SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Huizhen Sun,Xiuhua Chen,Shaoyuan Li,Wenhui Ma,Xiumin Chen,Dandan Wu,Kaixin Fu,Mingjun Xiao,Ming Wen
Developing efficient and selective recovery of Pd(II) adsorbents is crucial for addressing environmental pollution issues. Among them, covalent organic framework (COF) and metal organic framework (MOF) composites due to the multi-site functional groups are expected to exhibit excellent Pd(II) adsorption. However, the design and preparation of COF and MOF composite adsorbents for highly efficient adsorption of heavy metal Pd(II) still face many challenges. Herein, we constructed a series of novel core–shell structure UiO-66-NH 2 @TAP-COF (denoted as M@C) adsorbents (M@C-X, X = 1–5, representing different MOF doses) by Schiff base reaction and applied in the adsorption of Pd(II). The findings indicated that the M@C-3 exhibited ultra-high adsorption performance, reaching a capacity of 2134.1 mg/g, and displayed excellent selectivity, making it the best among similar materials. Experimental data and density functional theory (DFT) calculations revealed that the efficient and selective adsorption of Pd(II) is attributed to coordination interaction and strong electrostatic between Pd(II) and the abundant N and O groups in M@C. This work demonstrates the significant potential of the constructed core–shell M@C composites for the efficient and selective recovery of precious metal Pd(II).
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaosong Zhou,Xiaoxing Yu,Lanzhen Peng,Jin Luo,Xiaomei Ning,Xuliang Fan,Xunfu Zhou,Xiaoqin Zhou
The photocatalytic H 2 production activity of polymer carbon nitride (g-C 3 N 4 ) is limited by the rapid recombination of photoelectron-hole pairs and slow surface reduction dynamic process. Here, a supramolecular complex (named R-TAP-Pd(II)) was fabricated via self-assembly of (R)-N-(1-phenylethyl)-4-(4-(pyridin-2-yl)-1H-1,2,3-triazol-1-yl)benzamide (R-TAP) with Pd(II) and used to modify g-C 3 N 4 . In the R-TAP-Pd(II)@g-C 3 N 4 composite photocatalyst, the spin polarization of R-TAP-Pd(II) can promote charge transfer and inhibit photogenerated carrier recombination, as confirmed by spectral tests and photoelectrochemical performance tests. Electrochemical tests and in situ X-ray photoelectron spectroscopy (XPS) tests proved that the Pd(II) ion in the R-TAP-Pd(II) molecule can serve as active sites to accelerate H 2 production. The R-TAP-Pd(II)@g-C 3 N 4 presented a photocatalytic H 2 generation rate of 1085 μmol g −1 h −1 when exposed to visible light, which was a about 278-fold increase compared with g-C 3 N 4 . This work finds a new approach to boost the photocatalytic efficiency of g-C 3 N 4 via supramolecular self-assembly.
研究领域:
材料科学
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化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Yuqi Geng,Jiaqi Li,Wenjuan Lu,Ning Wang,Zeyang Xiang,Yanzhao Yang
In this paper, superparamagnetic Fe 3 O 4 @SiO 2 -NH 2 nanoparticles were applied to adsorb Au(III)/Pd(II)/Pt(IV) in HCl medium. The successful synthesis of Fe 3 O 4 @SiO 2 -NH 2 was characterized through TEM, SEM and FT-IR. Electrostatic interaction between magnetic NPs and metal anions was proposed as the main adsorption mechanism by zeta potential analysis. Maximum adsorption capacities and adsorption behaviors under metal anions concentrations, acidity, NaCl, kinetic and isotherm models were investigated. Notably, the Fe 3 O 4 @SiO 2 -NH 2 shows the excellent acidity and salinity resistance on Au(III), Pd(II) adsorption. The separation routine among Au(III), Pd(II) and Pt(IV) was proposed. As investigated, Pt(IV) could be isolated due to the less adsorption amount onto Fe 3 O 4 @SiO 2 -NH 2 (≤1%). Then, the adsorbed Au(III) was eluted selectively by HCl + N-hexanol alcohol + ethanol + H 2 O 2 mixing solution. Then, the adsorbed Pd(II) was completely eluted by thiourea solution. The recovery efficiencies of Au(III), Pd(II) and Pt(IV) were kept over 92%, 97% and 94% respectively, during 5 turns of cycling separation experiments. Total loss amount of Fe is around 7%. Hence that, the particle demonstrates the good stability and high adsorption capacity, which possess great potential for practical Au(III), Pd(II) and Pt(IV) separation.
