FUEL
·
2025
·
IF 7.5
Li-Li Xue,Qing He,Si-Wen Li,Jian-She Zhao
In recent years, the escalating global demand for clean energy has underscored the urgency of developing high-efficiency fuel desulfurization technologies. This study reports the facile synthesis of a molded fiber-supported composite catalyst, POM@UiO-66-NH 2 @CF (PU N C), via impregnation, integrating polyoxometalates (POMs) with amino-functionalized metal–organic frameworks (MOFs) on cellulose fibers (CF). The catalyst delivers exceptional performance in ultra-deep oxidative desulfurization (ODS), enabled by systematic optimization of reaction parameters using response surface methodology (RSM) with a Box-Behnken design (BBD). Through RSM optimization and adjustment, the actual desulfurization conditions were determined as 66 °C, O/S = 7, 7 mL DMF, and 2 catalyst pieces and PU N C achieved a validated 99.26 % desulfurization efficiency for dibenzothiophene (DBT) in model fuels, demonstrating close agreement with theoretical predictions. Kinetic analysis revealed the ODS reaction conformed to a pseudo-first-order kinetic model with a low activation energy of 2.45 kJ/mol, while EPR spectroscopy confirmed ·O 2 − radicals as the dominant reactive species, highlighting a POM-mediated radical oxidation pathway. PU N C exhibited robust reusability, maintaining >95 % efficiency over 5 consecutive cycles. The catalyst’s performance is attributed to the synergistic architecture of MOF-fiber supports, where 3-chloropropyltrimethoxysilane (CPTMS) enables covalent bonding of UiO-66-NH 2 to CF, creating amine-rich sites for electrostatic POM immobilization and enhanced stability. This work showcases the synergy between structural design and RSM-driven optimization, offering innovative insights for developing high-efficiency, environmentally benign molded catalysts for ultra-deep ODS and related oxidative processes.
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2018
·Vol. 5
·期 6
·1441-1453
·
IF 6.087
Jingmiao Wei,Wei Zhang,Weiyi Pan,Chaoran Li,Weiling Sun
Adsorption behaviors and mechanisms of selenite [Se(IV)] and selenate [Se(VI)] on two types of zirconium metal–organic frameworks (MOFs, UiO-66 and UiO-66-NH2) were investigated using batch experiments, spectroscopic analyses, and theoretical calculations. Se(IV) adsorption was substantially greater than Se(VI) adsorption. Intriguingly, with increasing solution pH, Se(IV) adsorption increased to a maximum at pH 7, whereas Se(VI) adsorption monotonically decreased. Se(IV) adsorption was not influenced by coexisting ions except for PO43−, whereas Se(VI) adsorption was in general decreased with increasing coexisting ion concentrations. The underlying molecular binding mechanisms were elucidated via zeta potential, XPS, and FTIR analyses as well as density functional theory calculations. Se(IV) formed a strong inner-sphere complex with the MOFs via Lewis acid/base complexation between the Zr coordinatively unsaturated sites and HSeO3− or SeO32− (−59.4 to −142 kJ mol−1) and hydrogen bonding between Zr–O–C and H2SeO3 (−24.4 to −29.8 kJ mol−1). Se(VI) formed outer-sphere complexes with the MOFs through electrostatic interactions (−50.6 to −62.1 kJ mol−1). Thus, the BET surface area was the predominant factor determining the Se(IV) adsorption, whereas both the surface charge and BET surface area controlled the Se(VI) adsorption. This study provided new insights on the molecular interactions between Se(IV) and the MOFs, and revealed the distinct differences between the Se(IV) and Se(VI) adsorptions.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Junhui He,Mingming Zhang,Xiaochu Zheng,Jianfeng Li,Linjuan Yang,Cong Luo,Xudong Cui,Zhuoyu Ji,Daopeng Sheng,Xiaofang Feng,Tao Chen,Wenkun Zhu
The synergistic coupling of nonthermal plasma (NTP) with catalysts offers a promising route for converting CO2/H2O into high-value-added chemicals, but its efficiency is hindered by low-activity catalysts and electron quenching by gaseous H2O. Herein, we propose a “surface electron-enriched microenvironment” strategy to construct a UiO-66(SH)2 catalyst to boost NPT CO2 conversion. Under dielectric barrier discharge (DBD) plasma conditions, the UiO-66(SH)2 catalytic system achieves a CO2 conversion rate of 42.19%, which is 1.88 and 38.87 times higher than that of the unmodified UiO-66 system and plasma-only system, respectively. CO was identified as the dominant carbon-containing product with a selectivity of 82.39%, along with CH4 and trace C2–C3 hydrocarbons. Theoretical calculations and experimental results confirm that the thiol groups in UiO-66(SH)2 create an electron-enriched microenvironment, which significantly enhances the adsorption and activation of CO2 while effectively suppressing the electron quenching effect of gaseous H2O on a plasma-induced CO2 dissociation process. Furthermore, thiol functional groups create an electron-rich microenvironment, effectively reducing the free-energy barrier for the formation of the key intermediate *COOH and thereby accelerating CO2 conversion kinetics. This research provides a rational strategy for achieving efficient and highly selective plasma catalytic CO2 conversion through the metal–organic frameworks (MOFs) functionalization.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
