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HYDROMETALLURGY · 2023 · IF 4.7

Highly efficient and selective adsorption of palladium(II) from simulated nuclear waste solution using Amberlite XAD-7 resin impregnated with a phenanthroline-derived diamide

Qian Xiao,Xueyu Wang,Lianjun Song,Fengfeng Li,Qiuju Li,Lanlan He,Zhen Shen,Fangxiang Luo,Songdong Ding

The increasing demand and limited natural resources for rare precious metal palladium render its separation and recovery from secondary sources such as acidic nuclear liquid waste greatly interesting. Herein, a novel Et-Tol-DAPhen extraction resin was prepared by impregnating Amberlite XAD-7 resin with a phenanthroline-derived diamide extractant N , N ′-diethyl- N , N ′-ditolyl-2,9-diamide-1,10-phenanthroline (Et-Tol-DAPhen), and the adsorption behavior of this new extraction resin towards Pd 2+ in HNO 3 solution was investigated through the batch and column experiments. The Et-Tol-DAPhen extraction resin exhibited strong adsorbability, high adsorption capacity, excellent selectivity and good reusability for Pd 2+ in highly acidic HNO 3 solution. In addition, the pseudo-second-order and Langmuir models were applied to understand the adsorption process of Pd 2+ on Et-Tol-DAPhen extraction resin, respectively. It demonstrated the characteristics of a uniform single-layer chemisorption . The maximum uptake capacity could reach as high as 74.6 mg g − 1 for Pd 2+ in 3.0 mol/L HNO 3 solution which is much higher than most adsorbent materials of palladium reported before. Furthermore, Et-Tol-DAPhen extraction resin could selectively uptake Pd 2+ from a simulated acidic nuclear waste solution containing 20 different kinds of ions with the separation factor SF Pd/M values as high as 100 to 10,000. Moreover, although the adsorption efficiency had a slight decrease after 5 times of adsorption-desorption process, it still remained at a high level. This new extraction resin displayed a potential application prospect in the field of separation and recovery of Pd 2+ from acidic nuclear liquid waste .

研究领域: 化学工程 · 环境科学
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MATERIALS CHEMISTRY AND PHYSICS · 2018 · IF 2.21

Adsorption of palladium(II) from aqueous solution using nanosilica modified with imidazoline groups

Bing Zhang,Likang Fu,Shixing Wang,Libo Zhang

Nanosilica was functionalized with imidazoline groups and used as a new sorbent to recycle Pd(II) from aqueous solution. The sorbent was investigated by thermogravimetric analysis (TGA), transmission electron microscopy (TEM), fourier transform infrared (FT-IR) and X-ray photoelectron spectroscopy (XPS). The influence of pH, adsorption time and original Pd(II) concentration on recovery was discussed. The optimal pH value for adsorption was 4. The maximum adsorption quantity of Pd(II) was 69.6 mg/g. The coexisting ions exhibit little interference on the Pd(II) separation. The separation process of Pd(II) matches a pseudo-second-order kinetic model. The separation data obeyed best with the Langmuir isotherm model. The adsorbent exhibited good recyclability for Pd(II). Separation of Pd(II) takes place via chelation and ion-exchange. The adsorbent has wide application prospect to selectively capture Pd(II) from aqueous solutions.

研究领域: 环境科学 · 材料科学
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JOURNAL OF MOLECULAR STRUCTURE · 2020 · IF 2.463

Highly selective extraction of Pd(II) using functionalized molecule of 2-[(2-ethylhexyl)thio]benzoxazole and its Pd(II) extraction mechanism

