Gradient electric fields at solid–liquid interfaces via partitioned Cu species for selective dehydrochlorination

Abstract Integrating segregated unit operations into a single “catalyst‐as‐a‐reactor” architecture represents a pivotal frontier in process intensification. Herein, a spatially resolved interface is engineered by strategically partitioning copper species between a carbon support and an ionic liquid (IL) overlayer. Within this design, carbon‐anchored Cu functions as an electron reservoir that drives charge toward solvated active sites, inducing a robust interfacial gradient electric field. This programmable electronic environment facilitates bidirectional electron transfer, thereby reducing the C–Cl activation barrier by 0.26 eV. Consequently, the spatially optimized 3Cu/C@2Cu‐10IL catalyst delivers near‐complete 1,1,2‐trichloroethane conversion (>99%) with >95% vinylidene chloride selectivity. This high performance translates to a space–time yield of 170.21 g VDC ·g metal −1 ·h −1 and a projected ~29.5% cost reduction via the elimination of saline wastewater. This work establishes spatial active‐site control as a versatile paradigm for streamlining complex chemical transformations.