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Constructing Z-scheme β-Bi2O3/ZrO2 heterojunctions with 3D mesoporous SiO2 nanospheres for efficient antibiotic remediation via synergistic adsorption and photocatalysis

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Abstract

A series of Z-scheme β-Bi2O3/ZrO2 heterojunction composites containing three-dimensional (3D) mesoporous silica nanospheres (MSNs) were synthesized as efficient catalysts for antibiotic remediation. The obtained MSN/β-Bi2O3/ZrO2 ternary composites possess novel lamellar cross structure, which is well constructed by β-Bi2O3 nanosheets, 3D MSNs, and ZrO2 nanoparticles. The optimal sample BZS-2 (Bi: Zr: Si = 1: 0.4: 0.33) shows an adsorptive-photocatalytic removal efficiency of 92.7% towards levofloxacin (LVF) and a total organic carbon (TOC) removal efficiency of 60.0% under simulated solar light irradiation for 100 min. BZS-2 can also remove 90.1% and 91.2% of tetracycline hydrochloride (TC) and oxytetracycline hydrochloride (OTC), respectively, and the maximum adsorption capacity of TC over BZS-2 is almost 10 times that of β-Bi2O3. The improvement of photocatalytic activity can be mainly attributed to the enhanced visible-light adsorption capacity and more efficient separation of photogenerated electron–hole pairs. A possible Z-scheme photocatalytic mechanism of β-Bi2O3/ZrO2 heterojunctions based on valence band offset (ΔEVBO) and conduction band offset (ΔECBO) is proposed. This study provides an efficient way to construct novel mesoporous ternary photocatalyst with increased accessible surface area and active sites for treatment of antibiotics by synergistic adsorption and photocatalysis.

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摘要

本文合成了一系列Z型β-Bi2O3/ZrO2异质结和3D介孔二氧化硅纳米球(MSNs)的复合光催化剂, 用于高效去除废水中的抗生素. 所合成的MSN/β-Bi2O3/ZrO2三元复合材料由β-Bi2O3纳米片, 3D MSNs和ZrO2纳米颗粒组成, 具有新颖的层状交叉结构. 在模拟太阳光照射100 min时, 最优化样品BZS-2 (Bi: Zr: Si 摩尔比为 1: 0.4:0.33)对废水中左氧氟沙星(LVF)的吸附-光催化协同去除率为92.7%, 并且对TOC的去除率可达60%。 BZS-2对盐酸四环素(TC)和盐酸土霉素(OTC)的去除率分别为90.1%和91.2%, 其对TC的最大吸附量几乎是β-Bi2O3的10倍。 光催化活性的提高主要是由于可见光吸附吸收能力的增强和光致电子-空穴对分离效率的提高。 基于价带偏移(ΔEVBO)和导带偏移(ΔECBO), 提出了Z型β-Bi2O3/ZrO2异质结光催化机理。本研究为构建具有较大的比表面积和较高活性的新型介孔三元光催化剂提供了一种有效的途径, 所制备的催化剂可用于吸附-光催化协同高效处理抗生素废水。

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Acknowledgments

This work was financially supported by National Natural Science Foundation of China (Nos. 21962006, 21607064 and 21707055), the Youth Key Project of Natural Science Foundation of Jiangxi Province (Nos. 20192ACBL20014 and 20192ACBL21011), the Natural Science Foundation of Jiangxi Province (Nos. 20181BAB203018 and 20181BAB213010) and Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology.

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  1. Chong Xu and Qin Zhou contributed equally to this work.

Authors and Affiliations

  1. Faculty of Materials, Metallurgical and Chemistry, Jiangxi University of Science and Technology, Ganzhou, 341000, China

    Chong Xu, Qin Zhou, Wei-Ya Huang & Kai Yang

  2. School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou, 225009, China

    Yong-Cai Zhang

  3. College of Rare Earths, Jiangxi University of Science and Technology, Ganzhou, 341000, China

    Tong-Xiang Liang

  4. School of Chemistry and Chemical Engineering/Institute of Clean Energy and Materials, Guangzhou Key Laboratory for Clean Energy and Materials/Huangpu Hydrogen Innovation Center, Guangzhou University, Guangzhou, 510006, China

    Zhao-Qing Liu

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  1. Chong Xu
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Xu, C., Zhou, Q., Huang, WY. et al. Constructing Z-scheme β-Bi2O3/ZrO2 heterojunctions with 3D mesoporous SiO2 nanospheres for efficient antibiotic remediation via synergistic adsorption and photocatalysis. Rare Met. 41, 2094–2107 (2022). https://doi.org/10.1007/s12598-021-01897-9

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