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Single‐Atomic‐Site Platinum Steers Middle Hydroxyl Selective Oxidation on Amorphous/Crystalline Homojunction for Photoelectrochemical Glycerol Oxidation Coupled with Hydrogen Generation

Xinyan Feng, Tingting Sun, Xuefan Feng, Hao Yu, Yu Yang, Limiao Chen, Fuqin Zhang

2024Advanced Functional Materials64 citationsDOI

Abstract

Abstract Photoelectrochemical (PEC) organic conversion is a promising approach to convert low‐cost organics to value‐added chemicals, which urgently needs the development of efficient and highly selective photoanodes. Here, a Pt single‐atom dispersed WO 3 amorphous/crystalline homojunction for anodic glycerol oxidation reaction (GOR) coupled with cathodic hydrogen generation is reported. In the coupled photoelectrocatalytic system, the novel Pt‐SA/WO x photoanode reaches a photocurrent density of 2.85 mA cm −2 at 1.2 V versus RHE, with up to 297.3 mmol m −2 h −1 of glycerol conversion rate and 60.2% of dihydroxyacetone (DHA) selectivity, realizing green synthesis of high‐value chemicals. The experimental data and theoretical calculations reveal the regulated band structure, build‐in electric field, and surface charge density of Pt‐SA/WO x , which can improve the carrier lifetime, accelerate charge transfer, and reduce the energy barrier for the GOR process, thus boosting PEC activity and DHA selectivity. This work provides a feasible plan for designing atomic‐level engineering and constructing amorphous/crystalline homojunction on photoanodes for efficient PEC high‐value products from biomass.

Topics & Concepts

HomojunctionMaterials sciencePhotocurrentAmorphous solidSelectivityChemical engineeringWater splittingAnodeReversible hydrogen electrodePhotocatalysisNanotechnologyElectrolyteCatalysisElectrodeOptoelectronicsPhysical chemistryChemistryOrganic chemistryWorking electrodeHeterojunctionEngineeringElectrocatalysts for Energy ConversionAdvanced Photocatalysis TechniquesCatalytic Processes in Materials Science