Shaoping Feng,Kun Huang,Zhangjie Huang,Guiyang Liu,Guowei Zhang,Gaozhang Gou

ABSTRACT In view of the separation and recycling of Pd(II) from multi-metal aqueous solution, a functionalized extractant of 2-[(2-ethylhexyl)thio]benzoxazole (EHBXS) with excellent selectivity for Pd(II) was synthesized and used to extract Pd(II) for the first time. The effects of EHBXS concentration, HCl concentration, organic/aqueous (O/A) phase ratio, contact time, and regeneration of EHBXS were investigated in detail. The extraction efficiency of Pd(II) was almost 100 % while the co-extraction efficiencies of Pt(IV), Rh(III), Cu(II), Fe(III) and Ni(II) existed in the aqueous solution were less than 10 %, which indicates that EHBXS is an effective extractant and can effectively remove Pd(II) from other metals at desired extraction conditions. Thiourea ((NH 2 ) 2 CS) solution (1.0 mol/L) could be used as an effective Pd(II) stripping agent and the one-step stripping efficiency of Pd(II) was higher than 98 %. EHBXS has excellent regeneration ability and the extraction efficiency of Pd(II) with regenerated EHBXS reaches to 87% even after 7 cycles. Moreover, the coordination mechanism between EHBXS and Pd(II) has been proven via the slope method, FT-IR spectra, 1 H NMR, 13 C NMR and single X-ray diffraction. Pd(II) and EHBXS formed a 1:2 complex of Pd(EHBXS) 2 Cl 2 during extraction. Pd(II) was coordinated with two Cl atoms and two EHBXS, and thus formed Pd(EHBXS) 2 Cl 2 molecule, in which EHBXS was coordinated with Pd(II) via the N atom in the benzoxazole ring as neutral unidentate ligand.

CAS / MDL: 18908-66-2 2382-96-9
研究领域: 化学 · 环境科学
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DALTON TRANSACTIONS · 2017 ·Vol. 46 ·期 22 ·7210-7218 · IF 4.029

Extraction behaviour and mechanism of Pt(IV) and Pd(II) by liquid–liquid extraction with an ionic liquid [HBBIm]Br

Wenhui Liu,Qi Wang,Yan Zheng,Shubin Wang,Yan Yan,Yanzhao Yang

In this study, a method of one-step separation and recycling of high purity Pd(II) and Pt(IV) using an ionic liquid, 1-butyl-3-benzimidazolium bromate ([HBBIm]Br), was investigated. The effects of [HBBIm]Br concentration, initial metal concentration, and loading capacity of [HBBIm]Br were examined in detail. It was observed that [HBBIm]Br was a very effective extractant for selectively extracting Pd(II) and precipitating Pt(IV). Through selectively extracting Pd(II) and precipitating Pt(IV), each metal with high purity was separately obtained from mixed Pd(II) and Pt(IV) multi-metal solution. The method of one-step separation of Pd(II) and Pt(IV) is simple and convenient. The anion exchange mechanism between [HBBIm]Br and Pt(IV) was proven through Job's method and FTIR and 1H NMR spectroscopies. The coordination mechanism between [HBBIm]Br and Pd(II) was demonstrated via single X-ray diffraction and was found to be robust and distinct, as supported by the ab initio quantum-chemical studies. The crystals of the [PdBr2 ·2BBIm] complex were formed first. Moreover, the influence of the concentrations of hydrochloric acid, sodium chloride, and sodium nitrate on the precipitation of Pt(IV) and extraction of Pd(II) was studied herein. It was found that only the concentration of H+ could inhibit the separation of Pt(IV) because H+ could attract the anion PtCl62−; thus, the exchange (anion exchange mechanism) between the anions PtCl62− and Br− was prevented. However, both the concentration of H+ and Cl− can obviously inhibit the extraction of Pd(II) because H+ and Cl− are the reaction products and increasing their concentration can inhibit the progress of the reaction (coordination mechanism).

