SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Henan Zhang,Qi Liu,Alena Novoselova,Valeri Smolenski,Jing Yu,Jingyuan Liu,Yongde Yan,Milin Zhang,Jun Wang
The efficient separation of the rare earth element Sm from spent nuclear fuel is of strategic importance for the nuclear industries. This study explored the feasibility of a novel liquid Ga-Pb hybrid electrode for electrochemical extraction of samarium compounds, and the electrochemical reduction mechanism and dynamic properties of Sm(III) ions were provided in NaCl-2CsCl molten salt. It was established that the reduction mechanisms of Sm(III) to Sm(II) and Pb(II) to Pb(0) on the Mo cathode were a one-step reaction processes, respectively, while Ga(III) to Ga(0) was a two-step reaction process. The co-deposition mechanisms of Sm(III), Ga(III) and Pb(II) ions on the Mo cathode were identified, and the types of intermetallic compounds, formation potentials and reaction processes were analyzed. The deposition potential of Sm on Ga-Pb mixed cathode is determined, and the value of its depolarization was greater than on the liquid Pb electrode. Simultaneously, Sm ions have higher exchange current densities and lower activation energies for electrode reactions on the liquid Ga-Pb mixed electrodes than on the liquid Pb electrodes. Furthermore, the electro-separation of NaCl-2CsCl-SmCl 3 molten salt was executed via potentiostatic electrolysis technique, and the separation efficiency and the effect of cathode product type were analyzed and compared in Ga-Pb hybrid electrode and Pb electrode. It was obtained that the maximum extraction efficiency on the Ga-Pb hybrid electrode and the separation efficiency of Sm could reach 91.3 % after 8 h of electrolysis.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Caiyong Nong,Xiaodong Li,Risto Koivula,Junhua Xu,Małgorzata Szlachta
This study aimed to provide new insights into the mechanism of Cs + sorption on titanium hexacyanoferrate (Ti–Fe PBA) focusing on the influence of the structure and vacancies. Ti–Fe PBA was synthesized with specific vacancies using a coprecipitation synthesis method. The study successfully demonstrated the unique structure of Ti–Fe PBA and determined the ratio of vacancies within its framework through various characterization techniques, including X-ray diffraction, Fourier transform-infrared spectrometry, thermogravimetry, scanning electron microscopy, X-ray photoelectron spectroscopy and sodium hydroxide titration. The synthesized Ti–Fe PBA exhibited an impressive Cs + sorption capacity of 3.53 mmol g −1 and demonstrated high selectivity, with a K d value 1.5 × 10 6 for Cs + sorption. In addition, Ti–Fe PBA displayed excellent stability, rapid uptake kinetics and maintained high selectivity, even in the presence of high concentrations of coexisting ions. Moreover, our new findings revealed that K–Cs ion exchange specifically occurring at the interstitial sites within the framework structure accounted for ∼35 % of the total Cs + sorption. A sorption-surface complexation model utilizing a coupling technique that integrated PHREEQC with Python enabled in-depth analysis of titration, pH effects and sorption isotherms. The modelling results revealed that the strong ion exchange sites ≡ S s O H and ≡ S s O N a on surfaces and vacancies contributed ∼65 % of the total Cs + sorption.
