Trifunctional electrocatalyst of N-doped graphitic carbon nanosheets encapsulated with CoFe alloy nanocrystals: The key roles of bimetal components and high-content graphitic-N

Wang, Saijun; Wang, Haiyan; Huang, Chuanqi; Ye, Pengcheng; Luo, Xiting; Ning, Jiqiang; Zhong, Yijun; Hu, Yong

doi:10.1016/j.apcatb.2021.120512

Cited by 128 publications

(40 citation statements)

References 52 publications

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“…The higher Fe content means the higher density of Fe-based active sites for catalyzing O 2 reduction, and the incorporation of Fe is also conducive to the formation of graphitic-N during high-temperature pyrolysis. [60] Compared with Fe-PoPD-800 and Fe-PmPD-800, Fe-PpPD-800 has the highest proportion of FeN, graphite-N and pyridine-N, and these nitrogen species are reported to have an active role in the enhancement of ORR performance. [51,52] Concretely, pyridine-N can capture protons and oxygen molecules to enhance the reduction of O 2 , graphite-N improves the conductivity of the catalyst and facilitates the four-electron ORR pathway, while FeN species is considered to be an efficient ORR catalytic active site.…”

Section: Resultsmentioning

confidence: 98%

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

Hong

Huang

et al. 2022

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Single atom Fe–nitrogen–carbon (Fe–N–C) catalysts have high catalytic activity and selectivity for the oxygen reduction reaction (ORR), and are possible alternatives for Pt‐based materials. However, the reasonable design and selection of precursors to establish their relationship with Fe–N–C catalyst performance is still a formidable task. Herein, precursors with controllable structures are easily achieved through isomer engineering, with the purpose of regulating the active site density and microscopic morphology of the final electrocatalyst. As‐proof‐of‐concept, phenylenediamine isomers‐based polymers are used as precursors to fabricate Fe–N–C catalysts. The Fe–PpPD‐800 derived from p‐phenylenediamine shows that the best ORR activity with a half‐wave potential (E1/2) reaches 0.892 V vs reversible hydrogen electrode (RHE), which is better than the counterparts derived from o‐phenylenediamine (Fe–PoPD‐800) and m‐phenylenediamine (Fe–PmPD‐800), even surpassing commercial Pt/C (E1/2 = 0.881 V vs RHE). Furthermore, the self‐made zinc–air battery based on Fe–PpPD‐800 achieves high power density and specific capacity up to 242 mW cm−2 and 873 mA h gZn−1 respectively, a stable open circuit voltage of 1.45 V, and excellent cycling stability. This work not only proves the practicability of adjusting the catalytic activity of single‐atom catalysts through isomer engineering, but also provides an approach to understand the relationship between precursors and target catalysts performance.

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Section: Resultsmentioning

confidence: 98%

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

Hong

Huang

et al. 2022

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“…Recently, several multifunctional electrocatalysts have been reported, including non-noble or noble metal catalysts. Non-noble metal catalysts usually involve iron, cobalt, and nickel-based alloys/oxides/phosphides/sulfides/carbides/nitrides coupled with carbon substrate, such as CoFe@NC/NCHNSs, Ni-NiO/N-rGO, FeCo/Co 2 P@NPCF, Co 2 P/CoNPC, FeS/Fe 3 C@N-S-C, Fe 2 N/S/N, etc. However, these non-noble metal catalysts still exhibit insufficient activities and durability, especially when used as trifunctional electrocatalysts for ORR/OER/HER simultaneously.…”

