APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Junzhe Jiang,Yushuai Jia,Yabin Wang,Ruifeng Chong,Liping Xu,Xin Liu
Antibiotic has become an important organic contaminant in surface water, which poses a huge threat to human health and ecosystem. SrTiO 3 is an attractive perovskite structured semiconductor material and shows promising applications in photocatalysis . Herein, a series of lanthanum and chromium codoped SrTiO 3 (denoted as SrTiO 3 (La,Cr)- x ) with different dopant amount of La and Cr have been successfully fabricated via a facile sol-gel hydrothermal method and employed as efficient photocatalysts for the elimination of tetracycline (TC) from aqueous solution under visible-light irradiation. It indicates that the photocatalytic performance is highly dependent on the La and Cr content in the samples. Among the catalysts, the porous SrTiO 3 (La,Cr)-6 spheres with a moderate dopant amount exhibit the best photocatalytic activity for TC removal, which is approximately 4.4 and 2.3 times as superior as SrTiO 3 (La,Cr)-2 with the least dopants and SrTiO 3 (La,Cr)-8 with the most dopants, respectively. Detailed characterizations reveal that the significant improvement of photocatalytic activity is attributed to the increasing molar ratio of Cr 3+ /Cr 6+ , which can be facilely adjusted by tuning the doping amount of La and Cr during the synthesis process. In addition, the catalyst shows excellent photocatalytic stability and can be recycled over ten times with negligible activity decline. Active species trapping experiments demonstrate that superoxide radicals, holes and hydroxyl radicals are responsible for TC degradation. On the basis of the intermediate products identified using HPLC-MS, four possible reaction pathways and TC degradation mechanism have been put forward. This study offers an effective strategy to modulate the photocatalytic properties of SrTiO 3 by simple tuning the dopant content for environment and energy applications, which can be facilely extended to the modification of other semiconductors.
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高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2018
·Vol. 29
·期 9
·7692-7700
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IF 2.324
Hu Zhen,Guo Haiyong,Zhao Li,Wu Yadan,Wang Shimin,Wan Li
A double-layer composite film (DLCF) that consists of upconversion composite La(OH) 3 :Er 3+ /Yb 3+ +P25 (UC + P25) as underlayer and large TiO 2 spheres (LS-TiO 2 ) as overlayer is designed as the photoelectrode of dye-sensitized solar cells (DSSCs). The upconversion luminescent material La(OH) 3 :Er 3+ /Yb 3+ can convert near-infrared region to visible light to improve the light absorption, and LS-TiO 2 has been used as light-scattering layer to increase the optical length in the film and enhance light harvesting. The DLCF with lower absorbed dye achieved the highest conversion efficiency due to the synergistic effect of the upconversion luminescent layer and the light-scattering layer, and with an optimum mixing ratio, a conversion efficiency of 9.24% is attained, which is a significant improvement of 68.3% compared with the pure P25 film photoelectrode.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Rui Cao,Xueqian Wang,Langlang Wang,Fangxian Cao,Xiang Li,Lu Wang,Jinghao Xiang,Ping Ning
The introduction of surface basic sites to COS hydrolysis catalysts can improve H 2 O activation and COS adsorption, leading to enhanced catalytic performance. However, maximizing the concentration of basic sites remains a challenge due to the limited exposed surface area of these catalysts. Herein, a La/Al 2 O 3 catalyst with abundant alkaline sites to catalyze the hydrolysis of COS was prepared by a simple ammonia-assisted hydrothermal method. This synthesized La/Al 2 O 3 catalyst exhibits a thin rod-like structure formed by the random accumulation of nanoparticles. Lanthanum, one of the most abundant rare earth metals, is an ideal doping aid to further promote the COS-catalyzed hydrolysis performance of Al 2 O 3 . Characterization studies show that the proper lanthanum loading effectively enhances the formation of basic sites, leading to improved lattice oxygen reactivity and –OH adsorption capacity. As a result, the prepared La-loaded Al 2 O 3 nanorod sample with abundant basic sites exhibits nearly 100 % COS conversion and total H 2 S yield at 160 °C. In addition, the reaction pathways and deactivation mechanisms for selective catalytic hydrolysis of COS on the La-doped Al 2 O 3 catalyst were revealed by using in situ DRIFTS to evaluate COS adsorption and hydrolysis. Density functional theory calculations showed that La loading enhances the electron transfer between the La and Al atoms, improves the formation of basic sites, and enhances the adsorption of –OH. This study provides new insights into the design of efficient alumina-based catalysts for the catalytic hydrolysis of COS.