研究领域: 化学 · 材料科学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2016 · IF 2.653

A convenient method for determination of quizalofop-p-ethyl based on the fluorescence quenching of eosin Y in the presence of Pd(II)

Huan Wu,Yanmei Zhao,Xuanping Tan,Xiaoqing Zeng,Yuan Guo,Jidong Yang

A convenient fluorescence quenching method for determination of Quizalofop-p-ethyl(Qpe) was proposed in this paper. Eosin Y(EY) is a red dye with strong green fluorescence (λex/λem   =   519/540   nm). The interaction between EY, Pd(II) and Qpe was investigated by fluorescence spectroscopy, resonance Rayleigh scattering(RRS) and UV–Vis absorption. Based on changes in spectrum, Pd(II) associated with Qpe giving a positively charged chelate firstly, then reacted with EY through electrostatic and hydrophobic interaction formed ternary chelate could be demonstrated. Under optimum conditions, the fluorescence intensity of EY could be quenched by Qpe in the presence of Pd(II) and the RRS intensity had a remarkable enhancement, which was directly proportional to the Qpe concentration within a certain concentration range, respectively. Based on the fluorescence quenching of EY-Pd(II) system by Qpe, a novel, convenient and specific method for Qpe determination was developed. To our knowledge, this is the first fluorescence method for determination of Qpe was reported. The detection limit for Qpe was 20.3   ng/mL and the quantitative determination range was 0.04–1.0   μg/mL. The method was highly sensitive and had larger detection range compared to other methods. The influence of coexisting substances was investigated with good anti -interference ability. The new analytical method has been applied to determine of Qpe in real samples with satisfactory results.

研究领域: 分析化学 · 环境科学
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2018 · IF 3.974

The effect of biotic and abiotic environmental factors on Pd(II) adsorption and reduction by Bacillus wiedmannii MSM

Yuan Chen,Yuancai Chen,Jingyi Wu,Jianyi Zhang

In this paper, we found a bacteria ( Bacillus wiedmannii MSM) that could not only culture quickly under aerobic condition , but also can biological reduction of Pd (II) under both aerobic and anaerobic conditions. For reducing Pd (II) by Bacillus wiedmannii MSM, the best electron donor was sodium formate and the best growth time was 24 h (mid-log growth phase cells). TEM indicated that a lot of palladium nanoparticles (Pd-NPs) were mainly located in the periplasmic space of the live cells. However, the autoclaved cells could not synthesize Pd-NPs, which proved the role of enzyme in the reduction of Pd (II). A few of Pd-NPs were only formed on the surface of Cu 2+ -treated cells, which proved the main but not the only role of periplasmic hydrogenase in the reduction of Pd (II). XRD and XPS also proved that Pd-NPs could be synthesized by live cells over broad ranges of temperature (20–40 °C) and pH (pH 3.0–7.0). This may be especially useful for in situ reduction and remediation of Pd (II) for both anaerobic and aerobic wastewater.

CAS / MDL: 13820-53-6
研究领域: 环境科学 · 微生物学
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RADIOCHIMICA ACTA · 2021 ·Vol. 109 ·期 5 ·367-375 · IF 1.44

Adsorption and separation behavior of palladium(II) from simulated high-level liquid waste using a novel silica-based adsorbents

Hao Wu,Naoki Osawa,Masahiko Kubota,Seong-Yun Kim

Aiming at selective adsorption and separation of Pd(II) in nitric acid solution, a hybrid soft N and hard O donor adsorbent (TAMIA-EH+TOA)/SiO 2 –P (P = Polymer) was successfully synthesized. The adsorption performances of (TAMIA-EH+TOA)/SiO 2 –P adsorbent towards Pd(II) were systematically investigated as a function of contact time, effect of concentration of nitric acid, effect of temperature etc. Adsorption speed of Pd(II) was fairly fast and can reach equilibrium state within only 0.5 h. The distribution coefficient of Pd(II) was more than 10 3 when [HNO 3 ] = 0.1. Though it decreased gradually with an increase in the concentration of HNO 3 , the adsorption selectivity of (TAMIA-EH+TOA)/SiO 2 –P adsorbent towards Pd(II) was still significant than other co-existing metal ions in the whole HNO 3 range from 0.1 to 5 M. The adsorption isotherm of Pd(II) onto (TAMIA-EH+TOA)/SiO 2 –P adsorbent fitted well with Langmuir adsorption model but Freundlich isotherm model. The calculated results of adsorption thermodynamic parameters indicated that the adsorption process of Pd(II) was exothermic and happened in a natural way. Furthermore, the separation chromatography experiment by utilizing (TAMIA-EH+TOA)/SiO 2 –P adsorbent packed column was carried out. Based on the results of plotted elution curves, it was found that the successful recovery of Pd(II) (96.27%) was achieved by eluting with thiourea solution.

