COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Jiang-Bo Huo,Kiran Gupta,Changyong Lu,Hans Chr. Bruun Hansen,Ming-Lai Fu
Efficient removal of aqueous arsenic is still a great challenge in particular for producing clean drinking water and for waste water treatment. To this end, a novel magnetic porous Fe-La composite, comprising La 2 O 2 CO 3 and Fe 2 O 3 , was fabricated via a self-sacrificing template method based on bimetallic (Fe, La)-MOFs calcined at 550 °C. Batch adsorption results demonstrated that Fe-LaXY (X and Y represent the feeding mole ratio of Fe and La precursors) exhibited a maximum adsorption capacity of As(V) (241, 251 and 410 mg g −1 for Fe-La51, Fe-La21 and Fe-La11, respectively), and they also showed satisfactory adsorption kinetics, which can be ascribed to a strong coordination between La and arsenate species. Coexisting sorbates including carbonate, silicate, sulfate, and humic acid had a slight influence on adsorption performance of arsenate, while phosphate isostructural to arsenate gave severe interference. More importantly, the Fe-La11 could be easily separated from water due to its magnetism (7.0 emu g −1 ), and it also exhibited excellent recyclability (above 80% of removal efficiency at the fifth cycle) as well as stability in terms of release of Fe and La ions (< 0.5 mg L −1 at pH 4.0–10.0). Based on results from X-ray photoelectron spectroscopy (XPS), Powder X-ray diffraction (PXRD) and Raman spectroscopy, it is demonstrated that ligand exchange of surface hydroxyl groups and the formation of inner-sphere surface complexes are main responsible for the As(V) removal mechanism. Combining the magnetic properties, the absorption properties and the recyclability make Fe-LaXY derived from bimetallic MOFs promising sorbents for arsenate removal.
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Chemical Engineering and Processing-Process Intensification
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2018
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IF 2.826
Yanyan Guo,Chengna Dai,Zhigang Lei
A series of Pd-La/SiO 2 /cordierite (cordierite = COR) and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts were prepared, characterized, and tested for the hydrogenation of 2-ethylanthraquinone (eAQ) as the key step of anthraquinone method for production of H 2 O 2 . It was found that the metal particle size is remarkably dependent on the Pd/M (M = La, and Zn) mass ratio of bimetallic monolithic catalysts. By virtue of its small metal particle size and the strong interaction, the 0.8% Pd-0.4% La/SiO 2 /COR monolithic catalyst presents the highest H 2 O 2 yield (7.7 g L −1 ) and selectivity toward active quinones (95%), which is attributed to the addition of La leading to the synergistic effect between Pd and La. Moreover, the density functional theory (DFT) calculations for the adsorption of eAQ over the surface of Pd-La/SiO 2 /COR and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts have been conducted to further understand the mechanism of molecule–surface interactions between eAQ and the PdM(1 1 1) or Pd(1 1 1) surfaces. Detailed studies showed that the high catalytic activity of Pd-La/SiO 2 /COR bimetallic monolithic catalyst is attributed to the stronger adsorption between Pd 3 La 1 (1 1 1) and the carbonyl group of eAQ.
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GREEN CHEMISTRY
·
2015
·Vol. 17
·期 5
·2888-2895
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IF 8.02
Jian-hua Guo,Guang-yue Xu,Fei Shen,Yao Fu,Ying Zhang,Qing-xiang Guo
The long-chain alkanes obtained from the hydrodeoxygenation of plant oils are ideal substitutes for diesel. In this work, a new efficient catalytic system was established for the conversion of plant oil to long-chain alkanes under mild conditions with a bi-functional Ru/La(OH)3 catalyst. The hydrodeoxygenation of stearic acid was performed in an autoclave with Ru-based catalysts with different supports (HZSM-5, ZSM-5, SiO2–Al2O3, SiO2, ZrO2, Mg(OH)2, La(OH)3, and La2O3). Among these catalysts, Ru supported on basic La(OH)3 showed a remarkable catalytic performance for the reaction. Over 98% of long-chain alkanes were obtained with 100% conversion of stearic acid at 200 °C and 4 MPa H2. When crude Jatropha oil was hydrogenated, about 80.7 wt% of long chain alkanes were obtained under the optimized conditions (200 °C, 4 MPa H2, 8 h). The high efficiency of the Ru/La(OH)3 catalyst could be due to a co-effect of the high hydrogenation activity of Ru and the basic La(OH)3 support which can attract the acidic raw material. Additionally, the Ru/La(OH)3 catalyst was recycled four times and maintained a good activity and stability. The reaction pathway was also explored by using stearic acid as a model compound. Hydrogenation–decarbonylation could be the main pathway to produce n-heptadecane, which has one carbon atom less than stearic acid.
