SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Rui Cao,Langlang Wang,Xueqian Wang,Yibing Xie,Xiang Li,Ping Ning
The low-temperature conversion of corrosive carbonyl sulfide (COS) in steel by-product gas is essential for the clean utilization of this gas. Herein, La-Ti@K catalysts doped with La nanoparticles were shown to exhibit significant photopromoted thermocatalytic activity and stability under UV light irradiation. At a reaction temperature of 60 °C, the TOF value increased from 4.84 × 10 -4 s −1 (TiO 2 , thermal treatment) to 8.43 × 10 -4 s −1 (La-Ti@K, photothermal treatment), and the H 2 S selectivity exceeded 99%. This was because La doping increased the density of basic sites on TiO 2 , which promoted the continuous dissociation of H 2 O in the system and the regeneration of –OH under UV irradiation. Moreover, the photogenerated electrons from TiO 2 were transferred to La to maintain the metallic La nanoparticles, as well as to ensure the activation and photothermal hydrolysis of COS. The presence of a suitable electron-metal-support interaction (EMSI) between the electron-rich La nanoparticles and TiO 2 might be responsible for these phenomena. In addition, theoretical calculations revealed that light-induced electron transfer was conducive to H 2 O dissociation and COS activation, while La doping reduced the free energy of the hydrolysis reaction. This work demonstrates the effectiveness of La-Ti@K catalyst in COS photothermal hydrolysis and provides a theoretical basis for further understanding of the photothermal catalytic mechanism.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Changjin Liang,Honghai Wu,Yufeng Guan
Ferrihydrite (Fh) is a vital geosorbent in the natural environment. Here, Fh materials with lanthanum (La) substituted in varied La/La + Fe ratios were synthesized, and these La-Fh materials were investigated in-depth via adsorption kinetic and isothermal experiments to explore their adsorption performance for chromate [Cr(VI)] in soils. Material properties of La-Fh were further characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectrometer (FTIR), and X-ray photoelectron spectroscopy (XPS). The results clearly indicate that La 3+ can be integrated into the Fh lattice, but the increase in La amount substituted into Fh is slowed down when the La/La + Fe ratio reaches to a larger value. Those La 3+ cations that fail to become integrated may either get adsorbed or form a phase of La(OH) 3 on La-Fh surfaces. We also find that La substitution reduces the specific surface area (SSA) of La-Fh samples but raises their pH pzc , which hampers La-Fh conversion to hematite and thus increases the chemical stability. These changes are related to the La-Fh structure and surface aspects, but they do not negatively affect the Cr(VI) adsorption efficacy, which can be promoted over a wide pH range to an alkaline pH. For instance, the maximum adsorption amount of Cr(VI) by 20%La-Fh is 30.2 mg/g at a near-neutral pH. However, the entire chromate adsorption processes are affected by H 2 PO 4 − and humic acid due to their strong affinities for Cr(VI), but almost not influenced by NO 3 − and Cl − . All the Cr(VI)-Fh reactions are well described by the fitted adsorption Freundlich model and conform to the pseudo-second-order reaction kinetic equation . The mechanisms which enhance La-Fh's adsorption ability for Cr(VI) are governed by chemical interactions, because La substitution can increase the hydroxyl density on Fh surfaces and thus improve the reactivity of La-Fh towards Cr(VI), leading to an evidently enhanced Cr(VI) immobilization onto La-Fh.
