CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Chenxi Feng,Junyang Liu,Kai Zhao,Lei Wang,Zengxi Li,Guoliang Zhang,Chunshan Li
Methyl methacrylate (MMA) synthesis via aldol condensation of methyl propionate with formaldehyde over Cs-based supported catalysts is intensively investigated, while the effect of their pore structures on catalytic performance still lacks in-depth understanding. Herein, series of Cs-Zr/SiO 2 catalysts with different pore structures were prepared for this aldol condensation. The physicochemical characteristics of as-prepared Cs-Zr/SiO 2 catalysts were characterized using physical N 2 adsorption–desorption isotherms and CO 2 -/NH 3 -TPD. In addition, the impact of pore structure on mass transfer, adsorption, and desorption of reactants and products was studied through in situ DRIFTS. The results show that the acid and base site densities elevated with the increasing pore volume. The mass transfer of reactants and products could be promoted with increasing pore size, while their adsorption energies exhibited a volcanic trend. As a result, the Cs-Zr/SiO 2 catalysts having average pore diameter of 12-18 nm and acid-base balance was considered as the optimal candidate for MMA production.
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高影响因子
MICROCHIMICA ACTA
·
2024
·Vol. 192
·期 1
·1-11
·
IF 5.3
Tian Siyu,Wang Jiahui,Jie Yu,Ding Zhu,Wang Xiao,Wang Jijiang,Hou Xiangyang
A novel nanobiosensor was constructed by in situ locating nanometer MnO 2 particles with controllable size and morphology in a Zr-MOF substrate to serve as an electrochemical probe. The synergistic effect of the two components, Zr-MOFs with high specific surface area and compatibility as a carrier for MnO 2 , resulted in improved electrochemical activity and excellent electrochemical identification performance for the MnO 2 @Zr-MOF/GCE biosensor. Under optimized experimental conditions and using CV and DPV technology, the biosensor showed a wide linear detection range (2–200 μM), a low detection limit (2.577 × 10 −8 M), a recovery range (106.26–115.01%), and maximum relative standard deviation (5.155) for tetracycline (TC) identification. The recognition mechanism of the sensor was investigated adopting Laviron adsorption theory. The applicability of the sensor was verified through practical measurements. Overall, the MnO 2 @Zr-MOF/GCE sensor possesses the advantages of fast analysis speed, high sensitivity, high selectivity, and simple operation, making it suitable for detecting trace amounts of TC in food. Graphical abstract
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高影响因子
LANGMUIR
·
2024
·
IF 3.7
Mian Gong,Yihui Dong,Minghai Zhu,Fengxiang Qin,Tianchi Wang,Faiz Ullah Shah,Rong An
Surface-enhanced Raman scattering (SERS) is a remarkably powerful analytical technique enabling trace-level detection of biological molecules. The interaction of a probe molecule with the SERS substrate shows important distinctions in the SERS spectra, providing inherent fingerprint information on the probe molecule. Herein, nonhalogenated phosphonium-based ionic liquids (ILs) containing cations with varying chain lengths were used as trace additives to amplify the interaction between the cytochrome c (Cyt c) and Zr–Al–Co–O (ZACO) nanotube arrays, strengthening the SERS signals. An increased enhancement factor (EF) by 2.5–41.2 times compared with the system without ILs was achieved. The improvement of the SERS sensitivity with the introduction of these ILs is strongly dependent on the cation chain length, in which the increasing magnitude of EF is more pronounced in the system with a longer alkyl chain length on the cation. Comparing the interaction forces measured by Cyt c-grafted atomic force microscopy (AFM) probes on ZACO substrates with those predicted by the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory, the van der Waals forces became increasingly dominant as the chain length of the cations increased, associated with stronger Cyt c–ZACO XDLVO interaction forces. The major contributing component, van der Waals force, stems from the longer cation chains of the IL, which act as a bridge to connect Cyt c and the ZACO substrate, promoting the anchoring of the Cyt c molecules onto the substrate, thereby benefiting SERS enhancement.
