Porous carbon framework derived from N-rich hypercrosslinked polymer as the efficient metal-free electrocatalyst for oxygen reduction reaction

Yang, Zifeng; Han, Jingxin; Jiao, Rui; Sun, Hanxue; Zhu, Zhaoqi; Liang, Weidong; An, Li

doi:10.1016/j.jcis.2019.09.069

Cited by 35 publications

(21 citation statements)

References 51 publications

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“…Figure 4A showed the N 1s XPS spectrum of Co-OPD-800, corresponding to oxide nitrogen (403 eV), graphite nitrogen (401.1 eV), pyrrole nitrogen (400.0 eV), pyridine nitrogen (398.3 eV) and Co-N (398.0 eV), which indicates that part of cobalt metal elements successfully entered the carbon skeleton. 49 Comparing with the characteristic peak in Figure 4A, the characteristic peak of Fe-N at 399.4 eV also appears in Figure 4B. Apart from the N peaks of various binding states, the characteristic peak of Fe-N appears at 399.4 eV in Figure 4C.…”

Section: Structure Characterization and Electrochemical Performance Test Of Co-opd-800 Fecl 3 -Opd-800 And Fecl 3 -Co-opd-800 Catalystsmentioning

confidence: 74%

“…The result implied the presence of more defective sites in Co-OPD-800, which are conductive to current conduction. 44,49 It indicates that the Co-OPD catalyst has more oxygen reduction activity at the pyrolysis temperature of 800 C, which has a significant influence on its ORR performance.…”

Section: Effect Of Pyrolysis Temperature On the Structure And Electrochemical Performance Of Co-opd Catalystmentioning

confidence: 99%

“…The content of pyridine nitrogen is consistent with the subsequent electrochemical performance, which verifies the conjecture that the Lewis basic carbon atom connected to the pyridine nitrogen is the catalytically active site. 43,44,49 Moreover, to further explore the degree of graphitization and defects of the samples, the experiments are carried out the Raman analysis of three catalysts. The ID/IG ratios of Co-OPD-800, FeCl 3 -Co-OPD-800, and FeCl 3 -OPD-800 are 1.348, 1.369, and 1.42, respectively.…”

Section: Structure Characterization and Electrochemical Performance Test Of Co-opd-800 Fecl 3 -Opd-800 And Fecl 3 -Co-opd-800 Catalystsmentioning

confidence: 99%

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N‐rich mesoporous carbon supported CoNC and FeNC catalysts derived from o‐phenylenediamine for oxygen reduction reaction

et al. 2021

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The exploitation of high efficiency non-precious electrocatalysts for oxygen reduction reaction (ORR) is of great significance for large-scale commercialization of next-generation fuel cells. Herein, we report the synthesis of conjugated polymers (CP) based on poly(o-phenylenediamine) as a nitrogen-containing precursor for preparation of Co-and FeCl 3 -doped N-rich carbon for ORR (abbreviated as Co-OPD and FeCl 3 -OPD). Based on their high specific surface, excellent porosity and large pyridine nitrogen content, the as-synthesized FeCl 3 -OPD, which is prepared at a pyrolysis temperature of 800 C (FeCl 3 -OPD-800), exhibits highest catalytic activity among the resulting electrocatalysts, that is, it possesses a largest half-wave potential of 0.854 V (≈20 mV more positive than Pt/C), a high diffusion limiting current density of 3.95 mA cm −2 and a biased 4e − reaction pathway. In addition, this catalyst also discloses an excellent methanol tolerance and better durability than the commercial Pt/C. Taking advantage of their high ORR activity as well as simple fabrication which makes it possible using inexpensive FeCl 3 as both catalysts for CP precursors and metal dopant for FeCl 3 -OPD only by a one-step pyrolysis, thus such FeCl 3 -OPD may hold great potentials as promising alternative of precious metal catalysts for next generation fuel cells.

