INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Jinguo Hao,Senlin Deng,Junyang Liu,Lei Wang,Shasha Cao,Junping Zhang,Gang Wang,Chunshan Li
Modification of supported Cs-based catalysts has stimulated researchers’ interests, considering their effective catalytic performance in methyl methacrylate (MMA) production via one-step aldol condensation. Herein, we developed a series of Zr-incorporated SiO2-supported Cs (Cs/Zr-SiO2) catalysts using sol–gel in combination with solvothermal and impregnation methods. The structure and physicochemical properties were analyzed systematically by employing multiple characterization techniques, which guided the optimization of synthesis parameters such as Si/Zr molar ratio, prehydrolysis time, and Cs loading. The effects of catalyst structure, acid–base properties and their balance, and the chemical state of Cs and Zr species on the catalytic performance were systematically correlated. Results indicate that Zr was incorporated into the SiO2 framework with a four-coordinated configuration to form Si–O–Zr structures to act as Lewis acid sites, while the Cs component provides base sites through the formation of Cs–O–Si configurations. As a result, the methyl propionate (MP) conversion could reach up to 34.9% with MMA selectivity of 88.4%, representing 10–12% enhancement over the traditional impregnation method. In situ IR spectroscopic insights elucidated that the activation of formaldehyde and MP proceeded severally on the Si–O–Zr and Cs–O–Si sites, which seemed to be more efficient than those on an impregnation-prepared sample. Kinetic studies determined the activation energy of 115 kJ/mol, with reaction orders of 1.04 and 1.14 for MP and FA, respectively. In addition, the catalyst exhibited excellent regeneration and recycling behavior during the long-term stability test, and the initial activity of sample deactivated due to carbon deposition could be easily recovered after thermal treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Lingyu Yu,Long Ma,Na Zhu,Yu Ren
Rare-earth element-based materials have attracted extensive interest due to their effectiveness in phosphate removal. However, there are ongoing challenges related to enhancing the phosphate adsorption capacity and regenerating the lanthanum-based adsorbents. This study focused on the preparation of La-Zr bimetallic modified diatomite composites with different molar ratios using a simple coprecipitation method. These composites were employed as efficient adsorbents for the removal of low-concentration phosphate. After conducting a preliminary assessment of the phosphate adsorption capacities of the synthesized La-Zr bimetallic modified diatomite composites, the composite with the La/Zr molar ratio of 1:1 (designated as La 1 Zr 1 -DE) was selected for further characterization and evaluation. The maximum phosphate adsorption capacity of La 1 Zr 1 -DE, determined using the Langmuir isotherm model, was found to be 116.2 mg P/g. The adsorption process of phosphate by La 1 Zr 1 -DE can be primarily attributed to mechanisms such as ligand exchange, inner-sphere complexation, and surface precipitation. Furthermore, La 1 Zr 1 -DE exhibited excellent selectivity for phosphate and demonstrated good regeneration capabilities. This study offers a comprehensive exploration of the adsorption mechanisms, providing a theoretical basis for the development of more effective and sustainable phosphate adsorbents.
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高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Cheng Su,Bingzhu Wang,Huan Guo,Jixiang Dai,Jianjun Sha
In view of the high sintering temperature and difficulty in densification of the ultra-high temperature ceramics(UHTCs), a novel reactive hot-pressing process was designed to achieve the low temperature densification of high strength (Zr,Ta)B 2 -SiC ceramics. It was found that the mechanical properties were closely associated with the microstructure, being dependent on the sintering temperature. The microstructure characterization revealed that the main phases of ceramic were incompletely solid soluted borides and SiC at the sintering temperature of 1600 °C; while at 1700 °C, the boride ceramics were completely solid soluted (Zr,Ta)B 2 and formed an interlocking structure with SiC. The evaluation of mechanical properties indicated that the flexural strength of the ceramics increased from 470.2 MPa to 736.7 MPa when the sintering temperature increased from 1600 °C to 1800 °C. Correspondingly, the fracture toughness increased from 3.54 MPa·m 1/2 to 4.10 MPa·m 1/2 . The improvement of mechanical properties were mainly attributed to the interlocking structure formed by the solid solution (Zr,Ta)B 2 and SiC, which caused the crack propagation path becoming tortuous along the interface of different phases.
