Towards highly-selective H2O2 photosynthesis:In-plane highly ordered carbon nitride nanorods with Ba atoms implantation
Graphitic carbon nitride(g-C3N4)shows great potential in photocatalytic H2O2 production.However,challenges arise from its low in-plane crystallinity and selectivity in two-electron oxygen reduction reaction(2e--ORR),greatly limiting its H2O2 photosynthesis efficiency.Herein,we develop an ingenious strategy to simultaneously increase the in-plane crystallinity and induce the highly-selective 2e--ORR by rationally designing barium(Ba)atom-implanted in-plane highly ordered g-C3N4 nanorods.The approach involves controllable synthesis of in-plane high crystallinity g-C3N4 nanorods with Ba implantation(BI-CN)using a BaCl2-mediated in-plane polymerization strategy.The unique Ba-N interaction induces the oriented polymerization of 3-s-triazine units to form well-arranged in-plane structures.Experimental and theoretical calculations clarify that the implanted Ba atoms function as positive charge centers,resulting in a Pauling-type O2 adsorption configuration.This minimizes O-O bond breaking energy,thus suppressing the four-electron oxygen reduction reaction(4e--ORR)and facilitating a highly-selective 2e--ORR pathway for efficient photocatalytic H2O2 production.Consequently,the optimized BI-CN3 photocatalyst exhibits an outstanding H2O2 production rate of as high as 353 pmol L-1 h-1,surpassing the pristine g-C3N4 by 6.1 times.This study concurrently optimizes the in-plane crystallinity and O2 adsorption sites of g-C3N4 photocatalysts for highly-selective H2O2 production,providing innovative insights for designing efficient photocatalysts with diverse applications.
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