Unraveling the amine oxidative coupling activity of hierarchical porous Fe–N<sub>4</sub>–O<sub>1</sub> single-atom catalysts: oxygen atom-mediated dual reaction pathway

He, Hong; Ma, Kui; Liu, Huibin; Li, Jing; Zheng, Lirong; Zhang, Fengbao; Fan, Xiaobin; Peng, Wenchao; Ji, Junyi; Li, Yang

doi:10.1039/d2ta07198c

Cited by 7 publications

(2 citation statements)

References 49 publications

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“…Nanocomposites of nickel–iron sulfide and carbon nanotubes are revealed for application of supercapacitors 10 . High atomic level Fe (Iron) loading density for the understanding of electronic structure modulation and intrinsic activity aimed at high-efficiency catalyst are designed toward oxidation-related reactions 11 . Pen et al 12 had developed a novel spin regularization strategy to prepare regularized GO membranes with ordered and stable laminar structures through uniform interlayer mass transfer channels (exhibits a high gravimetric capacitance) for high-performance electrodes for obtaining high electron and charge transfer capability that can meet the increasing requirement for high-rate energy storage devices.…”

Section: Introductionmentioning

confidence: 99%

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Zainab

Azeem

Awan

et al. 2023

Sci Rep

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In this report we have developed different fabrication parameters to tailor the optical bandgap of graphene oxide (GO) nanosheets to make it operational candidate in electronic industry. Here we performed two ways to reduce the bandgap of GO nanosheets. First, we have optimized the oxidation level of GO by reducing amount of oxidizing agent (i.e. KMnO4) to control the sp2/sp3 hybridization ratio for a series of GO nanosheets samples. We noticed the reduction in primary band edge 3.93–3.2 eV while secondary band edge 2.98–2.2 eV of GO nanosheets as the amount of KMnO4 is decreased from 100 to 30%. Second, we have fabricated a series of 2-dimensional nanocomposites sample containing GO/Iron-oxide by using a novel synthesis process wet impregnation method. XRD analysis of synthesized nanocomposites confirmed the presence of both phases,$$\alpha$$ α -Fe2O3 and Fe3O4 of iron-oxide with prominent plane (001) of GO. Morphological investigation rules out all the possibilities of agglomerations of iron oxide nanoparticles and coagulation of GO nanosheets. Elemental mapping endorsed the homogeneous distribution of iron oxide nanoparticles throughout the GO nanosheets. Raman spectroscopy confirmed the fairly constant ID/IG ratio and FWHM of D and G peaks, thus proving the fact that the synthesis process of nanocomposites has no effect on the degree of oxidation of GO flakes. Red shift in G peak position of all the nanocomposites samples showed the electronic interaction among the constituents of the nanocomposite. Linear decrease in the intensity of PL (Photoluminescence) spectra with the increasing of Iron oxide nanoparticles points towards the increased interaction among the iron oxide nanoparticles and GO flakes. Optical absorption spectroscopy reveals the linear decrease in primary edge of bandgap from 2.8 to 0.99 eV while secondary edge decrease 3.93–2.2 eV as the loading of $$\alpha$$ α -Fe2O3 nanoparticles is increased from 0 to 5% in GO nanosheets. Among these nanocomposites samples 5%-iron-oxide/95%-GO nanosheet sample may be a good contestant for electronic devices.

