K+-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study※

doi:10.6023/A21120603

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (4): 476-484.DOI: 10.6023/A21120603 Previous Articles Next Articles

Special Issue: 中国科学院青年创新促进会合辑

Article

钾位铈掺杂黄钾铁矾的磷吸附特性及机理研究^※

刘俊瑞^a^,^b^,^c, 陈晶琳^d, 杨杰^b^,^c, 许肖锋^b^,^c, 李若男^b^,^c, 黄有桂^b^,^c, 陈少华^d, 叶欣^d^,^*(), 王维^b^,^c^,^*()

a 福建师范大学化学与材料学院福州 350007
b 中国科学院福建物质结构研究所中国科学院功能纳米结构设计与组装重点实验室福州 350002
c 中国科学院海西研究院厦门稀土材料研究中心厦门 361021
d 中国科学院城市环境研究所中国科学院城市污染物转化重点实验室厦门 361021

投稿日期:2021-12-30 发布日期:2022-04-28
通讯作者: 叶欣, 王维
作者简介:
^※ 庆祝中国科学院青年创新促进会十年华诞.
基金资助:
中国科学院青年创新促进会专项基金(2021302); 中国科学院青年创新促进会专项基金(2021305); 中国科学院福建物质结构研究所与中国科学院城市环境研究所融合发展基金培育项目(RHZX-2019-003)

K⁺-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study^※

Junrui Liu^a^,^b^,^c, Jinglin Chen^d, Jie Yang^b^,^c, Xiaofeng Xu^b^,^c, Ruonan Li^b^,^c, You-Gui Huang^b^,^c, Shaohua Chen^d, Xin Ye^d(), Wei Wang^b^,^c()

a College of Chemistry and Materials Science, Fujian Normal University, Fuzhou 350007, China
b CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China
c Xiamen Institute of Rare Earth Materials, Haixi Institute, Chinese Academy of Sciences, Xiamen 361021, China
d CAS Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen 361021, China

Received:2021-12-30 Published:2022-04-28
Contact: Xin Ye, Wei Wang
About author:
^※ Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
Youth Innovation Promotion Association CAS(2021302); Youth Innovation Promotion Association CAS(2021305); FJIRSM&IUE Joint Research Fund(RHZX-2019-003)

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Abstract

Jarosite is a common iron-containing mineral. Researchers have studied its application for removing aqueous pollutants, such as Cr(VI) and As(V). Surprisingly, it shows adsorption for arsenates, but little for the structurally similar phosphate ions. In this study, we prepare cerium doped jarosite and prove the successful doping of cerium at the K⁺ site by X-ray diffraction (XRD), inductively coupled plasma-optical emission spectrometry (ICP-OES), energy dispersive spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS). Phosphorus adsorption experiments show that the small amount of cerium doping (Ce content: 8.75×10^-5 mol/g) significantly improves the phosphate adsorption of jarosite, from 1.69 mg/g to 29.33 mg/g (pH=7, 24 h). The phosphate adsorption of Ce-doped jarosite exhibits good pH stability (from pH=3 to pH=11) and excellent selectivity, which is capable of maintaining more than 91% of its adsorption capacity in the presence of various competing anions, such as HCO₃^-, CO₃^2-, humic acid anion, SO₄^2-, NO₃^-, and SiO₃^2-. Further analysis reveals that the adsorption process obeys the pseudo-second order kinetic model while the adsorption isotherms represent the Freundlich isotherm. The analysis indicates that the adsorption may be a chemical adsorption process that is easy to proceed. To explore the mechanism of adsorption enhancement, we first characterize the Zeta-potential of the pure jarosite and Ce-doped jarosite. The result indicates similarity of the surface potential between the two samples, which rules out the electrostatic adsorption mechanism. Next, based on the result of anion exchange chromatography, we confirm that the cerium doping greatly increases the exchange between the sulfate groups in jarosite and the phosphate groups in solution, from 2.85 mg/g to 24.90 mg/g. Finally, XPS high-resolution spectroscopy reveals that the chemical environment of Ce changes after the phosphate adsorption, likely indicating the formation of Ce—O—P chemical bonds to achieve specific chemisorption. These results may provide insights for the modification and application of jarosite, as a new adsorbent material for treating phosphorus rich wastewater.

Key words: jarosite, rare-earth doping, adsorption, phosphate pollutant, cerium

Cite this article

Junrui Liu, Jinglin Chen, Jie Yang, Xiaofeng Xu, Ruonan Li, You-Gui Huang, Shaohua Chen, Xin Ye, Wei Wang. K⁺-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study^※[J]. Acta Chimica Sinica, 2022, 80(4): 476-484.

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Fig. & Tab. 12

Figure 1. Crystal structure of jarosite

Figure 2. X-ray diffraction pattern (XRD) of jarosite before and after cerium doping

Figure 3. Jarosite doped with cerium before and after 2θ X-ray diffraction high resolution mapping of the angle: (a) 12.5°~20.3°, (b) 27.6°~30.4°, (c) 35.8°~44.3°, (d) 45.5°~51.0°, and (e) 54.1°~54.8°

序号	样品名	晶胞参数 a/nm	晶胞参数 b/nm	晶胞参数 c/nm
1	纯黄钾铁矾	0.73198	0.73198	1.70910
2	含铈黄钾铁矾	0.73082	0.73082	1.70024

Table 1. Unit cell parameters of jarosite before and after doping

Figure 4. SEM images of jarosite before (a) and after (b) cerium doping; (c) the SEM image of a cerium-doped jarosite particle and (d) its corresponding Ce EDS mapping

Figure 5. (a) Effect of initial pH on the adsorption properties of jarosite; (b) effect of initial pH on the adsorption properties of Ce-doped jarosite

Figure 6. Kinetic data and quasi first-order and quasi second-order kinetic fitting of phosphate adsorption by Ce-doped jarosite

Figure 7. Fitting curves of Langmuir equation and Freundlich equation for the phosphate adsorption isotherm of cerium doped jarosite

Figure 8. The effect of coexisting anion on the phosphate adsorption of cerium doped jarosite

Figure 9. XPS full spectra before and after phosphate adsorption (a) pure jarosite (b) cerium doped jarosite; high resolution Ce3d spectra before (c) and after (d) the phosphate adsorption by cerium doped jarosite

Figure 10. Relationship between pH value and Zeta potential of jarosite before and after cerium doping

Figure 11. Precipitation of SO42- from the filtrate after adsorption of jarosite (a) and cerium doped jarosite (b); High resolution S 2p XPS spectra of cerium doped jarosite before (c) and after (d) phosphate adsorption

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钾位铈掺杂黄钾铁矾的磷吸附特性及机理研究^※

K⁺-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study^※

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钾位铈掺杂黄钾铁矾的磷吸附特性及机理研究※

K+-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study※

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钾位铈掺杂黄钾铁矾的磷吸附特性及机理研究^※

K⁺-Site Ce-Doped Jarosite for Phosphate Adsorption: a Mechanism Study^※