Моно- та біметальні комплекси, закріплені на природному трепелі, у реакції низькотемпературного окиснення діоксиду сульфуру киснем повітря
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Файли
Дата
2019
Науковий керівник
Укладач
Редактор
Назва журналу
ISSN
2304-0947
E-ISSN
2414-5963
Назва тому
Видавець
Одеський національний університет імені І. І. Мечникова
Анотація
Вивчена кінетика окиснення діоксиду сульфуру в присутності закріплених на природному трепелі каталітичних композицій на основі d-металів. Показано, що монометальні композиції проявляють різний час захисної дії та час досягнення напівперетворення SO2, тривалість яких залежить від природи та вмісту МiLj/П-Тр(К-ІІ) (М = Cu2+, Cо2+, Fe3+, Pd2+; L = Cl-, NO−3, SO2−4). Показано, що для біметальних композицій CuCl2 –МCln/П-Тр(К-ІІ) (М = Fe3+, Со2+, Pd2+; n = 2 або 3) спостерігаються синергетичний ефект.
Изучена кинетика окисления диоксида серы в присутствии закрепленных на природном трепеле каталитических композиций на основе d-металлов. Показано, что монометальные композиции демонстрируют разное время защитного действия и время достижении полупревращения SO 2, продолжительность которых зависят от природы и содержания МiLj/П-Тр(К-ІІ) (М = Cu2+, Cо2+, Fe3+, Pd2+; L = Cl-, NO−3, SO2−4). Показано, что для биметальных композиций CuCl 2-МCln/П-Тр(К-ІІ) (М = Fe3+, Со2+, Pd2+; n = 2 или 3) наблюдаются синергетический эффект.
Sulfur dioxide is the most widespread environmental contaminant. For abatement of its concentrations in air, various chemosorbents and catalysts are used. Among the catalysts, liquid-phase metal complexes, metals and metal oxides (the latter are active only at high temperatures) are well studied. However, metal complexes anchored on different supports as catalysts are of interest now because of simple techniques of their preparing and the possibility to vary their activity over a wide range by changing the nature of d metal salts, supports and other components contained in their compositions. In the work, natural tripoli from Konoplianskiy deposit (Kirovohrads’ka Oblast’), N-Tr(K-II), is used as both a sulfur dioxide adsorbent and a support for d metal compounds. It has been found that this natural tripoli is not a true mineral and has a complicated composition, a developed mesoporous structure with pore sizes from 3.0 to 9.7 nm, and the high pH value (8.15) of its suspension. We investigated the kinetics of sulfur dioxide oxidation over some natural tripoli anchored catalytic compositions based on d metal compounds. It has been found that amounts of SO2 reacted, Qexp , at any MCln (n = 2 or 3) content are significantly larger than the amounts of SO2 adsorbed by N-Tr(K-II). That gives evidence of the direct participation of monometallic compositions based on d metal chlorides in the reaction of SO2 oxidation with oxygen. Qexp depends on the nature of d metal and contents of MCln (n = 2 or 3). For МiLj/N-Tr(K-II) compositions (М = Cu2+, Со2+, Pd2+, Fe3+; L = Cl-, NO−3 , SO2−4) the nature of anions also signifies. First, the concentrations of natural tripoli anchored d metal ions have been found being able to cause a synergetic action of these components in Cu(ІІ)-Fe(ІІІ)/N-Tr(K-II) and Cu(ІІ)-Pd(ІІ)/N-Tr(K-II) bimetallic compositions. Thus, monometallic, МiLj/N-Tr(K-II) (М = Cu2+, Со2+, Pd 2+, Fe3+; L = Cl-, NO−3 , SO2−4), and bimetallic, CuCl2-MCln/N-Tr(K-II) (М = Fe3+, Со2+, Pd2+; n = 2 or 3), compositions have been obtained whose activity in the reaction of sulfur dioxide oxidation with air oxygen depends on the nature of metal ions and ligands. It has been found that the synergetic effect is characteristic of СuCl2-PdCl2/N-Tr(K-II) and СuCl2-FeCl3/N-Tr(K-II) compositions and, on the contrary, Co2+ inhibits the activating action of СuCl2 in СuCl2-CoCl2/N-Tr(K-II) composition.
