Fe3O4负载Ti3C2Tx对Pb(II)的吸附性能研究

doi:10.15541/jim20220627

无机材料学报 ›› 2023, Vol. 38 ›› Issue (5): 521-528.DOI: 10.15541/jim20220627

所属专题：【能源环境】水体污染物去除(202309)；【信息功能】Max层状材料、MXene及其他二维材料(202309)

Fe₃O₄负载Ti₃C₂T_x对Pb(II)的吸附性能研究

王世怡¹^,²(), 冯爱虎², 李晓燕¹(), 于云²()

1.上海理工大学材料与化学学院, 上海200093
2.中国科学院上海硅酸盐研究所, 中国科学院特种无机涂层重点实验室, 上海 201899

收稿日期:2022-10-25 修回日期:2022-12-02 出版日期:2023-01-11 网络出版日期:2023-01-11
通讯作者: 李晓燕, 副教授. E-mail: lixiaoyan@usst.edu.cn;
于云, 研究员. E-mail: yunyush@mail.sic.ac.cn
作者简介:王世怡(1996-), 女, 硕士研究生. E-mail: wsysues051115114@163.com

Pb (II) Adsorption Process of Fe₃O₄ Supported Ti₃C₂T_x

WANG Shiyi¹^,²(), FENG Aihu², LI Xiaoyan¹(), YU Yun²()

1. School of Material and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China
2. Key Laboratory of Inorganic Coating Materials CAS, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 201899, China

Received:2022-10-25 Revised:2022-12-02 Published:2023-01-11 Online:2023-01-11
Contact: LI Xiaoyan, associate professor. E-mail: lixiaoyan@usst.edu.cn;
YU Yun, professor. E-mail: yunyush@mail.sic.ac.cn
About author:WANG Shiyi (1996-), female, Master candidate. E-mail: wsysues051115114@163.com

摘要/Abstract

摘要：

Ti₃C₂T_x MXene材料具有二维层状结构及丰富的表面官能团, 是一种非常有潜力的重金属离子吸附材料, 但其层间距较小, 且在水溶液中的稳定性较差。本工作探索了Ti₃C₂T_x的改性策略, 提高其化学稳定性与离子吸附容量, 利用一步水热方法制备出不同Fe₃O₄掺杂量的Fe₃O₄-Ti₃C₂T_x(FeMX)复合吸附剂材料。研究结果表明：FeMX吸附剂对Pb(II)的理论饱和吸附量可达到210.54 mg/g。研究进一步揭示了FeMX材料对Pb(II)离子的吸附机理, Fe₃O₄纳米颗粒均匀分散、插层在Ti₃C₂T_x纳米片层间, 有效增加了Ti₃C₂T_x纳米片的比表面积与层间距, 提高了对Pb(II)的去除能力。本研究可为发展优异重金属离子吸附特性的MXene基复合材料提供基础数据。

关键词: Mxene, Fe₃O₄纳米颗粒, 重金属离子吸附, 稳定性

Abstract:

Ti₃C₂T_x MXene is a potential adsorbent of heavy metal ions due to its two-dimensional layered structure and abundant surface functional groups. However, it has disadvantages of limited layer spacing and poor stability in aqueous solution. Here, the modification strategy of Ti₃C₂T_x was explored to improve its chemical stability and ion adsorption capacity among which Fe₃O₄-Ti₃C₂T_x(FeMX) adsorbent with different doping amounts of Fe₃O₄ were prepared by one-step hydrothermal method. The results showed that the maximum theoretical Pb(II) adsorption capacity of FeMX adsorbent could reach 210.54 mg/g. Its adsorption mechanism was further revealed that Fe₃O₄ nanoparticles were evenly dispersed and intercalated between Ti₃C₂T_x nanosheets, which effectively increased specific surface area and layer spacing of Ti₃C₂T_x nanosheets, leading to improving Pb(II) removal ability. Therefore, this study provides a promising route for developing MXene matrix composites with excellent heavy metal ion adsorption properties.

Key words: MXene, Fe₃O₄ nanoparticle, heavy metal ion adsorption, stability

中图分类号:

TB32

王世怡, 冯爱虎, 李晓燕, 于云. Fe₃O₄负载Ti₃C₂T_x对Pb(II)的吸附性能研究[J]. 无机材料学报, 2023, 38(5): 521-528.

WANG Shiyi, FENG Aihu, LI Xiaoyan, YU Yun. Pb (II) Adsorption Process of Fe₃O₄ Supported Ti₃C₂T_x[J]. Journal of Inorganic Materials, 2023, 38(5): 521-528.

图/表 13

图S1 (a)Ti3C2Tx MXene和(b)Fe3O4-MXene的制备流程

Fig. S1 Preparation process of Ti3C2Tx Mxene (a) and Fe3O4-Mxene (b)

图1 Ti3C2Tx MXene、FeMX0.5-1、FeMX1-1、FeMX2-1样品的XRD图谱

Fig. 1 XRD patterns of Ti3C2Tx MXene, FeMX0.5-1, FeMX1-1 and FeMX2-1 samples (b) Enlarged XRD patterns of (002) crystalline

图2 (a)Fe3O4掺杂Ti3C2Tx MXene示意图; Ti3AlC2(b)、Ti3C2Tx(c)和FeMX1-1(d)样品SEM照片; (e)FeMX1-1样品不同元素分布情况

Fig. 2 (a) Diagram of Ti3C2Tx MXene doped with Fe3O4; SEM images of (b)Ti3AlC2, (c)Ti3C2Tx and (d) FeMX1-1 sample; (e)Elements distributions of FeMX1-1 sample Colorful figures are available on website