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APPLIED SURFACE SCIENCE
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2017
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IF 3.387
Xin Liu,Junzhe Jiang,Yushuai Jia,Jinmin Qiu,Tonglin Xia,Yuhong Zhang,Yuqin Li,Xiangshu Chen
The efficient treatment of dye wastewater has been a hot topic of environment field. The integration of adsorption and photocatalytic degradation via fabrication of bi-component heterojunction photocatalyst is considered as a facile and effective strategy to enhance the dye elimination efficiency. In this report, a Z-scheme heterojunction material, SrTiO 3 (La,Cr)/WO 3 with bifunction of adsorption and photocatalysis was successfully synthesized for efficient removal of methylene blue (MB) under visible light irradiation. The morphology and microstructure characterization demonstrates that the SrTiO 3 (La,Cr) nanoparticles are uniformly decorated on the WO 3 nanosheets, forming an intimate heterojunction interface. MB degradation results indicate that the removal efficiency by the synergistic adsorption-photocatalysis process is greatly improved compared to pure WO 3 and SrTiO 3 (La,Cr) with the adsorption and photocatalytic activity closely related to the composition of the material. The possible mechanism for the enhanced photocatalytic activity could be ascribed to the formation of a Z-scheme heterojunction system based on active species trapping experiments. Furthermore, the investigations of adsorption kinetics and isotherm show that the adsorption process follows pseudo-second-order kinetic model and Langmuir isotherm, respectively. Due to the synergistic advantages of negative zeta potential, large surface area and accelerated separation of photogenerated carriers driven by Z-scheme heterojunction, SrTiO 3 (La,Cr)/WO 3 exhibits excellent adsorption-photocatalytic performance and stability on MB removal, which could be potentially used for practical wastewater treatment.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yin Hu,Wei Chen,Fen Zhang,Lingling Wang,Xuanye Chen,Fei Han,Weiguo Song
Photocatalytic degradation of aqueous organic pollutant while hydrogen evolution has become an attractive and potential approach to address environmental pollution and energy shortages. The design of highly efficient photocatalyst and the mechanism study are the keys for this issue. For this purpose, a series of rare earth La doped perovskite NaTaO 3 were prepared by an easy solid-phase synthesis method. La doping changed the morphology, structure and physicochemical properties of NaTaO 3 crystal. More importantly, it also found that controllable La dopants formed a concentration gradient between the surface and bulk of NaTaO 3 crystal, which would cause a gradient of energy band structure. Noteworthy, 0.5La/NaTaO 3 was identified as the intermediate state with the La doping from A sites to B sites and from bulk to surface in NaTaO 3 crystal. It possessed a large La concentration gradient, leading to the better photoelectrochemical properties and photocatalytic performance than any other xLa/NaTaO 3 catalyst. For the photocatalytic reaction over 0.5La/NaTaO 3 , HCHO was partially mineralized and gradually converted to HCOOH due to the large energy barriers of the intermediate reaction steps, while H 2 was produced stably in the five recycle runs. The active species of • O 2 − , •OH and h + were detected by the control experiments with trapping agents, and • O 2 − was confirmed to be the dominant one in the photocatalytic reaction. On this basis, the possible mechanism was proposed to understand the photocatalytic system in depth.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Huidan Guan,Miao Lei,Dongxue Liu,Junpeng Guo,Ling Yan,Tian Chen,Ye Li
A novel La-Zr@SA/NIPAM adsorbent was synthesized through bimetallic modification of sodium alginate (SA) and acrylamide (NIPAM)-based hydrogel for efficient phosphate removal. Compared to conventional adsorbents, La-Zr@SA/NIPAM exhibits abundant active sites and remarkable selectivity for phosphorus, with a maximum adsorption capacity of 105.3 mg/g for phosphate. The material properties were thoroughly characterized using scanning electron microscopy-energy dispersive X-ray analysis (SEM-EDS), N 2 adsorption/desorption isotherms, Fourier transform infrared (FTIR), and X-ray photoelectron spectroscopy (XPS) techniques. N 2 adsorption/desorption isotherms analysis showed that the specific surface area was 125 m 2 /g and consisted mainly of mesopores, and the network structure was clearly observed in the SEM images to provide a good support structure for the adsorbent. Meanwhile, the study investigated the impacts of pH, temperature, concentration, coexisting competitive ions, recycling regeneration, and actual wastewater on phosphate adsorption. The adsorption process is exothermic and spontaneous, favored by higher temperatures. Kinetic and thermodynamic studies support pseudo-secondary kinetics and Langmuir modeling indicating monolayer chemisorption. Cycle regeneration and real wastewater experiments demonstrated that La-Zr@SA/NIPAM maintained 80 % phosphate removal even after six regenerations. The phosphate removal mechanism involves electrostatic attraction, ligand exchange, and complexation. Moreover, the treatment of real wastewater is similar to the experimental results and also has a significant effect on the removal of other ions, which highlights the great potential of this method in mitigating phosphorus pollution.
