锆基金属有机框架与Fe<sub>2</sub>O<sub>3</sub>复合材料对砷的吸附及机理研究

引用本文: 余文婷, 罗明标. 锆基金属有机框架与Fe₂O₃复合材料对砷的吸附及机理研究[J]. 分析化学, 2023, 51(6): 1003-1012. doi: 10.19756/j.issn.0253-3820.221186 shu

Citation: YU Weng-Ting, LUO Ming-Biao. Characteristics and Mechanism Study of Arsenic Adsorption on Composite Material of Zr-based Metal Organic Framework and Fe₂O₃[J]. Chinese Journal of Analytical Chemistry, 2023, 51(6): 1003-1012. doi: 10.19756/j.issn.0253-3820.221186 shu

锆基金属有机框架与Fe₂O₃复合材料对砷的吸附及机理研究

余文婷 ^{1,
,} ,
罗明标 ^2,

1.
中国地质大学(北京)水资源与环境学院, 北京 100083;
2.
东华理工大学化学生物与材料科学学院, 南昌 330013

通讯作者: 余文婷,E-mail:wtyu@cugb.edu.cn

基金项目:
国家自然科学基金项目(No.21761001)资助。

摘要: 利用水热法制备UiO-66（OH）@Fe₂O₃复合材料，并将其用于As（Ⅲ）和As（Ⅴ）的吸附。结果表明，UiO-66（OH）@Fe₂O₃去除As（Ⅲ）的最佳pH=11，平衡吸附时间为180 min，最大吸附量为140.0 mg/g，此时去除As（Ⅲ）的主要形态为H₂AsO₃^-； UiO-66（OH）@Fe₂O₃去除As（Ⅴ）的最佳pH=9，平衡吸附时间为90 min，最大吸附量为260.0 mg/g，在该pH值下去除As（Ⅴ）的主要形态为HAsO₄^2-。进一步探究了此吸附剂对砷的吸附动力学和热力学行为，考察了共存离子对吸附的影响，并评价了吸附剂的重复使用效果。结果表明，此吸附剂对As（Ⅲ）和As（Ⅴ）的去除均满足拟二级动力学方程和Langmuir等温吸附模型，并且在不同温度下的ΔG⁰均小于零，表明整个吸附过程属于自发的单层的化学吸附。除PO₄^3-外，其它共存离子对吸附的影响较小。将吸附后的材料用0.25 mol/L Na₂SO₄洗脱，5次吸附-解吸实验结果表明，复合材料对As（Ⅲ）的去除率达60%以上，对As（Ⅴ）的去除率达80%以上。X射线衍射和红外光谱等的表征结果表明，此吸附剂对砷的吸附主要是以化学过程为主，砷主要通过与中心原子锆络合形成Zr—O—As键以及与Fe₂O₃水解产生的铁氢氧化物共沉淀而被去除。此吸附剂对于不同形态的砷具有较好的吸附活性，同时为以锆基框架材料作为基底材料的复合材料开发提供了理论参考。

关键词:

砷
/ UiO-66（OH）@Fe₂O₃
/ 吸附
/ 机理

English

Characteristics and Mechanism Study of Arsenic Adsorption on Composite Material of Zr-based Metal Organic Framework and Fe₂O₃

YU Weng-Ting ^{1,
,} ,
LUO Ming-Biao ^2,

1.
School of Water Resources and Environment, China University of Geosciences(Beijing), Beijing 100083, China;
2.
School of Biology, Chemistry and Material Science, East China University of Technology, Nanchang 330013, China

Corresponding author: YU Weng-Ting, wtyu@cugb.edu.cn

Received Date: 08 April 2022
Revised Date: 09 October 2022
Fund Project:
Supported by the National Natural Science Foundation of China (No. 21761001).

