Phosphorus-Doped PdSn Nanocatalyst with Abundant Defective Atoms for Enhanced Methanol Oxidation.

Abstract

The design of the nanostructure of palladium-based nanocatalysts is considered to be a very effective way to improve the performance of nanocatalysts. Recent studies have shown that multiphase nanostructures can increase the active sites of palladium catalysts, thus effectively improving the catalytic efficiency of palladium atoms. However, it is difficult to regulate the phase structure of Pd nanocatalysts to form a compound phase structure. In this work, PdSnP nanocatalysts with different compositions were synthesized by fine-regulating the doping amount of phosphorus atoms. The results show that the doping of phosphorus atoms not only changes the composition of PdSn nanocatalysts but also changes the microstructure, forming amorphous and crystalline multiphase structures. This multiphase nanostructure contains abundant interfacial defects, which effectively promotes the electrocatalytic oxidation efficiency of Pd atoms in small-molecule alcohols. Compared with the undoped PdSn nanocatalyst (480 mA mgPd-1 and 2.28 mA cm-2) and the commercial Pd/C catalyst (397 mA mgPd-1 and 1.15 mA cm-2), the mass (1746 mA mgPd-1) and specific activities (8.56 mA cm-2) of PdSn0.38P0.05 nanocatalysts in the methanol oxidation reaction were increased by 3.6 and 3.8 times and 4.4 and 7.4 times, respectively. This study provides a new synthesis strategy for the design and synthesis of efficient palladium-based nanocatalysts for the oxidation of small-molecule alcohols.