Анотація
Розглянуто розвиток уявлень про структуру активного центру твердофазних каталізаторів, починаючи від робіт Х. Тейлора до сучасного розуміння складної та багаторівневої структури каталітичних систем. Проаналізовано основні типи активних центрів каталізаторів окисно-відновлювальних процесів глибокого, селективного та вибіркового перетворення. Показано, що для кожного типу реакцій, незалежно від хімічної природи компонентів каталізатора, структура активного центра характеризується певними спільними ознаками та визначає напрямок перетворення. Особливу увагу приділено структурі активних центрів, сформованих за типом ізольованого активного центра (“single site isolation”), які дозволяють досягти високої селективності каталітичних процесів в напрямку створення цільових продуктів і забезпечити протікання нових реакцій. Зокрема, реакція окиснювального карбонілювання метану в оцтову кислоту вперше була проведена в газовій фазі з використанням як окисника молекулярного кисню та каталізаторах, активні центри яких являли собою изольовані іони Rh3+ у складі селенохлоридів родію. Окремий тип активних центрів представлено атомами, розташованими на границях розділу кристалітів, які виникають внаслідок міжфразної взаємодії між компонентами каталізатора: носієм, активним компонентом, модифікатором, а також границями між однорідними нанокристалітами в агломерованих системах. Показано, що важливу роль у прояві каталітичних властивостей відіграє доступність активних центрів для реагентів, яка обумовлена просторовою структурою каталізаторів. Прикладом таких каталітичних систем є цеоліти, металоорганічні сполуки (MOF), мезоструктурні оксиди, в яких активні центри розташовуються всередині порожнини каналів. Основна стратегія досліджень в галузі створення удосконалених каталізаторів спрямована на розроблення методів синтезу каталітичних матеріалів, у яких забезпечується як утворення максимальної кількості активних центрів, так їх доступність для реагентів і подальше селективне перетворення в цільові продукти. Конструювання таких систем є комплексним завданням, яке ґрунтується на встановленні кореляційних залежностей між складом, структурою і розмірними характеристиками каталітичних матеріалів.
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