g-C3N4/MIL-125(Ti)磁性复合材料制备及其去除罗丹明B

doi:10.16085/j.issn.1000-6613.2022-0302

化工进展 ›› 2022, Vol. 41 ›› Issue (12): 6469-6476.DOI: 10.16085/j.issn.1000-6613.2022-0302

g-C₃N₄/MIL-125(Ti)磁性复合材料制备及其去除罗丹明B

陈彰旭¹^,²^,³(), 李燕辉¹^,²^,³, 任红云⁴(), 张丽丹¹^,²^,³, 郑炳云¹^,²^,³

^1.莆田学院环境与生物工程学院，福建莆田 351100
^2.福建省新型污染物生态毒理效应与控制重点实验室，福建莆田 351100
^3.福建省高校生态环境及其信息图谱重点实验室，福建莆田 351100
^4.中国科学院城市环境研究所，福建厦门 361021

收稿日期:2022-02-28 修回日期:2022-04-07 出版日期:2022-12-20 发布日期:2022-12-29
通讯作者: 陈彰旭,任红云
作者简介:陈彰旭（1977—），男，博士，副教授，研究方向为环境功能材料。E-mail：xuzhangchen@163.com。
基金资助:
国家自然科学基金(51778598);福建省自然科学基金(2022J011163);国家级大学生创新项目(202011498004);2018年、2022年福建省科技特派员资金项目;2021年莆田市科技特派员资金项目;莆田学院功能材料研究创新团队(科研[2022]10号)

Preparation of g-C₃N₄/MIL-125(Ti) magnetic composites for Rhodamine B removal

CHEN Zhangxu¹^,²^,³(), LI Yanhui¹^,²^,³, REN Hongyun⁴(), ZHANG Lidan¹^,²^,³, ZHENG Bingyun¹^,²^,³

^1.College of Environmental and Biological Engineering, Putian University, Putian 351100, Fujian, China
^2.Fujian Provincial Key Laboratory of Ecology-Toxicological Effects & Control for Emerging Contaminants, Putian 351100, Fujian, China
^3.Key Laboratory of Ecological Environment and Information Atlas, Fujian Provincial University, Putian 351100, Fujian, China
^4.Institute of Urban Environment (IUE), Chinese Academy of Sciences (CAS), Xiamen 361021, Fujian, China

Received:2022-02-28 Revised:2022-04-07 Online:2022-12-20 Published:2022-12-29
Contact: CHEN Zhangxu, REN Hongyun

摘要/Abstract

摘要：

为解决能源短缺和环境污染等问题，探究半导体光催化材料去除有机污染物，以MIL-125(Ti)为光催化剂载体，g-C₃N₄为有机半导体，Fe₃O₄@SiO₂为磁性载体，通过溶剂热法合成了一系列不同质量配比的可见光响应型MIL-125(Ti)复合材料。通过傅里叶变换红外光谱仪、X射线衍射仪、场发射扫描电子显微镜、热重分析仪等对复合材料的样品组成、结构、形貌及光学性能等进行表征分析。进一步通过正交试验评价该复合材料去除罗丹明B的性能。研究结果表明，最适宜去除罗丹明B的操作工艺条件为：光催化时间为4.0h，g-C₃N₄与MIL-125(Ti)的质量配比为1∶20，催化剂投加量为0.01g，罗丹明B溶液的浓度为10.0mg/L。在该条件下罗丹明B的去除率可达到96.57%。经过4次循环实验后，去除率仍能达到86.52%。g-C₃N₄/MIL-125(Ti)磁性复合材料的制备工艺和去除有机染料机理可为相关研究提供借鉴。

关键词: 磁性, 石墨相氮化碳, MIL-125(Ti), 催化, 降解, 再生

Abstract:

To solve the problems of energy shortage and environmental pollution, semiconductor photocatalysis materials were used for organic pollutants removal in this paper. A series of visible light responsive MIL-125(Ti) composites with different mass ratios were synthesized by solvothermal method with using MIL-125(Ti) as photocatalyst carrier, g-C₃N₄ as organic semiconductor and Fe₃O₄@SiO₂ as magnetic carrier. The obtained composites were thoroughly characterized by Fourier transform infrared spectrometer, X-ray diffractometer, field emission scanning electron microscope and thermal gravimetric analyzer. The performance of the composite material for Rhodamine B removal was further investigated by L₁₆(4⁵) orthogonal array. The results showed that the optimum processing conditions for Rhodamine B removal were as follows: the photocatalysis time of 4.0h, the mass ratio of g-C₃N₄to MIL-125(Ti) of 1∶20, the catalyst dosage of 0.01g and the Rhodamine B solution concentration of 10.0mg/L. The removal rate of Rhodamine B reached 96.57% under the optimal condition. After 4 cycles of experiments, the removal rate can still reach 86.52%. The preparation process of g-C₃N₄/MIL-125(Ti) magnetic composites and the mechanism on organic dyes removal can be used as a reference for the treatment of organic dye wastewater.

Key words: magnetic, graphite phase carbon nitride, MIL-125 (Ti), catalysis, degradation, regeneration

中图分类号:

陈彰旭, 李燕辉, 任红云, 张丽丹, 郑炳云. g-C₃N₄/MIL-125(Ti)磁性复合材料制备及其去除罗丹明B[J]. 化工进展, 2022, 41(12): 6469-6476.

