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JOURNAL OF POLYMERS AND THE ENVIRONMENT · 2024 · IF 4.7

Fabrication of Kaolin Loaded Chitosan Hybrid Nanofibers for Recovery of Precious Palladium Cations from Aqueous Solution

Liu Yaqing,Cui Yixin,Meng Huibiao,Long Ke,Shao Linjun,Xing Guiying

Palladium plays an important role in modern industry, agriculture and medicine. The direct discharge of palladium results in serious environmental pollution and loses of precious palladium metal. Herein, kaolin/chitosan hybrid nanofibers were successfully prepared to recover Pd 2+ cations from aqueous solution. Chitosan and kaolin mixture was first electrospun into nanofibers with citric acid as the in situ crosslinking agent and poly(ethylene oxide) as the co-spinning polymer. Then, the chitosan molecules in these hybrid nanofibers were in situ crosslinked by critic acid at elevated temperatures to endow these nanofibers with excellent solvent resistance. Their structure characterization was conducted by Fourier-transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM) and positron annihilation lifetime spectroscopy (PLAS). The adsorption performances of these fibrous adsorbents were carefully investigated and optimized (e.g. kaolin content, temperature, pH of solution and initial Pd 2+ concentration). The adsorption results demonstrated that incorporation of kaolin powders into the nanofibers could enhance the adsorption capacity from 31 mg/g to 64 mg/g. Thermodynamic parameters studies revealed the endothermic and spontaneous natures of the adsorption process of Pd 2+ cations on these hybrid nanofibers. The Pd 2+ adsorption behavior of this fibrous adsorbent fitted well with the second-order kinetic model, suggesting the chemical adsorption behavior of Pd 2+ cations on this fibrous adsorbent. Moreover, this fibrous adsorbent can be easily regenerated and reused at least three times without significant loss of initial adsorption capacities. These results clearly indicate that this fibrous chitosan/kaolin hybrid absorbent holds great potential in the recovery of precious palladium cations from aqueous solution.

研究领域: 材料科学 · 环境科学
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Arabian Journal of Chemistry · 2020 · IF 4.762

Adsorption behavior of Pd(II) ions from aqueous solution onto pyromellitic acid modified-UiO-66-NH2

Zhen Huang,Chen Wang,Jiling Zhao,Shixing Wang,Yang Zhou,Libo Zhang

A new adsorbent was successfully fabricated by chemically linking pyromellitic acid onto a zirconium-based metal-organic framework composite for selective adsorption of Pd(II) from an aqueous solution. The adsorbent was characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller equation and scanning electron microscope. The adsorption capacity, selectivity and repeatability of the adsorbent were tested by batch experiments. The optimum pH was 2.0, and the maximum adsorption capacity at room temperature was 226.1 mg/g. In the kinetic experiments, the adsorption process achieved equilibrium within 5 h and generally conformed to the quasi-second kinetics and Freundlich isotherm model. The N-H and O H groups on the adsorbent interacted with Pd(II) by electrostatic and coordination action. The adsorbent maintained excellent adsorption capacity after at least 5 cycles. At the same time, the selectivity of the adsorbent in aqueous solution is excellent from interfering ions. Therefore, the new adsorbent will have an obvious application prospect on the recovery of palladium.

CAS / MDL: 10312-55-7
研究领域: 化学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2017 · IF 6.216

Biorecovery mechanism of palladium as nanoparticles by Enterococcus faecalis: From biosorption to bioreduction

Jiaying Cui,Nengwu Zhu,Naixin Kang,Chitam Ha,Chaohong Shi,Pingxiao Wu

In this study, the biorecovery mechanism of palladium ions (Pd(II)) as palladium nanoparticles by Enterococcus faecalis ( E. faecalis ), a typical Gram-positive bacterium, was explored from acting force, participated substance and reaction process. The XRD and TEM analysis showed that the deposit locations of Pd-NPs depended on the transfer of Pd(II) in biosorption, and the process was invested by effect factors and theory models of isotherm, thermodynamics, and kinetics, which was a spontaneous endothermic process fitted well by Langmuir isotherm and pseudo-second order kinetics. In addition, the surface characteristic changes of E. faecalis during biorecovery of Pd(II) were compared by FTIR and XPS, and it found that carboxyl groups, hydroxyl groups and amine groups were the main participated functional groups in biorecovery. Furthermore, the contrary pH change between biosorption and bioreduction combined with above results proved that electrostatic interaction, complex formation of Pd(II) on the cell and intracellular uptake were the acting forces for biosorption, and the bioreduction of adsorbed Pd(II) was via the hydrolysis and oxidation of sodium formate to deliver electron. Therefore, the biorecovery mechanism of Pd(II) can be divided into the biosorption from solution to cells, and then the bioreduction and crystallization in situ by the electron donor and the link frame of E. faecalis .

