CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuling Ma,Airong Li,Cheng Wang
Metal-organic frameworks (MOFs) with a high specific surface area, an adjustable pore structure, and functionalized pore environment have a broad application prospect in gas adsorption and separation. In this work, a series of defective UiO-66 (UiO-66-monocarboxylic acid) samples were prepared by adding different monocarboxylic acids during the synthesis of UiO-66. UiO-66-monocarboxylic acid samples (UiO-66-formic acid, UiO-66-acetic acid, UiO-66-benzoic acid, UiO-66-acrylic acid, and UiO-66-cyanoacetic acid) had a high specific surface area (1200–1400 m 2 /g) and a good thermal stability (560 °C). In the desulfurization experiment of simulated flue gas (SO 2 /CO 2 /O 2 /N 2 , 0.3/10.0/5.5/84.2 vol%), the breakthrough time of UiO-66-cyanoacetic acid for SO 2 was higher (194 min/g), and the selectivity of SO 2 /CO 2 reached 33.8. Through optimizing the moles of cyanoacetic acid added, the breakthrough time of SO 2 on 18-UiO-66-cyanoacetic acid increased to 251 min/g. At a pressure of 1.0 bar and a temperature of 298 K, the adsorption capacity of SO 2 by 18-UiO-66-cyanoacetic acid reached 762.1 mg/g. In addition, the adsorption behavior of 18-UiO-66-cyanoacetic acid for SO 2 was considered as a combination of chemical and physical adsorption, and fractional chemisorption sites was provided by cyanoacetic acid.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Chongfu Wu,Zhenhua Sun,Changshen Ye,Zhaoyang Qi,Jie Chen,Zhixian Huang,Ting Qiu
The development of catalysts with excellent performance in oxidative desulfurization (ODS) at room temperature will greatly facilitate the advancement of desulfurization technology. An efficient novel strategy, 4-aminopyridine molecular bridging combined with manual grinding, was presented to encapsulate HPW into UiO-66 for achieving stable loading of PW and to produce abundant defects that contribute to the formation of active complexes with strong oxidation ability. The prepared catalyst showed outstanding catalytic activity in the ODS system, achieving full desulfurization in 15 min at room temperature and a low O/S molar ratio. Further investigations reveal that the synergistic catalytic effect of the faulty UiO-66 and PW is mostly responsible for superior catalytic performance. UiO-66 rich in defects promote the decomposition of H 2 O 2 into radicals, and PW can combine with the radicals to form more stable active peroxide intermediates, then exerting the catalytic ability of ODS at room temperature. Such a synergistic catalytic mechanism provides a guide to improving the oxidation ability of PW-based catalysts at room temperature.
研究领域:
化学工程
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催化材料科学
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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
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催化化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2024
·Vol. 25
·期 12
·6779
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IF 4.9
Ming-Qin He,Xin-Yu Chang,Hong-Wei Li,Yuqing Wu
The oxidative esterification of aldehydes under mild conditions remains a significant challenge. This study introduces a unique defective UiO-66 to achieve gold nanoclusters (AuNCs) for efficient aldehyde oxidation under mild conditions. The construction and characterization of these materials are thoroughly investigated by techniques of XRD, SEM and TEM images, FT-IR, Raman, and XPS spectrum, emphasizing the unique microporous in defective UiO-66 are conducive to the fabrication of AuNCs. The catalytic performance of the prepared materials in aldehyde oxidation reactions is systematically evaluated, demonstrating the remarkable efficiency of dispersed Au@UiO-66-25 with high-content (9.09 wt%) Au-loading and ultra-small size (~2.7 nm). Moreover, mechanistic insights into the catalytic process under mild conditions (70 °C for 1 h) are provided, elucidating the determination of defective UiO-66 in the confined fabrication of AuNCs and subsequent furfural adsorption, which underlie the principles governing the observed enhancements. This study establishes the groundwork for the synthesis of highly dispersed and catalytically active metal nanoparticles using defective MOFs as a platform, advancing the catalytic esterification reaction of furfural to the next level.
