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n-doped graphene quantum dot-decorated n-TiO2/P-doped porous hollow g-C_(3)n_(4) nanotube composite photocatalysts for antibiotic photodegradation and H2 production

引用

International Journal of Minerals,Metallurgy and Materials 2024年第1期31卷 165-178页

作者： Jingshu Yuan Yao Zhang Xiaoyan Zhang Junjie Zhang Shen’gen Zhang Institute for Advanced Materials and Technology University of Science and Technology BeijingBeijing 100083China Xi’an Fanyi University Xi’an 710105China Shunde Graduate School of University of Science and Technology Beijing Foshan 528399China State Key Laboratory of Lunar and Planetary Sciences Macao University of Science and TechnologyMacao SAR 820000China

Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO_(2). We combined n-doped graphene quantum dots (n-GQDs), morphology regulation, and heterojunction construction strategies to synthesize n-GQD/n-doped TiO_(2)/P-doped porous hollow g-C_(3)n_(4) nanotube (PCn) composite photocatalysts (denoted as G-TPCn). The optimal sample (G-TPCn doped with 0.1wt% n-GQD, denoted as 0.1% G-TPCn) exhibits significantly enhanced photoabsorption, which is attributed to the change in bandgap caused by elemental doping (P and n), the improved light-harvesting resulting from the tube structure, and the upconversion effect of n-GQDs. In addition, the internal charge separation and transfer capability of0.1% G-TPCn are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of n-TiO_(2), PCn, and n-TiO_(2)/PCn(TPCn-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between n-TiO_(2) and PCns, the excellent electron conduction ability of n-GQDs, and the short transfer distance caused by the porous nanotube structure. Compared with those of n-TiO_(2), PCns, and TPCn-1, the H2 production activity of 0.1%G-TPCn under visible light is enhanced by 12.4, 2.3, and 1.4times, respectively, and its ciprofloxacin (CIP) degradation rate is increased by 7.9, 5.7, and 2.9 times, respectively. The optimized performance benefits from excellent photoresponsiveness and improved carrier separation and migration efficiencies. Finally, the photocatalytic mechanism of 0.1% G-TPCn and five possible degradation pathways of CIP are proposed. This study clarifies the mechanism of multiple modification strategies to synergistically improve the photocatalytic performance of 0.1% G-TPCn and provides a potential strategy for rationally designing novel photocatalysts for environmental remediation and solar energy conversion.

关键词： n-doped TiO_(2) n-doped graphene quantum dots P-doped g-C_(3)n_(4) porous hollow nanotube heterojunction photocatalysis

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