Key role of terminal hydroxyl groups and visible light in the reactive adsorption/catalytic conversion of mustard gas surrogate on zinc (hydr)oxides

Giannakoudakis, Dimitrios A.; Arcibar‐Orozco, Javier A.; Bandosz, Teresa J.

doi:10.1016/j.apcatb.2015.02.028

Cited by 47 publications

(31 citation statements)

References 48 publications

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“…Briefly, the transient cyclic sulfonium cation formed by an intermolecular cyclization process undergoes a bimolecular elimination (E2) reaction, where a labile hydrogen transfers to a negatively charged lattice group that acts as a Lewis base. The photoactivity likely contributes to the formation of cyclic sulfonium cation promoting formation of EVS radicals . The released HCl reacts with the amines groups of GCN and GCNox.…”

Section: Figurementioning

confidence: 99%

“…The released HCl reacts with the amines groups of GCN and GCNox. An identical degradation pathway was reported for the reactive adsorption of CEES on MOF, MgO, Zr(OH) 4 and Zn(OH) 2 …”

Section: Figurementioning

confidence: 99%

“…The photoactivity likely contributes to the formation of cyclic sulfonium cation promoting formation of EVS radicals. [25,27] The released HCl reacts with the amines groups of GCN andG CNox.A ni dentical degradationp athway wasr eported for the reactive adsorption of CEES on MOF,M gO, Zr(OH) 4 and Zn(OH) 2 . [27][28][29][30] In conclusion, to analyze the effects of oxidation both texture and surface chemistry must be taken into consideration.…”

Section: Figure2ca Nd Ta Ble S5mentioning

confidence: 99%

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Mesoporous Graphitic Carbon Nitride‐Based Nanospheres as Visible‐Light Active Chemical Warfare Agents Decontaminant

et al. 2016

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Graphitic carbon nitride, GCN, was oxidized using the Hummers' method. Both initial andm odified materials were extensively characterizedb yv ariousp hysical and chemical methods. The results showed the marked changes in morphology.E ven though the shortrange layered structure was still present in the oxidized sample, spherical nanoparticles with 5-50 nm sizes made up the bulk of the material. This resultsi nt he development of porosity in the mesopore range. Incorporation of oxygen groups at the edges of carbon nitrogen layers/ units is likely responsible for the formation of nanospheres (folding due to the polar forces). This process also increased the band gap energy from 2.85 to 3.39 eV.The initial ando xidized samples were used as reactivea dsorbents of am ustard gas surrogate. The results showeda n improvement in the adsorptive performance upon oxidation. Both samples were found photoactive in visible light. The degradation to ethyl vinyl sulfide was enhanced on the oxidized sample owing to the developed porosity and chemical heterogeneity.In recent years, an ew metal-freep olymeric semiconductor with al ayered structure, graphitic carbon nitride (GCN), entered the exclusive club of 'graphitic' compounds and attracted tremendous worldwide attention because of its visible-light range band gap energy,e xcellent thermal/chemical stability and tunable electronic structure. The main difference between GCN and graphite is the switch of every other carbon atom by nitrogen in the honeycomb motif where both Ca nd Nh ave sp 2 hybridization. Even thought he insertion of electrons to the anti-bonding molecular orbitals leads to the enhancedf ormation of holes, [1] the main drawback of the rapid recombination of electron-hole pairs limits the photocatalytic activity of GCN.[2] Since the first report from Wang et al. of GCN as a' metal-free' photocatalystf or visible-light-driven H 2 production from water in 2009, [3] many studies focusedo nt he improvement of the photocatalytic performance (especially for water splitting) via the incorporation of metals, quantum dots, polymers and graphene. [3][4][5][6][7][8][9][10][11] Av ariety of chemical andp hysical modifications has been appliedt oi ncrease the conductivity, delay charge recombination, increase proton concentration and open up the band gap.[12] They include an incorporation of heteroatoms, nanosheet preparation or buildingc omposites with visible-light-active or semiconducting phases. [13][14][15] It has been recently reported that some oxidationm ethods preserve the graphite-like structure in the nanoscale range.[15-17] For both initial and modifiedG CN nanosheets variousa pplications have been reported. [14,15,18] The objective of this study is to derive an ew form of GCN on which the visible-light driven oxidation would be improved. To do it,t he well-known and often appliedt og raphite Hummers' oxidation methodw as used.[20] As ar esult, an anospherical catalyst( GCNox)w ith an enhanced photocatalytic activity for the decomposition of 2-chloroethyl e...

