Abstract
Single-molecule and framework-based electrocatalysts are increasingly attractive in the field of electrocatalysis due to their precise atomic-level control and highly tunable properties, enabling the development of highly efficient and selective energy conversion processes. Tailoring charge and spin polarization within these structures presents a unique opportunity to significantly enhance catalytic activity, opening new avenues in developing efficient electrocatalytic systems. This presentation will outline methods our group has developed to synthesize and adjust charge and spin configurations in molecular and framework catalysts. We will explore a variety of pathways, including the design of single molecular catalysts with optimized spin states, the application of mesomeric and inductive effects for charge regulation, and the use of external magnetic fields and chirality to modulate spin polarization at the molecular level. Our findings indicate that such customization can accelerate the kinetics of spin-sensitive electrochemical reactions like oxygen electrocatalytic reactions. Furthermore, we will discuss how the inherent properties of the catalysts, particularly magnetic moments and spin-orbit interactions, play a crucial role in influencing catalytic performance in the presence of spin potentials. Hence, this presentation aims to provide an overview of our advanced strategies to reconfigure charge and spin states in framework and molecular catalysts, underscoring their potential to revolutionize electrochemical energy conversion technologies.
Published Version
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