Controlled Synthesis of Three Pdsn Nanocatalysts with Enhanced Electrocatalytic Performance for Alcohol Oxidation Reaction Via a Kinetic–Induced Method

Abstract

The preparation of active, stable and selective Pd-based nanocatalysts for alcohol oxidation reactions (AORs) is urgently desired. Nowadays, advanced ultrathin porous nanosheets (UPNSs) have emerged as efficient electrocatalysts due to their abundant accessible surfaces and low coordination sites. Herein, a template method is developed to prepare three PdSn nanocatalysts with different morphological features, involving UPNSs, nanonetworks (NNWs) and nanodentrites (NDs), only by altering temperature during the Sn deposition process. The growth mechanism of three PdSn nanocatalysts with different morphologies originates from the selective etching and different atom migration rates via kinetics–induced procedure. Benefiting from the boosted synergistic effect and favorable surface defects, the PdSn UPNSs exhibit preeminent electrocatalytic activity of 8846/6672 mA mg–1 for ethylene glycol/ethanol oxidation reaction (EGOR/EOR), coupled with excellent electrocatalytic durability through long-term Chronoamperometry (CA) tests and multiple cyclic voltammetry (CV) measures. The possible performance enhancement mechanism of the PdSn UPNSs is also investigated from the perspectives of electronic structure and surface structure. Mechanism shows that PdSn UPNSs possess the lowest d-band center and the superior conductivity, contributing to the distinguished poison resistance ability and accelerated reaction kinetics. The work not only emphasizes highly desired PdSn nanocatalysts with boosted EOR and EGOR performances, but also proposes the effect of morphology regulation on electrocatalytic properties, providing a significant guidance to fabricate efficient nanocatalysts by adjusting the reaction temperature.

Keywords: PdSn nanocatalysts, Ultrathin porous nanosheets, Nanoneworks, Nanodentrites, Ethylene glycol oxidation reaction, Ethanol oxidation reaction