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Journal of Water Process Engineering
·
2023
·
IF 7
Shuangli Li,Yu Zhang,Sen Qiao,Jiti Zhou
Although MIL-101(Fe) has a homogeneous distribution of active metal sites, the relatively low stability of its coordination bonds limits its potential for application, especially in harsh environments. Here, a novel lanthanum-doped MIL-101(Fe)-NH 2 @mesoporous SiO 2 yolk-shell (LMFN-YS) material, synthesized by green water-etching, has effectively improved the adsorption capacity and stability of MIL-101(Fe)-NH 2 . Compared to traditional acid-base etching methods, water etching offered a more co-friendly and cost-effective approach to producing yolk-shell structures. Due to the mesoporous protective shell of mesoporous SiO 2 and more exposed active sites, the yolk-shell materials showed a faster adsorption rate (30 min) and a larger uptake capacity (240.0 mg P/g) than those of MIL-101. The material also exhibited broad range of pH stability from 2 to 10 and displayed good cyclic regeneration ability, with a removal efficiency of 75.9 % after three cycles. Additionally, it demonstrated excellent selectivity towards various coexisting anions such as Cl − , NO 3 − , SO 4 2− , CO 3 2− and HCO 3 − at diverse ionic strengths ranging from 0.001 to 1 M. The superior performance of L 1 MFN-YS (yolk-shell materials of La: Fe = 1:1) was attributed to a combination of factors, including ligand exchange between La(Fe)-OH and phosphates, Lewis acid-base interaction and electrostatic attraction. Additionally, high phosphate removal performance was observed in the real petrochemical wastewater (initial concentrations of 5.48 mg P/g) with a residual effluent concentration of 0.05 mg P/L, which was below the A-level standard of phosphate effluent in China (0.5 mg/L). This work provides a green method for preparing yolk-shell materials with improved ability to treat phosphate wastewater.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Ze Zhu,Xiaoqian Zhang,Ying Peng,Zhenfeng Guo,Yongshuai Xie,Benxue Liu,Guanghui Zhang,Luyi Zhu,Xinqiang Wang,Yonggang Jiang,Jian Feng
Rare earth zirconates have incomparable chemical thermophysical properties , yet the difficulty of preparation methods limit their application as fibrous material. In present work, a spinnable La 2 Zr 2 O 7 precursor, named as carboxylate lanthanum-zirconium (COLZ), was developed using carboxylic acids as structural and functional ligands. When COLZ is in its liquid state, it can be readily processed into desired shapes, allowing preparation of high aspect ratio precursor fibers with dense and bonding-strong internal structures. The spinnability was explained by the transformation from solid to liquid state under external forces, in which dynamic bridging of carboxylate and hydroxyl between nano-sized colloidal particles play a key role. Due to weakly acidic ligands, organics in COLZ can be easily removed, making direct heat treatment at the target temperature possible, which is beneficial for massive production. The strategy of developing spinnable precursor could also be applied to prepare other rare earth zirconate fibers or new multi-oxide fibers.
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Journal of Materials Research and Technology-JMR&T
·
2023
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IF 6.4
Qiaoyun Liu,Yifeng Yu,Changjiang Liu,Yuhang Liu,Liangjie Yuan,Zheng Wang,Aixi Yu
Lanthanum (La) compounds have attracted much attention because of low toxicity and biocompatibility. In this study, a series of La-doped magnesium phosphate composites bone repair materials (LMPCs) were prepared by the precursor method, in which the molar ratio of lanthanum was 1%, 3% and 5%, respectively. The results of X-ray powder diffraction, scanning electron microscope and compressive strength test show that La-doped magnesium phosphates (LMPs) synthesized by the precursor method have uniform particle distribution, high purity and excellent degradability. In vitro research results show that LMPCs exhibited reliable biosafety and excellent bioactivity. The introduction of lanthanum enhances the antibacterial activity of Escherichia coli and Staphylococcus aureus of the composite. Furthermore, the combined system of released La 3+ and Mg 2+ is more conducive to promoting the proliferation of mesenchymal stromal cells (MSC) and angiogenesis of human umbilical vein endothelial cells (HUVECs) when the content of lanthanum is 3% (referred to as LMPC-2). By up-regulating the expression of alkaline phosphatase (ALP) and Runt-related transcription factor 2 (RUNX2), LMPC-2 is prominent in promoting osteogenic differentiation, and mineralized calcium deposition in vitro . Moreover, the results of micro-CT, H&E and Masson staining confirmed the beneficial effect of the combined system of La 3+ and Mg 2+ on the repair of rat skull defects in vivo . These achievements will provide new strategies for improving the biological activity of LMPCs and provide reference value for bone repairing in the clinic.