图3 不同FeMX样品的氮气吸附-脱附等温曲线

Fig. 3 Nitrogen adsorption-desorption isotherms of different FeMX samples

图4 (a)MXene和FeMX样品的XPS全谱; MXene材料的(b)O1s和(c)Ti2p图谱; FeMX复合材料的(d)Fe2p, (e)O1s和(f)Ti2p图谱

Fig. 4 (a) XPS spectra of FeMX before and after doping; (b) O1s and (c) Ti2p spectra of MXene materials; (d) Fe2p, (e) O1s and (f) Ti2p spectra of FeMX composite

图5 不同温度下FeMX1-1对Pb(II)的吸附性能

Fig. 5 Pb(II) adsorption properties of FeMX1-1 at different temperatures

表S1 不同温度下FeMX1-1对Pb(II)的吸附的Langmuir和Freundlich等温吸附模型的拟合参数

Table 1 Fitting parameters of Langmuir and Freundlich isothermal adsorption models for Pb (II) adsorption by FeMX1-1 at different temperatures

Temperature	Langmiur			Freundlich
Temperature	K_L	Q_m/(mg·g^-1)	R²	K_F	n	R²
30 ℃	0.05	110.54	0.8327	32.80	0.20	0.9881
40 ℃	0.21	126.04	0.8854	76.09	0.12	0.9435
50 ℃	0.29	120.24	0.9190	62.61	0.09	0.9934

图6 不同掺杂比例FeMX的吸附等温线(a)和吸附动力学曲线(b)

Fig. 6 (a) Adsorption isotherms and (b) adsorption kinetics curves of FeMX with different doping ratios

表S2 不同掺杂比例FeMX对Pb(II)的吸附的Langmuir和Freundlich等温吸附模型的拟合参数

Table S2 Fitting parameters of Langmuir and Freundlich isothermal adsorption models for Pb (II) adsorption by FeMX with different doping ratios

Absorbance	Langmiur			Freundlich
Absorbance	K_L	Q_m/(mg·g^-1)	R²	K_F	n	R²
MXene	0.0177	110.23	0.86006	15.8026	0.30	0.9106
FeMX0.5-1	0.1652	149.63	0.99028	67.9776	0.14	0.90833
FeMX1-1	0.2781	126.04	0.88536	76.0907	0.09	0.94345
FeMX2-1	0.0139	210.54	0.97478	22.1793	0.36	0.91117

表S3 不同掺杂比例FeMX复合材料对Pb(II)的吸附的拟一阶和拟二阶动力学吸附模型的拟合参数

Table S3 Fitting parameters of pseudo-first-order and pseudo-second-order kinetic adsorption models for Pb (II) adsorption by FeMX composites with different doping ratios

Absorbance	Pseudo first-order reaction			Pseudo second-order reaction
Absorbance	k₁/min^-1	Q_e/(mg·g^-1)	R²	k₂/(g·(mg·min)^-1)	Q_e/(mg·g^-1)	R²
MXene	2.0966	104.22	0.98786	0.4378	108.85	0.99402
FeMX0.5-1	0.6308	173.65	0.95009	0.0039	201.10	0.98103
FeMX1-1	0.7447	148.66	0.90406	0.0053	171.57	0.95077
FeMX2-1	1.1093	184.59	0.97027	0.0076	204.46	0.99135

图S2 pH与离子强度对FeMX2-1吸附Pb(II)能力的影响

Fig. S2 Effects of pH and ionic strength on Pb(II) adsorption capacity of FeMX2-1

图7 (a)FeMX1-1样品吸附Pb(II)前后XPS全谱; FeMX1-1样品吸附Pb(II)后的(b)Pb4f和(c)O1s图谱; (d)FeMX1-1样品吸附Pb(II)前后的Na1s图谱

Fig. 7 (a) XPS spectra of FeMX before and after Pb (II) adsorption ; (b) Pb4f and (c) O1s spectra of FeMX1-1 sample after Pb(II) adsorption; (d)Na1s spectra of FeMX1-1 sample before and after Pb(II) adsorption Colorful figures are available on website

表S4 现有吸附材料对Pb(II)的吸附性能与FeMX的对比

Table S4 Comparison of Pb(II) adsorption properties of existing adsorption materials and FeMX

Absorbance	Condition	Adsorption property/ (mg·g^-1)	Ref.
Zeolite A based on blast furnace slag	Shake for 60 min at room temperature, C₀=50 mg/L	39.37	[S1]
MXene (Ti₃C₂T_x)	T=293 K, pH 6, C₀=2 mg/L, 2 min contact time	~90	[S2]
Bead-supported MnFe₂O₄nanoparticles	T=298 K, pH 5, C₀= 20 mg/L, 2 h equilibrium time	11.98	[S3]
Polyhydroxyl-aluminum	T=298 K, shake for 270 min, C₀=1500 mg/L, 150 min equilibrium time	3.99	[S4]
Peanut shell-based biochar	T=293 K, pH 5.5, C₀=100 mg/L, 180 min contact time	56.5	[S5]
MnO₂ modified magnetic graphitic carbon nitride composite	T=298 K, pH 6, C₀=250 mg/L, shake for 270 min	187.6	[S6]
FeMX2-1	T=313 K, pH 6, C₀=500 mg/L, 3 h equilibrium time	210.54	This work

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Fe₃O₄负载Ti₃C₂T_x对Pb(II)的吸附性能研究

Pb (II) Adsorption Process of Fe₃O₄ Supported Ti₃C₂T_x

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