Efficient Photogenerated Carrier‐Assisted COads Removal via Schottky Barrier of PdSn/WO3 for Formic Acid Oxidation Reaction

Limiting the formation of CO adsorbed species (COads) or promoting its removal during formic acid oxidation reaction (FAOR) is essential to improving the activity and stability of Pd‐based catalysts. In this work, an innovative strategy is proposed to adjust the Schottky barrier height (SBH) through band structure design for effective utilization of photogenerated carriers to remove COads, thereby improving the FAOR performance of Pd‐based catalysts. Specifically, the electronic structure of Pd is adjusted by loading on the WO3 nanosheets and incorporating different amounts of Sn to reduce Fermi level pinning and adjust SBH. The accelerated migration of photogenerated electrons promotes the accumulation of photogenerated holes on the valence band of WO3 for the oxidation and removal of COads. The constructed Schottky barrier effectively regulates the electronic structure of the catalyst and optimizes the adsorption energy of intermediate CO, thus inhibiting the indirect reaction pathway. Therefore, the optimal Pd1Sn1/WO3 catalyst provides higher COads removal efficiency for photogenerated carrier‐assisted electrocatalytic FAOR, with a mass activity of 2262.3 mA mg−1Pd, outperforming most Pd‐based catalysts. This work offers a novel approach to designing Pd‐based catalysts, combining electronic structure modulation with photogenerated carrier assistance for the effective removal of COads to advance FAOR performance.