ДИФЕРЕНЦІЙНО-ТЕРМІЧНИЙ АНАЛІЗ СКЛАДНОЇ КАТАЛІТИЧНОЇ СИСТЕМИ ТИПУ хCrРО4уNi3(РО4)2

Автор(и)

  • N. P. Golub ДВНЗ "Ужгородський національний університет", Ukraine https://orcid.org/0000-0002-4084-4553
  • E. O. Golub ДВНЗ "Ужгородський національний університет", Ukraine
  • A. A. Kozma ДВНЗ "Ужгородський національний університет", Ukraine https://orcid.org/0000-0003-0820-9979
  • N. M. Foros ДВНЗ "Ужгородський національний університет", Ukraine
  • Yu. Yu. Kish ДВНЗ "Ужгородський національний університет", Ukraine
  • V. I. Gomonay ДВНЗ "Ужгородський національний університет", Ukraine

DOI:

https://doi.org/10.24144/2414-0260.2018.2.57-64

Ключові слова:

catalysis, catalyst, heterogeneous oxidation, partial oxidation of n-alkanes, C1-C4– hydrocarbons

Анотація

Individual phosphates of cobalt and nickel and seven new complex oxide catalytic systems based on chromium phosphate were synthesized by modifying it with ions of Nі2+ type xCrPO4´yNi3(PO4)2 with different content of both phosphates having acidic surface properties. The modern methods of analysis have studied the composition, structure and some physical and chemical parameters of all synthesized samples. The influence of the synthesis conditions on the nature of the formation of their structure and the corresponding physico-chemical and catalytic properties was studied with the help of differential-thermal analysis. It is established that for synthesized binary samples, various forms of water that are part of their composition are characteristic: adsorbed, structural, crystallization, constitutional, etc. Allocating them from the structure of catalysts in the process of heat treatment is accompanied by various effects and corresponding endo-effects. In this case, the kinetics of water thermosorption from the surface and from the volume of internal pores depends on the nature of the interaction between the molecules in the adsorption layers and water molecules on the surface. In the allocation of adsorbed water from phosphate catalysts, the change in the type of anion is not observed. However, the elimination of crystallization, and especially constitutional water, is accompanied by a rupture of chemical bonds, intense diffusion of water vapor from the lattice and rearrangement of phosphate anion. All synthesized phosphates have different curves of DTA, which are different from individual phosphates of cromium and nickel, and with each other. After calcining at 700°C and at higher temperatures, all synthesized complex catalytic phosphate systems exist in the form of anhydrous salts, which is confirmed by the data of X-ray diffraction, IR spectroscopic and chemical analyzes. Thus, the results obtained are in good agreement with [24, 25] and show that, as it was predicted, when changing the composition of the chromium-nickel-phosphate system, it was possible to obtain catalysts, on the surface of which formed certain chemical structures that could form the corresponding optimal surface complexes and detect special catalytic properties in the processes of partial oxidation of n-alkanes in valuable products.

Біографії авторів

N. P. Golub, ДВНЗ "Ужгородський національний університет"

к.х.н., доц., завідувач кафедри фізичної та колоїдної хімії

E. O. Golub, ДВНЗ "Ужгородський національний університет"

Викладач кафедри фармацевтичних дисциплін

A. A. Kozma, ДВНЗ "Ужгородський національний університет"

к.х.н., доцент кафедри фізичної та колоїдної хімії

N. M. Foros, ДВНЗ "Ужгородський національний університет"

студент

Yu. Yu. Kish, ДВНЗ "Ужгородський національний університет"

студент

V. I. Gomonay, ДВНЗ "Ужгородський національний університет"

д.х.н., проф., професор кафедри фізичної та колоїдної хімії

Посилання

Buyanov R.A. Nauchnyie osnovyi prigotovleniya i tehnologii katalizatorov. Kataliz i katalizatoryi. 1998, 151–152 (in. Russ.).

Gomonaj V.I. Fiziko-ximicheskie osnovy` podbora geterogenny`x katalizatorov parcial`nogo okisleniya n-alkanov: Avtoref. dis. dok. him. nauk: 02.00.04, IFX AN USSR. Kiev, 1990 (in Russ.).

Holub N.P. Zakonomirnosti katalitychnoho okysnennia etanu na kyslotnykh katalizatorakh: Avtoref. dis. kand. khim. nauk: 02.00.04, Kyivskyi natsionalnyi universytet im. Tarasa Shevchenka. Kyiv, 1996 (in Ukr.).

Golub N., Gomonay V., Gomonay P., Szekeresh K. Adsorpt. Sci. Technol. 1999, 17(5), 403–406.

Holub Ye.O., Holub N.P., Homonai V.I., Sekeresh K.Iu., Barenblat I.O., Kozma A.A. Doslidzhennia mekhanizmu peretvorennia etanu na deiakykh skladnykh systemakh impulsnym metodom. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 2016, 36, 60–64 (in. Ukr.).