Abstract: UiO-66(OH)@Fe₂O₃ synthesized by hydrothermal method was used for adsorption of As(Ⅲ) and As(V). results showed that the optimal pH value for As (Ⅲ) removal by UiO-66(OH)@Fe₂O₃ was pH=11, the equilibrium adsorption time was 180 min, and the maximum adsorption amount was 140.0 mg/g. At this time, the main form of As(Ⅲ) removal was H₂AsO₃^-. Meanwhile, the optimal pH value for As(V) removal by UiO-66(OH)@Fe₂O₃ was pH=9, the equilibrium adsorption time was 90 min, and the maximum adsorption amount was 260.0 mg/g. At this pH value, the main form of As(V) removal was HAsO₄^2-. The adsorption kinetics, thermodynamic, co-existing ions and repeatability of UiO-66(OH)@Fe₂O₃ were also investigated. It was shown that the adsorption fitted well with pseudo second-order kinetic model and Langmuir isotherm, and the ΔG° was less than zero under different temperatures, indicating that the entire adsorption process belongs to spontaneous monolayer chemical adsorption. Except PO₄^3-, other co-existing ions had little effects on adsorption. The adsorbed material was eluted with 0.25 mol/L Na₂SO₄. Through five times of adsorption and desorption experiments, it was shown that the removal rate of As(Ⅲ) and As(V) were more than 60% and 80%, respectively. The characterization results of X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM) and X-ray photoelectron spectroscopy (XPS) showed that the adsorption of arsenic by this adsorbent was mainly a chemical process, including the formation of Zr—O—As and the co-precipitation of ferric hydroxide produced by Fe₂O₃ hydrolysis. The prepared UiO-66(OH)@Fe₂O₃ had good adsorption activity for removing arsenic in different forms, and provided a theoretical reference for the development of composite materials with zirconium-based frame materials as the basic materials.

Key words:

