Ag@AgCl-Fe<sub>3</sub>O<sub>4</sub>/rGO复合材料对印染废水中染料和重金属离子的吸附和光催化降解性能

陈凤华; 梁娓娓; 石向东; 陈庆涛; 秦霄云; 张永辉

doi:10.13801/j.cnki.fhclxb.20200928.004

Ag@AgCl-Fe₃O₄/rGO复合材料对印染废水中染料和重金属离子的吸附和光催化降解性能

doi: 10.13801/j.cnki.fhclxb.20200928.004

郑州轻工业大学　材料与化学工程学院，郑州 450002

基金项目: 国家自然科学基金(21671179；21904120)；河南省科技厅科技攻关计划项目(202102210045)

详细信息

通讯作者:
陈凤华，博士，副教授，硕士生导师，研究方向为功能纳米复合材料及其在环境、生物医药领域中的应用　E-mail：phenix@zzuli.edu.cn

中图分类号: TB333
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出版历程
- 收稿日期: 2020-08-13
- 录用日期: 2020-09-17
- 网络出版日期: 2020-09-28
- 刊出日期: 2021-07-15

Adsorption and photocatalytic degradation of dyes and heavy metals in printing and dyeing wastewater by Ag@AgCl-Fe₃O₄/rGO composites

School of Materials and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou 450002, China

摘要

摘要: 依次利用溶剂热法和原位沉积法制备了Ag@AgCl-Fe₃O₄/还原氧化石墨烯(rGO)复合材料，并对其进行结构和形貌表征。分别以罗丹明B(RhB)和Cd²⁺为研究对象，探讨了Ag@AgCl-Fe₃O₄/rGO复合材料吸附和可见光光催化印染废水中重金属离子和芳香族染料的性能，考察了Ag@AgCl-Fe₃O₄/rGO复合材料中rGO含量、与RhB共存的亚甲基蓝(MB)和Cd²⁺对RhB降解效果的影响；同时研究了溶液的初始pH值及与Cd²⁺共存的MB对Cd²⁺吸附效果的影响。结果表明：Ag@AgCl-Fe₃O₄/rGO复合材料对RhB的吸附量为47%，可见光照50 min的光催化降解率可达98%；Ag@AgCl-Fe₃O₄/rGO复合材料的吸附-光催化降解活性随rGO含量的增加而提高；废水中与RhB共存的MB使Ag@AgCl-Fe₃O₄/rGO复合材料对RhB的降解效率和循环性能受到一定抑制，而与RhB共存的Cd²⁺对RhB的降解效率和循环性能几乎没有影响。Ag@AgCl-Fe₃O₄/rGO复合材料对Cd²⁺也有良好的吸附性能，具有一定的pH值依赖性，在pH值为5时，复合材料对Cd²⁺的吸附量可达68 mg/g，但废水中MB染料的存在会抑制复合材料对Cd²⁺的吸附。
- 石墨烯 /
- Fe₃O₄ /
- Ag@AgCl /
- 吸附 /
- 光催化降解
Abstract: The Ag@AgCl-Fe₃O₄/reduced graphene oxide (rGO) composites were obtained by solvothermal and in-situ precipitation method. The structure and morphology of the Ag@AgCl-Fe₃O₄/rGO composites were characterized. The effects of rGO content, other organic dyes (such as methylene blue (MB)) and heavy metal ions (such as Cd²⁺) co-existing with Rhodamine B (RhB) on the degradation of RhB were investigated, and the effects of initial pH value and other organic dyes (such as MB) co-existing with Cd²⁺ on the adsorption of Cd²⁺ were also studied. The results show that about 47% of RhB can be absorbed to Ag@AgCl-Fe₃O₄/rGO composites in the dark and the degradation of RhB could reach 98% within 50 min visible-light irradiation, and the adsorption-photocatalytic activity of the Ag@AgCl-Fe₃O₄/rGO composites increases with the increasing rGO content. The degradation efficiency on RhB and the good cycle performance of the catalyst will be suppressed by the coexisted MB, but are almost unaffected by the coexisted Cd²⁺. For the Cd²⁺ solution system, the adsorption amount of Cd²⁺ on Ag@AgCl-Fe₃O₄/rGO composites varies with the pH value and the adsorption capacity at pH=5 can be up to 68 mg/g. However, the adsorption of Cd²⁺ will be restrained by the presence of MB in wastewater.
- graphene /
- Fe₃O₄ /
- Ag@AgCl /
- adsorption /
- photocatalytic degradation