研究领域: 化学工程 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Effective and selective extraction of Au(III) and Pd(II) from practical e-waste by tridentate thioether extractants

Xuan Huang,Ming Yi,Kewen Tang

To address resources shortage and environmental degradation, noble metal recovery from e-waste is in desperate need. Herein, to achieve selective extraction of gold (Au) and palladium (Pd) from practical e-waste, a series of tridentate thioether extractants are designed with ester functional groups at both ends of the thioether. By varying the chain length of the ester alkyl, the relationship between extractant structure and performance is further explored. The results indicate that the as-introduced tridentate structure facilitate the Au(III) and Pd(II) extraction, demonstrating a complex mechanism involving both coordination substitution and ion association. Notably, the extractant with the shortest carbon chain length and smallest molecular weight delivers outstanding extraction capacities of 920.2 mg/g for Au(III) and 280.7 mg/g for Pd(II). More importantly, it exhibits superior selectivity (∼100 %) for Au(III) and Pd(II) in complex metal solutions. This work guides the design of thioether-based extractants for sustainable recovery of noble metal from practical e-waste.

研究领域: 化学工程 · 环境科学 · 材料科学
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RSC Advances · 2015 ·Vol. 5 ·期 81 ·66376-66383 · IF 3.84

Solvent extraction of palladium(II) with newly synthesized asymmetric branched alkyl sulfoxides from hydrochloric acid

Yixian Huang,Yu Tong,Chen Wang,Ke Tang,Yanzhao Yang

A group of new asymmetric branched alkyl sulfoxides was synthesized and applied in palladium(II) extraction for the first time. According to the experimental data, the concentration of hydrochloric acid in aqueous phase greatly influenced Pd(II) extraction, which could be interpreted by different mechanisms (ligand substitution mechanism at low acidity and ion association mechanism at high acidity). In regard to structure effect, the steric hindrance of branched alkyl showed remarkable influence on the extraction performance of sulfoxides. On the basis of thermodynamic analysis, it was demonstrated that higher temperature exerted positive influence on the Pd(II) extraction reaction. As for the separation of Pd(II) and Pt(IV), low concentration of hydrochloric acid was considered to be appropriate for highly effective separation. Furthermore, ammonia solution was proven to be an efficient stripping agent for palladium recovery from organic phase.

CAS / MDL: 74-83-9
研究领域: 化学 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 16 ·7695-7703 · IF 3.925

Successive preconcentration and mechanistic investigation of Au(III), Pd(II), Pt(IV) and Rh(III) via cloud point extraction using a functionalised ionic liquid

Qi Wu,Changfeng Zhao,Qinzhong Wang,Jing Liu

This study proposes the efficient separation of Au(III)/Pd(II)/Pt(IV)/Rh(III) through the 2-mercaptobenzothiazole-functionalised ionic liquid ([C6mim][2MBT]) using a cloud point extraction system. Direct cloud point extraction of Au(III) (about 99.9%) was realised without involving any functionalised ionic liquids. A significant enhancement of the Pd(II) extraction performance was found by adding rationally constructed [C6mim][2MBT]. Consequently, a fairly high extraction percentage of about 99.4% was obtained. However, further advancement of the proposed cloud point extraction showed that it could not be applied for the preconcentration of Pt(IV) and Rh(III) without adding stannous chloride, which plays a critical role in the segregation and could be adjusted by changing the hydrochloric acid concentration. Under the optimised conditions, the Rh(III) extraction process shows a high yield percentage (ca. 83.0%), where the majority of Pt(IV) was enriched in the aqueous phase. In addition, the underlying possible extraction mechanism was investigated using UV-vis, FT-IR and TEM measurements, which indicated that TX-114 acted as a solvent for the extracted metals. The developed procedure reveals efficient direct Au(III)/Pd(II)/Pt(IV)/Rh(III) separation using [C6mim][2MBT] via cloud point extraction.