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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DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2014
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IF 3.32
Xuanduong Le,Zhengping Dong,Zhicheng Jin,Qingqing Wang,Jiantai Ma
In this study, a novel Pd(II) complex functionalized core–shell magnetic mesoporous catalyst (Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II)) was synthesized by a simple cost effective procedure. It was characterized by transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, vibrating sample magnetometer, and nitrogen physical adsorption. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst offered high surface area and exhibited excellent activity towards Suzuki–Miyaura cross-coupling reaction of halides with aryl boronic acids in ethanol in air. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst was stable, reusable, and conveniently recovered by applying an external magnetic field. Moreover, it provided 91% conversion after the sixth catalytic run. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst examined in this study combined both the efficiency of a homogeneous catalyst and the durability of a heterogeneous catalyst. The results revealed that the Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst is promising as a candidate for various Pd-based catalytic applications.
研究领域:
化学
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材料科学
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2016
·Vol. 51
·期 18
·8502-8515
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IF 2.302
Ran Junhui,Wang Haiying,Cheng Xinjian
Fluorescent chemosensors based on silica nanoparticles and silicate glass slides were well designed and prepared. The as-prepared fluorescent silica particles and glass slides exhibited highly selective sensing and absorbing abilities to Pd 2+ ions in aqueous phase. SiO 2 nanoparticles were first synthesized by the hydrolysis of tetraethyl orthosilicate (TEOS), and then –NH 2 groups were introduced to silica by treating with 3-aminopropyltriethoxysilane (APTES). Subsequently, 4-amino-1,8-naphthalic anhydride (ANA) was incorporated with the reaction of –NH 2 groups. Finally, salicylaldehyde (SA) was introduced by the reaction between amino groups in ANA and the –CHO groups in SA. Thus, the fluorescent silica nanoparticles were obtained. This method was expanded to prepare fluorescent silicate glass slides. Upon the addition of Pd 2+ ions, the fluorescence quenched immediately. These chemosensors were selectively sensitive to Pd 2+ ions as low as 10 μM. The absorption efficiency of fluorescent nanoparticles and glass slides for Pd 2+ reached to 38.38 and 27.50 %, respectively. And the chemosensors also could be easily recycled and reused for at least five times. Fluorescent silica nanoparticles with only ANA or SA (not ANA and SA together) also exhibited the sensing ability to Pd 2+ ions; however, it showed the shortage of Pd 2+ ions selectivity. It suggested that it is necessary to introduce both ANA and SA for the high sensitivity and selectivity to Pd 2+ ions.
研究领域:
材料科学
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分析化学
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DOI
高影响因子
CHEMICAL PHYSICS LETTERS
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2021
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IF 2.328
Dongxin He,Wei Cao,Deshun Huang,Haimin Li,Jing Zhu,Pengxiang Zhao
Safety use of hydrogen leads to the development of highly sensitive materials for hydrogen sensing. Herein, Pd(II)@alkyne-PVA/ d -Ti 3 C 2 T x composite was prepared by spin-coating Pd(II)@alkyne-PVA solution onto the filter membrane supported with delaminated Ti 3 C 2 T x ( d -Ti 3 C 2 T x ). The properties of the composite were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, and X-ray photoelectron spectroscopy (XPS). The results demonstrate that the composite shows high sensitivity and stability for hydrogen sensing.
研究领域:
材料科学
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化学工程
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纳米技术
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DOI
高影响因子
CATALYSIS LETTERS
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2021
·Vol. 152
·期 4
·1160-1169
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IF 3.186
Cheng Lin,Cao Liumei,Ren Hao,Guo Qiaoqiao,Deng Huifang,Li Yiming
The construction of a multifunctional catalyst for multistep sequential\tandem reactions at the molecular level faces a formidable challenge. Multivariate (MTV)-MOFs can provide a facile and tunable platform for rationally designing such multifunctional catalysts via grafting different catalytic groups on the bridging ligands. However, the related investigations are still limited. Here, Pd(II) and l -proline are metalated and decorated to organic linkers, respectively, to build a MTV-MOF, which is then successfully applied to sequential Suzuki Coupling/asymmetric Aldol reactions with satisfied coupling performance (yields up to 99%) and good enantioselectivities ( ee anti up to 98%). Inductively coupled plasma optical emission spectrometer (ICP-OES) measurements of the supernatant and hot leaching test suggest the heterogeneous nature of the catalyst. Macrosubstrate tests verify that the reaction occurs inside the pores of the MOF. The heterogeneous catalyst can maintain structural stability and catalytic activity within three cycles. Graphic Abstract Versatile Pd(II) and l -proline were metalated and decorated, respectively, into stable UiO-67 to construct bifunctional and heterogeneous multivariate MOF catalyst, which displayed efficient and recyclable catalytic activity in sequential Suzuki Coupling/asymmetric Aldol reactions.