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Section: Introductionmentioning

confidence: 99%

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Zainab

Azeem

Awan

et al. 2023

Sci Rep

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“…When 5,5dimethyl-2-pyrrolidone-N-oxyl (DMPO) was used as trapping agent, signals originating from DMPO− • OH and DMPO− • OOH (Figure 8b) were detected under otherwise identical experimental conditions. A plausible reaction pathway (Figure 8c) for the synthesis of imines catalyzed by 3D Fe-600−800 is proposed based on the EPR results: 39 In the initial stage, Fe−N 3 moieties with cooperation with Fe 3 C NPs effectively activate benzylamine and molecular oxygen to form the corresponding cationic amine radical and 1 O 2 . The existence of singlet oxygen significantly promotes the transformation of the cation radical complex to the key imine intermediate (PhCH = NH), producing hydrogen peroxide (H 2 O 2 ) simultaneously.…”

Section: Reaction Mechanismmentioning

confidence: 99%

Macroporous Carbon-Supported Fe-Based Catalysts for the Solvent-Free Oxidative Coupling of Benzylamine

Lu,

Schwiderowski,

Shen

et al. 2024

Chem. Mater.

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Transition metal and nitrogen codecorated carbon materials have recently emerged as robust and efficient heterogeneous catalysts because of their unique electronic structure, superior activity, and high metal utilization. The most popular synthetic strategy for those catalysts is the direct pyrolysis of C-and N-containing precursors and metal salts, but the obtained products often suffer from structural heterogeneity of the active metal sites and poor mass transport. Herein, a hard template-assisted metal coordinated polymer is developed to synthesize a series of threedimensional (3D) M-600-X (M = Fe, Co, Ni, Cu; X = 700, 800, 900 °C) catalysts with an advanced trimodal pore structure via a well-controlled two-step pyrolysis. Due to a preliminary annealing at 600 °C, it is possible to control the coordination configuration of the M−N x moiety and the metal speciation by regulating the subsequent pyrolysis temperature. The 3D Fe-600-800 catalyst exhibited excellent catalytic performance in the oxidative coupling of benzylamine under solvent-free conditions due to the active Fe−N 3 moiety as well as the synergy between the atomic Fe sites and the Fe/Fe 3 C nanoparticles. Moreover, this synthetic approach can also be employed in gram-scale production, and the obtained catalysts still possess superior activity and favorable stability, even in large-scale imine production. Thus, this work enables the rational design of cost-effective carbon-supported transition metal-based catalysts for highly efficient organic transformation.

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Wastewater flocculation substrate derived three-dimensional ordered macroporous Co single-atom catalyst for singlet oxygen-dominated peroxymonosulfate activation

Guo

Zhang

et al. 2023

Applied Catalysis B: Environmental

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Unraveling the amine oxidative coupling activity of hierarchical porous Fe–N₄–O₁ single-atom catalysts: oxygen atom-mediated dual reaction pathway

Abstract: Heteroatom doping is an efficacious strategy for electronic structure modulation and intrinsic activity adjustment, but the mechanisms accounting for activity enhancement remains controversial. Herein, a controllably self–assembly strategy is applied...

Cited by 7 publications

References 49 publications

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Macroporous Carbon-Supported Fe-Based Catalysts for the Solvent-Free Oxidative Coupling of Benzylamine

Wastewater flocculation substrate derived three-dimensional ordered macroporous Co single-atom catalyst for singlet oxygen-dominated peroxymonosulfate activation

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Unraveling the amine oxidative coupling activity of hierarchical porous Fe–N4–O1 single-atom catalysts: oxygen atom-mediated dual reaction pathway

Abstract: Heteroatom doping is an efficacious strategy for electronic structure modulation and intrinsic activity adjustment, but the mechanisms accounting for activity enhancement remains controversial. Herein, a controllably self–assembly strategy is applied...

Cited by 7 publications

References 49 publications

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Optimization of bandgap reduction in 2-dimensional GO nanosheets and nanocomposites of GO/iron-oxide for electronic device applications

Macroporous Carbon-Supported Fe-Based Catalysts for the Solvent-Free Oxidative Coupling of Benzylamine

Wastewater flocculation substrate derived three-dimensional ordered macroporous Co single-atom catalyst for singlet oxygen-dominated peroxymonosulfate activation

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Unraveling the amine oxidative coupling activity of hierarchical porous Fe–N₄–O₁ single-atom catalysts: oxygen atom-mediated dual reaction pathway