CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yuling Ma,Airong Li,Cheng Wang,Xingbo Ge
Phosphotungstic acid (H 3 PW 12 O 40 , HPW) exhibits a good desulfurization performance towards the oxidative desulfurization (ODS) of oil-derived fuels. However, it presents two drawbacks: a small specific surface area and poor recovery. In this work, HPW was loaded on the support UiO-66 with a stable structure and large specific surface area, and a family of HPW@UiO-66 catalysts was prepared. Based on the structure and property analyses of powder FT-IR, ICP-OES, XRD, SEM, TG and BET, 0.5-HPW@UiO-66 with defects possessed a high crystallinity, regular morphology, stable structure and dispersed HPW clusters. The removal efficiency of DBT reached 100% and was maintained at 94.70% after 12 times of repeated use under the optimal reaction conditions. The results showed that the catalytic performance of HPW@UiO-66 catalyst for model oil desulfurization was improved when the defects existed.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Lu Lin,Yongjian Zeng,Suyu Zhang,Di Hu,Zhiwei Jiang,Guoqing Guan,Kai Yan
The hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) to biofuel 2,5-dimethylfuran (DMF) serves as a vital reaction in biomass refineries. Herein, Pd-UiO-66 catalysts with controlled contents of ligand-vacancies were developed for the HMF-to-DMF conversion. Strikingly, a volcano-like relationship between defect level and HDO activity was obtained. The DMF yield was promoted ∼3 times, reaching 92.2 % at 160 °C and 15 bar H 2 , which refers to a high-level turnover frequency value of 42.66 h −1 among the reported candidates. The Pd-UiO-66 catalysts also afforded >80 % yield for the HDO of 5-methyl furfural, furfural, and vanillin. Besides, high HDO activity could be retained in five recycles. Manipulating the contents of ligand-vacancies was confirmed to create more Pd 0 species and Bronsted acid sites, leading to remarkable performance. This work provides significant inspiration for tuning structural defects in MOFs to realize the efficient HDO of platform molecules in biomass valorization.
研究领域:
材料科学
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催化化学
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生物质能
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
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IF 6.609
Mengchang Zhou,Changsong Zhou,Dong Chen,Hao Wu,Zhen Zhang,Hongmin Yang,Wei Ruan,Yaming Zhou,Zengqiang Tan
Gaseous toluene, one of the volatile organic compounds, has aroused wide concerns in China due to its growing emissions and harmfulness. Herein, novel manganese decorated UIO-66 catalysts (Mn/UIO-66) were prepared by hydrothermal synthesis and applied to the vaporized hydrogen peroxide system for toluene removal. TEM, BET, XRD, ICP, and XPS were used to analyze the chemical and physical characteristics of Mn/UIO-66. A toluene removal efficiency of 82% with the 3-Mn/UIO-66 catalyst in the vaporized hydrogen peroxide system could achieved. The effects of different reaction conditions (reaction temperature, hydrogen peroxide concentration, and initial toluene concentration) on toluene removal were determined. The yield of hydroxyl radical in the Mn/UIO-66 catalyst combined with the hydrogen peroxide system was positively correlated with the Mn decorated ratio. Results suggested that the catalytic performance is related not only to the yield of hydroxyl radical but also to the catalyst specific surface. The intermediate products during toluene removal were analyzed by gas chromatography-mass spectrometry (GC–MS), and the possible reaction pathway of toluene removal was proposed.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
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IF 8.943
Yuhan Wang,Chang Liu,Chao Wang,Qing Hu,Longzhen Ding
Developing synergistic systems and taking environmental risks into account are two necessary aspects of being considered to remove persistent organic pollutants efficiently. Thus, a combined catalytic system uniting the Fenton-like process and simulated solar-light photocatalysis has been constructed. Moreover, a series of NiCo 2 O 4 /HP-UiO-66 catalysts (yNiCo-DUx) were also fabricated to improve tetracycline (TC) removal efficiency. The NiCo 2 O 4 nanoparticles (NPs) and hierarchically porous metal-organic frameworks (HP-MOFs) were synthesised using one-step calcination. The Z-scheme structure of the catalysts was confirmed by ESR, XPS, DRS, time-resolved PL (TR-PL) spectra and the quenching experiments. The NiCo 2 O 4 nanoparticles could be embedded and fixed into the defects of the MOF structure, and the leaching of toxic metals was also significantly suppressed. In the optimal reaction condition with 15NiCo-DU50, sunlight, and peroxymonosulfate (PMS), the total removal efficiency of TC could reach 98.5% within 8 min of irradiation, and the highest % RSE could reach 11.2%. Moreover, the corresponding reaction rate was 28.7, 3.6 and 1.3–10.2 times higher than photocatalysis, Fenton-like processes and other catalysts. Furthermore, the possible degradation mechanism, generation of reactive species and PMS excitation pathways were also investigated in depth. The present study sheds light on the fabrication of HP-MOFs based catalysts and the combination of various methods to eliminate organic pollutants.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Yun Fan,Haijun Zhang,Meihui Ren,Yichi Zhang,Yun Li,Longxing Wang,Jiping Chen
It is of great significance to develop the low-temperature catalysts for the reduction in emission of chlorinated aromatic hydrocarbons (CAHs) from the industrial thermal processes. In this work, the bimetallic Ce-Zr/UiO-66 catalysts were synthesized by a solvothermal method to degrade CAHs. Powder X-ray diffraction, Fourier transform infrared spectra and X-ray photoelectron spectroscopy analyses showed that cerium was successfully incorporated into the lattice of Zr/UiO-66 without destroying the structure of metal–organic frameworks. The activities of Ce-Zr/UiO-66 catalysts for CAHs degradation varied with the concentration of cerium. Ce 0.2 Zr 0.8 /UiO-66 with the highest surface area (1502 m 2 g −1 ) presented the highest efficiency (>85%) for hexachlorobenzene degradation at low heating temperature (100–150 °C) with less formation of polychlorinated dibenzo- p -dioxins and dibenzofurans. Appropriate amount of water (5 wt%) and nitrogen atmosphere were beneficial to improve degradation efficiency. The degradation products proved that hydrodechlorination and oxidation of CAHs both occurred on the catalysts.
研究领域:
环境化学
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催化
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Dong Wang,Tinglue Zhang,Mohamed Gamal El-Din,Xuefen Wang
In this work, the 2-fluoroterephthalic acid with asymmetric structure and high electronegative F species was introduced in the assembly of Ce-UiO-66 catalysts to increase the defect density and enlarge pore structure for enhancement in removal efficiency of sulfamethoxazole. Owing to the strong coordination ability from high electronegative F species of 2-fluoroterephthalic acid with Ce-oxo nodes, the designed CUF exhibited improved interfacial properties (accelerated electron transfer rate, available active sites and enhanced interaction with PMS), which was favorable for the exploration and accessibility of active sites with sulfamethoxazole and PMS to decrease the adsorption barrier and accelerate PMS activation. As a result, the CUF catalysts exhibited higher adsorption capacity (173.4 mg/g) than that of CUH (117.8 mg/g), the enhanced degradation efficiency of sulfamethoxazole with a rate constant higher than 2.3 times CUH, good elimination (>95 %) of methylene blue, tetracycline and ibuprofen. In addition, the CUF/PMS system possessed satisfactory stability in wide solution pH, recycling and real water and good potential application in continuous wastewater treatment based on the designed dynamic catalytic reactor. This work provided deep insight into the design of catalysts with high adsorption performance and degradation efficiency based on the structure–activity relationship.
研究领域:
环境科学
·
材料科学
✓ 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）