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Section: Structure Characterization and Electrochemical Performance Test Of Co-opd-800 Fecl 3 -Opd-800 And Fecl 3 -Co-opd-800 Catalystsmentioning

confidence: 74%

Section: Effect Of Pyrolysis Temperature On the Structure And Electrochemical Performance Of Co-opd Catalystmentioning

confidence: 99%

Section: Structure Characterization and Electrochemical Performance Test Of Co-opd-800 Fecl 3 -Opd-800 And Fecl 3 -Co-opd-800 Catalystsmentioning

confidence: 99%

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N‐rich mesoporous carbon supported CoNC and FeNC catalysts derived from o‐phenylenediamine for oxygen reduction reaction

et al. 2021

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“…Previously, the introduction of N plays a much important role for carbon‐based materials in ORR, which can be ascribed to doped N can form a strong covalent C–N bond with C. The electronegativity of N can destroy the charge neutrality of C on the sp 2 carbon lattice and provide more electrons to improve the adsorption of oxygen molecules. [ 23 ] The nitrogen modifies the band structure of carbon, raising the density of p states near the Fermi level and lowering the work function. In addition, the subsequent electrochemical test results also confirmed the doping of nitrogen atoms is beneficial to ORR activity.…”

Section: Resultsmentioning

confidence: 99%

Novel Porphyrin‐Based Hypercrosslinked Polymers as Highly Efficient Electrocatalysts for Oxygen Reduction Reaction

et al. 2022

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The exploration of high‐performance electrocatalysts is significant to improve the sluggish oxygen reduction reaction (ORR) speed in electrochemical systems. Here, the creation of novel non‐precious metal catalysts via knitting hypercrosslinked polymer (TPP‐HCP‐1) based on porphyrin as the building block which contains both mesopore and catalytic sites, is demonstrated. Interestingly, the TPP‐HCP can be converted into a nitrogen‐doped porous carbon skeleton through pyrolyzing the hybrid at 900 °C, which possesses an excellent ORR electrochemical performance in alkaline medium, with a more positive onset potential of 0.96 V (vs reversible hydrogen electrode, the same in the following), half‐wave potential of 0.85 V, and higher diffusion limiting current density of 4.00 mA cm−2. Moreover, it also exhibits much higher stability, comparable selectivity, and better methanol tolerance than the commercial Pt/C. Making good use of their high ORR activity and easy fabrication makes it possible to use low‐cost FeCl3 as both catalysts for HCP precursors and metal dopant for the porphyrin‐based hypercrosslinked polymer (TPP‐HCP‐1), thus the obtained TPP‐HCP‐1 may offer novel ideation to construct non‐precious metal catalysts for practical electrocatalytic applications.

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“…An HCP synthesized by direct knitting of pyrrole monomer and FDA cross‐linker was subjected to pyrolysis at 900 °C, and the obtained nitrogen‐doped carbon showed outstanding catalytic activity toward ORR in alkaline medium. [ 93 ] Therefore, pyrolysis of HCP materials may open a new possibility for the design of ORR metal‐free and cost‐effective catalyst of fuel‐cell technologies.…”

Section: Catalytic Applications Of Hypercrosslinked Polymers Construcmentioning

confidence: 99%

Low‐Cost Hypercrosslinked Polymers by Direct Knitting Strategy for Catalytic Applications

Son

et al. 2020

Adv Funct Materials

116

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Direct knitting of nucleophilic arene monomers in the presence of electrophilic cross‐linker, like formaldehyde dimethyl acetal, is proven to be a cost‐effective and versatile method for the synthesis of porous organic polymers. The resulting hypercrosslinked polymers (HCPs) are featured by hierarchical porous structure, high surface area, and pore volume. Coordinating functional groups can be easily installed with this method into the rigid aryl network. Direct knitting to HCPs has therefore been widely used in preparing heterogeneous solid catalysts. Wise selection of monomers with rational design of 3D structure and the synergy between the HCP support and the catalytically active species often lead to high efficiency of tailor‐made catalysts without sophisticated operations. On account of all these excellent properties, enthusiasm of researchers to use HCPs in catalysis is increasing rapidly. This review documents the necessity, feasibility, and the great contributions of using HCPs as invaluable tools for catalysis research, and summarizes state of the art of this chemistry. Similar type catalysts obtained by one‐step Scholl reaction are also included in this review.

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Porous carbon framework derived from N-rich hypercrosslinked polymer as the efficient metal-free electrocatalyst for oxygen reduction reaction

Cited by 35 publications

References 51 publications

N‐rich mesoporous carbon supported CoNC and FeNC catalysts derived from o‐phenylenediamine for oxygen reduction reaction

N‐rich mesoporous carbon supported CoNC and FeNC catalysts derived from o‐phenylenediamine for oxygen reduction reaction

Novel Porphyrin‐Based Hypercrosslinked Polymers as Highly Efficient Electrocatalysts for Oxygen Reduction Reaction

Low‐Cost Hypercrosslinked Polymers by Direct Knitting Strategy for Catalytic Applications

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