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BIOELECTROCHEMISTRY
·
2023
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IF 5
Qin Xia,Zhaode Mu,Min Qing,Jing Zhou,Lijuan Bai
In recent decades, the incidence of breast cancer has increased year by year, posing a serious threat to human health and quality of life, and about 30% of breast cancer patients have human epidermal growth factor receptor 2 (HER2) overexpression. Therefore, HER2 has become an important biomarker and indicator for the clinical evaluation of breast cancer in diagnosis, prognosis and recurrence. In this work, polyethyleneimine functionalized MoS 2 nanoflowers (PEI-MoS 2 NFs) with good electrical conductivity and abundant active binding sites were designed and employed as a sensing platform for immobilizing the primary antibody of HER2 (Ab 1 ). In addition, a La-MOF-PbO 2 composite with a large specific surface area and good conductivity was used to load lots of electroactive toluidine blue (TB) and the secondary antibody of HER2 (Ab 2 ) via gold nanoparticles (AuNPs) as the linker. Thus, the constructed sandwich-type electrochemical immunosensor was applied for sensitive detection of HER2, which showed a wide linear range from 100 fg mL −1 to 10 μg mL −1 with a lower limit of detection of 15.64 fg mL −1 . Therefore, the resulting immunosensor in this study would have a potential application in clinical bioanalysis.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Yiping Feng,Jingyi Wu,Haijian Lu,Wenhao Lao,Hongda Zhan,Longyong Lin,Guoguang Liu,Yirong Deng
The widespread application of rare earth elements (REEs) has raised concerns about their potential release into the environment and subsequent ingestion by humans. Therefore, it is essential to evaluate the cytotoxicity of REEs. Here, we investigated the interactions between three typical REEs (La, Gd, and Yb) ions as well as their nanometer/μm-sized oxides and red blood cells (RBCs), a plausible contact target for nanoparticles when they enter the bloodstream. Hemolysis of REEs at 50–2000 μmol L −1 was examined to simulate their cytotoxicity under medical or occupational exposure. We found that the hemolysis due to the exposure of REEs was highly dependent on their concentration, and the cytotoxicity followed the order of La 3+ > Gd 3+ > Yb 3+ . The cytotoxicity of REE ions (REIs) is higher than REE oxides (REOs), while nanometer-sized REO caused more hemolysis than that μm-sized REO. The production of reactive oxygen species (ROS), ROS quenching experiment, as well as the detection of lipid peroxidation, confirmed that REEs causes cell membrane rupture by ROS-related chemical oxidation. In addition, we found that the formation of a protein corona on REEs increased the steric repulsion between REEs and cell membranes, hence mitigating the cytotoxicity of REEs. The theoretical simulation indicated the favorable interaction of REEs with phospholipids and proteins. Therefore, our findings provide a mechanistic explanation for the cytotoxicity of REEs to RBCs once they have entered the blood circulation system of organisms.
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RSC Advances
·
2016
·Vol. 6
·期 34
·28331-28342
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IF 3.289
Lu Wang,Xi Xie,Di Liu,Xiao-Bin Fang,Peng Li,Jian-Bo Wan,Cheng-Wei He,Mei-Wan Chen
Reduction-sensitive micelles with crosslinked cores were developed to load the lipophilic chemotherapeutic drug docetaxel (DTX) in order to overcome the issues of toxicity, water insolubility, and rapid metabolism of DTX. These DTX-loaded micelles (MM(DTX/Crosslink)) provide efficient incorporation and sustained release of DTX. Using independently synthesized LA–PLGA–TPGS and DSPE–PEG polymers as vehicles, MM(DTX/Crosslink) was found to be reduction-responsive, and possessed desirable drug entrapment efficiency (84.17 ± 1.15%) and drug loading efficiency (6.21 ± 0.07%). The MM(DTX/Crosslink) quickly dissociated under reduction conditions that mimicked the reductive intracellular environment, suggesting that it can rapidly release the encapsulated DTX in vitro. Furthermore, to target MM(DTX/Crosslink) to tumors for cancer therapy, iRGD was conjugated to the surface of MM(DTX/Crosslink). The iRGD-MM(DTX/Crosslink) micelles significantly increased the cellular uptake of DTX and inhibited cell proliferation, compared to the micelles without iRGD modification. Moreover, the iRGD-MM(DTX/Crosslink) micelles presented enhanced antitumor effects based on the analyses of apoptosis and cell cycle arrest. The micelles developed in this work may constitute a stable, efficient, and powerful system to deliver DTX into cancer cells.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Xin Ke,HuiPing Shao,HaiHong Liu,Wengang Liu
