Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lulu Zhang,Long Jiang,Yaojie Liu,Zongjiang Yu,Ximin Chen,Xiaomeng Su,Mo Xian,Weizhi Sun,Chao Xu
Currently searching for effective noble metal separation material is generally blind and time-consuming. Although theoretical calculation has been widely applied to explain the adsorption mechanism, the quantitative coordination effect between ligand and metal remains to be explored especially in the material screening stage. In this study, Pearson’s theory and Koopmans' theory were used to calculate the electron transfer ratio (ΔN) from different ligands containing N, S, and O to PdCl 2 . The quantitative evaluation contributed to the design of efficient ligands including EA (ΔN =0.5929), DB (ΔN =0.5483), and AT (ΔN =0.4885). And the corresponding polystyrene materials CMPS-EA, CMPS-AT, CMPS-DB were successfully synthesized via chemical modification. According to the adsorption experiment, the per mmol of ligand adsorption capacity from CMPS-EA, CMPS-DB and CMPS-AT for Pd(II) were 0.67 mmol/mmol, 0.17 mmol/mmol and 0.11 mmol/mmol, respectively, exhibiting a positive correlation with the results of ΔN. Moreover, CMPS-EA could efficiently remove 98.01% Pd(II) in the presence of multiple competing metal ions with five times concentration higher than Pd(II). In column study, the breakthrough point (C t /C 0 =0.05) for CMPS-EA was 666–676 BV in 1 mmol/L Pd(II) solution and up to 95% desorption efficiency within 50 BV. The adsorption differences and mechanism of CMPS-EA, CMPS-AT and CMPS-DB were further investigated by FTIR, XPS, ESP, and NBO.
研究领域:
化学工程
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材料科学
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环境科学
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产品关联
DOI
高影响因子
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2019
·
IF 4.527
Jinghao Wang,Sijing Bi,Yuancai Chen,Yongyou Hu
Gram-negative Citrobacter freundii with high Pd (II) reduction capacity was isolated from electroplating wastewater, and the electron transfer involved in Pd (II) bio-reduction by C. freundii JH was investigated in phosphate buffer saline solution with sodium formate as sole electron donor under anaerobic condition . FTIR spectra indicated that hydroxyl and amine groups on cell wall participated Pd (II) bio-sorption. TEM , XRD, XPS results confirmed that Pd (0) nanoparticles (NPs) could be bio-synthesized intra/extracellularly. Meanwhile, pH turn-over were observed owing to the reduction of cytochrome c (c-Cyt) in bio-reduction process. EPR spectra indicated that free radicals ( OH) was generated from high concentration Pd (II), which would cause seriously damage to cell. Despite of the lower tolerance to Pd (II), the cells at logarithmic phase exhibited higher Pd (II) reduction capacity (72.21%) than that at stationary phase (56.21%), which might be related to the relatively stronger proton motive force (PMF) created by the substrate oxidation and the electron transfer, as evidenced by electrochemical experiments (CV, DPV, amperometric I-t curves) and protein denaturalization experiments. Additionally, c-Cyt and riboflavin were confirmed to be important participants in electron transfer. Finally, a putative synthesis mechanism of Pd (0)-NPs was deduced. This study contributed to further understanding the electron transfer in Pd (II) reduction, and provided more information for the bio-synthetic of metal nanoparticles.
研究领域:
环境微生物学
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生物技术
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纳米技术
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微生物生物化学
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Yuan Chen,Keqiang Hu,Yuancai Chen
In this study, we screened a new aerobic bacterium ( Bacillus megaterium Y-4) that can efficiently reduce Pd(II) with different electron donors. The best electron donor was sodium formate and the best reduction of Pd(II) were by log growth phase cells. The high removal capacity of Pd(II) (1658.3 mg/g) was obtained with 30 mg/L dry cell weight and 50 mg/L Pd (II) in the presence of 5 mM sodium formate. The removal amount of Pd(II) increased with initial Pd(II) concentrations ranging from 50 to 200 mg/L with 100 mg/L Pd(II) being completely removed by 148 mg/L dry cell weight in 6 h. The cell wall, periplasmic space and intracellular contents of B . megaterium Y-4 contains different kinds of enzymes for reducing Pd(II). In addition, the activity of extracellular and periplasmic enzymes was more sensitive to temperature than intracellular enzymes . XRD and XPS analysis revealed that the enzyme for reducing Pd(II) in B. megaterium Y-4 can tolerate a broad range of temperatures (20–60 °C) and pH (2.0–7.0) but was sensitive to oxygen. TEM analysis showed that biogenic palladium nanoparticles (Pd-NPs) were mainly distributed evenly in the periplasmic space of the live cells and were released from cells into aqueous solution, which reduced the toxicity of Pd(II), allowing Pd-NP recovery without cell destruction. B. megaterium Y-4 is a potential bacterium for efficient treatment and reclamation of Pd(II) pollution and formation of Pd-NPs.