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高影响因子
AICHE JOURNAL
·
2025
·
IF 4
Jia Xiong,Qiang Sun,Hongxia Gao,Zhiwu Liang
Catalytic amine–based solution regeneration has attracted considerable attention due to its potential to reduce energy consumption in carbon dioxide (CO 2 ) separation. However, the limited catalytic activity and cycling stability of catalysts under high–temperature alkaline conditions hinder their industrial application. Herein, zirconium hydrogenphosphate (ZrHP) catalysts, featuring abundant acidic sites, were first utilized for amine solution regeneration. By leveraging its proton donation and acceptance mechanism, efficient monoethanolamine solution regeneration was achieved. The ZrHP–4 catalyst demonstrated a 526% increase in the instantaneous CO 2 desorption rate compared to the non–catalytic test, reducing the relative heat duty by 48%. Moreover, ZrHP–4 exhibited remarkable stability over 10 cycles without requiring regeneration. Density functional theory calculations revealed that ZrHP promotes CO 2 desorption by elongating the C—N bond of carbamate and lowering the proton transfer energy barrier. Therefore, this study offers novel insights into the design and mechanistic understanding of efficient and stable catalysts for amine solution regeneration.
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高影响因子
MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Fengyan Xie,Chunlei Huang,Guofa Dong,Minghui Wu,Kechen Wu,Shaowu Du,Yafeng Li,Mingdeng Wei
Perovskite solar cells (PSCs) fabricated of TiO 2 electron transporting material (ETM) have aroused tremendous attention, but their power conversion efficiency (PCE) needs further improvements. In this study, for the first time, zirconium (Zr)-doped brookite TiO 2 nanorods (ZTO) are synthesized by a facile route and subsequently employed as an ETM in PSCs which finally achieves a considerable PCE of 19.42 % by optimizing all operating conditions. Further characterizations have been undertaken to explore in detail the effects of Zr doping on the nature of the perovskite active layer and the photovoltaic performance. As a consequence, the enhanced PCE can be ascribed to the high quality perovskite crystals and a more favorable energy level alignment between the perovskite layer and ZTO mesoporous layer.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·Vol. 109
·期 1
·e70407
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IF 3.8
Yuwei Zhang,Cuiwei Li,Guangjin Chen,Chenran Zhao,Zhikun Song,Kepi Chen,Haoran Sun,Linghao Wu,Junhui Xiang
A series of (Y, Yb, Zr, Hf, Sn, W)O 2−δ high-entropy ceramics with varying mole fraction of main elements were synthesized for the first time through the solid-state reaction synthesis method. The microstructure, phase composition, and properties of the prepared materials were thoroughly analyzed and tested. The results indicate that the phase composition transformed from a single-phase fluorite structure to a single-phase C-type rare earth sesquioxide structure as the mole fraction of +3 cations increases. The thermal conductivity of the prepared high-entropy ceramics with porosity of 49.8%–50.1% is very low ranging from 0.33 to 0.37 W·m −1 ·K −1 . Among them, the single-phase C-type rare earth sesquioxide with a higher oxygen vacancy concentration was employed as a catalyst in the CO 2 hydrogenation reaction, attaining a high CO 2 conversion rate of 82.0%. The obtained results have deepened understanding of the role of oxygen vacancies and have important guiding significance for the study of high-entropy oxides with fluorite derived structures.
