A novel (Zr/Ce)UiO-66(NH2)@g-C3N4 Z-scheme heterojunction for boosted tetracycline photodegradation via effective electron transfer

被引:34
作者
Ren, Susu [1 ]
Dong, Jiahuan [1 ]
Duan, Xinyu [1 ]
Cao, Tingting [1 ,2 ]
Yu, Hongbin [1 ,2 ]
Lu, Ying [1 ,2 ]
Zhou, Dandan [1 ,2 ]
机构
[1] Northeast Normal Univ, Sch Environm, Engn Lab Water Pollut Control & Resources Recovery, Changchun 130117, Peoples R China
[2] Northeast Normal Univ, Sci & Technol Innovat Ctr Municipal Wastewater Tre, Changchun 130117, Peoples R China
基金
中国国家自然科学基金;
关键词
UiO-66; -NH2; modification; Ce substitution; Z-scheme heterojunction; Effective electron transfer; Tetracycline; METAL-ORGANIC FRAMEWORKS; PHOTOCATALYTIC DEGRADATION; G-C3N4; UIO-66; CONSTRUCTION;
D O I
10.1016/j.cej.2023.141884
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Aiming at efficient tetracycline (TC) removal, a co-modified (Zr/Ce)U(NH2) was elaborately designed and in-tegrated with thin-layered g-C3N4, forming a novel (Zr/Ce)U(NH2)@CN Z-scheme heterojunction. XRD, XPS, FTIR, ISI-XPS and other analysis cooperatively demonstrated that within this (Zr/Ce)U(NH2)@CN composite organic linkers H2BDC was successfully modified by -NH2, metal Zr in Zr-oxo cluster was partially substituted by Ce, Z-scheme heterojunction was formed by the close interaction between MOFs and g-C3N4, as well as the excellent thermal stability and large specific surface area were achieved. Since g-C3N4 could serve as carrier skeleton to improve the precursor dispersion, the (Zr/Ce)U(NH2) with reduced particle size grew densely on it. DRS, PL and TRPL characterization proved more photogenerated carriers with prolonged lifetime were gener-ated. As expected, (Zr/Ce)U(NH2)@CN composite exhibited high TC degradation rate, whose kinetic constant was 23.73 times greater than that of UiO-66, and 5.89 folds larger than that of CN, respectively. This enhanced photocatalytic performance was ascribed to the effective electron transfer regulated by MOFs unit, where the Zr/ Ce improved the electron transfer from photoexcited organic linkers to metal-oxo clusters, as well as the MOFs/g-C3N4 Z-scheme heterojunction strengthened interfacial photogenerated carriers transfer. center dot OH was the vital species responsible for TC removal using (Zr/Ce)U(NH2)@CN. Furthermore, intermediate products and degra-dation pathways were proposed based on HPLC-MS. The toxicity estimation indicated the comprehensive toxicity of TC was significantly alleviated by (Zr/Ce)U(NH2)@CN photocatalysis.
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页数:15
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