Realizing Electrocatalytic Hydrogenation via Hydride Transfer

Hydrogenation is one of the most important transformations in chemical manufacturing and is widely used in the production of pharmaceuticals, agrochemicals, fine chemicals, and commodity materials. However, conventional hydrogenation often requires high-pressure hydrogen gas, elevated temperature, and precious-metal catalysts, which can increase energy consumption, safety concerns, and manufacturing cost. Electrocatalytic hydrogenation offers a promising alternative because it can use electricity to drive chemical reduction under ambient conditions. Nevertheless, conventional electrochemical systems often suffer from competing hydrogen evolution and limited control over hydride-transfer pathways, especially for challenging reactions such as asymmetric hydrogenation. This project will develop a new Janus palladium membrane electrode platform to generate reactive hydride species from water using electricity as the sole energy input. The research will advance fundamental understanding of heterogeneous hydride transfer and provide new strategies for selective, energy-efficient hydrogenation under mild conditions. Prof. Yujie Sun from the University of Cincinnati is developing Janus palladium membrane electrodes for electricity-driven hydride-transfer chemistry. In this system, water is reduced on one side of the palladium membrane electrode to form hydrogen atoms, which permeate through the palladium lattice and are converted into reactive hydride species on the opposite side under controlled electrochemical polarization. This unique dual-cell design separates hydrogen generation from substrate hydrogenation, enabling improved control over hydride reactivity and substrate selectivity. The project will investigate how the hydricity of palladium–hydrogen species can be tuned by applied potential, develop molecular hydride donor-mediated hydrogenation reactions, explore electrochemical regeneration of enzyme cofactors, and create chiral modifier-decorated palladium membrane electrodes for asymmetric hydrogenation. These studies will provide new knowledge at the interface of electrocatalysis, organic synthesis, and sustainable chemical manufacturing. This project will also contribute to the training of future scientists in the emerging field of organic electrocatalysis. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.