CHEN Zhangxu, LI Yanhui, REN Hongyun, ZHANG Lidan, ZHENG Bingyun. Preparation of g-C₃N₄/MIL-125(Ti) magnetic composites for Rhodamine B removal[J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6469-6476.

图/表 12

参考文献 18

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样品序号	样品名称	样品代号	g-C₃N₄∶ MIL-125(Ti)
S1	Fe₃O₄	F	0∶0
S2	g-C₃N₄	CN	1∶0
S3	MIL-125(Ti)	M	0∶1
S4	Fe₃O₄@SiO₂	FS	0∶0
S5	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-1	FSCNM1	1∶10
S6	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-2	FSCNM2	1∶20
S7	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-3	FSCNM3	1∶30
S8	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-4	FSCNM4	1∶40

样品序号	样品名称	样品代号	g-C₃N₄∶ MIL-125(Ti)
S1	Fe₃O₄	F	0∶0
S2	g-C₃N₄	CN	1∶0
S3	MIL-125(Ti)	M	0∶1
S4	Fe₃O₄@SiO₂	FS	0∶0
S5	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-1	FSCNM1	1∶10
S6	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-2	FSCNM2	1∶20
S7	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-3	FSCNM3	1∶30
S8	Fe₃O₄@SiO₂/g-C₃N₄/MIL-125(Ti)-4	FSCNM4	1∶40

序号	光催化时间（A）/h	g-C₃N₄∶MIL-125（Ti）（B）	催化剂投加量（C）/g	RhB浓度（D）/mg·L^-1	去除率/%
1	2.0	1∶40	0.01	1.0	21.24
2	2.0	1∶30	0.05	2.0	47.47
3	2.0	1∶20	0.10	5.0	40.17
4	2.0	1∶10	0.20	10.0	19.89
5	4.0	1∶40	0.10	10.0	67.04
6	4.0	1∶30	0.20	5.0	64.86
7	4.0	1∶20	0.01	2.0	87.13
8	4.0	1∶10	0.05	1.0	41.98
9	6.0	1∶40	0.20	2.0	54.05
10	6.0	1∶30	0.10	1.0	10.08
11	6.0	1∶20	0.05	10.0	77.06
12	6.0	1∶10	0.01	5.0	89.69
13	8.0	1∶40	0.05	5.0	34.57
14	8.0	1∶30	0.01	10.0	92.87
15	8.0	1∶20	0.20	1.0	46.67
16	8.0	1∶10	0.10	2.0	55.07
k₁	32.19	44.23	72.73	29.99
k₂	65.25	53.82	50.27	60.93
k₃	57.72	62.76	43.09	57.32
k₄	57.30	51.66	46.37	64.22
R	33.06	18.53	29.64	34.22
因素主次	D>A>C>B
最优方案	D₄A₂C₁B₃

序号	光催化时间（A）/h	g-C₃N₄∶MIL-125（Ti）（B）	催化剂投加量（C）/g	RhB浓度（D）/mg·L^-1	去除率/%
1	2.0	1∶40	0.01	1.0	21.24
2	2.0	1∶30	0.05	2.0	47.47
3	2.0	1∶20	0.10	5.0	40.17
4	2.0	1∶10	0.20	10.0	19.89
5	4.0	1∶40	0.10	10.0	67.04
6	4.0	1∶30	0.20	5.0	64.86
7	4.0	1∶20	0.01	2.0	87.13
8	4.0	1∶10	0.05	1.0	41.98
9	6.0	1∶40	0.20	2.0	54.05
10	6.0	1∶30	0.10	1.0	10.08
11	6.0	1∶20	0.05	10.0	77.06
12	6.0	1∶10	0.01	5.0	89.69
13	8.0	1∶40	0.05	5.0	34.57
14	8.0	1∶30	0.01	10.0	92.87
15	8.0	1∶20	0.20	1.0	46.67
16	8.0	1∶10	0.10	2.0	55.07
k₁	32.19	44.23	72.73	29.99
k₂	65.25	53.82	50.27	60.93
k₃	57.72	62.76	43.09	57.32
k₄	57.30	51.66	46.37	64.22
R	33.06	18.53	29.64	34.22
因素主次	D>A>C>B
最优方案	D₄A₂C₁B₃

序号	光催化时间（A）/h	材料（B）	g-C₃N₄∶MIL-125（Ti）（C）	催化剂投加量（D）/g	RhB浓度（E）/mg·L^-1	去除率/%
1	4.0	FSCNM-2	1∶20	0.01	10.0	96.57
2	4.0	MIL-125（Ti）	0∶1	0.01	10.0	15.63
3	4.0	g-C₃N₄	1∶0	0.01	10.0	11.38
4	4.0	Fe₃O₄@SiO₂	0∶0	0.01	10.0	7.15
5	4.0	Blank	Blank	0.00	10.0	5.37

g-C₃N₄/MIL-125(Ti)磁性复合材料制备及其去除罗丹明B

Preparation of g-C₃N₄/MIL-125(Ti) magnetic composites for Rhodamine B removal

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