Journal
SMALL
Volume 19, Issue 21, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202208117
Keywords
heteroatom-refilling; H-2 evolution; internal electric field; nitrogen vacancies; photocatalysis
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Traditional defect engineering and doping strategies are commonly used to enhance H-2 evolution, but their uncontrollability may not always result in efficient activity. This study presents a defect-induced heteroatom refilling strategy to synthesize carbon nitrides with controlled heteroatom introduction on efficient N1 sites. The refilling of B, P, and S sites shows stronger H2O adsorption and dissociation capacity compared to traditional doping, making it an optimal pathway for H-2 production. The heteroatom-refilled catalysts exhibit a high internal electric field strength, enabling fast electron transfer and achieving a hydrogen production rate of up to 20.9 mmol g(-1) h(-1). This work provides insights into controlled defect engineering of photocatalysts and offers a universal modification strategy for heteroatoms and co-catalyst systems in H-2 production.
Traditional defect engineering and doping strategies are considered effective means for improving H-2 evolution, but the uncontrollability of the modification process does not always lead to efficient activity. A defect-induced heteroatom refilling strategy is used here to synthesize heteroatoms introduced carbon nitride by precisely controlling the introduction sites on efficient N1 sites. Density functional theory calculations show that the refilling of B, P, and S sites have stronger H2O adsorption and dissociation capacity than traditional doping, which makes it an optimal H-2 production path. The large internal electric field strength of heteroatom-refilled catalysts leads to fast electron transfer and the hydrogen production of the best sample is up to 20.9 mmol g(-1) h(-1). This work provides a reliable and clear insight into controlled defect engineering of photocatalysts and a universal modification strategy for typical heteroatom and co-catalyst systems for H-2 production.
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