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Journal of Environmental Sciences
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2016
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IF 2.208
Zhuowei Cheng,Zhiqi Gu,Jianmeng Chen,Jianming Yu,Lingjun Zhou
The photocatalytic oxidation of gaseous chlorobenzene (CB) by the 365 nm-induced photocatalyst La/N–TiO 2 , synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology (RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–TiO 2 (0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD (X-ray diffraction), TEM (Transmission Electron Microscopy), FTIR (Fourier transform infrared spectroscopy), UV–vis (Ultraviolet–visible spectroscopy), and BET (Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped TiO 2 nanotubes than with reference TiO 2 . The removal of CB was effective when performed using the synthesized photocatalyst, though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS (Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC (volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification.
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APPLIED SURFACE SCIENCE
·
2016
·
IF 3.15
Yahui Zhang,Xiaoyan Lin,Quisheng Zhou,Xuegang Luo
The magnetic core-shell Fe 3 O 4 @Alg-La particles were fabricated successfully by a simple method of electro-coextrusion, and employed as an adsorbent for separation of fluoride from aqueous solution. Main factors affecting the removal of fluoride, including pH, adsorbent dosage, initial concentration, temperature and contact time were investigated. The adsorption isotherm and adsorption kinetics were studied to understand the adsorption process in detail. The experimental data were fitted well by the non-linear Freundlich isotherm and linear pseudo-second-order model, the maximum fluoride adsorption capacity was 45.230 mg/g at pH 4, 298.15 K. Thermodynamic parameters indicated that the fluoride adsorption process was feasible and spontaneous. The presence of other anions like Cl − , SO 4 2− , HCO 3 − and PO 4 3− had almost no effect on the fluoride adsorption. The adsorbent can be easily separated from the solution by a magnet. The magnetic core-shell Fe 3 O 4 @Alg-La particles before and after fluoride adsorption were studied by SEM, FTIR, EDX and XPS, which indicated that the adsorption mechanism may be related to electrostatic attraction and Lewis acid-base interaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiaomei Jiang,Min Ma,Yujie Cui,Boyang Lu,Zhiguo Lin,Fengzhi Jiang
To enhance the phosphate removal performance, a porous material (La MOF-20 %-C) was prepared by selectively removing the thermally unstable NH 2 -BDC ligand from a lanthanum dual organic ligand MOF through pyrolysis. This innovative approach equips La-MOF-20 %-C with dual functionalities: high phosphate adsorption capacity and robust antibacterial effects. The adsorbent showcased a remarkable phosphate adsorption capacity of 97.24 mg P/g and reached equilibrium within 90 min. The material exhibits good anti-interference capability, and the presence of multiple coexisting ions does not affect its adsorption performance. Additionally, it can be used over a wide pH range (3.0–8.0) and has good reusability. Mechanistic studies indicated that electrostatic attraction and ligand exchange were the primary mechanisms for phosphate adsorption. Moreover, La MOF-20 %-C effectively inhibited the metabolic activities of Escherichia coli and Staphylococcus aureus through phosphorus starvation and electrostatic attraction, demonstrating significant antibacterial properties. Importantly, the fabrication of this material into a filter membrane enabled the successful treatment of 16.8 L of actual wastewater, achieving an overall phosphate removal rate of over 85 %, and effectively removing total bacteria. These findings highlight La MOF-20 %-C as a highly promising material with dual functionality for phosphate removal and bacterial inhibition.
