CATALYSIS TODAY
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2023
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IF 5.3
Zhenyu Li,Enhui Du,Panpan Hao,Liyuan Huai,Yang Zhong,Soliman I. El-Hout,Chunlin Chen,Jian Zhang
The oxidation of biomass-derived 5-hydroxymethyl furfural (HMF) into 2,5-Furandicarboxylic acid (FDCA) is a favorable reaction since FDCA is an ideal alternative to petroleum-based monomer terephthalic acid in bio-based polyester industry. However, producing FDCA with high yield under mild conditions is still challenging, especially at energy-saving near-ambient temperatures. Here, we present a Pd nanoparticles catalyst supported on Vulcan XC-72 carbon (Pd/VC) that can completely convert HMF and achieve an encouraging FDCA yield (92.4%) at 30 ℃. The most important observations include yield declines at pure oxygen bubbling, and the transformation of intermediates becomes stagnant; instead, switching to the diluted oxygen is effectively driving the tandem oxidation as the over-oxidation, and thus, rapid deactivation of the Pd surface could be alleviated. The negative effect of high oxygen concentration also occurs in the dehydrogenation and oxygenation of an extended substrate. Since the decisive influence of oxygen content has often been neglected in past investigations of oxidative transformation over Pd-based catalysts, the current study may offer a critical reminder for other liquid-phase oxidation reactions.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2023
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IF 16.5
Zhiyue Zhao,Zhiwei Jiang,Yizhe Huang,Mebrouka Boubeche,Valentina G. Matveeva,Hector F. Garces,Huixia Luo,Kai Yan
The rational design and green synthesis of low-cost, robust, and efficient catalysts for the selective oxidation of various alcohols are highly challenging. Herein, we report a fast and solvent-free arc-melting (AM) method to controllably synthesize a semimetallic CoSi alloy catalyst (denoted as AM-CoSi) that is efficient in the base- and solvent-free oxidation of six types of aromatic alcohols. X-ray absorption fine structure analysis, electron paramagnetic resonance spectroscopy, and aberration-corrected high angle annular dark field scanning transmission electron microscopy confirmed the successful synthesis of AM-CoSi with abundant Si vacancies (Si v ). The as-prepared CoSi alloy catalysts exhibit an order of magnitude greater activity in the oxidation of a model reactant, benzyl alcohol (BAL) to benzyl benzoate (BBE), compared with their mono-counterparts, and provide 70% yield of BBE, the highest yield reported to date. Experimental results and density functional theory calculations suggest that the CoSi alloy structure improves the BAL conversion and that Si vacancy is the main contributor to the generation of BBE, based on which a potential reaction pathway is rationally proposed. Furthermore, the CoSi alloy maintains high stability and also exhibits high activity in the selective oxidation of various alcohols with different functional groups. This work demonstrates for the first time that semimetallic CoSi alloys can be robust catalysts for the green oxidation of various alcohols and proviedes a vast opportunity for the rational design and application of other semimetal alloy catalysts.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2021
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IF 2.694
Aocong Guan,Yucong Nie,Yue Shen,Sile Shi,Weiping Luo
In this study, the solubility of phthalic acid and o-toluic acid in propionic acid, N-methylformamide, N,N-dimethylformamide (DMF), N,N-dimethylacetamide (DMAC), dimethyl sulfoxide (DMSO), N-methylpyrrolidone (NMP), and acetonitrile are measured under atmospheric pressure (101.3 kPa) by the method of laser dynamics. The experimental temperature range is 286.35 to 338.75 K. The measured data shows that the solubility of phthalic acid and o-toluic acid increases with increasing temperature in the temperature range studied. The experimental data are correlated by the Apelblat model, the λh model, and the modified nonrandom two liquid activity coefficient model, and the calculated solubility is in agreement satisfactorily with the measured results. Akaike information criterion analysis results show that the Apelblat model was the most suitable model to correlate the solubility of phthalic acid in propionic acid, N-methylformamide, and DMSO and the solubility of o-toluic acid in propionic acid, DMSO, and NMP; the λh model was the most suitable model to correlate the solubility of phthalic acid in DMF and DMAC and the solubility of o-toluic acid in N-methylformamide and DMF; and the modified NRTL model was the most suitable model to correlate the solubility of phthalic acid in NMP and acetonitrile and the solubility of o-toluic acid in DMAC and acetonitrile.
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高影响因子
TALANTA
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2020
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IF 5.339
Qi Zhou,Xuelin Dong,Binbin Zhang,Shan Lu,Xinwei Zhang,Qin Wang,Yonggui Liao,Yajiang Yang,Hong Wang
The luminescent terbium (Tb 3+ )-loaded supramolecular gels were facilely prepared through the self-assembly of Fmoc-diphenylalanine (FmocPhePhe) at room temperature . Hydroxybenzoic acid (HA, the isomers are denoted as 2-HA, 3-HA, and 4-HA depending upon the positions of hydroxyl groups) was used as a sensitizer to Tb 3+ . The luminescence sensitization of Tb 3+ in the gels was realized by the coordination with hydroxybenzoic acids. The spectra of luminescence, UV–vis, FT-IR, and 1 H NMR verified that this sensitization was attributed to the energy transfer from hydroxybenzoic acids to Tb 3+ . The results of XRD, SEM, and phase transfer temperature further indicated that the initial molecule arrangement of the gels was significantly changed by 2-HA, resulting in more ordered and more compact morphology of the gels. 2-HA exhibited more effective sensitization to Tb 3+ in the gels than 3-HA and 4-HA. It was also found that 2-HA did not affect the self-assembly of FmocPhePhe. Due to the effective fluorescence sensitization by 2-HA, the as-prepared gels can be used for salicylic acid sensing with 6.8 μM of the detection limit. This strategy has been successfully used for the detection of salicylates in pharmaceuticals and cosmetics.
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Qiang Zhang,Xiangyue Wei,Chengfeng Shen,Pengbo Ye,Wenli An,Xuehui Liu,Shimei Xu,Yu-Zhong Wang
Upcycling of polyethylene into useful chemicals is highly demanding, yet challenging to address the waste plastic issue. New approaches are needed in a more cost-effective and energy-efficient way. Here, tandem oxidative degradation of polyethylene into functional chemicals was achieved with a carbon yield of up to 94.6%. This process relies on the oxidation of xylene in the presence of oxygen, generating a radical to induce the oxidation of polyethylene. It enables high-efficiency degradation of polyethylene despite using a non-noble-metal catalyst and a low reaction temperature of 120 °C. The methyl group and its location in xylene play key roles in degradation efficiency and product composition. The oxidation products show good adhesion and film-forming property as well as a recyclable emulsification/demulsification performance depending on the oxidation degree. The versatility of degradation products containing carbonyl and carboxyl groups offers many thrilling options for transforming waste PE into other diverse materials for circular recycling.
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高影响因子
危险品化学品经营许可证（带存储）