Physical-Inorganic Chemistry of Porous Materials
Our research program envisions porous materials as extended ligands for transition metal ions, providing access to unique active site geometric and electronic structures – and therefore functions – that are not readily accessible in small molecule chemistry. Our studies address diverse challenges of economic and environmental significance, including site-selective synthesis of heterogeneous catalysts, active sites for CO2 conversion and C-H functionalization, and metal-organic frameworks to capture toxic and high-value ions. A unifying theme is the use of site-selective spectroscopy to guide the installation of novel inorganic architectures in porous materials. In pursuit of this research, graduate students, postdoctoral fellows, and undergraduate mentees will develop a unique combined skillset including rigorous inorganic spectroscopy, experimentally calibrated density functional theory calculations, and framework materials chemistry.
Designer Active Sites in Zeolites
Metallozeolites are an important class of robust but synthetically inflexible heterogeneous catalysts. A lack of synthetic control over function and a lack of reliable spectroscopic data have slowed progress in metallozeolite catalysis for decades. We develop synthetic methods, guided by site-selective spectroscopy, to selectively install transition metals in zeolite lattices with molecular precision. The rational design of ‘single-site’ materials is thus envisioned, opening a promising new area at the nexus of coordination chemistry and heterogeneous catalysis.
On the Rack: Active Sites in Rigid Lattices
Metalloenzymes often enforce strained active site geometries associated with enhanced function – so-called ‘entatic states’. We seek to generate and spectroscopically characterize entatic active sites in zeolites and porous carbons for in situ CO2 capture and conversion, as well as C-H activation and functionalization.
Selective Ion Adsorption in Metal-Organic Frameworks
Selective ion adsorption is a growing area of interest for porous materials research, with direct relevance to some of our most pressing economic and environmental issues. We use advanced site-selective spectroscopy to guide the development of metal-organic frameworks as solid ion adsorbers, enabling the efficient capture of toxic cyanide and valuable cyanometallates derived from mining and e-waste/battery recycling.