硅酸盐学报

Fe₃O₄/CoS/g-C₃N₄催化剂的制备及降解罗丹明B

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郑佳红 , 黄植

硅酸盐学报 | 研究论文 2024,52(12): 3748-3760

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硅酸盐学报 |研究论文 2024 , 52 (12) : 3748 -3760

Fe₃O₄/CoS/g-C₃N₄催化剂的制备及降解罗丹明B

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郑佳红, 黄植

作者信息

长安大学材料科学与工程学院，西安 710021

作者简介:

郑佳红（1983—），女，博士，副教授。

Degradation of Rhodamine B by Using Fe₃O₄/CoS/g-C₃N₄ Catalyst

Jiahong ZHENG, Zhi HUANG

Affiliations

School of Materials Science and Engineering, Chang'an University, Xi'an 710061, China

ZHENG Jiahong (1983-), female, Ph.D, Associate Professor. E-mail: jhzheng@chd.edu.cn

出版时间: 2024-12-20 doi: 10.14062/j.issn.0454-5648.20240461

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摘要

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过一硫酸盐（PMS）的非均相活化技术，在废水处理领域表现出高效性。通过水热法成功制备了一种新型的复合催化剂Fe₃O₄/CoS/g-C₃N₄，证实该催化剂具备光催化和PMS活化的双重功能，并应用于罗丹明B（RhB）的降解实验中。催化剂中的Co离子通过氧化还原循环作用，与PMS自分解产生的自由基协同作用，有效保持了Fe₃O₄/CoS/g-C₃N₄的催化降解性能，并在光照条件下进一步提升了降解效率。实验结果表明，在PMS/可见光的催化体系中，Fe₃O₄/CoS/g-C₃N₄在5 min内对10 mg/L RhB溶液的降解效率达97.5%，并且该催化剂具有较宽的pH适应性，在pH值为3至11的范围内均表现出良好的降解性能。另外，由于引入Fe₃O₄，让该催化剂还具备优异的磁性回收特性，这使得它在实际应用具有很大的应用潜力。

关键词

普鲁士蓝类似物 / 罗丹明B / 四氧化三铁 / 硫化钴 / 石墨相氮化碳

Abstract

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Introduction

Rhodamine B (RhB) as a widely used organic dye often appears in industrial wastewater, posing a serious threat to human health. In response to this problem, an advanced persulfate oxidation technology can effectively remove organic pollutants by virtue of its highly activated free radicals, having a great potential for application in the field of wastewater treatment due to its significant advantages of easy operation and wide pH range. In the Fenton system, transition group metals show superior performance, especially the cobalt(II)/potassium peroxymonosulfate (PMS) system, whose activation performance is particularly outstanding, and can efficiently degrade harmful substances in wastewater. However, the direct utilization of substances derived from Prussian blue analogs results in severe leaching of metal ions. Therefore, in this study, we prepared Fe₃O₄/CoS/g-C₃N₄ composite catalysts by a hydrothermal method for the degradation of rhodamine B by photo-Fenton reaction. The effects of their structure, morphology and catalytic conditions on the performance were investigated. In addition, the preparation conditions and reaction parameters were also optimized.

Methods

An appropriate amount of Fe₃O₄/CoS/g-C₃N₄ catalyst (with a mass concentration of 35-65 mg/L) was added into 100 mL RhB solutions at different mass concentrations (i.e., 10-30 mg/L). Under dark conditions, the mixed suspension was stirred in a magnetic stirrer for 30 min to achieve the equilibrium of adsorption and desorption. After equilibrium, an xenon lamp was turned on and a specified amount of PMS (with a mass concentration of 60-90 mg/L) was added. During the reaction, the sample was taken once per minute. The supernatant was obtained by centrifugation. The absorbance of RhB was determined by an ultraviolet-visible spectrophotometer. After the reaction was completed, the catalyst collected using a magnet was rinsed with deionized water for several times, and dried for cycle experiments.