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confidence: 99%

RuCoO_x Nanofoam as a High-Performance Trifunctional Electrocatalyst for Rechargeable Zinc–Air Batteries and Water Splitting

et al. 2021

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Designing high-performance trifunctional electrocatalysts for ORR/OER/HER with outstanding activity and stability for each reaction is quite significant yet challenging for renewable energy technologies. Herein, a highly efficient and durable trifunctional electrocatalyst RuCoO x is prepared by a unique one-pot glucose-blowing approach. Remarkably, RuCoO x catalyst exhibits a small potential difference (ΔE) of 0.65 V and low HER overpotential of 37 mV (10 mA cm −2 ), as well as a negligible decay of overpotential after 200 000/10 000/10 000 CV cycles for ORR/OER/HER, all of which show overwhelming superiorities among the advanced trifunctional electrocatalysts. When used in liquid rechargeable Zn−air batteries and water splitting electrolyzer, RuCoO x exhibits high efficiency and outstanding durability even at quite large current density. Such excellent performance can be attributed to the rational combination of targeted ORR/OER/HER active sites into one electrocatalyst based on the double-phase coupling strategy, which induces sufficient electronic structure modulation and synergistic effect for enhanced trifunctional properties.

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“…Proverbially, at low scan rates (2 mV À 1 ~10 mV À 1 ), the electrolyte ion has enough time to migrate into micropores. [38,39] However, at high scan rates (200 mV À 1 ~500 mV À 1 ), the movement of ion in the micropores is delayed, resulting in capacitive decay. In this work, the superior rate ability of NPS-CN 2 is ascribed to the 3D cross-linked structure and the enhanced conductivity after heteroatoms doping.…”

Section: Resultsmentioning

confidence: 99%

Synthesis of N/P/S Co‐Doped 3D Cross‐Linked Carbon Nanosheets by Double Activation Method for High‐Performance Supercapacitors

et al. 2022

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It is still a challenge to prepare heteroatoms‐doped carbon materials for supercapacitors by an acid‐free and alkali‐free synthesis method. Herein, the N/P/S co‐doped carbon nanosheets (NPS‐CNs) were synthesized by an in‐situ K2CO3 and Na2S2O3 ⋅ 5H2O double activation method from pyrene as carbon source, melamine‐phytic acid supramolecular aggregate as N and P source without the presence of acid and alkali. The as‐prepared NPS‐CN featured three‐dimensional cross‐linked nanosheets with abundant pores, boosting the stability of carbon skeleton and promoting the transfer of ion and electron. The abundant micropores together with high heteroatom content (15.09 %) provided abundant active sites and defects for ion adsorption. Benefitting from these merits, the NPS‐CN electrode exhibits a high specific capacitance of 485.1 F g−1 at 0.05 A g−1 as well as good rate performance of 350.3 F g−1 at 20 A g−1 in three electrode system. Simultaneously, the specific capacitance of the NPS‐CN capacitor reached 305.0 F g−1 at 0.05 A g−1 and retained 201.2 F g−1 at 100 A g−1 in two electrode system. Importantly, NPS‐CN capacitor presented an excellent cycle stability (93.4 % of initial capacitance after 30,000 charge/discharge cycles). This work opened a less harmful route to prepare NPS‐CNs from small polycyclic aromatic hydrocarbons for energy storage devices.

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Trifunctional electrocatalyst of N-doped graphitic carbon nanosheets encapsulated with CoFe alloy nanocrystals: The key roles of bimetal components and high-content graphitic-N

Cited by 128 publications

References 52 publications

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

RuCoO_x Nanofoam as a High-Performance Trifunctional Electrocatalyst for Rechargeable Zinc–Air Batteries and Water Splitting

Synthesis of N/P/S Co‐Doped 3D Cross‐Linked Carbon Nanosheets by Double Activation Method for High‐Performance Supercapacitors

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Trifunctional electrocatalyst of N-doped graphitic carbon nanosheets encapsulated with CoFe alloy nanocrystals: The key roles of bimetal components and high-content graphitic-N

Cited by 128 publications

References 52 publications

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

Deciphering the Precursor–Performance Relationship of Single‐Atom Iron Oxygen Electroreduction Catalysts via Isomer Engineering

RuCoOx Nanofoam as a High-Performance Trifunctional Electrocatalyst for Rechargeable Zinc–Air Batteries and Water Splitting

Synthesis of N/P/S Co‐Doped 3D Cross‐Linked Carbon Nanosheets by Double Activation Method for High‐Performance Supercapacitors

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RuCoO_x Nanofoam as a High-Performance Trifunctional Electrocatalyst for Rechargeable Zinc–Air Batteries and Water Splitting