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CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Tianyang Liu,Junli Wang,Xuanbing Wang,Jinlong Wei,Xiaoning Tong,Shengyou Su,Ju Zhang,Yuantao Yang,Ruidong Xu,Linjing Yang
The traditional Pb-Ag anodes used in zinc electrowinning exhibit high overpotential for oxygen evolution reaction (OER) and poor mechanical strength, leading to high energy consumption. To overcome the shortcomings, Ti/SnO 2 -Sb 2 O 4 /PbO 2 -La-doped MnCo 2 O 4.5 composite anode was prepared by this work. It demonstrated enhanced electrochemical performance, requiring 565 mV to reach the benchmark current density of 50 mA cm −2 , and the Tafel slop of 179.79 mV dec –1 in the acidic media containing 50 g L –1 Zn 2+ and 150 g L –1 H 2 SO 4 . According to the results of XPS, the content of Mn 4+ and Co 3+ increased, which was beneficial to promote the OER catalytic activity of the electrode. The current efficiency was improved by 1.7 % compared with traditional Pb-0.76 % Ag anode, resulting in a significant reduction in energy consumption of 477.46 kW∙h for producing one ton of zinc. Moreover, the Ti/SnO 2 -Sb 2 O 4 /PbO 2 -La-doped MnCo 2 O 4.5 anode showed excellent corrosion resistance, and the accelerated service time was extended to 50 h at 2 A cm −2 . The service life of the electrode was extended thanks to the introduction of the intermediate layer and La-doped MnCo 2 O 4.5 powder. Therefore, this work provided a novel strategy to prepare the anodes with enhanced electrochemical performance applied in zinc electrowinning and other aspects.
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Desalination and Water Treatment
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2024
·
IF 1
Weikang Zheng,Boyan Wang,Zhenzhong Liu,Hongwei Yang,Zhanli Chen,Xiangrong Sun
Microplastics (MPs) in the aqueous environments has attracted widespread attention because of its potential risk to human health.Its high stability makes it difficult to be degraded and long term presence in the environment. Therefore, it is crucial to find an efficient and clean technology to remove microplastics in water. The advanced electrocatalysis oxidation process (AEOP) shows great potential for application. In this work, We focused on preparing Ti/Sb-SnO 2 electrodes doped with different rare earth elements (La, Ce, Sm or Nd) as active layer by sol-gel method. The electrooxidation system has efficiently degraded MPs in aqueous solution. The optimal parameters for the removal of MPs were electrode spacing of 1.5 cm, current density of 46.67 mA·cm −2 , Na 2 SO 4 electrolyte concentration of 0.22 mol·L −1 , and initial solution pH of 7. After 3 h, MPs removal rate by Ti/La-Sb-SnO 2 system reached 28.3 %, which was higher than the Ti/Ce-Sb-SnO 2 , Ti/Sm-Sb-SnO 2 , Ti/Nd-Sb-SnO 2 and Ti/Sb-SnO 2 electrode, the removal rates were increased by 8.23 %, 10.13 %, 16.28 % and 77 %, respectively. Electrochemical performance tests and •OH (Hydroxyl radicals) generation results indicated that the surface of Ti/La-Sb-SnO 2 electrode had abundant active sites, which promoted the formation of •OH to degrade microplastics effectively. In summary, the rare earth element-doped Ti/Sb-SnO 2 electrode provides crucial technological support for the electrooxidative removal of microplastics from water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Ruiyuan Jia,Xiaomeng Yu,Wenhui Wang,Kemeng Du,Yuru Liu,Yufei Wang,Wenjun Wu,Jin Guo
A lanthanum-modified polyethersulfone composite membrane (La-PES) loaded with nitrogen-doped carbon nanotubes (NCNT@La-PES) was successfully fabricated in this study. The NCNT@La-PES membrane could activate PMS, which enabled the degradation of phosphonate to phosphate, while also possessing the capability for adsorptive recycling of phosphorus. During the processing of 10.31 mg/L 1-hydroxyethane-1,1-diphosphonic acid (HEDP) in the NCNT@La-PES / PMS system, the removal efficiency of HEDP achieved 100 %, and almost 78 % of total phosphate (TP) in HEDP was transformed into phosphate, which were further adsorptive recycled by the La-PES membrane. The NCNT@La-PES/PMS system demonstrated exceptional performance across a broad pH range (4–10), with complete removal of HEDP and adsorption recovery of 73 % transformed phosphate. The decrease in pH caused by catalytic reaction reduced the hindrance of the alkaline environment to phosphate adsorption. The NCNT, acting as a catalyst, facilitated the formation of surface-bound radicals upon PMS activation, playing a pivotal role in the degradation of HEDP. The adsorption of phosphate by La-PES was primarily attributed to the ligand exchange between La(OH) 3 and phosphate. Moreover, NCNT@La-PES/PMS system showed significant catalytic and adsorption performance in consecutive cyclic treatment of HEDP in actual water, indicating its potential in practical application.
