Abstract
AbstractSolid–liquid interface engineering has recently emerged as a promising technique to optimize the activity. Here, the cation identity and induced interfacial electronic structure of Pt have been shown to have a particularly significant impact on the activity of desired photocatalytic hydrogen evolution. The behavior of Pt aggregation synergistically induced by photo‐electron accumulation on Pt surface and the ionic potential of alkalis was logically elucidated. X‐ray photoelectron spectroscopy (XPS) and photoconductive atomic force microscopy (pcAFM) results revealed that the surface of alkali‐triggered Pt nanoparticles (Pt NPs) aggregates are electron‐deficient, which favors photo‐induced charge separation, leading to improved reaction kinetics. Based on the density functional theory (DFT) calculation, alkalis‐triggered Pt NPs has lower Gibbs free energy and potential energy surface of H2 formation for hydrogen evolution in thermodynamics. As a result, K+ triggered Pt cocatalyst displays the highest activity (3306.6 μmol h−1 g−1) on pure CN, almost 4‐fold increase compared to the reference without the addition of alkalis, showing high utilization efficiency of Pt.
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