Defects enriched carbon nitride sponge with high surface area for enhanced photocatalytic hydrogen evolution

被引:1
作者
Wu, Ming [1 ]
Chen, Libo [1 ]
Sheng, Ying [1 ]
Song, Lizhi [2 ]
Zhou, Hu [1 ]
Jian, Jian [1 ]
Huang, Tiefan [1 ]
Liu, Botian [3 ]
Li, Xiaoning [4 ]
机构
[1] Hunan Univ Sci & Technol, Funct Film Mat Engn Res Ctr Hunan Prov, Sch Chem & Chem Engn,Hunan Prov Key Lab Adv Mat Ne, Key Lab Theoret Organ Chem & Funct Mol Minist Educ, Xiangtan 411201, Peoples R China
[2] Hunan Univ Sci & Technol, Sch Mat Sci & Engn, Xiangtan 411201, Peoples R China
[3] Guilin Univ Technol, Dept Chem & Biol Engn, Guangxi Key Lab Electrochem & Magneto Chem Funct M, Guilin 541004, Peoples R China
[4] RMIT Univ, Sch Sci, Melbourne, Vic 3000, Australia
基金
澳大利亚研究理事会; 中国国家自然科学基金;
关键词
Carbon nitride; Photocatalysis; Hydrogen production; Defects; Porous; G-C3N4; WATER; SEMICONDUCTOR;
D O I
10.1016/j.jcis.2025.02.130
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The limited efficiency of traditional photocatalysts necessitates innovative solutions for sustainable hydrogen production. In this study, a three-dimensional (3D) sponge-like porous carbon nitride (SCN-x) was successfully synthesized using a novel method involving the removal of unstable organic frameworks. The resulting SCN-x exhibits a highly interconnected network structure and significantly higher surface area (116.5 m2/g), compared to normal pure carbon nitride (PCN). Furthermore, this method introduces significant defects into SCN-x, such as additional foreign oxygen atoms, which not only modulate its band structure but also provide more active sites at the defects. These features increase the number of photo-induced electron-hole pairs due to enhanced light absorption, and suppresses their recombination by enabling them to efficiently participate in the reaction with increased number of active sites. As a result, compared to PCN, the optimal SCN-0.5 sample exhibits 86.6 times higher photocatalytic hydrogen production rate under visible light irradiation, along with excellent stability and a high apparent quantum yield (AQY) of 5.8 % under 420 nm illumination. Furthermore, with additional calcination under air, the 2SCN-0.5 sample delivers a record-high hydrogen evolution rate of 1663.5 mu mol center dot h-1 center dot g- 1 under natural sunlight irradiation. This work presents a novel method for preparing a metal-free photocatalyst by introducing significant defects and a high surface area, enabling efficient large-scale hydrogen production under natural sunlight.
引用
收藏
页码:59 / 66
页数:8
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