不同pH条件下硫化钼纳米片吸附Cd(II)的微观机制研究

doi:10.15541/jim20190381

无机材料学报 ›› 2020, Vol. 35 ›› Issue (3): 293-300.DOI: 10.15541/jim20190381 CSTR: 32189.14.10.15541/jim20190381

所属专题： 2020年环境材料论文精选(二)重金属元素去除

不同pH条件下硫化钼纳米片吸附Cd(II)的微观机制研究

董丽佳¹,郭筱洁²,李雪¹,陈朝贵¹,金阳¹(),AHMED Alsaedi³,TASAWAr Hayat^3,⁴,赵轻舟⁵,盛国栋⁶()

^1. 绍兴文理学院生命科学院, 绍兴 312000
^2. 杭州电子大学材料与环境工程学院, 杭州 310018
^3. NAAM Research Group, Department of Mathematics, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia
^4. Department of Mathematics, Quaid-I-Azam University, Islamabad 44000, Pakistan
^5. 中国科学院大学资源与环境学院, 北京 100049
^6. 绍兴文理学院化学与化工学院, 绍兴 312000

收稿日期:2019-07-24 修回日期:2019-09-11 出版日期:2020-03-20 网络出版日期:2019-09-20
作者简介:董丽佳(1984-), 女, 博士. E-mail: Donglijia@126.com

Microscopic Insights into pH-dependent Adsorption of Cd(II) on Molybdenum Disulfide Nanosheets

DONG Lijia¹,GUO Xiaojie²,LI Xue¹,CHEN Chaogui¹,JIN Yang¹(),AHMED Alsaedi³,TASAWAR Hayat^3,⁴,ZHAO Qingzhou⁵,SHENG Guodong⁶()

^1. School of Life Science, Shaoxing University, Shaoxing 312000, China
^2. College of Materials & Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, China
^3. NAAM Research Group, Department of Mathematics, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia
^4. Department of Mathematics, Quaid-I-Azam University, Islamabad 44000, Pakistan
^5. College of Resources and Environment, University of Chinese Academy of Sciences, Beijing 100049, China
^6. College of Chemistry and Chemical Engineering, Shaoxing Univeristry, Shaoxing 312000, China

Received:2019-07-24 Revised:2019-09-11 Published:2020-03-20 Online:2019-09-20
About author:DONG Lijia(1984-), female, PhD. E-mail: Donglijia@126.com
Supported by:
National Natural Science Foundation of China(31700476)

摘要/Abstract

摘要：

本研究结合静态实验和X射线吸收精细结构谱学(EXAFS)评估了硫化钼纳米片对重金属Cd(II)的吸附行为和微观机制。结果表明: Cd(II)在硫化钼纳米片上的吸附受溶液pH、反应时间和温度的显著影响, 但不受离子强度的影响。在pH 3.3~9.6范围内, pH升高显著促进了硫化钼对Cd(II)的吸附量, 但不改变吸收速率、吸附等温线和热力学。二级动力学模型能更好地拟合该吸附平衡, 且内表面颗粒扩散模型显示了吸附过程中的三个典型阶段。等温线和热力学分析说明Cd(II)在硫化钼上的吸附是异质性的、自发的、吸热的和不可逆的过程。EXAFS光谱学分析揭示了该吸附存在两种类型: 在较低的pH(3.56, 6.48)条件下, 内表面络合以Cd-S配位键为主; 在较高的pH(9.57)条件下, 出现Cd(OH)₂沉淀, 且配位键以Cd-O和Cd-Cd的形式存在。这些研究结果对于评估重金属离子和硫化钼纳米片在分子水平上的作用机理提供了新的视野。

关键词: 硫化钼纳米片, pH, 微观结构, EXAFS, Cd(II)

Abstract:

Herein, the retention mechanisms and microstructure of Cd(II) on MoS₂nanosheets were evaluated by batch experiments and EXAFS technology. The sorption of Cd(II) on MoS₂was strongly affected by solution pH, contact time, and temperature, but not by the ionic strength. The solution pH could only promote the sorption capacity, but does not improve the sorption rates and change the sorption isotherms and thermodynamics in the pH range of 3.3-9.6. The pseudo-second-order model could fit the equilibrium data better and the intra-particle diffusion model showed three typical stages in the sorption process. The isotherms and thermodynamics analysis indicated that the heterogeneity sorption of Cd(II) onto MoS₂was a spontaneous, endothermic, and irreversible process. The EXAFS spectra revealed the coexistence of two sorption types. The inner-sphere complexation was formed in the form of Cd-S bond at lower pH (3.56, 6.48), while the Cd(OH)₂precipitation occurred in the form of Cd-O and Cd-Cd bonds at higher pH (9.57). These results provide new insights into the interaction mechanisms between metal ions and MoS₂ nanosheets.

Key words: MoS₂ nanosheets, pH, microstructure, EXAFS, cadmium(II)

中图分类号:

TQ174

董丽佳, 郭筱洁, 李雪, 陈朝贵, 金阳, AHMED Alsaedi, TASAWAr Hayat, 赵轻舟, 盛国栋. 不同pH条件下硫化钼纳米片吸附Cd(II)的微观机制研究[J]. 无机材料学报, 2020, 35(3): 293-300.

DONG Lijia, GUO Xiaojie, LI Xue, CHEN Chaogui, JIN Yang, AHMED Alsaedi, TASAWAR Hayat, ZHAO Qingzhou, SHENG Guodong. Microscopic Insights into pH-dependent Adsorption of Cd(II) on Molybdenum Disulfide Nanosheets[J]. Journal of Inorganic Materials, 2020, 35(3): 293-300.

