The chemistry of heterobimetallic compounds in which a redox-active metal is paired with a Lewis acidic, redox-inactive metal ion has become an area of intense interest in recent years. Diverse efforts have shown that Lewis acids can reliably tune the reduction potential and chemical reactivity of heterobimetallic systems, inspiring important applications in redox chemistry and catalysis. On the other hand, understanding the roles of Lewis acids in tuning the kinetics of electron transfer to heterobimetallic systems remains a frontier area. In this talk, I will discuss our group’s recent observations regarding electron transfer and reactivity encountered with a library of compounds containing heterobimetallic diamond cores containing redox-active metals (Ni, Pd, and U) that have been paired with redox-inactive Lewis acids. We find that Lewis acidity (as judged by the p<i>K</i><sub>a</sub> values of corresponding metal aqua complexes) is a reliable descriptor for modulated electron transfer kinetics. Recent results, including work examining systems containing multiple redox-inactive metals, will also be discussed.

Electron transfer chemistry of heterobimetallic diamond cores assembled within tailored macrocycles

ACS Spring Meeting 2021

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