Chemical trapping of gaseous H 2 S at high and low partial pressures by an iron complex immobilized inside the montmorillonite interlayer

Malferrari, Daniele; Castellini, Elena; Bernini, Fabrizio; Rubio, Aida Serrano; Castro, Germán R.; Sainz‐Díaz, C. Ignacio; Caleffi, Matteo; Brigatti, Maria Franca; Borsari, Marco

doi:10.1016/j.micromeso.2018.01.017

Cited by 30 publications

(31 citation statements)

References 53 publications

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“…This hybrid material was proved to efficiently trap sulfur-bearing gas phases such as thiols and H 2 S, even at extremely low concentration, with a relevant environmental benefit. In both the cases, the immobilization mechanism occurs through a multistep process involving first a redox reaction and then the covalent binding of the R-SH or H 2 S molecule (Bernini et al, 2017;Malferrari et al, 2018). In addition, Mt-Fe 3+ Phen was recently used also to successfully entrap gaseous naphthalene and chloro-naphthalene (Castellini et al, 2019a).…”

Section: Introductionmentioning

confidence: 99%

A new material based on montmorillonite and Cu(II)-phenanthroline complex for effective capture of ammonia from gas phase

Castellini

Malferrari

Bernini

et al. 2020

Applied Clay Science

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The intercalation of [Cu(Phen)(H 2 O) 2 ] 2+ (CuPhen) in montmorillonite (Mt) produces a stable hybrid material that is very efficient in removing NH 3 from gas phase even at extremely low pressures.The process was studied by elemental analysis, X-ray powder diffraction, thermal analysis coupled with evolved gas mass spectrometry and DR UV-Vis, NMR and X-ray absorption spectroscopy. The adsorption of CuPhen on Mt consists of two consecutive steps. During the first one, CuPhen intercalates alone into Mt through a cation exchange process, afterwards CuPhen and SO 4 2− ions entry jointly into the mineral interlayer. The two-steps adsorption process is described by a VI-type isotherm, successfully fitted by two independent Frumkin isotherms. NH 3 trapping is long-lasting, easy, fast even at extremely low gas pressure and reversible under mild conditions. Mt containing CuPhen always results well performant in removing ammonia from gas phase, but an appreciably higher adsorption capacity of NH 3 is obtained when SO 4 2− ion is absent from the interlayer. This hybrid montmorillonite is thus a promising material to be used in industrial or environmental contexts, as an efficient air-cleaner.

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Section: Introductionmentioning

confidence: 99%

A new material based on montmorillonite and Cu(II)-phenanthroline complex for effective capture of ammonia from gas phase

Castellini

Malferrari

Bernini

et al. 2020

Applied Clay Science

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“…Mt-CuPhen captures a great amount of sulfur (up to 1.15 S moles/100 g Mt-CuPhen after 3 months of exposure) and its immobilization ability lasts for a very long time. The H2S capture proceeds without reaching completion, following a pathway that differs from that reported for Mt intercalated with the µ-oxo binuclear Fe(III)-phenanthroline 1:1 complex ([(H2O)3PhenFe-O-FePhen(H2O)3] 4+ , FePhen hereafter) [14]. For the latter, the H2S removal process occurs into two distinct steps: the former, lasting for about 20 h, is fast in the first 4 hours and then slows down, while the latter is completed within about 110 h. Overall, the process lasts 110 h; eventually the exhaust material must be regenerated by a thermal treatment at 295 °C for reuse.…”

Section: H2s Capture By Mt-cuphenmentioning

confidence: 78%

“…The larger maximum amount of S captured by Mt-CuPhen compared to Mt-FePhen (up to 1.15 moles (36.8 g) of S/100g vs. 0.12 moles (3.8 g) of S/100 g, respectively) and the longer uptime of the material indicate a radical change in the entrapping mechanism [14].…”