CAS / MDL: 13820-53-6
研究领域: 微生物学 · 环境科学 · 材料科学
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DYES AND PIGMENTS · 2017 · IF 3.473

Highly sensitive and selective ESIPT-based fluorescent probes for detection of Pd2+ with large Stocks shifts

Tiantian Chen,Tingwen Wei,Zhijie Zhang,Yahui Chen,Jian Qiang,Fang Wang,Xiaoqiang Chen

Highly sensitive and selective fluorescent probes 1 and 2 for detection of palladium ions (Pd 2+ ) were synthesized based on excited-state intramolecular proton transfer process (ESIPT) using 2-(2′-hydroxy-)benzothiazole moiety. Different metal ions were used to optimize their sensitivity and selectivity but best results were obtained with Pd 2+ . Probe 1 produced green fluorescence with Stokes shift of about 163 nm upon addition of Pd 2+ , whereas probe 2 displayed red fluorescence with a large Stokes shift of about 217 nm under similar conditions. The detection limits of 1 and 2 to Pd 2+ were found to be 285 nM and 14.6 nM, respectively. Mechanistic aspects of probes 1 and 2 were discussed to account for the optical changes leading to the strong ESIPT fluorescence in very short duration. Furthermore, the portable test strips were also prepared by direct deposition of the probe molecules onto the filter paper to detect the lowest possible ppm levels of Pd 2+ .

研究领域: 分析化学 · 材料科学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2020 · IF 3.232

A single molecular sensor for selective and differential colorimetric/ratiometric detection of Cu2+ and Pd2+ in 100% aqueous solution

Wenjun Zhou,Qiang Gao,Darui Liu,Chen Li,Shu Liu,Kaisheng Xia,Bo Han,Chenggang Zhou

A novel salicylaldehyde bis-Schiff-base probe decorated with imidazolium ionic liquid moieties at both ends (SAS-IMIs) was designed and facilely synthesized as a colorimetric/ratiometric sensor to visually detect Cu 2+ and Pd 2+ in pure aqueous media. Due to the positively charged characters of its head and tail, the SAS-IMIs exhibited high water solubility with a potential advantage in minimizing the self-aggregation. More importantly, simply by varying the solution pH, colorimetric/ratiometric sensing detection of individual metal ion (Cu 2+ or Pd 2+ ) was realized without any mutual interference. Subsequently, sensitive, selective, and differential detections for Cu 2+ (LOD: 0.080 μM) and Pd 2+ (LOD: 0.076 μM) in 100% aqueous solutions were achieved, which proved to be applicable for real water samples. Results from density functional theory (DFT) calculations unveiled the Cu 2+ /Pd 2+ -binding properties of SAS-IMIs, which were in accordance with the experimental observations. Furthermore, a SAS-IMIs-based solid phase sensor was fabricated, which manifested satisfactory detection abilities for Cu 2+ and Pd 2+ .

研究领域: 分析化学 · 环境科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2024 · IF 3.2

Efficient palladium ion adsorption and catalyst preparation from pharmaceutical wastewater using amino-functionalized Ti3C2

Dancheng Zhu,Yonghui Lin,Changhui Chen,Hao Xu,Jiabin Shen,Jun Qiao,Chao Shen

This paper reports the recovery and reuse of Pd ions from pharmaceutical wastewater using amino-modified Ti 3 C 2 . Ti 3 C 2 –NH 2 was synthesized by modifying (3-aminopropyl)triethoxysilane and the successful substitution of some surface functional groups of Ti 3 C 2 ; the decrease in material thickness was verified by characterization. This study revealed that the presence of amino groups significantly enhanced the Pd(II) adsorption capacity of Ti 3 C 2 . The effects of the adsorbent material, adsorbent dosage, pH, initial concentration of Pd ions, presence of competing cations, and contact time on the adsorption performance were investigated. The maximum adsorption capacity of 20 mg of Ti 3 C 2 –NH 2 was 986.65 mg/g in 100 ml of a Pd-ion solution with an initial concentration of 200 mg/l at pH 3. A pseudo-second-order kinetic model fitted well with the experimentally obtained rate data, indicating that the main mode of Pd-ion removal by Ti 3 C 2 –NH 2 was via chemical reduction. Finally, the catalyst exhibited excellent performances during the photocatalytic and Suzuki coupling reactions with yields of 81 % and 95 %, respectively. The results demonstrated that Ti 3 C 2 –NH 2 is an excellent material for adsorbing Pd ions and can effectively recycle these ions from pharmaceutical wastewater.

