磁性TiO<sub>2</sub>/GO对二元体系中U（Ⅵ）的去除效能及机理

doi:10.11894/iwt.2020-0118

工业水处理 ›› 2020, Vol. 40 ›› Issue (12): 54-59. doi: 10.11894/iwt.2020-0118

磁性TiO₂/GO对二元体系中U（Ⅵ）的去除效能及机理

唐振平^1,²(),肖莎莎¹,谢严兴¹,毕玉玺¹,刘迎九¹,周帅^1,*()

1. 南华大学污染控制与资源化湖南省重点实验室, 湖南衡阳 421001
2. 南华大学核燃料循环地质理论与技术衡阳市重点实验室, 湖南衡阳 421001

收稿日期:2020-11-03 出版日期:2020-12-20 发布日期:2020-12-22
通讯作者: 周帅 E-mail:zptang01@126.com;zs402606665@126.com
作者简介:唐振平(1962-),博士,教授。E-mail:zptang01@126.com
基金资助:
湖南省教育厅项目(18C0433);湖南省财政厅项目(190SJY001)

Performance and mechanism of U(Ⅵ) removal in binary system by magnetic titanium dioxide/graphene oxide composites

Zhenping Tang^1,²(),Shasha Xiao¹,Yanxing Xie¹,Yuxi Bi¹,Yingjiu Liu¹,Shuai Zhou^1,*()

1. Hunan Province Key Laboratory of Pollution Control and Resources Reuse Technology, University of South China, Hengyang 421001, China
2. Hengyang Key Laboratory of Theory and Technology of Nuclear Fuel Geological Cycle, University of South China, Hengyang 421001, China

Received:2020-11-03 Online:2020-12-20 Published:2020-12-22
Contact: Shuai Zhou E-mail:zptang01@126.com;zs402606665@126.com

摘要/Abstract

摘要：

合成了磁性二氧化钛/氧化石墨烯（磁性TiO₂/GO）复合材料，用其处理U（Ⅵ）-Cd（Ⅱ）共存二元体系废水。考察了初始pH、磁性TiO₂/GO投加量和反应时间对U（Ⅵ）去除效果的影响，并用红外光谱仪和X射线光电子能谱仪探究去除机理。结果表明，磁性TiO₂/GO为介孔层状聚集物，在可见光范围内光催化能力较好。在pH为6、投加量为15 mg、反应时间为120 min条件下对U（Ⅵ）的去除效果最佳（去除率为93.72%）。磁性TiO₂/GO选择性去除U（Ⅵ）的主要机制为氨基官能团络合作用和光催化还原作用。

关键词: 磁性二氧化钛, 氧化石墨烯, 含铀废水, 重金属, 选择性

Abstract:

Magnetic titanium dioxide/graphite oxide(magnetic TiO₂/GO) composites were synthesized and used to treat U(Ⅵ)-Cd(Ⅱ) coexisting binary system wastewater. The effects of initial pH, the dosage of magnetic TiO₂/GO, and the reaction time on the removal of U(Ⅵ) were investigated. The removal mechanism of U(Ⅵ) was explored using FTIR and X-ray photoelectron spectroscopy. The result showed that the synthesized magnetic TiO₂/GO was a kind of layered aggregate with mesoporous structure which had perfect photocatalytic ability in visible light range. With the pH of 6, the magnetic TiO₂/GO dosage of 15 mg and reaction time of 120 min, the maximum removal efficiency of U(Ⅵ) by magnetic TiO₂/GO was up to 93.72%. The complexation of amino functional groups and photocatalytic reduction of magnetic TiO₂/GO are probably the key points for selectivity of U(Ⅵ) removal.

Key words: magnetic titanium dioxide, graphene oxide, uranium wastewater, heavy metal, selectivity

中图分类号:

X703

唐振平,肖莎莎,谢严兴,毕玉玺,刘迎九,周帅. 磁性TiO₂/GO对二元体系中U（Ⅵ）的去除效能及机理[J]. 工业水处理, 2020, 40(12): 54-59.

