MOLECULES
·
2021
·Vol. 26
·期 19
·5736
·
IF 4.412
Chunhua Wang,Zhiquan Yu,Yuhao Yang,Zhichao Sun,Yao Wang,Chuan Shi,Ying-Ya Liu,Anjie Wang,Karen Leus,Pascal Van Der Voort
Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2reduction. The obtained Pd/UiO-66-NO2catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.Keywords:Pd/UiO-66-NO2;furfural;hydrogenative ring-rearrangement;cyclopentanone;double-solvent method
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Nanomaterials
·
2019
·Vol. 9
·期 12
·1698
·
IF 4.034
Yanliang Yang,Dongsheng Deng,Dong Sui,Yanfu Xie,Dongmi Li,Ying Duan
The hydrogenation of furan ring in the biomass-derived furans is of great importance for the conversion of biomass to valuable chemicals. Fabrication of high activity and selectivity catalyst for this hydrogenation under mild conditions was one of the focuses of this research. In this manuscript, UiO-66-v, in which vinyl bonded to the benzene ring, was first prepared. Then, the uniformly distributed vinyl was used as the reductant for the preparation of Pd/UiO-66-v. The catalyst was characterized by X-ray diffraction, thermogravimetric, N2physical adsorption/desorption, X-ray photoelectron spectroscopy, scanning electron microscope, transmission electron microscopy, energy dispersive spectrometer elemental mappings, and inductively coupled plasma atomic emission spectroscopy to find the Pd/UiO-66-v had a narrow palladium nanoparticles size of 3–5 nm and maintained the structure and thermal stability of UiO-66-v. The Pd/UiO-66-v was used for the hydrogenation of furfuryl alcohol to tetrahydrofurfuryl alcohol in water. 99% conversion of furfuryl alcohol was obtained with 90% selectivity to tetrahydrofurfuryl alcohol after reacted at 0.5 MPa H2, 303 K for 12 h. The Pd/UiO-66-v was proved to be effective for the hydrogenation of furan ring in furans and could be used for at least five times.Keywords:furfuryl alcohol;hydrogenation;tetrahydrofurfuryl alcohol;Pd/UiO-66-v;water solvent
研究领域:
催化化学
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生物质转化
·
绿色化学
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产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xin-Hao Shen,Feng Liu,Qin-Qin Chen,Ying Gao,Xiao-Wen Wang,Xin Liu
The efficient degradation of emerging pollutants in water, represented by CBZ, is receiving increasing attention from all sectors of society. Although advanced oxidation reactions represented by Fenton reaction can efficiently degrade emerging pollutants, the problem of iron sludge that comes with it is hindering the further promotion of this technology. Herein, UiO-66(Zr)-2OH material was synthesized by hydrothermal method and loaded with Pd 0 NPs on the surface of the material by in situ reduction. The MOFs-H 2 -Accelerated Catalytic Fenton system was constructed by accelerating the regeneration of Fe(II) in the system by activating the [H] produced by H 2 introduced into the system at room temperature and pressure. Within 180 min, the removal of the target pollutant CZB could reach more than 99 % under the condition of only 25 µmol of Fe(II) and 25 mmol of H 2 O 2 .
研究领域:
环境科学
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材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Tianjiao Meng,Ningzhao Shang,Anaclet Nsabimana,Huimin Ye,Huan Wang,Chun Wang,Yufan Zhang
MicroRNA-21 (miR-21) has been widely investigated as important biomarkers for cancer diagnosis and treatment. Herein, a highly sensitive nonenzymatic electrochemical biosensor based on [email protected] frameworks ( [email protected] ) and target-catalytic hairpin assembly (CHA) with target recycling approach has been proposed for the detection of miR-21. The proposed biosensor integrates the efficient CHA strategy and excellent electrocatalytic performance of [email protected] nanocomposites. The concentration of miRNA-21 is related to the amount of the adsorbed electrocatalyst , leading to the different electrochemical signals for readout towards paracetamol (AP). This biosensor shows a low limit of detection of 0.713 fM with the dynamic range of 20 fM −600 pM under the optimal experimental conditions, providing a powerful platform for detecting miR-21. Furthermore, the designed biochemical self-assembly strategy of this electrochemical biosensor is promising candidate for potential applications in the analysis of other important genetic biomarkers for early diagnosis of cancers.