In this study, an Fe-La-CS adsorbent with a reticulated structure was prepared by an in situ method, which was able to adsorb arsenate efficiently over a wide pH range of 3–11. The incorporation of iron and lanthanum ions broadened the tolerant pH range of the adsorbent compared with chitosan beads (CS). Arsenic was mainly present in the pH range of 3–9 as two forms, H 2 AsO 4 − and HAsO 4 2− . Calculations using the density-functional theory (DFT) showed that in the Ligand interactions and electrostatic interactions dominate in the pH range, with surface precipitation, and hydrogen bonding interactions playing a facilitating role. The background ions mainly compete with arsenic adsorption for electrostatic interaction sites. However, due to the different valence states of the background ions, the competition intensity is different. Such as low valence state representative ions Na + , K + competitiveness is weak, and arsenic competition adsorption first occupy different adsorption sites, therefore, from the quantum chemistry and molecular dynamics point of view of Na + , K + on arsenic adsorption almost no effect. Cl − , SO4 2− will have some influence on arsenic adsorption because of the same charge with arsenic, but the charged amount is smaller than arsenic and the molecular structure is different from that of arsenic, so the influence is not very big. In summary, the material design of Fe-La-CS adsorbent has great potential and theoretical significance for selective purification of heavy metal wastewater at wide pH.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Dongze Ren,Mingjie Liu,Min Cao,Shan Wang,Sixing Fan,Mozhen Liu,Jianbin Zhang,Huijun Sun
Osteoarthritis (OA) is an irreversible degenerative disease of articular cartilage that commonly occurs in the middle-aged and elderly people. However, effective intervention for early and middle-stage OA is still limited due to its complex and multifactorial nature. Excessive reactive oxygen species (ROS) and the inflammatory microenvironment are considered to play crucial roles in the occurrence and development of OA. Here, a novel HPB@LA@PDA nanoplatform is designed, which utilizes the mimicking enzyme activity of hollow prussian blue (HPB) nanozymes and antioxidant activity of lipoic acid (LA), to synergistically scavenge ROS and remodel the OA microenvironment. HPB@LA@PDA was firstly synthesized and the characterizations were confirmed by TEM, DLS, XPS, FTIR, UV–Vis, and XRD methods. It exhibited excellent multienzyme-like (SOD, GPx, CAT and POD-like) activities and antioxidant activities, converting •O 2 − , H 2 O 2 , •OH and reactive nitrogen species into harmless products. Importantly, at both the cellular and animal levels, we found HPB@LA@PDA could effectively scavenge excess ROS, protect against ROS-induced oxidative stress, apoptosis and ferroptosis, and ameliorate mitochondrial dysfunction, reduce inflammatory expression, and inhibit macrophage polarization in the chondrocytes. Finally, the results of in vivo study demonstrated that HPB@LA@PDA exhibited good biocompatibility and excellent therapeutic efficacy in the OA rat model. Micro-CT scaning, histopathological and immunofluorescence staining and western blotting analysis confirmed that HPB@LA@PDA attenuated the progression of OA by way of scavenging reactive oxygen species and remodelling the inflammatory microenvironment. The combination of drug and nanoenzyme vehicle offers a promising prospect for the treatment of various inflammatory diseases, including OA.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Yue Zhou,Fangbin Lin,XiaoDong Wang,Hui Wang,Bingchun Xue
The development of adsorbents with high adsorption capacity and wide adaptable pH range was crucial to effectively controlling of water environment pollution. In this study, three-dimensional porous chitosan gel microspheres loaded with Ni and La (Ni-La-CS) were prepared for the adsorption of excessive phosphorus. The performance was investigated using glyphosate isopropylamine salt (GIS) and KH 2 PO 4 , which were selected as representative substances for organic and inorganic phosphorus. Results showed that Ni-La-CS exhibited high phosphorus removal efficiency with wide adaptable pH range. The adsorption process was monomolecular layer chemisorption , and the adsorption was spontaneous and endothermic. The coexistence of F − promoted the adsorption of phosphorus, while Cl − , SO 4 2− , CO 3 2− and HCO 3 − inhibited the adsorption. The material retained stability even after 5 cycles and the actual phosphorus-containing wastewater with 3.13 mg·L −1 could be treated to meet Chinese first-class standard.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Tianyun Zhao,Qiuwan Shen,Martin Andersson,Shian Li,Jinliang Yuan
High-entropy perovskite catalyst was synthesized and utilized for the first time in the MSR catalytic reaction. Among the HEPs, La(CoCuFeAlCe) 0.2 O 3 exhibited excellent MSR activity and high selectivity. The mechanism of the MSR reaction on the catalyst (100) surface was studied by employing DFT. The results indicate that the surface of La(CoCuFeAlCe) 0.2 O 3 catalyst has the lowest energy barrier, where the aldehyde hydrogenation reaction is the rate-determining step, explaining its high activity and selectivity. This research contributes additional evidence for the creation of high-entropy perovskite catalysts for MSR.
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