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
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IF 8.456
Geng Chen,Yi Wang,Hanqin Weng,Zhihao Wu,Kebao He,Peng Zhang,Zifang Guo,Mingzhang Lin
The recovery of precious metals like palladium (Pd) from secondary resources has enormous economic benefits and is in favor of resource reuse. In this work, we prepared a high efficiency pyridine-functionalized reduced graphene oxide (rGO) adsorbent for selective separation of Pd(II) from simulated electronic waste leachate, by one-pot γ-ray radiation-induced simultaneous grafting polymerization (RIGP) of 4-vinylpyridine (4VP) from graphene oxide (GO) and reduction of GO. The poly(4-vinylpyridine)-grafted reduced graphene oxide (rGO-g-P4VP) exhibits fast adsorption kinetics and high maximum adsorption capacity. The adsorption capacity is 105 mg g–1 in the first minute and reaches equilibrium within 120 min. The adsorption process follows the Langmuir model, from which the maximum adsorption capacity of Pd(II) is estimated to be 177 mg g–1. We also proved that the adsorption mechanism of Pd(II) on rGO-g-P4VP involves both ion exchange and coordination adsorption by XPS analysis. Most importantly, the loss of oxygen-containing groups due to reduction of GO not only facilitates the separation of adsorbent from aqueous solution but also reduces the electrostatic repulsion toward Pd(II)Cl42– in hydrochloric acid solution, leading to a higher adsorption selectivity of Pd(II) over some common metal cations in electronic waste including Fe(III), Cu(II), and Al(III) compared with poly(4-vinylpyridine)-grafted graphene oxide (GO-g-P4VP) prepared by atom transfer radical polymerization. Other precious metals like Pt(IV) and Au(III) can also be recovered easily and selectively by rGO-g-P4VP. This work demonstrates that rGO-g-P4VP prepared by the facile RIGP is a promising adsorbent for recovery of precious metals from secondary resources like electronic waste leachate.
研究领域:
材料科学
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环境科学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zareen Zuhra,Shafqat Ali,Sajjad Ali,Hu Xu,Rongzhen Wu,Yuanyuan Tang
Designing materials for selective recovery of precious metals is a critical challenge in response to recent outbreaks of electronic wastes owing to economic and environmental concerns. We introduced high-performance hybrid materials (MCNTs) comprising of six-amino groups based on hexaaminobenzene metal-organic framework (HAB-MOF) and carbon nano-tube (CNT) sponge for selective recovery of Au(III) and Pd(II). Among all MOFs ever reported in the literature, the particular synthesized 30-MCNT (30 mg HAB-MOF on CNT sponge) exhibited the highest adsorption capacity ( q e ) of 1832 mg/g (45 °C, pH 3.0) for Au(III) and 1651 mg/g (45 °C, pH 1.0) for Pd(II), which can be regarded as a benchmark in the MOF family. The highly selective nature of 30-MCNT was examined in the presence of ten different metal ions and the results showed that the Au(III)/Pd(II) adsorption efficiency was decreased by only 5–10%. Moreover, the Au(III) and Pd(II) recovery was maintained ∼ 100% from the initial solution with metal concentration of 200 mg/L. The superior performance was mainly attributed to the role of abundant amino groups in the hybrid framework, developing several types of interactions with Au(III) and Pd(II) ions such as hydrogen bonding, electrostatic interactions, acid-base affinity and π-π inner sphere complexation. Furthermore, the remarkably high surface area and robust chemical and mechanical stability of CNT-sponge provided an exceptional support for impregnation of HAB-MOF to avail greater active sites and easier handpicked recycle. Density functional theory (DFT) simulation and X-ray photoelectron spectroscopy (XPS) studies were employed to explore the interaction mechanisms during the adsorption processes. Owing to facile and environment-friendly synthesis, excellent recovery and recycling, the material can be possibly considered for industrial application in precious metal recovery.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
RARE METALS
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2020
·Vol. 39
·期 12
·1473-1482
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IF 2.161
Feng Shao-Ping,Huang Kun