CAS / MDL: 171058-17-6
研究领域: 分析化学 · 环境科学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2023 · IF 5.2

Adsorption of Pd(II) from wastewater by a functionalized metal-organic framework with aminopyridine structure: Performance and mechanism

Zhenzhen Tang,Derong Xu,Hongyu Chen,Si Tang,Chunlin He,Shunyan Ning,Min Li,Guoyuan Yuan,Shuangkou Chen,Jian Feng

Metal-organic frameworks are recognized as a new kind of potential adsorbent for wastewater treatment because of their tunable pore size, high surface area and modifiable functionality. In this work, 2,6-diaminopyridine functionalized UiO-66-NH 2 (UiO-66-DAP) was synthesized by a post-modification strategy and was applied to the adsorption of Pd(Ⅱ) from aqueous solution. The aminopyridine structure on UiO-66-DAP greatly improved the adsorption performance for Pd(II), with an adsorption capacity of 190.95 mg/g. The adsorption process of Pd(Ⅱ) on UiO-66-DAP was consistent with the pseudo-second-order kinetic model and the Langmuir adsorption isotherm . Thermodynamic studies confirmed that the adsorption process was endothermic and spontaneous. Regeneration studies showed that UiO-66-DAP was stable and recyclable. Moreover, UiO-66-DAP could maintain high selectivity to Pd(Ⅱ) even in a wastewater containing multiple interfering metal ions. According to the results of Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), zeta potential , comparative experiments and DFT calculations, the chelation and electrostatic attraction between Pd(Ⅱ) and the aminopyridine structural unit are the dominant mechanisms. Using UiO-66-DAP as an adsorbent, this study provides a promising way for the separation of palladium form wastewater.

CAS / MDL: 10312-55-7 7647-10-1
研究领域: 环境科学 · 材料科学
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JOURNAL OF MOLECULAR LIQUIDS · 2022 · IF 6.633

A separation strategy of Au(III), Pd(II) and Pt(IV) based on hydrophobic deep eutectic solvent from hydrochloric acid media

Ronghao Liu,Jinjie Hao,Yangyang Wang,Yuanyuan Meng,Yanzhao Yang

A hydrophobic deep eutectic solvent (HDES) based on lidocaine and thymol was examined for selective extraction and separation of Au(III), Pd(II) and Pt(IV) in the acidic leaching solution of secondary resources. At first, the properties of HDES were characterized by 1 H NMR, DSC, TGA, RDF and ESP to prove its suitability for extraction process. In addition, extraction behaviors, maximum extraction capacities and competitive extraction experiment were investigated to explore the extraction ability of HDES. The results show that the maximum extraction capacity of Au(III), Pd(II) and Pt(IV) reached 761.2 g/L, 98.3 g/L and 299.3 g/L, respectively. Meanwhile, their extraction efficiency was affected by the changing acidity of aqueous. And then, ion-association mechanism in the extraction process was proposed through the analysis of FT-IR. Finally, a separation process was proposed for the recovery of Au(III), Pd(II) and Pt(IV) based on acidity control and KSCN, which achieved recovery efficiency of 97.8 % Au(III), 99.9 % Pd(II) and 89.5 % Pt(IV). After collecting and regenerating the used HDES, their extraction performance of Au(III), Pd(II) and Pt(IV) were still maintained.

研究领域: 化学工程 · 材料科学
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