研究领域:
分子生物学
·
分析化学
·
癌症诊断
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 43
·9031-9040
·
IF 6.331
Jilin Zheng,Peng Zhao,Shiying Zhou,Sha Chen,Yi Liang,Fengchun Tian,Jun Zhou,Danqun Huo,Changjun Hou
Integrating metal–organic frameworks (MOFs) of different components or structures together and exploiting them as electrochemical sensors for electrochemical sensing has aroused great interest. Furthermore, the incorporation of noble metals with MOFs is conducive to the improvement of catalytic performance. In this work, Pd@UiO-66-on-ZIF-L nanomaterials were successfully synthesised onto a self-supported flexible carbon cloth (Pd@UiO-66-on-ZIF-L/CC) through a novel strategy called MOF-on-MOF. Then, Au nanoparticles were electrodeposited onto Pd@UiO-66-on-ZIF-L/CC to obtain Au–Pd@UiO-66-on-ZIF-L/CC, which can serve as an excellent electrocatalyst for the reduction of hydrogen peroxide (H2O2). The obtained flower-like Pd@UiO-66-on-ZIF-L/CC hybrid MOF changes the structure of the monomeric MOF alone and adds more attachment sites. The synergy of the bimetals greatly improved the catalytic performance of the as-developed sensor. Electrochemical experiment results show that the proposed sensor based on Au–Pd@UiO-66-on-ZIF-L/CC has an extended linear range from 1 μM to 19.6 mM with a sensitivity of 390 μA mM−1 cm−2, and a low limit of detection (LOD) of 21.2 nM (S/N = 3). Moreover, it has good anti-interference, reproducibility, repeatability and excellent stability. Furthermore, the real-time in situ detection of H2O2 secreted from human adenocarcinomic alveolar basal epithelial cells (A549 cells) was achieved by culturing cells on Au–Pd@UiO-66-on-ZIF-L/CC, which indicates the potential of the sensor for applications in cancer pathology. Both the synthesis strategy and the sensor design provide new methods and ideas for the production of ultrasensitive H2O2 electrochemical sensors.
研究领域:
材料科学
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电化学
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生物传感器
·
癌症病理学
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2026
·
IF 4.8
Ying Gao,Jinxing Long
Conversion of ethyl levulinate to GVL was proposed using Pd 4 /UiO-66-NH 2 . • Pd 4 /UiO-66-NH 2 was constructed via a post-synthetic modification strategy. • Synergistic effects between Pd species and acidic sites drive superior performance. • GVL yield of 90% with 98.9% selectivity was achieved under 170 ℃ and 1.0 MPa H 2 . • The catalyst shows good recyclability, and can be reused for at least five runs. An efficient strategy is proposed for direct hydrogenation of ethyl levulinate (EL) to γ-valerolactone (GVL) using a highly dispersed palladium nanoparticles supported on the UiO-66-NH 2 framework (Pd/UiO-66-NH 2 ), which was prepared via a facile post-synthetic modification by anchoring palladium (Pd) nanoparticles on the framework's native -NH 2 groups. Under optimized conditions (170 °C, 1.0 MPa H 2 ), 90% yield and 98.9% selectivity of GVL were shown when the reaction was catalyzed by Pd 4 /UiO-66-NH 2 in cyclohexane. Catalyst characterization using XRD, N 2 adsorption-desorption, FT-IR, TEM, TGA, XPS and H 2 -TPR, confirmed that an intensive synergistic effect existed between the Pd and the acidic sites, which is responsible for the superior performance of Pd@UiO-66-NH 2 . The solvent effect and the feedstock adaptability were also investigated. Furthermore, the catalyst of Pd 4 /UiO-66-NH 2 demonstrated good stability and reusability, where no significant activity loss was shown even after five consecutive cycles. Therefore, this study provides new insights for efficient upgrading biochemical. Download: Download high-res image (188KB) Download: Download full-size image
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DOI
高影响因子
CATALYSIS LETTERS
·
2015
·Vol. 146
·期 1
·117-125
·
IF 2.307
Dong Wenhuan,Feng Cheng,Zhang Li,Shang Ningzhao,Gao Shutao,Wang Chun,Wang Zhi
Abstract
In this paper, the palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 was characterized via transmission electron microscopy, powder X-ray diffraction, N 2 adsorption and X-ray photoelectron spectroscopy. The Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition. Graphical Abstract The palladium nanoparticles were successfully encapsulated in metal–organic framework material, UiO-66, by a facile approach. Based on the microwave-assisted method, the pores of UiO-66 were activated and the metal precursors were reduced at the same time in the presence of reducing agent. The obtained Pd@UiO-66 exhibited efficient catalytic activity for the Suzuki–Miyaura coupling reactions at mild condition.