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International Journal of Minerals Metallurgy and Materials
·
2025
·Vol. 32
·期 6
·1441-1450
·
IF 7.2
Chen Xunlei,Chen Lin,Tian Jiang,Xu Cheng,Liao Jiaxin,Li Tianyu,Wang Jiankun,Feng Jing
Thermal and mechanical properties of yttrium tantalate (YTaO 4 ), a top coat ceramic of thermal barrier coatings (TBCs) for aeroengines, are enhanced by synthesizing Y 1− x Ta 1− x M 2 x O 4 (M = Ti, Zr, Hf; x = 0.06, 0.12, 0.18, 0.24) medium-entropy ceramics (MECs) using a two-step sintering method. In addition, the thermal conductivity, thermal expansion coefficients (TECs), and fracture toughness of MECs were investigated. An X-ray diffraction study revealed that the Y 1− x Ta 1− x M 2 x O 4 MECs were monoclinic, and the Ti, Zr, and Hf doping elements replaced Y and Ta. The variations in atomic weights and ionic radii led to disturbed atomic arrangements and severe lattice distortions, resulting in improving the phonon scattering and reduced thermal conductivity, with Y 1− x Ta 1− x M 2 x O 4 MECs ( x = 0.24) exhibiting the lowest thermal conductivity of 1.23 W·m −1 ·K −1 at 900°C. The introduction of MO 2 increased the configurational entropy and weakened the ionic bonding energy, obtaining high TECs (10.4 × 10 −6 K −1 at 1400°C). The reduction in the monoclinic angle β lowered the ferroelastic domain inversion energy barrier. Moreover, microcracks and crack extension toughening endowed Y 1− x Ta 1− x M 2 x O 4 MECs ( x = 0.24) with the highest fracture toughness of (4.1 ± 0.5) MPa·m 1/2 . The simultaneous improvement of the thermal and mechanical properties of the MO 2 (M = Ti, Zr, Hf) co-doped YTaO 4 MECs can be extended to other materials.
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CERAMICS INTERNATIONAL
·
2025
·Vol. 51
·期 22
·36739-36745
·
IF 5.6
Peilin Qing,Ning Guan,Yang Yang,Huizi Qiu,Weishuang Fang,Huaicheng Xiang,Ying Tang,Jie Li,Liang Fang
Crystal structure refinement and Raman spectroscopy were performed on Ca 3 M 2 Ga 2 GeO 12 (M = Ti, Sn, Zr) garnet-structured ceramics to explore the relationships between crystal structure, phonon modes, and microwave dielectric properties . The Ca 3 Ti 2 Ga 2 GeO 12 , Ca 3 Sn 2 Ga 2 GeO 12 , and Ca 3 Zr 2 Ga 2 GeO 12 ceramics were obtained by sintering at 1325–1475 °C for 6 h, and good microwave dielectric properties were achieved: ε r = 15.04, 9.53, and 11.89; Q × f = 59,515 GHz, 49,355 GHz, and 45,587 GHz; and τ f = −47.3 ppm/°C, −52.3 ppm/°C, and −43.0 ppm/°C, respectively. M 4+ (M = Ti, Sn, Zr) cations entirely occupied the octahedral site, leading to an average underbonding between cations and anions, a weak rattling effect, and measured ε r values deviating from theoretical values. The packing fraction and Raman FWHM (A 1g mode) correlated highly with the Q × f values. The negative τ f values were derived from the large positive temperature coefficient of permittivity ( τ ε ) and the temperature coefficient of ionic polarizability ( τ αm ).
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Huanjing Chen,Wanqiao Bai,Hongmei Chai,Loujun Gao
To achieve the rapid and sensitive detection of trace methyl parathion (MP) in river water and edible agricultural products, the catalytic composite material zirconium hydroxide (Zr(OH)4)/zeolite imidazolate framework-90 (ZIF-90) was prepared by a one-step synthesis method. The composite was further incorporated with a conductive poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) hydrogel to prepare a modified electrode. Then, an electrochemical sensing method based on the PEDOT:PSS/Zr(OH)4/ZIF-90 composite was successfully established for the analysis and detection of MP. The component ratio of the composite material, modification amount and pH value of the detection substrate were optimized. The electrochemical properties of the composite modified electrode were evaluated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV) techniques, and the results confirmed that it had good electrochemical properties. The electrochemical response of the established sensing method to MP showed a good linear relationship in the concentration range of 1–250 µmol L−1, and its detection limit and sensitivity reached 0.74 µmol L−1 and 0.09 µA µmol−1 L−1, respectively. The interference of common coexisting ions on the detection performance of the PEDOT:PSS/Zr(OH)4/ZIF-90 modified electrode was further investigated, and it was applied for the quantitative analysis of MP in actual river water and apple samples. The electrochemical sensing method developed in this work provides a new way for the efficient detection of MP residues in environmental water and agricultural products.
