Designing flexible TiO2/SrTiO3/BiOBr recyclable fiber membrane with spatial dual oxidation sites for photocatalytic uranium extraction under visible light

IF 13.3 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Zhenyu Cai, Jingjing Wang, Hao Fu, Yuehua Pan, Mingyue Ma, Yuqian Zhong, Yuxiang Deng, Yuezhou Wei, Toyohisa Fujita, Xinpeng Wang
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Abstract

The utilization of nuclear energy generates a substantial volume of wastewater containing uranium, posing a significant threat to both aquatic ecosystems and human health. The current photocatalytic materials utilized for uranium extraction commonly exhibit insufficient redox capabilities, inefficient separation of photogenerated carriers, and challenging recovery. Therefore, recyclable TiO2/SrTiO3/BiOBr (TSB) dual Z-scheme heterojunction fiber membrane materials with dual oxidation sites were successfully synthesized, with advantages of rapid carrier separation and transfer and a broad photo-response range of the dual Z-scheme heterojunctions. Due to the presence of dual oxidation sites, TSB exhibited an exceptional uranium extraction performance, achieving a remarkable 98.9 % extraction rate without the need for sacrificial agents, which was 2.48, 1.79, and 3.34 times of those of ordinary TiO2, SrTiO3, and BiOBr, respectively. The extraction rate of uranium from TSB was 85 % after five cycles. Optical and photoelectric tests revealed that TSB reduced the bandgap width by 0.25 eV compared to that of TiO2, enhanced the fluorescence lifetime by 1.3 ns, lowered the electrical resistance, and higher optical current density, confirming the effective charge transport at the catalyst interfaces. The charge transfer routes in the TSB dual Z-scheme were confirmed by X-ray photoelectron spectroscopy and density functional theory. The potent oxidizing ·OH generated by TSB played a crucial role in facilitating the conversion of U(VI) into insoluble (UO2)O2·2H2O. In conclusion, this work provides a novel strategy for the design of dual Z-scheme heterojunctions and offers a new method for practical and recoverable uranium extraction.

Abstract Image

设计具有空间双氧化位点的柔性 TiO2/SrTiO3/BiOBr 可回收纤维膜,用于可见光下的光催化铀提取
核能的利用会产生大量含铀废水,对水生生态系统和人类健康构成严重威胁。目前用于铀提取的光催化材料普遍存在氧化还原能力不足、光生载体分离效率低以及回收难度大等问题。因此,我们成功合成了具有双氧化位点的可回收 TiO2/SrTiO3/BiOBr (TSB) 双 Z 型异质结纤维膜材料,该材料具有载流子快速分离和转移以及双 Z 型异质结光响应范围广的优点。由于双氧化位点的存在,TSB 表现出了优异的铀萃取性能,在不需要牺牲剂的情况下,萃取率达到了惊人的 98.9%,分别是普通 TiO2、SrTiO3 和 BiOBr 的 2.48 倍、1.79 倍和 3.34 倍。经过五个循环后,TSB 中铀的提取率为 85%。光学和光电测试表明,与 TiO2 相比,TSB 的带隙宽度减小了 0.25 eV,荧光寿命延长了 1.3 ns,电阻降低,光电流密度增大,证实了催化剂界面上有效的电荷传输。X 射线光电子能谱和密度泛函理论证实了 TSB 双 Z 型结构中的电荷转移途径。TSB 产生的强氧化性 -OH 在促进 U(VI) 转化为不溶性 (UO2)O2-2H2O 的过程中发挥了关键作用。总之,这项工作为设计双 Z 型异质结提供了一种新策略,并为实用的可回收铀提取提供了一种新方法。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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