研究领域: 环境科学 · 材料科学 · 化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Adsorption behavior study and mechanism insights into novel isothiocyanate modified material towards Pd2+

Long Jiang,Yaojie Liu,Xu Meng,Mo Xian,Chao Xu

Removal of toxic heavy metals needs to be assured from drug substances and catalyst residues from waste streams at the ppm level which has sometimes proved difficult, causing irreversible harm to human health and environment. Herein, on basis of binding evaluation between isothiocyanate derivatives in Pd(MeCN) 2 Cl 2 model solution, the corresponding functional materials were prepared by efficiently nucleophilic substitution and isomerization reaction on polystyrene framework. The isomerization from thiocyanide to isothiocyanate gifted SCN-2-NCS excellent Pd 2+ adsorption capacity which could tolerate various composite solvent systems and was generally superior than the widely-used isothiourea modified material PSTU. Systematic thermodynamics and kinetics study indicated the complexation with Pd 2+ was kinetically hindered and the increase of temperature contributed to the adsorption process as the maximum adsorption capacity was evaluated as 4.995 mmol·g −1 . The breakthrough point for SCN-2-NCS was 385–390 BV in Pd(MeCN) 2 Cl 2 solution (1.000 mmol·L -1 ) and reached to 126–130 BV in Pd-catalyzed debenzylation waste stream (5.433 mmol·L -1 ). Subsequently, computational chemistry certified an electrophilic addition reaction occurred to generate a five-member Pd 2+ complex in adsorption process which could be converted to N-substituted thiocarboxylic acid in acid condition, and FTIR, NMR and XPS analysis were further employed to probe the proposed adsorption mechanism.

CAS / MDL: 7647-10-1
研究领域: 环境科学 · 材料科学 · 化学工程
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RSC Advances · 2016 ·Vol. 6 ·期 83 ·79781-79791 · IF 3.289

Facile synthesis of porous organic polymers for the absorption of Pd(II) ions and organic dyes

Yanmei Luo,Junhui Ran,Rong Chen,Xinjian Cheng

Porous organic polymers (POPs) were prepared via two-step reactions. In the first step, dialdehyde compounds were synthesized using the Suzuki–Miyaura coupling reaction, and in the second step, the dialdehyde compounds reacted with hydrazine hydrate to form polymers using Schiff’s base formation reactions. These POPs are nanosheet-layer structured, crystalline and fluorescent. They were studied using FTIR, fluorescence spectra, UV-Vis, SEM, TEM, XRD, DSC, and TGA. It was found that the pore parameters, such as specific surface areas and pore diameters, of the POPs could be adjusted by changing the reaction time and temperature. The specific surface areas increased with the increasing of reaction time and temperature. The maximum specific surface area could reach 715.6 m2 g−1. Furthermore, the POPs could detect and remove Pd(II) ions and organic dyes. When in contact with Pd(II) ions, the fluorescence of the POPs was quenched, and the POPs could absorb Pd(II) ions as well. The maximum absorption capacity for Pd(II) ions could reach 20.6 mg g−1 within 5 min. Meanwhile, the POPs could absorb two model dyes, rhodamine B (RhB) and methylene blue (MB), with high efficiency within 5 min.

研究领域: 材料科学 · 环境科学
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JOURNAL OF MOLECULAR LIQUIDS · 2019 · IF 4.561

Experimental and DFT studies on the selective adsorption of Pd(II) from wastewater by pyromellitic-functionalized poly(glycidyl methacrylate) microsphere

Jiling Zhao,Chen Wang,Shixing Wang,Yang Zhou,Bing Zhang

Palladium wastewater is produced from various industrial activities and seriously pollutes the environment. In here, a new adsorbent (PMDA-PGMA) was manufactured by functionalizing poly(glycidyl methacrylate) microspheres with pyromellitic acid and introduced to recover Pd(II) from wastewater. The main influencing factors including pH, palladium ionic content, reaction time and temperature were evaluated. The selectivity , reusability and sorption mechanism have been systematically examined. The pH 2 was optimal for Pd(II) adsorption and only 300 min was required to reach maximum adsorption capacity about 206.71 mg/g. The experimental data were is in tune with pseudo-secondary kinetics and Langmuir model well. So, the Pd(II) adsorption process was monolayer chemical adsorption. Thermodynamic parameters indicate that Pd(II) adsorption on PMDA-PGMA was an endothermic reaction . The main adsorption mechanism is ion exchange, electrostatic attraction and coordination between palladium ions and pyromellitic acid groups. Additionally, PMDA-PGMA can be easily regenerated by 10% thiourea and can be recycled at least five times. PMDA-PGMA exhibited good selective extraction ability for Pd(II) and effectively separated Pd(II) (≥95%) from laboratory wastewater in the presence divers metal ions . Density functional theory calculations show that PMDA-PGMA combines with Pd(II) through monodentate N atoms and bidentate O groups. The application prospect of PMDA-PGMA is encouraging in removing palladium from wastewater due to its high adsorption capacity and better reusability.