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Ying Zhong,Xiao Chen,Shiyao Liu,Huibin Liu,Deng Hu,Gwendoline Lafaye,Changhai Liang
The industrial advancement of downstream products resulting from the directed hydrogenation of maleic anhydride is hindered by the limitations related to the activity and stability of catalysts. The development of nonprecious metal intermetallic compounds, in which active sites are adjustable in the local structures and electronic properties embedded within a distinct framework, holds immense potential in enhancing catalytic efficacy and stability. Herein, we report that nickel-based silicides catalysts, RNi2Si2 (R = Ca, La, and Y), afford high efficiency in the selective hydrogenation of maleic anhydride. Among the RNi2Si2 with the same tetragonal structure, CaNi2Si2 with complete isolation and highest electron density of Ni sites presents the low apparent activation energy (98.4 kJ/mol). Preferential adsorption of intermediate succinic anhydride via C═O bonds is achieved by the high oxygen affinity of CaNi2Si2, resulting in chemoselectivity to γ-butyrolactone (>80%). Additionally, the silicide with good resistance to sintering and acid corrosion presents remarkable stability for at least 130 h. The design of the silicide structure will offer fresh perspectives on the development of effective and enduring selective hydrogenation catalysts.
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yutong Yang,Lijie Zhao,Danfeng He,Dongmei Shi,Bing Zhao,Haixia Yu,Wanxia Tang,Jianhua Zheng
Considering the potential effects of physical and chemical properties and morphology on photocatalytic performance, La doped Bi 2 WO 6 nanosheets (La/Bi 2 WO 6 -NS) were synthesized by immersion method using Na 2 WO 4 ·2 H 2 O, Bi(NO 3 ) 3 ·5 H 2 O and La(NO 3 ) 3 as raw materials. The synthesized La/Bi 2 WO 6 -NS was characterized by SEM, TEM, XPS, XRD, UV–vis, PL, I-t and EIS. The enhancement of the photocatalytic activity of La/Bi 2 WO 6 -NS in the degradation of tetracycline (TC) and reduction of chromium (VI) can be attributed to the oxygen vacancy level generated by La doping, which played a crucial role in improving the performance of Bi 2 WO 6 -NS. Moreover, the unique 2D nanosheets feature afforded abundant active sites and endowed an enhanced the visible light response, further improved photocatalytic performance. Additionally, 4 % La/Bi 2 WO 6 -NS exhibited extraordinary the simultaneously photocatalytic degradation of Cr(VI)/TC efficiency with 92.0 % and 90.8 %, which are much higher than that of single Cr(VI) and TC. Combining of the experimental confirmations and the deep DFT calculations, the synergistic photocatalytic mechanism of the synthesized material was investigated systematically.
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CERAMICS INTERNATIONAL
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2024
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IF 5.1
Keyang Shang,Yongbo Fan,Yuxin Jia,Xinghong Chen,Zhenhai Yang,Huiqing Fan,Weijia Wang
The poor electrical properties and high leakage current of BiFeO 3 -BaTiO 3 -based ceramics are the main reasons that hinder their application. A two-step sintering method prepared the 0.68Bi 1-x La x (Fe 99.8% Sb 0.2 % )O 3 -0.32BaTiO 3 ceramics (x = 0, 0.005, 0.01, 0.015, abbreviated as BL x FS-BT). The surface morphology and properties of the ceramic were observed and tested using different techniques. La ion doping significantly affects the crystal structure, leakage current, and the electro-induced strain of the BL x FS-BT ceramics. BL 0.005 FS-BT ceramics achieve 0.198 % unipolar electro-induced strain and 396 pm/V inverse piezoelectric coefficient under a 50 kV/cm electric field, and they can maintain good temperature stability at high temperatures. A large strain of 0.43 % was obtained at 150 °C. The inhibition effect of La ion on Fe valence and oxygen vacancy formation also greatly improves the insulation performance of ceramics. This work shows that BF-BT-based ceramics via ion substitution defect engineering effectively enhance electrical and insulating properties.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Shasha Zhang,Pengfei Zhu,Ming Duan,Bing He,Xinglin Li,Xiya Xin
In this paper, a novel direct Z-scheme heterojunction La-Bi 2 WO 6 /CdS composed of 3-dimensional flower-like Bi 2 WO 6 and hexagonally stacked succulent CdS was successfully designed and synthesized. The morphology, optical properties, element valence and crystal structure of the catalysts were systematically characterized. When the dosage of LBC-40 was 1.0 g/L, the degradation rate of oxytetracycline (OTC, 20 mg/L, pH = 6) was 85.28 %, under low visible light illumination (65 W energy saving lamp) for 120 min and the reaction kinetic constant (0.01336 min −1 ) was 2.50 and 1.56 times that of pure Bi 2 WO 6 and La-Bi 2 WO 6 , respectively. Moreover, La-Bi 2 WO 6 /CdS showed good photocatalytic activity for other single antibiotics, mixed antibiotics and antibiotics from different water sources. The photocatalytic activity only decreased by 7.69 % after 3 cycles. Furthermore, the possible photocatalytic degradation pathway and photocatalytic mechanism of OTC were proposed. The excellent photocatalytic performance of La-Bi 2 WO 6 /CdS is for that the doping of La 3+ and the construction of direct Z-scheme heterojunction enhances the visible light absorption capacity and separation efficiency of photogenerated electron-hole pairs. This paper reports a new method, which can provide a reference for the design and development of visible light responsive photocatalysts with excellent photocatalytic properties.