图/表 13

Fig. S1 SEM image (a), TEM image (b), XRD pattern (c), FT-IR spectrum (d), Zeta potentials (e), and height cross-section profile (inset) and corresponding AFM image (f) of MoS2 samples

Fig. 1 SEM image (a), EDX spectra, and corresponding elemental maps (b) for MoS2 nanosheets

Fig. 2 Effects of pH and ionic strength on Cd(II) adsoprtion onto MoS2 nanosheets Cd(II) initial concentration=10 mg/L, m/V=0.15 g/L, T=293 K

Fig. 3 Cd(II) adsorption on MoS2 nanosheets as a function of contact time (a) and the fitting of pseudo-first-order kinetic model (b), pseudo-second-order kinetic model (c) and intra-particle diffusion model (d) at different pH Cd(II) initial concentration=10 mg/L, m/V=0.15 g/L, I=0.01 mol/L NaNO3, T=293 K

Fig. S2 Adsorption isotherms (a) and fitting results of Langmuir (b) and Freundlich (c) sorption isotherms of Cd(II) sorption on MoS2 at different temperatures and different pH Cd(II) initial concentration=10 mg/L, m/V=0.15 g/L, I = 0.01 mol/L NaNO3

Fig. S3 Linear plots of lnKd versus Ce for Cd(II) at different temperatures and different pH(a), and linear regression plots of lnKθ versus 1/T for Cd(II) sorption on MoS2 at different pH(b) Cd(II) initial concentration=10 mg/L, m/V=0.15 g/L, I=0.01 mol/L NaNO3

Table S1 Parameters of Langmuir and Freundlich equations for the sorption of Cd(II) onto MoS2 at different temperatures and different pH

	pH	T/K	K_F/(mg^1-ⁿ·Lⁿ∙g^-1)	n	R²
Freundlich equation	4.55	293	1.624	1.440	0.887
		313	4.256	1.160	0.881
		333	7.461	1.052	0.904
	5.34	293	9.363	0.899	0.801
		313	21.627	0.603	0.907
		333	32.734	0.526	0.939
	6.12	293	17.298	0.650	0.812
		313	28.054	0.542	0.935
		333	34.119	0.499	0.919
	pH	T/K	q_max/(mg∙g^-1)	K_L/(L∙mg^-1)	R²
Langmuir equation	4.55	293	0.040	64.516	0.299
		313	0.016	305.157	0.069
		333	0.001	754.717	0.017
	5.34	293	0.036	262.536	0.162
		313	0.132	149.276	0.918
		333	0.236	147.580	0.978
	6.12	293	0.114	140.449	0.759
		313	0.172	152.022	0.974
		333	0.224	151.492	0.978

Table 1 Parameters of kinetic models for the adsorption of Cd(II) on MoS2 as a function of pH

	pH	q_e/(mg·g^-1)	k₁/h^-1	R²
	4.55	33.023	0.059	0.9896
Pseudo-first- order model	5.34	23.903	0.053	0.9069
	6.12	41.777	0.074	0.9835
	pH	q_e/(mg·g^-1)	k₂/(g·mg^-1·h^-1)	R²
	4.55	35.638	0.038	0.9869
Pseudo-second- order model	5.34	42.230	0.078	0.9978
	6.12	52.659	0.077	0.9986
	pH	C/(mg·L^-1)	k_i/(g·mg^-1·h^-1/2)	R²
	4.55	19.985	2.628	0.942
Intra-particle diffusion model	5.34	32.500	1.877	0.987
	6.12	39.759	3.004	0.980

Fig. 4 Normalized, background-subtracted and k3-weighted EXAFS spectra (a) and corresponding RSF magnitudes and imaginary parts (b) of Cd reference samples

Fig. S4 EXAFS spectra (a) and the corresponding RSF magnitudes and imaginary parts (b) of Cd reference samples

Fig. S5 Schematic representation of possible sorption sites on the surface of MoS2

Table S2 Parameters of thermodynamics for adsorption of Cd(II) onto MoS2 at 3 temperatures and different pH

pH	T	ΔG^θ/(kJ/mg)	ΔS^θ/(J∙mg^-1· K^-1)	ΔH^θ/(kJ∙mg^-1)
4.55	293	-19.291	143.66592	22.803
	313	-22.333		22.635
	333	-25.022		22.818
5.34	293	-22.331	147.73978	20.957
	313	-25.312		20.930
	333	-28.239		20.958
6.12	293	-23.412	121.71696	12.251
	313	-25.986		12.111
	333	-28.267		12.265

Table s3 Structural parameters of Cd(II) reference and sorption samples

Sample conditions	shells	R/nm	CN	σ²/nm²
Cd(NO₃)₂(aq)	Cd-O	0.233(4)	6.2(3)	0.0010(1)
Cd(OH)₂	Cd-O	0.238(2)	6.1(4)	0.0014(5)
Cd(OH)₂	Cd-Cd	0.359(3)	5.9(4)	0.0032(5)
CdS	Cd-S	0.259(1)	4.1(3)	0.0024(2)
pH 3.56, sorption	Cd-S	0.255(2)	3.9(5)	0.0027(3)
pH 6.48, sorption	Cd-S	0.257(1)	3.8(4)	0.0023(5)
pH 9.57, sorption	Cd-O	0..34(5)	5.9(6)	0.0016(3)
pH 9.57, sorption	Cd-Cd	0.357(3)	5.6(4)	0.0037(2)

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不同pH条件下硫化钼纳米片吸附Cd(II)的微观机制研究

Microscopic Insights into pH-dependent Adsorption of Cd(II) on Molybdenum Disulfide Nanosheets

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