EAGER: Alkyl Precursors for Tuning Local Composition in Zeolites as an Enabling Platform for Catalysis

Many products used in daily life depend on catalysts to be manufactured. Catalysts help chemical reactions happen faster, use less energy, and produce less waste. This project will study solid catalysts to help make an important class of chemicals that are used in battery materials, solvents, plastics, and other products. Most solid catalysts are designed around single active atoms, which can limit how well they guide reactions that involve several steps. This project will test whether precisely positioning two atoms in a catalyst can work together to control these steps more effectively. The researchers will make these materials, measure how their structure affects reaction behavior, and use computer models to explain what they observe. The project will provide new design rules for catalysts that support cleaner and more selective chemical manufacturing. The project will also provide advanced training for students in modern experimental and computational methods. Additionally, the project will use three-dimensional printed models to explain catalyst design to students and the public. The project will create paired Lewis acid sites in zeolite Beta and test how these sites affect cyclic carbonate synthesis. The researchers will use methyl-germanium precursors to create defects near framework germanium atoms. They will then add catalytically active atoms such as tin, zirconium, or hafnium to those sites. The new materials will be compared with control zeolites that contain isolated sites, conventional defect-derived sites, or non-directed mixtures of atoms. Site proximity will be tested with standard characterization methods and with probe molecules designed to bind to two nearby Lewis acid centers. Computer models will predict stable site structures, probe binding, spectra, and reaction pathways. Catalytic tests will measure conversion, selectivity, rates, activation energies, and catalyst reuse. Together, these results will show whether nearby atoms change epoxide activation, ring opening, carbonate intermediate formation, ring closure, or product release. The project will advance catalysis, chemical engineering, and surface chemistry by testing whether atomic neighborhoods in zeolites can be used as a catalyst design variable beyond pore structure and isolated active-site identity. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.