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ChemistrySelect
·
2023
·Vol. 8
·期 43
·e202303563
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IF 2.1
Chong Liang,Wei Zhao,Xutang Liu,Fei Wang,Zhijie Jiang
Graphical This attractive work examines the changes in CAs selectivity when lignite is oxidized by H 3+n [PMo 12-n V n O 40 ] (HPA-n, n=1-5) and discloses the catalytic mechanism of HPA. The catalytic process of HPA follows the electron transfer-oxygen transfer (ET-OT) mechanism, where it not only activates lignite through electron transfer, but also activates oxygen, leading to the generation of active substance ⋅OH in water. The ⋅OH promotes the breakage of lignite. Although the oxidation of lignite has been extensively studied, the factors affecting the selectivity of carboxylic acids (CAs) are unclear. This attractive work examines the changes in CAs selectivity when lignite is oxidized by H 3+n [PMo 12-n V n O 40 ] (HPA-n, n=1-5) and discloses the catalytic mechanism of HPA. The results show that the selectivity of benzene polycarboxylic acids and acetic acid (AA) increases with increasing vanadium content of HPA-n, such as mellitic acid and benzenepentacarboxylic acid from 0.8 % and 3.0 % to 5.4 % and 16.2 %, respectively. Consequently, the differences in the concentration of HPA or H 2 SO 4 used to obtain optimal formic acid and AA yields confirm that the intrinsic properties of CAs calculated by Gaussian 09 can also affect their selectivity. HPA can not only activate lignite through electron transfer, but also further activate oxygen, leading to the generation of active substance ⋅OH in water. Consequentially, ⋅OH as the key reactive substance can promote the breakage of bridge bonds, side chains and condensed aromatic rings during HPA-catalyzed oxidation of lignite. Thus, the oxidation pathway of lignite over HPA is proposed. This work constructs a relationship between oxidation capacity and CAs selectivity and discloses the lignite oxidation pathway at the molecular level, which is a significant progress in HPA-catalyzed conversion of lignite.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Tongxu Gu,Jiajun Zhong,Minghao Ge,Ruiju Shi,Liang He,Pengli Bai
All-inorganic lead halide perovskite nanocrystals exhibiting bright luminescence have great potential as fluorescence elements for optical encoding. However, their limited stability in water hinders the application in biosensing. In this study, novel optical encoded microbeads based on CsPbX 3 (X = Cl, Br) nanocrystals are developed and applied in bead-based suspension arrays for the first time. Through the in-situ crystallization of CsPbX 3 nanocrystals within mesoporous silica nano-templates (MSNs), accompanied by mesopores collapse after sintering, CsPbX 3 @MSNs (X3M) nanocomposites with uniform morphology and stable fluorescence intensity in aqueous solutions for up to 50 days are obtained. By assembling X3M with microspheres to form a host–guest structure, an optical encoding microbead (MX3M) library is established by varying the X3M ratio, halide composition , and the size of host microspheres, which can be easily decoded under multi-channel flow cytometer. As a result, MX3M exhibits outstanding capacity for specific target capture and negligible nonspecific absorption performance in the multiplex nucleic acid detection of respiratory viruses, with a low limit of detection (10 copies/rxn). This result highlights the tremendous potential of MX3M encoded microbeads constructed based on CsPbX 3 nanocrystals for multiplexed bioassays.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Yaheng Zhang,Chao Fan,Dongdong Ge,Qinggang Zhang,Shouqiang Huang,Guohua Zhang,Jiayu Su
For the detection of anions from wastewater, the perovskite materials synthesized should have suitable stability and be as hydrophilic as possible, and it’s not appropriate to introduce organic ligands. Mechanochemical reaction can avoid the use of organic solvents and provide improved stability for the perovskite materials due to their large particle size and compact structure, but their fluorescence is often too weak. To solve this problem, the Mn 2+ doping effect was introduced into the CsPbCl 3 crystals, and their synthesis doping strategies driven by mechanical grinding were systematic studied. The optimal Mn 2+ -doped CsPbCl 3 (CsPbCl 3 :Mn) product was obtained by optimizing the synthesis conditions of Mn 2+ source, grinding time on each reaction stage, Mn: Pb feeding ratio, and the sintering temperature . CsPbCl 3 :Mn had the same crystal structure as its undoped counterpart, while an obvious photoluminescence emission peak at 604 nm was obtained, which was originated from the doped Mn 2+ ions. CsPbCl 3 :Mn had good stability against the ethanol environment and there was no organic ligands to hinder the ion exchange between Cl - and Br - from wastewater. Through testing the color difference of the resultant powders, a linear relationship with high correlation coefficient above 0.99 was established between chroma and Br - concentrations, and the Br - concentration in wastewater was accurately determined, demonstrating a promising application prospect of CsPbCl 3 :Mn in the fast detection of Br - ions.