研究领域:
化学
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材料科学
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催化领域
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Yuan Chen,Yuancai Chen,Yexia Qin
In the present study, we found that nanoparticles (Pd-NPs) were biosynthesized by Bacillus wiedmannii MSM ( B. wiedmannii MSM) with endogenous carbon under O 2 condition, and more favorablity under N 2 purging condition. XRD results indicated that crystal planes of Pd-NPs were attributed to Pd 0 (111), Pd 0 (200), Pd 0 (220), and Pd 0 (311), respectively. TEM and STEM-EDX results showed that the bio-reduction of Pd (II) ( k pd,1 =4.799 min −1 ) occurred predominately in periplasm space. FTIR results showed that the -COOH, -OH, and -NH 2 were the main groups participating in the removal of Pd (II). The aerobic reduction of Pd (II) by B. wiedmannii MSM was proposed, including extracellular superoxide radicals produced by NAD(P)H oxidases , endogenous electron donors, and O 2 -insensitive hydrogenase. These studies provide new methods and insights for reduction of Pd (II).
研究领域:
环境科学
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材料科学
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微生物学
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化学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yangyang Wang,Shuwen Chen,Ronghao Liu,Lixin Zhang,Wenfeng Xue,Yanzhao Yang
The development of efficient ionic liquids (ILs) for disposable separation and recovery of various precious metals was of great importance, but still faced difficult challenges. A phase change temperature-controlled system composed of IL and HCl solution was developed for the extraction and separation of Au(III), Pd(II) and Pt(IV) from secondary resources. UCST (upper critical solution temperature)-type IL ([1,4,7-TMTA][Tf 2 N]) possessed outstanding selectivity of precious metals and the property of temperature-controlled phase transition. The ability of ILs to form solvated hydrogen bonds was confirmed by quantum-chemical calculation to be correlated with their corresponding UCST. Different experimental parameters were optimized to explore the extraction behavior of IL. It is noteworthy that homogeneous liquid-liquid extraction system (HLLE) constructed by UCST-type IL could significantly enhance the extraction kinetic of Au(III), Pd(II) and Pt(IV) by decreasing phase interface resistance. For Au(III), Pd(II) and Pt(IV), when the system temperatures were higher than 40 °C, 49 °C and 65 °C, the maximum values were 98.5%, 98.3% and 93.2% at the highest efficiency. In addition, the extraction mechanism of anion exchange was revealed by UV–vis, IR, NMR and LC-MS spectrometry. At last, Au(III), Pd(II) and Pt(IV) could be selectively separated from multi-metal solutions where impurity ions coexist by K 2 C 2 O 4 , NH 3 ·H 2 O and CS(NH 2 ) 2 /HCl, respectively. After 5 cycles, the extraction performance of [1,4,7-TMTA][Tf 2 N] maintained. In summary, this paper overcame the obstacle of slow kinetics of solvent extraction technology, and pointed out a way for polymetallic co-extraction and separation in HLLE system.
研究领域:
材料科学
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环境化学
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分析化学
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绿色化学
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Wang Jinlin,Shi Jiangjian,Yin Kang,Meng Fanqi,Wang Shanshan,Lou Licheng,Zhou Jiazheng,Xu Xiao,Wu Huijue,Luo Yanhong,Li Dongmei,Chen Shiyou,Meng Qingbo
Charge loss at grain boundaries of kesterite Cu 2 ZnSn(S, Se) 4 polycrystalline absorbers is an important cause limiting the performance of this emerging thin-film solar cell. Herein, we report a Pd element assisted reaction strategy to suppress atomic vacancy defects in GB regions. The Pd, on one hand in the form of PdSe x compounds, can heterogeneously cover the GBs of the absorber film, suppressing Sn and Se volatilization loss and the formation of their vacancy defects (i.e. V Sn and V Se ), and on the other hand, in the form of Pd(II)/Pd(IV) redox shuttle, can assist the capture and exchange of Se atoms, thus contributing to eliminating the already-existing V Se defects within GBs. These collective effects have effectively reduced charge recombination loss and enhanced p-type characteristics of the kesterite absorber. As a result, high-performance kesterite solar cells with a total-area efficiency of 14.5% (certified at 14.3%) have been achieved.