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CATALYSIS COMMUNICATIONS
·
2017
·
IF 3.33
Baohuai Zhao,Rui Ran,Li Sun,Zesheng Yang,Xiaodong Wu,Duan Weng
A high-surface-area La-Ce-Mn mixed oxide was synthesized by citrate method, with further acid etching to dissolve the La 3 + ions in the lattice. The acid etching process efficiently improved the specific surface area, increased the ratios of Mn 4 + /Mn n + , Ce 3 + /Ce n + , O α /O tot , and enhanced the oxygen mobility of the catalyst, which were responsible for the superior catalytic performance. Compared to the pristine La 0.8 Ce 0.2 MnO 3 + δ catalyst, the etched one could convert CO and C 3 H 8 more efficiently, with 90% conversion of CO and C 3 H 8 at only 73 and 196 °C, respectively. Such superior catalytic performance made it possible to be used for automotive emission control during cold-start period.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiahao Cui,Xiaolong Gao,Kejing Pang,Wenbing Wu,Mrigendra Kumar Awasthi,Yihua Zhao,Xianqiang Yin
Current single-atom studies in the perdisulfate (PDS) system were focused on transition metals, but researching La-series metals might provide new insights for the efficient utilization of this system. The original structure’s Zn was evaporated at high temperatures, thereby we utilized Zeolitic Imidazolate Frameworks (ZIFs) as a substrate to synthesize a type of La-SACs catalysts. The La single atom in this work was identified to the La-N 4 configuration through La-L3 X-ray edge absorption spectroscopy. Experimental observations in suspension demonstrated that the PDS activation capability of La is on par with, if not superior to, that of transition metals such as Co and Cu. Tetracyclines (10 mg/L) were eliminated within 30 min via La-N-C + PDS systems and the pseudo-first-order was higher than 0.0929 min −1 . The Hydrogen bond between PDS and La-N-C and active electron of d orbital in La atoms had the significant influence on the generation of ROS ( 1 O 2 and •OH). Furthermore, the excellent electron transfer of La-N-C also promoted the activation rate of PDS. The findings of this study indicated that La could play a crucial part in PDS catalyst for degradation of organic pollutes in aquatic environment, providing the new method for exploration of single-atom materials in PDS systems.
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VACUUM
·
2024
·
IF 3.8
Zuhong Ji,Yunfei Sun,Xiaodong Guan,Yang Zhou,Junchao Qian,Feng Chen
In this work, the La substitution of iron and replacing the oxygen with fluorine are both adopted to expectantly enhance the rate performance and structure stability of LiFePO 4 during working. The characterizations of X-ray diffraction, scanning electron microscope , transmission electron microscope, charging-discharging tests, electrochemical impedance spectroscopy and safety tests are used to investigate the influences of La 3+ and F − doping on the LiFePO 4 . The results indicate the cathodes after La 3+ doping not only deliver the larger lattice parameters and unit cell volume to broaden the lithium ions migration pathway and accelerate the Li + diffusion speed, but also strengthen the whole bond energy of LiFePO 4 owing to the high bond energy of La–O. In addition, the F replacement of O could increase the length of Li–O bonds and decrease the length of P–O bonds, further be helpful to enhance the Li + diffusion between LiFePO 4 phase and FePO 4 phase due to the weakening of Li–O bonds. Finally, the La 3+ and F − co-doped cathode delivers the superior discharge capacity of 139.3 mAh g −1 at 5C high rate and 127.2 mAh g −1 at −20 °C, with the high discharging capacity of 160.1 mAh g −1 after 100 cycles at 45 °C.
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