On the mechanism of air nitrogen fixation on activated carbon surface in water

Пичугина, Д. А.; Ibragimova, R. I.; Emel’yanova, N. S.; Koryagina, N. L.; Shestakov, A. F.; Vorob'ev-Desyatovskii, N. V.

doi:10.1134/s1070363208040087

Cited by 6 publications

(10 citation statements)

References 45 publications

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“…30 Further, consumed O 2 may lead to formation of ROS on the surface of AC which may participate in fixation of atmospheric nitrogen in the carbon matrix. 51 Dissolved oxygen uptake experiments were conducted as described in the Materials and Methods section. Among the 3 carbons tested in this study, AqC consumed the most DO (4.73 mg/L), followed by PSC (4.29 mg/L), and last F400 (2.09 mg/L).…”

Section: ' Results and Discussionmentioning

confidence: 99%

N-Nitrosamines Formation from Secondary Amines by Nitrogen Fixation on the Surface of Activated Carbon

Padhye

Hertzberg

Yushin

et al. 2011

Environ. Sci. Technol.

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Our previous study demonstrated that many commercial activated carbon (AC) particles may catalyze transformation of secondary amines to yield trace levels of N-nitrosamines under ambient aerobic conditions. Because of the widespread usage of AC materials in numerous analytical and environmental applications, it is imperative to understand the reaction mechanism responsible for formation of nitrosamine on the surface of ACs to minimize their occurrence in water treatment systems and during analytical methods employing ACs. The study results show that the AC-catalyzed nitrosamine formation requires both atmospheric oxygen and nitrogen. AC's surface reactive sites react with molecular oxygen to form reactive oxygen species (ROS), which facilitate fixation of molecular nitrogen on the carbon surfaces to generate reactive nitrogen species (RNS) likely nitrous oxide and hydroxylamine that can react with adsorbed amines to form nitrosamines. AC's properties play a crucial role as more nitrosamine formation is associated with carbon surfaces with higher surface area, more surface defects, reduced surface properties, higher O(2) uptake capacity, and higher carbonyl group content. This study is a first of its kind on the nitrosamine formation mechanism involving nitrogen fixation on AC surfaces, and the information will be useful for minimization of nitrosamines in AC-based processes.

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Section: ' Results and Discussionmentioning

confidence: 99%

N-Nitrosamines Formation from Secondary Amines by Nitrogen Fixation on the Surface of Activated Carbon

Padhye

Hertzberg

Yushin

et al. 2011

Environ. Sci. Technol.

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“…The ability of AC surfaces to react with oxygen to generate ROS has been well recognized and is related to surface defects (66). ROS generated or carbene centers created by reactions on carbon surfaces could be responsible for nitrogen fixation by reacting with dissolved N 2 to form RNS like N 2 O or diazo intermediates (67,68). Reductive transformation promoted by AC surfaces may convert N 2 O to yield NH-containing species such as Н 2 N 2 O, NН 2 OH and ammonia (69).…”

Section: Reaction Mechanismsmentioning

confidence: 99%

Catalytic Impact of Activated Carbon on the Formation of Nitrosamines from Different Amine Precursors

Huang

Padhye

Wang

2013

ACS Symposium Series

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N-nitrosamines are emerging carcinogenic contaminants and can be generated from transformation of amines. Activated carbon (AC) materials with micro-and nano-porous structures are commonly used for extraction of nitrosamines in water, and for removal of micropollutants in water and wastewater treatment. Recent research demonstrated that AC materials may catalyze transformation of amine precursors to yield nitrosamines under environmentally relevant conditions. AC catalyzes the formation of nitrosamine primarily via two different types of reactions: (I) catalyzing nitrosation of amine with nitrite or nitrate to yield nitrosamine, and (II) catalyzing oxidation of amine in the presence of molecular oxygen and nitrogen to generate nitrosamine. The AC-catalyzed nitrosamine formation is highly influenced by AC's properties, amine precursors' structures and reaction conditions. Considering the widespread usage of AC in environmental and industrial applications, a better understanding of the catalytic impact of AC on nitrosamine formation is critical to minimize undesirable nitrosamine formation where co-existence of AC and amine precursors is encountered.