研究领域:
材料科学
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催化
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纳米技术
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化学工程
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
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2025
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IF 4.2
Kai Yan,Zhihao Yu,Yingqing Li,Mengyan Guo,Yuanyu Wang,Xuebin Lu
The efficient dehydration of fructose to 5-hydroxymethylfurfural (HMF) is a crucial step in biomass valorization, requiring solid acids with precisely balanced Brønsted acidity. Defect engineering in Zr-based metal–organic frameworks (MOFs), such as UiO-66, is well known to enhance Lewis acidity; however, its impact on tailoring Brønsted acid sites remains insufficiently understood. Here, we demonstrate that defective UiO-66 possesses a dual-origin Brønsted acid system, comprising intrinsic μ3–OH groups and water molecules coordinated to defect-generated Lewis acidic Zr centers (Zr–H2O). The concentration of these Brønsted acid sites can be finely regulated by thermal activation treatment. A volcano-shaped dependence of catalytic activity on activation temperature is observed, with an optimum at 200 °C. At moderate activation temperatures below 200 °C, the removal of physisorbed water exposes both μ3–OH and Zr–H2O sites, maximizing Brønsted acid density and HMF yield. Activation beyond 200 °C reduces both types of Brønsted acid sites, resulting in diminished catalytic performance. This study reveals the cooperative effect of defect engineering and thermal activation in tuning the Brønsted acidity of MOFs, providing a rational strategy for designing highly selective catalysts for the sustainable production of platform chemicals.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yaofei Zhang,Jiani Chen,Tegexi Buren,Zhuo Li,Xiaojin Zhang,Shuting Ma,Jiafeng Wei,Fukun Bi,Xiaodong Zhang
Electron beam (EB) irradiation has emerged as an effective post-synthetic strategy to modify the structural properties of metal-organic frameworks (MOFs), offering enhanced defect engineering and improved active site dispersion. In this study, UiO-66-100, pretreated under the optimal EB irradiation dose of 100 kGy with abundant structural defects, was selected as the support to synthesize supported noble metal catalysts M-UiO-66-100 (M = Pt, Pd, Ru, Ag, Au). The catalytic performance of M-UiO-66-100 was evaluated by toluene and 2-propanol degradation. Among them, Pt-UiO-66-100 exhibited superior performance for toluene oxidation (T 90 = 187 °C), while Pd-UiO-66-100 showed excellent activity for 2-propanol degradation (T 90 = 229 °C). Both catalysts exhibited distinct physicochemical properties and adsorption behaviors in single-component Volatile organic compound (VOC) systems. Interestingly, further studies revealed that both Pt- and Pd-based catalysts displayed significantly enhanced catalytic activity for toluene and 2-propanol mixture oxidation, highlighting a mutual promotion effect. VOC- temperature-programmed desorption/oxidation (TPD/TPO) and thermal desorption-gas chromatography–mass spectrometry (TD-GC–MS) results elucidated the mutual promotion effect that compared with single VOC systems, Pd-UiO-66-100 and Pt-UiO-66-100 produce fewer intermediates during mixed VOC degradation, which reduced the accumulation of intermediates on the catalysts surface, released the surface active sites, and accelerated their mineralization. This work provides a rational design approach for EB-modified MOF-supported catalysts and deepens the insights into the synergistic oxidation mechanism in mixed-VOC systems.
研究领域:
材料化学
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环境催化
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纳米催化
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多孔材料
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大气污染控制
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Yang Li,Xiaohuan Zang,Yahuan Li,Shuaihua Zhang,Chun Wang,Zhi Wang
A defective UiO-66 with rich defect sites was synthesized by a modulator-induced defect formation approach and used as the solid-phase microextraction (SPME) fiber coating material. The extraction experimental results showed that the defective UiO-66 coating can selectively extract the fungicides chlorothalonil, vinclozolin, dimethachlon, procymidone and iprodione with a high adsorption capability. The superior adsorption capability can be attributed to hydrophobic, Lewis acid-base and hydrogen bonding interactions. After optimization, a SPME with the defective UiO-66 as the fiber coating combined with GC–MS detection was established for the sensitive and selective determination of the five fungicides in fruit samples. Under the optimized experimental conditions, the quantitative linear response was in the range of 0.83–300 ng g −1 , with the coefficients of determination in the range from 0.9970 to 0.9986 and the limits of detection between 0.25 and 9.0 ng g −1 for the analytes. The method was successfully applied for the determination of the fungicides in different fruit samples. Satisfactory method recoveries (82.7%-117.7%) and good precisions with the relative standard deviations being from 3.2% to 12% were achieved.
研究领域:
分析化学
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环境科学
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食品科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）