Molecular Catalysis
·
2018
·
IF 0
Ke Li,Ke Liu,Hong Ni,Bin Guan,Reggie Zhan,Zhen Huang,He Lin
A novel catalytic system combining oxidation catalyst with electric field was applied for low-temperature CH 4 oxidation at low CH 4 concentration (0.2% CH 4 ). Compared with conventional catalytic process, significant improvement in activity was observed over PdCeZrO x catalyst in electric field. For example, the light-off temperature (T 50 ) of CH 4 (0.2% CH 4 ) of 1 wt % PdCe 0.75 Zr 0.25 O x catalyst was approximately 255 °C in an electric field with 3 mA electric current. The impact of electric field in CH 4 oxidation over PdCeZrO x catalyst was thoroughly investigated. The XRD and XPS results revealed that electric field provided free electrons that facilitated the release of lattice oxygen in the ceria-zirconia solid solution, therefore reinforced Pd0 oxidation and the formation of palladium oxide (PdO x , x > 0) on catalyst surface. Electric field also enhanced the reducibility of the PdO x , which provided active oxygen for CH 4 oxidation at low temperature. With in-situ FTIR technique, it was found that electric field greatly promotes the chemisorption and dehydrogenation of CH 4 , thereby accelerates the chemical reactions of the intermediate products, so as to promotes CH 4 oxidation. The mechanism of catalytic oxidation of CH 4 in electric field was proposed based on comprehensive investigations above.
研究领域:
催化化学
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环境科学
·
材料化学
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能源化学
·
表面科学
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DOI
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Fengnian Zhang,Fuhao Cheng,Chufei Cheng,Meng Guo,Yufeng Liu,Yang Miao,Feng Gao,Xiaomin Wang
Abatract A series of compositionally complex fluorite oxides (CCFOs) were prepared by ball milling the mixture of ZrO 2 , HfO 2 , Y 2 O 3 , La 2 O 3 , and Pr 6 O 11 followed by conventional solid-state sintering. Both XRD and TG-DSC results demonstrated that single-phase (Zr 0.2 Hf 0.2 Pr 0.2 Y 0.2 La 0.2 )O 2-δ was formed at 1400 °C. Elements in bulk ceramic were uniformly distributed without evident accumulation according to SEM-EDS pictures. TEM results revealed that polycrystalline ceramic powder was assignable to cubic Fm-3m fluorite structure. The electrical conductivity ( σ ) was measured via EIS technology and activation energy ( E a ) of CCFOs was calculated in Arrhenius plots. In the temperature range of 300-750 °C, CCFOs preserved the same conduction mechanism and (Zr 0.1667 Hf 0.1667 Pr 0.1667 Y 0.25 La 0.25 )O 2-δ possessed higher σ and lower E a than other high entropy fluorite oxides which is related to the incorporation of Pr element or the connection of cation-V o complex.
研究领域:
材料科学
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无机非金属材料
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固体离子学
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功能陶瓷
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能源材料
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DOI
高影响因子
MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2020
·
IF 4.652
Yingnan Shi,Zheng Lu,Li Yu,Rui Xie,Yuhang Ren,Guang Yang
Oxide dispersion strengthened (ODS) FeCrAl alloys have been considered as the promising candidate fuel cladding materials for the Gen-IV fission reactors due to excellent radiation tolerance, mechanical properties and corrosion resistance , but their manufacturing is complex process. Laser engineered net shaped (LENS) technology followed by post-build heat treatment was employed successfully to fabricate Zr-containing ODS-FeCrAl alloy. The microstructure of as-deposited and heat-treated alloys was characterized by optical microscope (OM), electron backscatter diffraction (EBSD), scanning electron microscope (SEM) and high-resolution transmission electron microscope (HRTEM). The tensile tests were carried out at room temperature. The results show that the coarse columnar grains with preferred orientation ([001] fibre texture) are obtained after LENS deposit and are remained after post-build heat treatment. The average width of columnar grains for both as-deposited and heat-treated samples is ~180–190 μm. A slag-like layer which is made up of Y 3 Al 5 O 12 , ZrO 2 and Al 2 O 3 is observed at the surface of deposited sample. Some coarse appendage oxides which consist of Al 2 O 3 and Y 4 Zr 3 O 12 are distributed in the matrix of as-deposited sample. Post-build heat treatment produces high-density nanoscale Y 4 Zr 3 O 12 oxides in the matrix. The formation mechanism of different type oxides is explained. Both as-deposited and heat-treated samples present anisotropic tensile properties . After post-build heat treatment, the tensile strength is improved significantly by the formation of high-density nanoscale Y 4 Zr 3 O 12 .