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Section: Figurementioning

confidence: 99%

“…The released HCl reacts with the amines groups of GCN and GCNox. An identical degradation pathway was reported for the reactive adsorption of CEES on MOF, MgO, Zr(OH) 4 and Zn(OH) 2 …”

Section: Figurementioning

confidence: 99%

Section: Figure2ca Nd Ta Ble S5mentioning

confidence: 99%

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Mesoporous Graphitic Carbon Nitride‐Based Nanospheres as Visible‐Light Active Chemical Warfare Agents Decontaminant

et al. 2016

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“…33 In addition, the photocatalytic properties of the iron oxyhydroxide and the presence of atmospheric O 2 and H 2 O on the surface of ferrihydrite 12 promote the formation of hydroxyl and superoxide radicals (reaction (6)). Its presence is due to the direct oxidation of the sulde group by oxygen groups on the surface of the iron(III) oxide (reaction (6)), therefore reducing its surface.…”

Section: Sample Namementioning

confidence: 99%

Reactive adsorption of CEES on iron oxyhydroxide/(N-)graphite oxide composites under visible light exposure

2015

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The interactions of 2-chloroethyl ethyl sulfide (CEES) with the surface of iron oxyhydroxide and its composites with graphite oxide and/or aminated graphite oxide were studied under visible light irradiation. Materials exposed to CEES were extensively characterized by FTIR-STR, UV-VIS-NIR, and TA-MS. The gaseous/vaporous reaction products were identified by GC-MS. The compounds deposited on the surface of the materials were analyzed in acetonitrile extracts by NMR and MS-MS. The FTIR results indicated the existence of alcohol groups on the surface of the exhausted samples and the involvement of OH groups in the CEES reactive adsorption. Ethyl vinyl sulfide (EVS) was the only volatile compound detected as a result of the reaction with the surface. Two adsorption sites for either CEES or EVS were identified on the adsorbent surfaces. As a result of CEES reactive adsorption Fe(III) was reduced, which indicates its crucial role in the oxidation of CEES and EVS. On the composites, the detection of disulfides as products of advanced oxidation of CEES suggests the activation of thiyl and oxygen radicals. This indicates that the incorporation of GO and GOU into iron oxyhydroxides strongly increases the oxidation potential of oxyhydroxides and induces the formation of radicals. The main promoters of CEES transformation are proposed to be OH groups and thiyl radicals.

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“…Among different metal oxides, pure or combined zinc oxide (ZnO) nanoparticles have been commonly used in pigments, cosmetics, chemical sensors, solar cells, lithium ion batteries or catalysts . ZnO is an economical, reusable, commercially available, air‐ and moisture‐stable, and environmentally benign material.…”

Section: Introductionmentioning

confidence: 99%

A practical and highly efficient synthesis of densely functionalized nicotinonitrile derivatives catalyzed by zinc oxide‐decorated superparamagnetic silica attached to graphene oxide nanocomposite

Davoodi

Dekamin

Alirezvani

2019

Applied Organom Chemis

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Zinc oxide‐decorated superparamagnetic silica attached to graphene oxide (Fe3O4/SiO2/PTS‐GO‐ZnO), as a novel nanocomposite, was designed, and its core‐shell structure was appropriately characterized by different spectroscopy or microscopy methods and thermal techniques as well as measuring of its porosity and magnetic properties. The catalytic activity of Fe3O4/SiO2/PTS‐GO‐ZnO, as a reusable heterogeneous catalyst, was investigated for efficient one‐pot multi‐component synthesis of medicinally important functionalized 2‐amino‐6‐(2‐oxo‐2H‐chromen‐3‐yl)‐4‐arylnicotinonitrile derivatives. The significant features of the present procedure are mild reaction conditions, low loading of the catalyst, high to quantitative yields of the desired products, avoiding the use of toxic heavy metals or solvents, simple isolation and purification of the products, and stability as well as reusability of the catalyst after at least six consecutive runs.

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Key role of terminal hydroxyl groups and visible light in the reactive adsorption/catalytic conversion of mustard gas surrogate on zinc (hydr)oxides

Cited by 47 publications

References 48 publications

Mesoporous Graphitic Carbon Nitride‐Based Nanospheres as Visible‐Light Active Chemical Warfare Agents Decontaminant

Mesoporous Graphitic Carbon Nitride‐Based Nanospheres as Visible‐Light Active Chemical Warfare Agents Decontaminant

Reactive adsorption of CEES on iron oxyhydroxide/(N-)graphite oxide composites under visible light exposure

A practical and highly efficient synthesis of densely functionalized nicotinonitrile derivatives catalyzed by zinc oxide‐decorated superparamagnetic silica attached to graphene oxide nanocomposite

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