Microdroplet-Mediated Multiphase Cycling in a Cloud of Water Drives Chemoselective Electrolysis

Electrification of water in clouds leads to fascinating redox reactions on Earth. However, little is known about cloud electrochemistry, except for lightning, a natural hazard that is nearly impossible to harness. We report a controllable electrochemistry that can be enabled in microclouds by fast phase switching of water between the microdroplet, vapor, and bulk phase. Due to the size-dependent charge transfer between droplets during atomization, this process generates an alternating voltage arising from the self-electrification and discharging of microdroplets, vapor, and bulk phase by electron and ion transfer. We show that the microclouds with alternating voltage cause 1,2-dichloroethane (ClH₂C-CH₂Cl) to be converted to vinyl chloride (H₂C═CHCl) at ∼80% selectivity. These findings highlight the importance of controlled cloud electrochemistry in accelerating the removal of volatile organic compounds and treating contaminated water. We suggest that this work opens an avenue for harnessing cloud electrochemistry to solve challenging chemoselectivity problems in aqueous reactions of environmental and industrial importance.