Synergistic Integration of Thermocatalysis and Electrocatalysis for Isopropanol Dehydrogenation Toward Efficient Hydrogen Production.

Isopropanol dehydrogenation represents a pivotal step in the liquid organic hydrogen carrier cycle. Conventional thermocatalytic routes require high temperatures and entail substantial energy penalties, while low-temperature electrocatalytic processes suffer from sluggish reaction kinetics. Herein, we report an integrated thermo-electrocatalytic strategy within a high-temperature proton exchange membrane electrolyzer (HT-PEME), enabling highly efficient isopropanol dehydrogenation. A RuIr bimetallic catalyst was designed, wherein Ru sites effectively promote the cleavage of both O─H and C─H bonds in isopropanol, while the incorporation of Ir optimizes the adsorption behavior of reaction intermediates, thereby mitigating Ru site poisoning and significantly enhancing catalytic stability. At 200°C and 0.5 V, the integrated system delivers an exceptional anodic acetone production rate of 1336.36 mmol g-1 h-1, coupled with a cathodic H2 evolution rate of 1451.31 mmol g-1 h-1. This synergistic approach provides a robust and broadly applicable pathway for efficient H2 production.