1. [1]
  ZOU S W, KOH K Y, CHEN Z, WANG Y Y, CHEN J P, ZHENG Y M. Chemosphere, 2022, 288(3):132634.ZOU S W, KOH K Y, CHEN Z, WANG Y Y, CHEN J P, ZHENG Y M. Chemosphere, 2022, 288(3):132634.
2. [2]
  GIRI D D, JHA J M, SRIVASTAVA N, HASHEM A, ABD ALLAH E F, SHAH M, PAL D B. Chemosphere, 2022, 287(3):132308.GIRI D D, JHA J M, SRIVASTAVA N, HASHEM A, ABD ALLAH E F, SHAH M, PAL D B. Chemosphere, 2022, 287(3):132308.
3. [3]
  CAMEIRO M A, PINTOR A M A, BOAVENTURA R A R, BOTELHO C M S. J. Hazard. Mater., 2022, 432:128657.CAMEIRO M A, PINTOR A M A, BOAVENTURA R A R, BOTELHO C M S. J. Hazard. Mater., 2022, 432:128657.
4. [4]
  PI K, XIE X, MA T, SU C, LI J, WANG Y. Water Res., 2020, 181:115859.PI K, XIE X, MA T, SU C, LI J, WANG Y. Water Res., 2020, 181:115859.
5. [5]
  ALKA S, SHAHIR S, IBRAHIM N, NDEJIKO M J, VO D V N, ABD MANAN F. J. Cleaner Prod., 2021, 278:123805.ALKA S, SHAHIR S, IBRAHIM N, NDEJIKO M J, VO D V N, ABD MANAN F. J. Cleaner Prod., 2021, 278:123805.
6. [6]
  ZHANG Jian. Mod. Chem. Res., 2021, (11):111-112. 张坚. 当代化工研究, 2021, (11):111-112.
7. [7]
  SUN Dong, SHEN Li-Ping, ZHANG Zhi-Peng, CAO Nan, XIONG Ting-Ting, GONG Zheng-Jun. J. Civ. Environ. Eng., 2021, 43(6):180-186. 孙东, 沈莉萍, 张志鹏, 曹楠, 熊亭亭, 龚正君. 土木与环境工程学报, 2021, 43(6):180-186.
8. [8]
  JIN Ke-Yan, BAI Pu, LI Xiao-Long, ZHANG Jia-Nan, YAN Wen-Fu. Chem. J. Chin. Univ., 2022, 43(2):9-18. 靳科研, 白璞, 李小龙, 张佳楠, 闫文付. 高等学校化学学报, 2022, 43(2):9-18.
9. [9]
  CHEN Peng, LI Rong, CHEN Bin. Chin. J. Anal. Chem., 2022, 50(2):300-309. 陈鹏, 李蓉, 陈斌. 分析化学, 2022, 50(2):300-309.
10. [10]
  HUANG Bo, GUO Zhao-Hui, XIAO Xi-Yuan, PENG Chi, ZHU Hui-Wen, SHI Lei, YANG An-Di. Environ. Sci., 2019, 40(5):2287-2294. 黄博, 郭朝晖, 肖细元, 彭驰, 朱惠文, 史磊, 阳安迪. 环境科学, 2019, 40(5):2287-2294.
11. [11]
  NIAN Ya-Xin, WU Hui-Ying, JIANG Kai-Bing, HUANG Bo-Fan, HU Mo-Nong. Appl. Chem. Ind., 2021, 50(12):3477-3481. 粘雅鑫, 吴慧英, 江凯兵, 黄博凡, 胡墨浓. 应用化工, 2021, 50(12):3477-3481.
12. [12]
  HUO Xiao-Wen, YU Shou-Wu, XIAO Shu-Juan, TAN Xiao-Yao. J. Mater. Eng., 2021, 49(7):10-20. 霍晓文, 于守武, 肖淑娟, 谭小耀. 材料工程, 2021, 49(7):10-20.
13. [13]
  CHEN Su-Qing, SHEN Mao, LIANG Hua-Ding, BAO Ming-Hui. Chin. J. Anal. Chem., 2020, 48(7):912-919. 陈素清, 沈茂, 梁华定, 鲍明辉. 分析化学, 2020, 48(7):912-919.
14. [14]
  GHOSAL P S, KATTIL K V, YADAV M K, GUPTA A K. J. Environ. Manage., 2018, 209:176-187.GHOSAL P S, KATTIL K V, YADAV M K, GUPTA A K. J. Environ. Manage., 2018, 209:176-187.
15. [15]
  AREDES S, KLEIN B, PAWLIK M. J. Cleaner Prod., 2013, 60:71-76.AREDES S, KLEIN B, PAWLIK M. J. Cleaner Prod., 2013, 60:71-76.