Zhenping Tang,Shasha Xiao,Yanxing Xie,Yuxi Bi,Yingjiu Liu,Shuai Zhou. Performance and mechanism of U(Ⅵ) removal in binary system by magnetic titanium dioxide/graphene oxide composites[J]. Industrial Water Treatment, 2020, 40(12): 54-59.

https://www.iwt.cn/CN/Y2020/V40/I12/54

图/表 6

参考文献 25

1	刘金香, 陈子庚, 谢水波, 等. 氧化石墨相氮化碳吸附U (Ⅵ)的性能与机理[J]. 精细化工, 2019, 36 (7): 1446- 1452.
2	杨冰洋.二氧化钛及其复合物的光催化性能研究[D].北京:北京交通大学, 2016.
3	Khalid N R , Majid A , Tahir M B , et al. Carbonaceous-TiO₂ nanomaterial for photocatalytic degradation of pollutants:a review[J]. Ceramics International, 2017, 43 (17): 14552- 14571. doi: 10.1016/j.ceramint.2017.08.143
4	Li Leilei , Li Xiangjun , Duan Huimin , et al. Removal of Congo Red by magnetic mesoporous titanium dioxide-graphene oxide core-shell microspheres for water purification[J]. Dalton Transactions, 2014, 43 (22): 8431- 8438. doi: 10.1039/c3dt53474j
5	Chen Diyun , Zhang Zhiqiang , Zhan Yongge , et al. Removal of uranium from uranium-containing wastewater by zero-valent iron[J]. Journal of Guangzhou University, 2012, 11 (4): 84- 89. URL
6	Song Wencheng , Wang Xiangxue , Wang Qi , et al. Plasma-induced grafting of polyacrylamide on graphene oxide nanosheets for simultaneous removal of radionuclides[J]. Physical Chemistry Chemical Physics, 2015, 17 (1): 398- 406. doi: 10.1039/C4CP04289A
7	Wang Feihong , Li Hongpeng , Liu Qi , et al. A graphene oxide/amidoxime hydrogel for enhanced uranium capture[J]. Scientific Reports, 2016, 6, 19367. doi: 10.1038/srep19367
8	毕玉玺, 凌辉, 唐振平, 等. 磁性介孔TiO₂/氧化石墨烯复合材料的制备及其对U (Ⅵ)的吸附[J]. 复合材料学报, 2019, 36 (9): 2176- 2186. doi: 10.13801/j.cnki.fhclxb.20181220.002
9	唐振平, 毕玉玺, 刘迎九, 等. 氧化石墨烯/有机改性膨润土复合材料的制备及其对Cd (Ⅱ)的吸附[J]. 复合材料学报, 2018, 35 (11): 3196- 3204. doi: 10.13801/j.cnki.fhclxb.20180310.002
10	Hu Xinjiang , Liu Yunguo , Wang Hui , et al. Removal of Cu (Ⅱ) ions from aqueous solution using sulfonated magnetic graphene oxide composite[J]. Separation and Purification Technology, 2013, 108, 189- 195. doi: 10.1016/j.seppur.2013.02.011
11	Wang Chaoxia , Mao Haiyan , Wang Chunxia , et al. Dispersibility and hydrophobicity analysis of titanium dioxide nanoparticles grafted with silane coupling agent[J]. Industrial & Engineering Chemistry Research, 2011, 50 (21): 11930- 11934.
12	Dong Ruilin , Mo Jianchen , Zhang Hanping , et al. Synthesis of the titania/graphene oxide composite photocatalyst[J]. Chemical Industry & Engineering Progress, 2014, 33 (3): 679- 684.
13	Zhang Zhibin , Qiu Yanfang , Dai Ying , et al. Synthesis and application of sulfonated graphene oxide for the adsorption of uranium (Ⅵ) from aqueous solutions[J]. Journal of Radioanalytical and Nuclear Chemistry, 2016, 310 (2): 547- 557. doi: 10.1007/s10967-016-4813-6
14	张雪红, 罗来涛. 室温水解制备介孔二氧化钛的表征[J]. 硅酸盐学报, 2005, (1): 12- 16. doi: 10.3321/j.issn:0454-5648.2005.01.003
15	黄靓, 李俊, 王军. 二氧化钛介孔材料的制备[J]. 化工进展, 2009, 28 (3): 453- 457. doi: 10.3321/j.issn:1000-6613.2009.03.018
16	Zhao Yingguo , Li Jiaxing , Zhang Shouwei , et al. Amidoxime-functionalized magnetic mesoporous silica for selective sorption of U (Ⅵ)[J]. RSC Advances, 2014, 4 (62): 32710- 32717. doi: 10.1039/C4RA05128A
17	薛晓芹.氧化石墨烯的制备、改性及对水中镉的去除研究[D].杭州:浙江大学, 2015.
18	史冬峰, 唐振平, 黄华勇, 等. 磁性氧化石墨烯/β-环糊精复合材料对U (Ⅵ)的吸附性能及机理[J]. 原子能科学技术, 2016, 50 (9): 1556- 1564.
19	李瑞月, 陈德, 李恋卿, 等. 不同作物秸秆生物炭对溶液中Pb²⁺、Cd²⁺的吸附[J]. 农业环境科学学报, 2015, (5): 1001- 1008. URL
20	Ge Huacai , Ma Ziwei . Microwave preparation of triethylenetetramine modified graphene oxide/chitosan composite for adsorption of Cr (Ⅵ)[J]. Carbohydrate Polymers, 2015, 131, 280- 287. doi: 10.1016/j.carbpol.2015.06.025
21	Shao Dadong , Hou Guangshun , Li Jiaxing , et al. PANI/GO as a super adsorbent for the selective adsorption of uranium (Ⅵ)[J]. Chemical Engineering Journal, 2014, 255, 604- 612. doi: 10.1016/j.cej.2014.06.063
22	Pan Ning , Li Long , Ding Jie , et al. Preparation of graphene oxidemanganese dioxide for highly efficient adsorption and separation of Th (Ⅳ)/U (Ⅵ)[J]. Journal of Hazardous Materials, 2016, 309, 107- 115. doi: 10.1016/j.jhazmat.2016.02.012
23	Hu Rui , Shao Dadong , Wang Xiangke . Graphene oxide/polypyrrole composites for highly selective enrichment of U (Ⅵ) from aqueous solutions[J]. Polymer Chemistry, 2014, 5 (21): 6207- 6215. doi: 10.1039/C4PY00743C
24	谢水波, 陈胜, 马华龙, 等. 硫酸盐还原菌颗粒污泥去除U (Ⅵ)的影响因素及稳定性[J]. 中国有色金属学报, 2015, (6): 1713- 1720. URL
25	Skubal L R , Meshkov N K , Rajh T , et al. Cadmium removal from water using thiolactic acid-modified titanium dioxide nanoparticles[J]. Journal of Photochemistry & Photobiology A:Chemistry, 2002, 148 (1/2/3): 393- 397. doi: 10.1016/S1010-6030(02)00069-2