Holub Ye.O., Holub N.P., Homonai V.I., Sekeresh K.Iu., Barenblat I.O. Doslidzhennia vplyvu vysoty sharu katalizatora na kinetyku partsialnoho okysnennia etanu na deiakykh skladnykh katalitychnykh systemakh. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 2016, 2(36), 64–67 (in. Ukr.).

Holub Ye.O., Holub N.P., Homonai V.I., Sekeresh K.Iu., Borko V.O., Barenblat I.O. Vplyv vidnovlennia poverkhni katalizatoriv na yikh katalitychni vlastyvosti v reaktsii partsialnoho okysnennia n-alkaniv. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 2015, 1(33), 58–62 (in Ukr.).

Holub Ye.O., Holub N.P., Homonai V.I., Sekeresh K.Iu., Borko V.O., Barenblat I.O. Kinetychni zakonomirnosti partsialnoho okysnennia nyzhchykh vuhlevodniv na fosfatnykh katalizatorakh. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 2015, 2(34), 75–79 (in Ukr.).

Mirkin L.I. Spravochnik po rentgenostrukturnomu analizu polikristallov. Pod red. prof. Umanskogo Ya. Moskva: Gos. izd-vo fiz.- mat. literaturyi, 1961, S. 860 (in Russ.).

Diller Ya.L. Tablitsyi mezhploskostnyih rasstoyaniy. T.2. Moskva: Nedra, 1966. S. 362 (in Russ.).

Nebola I.I. Rasshifrovka rentgenogramm poroshkov. Moskva: Metallurgiya, 1975. S. 247 (in Russ.).

Staszczuk P., Danielkiewicz T., Klinowski J. The investigations of the adsorbend layers and heterogeneous properties of the MCM-41 molecular sieve using the special thermal analysis method. IV Polish-Ukrainian Symposium “Theoretical and experimental studies of interfacial phenomena and their technological applications”. Lublin, Poland. 1999, Р.51.

Berg L.G. Vvedenie v termografiyu. Moskva: Nauka, 1969. S. 395 (in Russ.).

Berg L.G., Burmistrova N.P., Ozerova N.I., Tsurinov G.G. Prakticheskoe rukovodstvo po termografii. Kazan: Izd-vo Kazanskogo un-ta, 1967. S. 219 (in Russ.).

Nakamoto K. Infrakrasnyie spektryi neorganicheskih i koordinatsionnyih soedineniy. Moskva: Mir, 1982. S. 160 (in Russ.).

Nakamoto K. Atlas infrakrasnyih spektrov fosfatov. Ortofosfatyi. Moskva: Nauka, 1981. S. 247 (in Russ.).

Yuhnevich G.V. Infrakrasnaya spektroskopiya vodyi. Moskva: Nauka, 1973. S.209 (in Russ.).

Littl L. Infrakrasnyie spektryi adsorbirovannyih molekul. Moskva: Mir, 1969. S.35 (in Russ.).

Golodecz G.I. Geterogenno-kataliticheskie reakcii s uchastiem molekulyarnogo kisloroda. Kiev: Naukova dumka, 1977. S. 173 (in Russ.).

Holub N.P., Holub Ye.O., Barenblat I.O., Homonai V.I., Sekeresh K.Iu. Dyferentsiino-termichnyi analiz skladnoi katalitychnoi systemy typu хСо3(РО4)2•уNi3(РО4)2. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 2018, 1(39), 83–88 (in. Ukr.)

Yaglov V.N., Volkov A.I., Novikov G.I. Termicheskoe razlozhenie kristallogidrata CrPO4•6H2O. Zhurnal neorganicheskoy himii. 1977, 22, 37–40 (in Russ.).

Schegrov L.N., Pechkovskiy V.V., Eschenko L.S. Termicheskaya degidratatsiya Ni3(PO4)2•8H2O. Dokladyi Akademii nauk SSSR. 1969, 184(2), 391–394 (in Russ.).

Syichev M.M., Komlev V.G. Tverdenie zhelezo-, kobalt- i nikel-fosfatnyih tsementov. Izv. AN SSSR. Neorganicheskie materialyi. 1971, 7(9), 1612–1615 (in Russ.).

Golodets G.I. Rol kislotnyih svoystv poverhnosti v reaktsiyah geterogennogo kataliticheskogo okisleniya. Kataliz i katalizatoryi. 1980, 18, 66–75 (in Russ.).

Homonai V.I. Shliakhy partsialnoho peretvorennia С1-С4 vuhlevodniv. Nauk. visnik Uzhgorods'kogo un-tu. Serіya «Khimiya». 1997, 2, 81–86 (in. Ukr.).

##submission.downloads##

Номер

Розділ

Статті