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OPTICAL MATERIALS
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2023
·
IF 3.9
Qun Jing,Menglin Zhu,Lu Li,Xu Ji,Haiming Duan,Henglei Chen,Ming-Hsien Lee
In recent years, phosphates have become a research hotspot to explore new ultraviolet (UV) nonlinear optical (NLO) materials. Herein, two NLO materials MZnPO 4 (M = Rb, Cs) are synthesized by cation substitution in alkali-zinc orthophosphates. Although they crystallize in different space groups P 2 1 and Imm 2, respectively, they both have a honeycomb-like topological structure consisting of corner-shared PO 4 and ZnO 4 tetrahedra and separated by "M" cations. Two compounds exhibit mild powder second harmonic generation (SHG) responses (1.2 and 0.5 × KDP for RbZnPO 4 and CsZnPO 4 , respectively) with type I phase matching behaviors and short absorption edges (226 nm for RbZnPO 4 and 231 nm for CsZnPO 4 ). Furthermore, their thermal properties , infrared (IR) spectra and theoretical calculations are also mentioned in the paper. The synthesis and structure-property relationship described in the system will enable discovery of new NLO materials.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2023
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IF 5.8
Yan Changhan,Sun Qihang,Zhang Juan,Fu Hongquan,Gao Hejun,Liao Yunwen
Prussian blue (PB) is widely used for the selective removal of radioactive cesium ions (Cs + ) from aqueous solutions. Due to its small size and easy dispersion in water, PB requires a carrier that is both inexpensive and easily separable. Magnetic porous biochar (MPBC) was formed by activating starch with FeCl 3 through a one-step calcination method. MPBC can be used as a carrier for Prussian blue, which is easily separated from the solution. This composite material (PB/MPBC) has a rich pore structure and maintains effective surface area, which can facilitate the penetration of Cs + into the adsorbent. Besides, PB/MPBC exhibits high selectivity and good adsorption capacity achieving a large removal capacity of 101.43 mg/g. Thus, this study provides a novel approach for preparing composites with efficient removal of Cs + .
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Advanced Photonics Research
·
2023
·
IF 3.7
Yaoyu Liu,Tianyu Wang,Zongshuai Ji,Guanfeng Liu,Yunhe Chen,Xin Ding,Bing Teng,Shaohua Ji
Cs 3 Cu 2 Cl 5 is unstable owing to ionic migration and lattice decomposition in the atmosphere. In addition, obtaining large bulk single crystals of Cs 3 Cu 2 Cl 5 is challenging. Herein, a novel strategy is proposed for synthesizing a Cs 3 Cu 2 Cl 5 single crystal that exhibits excellent crystallinity and photoluminescence (PL) properties using an antisolvent-assisted method. Na + is doped into the Cs 3 Cu 2 Cl 5 lattice to replenish the lattice defects caused by chlorine vacancies, thus leading to stronger chemical interactions between Cu + and Cl − ions. Moreover, Na + doping circumvents ionic migration and lattice decomposition, thereby enhancing the PL intensity and maintaining the long-term stability of Cs 3 Cu 2 Cl 5 in the atmosphere. Incorporating 10% Na + into the Cs 3 Cu 2 Cl 5 lattice enhances the PL intensity by 18%, and the high-stability PL can maintain more than 48.5% of the PL intensity after 90 d in an atmospheric environment. In addition, a white light-emitting device (LED) is fabricated using the 10% Na + -doped Cs 3 Cu 2 Cl 5 crystal powder and it exhibits a high color-rendering index (93.7) and correlated color temperature (7120 K). Additionally, it exhibits superior stability, even at a high temperature of 120 °C. Thus, the excellent high-temperature stability of Cs 3 Cu 2 Cl 5 can promote its practical application in LED.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chaoyao Geng,Jiaqi Niu,Dan Zhao,Xiaoxin Jin,Jiaojiao Liu,Xiaoqiang Liu,Danny K.Y. Wong
In this work, we study the electrocatalytic detection of H 2 O 2 at electrodes correspondingly modified by four hourglass-shaped polyoxometallates (POMs) with Cu, Co, Mn and Cs as their individual central metal atoms, and four representative Wells-Dawson POMs with the same metal atoms. In this way, we have related their analytical performance to the open structures of hourglass-shaped POMs and the cage-like structures of Wells-Dawson POMs. Among them, we found the three-dimensional hourglass phosphomolybdate (POM 1 ) with plentiful exposed Cu active sites exhibits a dynamic range of 0.1–10 μM, a sensitivity of 11.6 μA μM −1 cm −2 , and a limit of detection as low as 44 nM for H 2 O 2 . It also offers high selectivity, fast response time (2 s), a reproducibility of ∼1.69% and retains ∼97.9% of the initial current after 15 days, verifying its good stability. Accordingly, the POM 1 -modified electrode was applied to monitoring H 2 O 2 converted from superoxide anion radical (O 2 − ) generated by mitochondria isolated and purified from human liver cancer cells (HepG2) without pharmaceutical stimulation. Meanwhile, by exploiting four specific inhibitors (rotenone, 2-thenoyltrifluoroacetone, antimycin A and paclitaxel) known to bind with targeted sites in the corresponding complex within mitochondria to produce a high H 2 O 2 concentration, our results indicated that O 2 − was mainly produced by mitochondrial complex I (ubiquinone oxidoreductase) via electron leakage in the mitochondrial electron transport chain of liver cancer. The electrochemical detection strategy in our work has provided a direct insight into the electron leakage of mitochondrial complexes caused by targeted oxidative stress diseases.
