Abstract
Photocatalytic oxygen reduction reaction (ORR) offers a promising pathway for sustainable hydrogen peroxide (H2O2) production but faces challenges in developing catalysts with good ORR selectivity. Herein, we report that tailoring O2 adsorption on non-metallic active sites can optimize ORR selectivity. This concept is demonstrated on three carbon nitrides with different atomic configurations: polymeric carbon nitride (PCN), lithium-poly triazine imide (Li-PTI), and sodium-poly heptazine imide (Na-PHI). Na-PHI emerges as a strong candidate for H2O2 production due to the end-on adsorption mode and suitable adsorption strength with O2. Synthesized Na-PHI, PCN, and Li-PTI are characterized, with Na-PHI showing superior light absorption, charge carrier separation, and remarkable selectivity (92 %) for two-electron ORR. Consequently, Na-PHI achieves a high H2O2 generation rate of 3.48 mmol g−1 h−1, surpassing Li-PTI and PCN by 9.2 and 33 times, respectively. This study underscores the importance of O2 adsorption on non-metallic active sites for selective photocatalytic H2O2 generation.
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