HTML全文

图 1 氧化石墨烯(GO)、Fe₃O₄/还原氧化石墨烯(rGO)和Ag@AgCl-Fe₃O₄/rGO复合材料的XRD图谱

Figure 1. XRD patterns of graphene oxide (GO), Fe₃O₄/reduced graphene oxide (rGO) and Ag@AgCl-Fe₃O₄/rGO composites

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图 2 GO (a)，Fe₃O₄/rGO (b)和Ag@AgCl-Fe₃O₄/rGO (c)样品的TEM图

Figure 2. TEM images of GO (a)，Fe₃O₄/rGO (b) and Ag@AgCl-Fe₃O₄/rGO composites (c)

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图 3 Ag@AgCl-Fe₃O₄/rGO复合材料的SEM图像(a)和EDS图谱(b)

Figure 3. SEM image (a) and EDS spectrum (b) of Ag@AgCl-Fe₃O₄/rGO composites

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图 4 Ag@AgCl-Fe₃O₄/rGO复合材料的XPS全谱(a)及C 1s (b)、Fe 2p (c)、Ag 3d (d)和Cl 2p (e)的高分辨XPS图谱

Figure 4. XPS survey spectrum of Ag@AgCl-Fe₃O₄/rGO composite (a) and high resolution XPS spectra of C 1s (b), Fe 2p (c), Ag 3d (d) and Cl 2p (e)

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图 5 Ag@AgCl-Fe₃O₄/rGO复合材料的UV-vis图谱

Figure 5. UV-vis absorption spectrum of Ag@AgCl-Fe₃O₄/rGO composite

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图 6 Ag@AgCl-Fe₃O₄/rGO复合材料的N₂吸附-脱附等温曲线(a)和孔径分布(b)

Figure 6. N₂ adsorption-desorption isotherms (a) and pore size distribution (b) of prepared Ag@AgCl-Fe₃O₄/rGO composite

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图 7 Ag@AgCl-Fe₃O₄/rGO复合材料光催化降解RhB的时间相关UV-vis图谱(a); rGO含量对Ag@AgCl-Fe₃O₄/rGO复合材料光催化降解性能的影响(b)

Figure 7. Temporal evolution UV-vis absorption spectra of photocatalytic degradation of RhB by Ag@AgCl-Fe₃O₄/rGO composite (a); Effect of rGO content on adsorption-photocatalytic degradation properities of Ag@AgCl-Fe₃O₄/rGO composites (b)

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图 8 Ag@AgCl-Fe₃O₄/rGO复合材料光催化降解罗丹明B(RhB)和亚甲基蓝(MB)混合溶液的时间相关UV-vis图谱

Figure 8. Temporal evolution UV-vis absorption spectra of photocatalytic degradation of mixed Rhodamine B (RhB) and methylene blue (MB) solutions by Ag@AgCl-Fe₃O₄/rGO composite

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图 9 Ag@AgCl-Fe₃O₄/rGO复合材料光催化降解含不同浓度的Cd²⁺的RhB溶液的时间相关UV-vis图谱

Figure 9. Temporal evolution UV-vis absorption spectra of photocatalytic degradation of RhB solution containing different concentrations of Cd²⁺ by Ag@AgCl-Fe₃O₄/rGO composite

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图 10 Ag@AgCl-Fe₃O₄/rGO复合材料降解RhB溶液、RhB-MB混合溶液和RhB-Cd²⁺混合溶液时循环重复次数与降解效率的关系

Figure 10. Relationships between cycle numbers and degradation efficiency of Ag@AgCl-Fe₃O₄/rGO composites on RhB solution, RhB-MB mixture and RhB-Cd²⁺ mixture solution

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图 11 不同pH值下Ag@AgCl-Fe₃O₄/rGO复合材料对Cd²⁺的吸附曲线

Figure 11. Adsorption curves of Cd²⁺ on Ag@AgCl-Fe₃O₄/rGO composite at different pH values

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图 12 不同初始浓度下Ag@AgCl-Fe₃O₄/rGO复合材料对Cd²⁺的吸附曲线

Figure 12. Effect of initial pollutant concentration on adsorption of Cd²⁺ on Ag@AgCl-Fe₃O₄/rGO composites

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图 13 Ag@AgCl-Fe₃O₄/rGO复合材料吸附Cd²⁺溶液的循环重复次数与吸附去除效率的关系

Figure 13. Relationships between cycle numbers and adsorption efficiency of Ag@AgCl-Fe₃O₄/rGO composite on Cd²⁺ solution

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