Electronic structure engineering of asymmetric coupled dual-cocatalysts on carbon nitride for synergistically enhancing photocatalytic H2 evolution
关键字:Polymeric carbon nitride; Dual cocatalysts; Asymmetrically geometrical deployment; Synergistic interactions; Photocatalytic hydrogen evolution
摘要:Photocatalytic hydrogen production is a promising strategy to solve the energy crisis and environmental issues. Herein, an efficient photocatalyst consisting of the MoP quantum dots and Pt nanoclusters dual cocatalysts anchored on polymeric carbon nitride matrix (denoted as Mo-Pt/CN) is designed for achieving boosted photocatalytic H2 production. Benefiting from the synergy of dual cocatalysts, Mo-Pt/CN photocatalyst delivers an impressive H2 evolution rate of 11.26 mmol center dot g- 1 center dot h- 1, which is 6.43 and 25.02 times higher than those of the Pt/ CN and Mo/CN photocatalyst, respectively. Systematic experiments combining with theoretical calculations reveal that the enhanced photocatalytic activity attributes to the synergy of asymmetrically geometrical deployment between MoP and Pt NCs dual cocatalysts, which induces asymmetric charge distributions and tailors the d-band center to optimize the adsorption behaviors of H2O* and H* intermediates on Mo-Pt dual sites, respectively, thus facilitating H2O* activation-dissociation and simultaneously achieving thermoneutral H* adsorption free energy (Delta GH*) for speeding up the H2 evolution kinetics.
卷号:498
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是否译文:否