Abstract Separation of palladium (Pd) and platinum (Pt) by solvent extraction is difficult because of their extremely similar physicochemical properties. Development of new extractants with a high extraction efficiency and excellent separation selectivity is the primary focus for enhancing the separation of Pd and Pt by solvent extraction. In this study, a new extractant, 2-((2-methoxyethyl)thio)-1H-benzimidazole (MOBI), which contains N, S, and O atoms, was synthesized and used to separate Pd(II) and Pt(IV) from a hydrochloric acid aqueous solution. The experimental results revealed that Pd(II) and Pt(IV) were effectively separated under the optimal conditions: MOBI concentration of 0.005 mol·L −1 , HCl concentration of 0.2 mol·L −1 , organic/aqueous (O/A) phase ratio of 1.0, and contact time of 15 min. The separation coefficient between Pd(II) and Pt(IV) was 1246.40, which indicates that MOBI has a higher selectivity for Pd(II) than Pt(IV). In addition, the mechanism of coordination between Pd(II) and MOBI was demonstrated through the slope method, Fourier transform infrared spectroscopy (FTIR), hydrogen-1 nuclear magnetic resonance spectroscopy ( 1 H NMR), and carbon-13 nuclear magnetic resonance spectroscopy ( 13 C NMR). The results revealed that MOBI could coordinate with Pd(II) via the N atom in the benzimidazole ring of MOBI molecules to form [Pd(MOBI) 2 Cl 2 ] (O) . Graphic abstract
研究领域:
化学
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材料科学
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DOI
高影响因子
DALTON TRANSACTIONS
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2017
·Vol. 46
·期 22
·7210-7218
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IF 4.029
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
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2019
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IF 4.561
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
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材料科学
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产品关联
DOI
高影响因子
HYDROMETALLURGY
·
2022
·
IF 4.217
Dechao Xiao,Haitao Zhou,Kaihui Cui,Kun Huang
This study proposes a new thin-layer oil membrane (TOM) extraction strategy for enhanced mutual separation of Pd(II) and Pt(IV) chlorocomplex anions in concentrated aqueous hydrochloric acid solutions using di- n -butyl sulfoxide (DBSO) as an extractant. It was discovered that Pd(II) could be preferentially extracted even in concentrated hydrochloric acid solutions. The separation coefficient between Pd(II) and Pt(IV) considerably increased than that between them during conventional extraction using a separating funnel. A new extractor was designed to perform TOM extraction by spreading a thin layer of organic extractant liquid membrane on the surface of aqueous feed solutions under laminar flow . A simplified TOM extraction model and controlled experiments were used to investigate the effect of H + and Cl − ion concentrations on the mutual separation between Pd(II) and Pt(IV). Molecular dynamics (MD) simulations were used to understand the microscopic separation mechanisms at the molecular level. Experimental results revealed that the competitive distribution of H + and Cl − ions in the boundary layer along the normal vertical direction of the organic-aqueous interface are crucial in enhancing the separation between Pd(II) and Pt(IV). The competitive adsorption and enrichment of Cl − ions at the interface prevent DBSO molecules from being protonated by H + ions, which is beneficial for the substituted coordination of DBSO molecules with PdCl 4 2− . However, the ionic association of protonated DBSO molecules with PtCl 6 2− remains dominant at the interface. As a result, even in concentrated hydrochloric acid solutions, the difference in mass transfer between PdCl 4 2− and PtCl 6 2− toward the interface was intensified.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2019
·
IF 10.159
Hao Zhao,Jiabao Xu,Wenjing Huang,Yanbing Zhao,Xiangliang Yang
