硅酸盐学报

声化学改性钨酸锌光催化净化印染废水性能

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颜有缘 ¹ , 杜乐添 ¹ , 曹美茹 ¹ , 胡楠 ¹ , 叶丽娟 ¹ , 蒋建宏 ¹ , 邓斌 ¹ , 余长林 ² , 何洪波 ¹

硅酸盐学报 | 研究论文 2024,52(1): 133-142

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硅酸盐学报 |研究论文 2024 , 52 (1) : 133 -142

声化学改性钨酸锌光催化净化印染废水性能

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颜有缘¹, 杜乐添¹, 曹美茹¹, 胡楠¹, 叶丽娟¹, 蒋建宏¹, 邓斌¹, 余长林², 何洪波¹

作者信息

^1．湘南学院化学与环境科学学院，湖南郴州 423000

^2．广东石油化工学院化学工程学院，广东茂名 525000

通讯作者:

何洪波（1992—），男，博士，助理研究员。

作者简介:

颜有缘（2004—），女，本科生。

Improvement of Photocatalytic Performance of ZnWO₄ by Sonochemical Method for Purifying Dyeing Wastewater

Youyuan YAN¹, Letian DU¹, Meiru CAO¹, Nan HU¹, Lijuan YE¹, Jianhong JIANG¹, Bin DENG¹, Changlin YU², Hongbo HE¹

Affiliations

^1.School of Chemistry and Environmental Sciences, Xiangnan University, Chenzhou 423000, Hunan, China

^2.School of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming 525000, Guangdong, China

Corresponding Author:

HE Hongbo (1992-), male, Ph.D., Assistant Professor. E-mail: hehb5@mail2.sysu.edu.cn

YAN Youyuan (2004-), female, Undergraduate. E-mail: 2844585659@qq.com

出版时间: 2024-01-20 doi: 10.14062/j.issn.0454-5648.20230488

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摘要

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光催化技术是当前高效、理想的环境污染治理技术之一。钨酸锌作为最具有潜力的金属钨酸盐光催化剂之一，具有很大的研究价值。目前改性钨酸锌光催化性能的方法主要聚焦于材料复合和掺杂等方面，而声化学改性钨酸锌光催化活性相关的研究鲜有报道。以声化学辅助水热法成功制备了具有氧空位缺陷的钨酸锌纳米材料，并通过X射线衍射、N₂吸附-脱附曲线、扫描电子显微镜、红外光谱、紫外-可见漫反射光谱、电化学阻抗谱等技术表征了其物理化学性质；以亚甲基蓝染料废水为目标污染物，探究了声化学处理对钨酸锌光催化活性的影响。结果表明：超声波处理可以诱导钨酸锌氧空位缺陷的形成，从而优化电子结构，暴露出更多的活性位点，拓宽光响应范围，提高光生载流子的转移效率，从而显著提高钨酸锌对印染废水的光催化降解性能。

关键词

钨酸锌 / 光催化 / 声化学 / 亚甲基蓝

Abstract

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Introduction

Dyeing wastewater is one of environmental pollutions, having a serious threat to the environment and human-being health. Therefore, the purification of dyeing wastewater becomes a challenge. Among various methods for treating dyeing wastewater, photocatalysis is developed as an efficient environmental pollution control technology due to its mild reaction conditions, sustainable driving energy sources, and no secondary pollution after the reaction. Zinc tungstate (ZnWO₄) as a semiconductor photocatalyst material with stable physical and chemical properties has a promising application potential in photocatalytic removal of environmental pollutants. However, ZnWO₄ has a wide bandgap and a low migration efficiency of carriers, resulting in unsatisfactory photocatalytic intrinsic activity. Therefore, researchers attempted to optimize the photocatalytic performance of ZnWO₄ via regulating its morphology, size and crystallinity. Sonochemical method is a highly concerned method for synthesizing nanomaterials. Under ultrasonic cavitation conditions, the physical and chemical environment of the reaction system will undergo significant changes, i.e., the instantaneous generation of high temperature, high pressure, and strong shock waves, which are beneficial for strengthening the fracture of chemical bonds and the generation of new chemical bonds, thereby regulating the morphology and structure of material. In this work, ZnWO₄ with oxygen defects nanomaterials were prepared by a sonochemistry-assisted hydrothermal method, and the influence of sonochemical treatment time on the photocatalytic activity of ZnWO₄ was investigated as methylene blue was used as a target pollutant.

Methods

ZnWO₄ with oxygen defects nanomaterials were prepared by a sonochemistry-assisted hydrothermal method. In the preparation, 0.297 g Zn(NO₃)₃·6H₂O was dissolved in 8 mL distilled water under constant stirring, to obtain solution A. Also, 7 mL distilled water containing 0.392 g Na₂WO₄·2H₂O was added in dropwise to solution A and mixed by stirring for 30 min. Afterwards, LC-UP-400 ultrasonic signal connected Φ10 luffing rod (selecting ultrasonic power was 50%, ultrasonic treatment for 2 s, and stay for 2 s) was used to irradiate the white suspension for 1h, and then the suspensions were put into Teflon-lined autoclave, sealed and maintained at 140 ℃ for 20 h. After cooling to room temperature, the product was washed with distilled water and ethanol for several times. The final products were obtained after drying at 60 ℃ for 12 h. The samples of ZnWO₄ nanomaterials treated at different ultrasonic treatment time (X min) were named as ZnWO₄-X.