Results and Discussion

In the PMS+Vis system, the degradation efficiencies of RhB by CoS and Fe₃O₄/CoS within 2 minutes are 87.7% and 88.6%, respectively. In the PMS+Vis system, the degradation efficiencies of RhB by Fe₃O₄/CoS/g-C₃N₄ within 1 min and 2 min are 90.3% and 96.7%, respectively, which are higher than those of RhB in the single PMS system (i.e., 83.4% and 94.7%). Since the degradation efficiencies of Fe₃O₄/CoS/g-C₃N₄ and Fe₃O₄/CoS/g-C₃N₄-2 for RhB are similar, and the content of transition metal elements in Fe₃O₄/CoS/g-C₃N₄-2 is relatively small, 100 mg g-C₃N₄ can be used as an optimal addition amount to avoid the secondary pollution to the environment caused by transition metal ion clusters. Under different catalytic conditions, the degradation efficiency of RhB increases with the increase of PMS as the addition amount of PMS increases from 60 mg/L to 75 mg/L. The degradation efficiency of RhB remains unchanged when the addition amount of PMS increases from 75 mg/L to 90 mg/L. This is because Fe₃O₄/CoS/g-C₃N₄-2 catalyst is completely consumed at the addition amount of PMS of 75 mg/L. The excessive PMS has no more catalyst to activate it when the addition amount of PMS is 90 mg/L. From the perspectives of cost saving and environmental protection, a subsequent selection of 75 mg/L is the optimum addition amount of PMS. The degradation efficiency of RhB firstly increases and then remains unchanged as the addition amount of the catalyst increases. The catalytic degradation efficiency of RhB does not increase when the addition amount of the catalyst exceeds 50 mg/L. This is mainly because RhB all is degraded at the addition amount of the catalyst of 50 mg/L. There is no more RhB for degradation after further increasing the amount of the catalyst. Therefore, 50 mg/L is the optimal addition amount of the catalyst. The results clearly show that the degradation effect of RhB is dominant in the pH value range from 5 to 9, showing a good stability. However, the degradation efficiency of RhB decreases significantly when the pH value decreases to 3. This phenomenon is mainly attributed to the increase in the concentration of H⁺ in the reaction system in an acidic environment. At a high H⁺ concentration, the key active species in the reaction process, such as SO₄^•- and OH⁻, may be consumed, resulting in a decrease in the number of active species. The reduction of active species affects negatively the efficiency of the degradation process, thereby leading to a decrease in the degradation efficiency of RhB. The degradation efficiency of RhB also decreases at the pH value of the solution of 11. This is because under strongly alkaline conditions, OH⁻ reacts with the active species SO₄^•- in the degradation process to generate ·OH, and the oxidation capacity of ·OH is much lower than that of SO₄^•−, thus causing the decreased degradation efficiency of RhB.

Conclusions

The results indicated that this catalyst outperformed pure CoS in terms of both stability and degradation efficiency. A significant advantage of introducing Fe₃O₄ was a capability for rapid recovery via magnet and reuse, thus greatly enhancing the efficiency and economic viability of the catalyst. Moreover, CoS derived from Co-Co PBA had an adaptability in a broad pH value range, thereby improving the catalyst's stability and applicability under diverse environmental conditions. In summary, Fe₃O₄/CoS/g-C₃N₄ catalyst had an outstanding performance in degradation efficiency, environmental friendliness, cycle stability, and broad applicability, specially for the treatment of RhB.

Key words

prussian blue analogs / Rhodamine B / ferrosoferric oxide / cobaltous sulfide / graphite carbon nitride

引用本文

郑佳红, 黄植. Fe₃O₄/CoS/g-C₃N₄催化剂的制备及降解罗丹明B. 硅酸盐学报, 2024 , 52 (12) : 3748 -3760 . DOI: 10.14062/j.issn.0454-5648.20240461

Jiahong ZHENG, Zhi HUANG. Degradation of Rhodamine B by Using Fe₃O₄/CoS/g-C₃N₄ Catalyst[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (12) : 3748 -3760 . DOI: 10.14062/j.issn.0454-5648.20240461

基金

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陕西省重点研发项目(S2024-YF-YBGY-0137)
长安大学中央高校基本科研业务费专项资金资助(300102312405; 300102312406)
大学生创新创业计划训练项目(S202410710350; X202410710588)

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2024年第52卷第12期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240461

接收时间：2024-07-12
首发时间：2026-10-22
出版时间：2024-12-20

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收稿日期：2024-07-12
修回日期：2024-08-18

基金

陕西省重点研发项目(S2024-YF-YBGY-0137)

长安大学中央高校基本科研业务费专项资金资助(300102312405; 300102312406)

大学生创新创业计划训练项目(S202410710350; X202410710588)

作者信息

长安大学材料科学与工程学院，西安 710021

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240461

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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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