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高影响因子
RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3033-3052
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IF 2.8
Huang Guihua,Yang Zizhen,Li Sijia,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In-situ crystallization was used to prepare the composite molecular sieve ZSM-5/MOR (Z/M) successfully, and FeLa-ZSM-5/MOR (FeLa-Z/M) was obtained by loading Fe and La on the surface of the composite molecular sieve by hydrothermal method. The composite molecular sieve combined the water absorption of mordenite (MOR) and the mass transfer performance of ZSM-5, and effectively improved the surface area and porous structure. This zeolite improved the dispersion performance of active sites in Z/M and reduced mutual aggregation between particles, which was conducive to catalytic efficiency. The addition of La increases the number of oxygen vacancies, according to XRD, TEM, XPS, UV-DRS, and other data analyses. Because doping of La stretched the Fe–O bond, reduced the oxygen vacancies’ formation energy, and promoted oxygen vacancies’ formation, which was an essential reason for Fe 3+ reduction and Fe 3 O 4 formation. The addition of La also had a highly dispersed effect on Fe. Under the optimal conditions, with a FeLa mass ratio of 1:1, FeLa-Z/M at 25 mg, H 2 O 2 at 0.5 ml, and a pH of 3, the degradation rate of IC was found to be 97.8% and 99.5% in 5 min and 10 min respectively. Analysis of the reaction indicated that the catalyst followed a first-order reaction kinetic. Free radical quenching experiments confirmed that the main free radicals in the FeLa-Z/M Fenton-like system were hydroxyl radicals (·OH), suggesting a possible catalytic mechanism. Furthermore, the synthesized FeLa-Z/M catalyst exhibited superior performance compared to other methods of IC removal, demonstrating high reusability and efficient degradation even after multiple uses. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Chongming Wang,Sujie Shan,Zhengyu Yang,Xinpeng Xu,Xingning Huang,Xi Li,Songqi Liu,Boling Li,Yao Xu,Dapeng Li
Mounting evidence indicates that eliminating phosphate (P i ) alone is not enough to lower outbreak risks of undesirable algae, and synchronously sequestrating organic phosphorus species (OPs) dissolved in overlying water and residing in sediments cannot be ignored. However, more efforts were focused on the immobilization of P i than OPs because of insufficient understanding and analytical challenges. Herein, CaO 2 -loaded halloysite nanotubes/lanthanum-crosslinked sodium alginate (La-CaO 2 @HNTs/SA) hydrogel beads were newly developed and employed as a capping material for efficiently sequestrating P i and OPs from eutrophic water and sediment. Batch sorption results showed that the La-CaO 2 @HNTs/SA has a high uptake capacity towards P i (i.e., 44.05 mg-P/g) and Myo -inositol hexakisphosphate (IHP, a representative pollutant of OPs, 36.28 mg-P/g), and good selectivity for P in the presence of NO 3 – , Cl − , and HCO 3 – , profited by synergy of electrostatic attraction, inner-sphere complexation, surface precipitation, and partial degradation. After applying La-CaO 2 @HNTs/SA, P levels in overlying water could rapidly reduce from 0.95 to 0.01 mg-P/L within 120 min. Further thin-layer capping experiments (60 days) indicated that La-CaO 2 @HNTs/SA performed very well in immobilizing P i and OPs in overlying and pore waters and enhancing reductant-soluble P transformation (BD-P; ∼19 % to 11 %) to more stable HCl-extracted P (HCl-P; ∼33 % to 43 %) in sediments under continuous P input, with minor effect on benthic microorganisms. These findings advance the use of eco-friendly La-CaO 2 @HNTs/SA in eutrophication alleviation via simultaneous sequestration of P i and OPs.
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