Preparation Strategy Using Pre-Nucleation Coupled with In Situ Reduction for a High-Performance Catalyst towards Selective Hydrogen Production from Formic Acid

Formic acid decomposition (FAD) is one of the most promising routes for rapid hydrogen (H2) production. Extensive efforts have been taken to develop efficient catalysts, which calls for the simultaneous regulation of the electronic structure and particle size of the catalyst. The former factor determines the intrinsic performance, while the latter corresponds to the active site utilization. Here, an effective preparation strategy, pre-nucleation coupled with in situ reduction, is developed to realize and well-tune both surface electronic states and particle size of the pallidum (Pd) catalyst. Benefiting from the structural merits, the as-prepared catalyst exhibits high mass-specific activity of 8.94 molH2/(gPd·h) with few carbon monoxide (CO) molecules, and the activation energy could reach a value as small as 33.1 kJ/mol. The work not only affords a highly competitive FAD catalyst but also paves a new avenue to the synthesis of ultra-fine metal nanoparticles with tailorable electronic structures.Keywords:hydrogen evolution;formic acid;heterogeneous catalysis;high selectivity;Pd-PdO interface