A simple decagram-scale synthesis of an atomically dispersed, hierarchically porous Fe–N–C catalyst for acidic ORR

Koyutürk, Burak; Farber, Eliyahu M.; Wagner, F. E.; Fellinger, Tim‐Patrick; Eisenberg, David

doi:10.1039/d2ta00925k

Cited by 15 publications

(14 citation statements)

References 71 publications

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“…In the active site imprinting concept, proposed by Fellinger et al, the templating lanthanoid ions bind and retain the nitrogen atoms during the pyrolysis, and can later be replaced (transmetalated) with a catalytically active metal such as iron. [55][56][57][58] We have performed such an iron transmetalation by refluxing the NC Ln in a methanol solution of an iron salt, followed by washing and drying. The resulting materials (dubbed FeNC Ln ) contain very high nitrogen content (8.9-12.1 at%, Table 1).…”

Section: Formation Of Lanthanoid-imprinted Fe-n-c Active Sitesmentioning

confidence: 99%

“…The self-templating strategy can be enhanced even further with the simultaneous imprinting of catalytic sites, following the Fellinger method (Figure 1). [55][56][57][58] Metal-nonmetal moieties that form during pyrolysis (e.g. Zn 2+ -N 4 or Mg 2+ -N 4 ), can be transmetalated by catalytic elements such as Fe 2+ .…”

Section: Introductionmentioning

confidence: 99%

“…1). [55][56][57][58] Metal-nonmetal moieties that form during pyrolysis (e.g. Zn 2+ -N 4 or Mg 2+ -N 4 ), can be transmetalated by catalytic elements such as Fe 2+ .…”

Section: Introductionmentioning

confidence: 99%

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Lanthanoid coordination compounds as diverse self-templating agents towards hierarchically porous Fe–N–C electrocatalysts

et al. 2022

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Section: Formation Of Lanthanoid-imprinted Fe-n-c Active Sitesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Lanthanoid coordination compounds as diverse self-templating agents towards hierarchically porous Fe–N–C electrocatalysts

et al. 2022

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“…For instance, magnesium was used as a dual template to form Mg-N4 sites by pyrolysis and generate graphitized carbon containing 43% "surface Fe-N4" sites via a low-temperature transmetalation step. 17 Zinc is used as a sacrificial metal with MOF as the precursor, largely removed after high-temperature pyrolysis and washing, leaving empty Nx sites. Then the obtained sites were converted to the Fe-Nx sites with high ORR activity, 20 or by adsorption and heat-treatment to get the Ni-Nx sites with CO2RR activity.…”

Section: Introductionmentioning

confidence: 99%

“…Recently, the coordination synthesis of M-N-C electrocatalysts on nitrogen-doped carbon (N-C) templates with rich MNx sites induced by sacrificial metals (SM) has received great attention. [15][16][17][18][19][20][21][22][23] The related works introduced SM to create SMNx structures or metal-vacancy-Nx (MVNx) sites on the carbon matrix, and then formed MNx sites with high activity and site density via a wet-chemical metal-coordination step and high-temperature treatment. For instance, magnesium was used as a dual template to form Mg-N4 sites by pyrolysis and generate graphitized carbon containing 43% "surface Fe-N4" sites via a low-temperature transmetalation step.…”

Section: Introductionmentioning

confidence: 99%

Solution-Phase Synthesis of Co-N-C Catalysts Using Alkali Metals-Induced N-C Templates with Metal Vacancy-Nx sites

Huang

Chen

Ding

et al. 2022

Preprint

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Nitrogen-coordinated metal sites (MNx) in metal- and nitrogen-co-doped carbon (M-N-C) catalysts are known for their versatile and promising electrocatalytic activity. However, the synthesis of MNx moieties with desired configuration and catalytic property is still quite challenging using the conventional high-temperature treatment approach. In this study, we demonstrate the solution-phase synthesis of Co-N-C catalysts via the formation of CoNx moieties at metal vacancy-Nx (MVNx) sites on nitrogen-doped carbon (N-C) templated by alkali metals, including sodium and potassium. The formation of CoNx sites is confirmed via a combined approach of various physical characterization techniques, elemental analysis, and electrochemical analysis. For each series of Co-N-C catalysts templated by the same alkali metal (e.g., Na or K), there is a correlation between the CoNx content and the electrocatalytic activity for the oxygen reduction reaction (ORR). Moreover, the correlation of CoNx content with ORR activity also depends on the type of sacrificial alkali metals, suggesting the role of sacrificial metals in creating MVNx sites with a diverse coordination environment. These findings may further guide the future development of M-N-C electrocatalysts with abundant and versatile MNx moieties through this solution-phase coordination approach.

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F‐Doped Co−N−C Catalysts for Enhancing the Oxygen Reduction Reaction in Zn‐Air Batteries

Guo

Yang

et al. 2023

ChemCatChem

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Zn‐air battery is a promising next‐generation energy storage device. Its performance, however, is limited by a high overpotential resulted from the slow kinetics of the cathodic oxygen reduction reaction (ORR). This study reports a simple strategy for preparation of a fluorine‐doped Co−N−C composite as highly efficient electrocatalyst for ORR. The C@PVI‐(TPFC)Co‐800 catalyst was prepared by pyrolysis of F‐containing Co‐corrole that was assembled on PVI‐functionalized carbon black through the axial imidazole coordination (PVI=polyvinylimidazole, TPFC=5,10,15‐triperfluorophenyl‐21H, 22H‐corrole). The C@PVI‐(TPFC)Co‐800 catalyst exhibited much more positive ORR half‐wave potential (E1/2=0.88 V vs. RHE) than its counterpart C@PVI‐(TPC)Co‐800 (E1/2=0.82 V, TPC=5,10,15‐triphenyl‐21H, 22H‐corrole) without F‐doping in 0.1 M KOH electrolyte. C@PVI‐(TPFC)Co‐800 also achieved a greater kinetic current density and enhanced durability in alkaline media. In addition, a Zn‐air battery with C@PVI‐(TPFC)Co‐800 loaded at the cathode delivered much higher peak power density (Pmax=141 mW/cm2) and open‐circuit voltage (OCV=1.45 V) over the C@PVI‐(TPC)Co‐800 counterpart (Pmax=110 mW/cm2, OCV=1.39 V) and the commercial 20 % Pt/C (Pmax=119 mW/cm2, OCV=1.42 V) as well. The promoted catalyst performance for ORR was attributed to the increased specific surface area, more defects generated, and reduced electron density distribution around the Co metal center after F‐doping.

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A simple decagram-scale synthesis of an atomically dispersed, hierarchically porous Fe–N–C catalyst for acidic ORR

Abstract: Carbons doped with iron and nitrogen (Fe–N–Cs) are highly promising electrocatalysts for energy conversion reactions in the oxygen, nitrogen and carbon cycles. Containing no platinum group metals, they nevertheless compete...

Cited by 15 publications

References 71 publications

Lanthanoid coordination compounds as diverse self-templating agents towards hierarchically porous Fe–N–C electrocatalysts

Lanthanoid coordination compounds as diverse self-templating agents towards hierarchically porous Fe–N–C electrocatalysts

Solution-Phase Synthesis of Co-N-C Catalysts Using Alkali Metals-Induced N-C Templates with Metal Vacancy-Nx sites

F‐Doped Co−N−C Catalysts for Enhancing the Oxygen Reduction Reaction in Zn‐Air Batteries

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