研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2018 · IF 6.434

Plant tannin immobilized Fe3O4@SiO2 microspheres: A novel and green magnetic bio-sorbent with superior adsorption capacities for gold and palladium

Ruiyi Fan,Huiyu Min,Xingxing Hong,Qingping Yi,Wei Liu,Qinglin Zhang,Zhengrong Luo

In this paper, a new core-shell nanostructured magnetic bio-based composite was prepared by immobilizing persimmon tannin (PT) onto Fe 3 O 4 @SiO 2 microspheres, and the as designed Fe 3 O 4 @SiO 2 @PT was utilized for adsorptive recovery of Au(III) and Pd(II). The preparation, morphology, composition and magnetic property of Fe 3 O 4 @SiO 2 @PT were characterized. Adsorption parameters of Fe 3 O 4 @SiO 2 @PT towards Au(III) and Pd(II) including initial pH, reaction time, initial concentration of metal ions , effect of acidity and interference of coexisting metal ions were investigated. It is sufficiently confirmed that silica was coated on Fe 3 O 4 and persimmon tannin was immobilized on aminated Fe 3 O 4 @SiO 2 . The thickness of silica and loaded persimmon tannin are around 18 nm and 14 nm, respectively. With only 1.00 wt% of persimmon tannin, however, the maximum adsorption capacities of Fe 3 O 4 @SiO 2 @PT for Au(III) and Pd(II) were as high as 917.43 and 196.46 mg·g −1 , respectively. In addition, after adsorption of Au(III) and Pd(II), the magnetization saturation values ( Ms ) of Fe 3 O 4 @SiO 2 @PT were high enough to guarantee efficient magnetic seperation. Metallic gold could be facilely recovered from wastewaters containing Au(III).

研究领域: 材料科学 · 环境科学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

UV-induced graft polymerization of polyamide-6 for electroless copper deposition

Yuanming Chen,Shaorong Liang,Wei He,Shouxu Wang,Chong Wang,Zhuoming Du,Yongjie Du,Weiguo Yang,Binyun Liu,Yan Hong

A simple and chromium-free method for the metallization on engineering plastic polyamide-6 (PA6) by UV irradiation is proposed in this article. The surface graft polymers with specific adsorption activity are developed through one-step UV exposure operation, which captures Pd 2+ in the activation process. The chemisorption of Pd 2+ is further reduced into catalytic Pd 0 to enable the substrate with catalytic nucleus for conventional copper electroless deposition (ELD). The grafting layer and the deposited copper coating are characterized by Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, contact angle measurements, scanning electron microscopy, and X-ray diffraction. The results indicate that successful grafting occurs on PA6 after UV excitation. In addition, the as-deposited copper layer shows excellent conductive performance and high adhesion with the PA6 substrate. It’s expected that this emerging and feasible approach would have broad prospects for the metallization of plastic and offer significant value in the plating industry.

CAS / MDL: 79-10-7 107-98-2
研究领域: 材料科学 · 表面工程
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CHINESE JOURNAL OF CATALYSIS · 2016 · IF 2.628

Ionic palladium complex as an efficient and recyclable catalyst for the carbonylative Sonogashira reaction

Da Yang,Dongliang Wang,Huan Liu,Xiaoli Zhao,Yong Lu,Shijun Lai,Ye Liu

The neutral palladium(II) complex bis-[1-(5’-diphenylphosphinothiazol-2’-yl)-imidazolyl] dichloropalladium(II) ( 1A ) ligated by thiazolylimidazolyl-based phosphine ( L1 ) in which thiazolylimidazolyl acted as an S- and N-donor provider with weak coordinating nature, and the ionic complex bis-[1-(5’-diphenylphosphinothiazol-2’-yl)-3-methylimidazolium] dichloropalladium(II) trifluoromethanesulfonate ( 2A ) ligated by thiazolylimidazolium-based phosphine ( L2 ) after quaternization of L1 using methyl trifluoromethanesulphonate were synthesized. It was found that the introduced positive charges and strong electron-withdrawing effect in 2A not only led to changes in the configuration and structural stability of the complex, but also lowered its catalytic performance in carbonylative Sonogashira reactions. These effects reveal the important role of the N-donor in 1A . In addition, as an ionic palladium complex, 2A combined with the room-temperature ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate could be recycled eight times as the catalyst in carbonylative Sonogashira reactions without detectable metal leaching.

研究领域: 有机化学 · 催化化学
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