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“…The simulation of the activated carbon structure by quantum mechanical methods shows that defects in the structure of graphenes can be carbene-like atoms, which are preferably in a triplet state in particles with a considerable number of condensed aromatic rings [52]. Triplet carbenes can be rather stable also in the case of delocalization of unpaired electrons over an aromatic net, they are capable to form polycarbenes possessing paramagnetic properties, and to capture О 2 molecules [53].…”

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confidence: 99%

“…The presence of oxygen dissolved in water favors the appearance of oxidative properties of activated carbons on the adsorption of complexes of transition elements in rather low oxidation states. As a result of the reaction of О 2 molecules with carbene-like centers of activated carbon, reactive species including OH · radicals appear in solution [52,54]. The treatment of activated carbons by oxidizing agents (nitric acid, chlorine, or bromine in aqueous suspension) results in the complete loss of their adsorption properties with respect to [Au(CN) 2 ] -ions in aqueous solutions [45].…”

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Study of sorption of platinum and palladium cyanometallate complexes as the key to understanding the mechanism of binding the [Au(CN)2]− anion with carbon adsorbents

Vorob'ev-Desyatovskii¹,

Kubyshkin²,

Ibragimova³

et al. 2012

Russ J Gen Chem

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Goldcarb WSC-207C GR activated carbons with platinum and palladium complexes adsorbed from aqueous solutions of K 2 [Pt(CN) 4 ], K 2 [Pt(CN) 6 ], and K 2 [Pd(CN) 4 ] were studied by the methods of X-ray photoelectron spectroscopy and IR spectroscopy with Fourier transformation, and also by MALDI massspectrometry. Platinum and palladium cyanide complexes are not reduced onto surface of active charcoal while adsorption. A certain part of the [Pd(CN) 4 ] 2-and [Pt(CN) 4 ] 2-anions directly bound to active centers on the activated carbon is oxidized more deeply and functions as particles-anchors, forming oligomers resembling Krogmann salt. A correspondence between the structure of the complex cyanometallate ion and a mode of its binding with active carbon is found. The adsorption of complex species with a linear structure or a square planar structure is defined by a possibility of the formation of donor-acceptor and metallophilic bonds. The mode of the anion [Au(CN) 2 ] -binding with the surface of active carbon was considered.In last 30 years a stable interest arose to the application of activated carbons in hydrometallurgical processes. First of all, it is connected with industrial usage of coals as main adsorbents for extraction of gold(I) from cyanide solutions and pulps. In spite of it the reason of a selective sorption of gold(I) cyanide complex on carbon adsorbents is not yet elucidated at present. Unlike the corresponding complexes of gold, adsorption of platinum and palladium cyanide complexes is by no means studied though the knowledge of specificity of their behavior in relation to carbon adsorbents can present both theoretical and practical interest. This interest is connected, firstly, with the study of mechanisms of binding complexes of noble metals with active carbons and also with the search for methods improving kinetic and capacity properties of carbon adsorbents and increasing their selectivity. Results of such studies promote the improvement of the process of mining and refining platinum metals and gold.Depending on the nature of a central atom and its ligand environment, and also on the composition of a solution and conditions, in which transition metal complexes contact carbon adsorbents, partial or complete reduction of a metal center and (or) chemisorption, which is accompanied by a change in its oxidation state, can occur at the adsorption. To predict a possible result of the interaction between activated carbon and complexes of noble metals, it was suggested to use a comparison of working and stationary potentials of coal in a solution with appropriate redox potentials of complex compounds [1]. The nature of adsorbate at the adsorption of transition metal complex compounds on activated carbons depends on several factors. The composition

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On the mechanism of air nitrogen fixation on activated carbon surface in water

Cited by 6 publications

References 45 publications

N-Nitrosamines Formation from Secondary Amines by Nitrogen Fixation on the Surface of Activated Carbon

N-Nitrosamines Formation from Secondary Amines by Nitrogen Fixation on the Surface of Activated Carbon

Catalytic Impact of Activated Carbon on the Formation of Nitrosamines from Different Amine Precursors

Study of sorption of platinum and palladium cyanometallate complexes as the key to understanding the mechanism of binding the [Au(CN)2]− anion with carbon adsorbents

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