研究领域:
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
TURKISH JOURNAL OF CHEMISTRY
·
2026
·Vol. 50
·期 3
·285-299
·
IF 2
LI JUANHONG,WANG SUQIN,LIU XIN,LIU FENG
A [H]-accelerated catalytic Fenton system was developed using Pd/UiO-66(Zr)-F4 as the catalyst. This system enabled the regeneration of Fe²⁺ and facilitated the continuous generation of both ·OH and 1O2 through [H]-mediated electron transfer at ambient temperature and pressure. Under the conditions of 0.2 g L−1 catalyst (Pd loading 0.516 wt%), 25 μM Fe2+, 60 mL min−1 H2 flow (as the [H] source), 20 mM H2O2, and pH 3, approximately 89% of carbamazepine (initial concentration 20 mg L−1) was degraded within 3 h using trace iron. However, the catalytic activity of Pd/UiO-66(Zr)-F4 gradually declined from 89% to 53% over six reaction cycles. This decrease was likely due to loss of specific surface area caused by microstructural degradation associated with hydrogen spillover effects.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
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
·
催化化学
·
生物质能
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Yijun Chen,Hailiang Yang,Sanjian Ma,Meina Cheng,Zixia Lin,Long Jin,Xin Liu
As a representative antibiotic, trimethoprim (TMP), the emerging pollutant has been frequently detected in water bodies, and its potential harm has aroused the attention of society. Although the emerging pollutant could be efficiently degraded by the advanced oxidation process (AOP) represented by the Fenton reaction , both the problem of iron sludge disposal and the safe use of H 2 O 2 have plagued the further promotion of this technology. The H 2 (precursor of the active hydrogen [H]) and catalyst Pd/UiO-66(Zr) were introduced into the Fenton reaction in this paper. It was found that the process of reducing Fe(III) and self-generating H 2 O 2 could be facilitated due to the reduction of [H]. Under certain reaction conditions (initial pH 3, trace total iron 25 μM, H 2 30 mL·min −1 , catalyst 2 g·L −1 ) and without H 2 O 2 , a Fenton-like system was constructed, named MHORF-UiO-66(Zr). While achieving zero iron sludge discharge, 100 % of 20 mg·L −1 TMP was rapidly degraded within 1 h. It was found that the degradation of TMP could be attributed to the attack of singlet oxygen and hydroxyl radical . Furthermore, the performance changes of catalyst before and after six rounds of reactions were studied and it was found that Pd/UiO-66(Zr) had excellent and stable catalytic performance.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Yijun Chen,Meina Cheng,Long Jin,Hailiang Yang,Sanjian Ma,Zixia Lin,Guoliang Dai,Xin Liu
The Fenton reaction is recognized as an effective technique for degrading persistent organic pollutants , such as the emerging pollutant trimethoprim (TMP). Recently, due to the excellent reducibility of active hydrogen ([H]), Pd–H 2 has been preferred for Fenton-like reactions and the specific H 2 activation of Pd-based catalysts. Herein, a heterogeneous Fenton catalyst named the hydrogen-accelerated oxygen reduction Fenton (MHORF@UiO-66(Zr)) system was prepared through the strategy of building ships in the bottle. The [H] has been used for the acceleration of the reduction of Fe(III) and self-generate H 2 O 2 . The systematic characterization demonstrated that the nano Pd 0 particle was highly dispersed into the UiO-66(Zr). The results found that 20 mg L −1 of TMP was thoroughly degraded within 90 min in the MHORF@UiO-66(Zr) system under conditions of initial pH 3, 30 mL min −1 H 2 , 2 g L −1 Pd@UiO-66(Zr) and 25 μM Fe 2+ . The hydroxyl radical as well as the singlet oxygen were evidenced to be the main reactive oxygen species by scavenging experiments and electron spin resonance . In addition, both reducing Fe(III) and self-generating H 2 O 2 could be achieved due to the strong metal-support interaction (SMSI) between the nano Pd 0 particles and UiO-66(Zr) confirmed by the correlation results of XPS and calculation of density functional theory. Finally, the working mechanism of the MHORF@UiO-66(Zr) system and the possible degradation pathway of the TMP have been proposed. The novel system exhibited excellent reusability and stability after six cyclic reaction processes.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 10
·1-12
·
IF 2.4
Huang Qiuyun,Liu Shiyu,Shen Weihua,Fang Yunjin
Due to the modifiable properties and excellent stability, metal-organic frameworks (MOFs) are considered potential catalyst supports in heterogeneous reactions. UiO-66 with varying water contents were synthesized as supports of Pd for the carbonylation of methyl nitrite (MN) to dimethyl carbonate (DMC). In accordance with XRD, NH 3 -TPD, and SEM, the water contents showed a negative correlation on the amounts of acid sites and accelerated crystal aggregation. The Pd/UiO-66(x) demonstrated perfect selectivity of DMC (> 99%) and good CO conversion which were increased with the decrease of water contents. Moreover, the catalysts deactivated at the beginning of the reaction, and the catalytic deactivation was due to the damage of the C = O structure in UiO-66 frameworks. This work revealed the influence of water contents on the synthesis of UiO-66 and the deactivation process of MOF-based catalysts in MN carbonylation to DMC. Graphical
研究领域:
材料化学
·
催化化学
·
无机化学
·
多孔材料
·
工业催化
✓ 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）