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Reductive Degradation of CCl4 by Sulfidized Fe and Pd-Fe Nanoparticles: Kinetics, Longevity, and Morphology Aspects.

ABSTRACT: In this study a systematic comparison in morphology, long-term degradation, regeneration and reuse were conducted between palladized and sulfidized nanoscale zero-valent iron (Pd-Fe and S-Fe). Pd-Fe and S-Fe were prepared, after the synthesis of precursor Fe0 nanoparticles (spherical, ~35 nm radius) for carbon tetrachloride (CTC) treatment. With HAADF-TEM-EDS characterization, dispersive Pd islets were found on the Fe core of Pd-Fe. However, the Fe core was covered by the FeSx shell of S-Fe (FeS/FeS2 = 0.47). With an excessive Pd dose (10 mol%), the Pd-Fe were dramatically deformed to dendritic structures which significantly decreased reactivity. For CTC degradation, Pd-Fe (0.3 atomic% Pd) increased the degradation rate by 20-fold (ksa= 0.580 Lm-2min-1) while S-Fe presented a greater life time. The major intermediate chloroform (CF) was further degraded and less than 5% CF was observed after 24 h using Pd-Fe or S-Fe while above 50% CF remained using Fe. During aging, the Fe core was converted to FeOOH and Fe3O4/γ-Fe2O3. The restoration of Fe0 was achieved using NaBH4, which regenerated Fe and Pd-Fe. However, the formed FeSx shell on S-Fe was disappeared. The results suggest that S-Fe extends longevity of Fe, but the loss of FeSx after aging makes S-Fe eventually perform like Fe in terms of CTC degradation.

SUBMITTER: Wan H

PROVIDER: S-EPMC7654737 | biostudies-literature | 2020 Aug

REPOSITORIES: biostudies-literature

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Reductive Degradation of CCl4 by Sulfidized Fe and Pd-Fe Nanoparticles: Kinetics, Longevity, and Morphology Aspects.

Wan Hongyi H Islam Mohammad Saiful MS Qian Dali D Ormsbee Lindell L Bhattacharyya Dibakar D

Chemical engineering journal (Lausanne, Switzerland : 1996) 20200408

In this study a systematic comparison in morphology, long-term degradation, regeneration and reuse were conducted between palladized and sulfidized nanoscale zero-valent iron (Pd-Fe and S-Fe). Pd-Fe and S-Fe were prepared, after the synthesis of precursor Fe0 nanoparticles (spherical, ~35 nm radius) for carbon tetrachloride (CTC) treatment. With HAADF-TEM-EDS characterization, dispersive Pd islets were found on the Fe core of Pd-Fe. However, the Fe core was covered by the FeSx</s ...[more]

PMID: 33184558

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Project description:Precisely locating extra-framework cations in anionic metal-organic framework compounds remains a long-standing, yet crucial, challenge for elucidating structure-performance relationships in functional materials. Single-crystal X-ray diffraction is one of the most powerful approaches for this task, but single crystals of frameworks often degrade when subjected to post-synthetic metalation or reduction. Here, we demonstrate the growth of sizable single crystals of the robust metal-organic framework Fe2(bdp)3 (bdp2- = benzene-1,4-dipyrazolate) and employ single-crystal-to-single-crystal chemical reductions to access the solvated framework materials A2Fe2(bdp)3·yTHF (A = Li+, Na+, K+). X-ray diffraction analysis of the sodium and potassium congeners reveals that the cations are located near the center of the triangular framework channels and are stabilized by weak cation-π interactions with the framework ligands. Freeze-drying with benzene enables isolation of activated single crystals of Na0.5Fe2(bdp)3 and Li2Fe2(bdp)3 and the first structural characterization of activated metal-organic frameworks wherein extra-framework alkali metal cations are also structurally located. Comparison of the solvated and activated sodium-containing structures reveals that the cation positions differ in the two materials, likely due to cation migration that occurs upon solvent removal to maximize stabilizing cation-π interactions. Hydrogen adsorption data indicate that these cation-framework interactions are sufficient to diminish the effective cationic charge, leading to little or no enhancement in gas uptake relative to Fe2(bdp)3. In contrast, Mg0.85Fe2(bdp)3 exhibits enhanced H2 affinity and capacity over the non-reduced parent material. This observation shows that increasing the charge density of the pore-residing cation serves to compensate for charge dampening effects resulting from cation-framework interactions and thereby promotes stronger cation-H2 interactions.

Dataset Information

Reductive Degradation of CCl4 by Sulfidized Fe and Pd-Fe Nanoparticles: Kinetics, Longevity, and Morphology Aspects.

Publications

Reductive Degradation of CCl<sub>4</sub> by Sulfidized Fe and Pd-Fe Nanoparticles: Kinetics, Longevity, and Morphology Aspects.

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