16. [16]
  SIDDIQUI S I, CHAUDHRY S A. Process Saf. Environ. Protection, 2017, 111:592-626.SIDDIQUI S I, CHAUDHRY S A. Process Saf. Environ. Protection, 2017, 111:592-626.
17. [17]
  FAN Jia, HU Shi-Qin, WEI Bai, YANG Jin-Hui, ZENG Qian, YANG Fang-Ting. Acta Mater. Compos. Sin., 2022, 39(10):4898-4807. 范甲, 胡世琴, 魏柏, 杨金辉, 曾倩, 杨芳婷. 复合材料学报, 2022, 39(10):4898-4807.
18. [18]
  DENG Tian-Tian, HU Ye, LIU Shuai-Xia, LI Han-Sheng, HOU Yu-Meng. J. Ecol. Rural Environ., 2018, 34(10):930-938. 邓天天, 胡烨, 刘帅霞, 李晗晟, 侯宇梦. 生态与农村环境学报, 2018, 34(10):930-938.
19. [19]
  YAN C S, GAO H Y, LE GONG L, MA L F, DANG L L, ZHANG L, MENG P P, LUO F. J. Mater. Chem. A, 2016, 4(35):13603-13610.YAN C S, GAO H Y, LE GONG L, MA L F, DANG L L, ZHANG L, MENG P P, LUO F. J. Mater. Chem. A, 2016, 4(35):13603-13610.
20. [20]
  LI Wen, QIAO Jun-Yi, LIU Xin-Yao, LIU Yun-Ling. Chem. J. Chin. Univ., 2022, 43(1):1-8. 李文, 乔珺一, 刘鑫垚, 刘云凌. 高等学校化学学报, 2022, 43(1):1-8.
21. [21]
  SINGH N, SRIVASTAVA I, DWIVEDI J, SANKARARAMAKRISHNAN N. Chemosphere, 2021, 270:129490.SINGH N, SRIVASTAVA I, DWIVEDI J, SANKARARAMAKRISHNAN N. Chemosphere, 2021, 270:129490.
22. [22]
  ZHANG Jin-Hui, ZHANG Huan, ZHU Xin-Feng, SONG Zhong-Xian, KANG Hai-Yan, LIU Hong-Pan, DENG Wei, HOU Guang-Chao, LI Gui-Ting, HUANG Zhen-Zhen. Chem. Ind. Eng. Prog., 2022. 42(1):445-456. 张金辉, 张焕, 朱新锋, 宋忠贤, 康海彦, 刘红盼, 邓炜, 侯广超, 李桂亭, 黄真真. 化工进展, 2022. 42(1):445-456.
23. [23]
  XU Ao, QI Jing-Xiong, ZHU Zhong-Quan, LI Xu-Fei, HUANG Wei-Qiu. New Chem. Mater., 2021, 49(10):81-86. 徐奥, 綦竞雄, 朱忠泉, 李旭飞, 黄维秋. 化工新型材料, 2021, 49(10):81-86.
24. [24]
  PENG Y, HUANG H, ZHANG Y, KANG C, CHEN S, SONG L, LIU D, ZHONG C. Nat. Commun., 2018, 9(1):187-195.PENG Y, HUANG H, ZHANG Y, KANG C, CHEN S, SONG L, LIU D, ZHONG C. Nat. Commun., 2018, 9(1):187-195.
25. [25]
  TANG Chao-Chun, WANG Shun-Teng, HUANG Cong-Xin, FENG Wen-Tao, RUAN Yi-Xuan. Chem. Indus. Eng. Prog., 2021, 41(6):3263-3278. 唐朝春, 王顺藤, 黄从新, 冯文涛, 阮以宣. 化工进展, 2021, 41(6):3263-3278.
26. [26]
  PENG Ying, ZHANG Xiao-Wen, LI Mi, ZHANG Yu, WU Xiao-Yan. Chem. Ind. Eng. Prog., 2019, 38(7):3227-3242. 彭莹, 张晓文, 李密, 张宇, 吴晓燕. 化工进展, 2019, 38(7):3227-3242.
27. [27]
  ZHAO Zhong-Kun, XU Zhi-Zhi, CHEN Xin. New Chem. Mater., 2021, 49(10):76-80. 赵中昆, 许志志, 陈鑫. 化工新型材料, 2021, 49(10):76-80.
28. [28]
  KIM M, CAHILL J F, SU Y, PRATHER K A, COHEN S M. Chem. Sci., 2012, 3(1):126-130.KIM M, CAHILL J F, SU Y, PRATHER K A, COHEN S M. Chem. Sci., 2012, 3(1):126-130.
29. [29]
  HU Q, LIU Y, GU X, ZHAO Y. Chemosphere, 2017, 181:328-336.HU Q, LIU Y, GU X, ZHAO Y. Chemosphere, 2017, 181:328-336.
