Structure and Properties of Catalytically Active Palladium Centers in Zeolites and Metal-Organic Frameworks: Ab Initio Calculations and Experimental Studies at Megascale Research Facilities

Грант Президента. Бугаев. 2021-2022
From 12.04.2021 till 31.12.2022
Grant holder: Aram Bugaev
Members: Oleg Usoltsev, Alina Skorynina, Elizaveta Kozyr, Anna Pnevskaya

Materials based on zeolites and metal-organic frameworks, functionalized with isolated active palladium centers, are promising heterogeneous catalysts having many advantages with respect to their homogeneous analogs. A mechanistic understanding of the reaction processes occurring at the active sites of palladium during catalytic reactions, as well as the deactivation mechanisms associated with a change in the oxidation state and the formation of palladium nanoclusters, is key steps towards the creation of new durable catalysts with desired practical properties. This project focuses on the use of X-ray absorption spectroscopy at Megascale research facilities using in situ and operando regimes, original methods of data processing and analysis, including the use of machine learning methods, as well as modern quantum-chemical methods for determining the local atomic and electronic structure of active centers of palladium. in zeolites and metal-organic framework structures, as well as their evolution in the course of catalytic reactions. The results to be obtained will explain the mechanisms of a number of the most important reactions in the petrochemical and fine chemical industries and to isolate the processes responsible for the aging and deactivation of catalysts.