研究领域:
材料科学
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增材制造
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核材料
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金相学
·
力学性能
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DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2023
·Vol. 106
·期 7
·4382-4389
·
IF 3.9
Yongqiang Tan,Wei Liao,Zhen Teng,Haibin Zhang
Two high-entropy carbides, including stoichiometric (Zr,Ti,Nb,Ta,Hf)C and nonstoichiometric (Zr,Ti,Nb,Ta,Hf)C 0.8 , were prepared from monocarbides and ZrH 2 . Their sinterability, microstructures, mechanical properties, thermophysical properties, and oxidation behaviors were systematically compared. With the introduction of carbon vacancy, the sintering temperature was lowered up to 300°C, Vickers hardness was almost unaffected, whereas the strength decreased significantly generally due to the decrease of covalent bonds. The thermal conductivity shows a 50% decrease for nonstoichiometry high-entropy carbide, which is a major consequence of the lower electrical conductivity. The oxidation resistance in high temperature water vapor was not sensitive to carbon stoichiometry.
研究领域:
材料科学
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机械工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 32
·15405-15413
·
IF 3.925
Yuzhu Zhai,Yijing Li,Qin Hou,Yuanhong Zhang,Enlong Zhou,Houshen Li,Shiyun Ai
A phosphate ion (Pi) is usually considered as an important index of eutrophication in water and can cause great harm to the water ecological environment. In this work, MOF-808(Zr/Ce) was synthesized simply for phosphate detection and removal. MOF-808(Zr/Ce) with oxidase-like activity can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB). The colorimetric sensing of phosphate was performed based on the enhancement of the oxidase-like activity of MOF-808(Zr/Ce). The linear detection range for phosphate detection was 11–581 μM, and the detection limit (LOD) was 3.7 μM. The MOF-808(Zr/Ce)/CNF (cellulose nanofibers) flexible film synthesized by the filtration method also enables the rapid identification of phosphate. Besides, the phosphate adsorption performance of MOF-808(Zr/Ce) was also investigated. The adsorption capacities are 54.9, 65.1, and 68.5 mg g−1 at 298, 308, and 318 K, respectively. The results show that MOF-808(Zr/Ce) has great potential for phosphate detection and removal.
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xiaoya Zhao,Jilin Zhang,Zi Dai,Yunyun Lei,Xiaoxun Liu,Guixia Liu
Excess fluoride in drinking water from groundwater can cause dental and skeletal fluorosis affecting millions of people worldwide. Adsorption is an appealing strategy for defluoridation due to its simple operation and environmental friendliness. However, conventional adsorbents exhibit low adsorption capacity because few exposed active sites. In this work, La anchored Zr-based metal-organic framework (La-UiO-66-(COOH) 2 ) adsorbent with dual-metal sites was designed and synthesized to remove fluoride effectively. The doping of La(III) using uncoordinated carboxyl group of UiO-66-(COOH) 2 increased the adsorption capacity. The morphology, composition, structure, surface area, and thermal stability of adsorbent were carefully characterized by powder X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectrometer (EDX), fourier transform infrared (FT-IR), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS) techniques. The adsorbent is a polyhedral shape with aggregated and smaller crystalline particles and La is uniformly distributed over the adsorbent, favoring the effective adsorption of fluoride. La-UiO-66-(COOH) 2 showed excellent adsorption performance in a wide pH range of 3–9, and the maximum adsorption capacity was 57.23 mg g −1 . The fluoride removal rate of as-prepared adsorbent reached as high as 87 % within 5 min. The adsorption process conformed to the pseudo-second-order equation model and the Freundlich isotherm model. Thermodynamic research indicated that the adsorption process was spontaneous and endothermic. After four adsorption-desorption cycles, the fluoride removal rate of the adsorbent was still retained at 79.7%. The design of dual-metal site adsorbents provides a potential strategy for highly efficient removal of fluoride.
