Photochemistry Journey to Multielectron and Multiproton Chemical Transformation

The odyssey of photochemistry is accompanied by the journey to manipulate electrons and protons in time, in space, and in energy. Over the past decades, single-electron (1e(-)) photochemical transformations have brought marvelous achievements. However, as each photon absorption typically generates only one exciton pair, it is exponentially challenging to accomplish multielectron and proton photochemical transformations. The multistep differences in thermodynamics and kinetics urgently require us to optimize light harvesting, expedite consecutive electron transfer, manipulate the interaction of catalysts with substrates, and coordinate proton transfer kinetics to furnish selective bond formations. Tandem catalysis enables orchestrating different photochemical events and catalytic transformations from subpicoseconds to seconds, which facilitates multielectron redox chemistries and brings consecutive, value-added reactivities. Joint efforts in molecular and material design, mechanistic understanding, and theoretical modeling will bring multielectron and proton synthetic opportunities for fuels, fertilizers, and chemicals with enhanced versatility, efficiency, selectivity, and scalability, thus taking better advantage of photons (i.e., sunlight) for our sustainable society.

Automated summary

The Odyssey of photochemistry involves manipulating electrons and protons in time, space, and energy. While single-electron photochemical transformations have achieved remarkable success, achieving multielectron and proton reactions is exponentially challenging. Optimizing light harvesting, accelerating consecutive electron transfer, manipulating catalyst-substrate interactions, and coordinating proton transfer kinetics are necessary to achieve selective bond formations. Tandem catalysis enables coordination between different photochemical events and catalytic transformations, facilitating multielectron redox chemistries and consecutive, value-added reactivities. Collaborative efforts in molecular and material design, mechanistic understanding, and theoretical modeling will unlock opportunities for multielectron and proton transformations with enhanced versatility, efficiency, selectivity, and scalability, ultimately leading to a more sustainable society.