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FUEL
·
2025
·
IF 7.5
Yake Wu,Suning Li,Jiawen Zhang,Shuai Li,Tao Zhong,Yanlong Zhu,Hong Li,Liuting Zhang
By constructing Ni-O-Zr interfaces, oxygen vacancies were generated and the interaction between the metal and the support in the catalyst was significantly enhanced. This synergy between Ni 0 and oxygen vacancies greatly boosted the catalytic activity of Ni 50 /ZrO 2 in the hydrogen storage system. Experimental tests showed that the MgH 2 + 10 wt%Ni 50 /ZrO 2 composite had a reduced initial hydrogen desorption temperature of 194.5 °C and released 6.30 wt%H 2 within 10 min at 265 °C. Notably, this composite exhibited excellent low-temperature hydrogen absorption kinetics, initiating absorption at 29 °C and nearly completing it (6.67 wt%H 2 ) at 134 °C. Furthermore, the activation energy for the modified MgH 2 had been substantially decreased from 76.66 kJ/mol to 32.01 kJ/mol (absorption) and 155.84 kJ/mol to 83.93 kJ/mol (desorption), respectively. The presence of oxygen vacancies at the Ni-O-Zr interface significantly amplified the catalyst’s charge conduction capabilities and provided a promising avenue for the development of effective catalysis for robust hydrogen storage.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Wenrong Cai,Yanjing Shi,Datong Wu,Junyao Li,Laidi Xu,Yong Kong
This work proposes a novel dual-signal electrochemiluminescence ( ECL) immunosensor based on energy resonance transfer (RET) for the detection of β2-Microglobulin (β2-MG). Introducing carbon vacancy into g-C 3 N 4 (V C -g-C 3 N 4 ) can lead to the narrowing of the band gap and the reduction of LUMO, thereby significantly enhancing the ECL efficiency of the material. Meanwhile, Zr-MOF can effectively load Ru(bpy) 3 2+ (Ru-Zr-MOF), enabling its stable existence on the electrode. The ECL emission spectrum of V C -g-C 3 N 4 overlaps well with the fluorescence excitation spectrum of Ru-Zr-MOF, indicating an effective ECL-RET effect between them. As the concentration of β2-MG increases, the intensity of anodic ECL signal gradually increases, while the intensity of cathodic ECL signal gradually decreases. The difference between the cathodic and anodic ECL signals has a good linear relationship within the concentration range from 0.2 pg/mL to 200 ng/mL, with a detection limit of 27.73 fg/mL. The constructed immunosensor can be used for practical analysis in human serum. The proposed sensor has great potential in clinical detection of β2-MG, providing new insights for biomolecular detection and disease diagnosis.
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Sensors and Actuators Reports
·
2024
·
IF 6.5
Zhiming Chen,Zhiwen Shi,Peng Zhang,Li Gao,Bingxin Liu,Lijuan Qiao
The presence of ammonia in exhaled human breath serves as a crucial biomarker for renal diseases. This paper presents a highly sensitive ammonia sensor operable at room temperature, utilizing a Ti/Zr dual metal MOF as its core component, synthesized through a straightforward solvothermal reaction approach. The Ti/Zr-MOF demonstrates excellent responsiveness to ammonia gas, with a detection limit of remarkable sensitivity, reaching as low as 2 ppm. Notably, the sensor exhibits practical insensitivity to similar concentrations of other major interfering breath volatiles, including acetone, ethanol, and saturated moisture. Electron Paramagnetic Resonance (EPR) analysis confirms the presence of oxygen vacancies (Ov) in Ti/Zr-MOF materials, with Ti/Zr-MOF exhibiting stronger Ov signals and the potential for enhanced NH3 adsorption and capture. In-situ FTIR spectrum analysis reveals ammonia-induced -OH (H 2 O) moiety formation, indicating a reaction between adsorbed O 2 − species and ammonia, resulting in decreased electrical resistance of Ti/Zr-MOF.
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JOURNAL OF SEPARATION SCIENCE
·
2025
·Vol. 48
·期 7
·e70221
·
IF 2.8
Suling Zhang,Hengli Liu,Xiaoyang Li,Weixuan Yao,Jianbo Ying,Ting Lü,Dong Zhang,Hongting Zhao,Ying Pan
A facile dispersive micro-solid phase extraction (D-μ-SPE) method that uses spherical cellulose aerogels is proposed herein for the trace detection of seven benzodiazepines in biological samples. Zirconium metal–organic framework (MOF) particles were dispersed in the cellulose aerogels to improve the extraction efficiency. The prepared lightweight spherical aerogels (diameter of approximately 2 mm) were easily collected from the solution using a disposable dropper, overcoming the difficult recycling of powdered MOFs. The effect of the MOF loading (39, 56, and 66 wt%) and the organic ligand (terephthalic acid, 2-aminoterephthalic acid, and 4,4′-biphenyldicarboxylic acid) in the Zr-MOF on the extraction ability of the hybrid aerogels towards benzodiazepines was studied. The hybrid aerogel with a UiO-67 loading of 66% showed the best extraction performance primarily because of the enhanced surface area, pore volume, and π–π stacking interactions. Moreover, the UiO-67/cellulose aerogel spheres were mechanically stable and showed reusability for at least eight consecutive extraction cycles. The main factors affecting extraction, such as solution pH, extraction time, type and volume of desorption solvent, and desorption time, were also examined. Under the optimal conditions, the limits of detection ranged from 0.01 to 0.03 µg/L, and the limits of quantification ranged from 0.02 to 0.10 µg/L. The recoveries were 81.8%–104.2% for urine samples and 81.5%–99.5% for hair samples. The results suggest that the spherical aerogel-based D-μ-SPE is a simple and effective method for the quantification of benzodiazepines in biological samples.
