Механизмы активации и превращения малых алканов на Zn-и Ga-содержащих цеолитах бета по данным ЯМР in situ
Диссертация
Продемонстрировано, что модифицирование цеолита бета цинком или галлием существенным образом влияет на активацию С-Н связи в алканах бренстедовскими кислотными центрами цеолита. Установлено, что промотирующее влияние частиц оксида цинка или галлия на активацию С-Н связи бренстедовскими центрами цеолита заключается в предварительной диссоциативной адсорбции алканов на частицах оксида цинка или… Читать ещё >
Содержание
- ВВЕДЕНИЕ 5 ЛИТЕРАТУРНЫЙ ОБЗОР
- Глава 1. Механизмы активации алканов на твердых кислотных катализаторах
- 1. 1. Активация алканов на твердых кислотных катализаторах
- 1. 1. 1. Карбений-ионный механизм активации
- 1. 1. 2. Карбоний-ионный механизм активации
- 1. 2. Активация алканов на 2п- и ва-содержащих цеолитах
- 1. 2. 1. Строение Zn-цeнтpoв в цеолитах
- 1. 2. 2. Природа активных ва-центров в цеолитах
- 1. 2. 3. Активация алканов на Хп- и ва-содержащих цеолитах
- 1. 3. ЯМР спектроскопия. Исследование механизмов каталитических реакций 35 ЭКСПЕРИМЕНТАЛЬНАЯ ЧАСТ
- 1. 1. Активация алканов на твердых кислотных катализаторах
- Глава 2. Характеристика катализаторов. Методы исследования
- 2. 1. Характеристика используемых катализаторов
- 2. 2. Методика приготовления ЯМР образцов
- 2. 3. Регистрация ЯМР спектров высокого разрешения в твердом теле
- 2. 4. Кинетический анализ
- 2. 5. Регистрация ИК и УФ спектров
- 2. 6. ГХ-МС анализ
- РЕЗУЛЬТАТЫ И ОБСУЖДЕНИЕ
- Глава 3. Кислотные свойства ОН групп цеолита бета
- 3. 1. Характеристика ОН групп цеолита Н-ВЕА методом ИК
- 3. 2. Характеристика ОН групп цеолита Н-ВЕА методом ЯМР
- 3. 3. Структура сильнокислотных БЮН групп цеолита бета
- Глава 4. Активация малых алканов и молекулярного водорода на Zn- и ва-содержащих цеолитах бета
- 4. 1. H/D обмен в С1-С4 алканах на Zn- и Ga-содержащих цеолитах бета
- 4. 1. 1. Кинетическая модель H/D обмена
- 4. 1. 2. Обмен в метане-^ и этане-d6 на Н-ВЕА, H-ZSM5, Zn/H-BEA и Ga/H-BEA цеолитах
- 4. 1. 3. Обмен в пропане-г/8 и н-бутане-^10 на H-ZSM-5, Zn/H-ZSM-5, Zn/H-BEA и Ga/H-BEA цеолитах
- 4. 2. Хемосорбция малых алканов на Zn/H-BEA и Ga/H-BEA цеолитах по данным 13С ВМУ ЯМР спектроскопии
- 4. 2. 1. Хемосорбция алканов на цеолите Zn/H-BEA
- 4. 2. 2. Хемосорбция алканов на оксиде галлия (III) и цеолите Ga/H-BEA
- 4. 3. Механизм активации связи С—Н малых алканов бренстедовскими кислотными центрами Zn- и Ga-содержащих цеолитов бета
- 4. 4. H/D обмен молекулярного водорода с бренстедовскими кислотными центрами Н-ВЕА, Zn/H-BEA и Ga/H-BEA цеолитов
- 4. 1. H/D обмен в С1-С4 алканах на Zn- и Ga-содержащих цеолитах бета
- Глава 5. Ароматизация малых алканов на Zn- и Ga-содержащих цеолитах бета
- 5. 1. Превращение этана на цеолите Zn/H-BEA
- 5. 1. 1. Анализ продуктов превращения этана методом 13С КП/ВМУ ЯМР
- 5. 1. 2. Анализ кинетики превращения этана на цеолите Zn/H-BEA с помощью ]Н ВМУ ЯМР спектроскопии
- 5. 1. 3. Анализ кинетических схем
- 5. 2. Превращение пропана на цеолите Zn/H-BEA
- 5. 2. 1. Превращение пропана на цеолите Zn/H-BEA по данным 13С КП/ВМУ ЯМР метода
- 5. 2. 2. Анализ кинетики превращения пропана на цеолите Zn/H-BEA
- 5. 3. Совместная ароматизация метана и пропана на цеолите Ga/H-BEA
- 5. 3. 1. Активация метана на цеолите Ga/H-BEA
- 5. 3. 2. Совместное превращение метана и пропана на цеолите Ga/H-BEA
- 5. 3. 3. Механизм внедрения метана в ароматические углеводороды
- 5. 3. 4. Механизм внутримолекулярного переноса атомов углерода в толуоле
- 5. 1. Превращение этана на цеолите Zn/H-BEA
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