研究领域:
环境科学
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材料科学
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水处理
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124617
·
IF 7.5
Jinyun Lyu,Yanqian Liu,Chanjuan Liu,Xiaohua Huang
Mixed matrix membranes (MMMs) combine the flexibility of polymer membranes and the excellent gas separation performance of porous materials, and have attracted extensive attention in the field of gas separation in recent years. In this work, a novel fluorinated non-coplanar diamine monomer 2,2-bis(4-(4-amino-2-methoxyphenoxy)phenyl)hexafluoropropane (AMPH) was synthesized through molecular design. Fluorinated non-coplanar copolyimide (AFPI) was fabricated by copolymerizing AMPH with 4,4′-(hexafluoroisopropylidene)diphthalic anhydride (6FDA) and 9,9-bis(4-amino-3-fluorophenyl)fluorene (FFDA). Subsequently, Zr-BTB, a zirconium-based metal-organic framework with high CO 2 affinity and structural stability, was incorporated into the AFPI matrix to fabricate AFPI/Zr-BTB MMMs with different mass loadings. Benefiting from the introduced fluorine groups, AFPI possesses enlarged free volume to accelerate gas permeation. Meanwhile, two-dimensional Zr-BTB facilitates selective CO 2 adsorption over N 2 through thermodynamic adsorption affinity for improved separation performance. Compared with the pristine membrane, the CO 2 and O 2 permeabilities of MMMs increase by 277% and 237% at 15 wt% Zr-BTB loading, and the ideal CO 2 /N 2 and O 2 /N 2 selectivities rise by 45% and 33% at 5 wt% loading. This confirms that embedding Zr-BTB into copolyimide to fabricate MMMs is a promising strategy for developing high-performance gas separation membranes.
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Zemin Li,Hui Wang,Yawen Bo,Yanjun Wang,Sheng Liu,Jingxian Hua,Yawei Gu,Qihan Gong,Yichang Pan,Rujing Hou
The separation of hexane isomers from light naphtha is critical to advancing energy-efficient refining and supporting environmental sustainability. However, this application requires membranes capable of precise molecular discrimination. In this work, we focus on hard acid–hard base coordinated Al-/Zr-MOFs due to their exceptional stability and tunable pore environments. Through combined thermodynamic and kinetic evaluations, four Al-MOFs (KMF-1, CAU-23, MIL-160, Al-bttotb) and Zr-MOF(UiO-66) emerged as promising candidates. UiO-66 was ultimately identified as the optimal platform due to its excellent membrane compactness and techno-economic potential. We subsequently employed a mixed-linker strategy to achieve Ångstrom-level pore size engineering in UiO-66, the resulting UiO-66-NH 2 membrane exhibited superior discrimination between linear/mono-branched (n-hexane, 3-methylpentane) and di-branched (2,2-dimethylbutane) isomers, achieving an ideal selectivity of 4.8—a performance that exceeds most current state-of-the-art MOF membranes. Pervaporation experiments with a simulated C 5 –C 6 naphtha mixture further confirmed the ability of the membrane to efficiently enrich ethylene cracking precursors, while the retentate effectively concentrated high-octane gasoline additives. These results underscore the strong industrial potential of Ångstrom-precision engineered MOF membranes for simultaneous production of high-value chemical feedstocks and premium fuel components from light naphtha.
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产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2026
·
IF 8.3
Fan Feng,Haicheng Gao,Yuan Xue,Qing Dong,Junfeng Zhai,Dan Li,Erkang Wang,Jin Wang
Exosomes, as extracellular vesicles, represent ideal biomarkers for liquid biopsy, enabling non-invasive, sensitive, and dynamic disease monitoring. Detection or profiling of exosomes are essential for advancing exosome-based cancer diagnostics or prognostic prediction. Here, we developed an enhanced electrochemiluminescence (ECL) biosensing platform that combines magnetic enrichment with catalytic hairpin assembly (CHA), an enzyme-free DNA amplification circuit triggered by the complementary sequences of CD63 aptamer (Apt), to achieve sensitive exosome detection. The enhanced ECL signal relies on a nanocomposite of a zirconium-based metal-organic framework (Zr-MOF) and water soluble gold nanoclusters (AuNCs), denoted as Zr-MOF/AuNCs. The platform exhibits a wide linear range (6.12 × 10² - 6.12 × 10⁷ particles/mL) and a low detection limit (187.4 particles/mL) for tumor-derived exosomes. Spike-recovery assays in complex serum matrices and high specificity confirm its robustness and clinical potential. By combining magnetic preconcentration, signal amplification via Zr-MOF and CHA, and Apt-mediated recognition, this work establishes a new paradigm for non-invasive cancer diagnostics.
