheres as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

et al. 2018

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“…Besides, three diffraction peaks were found at approximately 44.4°, 51.6°, and 75.7°, which were ascribed to the corresponding (111), (200), and (220) crystalline lattice facets of composites respectively (JCPDS 43‐1003), illustrating the formation of cobalt nanoparticles. Clearly, the peak intensity of cobalt‐based nanocomposites decreased gradually with the decrease of pyrolysis temperature, which was because the formed graphite was not only used as a supporting material but also served as a reducing agents to reduce cobalt ions to metallic cobalt particles at high temperature . No obvious other diffraction peaks were observed, indicating the purity of the nanoparticles.…”

Section: Resultsmentioning

confidence: 99%

Cobalt‐based Catalysts Modified Cathode for Enhancing Bioelectricity Generation and Wastewater Treatment in Air‐breathing Cathode Microbial Fuel Cells

Zhong

Zhang

et al. 2019

Electroanalysis

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To seek an efficient way to enhance the power output and wastewater treatment of microbial fuel cell (MFC), several cobalt‐based composites are successfully synthesized by a facile hydrothermal method under different pyrolysis temperature, and these composites are used as electrocatalyst in air‐breathing cathode of MFC. Different species of nitrogen atom are successfully grafted on the cobalt‐based composites and confirmed by physical and electrochemical analyses. In MFC tests, the maximum power density increases from 577.8 mW m−2 to 931.1 mW m−2 with pyrolysis temperature (except for 1000 °C). These electrochemical tests and high COD removal show that Co/N/C‐900 can rapidly transfer electron via a 2×2 e− transfer pathway, mainly due to the exposure of large electrochemical active area and introduction of the defects of pyridinic−N and abundant oxygen vacancies. Although the power density of MFC with Co/N/C‐900 is 81.1 % of that of commercial Pt/C, the MFC with Co/N/C‐900 is more stable than that of Pt/C, and the power density for Co/N/C‐900 has only a 2.8 % decrease during 25‐cycles operation. The great electrocatalytic activity of the novel Co/N/C‐900 composite exhibits a superior outlook for scale‐up application of MFC in the future.

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“…The development of highly efficient materials for energy conversion and storage devices is paramount to minimize the consumption of fossil fuels [1][2][3][4]. Fuel cells and supercapacitors, as two of the promising alternatives for traditional energy conversion and storage devices, have attracted special attention [5][6][7].…”

Section: Introductionmentioning

confidence: 99%

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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Novel highly active and selective Fe-N-C oxygen reduction electrocatalysts derived from in-situ polymerization pyrolysis

Cited by 86 publications

References 54 publications

Isolated Fe Single Atomic Sites Anchored on Highly Steady Hollow Graphene Nanospheres as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

Isolated Fe Single Atomic Sites Anchored on Highly Steady Hollow Graphene Nanospheres as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

Cobalt‐based Catalysts Modified Cathode for Enhancing Bioelectricity Generation and Wastewater Treatment in Air‐breathing Cathode Microbial Fuel Cells

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

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