Results and discussion

The photocatalytic activity of as-prepared samples was evaluated by MB photocatalytic removal in 10 mg/L of MB dyeing wastewater. Herein, MB dyeing wastewater under light illumination without the addition of photocatalysts as a blank test for comparison, having an unsatisfactory photoreduction effect. After 40 min of illumination, ZnWO₄ has a weak photocatalytic activity for MB photodegradation, i.e., 52% of MB is photocatalytically degradated by pure ZnWO₄. However, the induction of oxygen vacancy defects results in an enhanced photocatalytic performance for MB removal over ZnWO₄-5 min. The optimized ZnWO₄-5 min displays a superior photocatalytic activity for MB removal, which can remove 95.0% of MB after 40 min of illumination. The kinetic of MB photodegradation was further analyzed by plotting the -ln(c/c₀) as a function of irradiation time. The calculated rate constant k of ZnWO₄-5min is 0.067 min^-1, which is 4.5 times greater than that of ZnWO₄. The reusability of ZnWO₄-5min was investigated by performing 5 consecutive cycles for MB photodegradation. The results show that the photoreduction efficiency maintains at a high level (i.e., >90%) after five cycling experiments, indicating the superior stability and huge potential value of ZnWO₄-5 min for the treatment of dyeing wastewater. The oxygen vacancy defects induced by ultrasound cause the lattice contraction within ZnWO₄, which is beneficial for optimizing electronic structure, exposing more catalytic active sites, broadening the photocatalytic response range, and improving the migration efficiency of photogenerated carriers, thereby significantly enhancing the photocatalytic degradation performance of ZnWO₄ in dyeing wastewater.

Conclusions

ZnWO₄ with oxygen defects nanomaterials were prepared by a sonochemistry-assisted hydrothermal method, and the influence of sonochemical treatment time on the photocatalytic activity of ZnWO₄ was investigated when MB was used as a target pollutant. The results showed that sonochemical treatment could induce the formation of oxygen vacancy defects in ZnWO₄ nanoparticles, thereby optimizing electronic structure, exposing more active sites, broadening the light response range and improving the transfer efficiency of photogenerated carriers, thus enhancing the photocatalytic degradation performance of ZnWO₄ for dyeing wastewater. The optimized ZnWO₄-5 min displayed a superior photocatalytic activity for MB removal, which removed 95.0% of MB after 40 min of illumination. The calculated rate constant k of ZnWO₄-5 min was 0.067 min^-1, which was 4.5 times greater than that of ZnWO₄. Furthermore, ZnWO₄-5min displayed a superior photocatalytic stability, and the photoreduction efficiency maintained at a high level (>90%) after five cycling experiments. This indicated that sonochemically-induced oxygen vacancy defects be an effective method to improve the photocatalytic performance of ZnWO₄. This work can provide some ideas for the preparation of high-performance semiconductor photocatalytic materials for the treatment of dyeing wastewater.

Key words

zinc tungstate / photocatalysis / sonochemistry / methylene blue

引用本文

颜有缘, 杜乐添, 曹美茹, 胡楠, 叶丽娟, 蒋建宏, 邓斌, 余长林, 何洪波. 声化学改性钨酸锌光催化净化印染废水性能. 硅酸盐学报, 2024 , 52 (1) : 133 -142 . DOI: 10.14062/j.issn.0454-5648.20230488

Youyuan YAN, Letian DU, Meiru CAO, Nan HU, Lijuan YE, Jianhong JIANG, Bin DENG, Changlin YU, Hongbo HE. Improvement of Photocatalytic Performance of ZnWO₄ by Sonochemical Method for Purifying Dyeing Wastewater[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (1) : 133 -142 . DOI: 10.14062/j.issn.0454-5648.20230488

基金

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国家自然科学基金项目(42020619)
湖南省自然科学基金项目(2023JJ40608)
湖南省教育厅优秀青年项目(22B0813)
湘南学院校级科研项目青年项目(2022XJ09)
湘南学院开放性实验项目(校发〔2023〕18号NO13)

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2024年第52卷第1期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230488

接收时间：2023-07-11
首发时间：2026-10-22
出版时间：2024-01-20

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收稿日期：2023-07-11
修回日期：2023-08-03

基金

国家自然科学基金项目(42020619)

湖南省自然科学基金项目(2023JJ40608)

湖南省教育厅优秀青年项目(22B0813)

湘南学院校级科研项目青年项目(2022XJ09)

湘南学院开放性实验项目(校发〔2023〕18号NO13)

作者信息

^1．湘南学院化学与环境科学学院，湖南郴州 423000

^2．广东石油化工学院化学工程学院，广东茂名 525000

通讯作者:

何洪波（1992—），男，博士，助理研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230488

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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