Photocatalytic H2O2 production over boron-doped g-C3N4 containing coordinatively unsaturated FeOOH sites and CoOx clusters

Ping Liu, Teng Liang, Yutong Li, Ziqing Zhang (), Zhuo Li, Ji Bian () and Liqiang Jing ()
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Ping Liu: Heilongjiang University
Teng Liang: Heilongjiang University
Yutong Li: Heilongjiang University
Ziqing Zhang: Heilongjiang University
Zhuo Li: Heilongjiang University
Ji Bian: Heilongjiang University
Liqiang Jing: Heilongjiang University

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Graphitic carbon nitride (g-C3N4) has gained increasing attention in artificial photosynthesis of H2O2, yet its performance is hindered by sluggish oxygen reduction reaction (ORR) kinetics and short excited-state electron lifetimes. Here we show a B-doped g-C3N4 (BCN) tailored with coordinatively unsaturated FeOOH and CoOx clusters for H2O2 photosynthesis from water and oxygen without sacrificial agents. The optimal material delivers a 30-fold activity enhancement compared with g-C3N4 under visible light, with a solar-to-chemical conversion efficiency of 0.75%, ranking among the forefront of reported g-C3N4-based photocatalysts. Additionally, an electron transfer efficiency reaches 34.1% for the oxygen reduction reaction as revealed by in situ microsecond transient absorption spectroscopy. Experimental and theoretical results reveal that CoOx initiates hole–water oxidation and prolongs the electron lifetime, whereas FeOOH accepts electrons and promotes oxygen activation. Intriguingly, the key to the direct one-step two-electron reaction pathway for H2O2 production lies in coordinatively unsaturated FeOOH to adjust the Pauling-type adsorption configuration of O2 to stabilize peroxide species and restrain the formation of superoxide radicals.

Date: 2024
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DOI: 10.1038/s41467-024-53482-0

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