Although bivalent palladium [Pd(II)] compounds exhibit favorable antitumor efficacy against platinum-resistant cancers, the mechanism remains unclear. Moreover, some drawbacks, such as structural lability, rapid elimination in vivo, and poor intratumoral retention, heavily limit their application in systemic tumor chemotherapy. Here, thermosensitive Pd-PNS nanogels are rationally designed by cross-linking coordination of Pd(II) ions with poly(styrenesulfonate-b-N-isopropylacrylamide-b-styrenesulfonate) (PNS), achieving high drug-loading ability (ca. 80% of entrapment efficiency and 40% of drug-loading efficiency), sustained release, and long-term retention of highly water-soluble K2PdCl4 in intratumoral administration. Cytotoxicity on sensitive/resistant MCF-7 cells and cancer stem cell (CSC) spheroids indicates that Pd-PNS nanogels could inhibit the palladium efflux of P-glycoprotein and multidrug resistance-associated protein-1 and thus enhance the DNA damage and toxicity of platinum-resistant MCF-7/Pt cells and their CSCs. Based on their temperature-sensitive sol–gel transition, Pd-PNS nanogels show sustained release profiles and long-term retention in tumors, further enhancing in vivo antitumor efficacy on MCF-7/Pt tumor-bearing BALB/c nude mice. Owing to these advantages of prolonged retention, efflux inhibition, and efficient CSCs killing ability, Pd-PNS nanogels are promising to be developed as a new temperature-sensitive delivery nanoplatform for injectable regional chemotherapy on platinum-resistant cancers.
研究领域:
药学
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纳米技术
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肿瘤学
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生物医学工程
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DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2017
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IF 3.154
Ahmed M. Senan,Sicheng Zhang,Miao Zeng,Zhuqi Chen,Guochuan Yin
Utilization of renewable biomass to partly replace the fossil resources in industrial applications has attracted attention due to the limited fossil feedstock with the increased environmental concerns. This work introduced a modified Wacker-type oxidation for transformation of unsaturated fatty acids/esters to the corresponding keto fatty acids/esters, in which Cu2+ cation was replaced with common nonredox metal ions, that is, a novel Pd(II)/Lewis acid (LA) catalyst. It was found that adding nonredox metal ions can effectively promote Pd(II)-catalyzed oxidation of unsaturated fatty acids/esters to the corresponding keto fatty acids/esters, even much better than Cu2+, and the promotional effect is highly dependent on the Lewis acidity of added nonredox metal ions. The improved catalytic efficiency is attributed to the formation of heterobimetallic Pd(II)/LA species, and the oxidation mechanism of this Pd(II)/LA catalyst is also briefly discussed.
研究领域:
化学
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生物化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
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2026
·
IF 2.7
Zheng Li,Yi Dou,Chang-Liang Sun,Valerian Dragutan,Xueqing Wang,Baodi Zhang,Jiaying Li,Zhixiong Luo,Fu Ding
Integrating homogeneous catalytically active components onto solid supports represents a primary strategy for the heterogenization of homogeneous catalysts. The purpose is to streamline catalyst separation and recovery processes while enhancing stability and reusability, all while retaining the inherent advantages of homogeneous catalysts. In this study, we synthesized immobilized Pd(II) complexes loaded with 3.5 nm palladium nanoparticles in a single step by incorporating imidazole precursors into porous organic polymer (POP) backbones through free radical polymerization. This process was conducted without resorting to complex synthetic conditions or toxic monomers, utilizing DMF as both solvent and reductant precursor. Pd NPs@POP-Pd was synthesized and thoroughly characterized by FT-IR, PXRD, ICP-OES, XPS, BET, TEM, EDX, and TGA studies. The Pd(0) and Pd(II) contained in the catalyst play a synergistic activating-stabilizing effect that enabled the Pd NPs@POP-Pd to exhibit excellent catalytic performance towards Suzuki reactions between phenylboronic acid and a wide range of aryl halides at an ultra-low Pd loading of 1.92 mmol%. Notably, this catalyst can be recycled 9 times in pure ethanol while maintaining efficient catalytic activity throughout its use.
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DOI
高影响因子
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