LUMINESCENCE
·
2026
·Vol. 41
·期 7
·e70567
·
IF 2.8
Fenqiang Luo,Liyan Zheng
Novel multifunctional metal–organic frameworks prepared by encapsulating luminol, hemin, and glucose oxidase within UiO-66 have been employed for the chemiluminescent determination of glucose via a one-step method. Benefitting from the encapsulating cascade catalyst with luminescent reagent in UiO-66, the as-prepared material can be utilized to fabricate practical glucose sensors with a wide response range, a low detection limit, and a short detection time. This promising sensing material is anticipated to have widespread applications in biotechnology and demonstrates significant potential for the green, selective, and sensitive detection of target analytes.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2026
·
IF 2.1
Gao Shuang,Yu Yue,Li Yunheng,Han Lu,Song Yakai,Chen Xiaolu
A set of phosphomolybdic acid catalysts was synthesized by employing ligand-functionalized UiO-66 as the support. The structural properties of these catalysts were characterized via XRD, FT-IR, BET, TEM, and XPS techniques. To explore the influence of catalyst structure on its catalytic performance, the desulfurization of dibenzothiophene (DBT) from simulated fuel was utilized as a model reaction. Under optimized reaction parameters, the Co-POM-UiO-66-NO 2 -F catalyst exhibited the highest DBT conversion efficiency, achieving 99.3%. After five consecutive desulfurization cycles, the catalyst retained a desulfurization activity of 91.8%. This excellent stability was attributed to the incorporation of the –F group, which enhanced the catalyst’s lipophilicity and hydrophobicity. Additionally, the incorporation of –F groups increased the content of the Mo active species (Mo 5+ ), regulated the electronic structure of the catalyst, and optimized the microenvironment surrounding the active centers, which collectively contributed to the enhanced catalytic performance. Graphic abstract
The alternative text for this image may have been generated using AI.
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2026
·Vol. 18
·期 7
·e70718
·
IF 4.1
Somboon Chaemchuen,Xingxing Chen,Deshuang Lu,Panchan Sricharoon,Suwin Apichartpattanasiri,Nikom Klomkliang,Francis Verpoort
Highly dispersed palladium nanoparticles (Pd NPs) embedded within a hierarchical UiO-66 structure, referred to as Pd@U-12, have been successfully synthesized via a green, straightforward of solid-solid thermal (SST) method. This innovative SST technique enables uniform dispersion of Pd NPs, allowing their encapsulation within the hierarchical framework of UiO-66. The unsaturated sites in the host UiO-66 facilitate the coordination of Pd, which are subsequently reduced to nanoparticles during the SST process, forming Pd@U-12. The Pd NPs are highly dispersed on the hierarchical support (U-12) and serve effectively as catalytic sites for hydrogenation reactions. The optimally synthesized 20%Pd@U-12 demonstrated exceptional performance as a heterogeneous catalyst for the hydrogenation of cyclohexene, achieving 99% conversion with stable activity over five consecutive cycles. Notably, the SST method for encapsulating Pd NPs (Pd@U-12) offers several advantages, including rapid incorporation of metal nanoparticles within a short time, a green, solvent-free synthesis process, high dispersion and stability of the metal content within the host material. These features could significantly enhance the effectiveness of Pd@U-12 as a robust heterogeneous catalyst in various catalysis applications. Graphical
✓ 已验证
DOI
高影响因子
LANGMUIR
·
2026
·
IF 4.4
Yunyun Li,Xiaohui Zeng,Ge Wang,Dingyi Zhang
The widespread misuse of nonsteroidal anti-inflammatory drugs (NSAIDs) has become a growing concern due to their severe threats to aquatic ecosystems and human health. Current adsorption technologies face limitations including low capacity, poor efficiency for trace-level contaminants, and unclear removal mechanisms. These limitations stem from poorly optimized pore architectures and surface chemistries in existing materials, necessitating the development of multifunctional adsorbents with tailored active sites. Herein, a series of MnO2/UiO-66-x composites were rationally designed via a solvothermal approach and comprehensively characterized using powder X-ray diffraction (PXRD), Fourier transform infrared (FTIR) spectroscopy, N2 physisorption, scanning electron microscopy (SEM), and zeta potential analysis. Systematic optimization demonstrated that MnO2/UiO-66-1 (5 mg) achieved exceptional adsorption capacity (qmax = 659.49 mg·g–1) for diclofenac sodium (DCF, 20 mg·L–1, 30 mL), with >90% removal within 10 min (k2 = 0.0081 g·mg–1·min–1). Mechanistic studies revealed that this performance was attributed to hierarchical porosity (micro-/mesopores), which enables size-selective uptake, synergistic binding, and pH-dependent electrostatic enhancement. Structure–activity relationships indicated that NSAIDs adsorption efficiency (naproxen ≈ ibuprofen ≈ ketoprofen > indomethacin > paracetamol) was governed by molecular structure, size, and pKa values. Thermodynamic and kinetic studies confirmed a spontaneous (ΔG0 < 0), endothermic (ΔH0 > 0), and entropy-driven (ΔS0 > 0) process dominated by chemisorption through synergistic interactions (including coordination bonding, hydrogen bonding, Lewis acid–base effects, electrostatic attraction, and π–π stacking). This study establishes a new paradigm for metal–organic-framework-based adsorbent design through precise control of metal–organic interfaces and defect engineering. With 87% capacity retention after 5 regeneration cycles, MnO2/UiO-66-x shows strong potential for practical water remediation applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PAPERS
·
2026
·
IF 2.7
Zhong Xiangyan,He Xinye,Long Ruiqing,Qi Linfeng,Zhao Qiang
Efficient utilization of long-wavelength visible light remains a key challenge in developing metal-organic-framework-based photocatalysts for solar-driven pollutant removal. To address this issue, carbon quantum dot (CQD)-modified UiO-66-NH 2 hybrid materials with different nominal CQD loadings were constructed through induced loading and secondary thermal fixation to combine spectral conversion with interfacial photophysical regulation. Structural and textural characterizations showed that CQD incorporation preserved the crystalline and porous framework of UiO-66-NH 2 while modifying its surface composition, pore characteristics, and optical response. The CQDs displayed visible-to-ultraviolet anti-Stokes emission centered at approximately 340 nm under 600 nm excitation. CQD incorporation also enhanced visible-light absorption and induced photoluminescence quenching consistent with interfacial photophysical coupling. Transient-current measurements showed reproducible light-switching responses, while EIS revealed a lower impedance response for CU-3 under illumination; together, these results are consistent with facilitated interfacial charge migration. Under visible-light irradiation in the presence of FeCl 3 as an electron scavenger, CU-3, containing 3 wt% CQDs, achieved a background-corrected net methyl orange removal of 67% within 90 min. Its apparent rate constant was 1.203 × 10 − 2 min − 1 , approximately 6.6 times that of pristine UiO-66-NH 2 . Tert-butanol inhibition and DMPO spin-trapping ESR measurements jointly supported the involvement of hydroxyl radicals, with CU-3 exhibiting a stronger light-induced DMPO–·OH signal than pristine UiO-66-NH 2 . The effect of EDTA-2Na could not be assigned exclusively to photogenerated holes because of its complexation with Fe 3+ . These findings demonstrate the importance of optimizing CQD loading and suggest that spectral conversion and interfacial photophysical coupling contribute to the enhanced apparent visible-light activity.
✓ 已验证
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2026
·
IF 11.8
Jixiang Li,Genyun Zhou,Fei Wu,Jinping Yuan,Linan Hu,Qiang Zhang,Wenge Yang,Yonghong Hu
Tetracycline (TC) is a persistent broad-spectrum antibiotic that poses significant threats to human health and the environment. Herein, we developed an ultrasensitive photoelectrochemical (PEC) biosensor for rapid TC detection. The sensor utilizes a flexible Si-doped carbon fiber membrane derived from polyacrylonitrile and dimethyldiethoxysilane as a conductive substrate. After coating with poly (3,4-ethylenedioxythiophene) and polystyrene sulfonate (PEDOT: PSS), a ternary UiO-66-NH 2 /Ag/g-C 3 N 4 Z-scheme heterojunction is assembled as the photoactive core, followed by electrostatic immobilization of laccase to achieve specific TC recognition. Electrochemical characterization confirmed that laccase improved both the biocatalytic activity and electron-transfer efficiency of the electrode. Combined with transient photocurrent measurements and molecular dynamics simulations, the sensing mechanism was shown to be dominated by steric hindrance arising from TC occupation of the laccase active site, followed by oxygen consumption, yielding a detection limit of 0.012 μM over 0-30 μM TC (R 2 = 0.993). UV diffuse reflectance spectra (UV-DRs), Mott–Schottky analysis (M-S), and electron paramagnetic resonance (EPR) measurements further verified that the Ag-mediated Z-scheme pathway significantly enhanced carrier separation. With excellent stability and anti-interference performance in real river water and complex matrices, this work provides an effective strategy for antibiotic detection by integrating flexible carbon-based substrates with advanced Z-scheme photocatalytic systems.