Section: H2s Capture By Mt-cuphenmentioning

confidence: 95%

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Interlayer-Confined Cu(II) Complex as an Efficient and Long-Lasting Catalyst for Oxidation of H2S on Montmorillonite

et al. 2020

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Removal of highly toxic H2S for pollution control and operational safety is a pressing need. For this purpose, a montmorillonite intercalated with Cu(II)-phenanthroline complex [Cu[(Phen)(H2O)2]2+ (Mt-CuPhen) was prepared to capture gaseous H2S under mild conditions. This hybrid material was simple to obtain and demonstrated an outstanding ability to entrap H2S at room temperature, retaining high efficiency for a very long time (up to 36.8 g of S/100 g Mt-CuPhen after 3 months of exposure). Sorbent and H2S uptake were investigated by elemental analysis, X-ray powder diffraction measurements, diffuse reflectance (DR) UV–Vis and infrared spectroscopy, thermal analysis and evolved gas mass spectrometry, scanning electron microscopy equipped with energy-dispersive X-ray spectrometer, and X-ray absorption spectroscopy. The H2S capture was studied over time and a mechanism of action was proposed. The entrapping involves a catalytic mechanism in which [Cu[(Phen)(H2O)2]2+ acts as catalyst for H2S oxidation to S0 by atmospheric oxygen. The low cost and the long-lasting performance for H2S removal render Mt-CuPhen an extremely appealing trap for H2S removal and a promising material for many technological applications.

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“…-phenanthroline complex, both on external surfaces and in the interlayer, assumes a bi-dimensional disposition. Montmorillonite treated with Fe 3+ phenanthroline can be used for the removal of sulfur containing phases from waste gasses [22,23], similarly to synthetic phases commonly used for the same purpose [24]. In sepiolite, hosted molecules, such as indigo, are expected to interact with water located inside structural channels due to the absence of layer charge and the needle-like morphology of the mineral, thus defining a linear rather than a bi-dimensional distribution [10,25].…”

Section: +mentioning

confidence: 99%

Structural properties of adsorbent phyllosilicates rule the entrapping ability of intercalated iron-phenanthroline complex towards thiols

Castellini

Malferrari

Bernini

et al. 2019

Microporous and Mesoporous Materials

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The interaction of volatile organic sulfur derivatives, such as 1-heptanethiol (C 7 H 16 S), with clay minerals treated with a μ-oxo Fe 3+-phenanthroline 1:1 complex results strongly affected by crystal chemical properties of pristine mineral phases. In particular, two sepiolite clays with different structural features demonstrated significantly different ability to immobilize the Fe 3+-phenanthroline complex at two pH values (pH = 5.4 and pH = 2.3). The most effective binding was obtained with sepiolite with higher structural disorder at pH 5.4. Accordingly, the resulting hybrid material showed also the greatest efficiency in removal of thiol in gas phase. A direct correlation can be established between the adsorption of the Fe 3+-phenanthroline complex and the gas binding process at room temperature. In fact, 1-heptanethiol entrapping occurs via redox reactions between Fe 3+ and a first thiol molecule to give the reduced Fe 2+-phenanthroline complex and disulfide, followed by the binding of further thiols to the reduced metal centre. The extremely high amount of thiol immobilized by the hybrid material also suggests the co-presence of a catalytic mechanism that guarantees the reoxidation of Fe +2 to Fe +3 and the restoration of redox reactions with thiol. Investigation and conclusions were supported by the several experimental techniques: elemental analysis, X-ray powder diffraction analyses, UV-Vis measurements, FT-IR and NMR spectroscopies, thermogravimetric analyses.

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Chemical trapping of gaseous H 2 S at high and low partial pressures by an iron complex immobilized inside the montmorillonite interlayer

Cited by 30 publications

References 53 publications

A new material based on montmorillonite and Cu(II)-phenanthroline complex for effective capture of ammonia from gas phase

A new material based on montmorillonite and Cu(II)-phenanthroline complex for effective capture of ammonia from gas phase

Interlayer-Confined Cu(II) Complex as an Efficient and Long-Lasting Catalyst for Oxidation of H2S on Montmorillonite

Structural properties of adsorbent phyllosilicates rule the entrapping ability of intercalated iron-phenanthroline complex towards thiols

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