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高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Jianzhong Ma,Tongtong Ma,Qianqian Fan,Yiming Shen,Mi Liu,Wenbo Zhang
The development of green chromium-free tanning agents continues to be actively researched as a prominent topic in the leather industry. Zirconium tanning agents have good tanning performance, but their permeability is poor. Halide perovskites, composed of metal ions and organic ligands, are metal-tunable nanomaterials. In order to improve the permeability of zirconium. In this study, Cs 2 ZrCl 6 was synthesized using zirconium ions and combined with Zr(SO 4 ) 2 for collagen modification application. Based on the principle of reversible reactions, the introduction of Zr(SO 4 ) 2 effectively alleviated the rapid hydrolysis of Cs 2 ZrCl 6 , ensuring the preservation of its nanostructure and enabling continuous penetration during the tanning process. The EDS analysis confirmed the uniform distribution of zirconium in leather collagen tanned with Cs 2 ZrCl 6 /Zr(SO 4 ) 2 . Compared with Zr(SO 4 ) 2 tanned leather (73.1 °C), the shrinkage temperatures of Cs 2 ZrCl 6 /Zr(SO 4 ) 2 tanned leather collagen (83.7 °C) is better. Additionally, the BOD 5 /COD cr ratio of the tannery wastewater in this system is 0.65, indicating excellent biodegradability. The development of the Cs 2 ZrCl 6 /Zr(SO 4 ) 2 tanning system provides a new approach for creating chromium-free tanning agents.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Fangfang Li,Jingya Kong,Ziyuan Fang,Laili Wan,Jing Gu,Changchun Ji,Ying-Hua Zhou
The catalytic transformation of epoxides into cyclic carbonates offers a promising strategy to mitigate excessive CO 2 emissions while producing valuable chemicals. However, attaining high catalytic efficiency and selectivity with MOF-based catalysts under mild conditions continues to be a significant challenge. Additionally, many existing catalytic systems rely on cocatalysts or solvents, compromising sustainability and practicality. In this study, a series of alkyl chain-tunable Zr-MOF catalysts, denoted as TCPP-UiO-66-PDC-DIL(R) (R = Et, Pr, Bu, Pe), were synthesized via a two-step approach. Initially, Zr 4 + ions were coordinated with meso-tetra(4-carboxyphenyl) porphine (TCPP) and 2,5-pyridine dicarboxylic acid (PDC) to create TCPP-UiO-66-PDC. Subsequently, dicationic ionic liquids (DIL) with varying alkyl chains lengths were decorated through post-synthetic modification. Their catalytic performance was assessed for CO 2 -epoxide cycloaddition without the use of cocatalysts or solvents. Among them, TCPP-UiO-66-PDC-DIL(Bu) exhibited the best catalytic performance, achieving a 98 % yield for producing chloropropene carbonate at a low CO 2 pressure (1.0 bar) within 12 h. This exceptional activity was attributed to the synergistic interplay of Lewis-acidic Zr 4+ nodes for epoxide activation, the porphyrin moiety of the TCPP ligand enhancing CO 2 adsorption, and the strong nucleophilicity of bromide anions in DIL to facilitate the halide ion-mediated nucleophilic attack on the epoxide-CO 2 adduct. Additionally, the catalyst demonstrated superior universalities toward other substrates and recyclability. These findings expand the potential of the multifunctional MOF-based heterogeneous catalysts, enhancing their efficiency and sustainability for use in CO 2 conversion.