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ANALYTICAL LETTERS
·
2023
·
IF 2
Yongzheng Yin,Huanhuan Lu,Weijun Song,Xiaofeng Hu,Chunyan Sun
Carbon quantum dots (CQDs) were derived from saponin and introduced into polyacrylamide hydrogel to prepare a novel bifunctional material (CQDs@HG). This hydrogel emitted strong blue fluorescence under ultraviolet light (365 nm) and exhibited stable adsorption and detection of iron(III) in water samples. The morphological characteristics, chemical composition, Fe3+ adsorption performance, and optical properties of CQDs@HG were characterized. Depending upon the Fe3+ concentration, CQDs@HG exhibited different quenching effects to allow Fe3+ determination. The limit of detection was 0.115 μM, and the adsorption was as high as 12.13 mg/g. The mechanism was due to both static and dynamic quenching. Notably, the sensor based on CQDs@HG successfully determined Fe3+ in water samples, with spiked recoveries between 95.32% and 103.11%. When combined with software image analysis, the sensor semi-quantitatively determined Fe3+ in the field. This fluorescent hydrogel provides a reference for constructing portable sensors for monitoring hazardous substances in water.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Zhihui Rao,Mengyan Cao,Zehui Chen,Xiujian Zhao,Xiao Gong
Ho-based lead-free double perovskite microcrystals (MCs), Cs 2 NaHo 1-x Yb x Cl 6 , are synthesized and demonstrated to be promising optical temperature sensing materials by understanding the concentration-dependent upconversion (UC) luminescence mechanisms. By optimizing the dopant concentration, a dominant emission shifting from red to green is successfully achieved in an activator-rich system. During this process, the red to green emission intensity ratio (R/G) can be changed from 12.5 (pure red light) to 0.14 (pure green light). It is clarified that the cross-relaxation (CR) process between activator and the energy transfer process between Yb 3+ and Ho 3+ are the key mechanisms of UC luminescence intensity and R/G ratio variation. Moreover, the intensity of red and green UC emission shows strong dependence on temperature, resulting from the competition between CR and energy transfer in the emission levels. The high-sensitivity Ho-based thermometer can be obtained by Cs 2 NaHo 0.99 Yb 0.01 Cl 6 MCs with bright red UC luminescence, whose fluorescence intensity ratio thermometer gains maximum relative sensitivities reaching 0.68% K −1 at 400 K. The multicolor UC luminescence quantitative modeling mentioned here is crucial for understanding the concentration-dependence UC luminescence characteristics and to optimize the design of the Ho-based thermometer. This study can be an extension of the application range for perovskite UC materials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
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IF 6.2
Yudong Xu,Yifei Song,Saisai Chen,Mengting Zhang,Jingqi Chen,Hongyu Li,Min Shi,Fabao Zhang
Lead-based halide perovskite is considered to be a potential visible-light-activated photocatalyst owing to its excellent optoelectronic properties. However, the toxicity of lead and the instability of the material restrict its wide application in the field of photocatalysis . A double perovskite structure is thought to be a solution to this problem. The authors prepared a series of samples, including Cs 2 AgInCl 6 , Cs 2 AgIn 1−x Fe x Cl 6 , and Cs 2 AgFeCl 6 through co-precipitation in acidic solutions. The effects of Fe 3+ doping on the crystal structure and morphology of Cs 2 AgInCl 6 were characterized by XRD and SEM. Based on density functional theory, VB-XPS and UV-Vis absorption characterizations, the band structure of Cs 2 AgInCl 6 and Cs 2 AgFeCl 6 were determined, showing that the bandgap of Cs 2 AgIn 1−x Fe x Cl 6 was reduced linearly by Fe 3+ doping. And Sudan Red III can be photocatalytically degraded by all samples under concentrated xenon lamp irradiation of 175 W, with Cs 2 AgFeCl 6 degrading 96% of Sudan Red III in 45 min. In addition, the Cs 2 AgFeCl 6 sample exhibits good cyclic stability and does not demonstrate any significant changes after two months in storage, showing that Cs 2 AgFeCl 6 may serve as an effective and relatively stable Xenon lamp-activated photocatalyst in degradation of organic dyes.
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