离子种类	q_{e, exp}/(mg·g^-1)	准一级动力学			准二级动力学			颗粒内扩散
离子种类	q_{e, exp}/(mg·g^-1)	k₁	q_{e, cal}	R²	k₂	q_{e, cal}	R²	c	k_dif	R²
U(Ⅵ)(二元)	31.33	0.003	25.482	0.477	0.032	31.656	0.999	34.105	0.939	0.711
Cd(Ⅱ)(二元)	26.200	0.025	11.677	0.907	0.007	26.738	0.999	67.148	0.546	0.650
U(Ⅵ)(单组分)	49.825	0.034	12.452	0.929	0.015	50.000	0.999	41.833	0.585	0.700
Cd(Ⅱ)(单组分)	47.622	0.030	6.138	0.798	0.018	47.847	0.999	37.044	0.800	0.391

离子种类	q_{e, exp}/(mg·g^-1)	准一级动力学			准二级动力学			颗粒内扩散
离子种类	q_{e, exp}/(mg·g^-1)	k₁	q_{e, cal}	R²	k₂	q_{e, cal}	R²	c	k_dif	R²
U(Ⅵ)(二元)	31.33	0.003	25.482	0.477	0.032	31.656	0.999	34.105	0.939	0.711
Cd(Ⅱ)(二元)	26.200	0.025	11.677	0.907	0.007	26.738	0.999	67.148	0.546	0.650
U(Ⅵ)(单组分)	49.825	0.034	12.452	0.929	0.015	50.000	0.999	41.833	0.585	0.700
Cd(Ⅱ)(单组分)	47.622	0.030	6.138	0.798	0.018	47.847	0.999	37.044	0.800	0.391

