Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation Herein, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 182 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe Mossbauer spectroscopy The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions

https://par.nsf.gov/servlets/purl/10092377

High-Density Ultra-small Clusters and Single-Atom Fe Sites Embedded in Graphitic Carbon Nitride (g-C3N4) for Highly Efficient Catalytic Advanced Oxidation Processes

Benchmarking recent advances and innovative technology approaches of Fenton, photo-Fenton, electro-Fenton, and related processes: A review on the relevance of phenol as model molecule

Interaction with electron donor and acceptor molecules such as aniline and nitrobenzene brings about marked changes in the Raman spectrum and the electronic structure of graphene, prepared by the exfoliation of graphitic oxide.

Changes in the electronic structure and properties of graphene induced by molecular charge-transfer

The maximization of the numbers of exposed active sites in supported metal catalysts is important to achieve high reaction activity. In this work, a simple strategy for anchoring single atom Fe on SBA-15 to expose utmost Fe active sites was proposed. Iron salts were introduced into the as-made SBA-15 containing the template and calcined for simultaneous decomposition of the iron precursor and the template, resulting in single atom Fe sites in the nanopores of SBA-15 catalysts (SAFe-SBA). X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (UV-vis DRS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and extended X-ray absorption fine structure (EXAFS) imply the presence of single atom Fe sites. Furthermore, EXAFS analysis suggests the structure of one Fe center with four O atoms, and density functional theory calculations (DFT) simulate this structure. The catalytic performances of SAFe-SBA were evaluated in Fenton-like catalytic oxidation of p-hydroxybenzoic acid (HBA) and phenol. It was found that the single atom SAFe-SBA catalysts displayed superior catalytic activity to aggregated iron sites (AGFe-SBA) in both HBA and phenol degradation, demonstrating the advantage of SAFe-SBA in catalysis.

Boosting Fenton-Like Reactions via Single Atom Fe Catalysis

Enhanced visible light activity on direct contact Z-scheme g-C3N4-TiO2 photocatalyst

Iron(II) phthalocyanine (FePc) is immobilized on graphene sheets to form a graphene(G)/iron(II) phthalocyanine hybrid (G/FePc) by the π–π stacking method. The resultant hybrids are characterized by UV–vis absorption spectra, FTIR, Raman spectra, BET, TEM, SEM and XRD. The result suggests that the interaction between graphene and FePc follows a donor-acceptor mode and the loading of FePc on graphene sheets not only facilitates the dispersion of FePc on graphene but also promotes the exfoliation of the graphene sheets. These samples are tested for photocatalytic degradation of phenol under visible light irradiation (λ ≥ 420 nm). And the photocatalytic activity of graphene, which is not presented when graphene individually acts on phenol, is greatly enhanced because of the π–π stacking interaction when FePc loaded on graphene. The G/FePc hybrid containing 25 wt.% FePc (G/FePc-0.25) exhibits the best photoactivity among the different loading content of FePc, whose degradation rate for phenol achieves 77.1% in the presence of H2O2 under visible light irradiation for 3 h.

Iron phthalocyanine-graphene donor-acceptor hybrids for visible-light-assisted degradation of phenol in the presence of H2O2

Nanotubular titanic acid (denoted as NTA) was calcined in air to generate TiO2 containing a large amount of single-electron-trapped oxygen vacancy (abridged as SETOV and denoted as V0 ) Resultant V0 self-modified (or self-doped) TiO2 (denoted as V0 –TiO2), visible light responsive but photocatalytically inactive under visible-light irradiation, was grafted with Fe(III) nanoclusters via an impregnation method to afford Fe(III)–V0 –TiO2 possessing visible-light phtocatalytic activity The photocatalytic performance of as-prepared Fe(III)–V0 –TiO2 photocatalysts was evaluated and compared with that of N-doped TiO2, and the experimental results were further discussed based on density functional theory calculations Results reveal that grafting Fe(III) leads to nearly no changes in the crystalline structure as well as morphology and grain size of V0 –TiO2 but results in good visible-light photocatalytic performance for the photodegradation of gaseous propylene under visible-light irradiation This is because the grafted Fe(III) nanoclusters act as efficient electron trapping centers to significantly enhance the electron transfer from oxygen vacancy state and the conduction band of TiO2 to the adsorbed oxygen, thereby inducing the rapid separation of the photogenerated electrons and holes Besides, the photocatalytic activity of Fe(III)–V0 –TiO2 photocatalysts is dependent on the dosage of grafted Fe(III), and it is critical to maintain a good matching between the energy level of V0 and surface-grafted Fe(III) cocatalyst so as to facilitate fast and efficient charge transfer Thanks to the good availability, low cost, and nontoxicity, Fe as the cocatalyst could find promising applications in the development of high-performance photocatalysts

Endowing single-electron-trapped oxygen vacancy self-modified titanium dioxide with visible-light photocatalytic activity by grafting Fe(III) nanocluster

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Iron phthalocyanine-graphene donor-acceptor hybrids for visible-light-assisted degradation of phenol in the presence of H2O2

Endowing single-electron-trapped oxygen vacancy self-modified titanium dioxide with visible-light photocatalytic activity by grafting Fe(III) nanocluster