30. [30]
  LEE S Y, CHANG B, KIM Y J, JANG H, LEE Y J. J. Colloid Interface Sci., 2022, 613:499-514.LEE S Y, CHANG B, KIM Y J, JANG H, LEE Y J. J. Colloid Interface Sci., 2022, 613:499-514.
31. [31]
  NGUYEN T T Q, LOGANATHAN P, NGUYEN T V, VIGNESWARAN S. Environ. Sci. Pollut. Res., 2020, 27(5):5490- 5502.NGUYEN T T Q, LOGANATHAN P, NGUYEN T V, VIGNESWARAN S. Environ. Sci. Pollut. Res., 2020, 27(5):5490- 5502.
32. [32]
  ZHANG Wei-Jie, CHEN Jin-Ping, YU Tian-Jun, ZENG Yi, GUO Xu-Dong, WANG Shuang-Qing, YANG Guo-Qiang, LI Yi. Chin. J. Anal. Chem., 2021, 49(10):1750-1757. 张卫杰, 陈金平, 于天君, 曾毅, 郭旭东, 王双青, 杨国强, 李嫕. 分析化学, 2021, 49(10):1750-1757.
33. [33]
  LUO Hai-Cui, ZHOU Yue-Fei. J. Green Sci. Technol., 2020, (14):105-107. 罗海翠, 周跃飞. 绿色科技, 2020, (14):105-107.
34. [34]
  ZHANG Jin-Yao, LI Xiao-Ning, XIE Hong-Tian, XIAO Hui-Ning, PAN Yuan-Feng. Guangdong Chem. Ind., 2019, 7(46):42-45. 张金瑶, 李萧宁, 解鸿天, 肖惠宁, 潘远凤. 广东化工, 2019, 7(46):42-45.
35. [35]
  LIU Si-Yan, YANG Xiao, FENG Yi-Tao, YAN Xiu-Lan. Acta Sci. Circumstantiae, 2022, 42(3):418-430. 刘思言, 杨潇, 冯依涛, 闫秀兰. 环境科学学报, 2022, 42(3):418-430.
36. [36]
  DONG Shuang-Kuai, JIA Hong-Tao, WU Fu-Fei. J. Water Resour. Water Eng., 2020, 31(5):51-61. 董双快, 贾宏涛, 吴福飞. 水资源与水工程学报, 2020, 31(5):51-61.
37. [37]
  DENG Sheng, HU Yu-Han, YANG Yu, HAN Xu, XIA Fu, XIAO Han, JU Tian-Yu, WU Shu-Xuan, XU Xiang-Jian, JIANG Yong-Hai. Res. Environ. Sci., 2022, 35(11):2435-2446. 邓圣, 胡宇晗, 杨昱, 韩旭, 夏甫, 肖翰, 鞠天宇, 吴叔璇, 徐祥健, 姜永海. 环境科学研究, 2022, 35(11):2435-2446.
38. [38]
  WU L K, WU H, ZHANG H B, CAO H Z, HOU G Y, TANG Y P, ZHENG G Q. Chem. Eng. J., 2018, 334:1808-1819.WU L K, WU H, ZHANG H B, CAO H Z, HOU G Y, TANG Y P, ZHENG G Q. Chem. Eng. J., 2018, 334:1808-1819.
39. [39]
  LIU T, ZHANG Z, WANG Z, WANG Z L, BUSH R. RSC Adv., 2019, 9(67):39475-39487.LIU T, ZHANG Z, WANG Z, WANG Z L, BUSH R. RSC Adv., 2019, 9(67):39475-39487.

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

锆基金属有机框架与Fe₂O₃复合材料对砷的吸附及机理研究

通讯作者: 余文婷,E-mail:wtyu@cugb.edu.cn

English

Characteristics and Mechanism Study of Arsenic Adsorption on Composite Material of Zr-based Metal Organic Framework and Fe₂O₃

Corresponding author: YU Weng-Ting, wtyu@cugb.edu.cn

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通讯作者: 余文婷,E-mail:wtyu@cugb.edu.cn

English

Characteristics and Mechanism Study of Arsenic Adsorption on Composite Material of Zr-based Metal Organic Framework and Fe2O3

Corresponding author: YU Weng-Ting, wtyu@cugb.edu.cn

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