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Abstract
Abstract Hydrogen peroxide (H2O2) is a platform green oxidant for high‐value chemical synthesis, but its centralized production hinders its widespread use in a safe manner. Here, we describe a practical tandem electro‐thermochemical H2O2‐mediated oxygenation platform for the synthesis of various high‐value oxygen‐containing compounds. The integration of solid‐electrolyte H2O2 electrosynthesis with heterogeneous zeolite thermocatalysis enables atom‐efficient oxygenations without the need for downstream electrolytes or catalysts separation. A spatially decoupled tandem system integrating aqueous H2O2 electrosynthesis with nonaqueous thermocatalysis offers independent optimization capabilities, thus maximizing the overall space–time yield (STY). With microfluidic packed‐bed intensification for heterogeneous thermocatalysis, this tandem system achieved H2O2‐mediated oxygenation of thioesters to sulfoxide at a high current density (300 mA cm−2) and STY (7.07 mmol cm−3 h−1). Furthermore, the platform's broad applicability was showcased with titanium‐silicalite‐1 zeolite catalyzed olefin epoxidation and cyclohexanone oxime synthesis, underscoring its potential for diverse catalytic oxygenation applications.
Published Version
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