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LANGMUIR
·
2025
·
IF 3.9
Haiqing Liu,Muhammad Jawad,Jingmao Zhao,Baomin Fan,Mohammad Tabish,Muhammad Mubeen,Mubashar Mahmood,Jingbao Wang
Under-film filiform corrosion (FFC) poses a significant challenge to the durability and reliability of Zn–Al–Mg-coated steel (ZM-steel), necessitating the development of advanced protective strategies. Herein, benzotriazole 5-carboxylic acid (BTC)-modified titanium zirconium (TiZr) conversion coatings (CCs) were developed as a sustainable solution to mitigate FFC, enhance corrosion resistance, and improve the adhesion of epoxy (EP) coatings on ZM-steel. Through electrochemical impedance spectroscopy, potentiodynamic polarization, FFC, and neutral salt spray (NSS) tests, the optimized BTC-TiZr CC, prepared in a Ti–Zr solution containing 0.5 g/L BTC, a treatment temperature of 25 °C, and a short immersion duration of 120 s, exhibited superior corrosion resistance, robust adhesion strength, and exceptional FFC inhibition. Metal–organic complexes (MOCs) of Ti/Zr/Zn with BTC were identified alongside mixed Ti/Zr/Zn/Al/Mg oxides and fluorides within the BTC-TiZr CC. BTC not only exerted strong corrosion inhibition efficacy for ZM-steel but also facilitated the formation of MOCs with metal ions in TiZr conversion solutions (CSs). Density functional theory calculations revealed that BTC preferentially adsorbs onto the MgZn2 phase, effectively suppressing its dissolution within the ZM layer. These findings establish BTC-TiZr CCs as a promising, environmentally friendly solution for advanced corrosion protection of ZM-steel, especially FFC suppression.
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Catalysis Science & Technology
·
2025
·
IF 4.2
Haoxi Jiang,Qian Ran,Yingying Zhao,Guochao Yang,Lingtao Wang
In response to the challenges of equipment corrosion and environmental pollution associated with the homogeneous catalytic production of crotonaldehyde via acetaldehyde aldol condensation, this work focused on the synthesis of Zr-β zeolites with Lewis acidity. The crotonaldehyde selectivity was significantly improved by tailoring the acidic properties of the zeolites. A comparative study of three distinct Lewis acid sites identified isolated framework tetra-coordinated Zr sites as the most efficient catalytic centers, which were successfully constructed using hydrothermal synthesis and liquid-phase incorporation methods. Zr-β zeolites synthesized via liquid-phase incorporation demonstrated higher conversion and selectivity owing to larger pore size, greater total Lewis acidity and a higher proportion of weak and medium Lewis acid sites. These properties were further optimized by adjusting the precursor and solvent during the synthesis process. In situ DRIFTS analysis revealed that the Lewis acid sites activated the α-H of acetaldehyde, forming carbanion intermediates essential for the enolization and subsequent aldol condensation. The main by-product, methyl cyclopentenone, was found to originate from the Prins reaction of sorbaldehyde formed through excessive aldol condensation, which was mediated by Brønsted acid sites. To suppress this side reaction, the zeolites were modified with alkali cations (Na+, K+) to selectively passivate the Brønsted acid sites while enhancing the Lewis acidity significantly. This strategy effectively reduced by-product formation and ultimately achieved a crotonaldehyde selectivity of 94.7%.
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Nano Energy
·
2025
·
IF 17.1
Zhao Sun,Huicai Wang,Xingxu Wang,Riguang Zhang,Zhiqiang Sun
Sorption-enhanced steam reforming of methanol (SE-SRM) offers a promising route for high-quality hydrogen production with in situ CO 2 capture; however, achieving an optimal balance between catalytic activity and CO 2 uptake capability, while ensuring catalyst stability, remains a significant challenge. In this study, a series of Zr-doped (0 wt%, 5 wt%, 15 wt%, 25 wt%) Cu-MgO catalytic sorbents are synthesized for SE-SRM. At 180℃, the hydrogen concentration and yield reach nearly 100 % and 10.35 μmol·g −1 ·s −1 . Moreover, the catalytic sorbent basically retains its catalytic activity and CO 2 uptake capacity after 30 cycles with merely slight deactivation. Results demonstrate that the doped Zr, presents as tetragonal ZrO 2 , enhances metal-support interactions with the formation of a Cu-O-Zr interfacial structure, promoting Cu nanocluster dispersion and altering the Cu + /Cu 0 distributions. Zr doping also enables the modulation of the medium-strong basic sites. Moreover, the AFM and TEM confirmed the formation of high-roughness MgO surface on the substrate, thereby facilitating CO 2 diffusion and adsorption. DFT calculation results further confirm the advantages of Zr-doped Cu-MgO catalytic sorbents due to its stronger capability on CH 3 OH activation and CO 2 adsorption.
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