A cleaner energy future requires new classes of multifunctional and tunable materials that can be synthesized and modified under mild conditions. Metal oxides are versatile and ubiquitous materials that feature broadly tunable electronic properties and high chemical and thermal stability, yet their syntheses and post-synthetic modification remain energy intensive and challenging to control. In contrast, molecular species offer fine synthetic control, but can lack the desirable mechanical and electronic properties associated with extended solids, including facile intermolecular electron transfer. Layered hybrid materials can address this challenge by placing molecular centers in close contact with inorganic conduction pathways that possess high charge carrier mobility. We are building a material platform based on hybrid organic-inorganic metal oxides that we have termed <b>hybrid bronzes</b>. These place metal oxide layers capable of sustaining multiple metal oxidation states and therefore variable concentrations of mobile electrons in atomic-scale proximity to molecular species that can be judiciously modified to incorporate functional handles and potential redox- and photoactivity. Hybrid bronzes display promising qualities for energy-related applications, including tunable electronic band gaps, mixed electronic and ionic conductivity, and electrochromism. We synthesize them under mild, solution-state conditions to yield bulk microcrystalline powders and single crystals and we have already developed a library of these intriguing materials. Now, utilizing a diverse suite of diffractive, electrochemical, and spectroscopic characterization techniques including measurements under extreme conditions, we elucidate fundamental relationships between structural and electronic properties to inform future design of this promising new class of materials.

Structural and electronic versatility of hybrid bronzes

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ACS Fall 2022

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