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Jingshu Yuan, Yao Zhang, Xiaoyan Zhang, Junjie Zhang, and Shen’gen Zhang, N-doped graphene quantum dot-decorated N-TiO2/P-doped porous hollow g-C3N4 nanotube composite photocatalysts for antibiotic photodegradation and H2 production, Int. J. Miner. Metall. Mater., 31(2024), No. 1, pp.165-178. https://dx.doi.org/10.1007/s12613-023-2678-6
Jingshu Yuan, Yao Zhang, Xiaoyan Zhang, Junjie Zhang, and Shen’gen Zhang, N-doped graphene quantum dot-decorated N-TiO2/P-doped porous hollow g-C3N4 nanotube composite photocatalysts for antibiotic photodegradation and H2 production, Int. J. Miner. Metall. Mater., 31(2024), No. 1, pp.165-178. https://dx.doi.org/10.1007/s12613-023-2678-6
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N掺杂石墨烯量子点修饰的N-TiO2/P掺杂多孔g-C3N4纳米管复合光催化剂用于降解抗生素和产氢

摘要: 仅响应紫外光(~3.2 eV)和光生电荷复合率高是纯TiO2的两个主要缺点。本文联合N掺杂石墨烯量子点(N-GQDs)、形貌调控和异质结构筑合成了N-GQD/N掺杂TiO2/P掺杂多孔中空g-C3N4纳米管(PCN)复合光催化剂(简称G-TPCN)。最佳样品(掺杂0.1wt% N-GQD的G-TPCN,记为0.1%G-TPCN)的光吸收性能显著增强,归因于P/N元素掺杂改变带隙、管状结构改善光捕集以及N-GQDs的上转换效应。此外,0.1%G-TPCN内部电荷分离和转移能力显著提高,其载流子浓度分别是N-TiO2、PCN和N-TiO2/PCN (TPCN-1)的3.7倍、2.3倍和1.9倍。这一结果归因于N-TiO2与PCN之间形成的Z型异质结、N-GQDs优异的电子传导能力及多孔纳米管结构缩短电荷传输距离。与N-TiO2、PCN和TPCN-1相比,0.1%G-TPCN在可见光下产H2活性分别提高了12.4、2.3和1.4倍,环丙沙星(CIP)降解率分别提高了7.9、5.7和2.9倍。优化的性能得益于出色的光响应能力及提高的载流子分离和迁移效率。最后,提出了0.1%G-TPCN的光催化机理及CIP可能的五种降解途径。本研究阐明了多种改性策略协同提高0.1%G-TPCN光催化性能的机制,为合理设计新型光催化剂用于环境修复和太阳能转换提供了一种潜在方法。

 

N-doped graphene quantum dot-decorated N-TiO2/P-doped porous hollow g-C3N4 nanotube composite photocatalysts for antibiotic photodegradation and H2 production

Abstract: Exclusive responsiveness to ultraviolet light (~3.2 eV) and high photogenerated charge recombination rate are the two primary drawbacks of pure TiO2. We combined N-doped graphene quantum dots (N-GQDs), morphology regulation, and heterojunction construction strategies to synthesize N-GQD/N-doped TiO2/P-doped porous hollow g-C3N4 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 of 0.1%G-TPCN are dramatically boosted, and its carrier concentration is 3.7, 2.3, and 1.9 times that of N-TiO2, PCN, and N-TiO2/PCN (TPCN-1), respectively. This phenomenon is attributed to the formation of Z-scheme heterojunction between N-TiO2 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-TiO2, PCNs, and TPCN-1, the H2 production activity of 0.1%G-TPCN under visible light is enhanced by 12.4, 2.3, and 1.4 times, 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.

 

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