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Mingming Dong,Zewen Huang,Shuyong Yang,Peng Zhou,Shenghui Tu
The growing prevalence of antibiotic residues in aquatic environments, particularly recalcitrant antibiotics like tetracycline (TC), poses significant ecological risks. In this study, a novel Bi 2 WO 6 /Mo-doped BiVO 4 /NH 2 -UiO-66 (BBU) ternary heterojunction photocatalyst was successfully synthesized via a solvothermal method to enhance visible-light-driven TC degradation through component synergy. Systematic characterization revealed that Mo doping induced lattice distortion in BiVO 4 , while the incorporation of NH 2 -UiO-66 drastically increased the specific surface area from 23.647 to 398.804 m 2 ·g −1 , providing abundant active sites. Photoluminescence (PL) and Electrochemical Impedance Spectroscopy (EIS) analyses demonstrated that the optimized BBU-3 sample exhibited the lowest charge carrier recombination rate. Under visible light irradiation for 80 min, BBU-3 achieved 95.2% degradation of TC, with reaction kinetics 8.61, 15.76, and 5.01 times higher than those of pristine Bi 2 WO 6 , BiVO 4 , and binary heterojunctions, respectively. Degradation-trapping experiments and electron paramagnetic resonance (EPR) measurements indicate that h + , 1 O 2 and ·O 2 - are the primary reactive species, suggesting that this system is a synergistic radical-non-radical degradation system. Additionally, possible degradation pathways and intermediate toxicity were evaluated. This work offers a promising strategy for designing efficient bismuth-based MOF heterojunctions for antibiotic remediation in water.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Bin Zhao,Yue Li,Min Sun,Zhaohui Zhang,Liang Wang,Jiaxue Yao
The growing concern over pharmaceutical and personal care products (PPCPs) in drinking water sources underscores a serious public health risk. Although polyamide (PA) nanofiltration (NF) membranes are highly effective at removing PPCPs, their performance for neutral and hydrophobic PPCPs requires improvement. To overcome this challenge, we fabricated a hydrophilic NF membrane containing a calcium alginate (CaAlg) hydrogel interlayer and UiO-66-NH 2 nanofillers (PA/UiO-66-NH 2 /CaAlg) to reduce membrane affinity for hydrophobic PPCPs. A fishnet-like structure was created on the membrane surface, which enhanced the effective area for filtration. Consequently, the water permeance of the PA/UiO-66-NH 2 /CaAlg membrane reached 22.7 L·m −2 ·h −1 ·bar −1 , representing an 83 % increase over the control thin-film composite (TFC) membrane. The hydrophilic CaAlg interlayer also restricted the diffusion of piperazine (PIP), thereby slowing its interfacial polymerization with trimesoyl chloride (TMC). This resulted in a highly hydrophilic PA film, evidenced by a water contact angle below 10°. The reduced adsorption of hydrophobic PPCPs on this hydrophilic surface diminished the driving force for their penetration. Furthermore, the inherent hydrophilicity of the CaAlg hydrogel interlayer suppressed the diffusion of hydrophobic PPCPs across the membrane. As a result, the removals for hydrophobic methylparaben (MP), propylparaben (PP), bisphenol A (BPA), and benzylparaben (BP) were significantly enhanced. The selectivity ( A/B ) for BPA increased by more than four times compared to that of the TFC membrane. This study demonstrates that integrating a hydrogel interlayer with MOF nanofillers offers a promising approach for developing high performance NF membranes that exhibit both improved water permeance and superior PPCP removal.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Ruihua Chen,Hao Deng,Junpeng Jiang,Daoyang Han,Gang Shao,Hailong Wang,Rui Zhang,Chao Ma
To overcome the problem of insufficient molybdenum adsorption capacity of commercially utilized alumina in 99 Mo/ 99m Tc generator, UiO-66(Ce)@MXene composites as potential molybdenum adsorbents were successfully prepared via in-situ growth method in this work. The adsorption performance and adsorption mechanism were investigated. The results indicate that the UM3 possesses superlative adsorption behavior compared to the other two samples. The adsorption kinetics are well described by the quasi-second-order model and the adsorption reaches equilibrium within 30 min. The adsorption isotherm can be well fitted with the Langmuir model, displaying the maximum molybdenum adsorption capacity of 833 mg/g at pH 3, superior to other reported adsorbents. The adsorption capacity manifests that polymolybdates are captured by the hydroxyl groups on MXene through hydrogen bonds. The monomolybdates can diffuse into micropores and are adsorbed on adsorption sites, e.g. missing-linker defects and Ce-OH groups. Consequently, the constructed hierarchical frameworks promote molybdenum adsorption and increase adsorption capacity significantly. The unrivalled adsorption performance of UiO-66(Ce)@MXene composites as molybdenum adsorbents have promising potential for the application in 99 Mo/ 99m Tc generator.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）