Изучена кинетика окисления диоксида серы в присутствии закрепленных на природном трепеле каталитических композиций на основе d-металлов. Показано, что монометальные композиции демонстрируют разное время защитного действия и время достижении полупревращения SO 2, продолжительность которых зависят от природы и содержания МiLj/П-Тр(К-ІІ) (М = Cu2+, Cо2+, Fe3+, Pd2+; L = Cl-, NO−3, SO2−4). Показано, что для биметальных композиций CuCl 2-МCln/П-Тр(К-ІІ) (М = Fe3+, Со2+, Pd2+; n = 2 или 3) наблюдаются синергетический эффект.
Sulfur dioxide is the most widespread environmental contaminant. For abatement of its concentrations in air, various chemosorbents and catalysts are used. Among the catalysts, liquid-phase metal complexes, metals and metal oxides (the latter are active only at high temperatures) are well studied. However, metal complexes anchored on different supports as catalysts are of interest now because of simple techniques of their preparing and the possibility to vary their activity over a wide range by changing the nature of d metal salts, supports and other components contained in their compositions. In the work, natural tripoli from Konoplianskiy deposit (Kirovohrads’ka Oblast’), N-Tr(K-II), is used as both a sulfur dioxide adsorbent and a support for d metal compounds. It has been found that this natural tripoli is not a true mineral and has a complicated composition, a developed mesoporous structure with pore sizes from 3.0 to 9.7 nm, and the high pH value (8.15) of its suspension. We investigated the kinetics of sulfur dioxide oxidation over some natural tripoli anchored catalytic compositions based on d metal compounds. It has been found that amounts of SO2 reacted, Qexp , at any MCln (n = 2 or 3) content are significantly larger than the amounts of SO2 adsorbed by N-Tr(K-II). That gives evidence of the direct participation of monometallic compositions based on d metal chlorides in the reaction of SO2 oxidation with oxygen. Qexp depends on the nature of d metal and contents of MCln (n = 2 or 3). For МiLj/N-Tr(K-II) compositions (М = Cu2+, Со2+, Pd2+, Fe3+; L = Cl-, NO−3 , SO2−4) the nature of anions also signifies. First, the concentrations of natural tripoli anchored d metal ions have been found being able to cause a synergetic action of these components in Cu(ІІ)-Fe(ІІІ)/N-Tr(K-II) and Cu(ІІ)-Pd(ІІ)/N-Tr(K-II) bimetallic compositions. Thus, monometallic, МiLj/N-Tr(K-II) (М = Cu2+, Со2+, Pd 2+, Fe3+; L = Cl-, NO−3 , SO2−4), and bimetallic, CuCl2-MCln/N-Tr(K-II) (М = Fe3+, Со2+, Pd2+; n = 2 or 3), compositions have been obtained whose activity in the reaction of sulfur dioxide oxidation with air oxygen depends on the nature of metal ions and ligands. It has been found that the synergetic effect is characteristic of СuCl2-PdCl2/N-Tr(K-II) and СuCl2-FeCl3/N-Tr(K-II) compositions and, on the contrary, Co2+ inhibits the activating action of СuCl2 in СuCl2-CoCl2/N-Tr(K-II) composition.
Опис
Ключові слова
природний трепел, закріплені 3d‑метали, діоксид сульфуру, окиснення, кисень повітря, природный трепел, закрепленные d‑металлы, закрепленные d‑металлы, диоксид серы, диоксид серы, окисление, кислород воздуха, natural tripoli, anchored d metals, sulfur dioxide, oxidation, air oxygen
Бібліографічний опис
Кіосе Т. О. Моно- та біметальні комплекси, закріплені на природному трепелі, у реакції низькотемпературного окиснення діоксиду сульфуру киснем повітря / Т. О. Кіосе, Т. Л. Ракитська, А. П. Назар, Л. А. Раскола // Вісник Одеського національного університету. Хімія. – 2019. – Т. 24, вип. 4(72). – С. 6–17.
ORCID:
УДК
546.98:562:544.723.2-3:549.6