Events in inorganic chemistry.

Synthesis as a Gate to Materials Science, Physics, and Biology: The Chemistry of Tetrathiafulvalene-2,3,6,7-Tetrathiolate

Abstract: I will discuss our laboratory’s exploration of tetrathiafulvalene tetrathiolate (TTFtt) ligands in coordination complexes and molecular materials. TTFtt is a fusion of the common organic electronic TTF unit with two dithiolene motifs which are known to support unusual physical properties. The incorporation of these fragments into polymeric materials results in unusual physical properties, namely signatures of metallic conductivity without structural order.

Sila-Diamondoids: Atomically Precise Clusters of Crystalline Silicon

This talk will describe the synthesis, derivatization, and quantum transport properties of silicon diamondoids—atomically precise clusters of crystalline silicon. First, we describe strategies for the functionalization of the fundamental silicon diamondoid cluster, sila-adamantane. Mechanistic insights support that an aluminate-stabilized silylium at the 2-position of sila-adamantane is the terminal intermediate in its isomerization synthesis; we can intercept this intermediate to install halides at the 2-position.

More Than Simple Lewis Acids - Molecular Perspectives of Rare-Earths at the Interfaces of Catalysis, Sustainability, and Materials

The rare-earths (lanthanides + group III) are critical materials that underlie numerous technological advances ranging from information storage, human health, high-performance electronics, energy and the environment, and catalysis. Robust connections between molecular structure, properties, and function are central to advancing the performance and sustainability of these materials; however, achieving this can be limited by the complexity and heterogeneity in homogeneous and heterogeneous systems alike.

Molecular Approaches to Advancing 2D Conductive MOFs for Tailored Properties and Applications

Abstract: 2D electrically conductive metal-organic frameworks (EC-MOFs) represent a distinctive class of porous electronic materials with significant potential in applications ranging from energy storage to advanced electronics. However, their broader impact has been limited by the constrained diversity of structural motifs and chemical functionalities. In this talk, I will present our research efforts demonstrating how molecular approaches drive the advancement of EC-MOFs by tailoring their electronic properties and functionalities.

Discovery of Manganese-Dependent Monooxygenases

The aerobic oxidation of carbon–hydrogen (C–H) bonds in biology is currently known to be accomplished by a limited set of cofactors that largely include heme, nonheme iron, and copper. While manganese cofactors perform difficult oxidation reactions, including water oxidation within Photosystem II, they are generally not known to be used for C–H bond oxidation, and those that do catalyze this important reaction display highly limited intrinsic reactivity.

C-H functionalization inspired by copper enzymes

Abstract: High-valent Cu(III) complexes have long been proposed as important intermediates in biological redox processes and organic transformations involving the activation of C-H bonds. However, the proposed high-valent Cu(III) intermediates often elude detection due to their fleeting lifetimes. In the first part of my talk, I will present a series of dicopper (II,III) coordination complexes as models to understand the reactivity of NO and NO2- at dicopper enzymes.

Control of Reaction Outcome by Iron Oxygenases

Enzymes that use iron cofactors to activate molecular oxygen for hydroxylation, halogenation, desaturation, epoxidation, fragmentation, and peroxidation of unactivated carbon centers must guide their very reactive intermediates down preferred reaction paths to their specific outcomes. Our growing understanding of the general and enzyme-specific control strategies used by these enzymes has enabled the development of new catalytic capabilities and provided a roadmap for deployment of these enzymes in biocatalysis.

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