研究领域:
材料科学
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太阳能
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半导体物理
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产品关联
DOI
PubMed
高影响因子
CELLULOSE
·
2020
·Vol. 27
·期 17
·10167-10181
·
IF 4.21
Guo Wanghuan,Zhao Zhigang,Yang Fan,Xie Meiying,Shao Zhiheng,Xue Liyan,Zhang Yang,Lin Wanqing,Du Chang,Zhang Yongjian
Abstract The separation and recovery of Au(III), Pd(II), and Pt(IV) is a challenge in hydrometallurgy, and finding good adsorbents is a way to solve this problem. In this work, two novel adsorbents, carboxymethyldiethylammoniumethyl cellulose (CM-n-DEAEC) and carboxymethyl-2-diethylaminoethyl cellulose (CM-o-DEAEC), were synthesized by changing the grafting site of carboxymethyl on diethylaminoethyl cellulose (DEAEC). The structures and morphologies of the adsorbents were examined by NMR, FT-IR, EA, TGA, and SEM analyses. The effects of adsorbents on the separation performance of Au(III), Pd(II), and Pt(IV) at different adsorption conditions were studied. The performances of stripping and recycling were investigated. At a 3 M chloride ion concentration, CM-n-DEAEC's adsorption rates for Pd(II), Au(III), and Pt(IV) were stabilized at 60%, 30%, and 7% in the pH range of 1.0–3.0 and were unaffected by coexisting metal ions. However, at a 0.1 M chloride ion concentration, CM-o-DEAEC separated Pt(IV) before Au(III) and Pd(II) in the pH range from 1.0 to 2.0 without being affected by coexisting metal ions. In addition, the absorbed metal ions can be easily stripped by a 0.1 M thiourea-0.1 M HCl solution, and the adsorption rate only decreased by 3.0% and 1.8% after seven adsorption–desorption cycles. Therefore, it was shown that CM-n-DEAEC and CM-o-DEAEC are excellent adsorbents that can control the adsorption order of precious metals and can selectively and quickly recover Pd(II) or Pt(IV) from wastes containing Au(III). Graphic abstract
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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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 2
·1824-1835
·
IF 4.223
Chen Yuan,Chen Yuancai
At present, there are many studies on microbial reduction of Pd (II), although few of these studies assess the bacterial toxicity of Pd (II) before and after reduction by microorganisms. In this study, the toxicity of Pd (II) to Bacillus wiedmannii MSM ( B. wiedmannii MSM) was assessed before and after reduction by live B. wiedmannii MSM cells (referred to as “Pd (0)-loaded cells”) and after biosorption by dead B. wiedmannii MSM cells (referred to as “Pd (II)-loaded cells”). B. wiedmannii MSM is a widely occurring, nonpathogenic aerobic bacterium. Compared with Pd (II), the EC 20 , EC 50 , and EC 80 of Pd (0)-loaded cells increased by 77.73-, 112.75-, and 163.91-fold, respectively, while the EC 20 , EC 50 , and EC 80 of Pd (II)-loaded cells increased by only 11.55-, 9.77-, and 8.29-fold, respectively. The sterilization contribution rates of the mechanisms of action of Pd (0)-loaded cells were ranked in the order of: remaining Pd (II) > oxidative stress > physical puncture. Pd (II) was found to increase cell membrane permeability, glutathione S-transferase (GST) enzyme activity, and reactive oxygen species levels in cells and decrease the cell membrane potential. XPS results indicated that Pd (II) increased the content of polysaccharides and peptides and decreased the content of hydrocarbons in cells. These findings reveal the bactericidal mechanism of toxicity of Pd (II) and Pd (0)-loaded cells on Bacillus wiedmannii MSM and provide an environmentally friendly and inexpensive method for Pd (II) detoxification.
研究领域:
环境科学
·
微生物学
·
毒理学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）