Катализаторы на основе оксида вольфрама и Al–SBA-15 для окисления сернистых соединений нефтяного происхождения

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Abstract

Синтезированные катализаторы на основе оксида вольфрама и содержащего алюминий мезопористого носителя Al–SBA-15 исследованы в окислении пероксидом водорода серосодержащих соединений нефтяного происхождения. Катализаторы исследованы методами низкотемпературной адсорбции–десорбции азота, рентгенофазового анализа (РФА), просвечивающей электронной микроскопии (ПЭМ) с элементным картированием, ядерного магнитного резонанса (ЯМР), термопрограммируемой десорбции аммиака, ИК-спектроскопии и спектроскопии комбинационного рассеяния света (КРС). Изучена зависимость конверсии дибензотиофена (ДБТ) от продолжительности реакции, температуры, состава, кислотности, количества катализатора и количества окислителя. Подобраны оптимальные условия окисления модельной смеси на основе ДБТ с содержанием серы 10000 ppm: 80°С, 3 мас. % катализатора, 3 мл ацетонитрила, 60 мин. После промывки катализаторов от продуктов окисления они могут быть повторно использованы не менее пяти циклов без значительной потери своей активности.

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About the authors

Олеся Олеговна Гуль

Московский государственный университет имени М.В. Ломоносов

Author for correspondence.
Email: lesi00gul@gmail.com
ORCID iD: 0000-0001-6708-0058

химический факультет, аспирант

Russian Federation, 119991, Москва

Полина Димитровна Домашкина

Московский государственный университет имени М.В. Ломоносова

Email: lesi00gul@gmail.com
ORCID iD: 0000-0002-0456-8248

химический факультет, к.х.н.

Russian Federation, 119991, Москва

Аргам Виликович Акопян

Московский государственный университет имени М.В. Ломоносова

Email: lesi00gul@gmail.com
ORCID iD: 0000-0001-6386-0006

химический факультет, д.х.н.

Russian Federation, 119991, Москва

Александр Владимирович Анисимов

Московский государственный университет имени М.В. Ломоносова

Email: lesi00gul@gmail.com
ORCID iD: 0000-0001-9272-2913

химический факультет, д.х.н., проф.

Russian Federation, 119991, Москва

Владимир Маркович Сенявин

Московский государственный университет имени М.В. Ломоносова

Email: lesi00gul@gmail.com
ORCID iD: 0009-0001-4228-6903

химический факультет, к.х.н.

Russian Federation, 119991, Москва

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Supplementary files

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2. Fig. 1. Low-temperature nitrogen adsorption–desorption isotherms. Catalysts: curve 1 — SBA-15; curve 2 — 1% Al–SBA-15; curve 3 — 5% Al–SBA-15; curve 4 — 5% W/Al–SBA-15.

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3. Fig. 2. NMR Al27 spectrum of the 5% Al–SBA-15 catalyst.

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4. Fig. 3. X-ray diffraction patterns of SBA-15 catalysts and support.

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5. Fig. 4. TEM images: (a) – SBA-15, (b) – 5% W/1% Al–SBA-15 and (c) – 5% W/5% Al–SBA-15.

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6. Fig. 5. TEM images with mapping of the 5% W/5% Al–SBA-15 catalyst with the distribution of elements: (a) – silicon; (b) – tungsten; (c) – aluminum; (d) – oxygen.

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7. Fig. 6. FT-IR (a) and Raman spectra (b) of W/Al–SBA-15 catalysts and SBA-15 support: 1 – SBA-15; 2 – 5% W/5% Al–SBA-15; 3 – 10% W/5% Al–SBA-15.

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8. Fig. 7. Comparison of the activity of 2.5% W/1% Al–SBA-15 catalysts; 5% W/1% Al–SBA-15; 10% W/1% Al–SBA-15; 2.5% W/5% Al–SBA-15; 5% W/5% Al–SBA-15; 10% W/5% Al–SBA-15. Oxidation conditions: H2O2 : S = 6 : 1 (mol), 0.5 wt. %, 60°C, S = 500 ppm.

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9. Fig. 8. Dependence of DBT conversion on the aluminum content and the amount of oxidizer. Oxidation conditions: 0.5 wt. % catalyst, 60°C, H2O2 : S (mol) – 2 : 1 (■); 4 : 1 (●); 6 : 1 (▲).

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10. Fig. 9. Dependence of DBT conversion on the amount of catalyst. Oxidation conditions: H2O2 : S = 4 : 1 (mol), 60°C, 20 min, S = 500 ppm.

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11. Fig. 10. Dependence of DBT conversion on temperature and time. Oxidation conditions: cat. 5% W/5% Al–SBA-15, H2O2 : S = 4 : 1 (mol), 0.5 wt. % catalyst, S = 500 ppm.

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12. Fig. 11. Oxidation of different classes of sulfur compounds with hydrogen peroxide. Oxidation conditions: H2O2 : S = 4 : 1 (mol), 0.5 wt. % catalyst, 60°C, 30 min, S = 500 ppm.

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13. Fig. 12. Dependence of oxidation of model mixtures on the addition of acetonitrile: (a) oxidation of model mixtures with different sulfur content of 500–5000 ppm (H2O2 : S = 4 : 1 (mol), 0.5 wt. % catalyst, 60°C); (b) oxidation of a model mixture based on DBT in n-dodecane with a content of 10000 ppm total sulfur (H2O2 : S = 4 : 1 (mol), cat. 0.5 wt. %, 80°C).

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