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Sub-5 nm Ultra-Fine FeP Nanodots as Efficient Co-Catalysts Modified Porous g-C <sub/>3</sub> N <sub/>4</sub> for Precious-Metal-Free Photocatalytic Hydrogen Evolution under Visible Light

DOI:10.1021/acsami.8b20958 期刊:ACS Applied Materials & Interfaces 出版年份:2019 更新时间:2025-09-23 15:23:52
摘要: Sub-5 nm ultra-fine iron phosphide (FeP) nano-dots-modified porous graphitic carbon nitride (g-C3N4) heterojunction nanostructures are successfully prepared through the gas-phase phosphorization of Fe3O4/g-C3N4 nanocomposites. The incorporation of zero-dimensional (0D) ultra-small FeP nanodots co-catalysts not only effectively facilitate charge separation but also serve as reaction active sites for hydrogen (H2) evolution. Herein, the strongly coupled FeP/g-C3N4 hybrid systems are employed as precious-metal-free photocatalysts for H2 production under visible-light irradiation. The optimized FeP/g-C3N4 sample displays a maximum H2 evolution rate of 177.9 μmol h?1 g?1 with the apparent quantum yield of 1.57% at 420 nm. Furthermore, the mechanism of photocatalytic H2 evolution using 0D/2D FeP/g-C3N4 heterojunction interfaces is systematically corroborated by steady-state photoluminescence (PL), time-resolved PL spectroscopy, and photoelectrochemical results. Additionally, an increased donor density in FeP/g-C3N4 is evidenced from the Mott-Schottky analysis in comparison with that of parent g-C3N4, signifying the enhancement of electrical conductivity and charge transport owing to the emerging role of FeP. The density functional theory calculations reveal that the FeP/g-C3N4 hybrids could act as a promising catalyst for the H2 evolution reaction. Overall, this work not only paves a new path in the engineering of monodispersed FeP-decorated g-C3N4 0D/2D robust nanoarchitectures but also elucidates potential insights for the utilization of noble-metal-free FeP nanodots as remarkable co-catalysts for superior photocatalytic H2 evolution.
作者: Deqian Zeng,Yuanzhi Chen,Ting Zhou,Yi-An Zhu,Wee-Jun Ong,Xiaoguang Duan,Mingda Wu,Wanjie Xu,Dong-Liang Peng
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To develop sub-5 nm ultra-fine FeP nanodots as efficient co-catalysts modified porous g-C3N4 for precious-metal-free photocatalytic hydrogen evolution under visible light.

The FeP/g-C3N4 heterojunctions exhibit enhanced photocatalytic H2 evolution due to efficient charge separation and migration at the interface, with an optimal rate of 177.9 μmol h?1 g?1 and AQY of 1.57% at 420 nm. The work demonstrates the potential of noble-metal-free co-catalysts for solar energy conversion, with insights from experimental and theoretical analyses suggesting future directions for material design and application in photocatalysis.

The study may have limitations in scalability of the synthesis method, potential aggregation of nanoparticles at higher loadings reducing activity, and the need for further optimization for industrial applications. The use of TEOA as a sacrificial agent may not be sustainable for large-scale H2 production.

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