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Materials Today Chemistry
·
2025
·
IF 6.7
Liang Chu,Teng Zhao,Zhaokun Wang,Xinyu Zhao,Zhiyong Zhu,Mu Yang,Ge Wang
The development of efficient oxidative desulfurization (ODS) catalysts is of great importance for clean energy. In this study, we report a method for the preparation of defect-enriched UiO-66(Zr) materials via a high-energy ball-milling pretreatment-assisted followed by rapid ethanol crystallization. This method significantly enhances ligand deficiency (46.1 %) and average pore diameter (4.1 nm) without using toxic solvents or pre-synthesized clusters, distinguishing it from conventional solvothermal and one-step mechanochemical approaches. Under the optimal parameters, the resulting UiO-66-BM catalyst exhibits excellent ODS performance, achieving full conversion of dibenzothiophene (DBT, 1000 ppm) within 6 min at 50 °C and 20 min at 30 °C using only 20 mg of catalyst and an O/S molar ratio of 5. The turnover frequency (19.85 h −1 ) and mass specific activity (53 mmol g −1 h −1 ) surpass those of most reported pristine MOFs-based catalysts. Moreover, the catalyst reaction activity maintains high activity over six consecutive cycles, showing excellent stability. The superior performance is attributed to the synergistic effect of ball milling and ethanol crystallization, which generates the enriched structural defects and enlarged mesopores, facilitating mass transfer and active site accessibility. This work presents an effective and eco-friendly strategy for the scalable synthesis of high-performance MOF catalysts for deep desulfurization.
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Small
·
2020
·Vol. 16
·期 7
·1906240
·
IF 11.459
Mian Chen,Zhou Long,Ruihua Dong,Le Wang,Jiangjiang Zhang,Sixiang Li,Xiaohui Zhao,Xiandeng Hou,Huawu Shao,Xingyu Jiang
This study uses metal–organic frameworks (MOFs) alone without any added antibacterial ingredients as the nonantibiotic agent for photodynamic therapy (PDT) of chronic wounds infected by multidrug-resistant (MDR) bacteria. Nanoparticles (NPs) of MOFs (PCN-224) are incorporated with titanium through a facile cation exchange strategy. The obtained bimetallic PCN-224(Zr/Ti) shows greatly enhanced photocatalytic performance for the generation of reactive oxygen species under visible light, which is responsible for the effective antibacterial activities. The PCN-224(Zr/Ti) NPs are loaded onto lactic- co -glycolic acid nanofibers to prepare a wound dressing, which shows high biocompatibility and minimal cytotoxicity. The wound dressing is efficient for PDT-based in vivo healing of the chronic wound infected by MDR bacteria. Most importantly, this work does not involve any additional antibacterial agents, which is facile, low cost, and in particular, greatly explores the potential of MOFs as a powerful nonantibiotic agent in PDT.
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PubMed
高影响因子
ELECTROPHORESIS
·
2022
·Vol. 43
·期 11
·1161-1173
·
IF 3.595
Lidi Gao,Xingfang Hu,Shili Qin,Hongtao Chu,Yimin Tang,Xue Li,Binbin Wang
A novel chiral stationary phase (CSP) of Zr-based metal-organic framework, l -Cys-PCN-224, was prepared by one-pot method and applied for the enantioseparation by capillary electrochromatography. The CSP was characterized by X-ray diffraction, thermogravimetric analysis, X-ray photoelectron spectroscopy, Fourier-transform infrared spectra, nitrogen adsorption/desorption, circular dichroism spectrum, zeta-potential, and so on. The results revealed that the CSP had good crystallinity, high specific surface area (2580 m 2 /g), and good thermal stability. Meanwhile, the cross-section of l -Cys-PCN-224-bonded open-tubular (OT) column was observed by a scanning electron microscope, which proved the successful bonding of l -Cys-PCN-224 particles to the inner wall. Relative standard deviations of the column efficiencies were 3.87%–9.14%, and not obviously changed after 200 runs, which indicated that l -Cys-PCN-224-bonded OT column had the better stability and reproducibility. Excellent chiral separation performance was verified with nine kinds of natural amino acids including acidic, neutral, and basic as the analytes. All amino acids studied achieved good separation with the resolution of 1.38–13.9 and selector factor of 1.11–3.71. These results demonstrated that the CSP had an excellent potential in the chiral separation field.
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