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产品关联
DOI
高影响因子
ChemistrySelect
·
2026
·Vol. 11
·期 31
·e74143
·
IF 2.3
Yan Gao,Fuyuan Han,Yuxin Ma,Chenxi Bai,Junyu Xia,Kaiyue Shen,Wenlin Xu,Xue Ye,Jie Li
Zinc-based heterogeneous catalysts for the synthesis of dimethyl carbonate (DMC) suffer from unstable active sites and rapid deactivation during recycling. To address this issue, a series of zirconium-doped zinc oxide microspheres (ZnO@x%ZrO 2 ) were prepared. Among them, the optimal sample ZnO@5%ZrO 2 achieved a propylene carbonate (PC) conversion of 58.20%, a DMC selectivity of 89.90%, and a yield of 52.30%. Moreover, after five cycles, the selectivity of this catalyst decreased by only 4.10%, whereas undoped ZnO experienced a 15.70% drop in selectivity after just one use. Various characterization techniques (SEM, XRD, XPS, NH 3 -TPD, CO 2 -TPD, H 2 -TPR) revealed that high-valent Zr 4+ ions substituted Zn 2+ in the ZnO lattice, inducing a large number of oxygen vacancies to maintain charge balance and generating the required acid-base sites for the reaction. By tuning the zirconium loading, the electronic structure, vacancy concentration, and acid-base synergistic effects could be optimized, primarily dominated by moderate-strength basic sites complemented by acidic sites. This cooperative effect reduces the activation energy of the ester exchange reaction, significantly enhancing catalytic activity and excellent cycling stability. Graphical A Zr-doped ZnO microsphere catalyst was developed, in which Zr 4+ replaced Zn 2+ , resulting in a defect structure with abundant oxygen vacancies and the formation of a solid solution structure, which significantly enhanced the activity and stability of ZnO.
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Huashuai Hu,Zhihang Xu,Xiyang Wang,Chi Zhang,Molly Meng-Jung Li,Ye Zhu,Jiacheng Wang,Dingsheng Wang,Ling Liu,Kuo Liu,Minghui Yang
Asymmetric Zr single-atom sites with axial S atom are constructed. • Efficient oxygen reduction reaches 0.913 V with 110 h stability. • Electronic structure is tuned to optimize intermediate adsorption. • Breaking the scaling relationship enables improved ORR kinetics. Asymmetry engineering in single-atom catalysts (SACs) has emerged as a powerful approach to modulate electrocatalytic performance. However, Zr-based SACs have been rarely investigated for the oxygen reduction reaction (ORR) due to limited synthetic precedents and unclear coordination-activity relationships. Here, we report a novel A -S-Zr-N 2 O 2 @NC catalyst in which axial sulfur incorporation creates an asymmetric Zr-N/O/S coordination environment, inducing electronic redistribution and generating highly active catalytic sites. The catalyst exhibits a half-wave potential (E 1/2 ) of 0.913 V, surpassing commercial Pt/C and most state-of-the-art non-noble-metal nanomaterials, while maintaining excellent Zn-air battery (ZAB) durability over 28 days and high methanol tolerance. Mechanistic studies confirm that S atom enhances *OOH adsorption on Zr sites, breaks the scaling relationship, and lowers the O-O bond cleavage barrier, enabling an efficient four-electron reaction pathway. Our findings highlight the immense potential of the Zr-based SACs platform for electrocatalysis, elucidate the mechanistic role of asymmetric ligand engineering, and provide a rational design framework for high-performance catalytic materials. Download: Download high-res image (166KB) Download: Download full-size image
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DOI
高影响因子
Molecular Catalysis
·
2026
·
IF 4.3
Kang Cheng,Yuting Hu,Tianyu Liu,Ting Cheng,Taotao Liu,Chengzhu Zhu
MOF derivative (Zr (0.9)/CuO x (400)) had excellent denitrification activity, N 2 selectivity and stability. • Systematically revealed the regulation mechanism of Zr doping on the Cu 2+ /Cu + ratio and acid balance. • Proved that Zr doping could act as sacrificial sites to greatly improve the H 2 O and SO 2 resistance of the catalyst. Zr/CuO x composite were synthesized by hot-solvent and calcination method using metal-organic framework (MOF) as the precursor, and were applied for selective catalytic reduction of NO x with NH 3 (NH 3 -SCR). The effects of Zr/Cu molar ratio, calcination temperature and time on catalyst activity and the physicochemical properties of the composites were systematically investigated. The results showed that Zr/CuO x composite revealed a favorable denitrification activity, stability and resistance to sulfur and water while Zr/Cu molar ratio was 0.9 and calcination temperature was 400 °C. When the NO concentration of 500 ppm and gas hourly space velocity (GHSV) of 35,000 h -1 , NO conversion efficiency was achieved 100% and over 94% N 2 selectivity at 275–375 °C. In the presence of 100 ppm SO 2 and 10 vol% H 2 O, the NO conversion of Zr (0.9)/CuO x (400) approached 92%. The enhanced activity was attributed to a synergistic Zr/Cu interaction that optimized the surface Cu 2+ /Cu + redox couple, enriched Cu + sites, and thereby accelerated the low-temperature “fast” SCR pathway. Moreover, doping Zr generated a larger number of well-dispersed acid sites and maintained strong reducibility across a broad temperature range, collectively providing favorable conditions for the NH 3 -SCR. Download: Download high-res image (230KB) Download: Download full-size image
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DOI
高影响因子
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