Abstract
Graphitic carbon nitride with nitrogen vacancies (NV-g-C3N4) as a photocatalyst has been studied in solar-driven energy conversion. However, expensive and rare noble metal co-catalysts such as Pt or Pd are required in the photocatalytic H2 evolution. Consequently, the exploration of low-cost and high-performance co-catalysts to replace expensive and rare noble metals has received more and more attention. Herein, a novel hierarchical porous NiO anchored on NV-g-C3N4 is successfully fabricated. The NV-g-C3N4/NiO photocatalysts exhibited outstanding H2 evolution rate under visible light irradiation in absence of noble metal co-catalysts. The optimized NV-g-C3N4/NiO (the mass ratio of NiO is ~ 1.7%) achieved a maximum H2 evolution rate of 170.60 μmol·g−1·h−1, exhibiting ∼ 8.3-fold enhancement as compared to that of NV-g-C3N4. NiO as co-catalyst provided more active sites for photocatalytic H2 evolution. Moreover, on the interface of NV-g-C3N4/NiO, an interface electric field is formed between NiO and host nitrogen-vacated g-C3N4, facilitating the transfer of the photogenerated electrons from NV-g-C3N4 to NiO co-catalyst, resulting in significantly promoted migration and separation efficiency of the photogenerated charge carriers.
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摘要
氮空位石墨相氮化碳 (NV-g-C3N4) 光催化剂由于可以利用太阳光进行能量转换, 因而受到广泛的研究. 然而, 在光催化制氢过程中, Pt和Pd等价格昂贵的贵金属助催化剂必不可少. 因此, 探索出价格低廉且性能优异的助催化剂来取代贵金属迫在眉睫. 在本文中, 我们成功制备了一种新型分级多孔NiO修饰NV-g-C3N4的NV-g-C3N4/NiO复合光催化剂. 实验结果表明, 在不借助贵金属助催化剂的情况, NV-g-C3N4/NiO光催化剂表现出增强的可见光光催化制氢性能. 当NiO的质量分率约为1.7%时, NV-g-C3N4/NiO具有最好的制氢活性, 制氢速率为170.60·μmol·g-1·h-1, 是NV-g-C3N4的8.3倍. 这可能归因于分级多孔NiO助催化剂在光催化制氢反应过程中提供了更多的活性位点. 同时, 在NiO和NV-g-C3N4界面形成的内建电场促使光生电子从NV-g-C3N4的导带转移至NiO的表面, 导致光生载流子的迁移和分离效率显著提升.
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Acknowledgements
This study was financially supported by the National Natural Science Foundation of China (Nos. 22075072 and 52003079) and Hubei Provincial Natural Science Foundation of China (No. 2019CFB568).
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Liao, YW., Yang, J., Wang, GH. et al. Hierarchical porous NiO as a noble-metal-free cocatalyst for enhanced photocatalytic H2 production of nitrogen-deficient g-C3N4. Rare Met. 41, 396–405 (2022). https://doi.org/10.1007/s12598-021-01784-3
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DOI: https://doi.org/10.1007/s12598-021-01784-3