Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Abstract

AbstractMetal promotion is the most widely adopted strategy for enhancing the hydrogenation functionality of an oxide catalyst. Typically, metal nanoparticles or dopants are located directly on the catalyst surface to create interfacial synergy with active sites on the oxide, but the enhancement effect may be compromised by insufficient hydrogen delivery to these sites. Here, we introduce a strategy to promote a ZnZrOxmethanol synthesis catalyst by incorporating hydrogen activation and delivery functions through optimized integration of ZnZrOxand Pd supported on carbon nanotube (Pd/CNT). The CNT in the Pd/CNT + ZnZrOxsystem delivers hydrogen activated on Pd to a broad area on the ZnZrOxsurface, with an enhancement factor of 10 compared to the conventional Pd-promoted ZnZrOxcatalyst, which only transfers hydrogen to Pd-adjacent sites. In CO2hydrogenation to methanol, Pd/CNT + ZnZrOxexhibits drastically boosted activity—the highest among reported ZnZrOx-based catalysts—and excellent stability over 600 h on stream test, showing potential for practical implementation.