Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 324, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2022.122216
Keywords
Surface hydroxyl; Carbon nitride homojunction; Photocatalytic H 2 O 2 production; Spatial charge separation; Surface reaction kinetics
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This study presents a novel approach for scalable solar-driven H2O2 evolution from water, which achieves a 2.1% apparent quantum yield and a 4.5-fold improvement in H2O2 production. The strategy involves optimizing spatial charge separation and suppressing surface reaction kinetics.
Scalable solar-driven H2O2 evolution from water holds great promise for industrial applications. Efficient H2O2 generation relies on excellent spatial charge separation but simultaneously suffers from severe surface H2O2 backreaction, which becomes a bottleneck for scalable H2O2 evolution. Herein, a hydroxyl-induced carbon nitride (CN) homojunction coherently optimizes the bulk charge separation and suppresses surface backreaction. Surface hydroxyls provide extra electron accommodation bands for electron extraction from the bulk to the surface which are visually observed with oFM and rationalized by DFT calculations. 2e- oxygen reduction re-action (ORR) kinetic became more favorable than 4e- ORR in the presence of hydroxyl, showing suppressed H2O2 decomposition. This homojunction achieves a 4.5-fold improvement in H2O2 production compared to pristine CN, and an apparent quantum yield (AQY) of 2.1 % at 500 nm in water. This work demonstrates a strategy for coherently improving spatial charge separation and surface reaction kinetics, which is applicable for various photocatalytic reactions.
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