[1]	杨伟球, 史广宇. 锂电池生产废水处理工程设计和运行实例[J]. 工业水处理, 2025, 45(3): 206-211.
[2]	陈召, 刘世豪, 朱丽娟, 常德政, 高岩. 微藻-亚硝化颗粒污泥对镉胁迫的响应研究[J]. 工业水处理, 2025, 45(2): 126-131.
[3]	李典, 汪洵, 刘应明. 新能源汽车产业园区工业废水特征及处理模式[J]. 工业水处理, 2025, 45(1): 26-31.
[4]	邓志华, 刘蕊, 李碧青. 不同生物炭的制备及其对重金属和抗生素的吸附性能[J]. 工业水处理, 2025, 45(1): 94-103.
[5]	胡雅, 孙晓蕾, 陆静宇, 孙秀云. 泰妙菌素废盐活性炭的制备及吸附EDTA-Pb（Ⅱ）的研究[J]. 工业水处理, 2024, 44(8): 133-139.
[6]	唐朝春, 徐豪佑, 陈钧杰, 冯文涛, 阮以宣, 何兴龙, 刘耀中. MOFs@气凝胶吸附去除水中污染物的研究进展[J]. 工业水处理, 2024, 44(6): 12-21.
[7]	柯平超, 钟婷婷, 吴天楠, 王坤坤, 李家乐, 周义朋, 孙占学. 磷酸盐矿物固铀法处理含铀废水研究现状与进展[J]. 工业水处理, 2024, 44(6): 34-39.
[8]	刘洁, 白圆, 马睿, 敬宗显, 万馨雯, 吴海龙, 黄玮婷. MXene吸附法去除水中污染物的研究进展[J]. 工业水处理, 2024, 44(6): 40-52.
[9]	冯雪敏, 张晓青, 张爱君, 曹军瑞, 寇希元, 宋翰文, 邱金泉. 海水淡化工艺排放浓海水中风险物质的识别[J]. 工业水处理, 2024, 44(6): 53-59.
[10]	张伟, 罗旭彪, 欧阳婷, 柳正葳, 熊萍. 吸附法去除水中典型有机络合态重金属的研究进展[J]. 工业水处理, 2024, 44(6): 60-68.
[11]	赵丹华, 廖欣欣, 邓颖欣, 陈柳名, 梁兰芳, 黄嘉豪, 陈作义. 重金属捕获剂EDTC协同处理EDTA-Cu/RhB的去除特性[J]. 工业水处理, 2024, 44(5): 141-148.
[12]	李冰, 吴迪, 石岩, 李海翔, 李甫, 马毅. 膜耦合技术对沼液浓缩及净水效果的影响[J]. 工业水处理, 2024, 44(5): 156-163.
[13]	孙采蕊, 欧阳铸, 曹露, 胡莹, 黄海明, 王炳乾, 龙柯桦, 陶乐瑶. 鸟粪石结晶法回收电镀废水中氮磷试验研究[J]. 工业水处理, 2024, 44(4): 113-119.
[14]	冯颖, 李可心, 张宏, 于汉哲, 马标, 张建伟, 董鑫. 壳聚糖复合水凝胶的制备方法及在水处理中的应用[J]. 工业水处理, 2024, 44(2): 17-26.
[15]	贺自帅, 李海涛, 高红. 污泥活性炭的制备及其对含磷污水的吸附研究[J]. 工业水处理, 2024, 44(12): 138-146.

选择文件类型/文献管理软件名称

选择包含的内容

磁性TiO₂/GO对二元体系中U（Ⅵ）的去除效能及机理

Performance and mechanism of U(Ⅵ) removal in binary system by magnetic titanium dioxide/graphene oxide composites

RichHTML

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 6

参考文献 25

相关文章 15

编辑推荐

Metrics

本文评价

模态框（Modal）标题

选择文件类型/文献管理软件名称

选择包含的内容

磁性TiO2/GO对二元体系中U（Ⅵ）的去除效能及机理

Performance and mechanism of U(Ⅵ) removal in binary system by magnetic titanium dioxide/graphene oxide composites

RichHTML

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 6

参考文献 25

相关文章 15

编辑推荐

Metrics

本文评价

磁性TiO₂/GO对二元体系中U（Ⅵ）的去除效能及机理