LANGMUIR
·
2026
·
IF 4.4
Zhipeng Su,Xueyin Zhang,Haiwei Li,Pingchuan Sun,Tiehong Chen
Desilication by alkali etching is generally used to prepare hierarchical zeolites to enhance their mass transfer properties; however, for high Si/Al ratio zeolites, the alkali etching would greatly reduce the framework crystallinity or even give rise to amorphous product. Though organic amines have been used as additives during alkali etching to protect the microporous framework, the problems of toxicity, volatility, high cost, and nitrogen-containing wastes induced by organic amines would hinder their scalable application. In this study, we provide a different viewpoint on the protective mechanism of zeolite micropores during alkali etching, and the attention is focused on the framework polarity, which has not been studied before. We develop a hydrophobic nitrogen-free organic molecule (such as acetophenone)-protected alkali etching method to prepare hierarchical zeolites with high crystallinity and high porosity, and the prepared hierarchical Y zeolites showed enhanced performance in the catalytic cracking of bulky molecules. This method is based on the principle that the hydrophobic micropores of high-silica zeolites could adsorb hydrophobic organic molecules from aqueous solution, which would fill in the zeolite micropores and prevent excessive OH– damage to Si–O–Si bonds. Thus, our method is facile for scalable production without the tedious pretreatment of vacuum dehydration, organic amine impregnation, and drying before alkali etching. Furthermore, concerning the characteristics of a nitrogen-free process and low volatility, using acetophenone as a protective agent would reduce the cost and avoid nitrogen-containing wastes in practical applications.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Jingwei Cao,Hongyue Guo,Qingsong Li
Ternary liquid–liquid phase equilibrium (LLE) data of water + 3-pentanone + extractants (methyl tert-butyl ether, 2-ethyl-1-hexanol, o-xylene, ethyl acetate) were measured to separate 3-pentanone of high purity from aqueous solutions at 308.2 K under 101.3 kPa. The ability to extract 3-pentanone from aqueous solutions was assessed by distribution coefficient (D) and separation factor (S). Hand and Bachman equations tested the reliability of the experimental data with linear coefficients (R2) not less than 0.99. Meanwhile, UNIQUAC and NRTL thermodynamic models regressed experimentally measured data to get the optimal binary interaction parameters, and the root mean square deviation (RMSD) was not more than 0.4%. The GUI-MATLAB program verified the consistency of binary parameters obtained from the NRTL model well.
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ORGANOMETALLICS
·
2023
·
IF 2.8
Yanru Zhang,Jingjing Zhang,Ying Wang,Yang Li,Jun He,Yanyan Wang,Longbo Zhang,Zhenpeng Wang,Qingli Qian,Buxing Han
Synthesis of basic C2+ chemicals using CO2 and H2 is very promising. Herein, we present a protocol for the synthesis of different carboxylic acids by the reaction of ketones or aldehydes with CO2 and H2. The catalytic system consisted of the IrCl3 catalyst, LiI promoter, and acetic acid solvent. The yield can reach 52.9% based on the cyclohexanone substrate which can be derived from biomass. Various Cn ketones and aldehydes could be used as a substrate in the reaction, where the corresponding Cn+1 carboxylic acids were obtained. According to the mechanistic study, the reaction involved substrate conversion, reverse water–gas shift (RWGS) reaction, and carbonylation. This strategy provides an optional way of carboxylic acid production and CO2 utilization.
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FUEL
·
2023
·
IF 7.4
Yuan Zhang,Yongshuai Wang,Hongyou Cui,Fang Wang,Zhihe Li,Changhua Sun,Yun Jia,Yujiao Xie,Feng Song,Jiangang Wang,Weiming Yi
Co-pyrolysis of biomass with Red Mud was used to boost up the quality of the produced bio-oil and recover iron from Red Mud. The influences of five different biomass species and impregnation pretreatment were investigated. It was found that co-pyrolysis could significantly improve the bio-oil quality, decreasing the acidity from 173.28 to 1.18 mg KOH/g due to the decarboxylation of carboxylic acids into ketones under the catalysis of Red Mud and boosting up the HHV from 20.05 to 31.80 MJ/kg with an energy efficiency of 72.56%. Meanwhile, the soluble alkalinity of Red Mud declined from 65.34 to 5.26 mg HCl/g, which is very crucial to mitigate the harmfulness and perniciousness to the environment. The characterizations of XRD, 57 Fe Mössbauer spectroscopy and XPS confirmed that the weak magnetic Fe 2 O 3 and FeOOH in Red Mud could be completely transformed into stronger magnetic Fe 3 O 4 . For this reason, the magnetic separation iron recovery reached up to 92.25% with iron grade of 66.12%. The findings in the research not only open the avenue for efficient biomass conversion to high quality fuels, but also provide an efficient approach to resourceful utilization of Red Mud.
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ChemCatChem
·
2023
·Vol. 15
·期 21
·e202300852
·
IF 4.5
Mengyang Liu,Bin Gu,Jingmei Li,Huangzhao Wei,Weiyang Xue,Yukun Jiang,Chenglin Sun
Graphical Benefiting from the synergistic effect of supported bimetallic CeFe which induces higher metal dispersion and higher content of reactive oxygen, and the buffering effect of resin-derived-carbon on free radicals, the aerobic oxidation of cyclohexanone to ϵ-caprolactone (ϵ-CL) is performed over CeFe@RDC-x, and the catalytic efficiency is significantly improved. Especially, when solvent-free and green solvents (such as ethyl acetate) are used, excellent catalytic conversion effects are achieved. Upgrading cyclohexanone to ϵ-caprolactone (ϵ-CL) is of great importance to the synthesis of high value-added downstream chemicals and the reduction of foam plastic. The catalytic synthesis of ϵ-CL from cyclohexanone through O 2 /aldehyde method is an environmentally benign one-pot tandem reaction without using peroxy acid, balancing the requirements of safety and efficiency. However, due to lack of elaborate design and collaboration of multiple active sites for catalysts, the catalytic efficiency of O 2 /aldehyde method still remains to be improved. Herein, a pitaya-like catalyst (CeFe@RDC-3) with Ce and Fe highly dispersed on resin-derived-carbon is synthesized through high temperature self-assembly. On this bimetallic catalyst, high yield (97 %) of ϵ-CL is achieved through aerobic oxidation of cyclohexanone with only 1.5 equivalent benzaldehyde. Moreover, considerable yields of ϵ-CL, 88.3 % and 74.7 %, respectively, are also obtained over CeFe@RDC-3 with green solvent (EtOAc) or even without solvent. No loss of activity is observed after five successive cycles, demonstrating high stability of CeFe@RDC-3. The mechanism study reveals that the high performance of CeFe@RDC-3 is ascribed to the Ce−Fe bimetallic synergy, uniform metal dispersion, abundant active oxygen and stabilizing effect of resin-derived-carbon to free radicals. This work provides prospect for a green, safe and low-cost strategy for Baeyer-Villiger process.
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RENEWABLE ENERGY
·
2022
·
IF 8.634
Shanshan Shao,Pengfei Zhang,Xianliang Xiang,Xiaohua Li,Huiyan Zhang
Ketonization of bagasse pyrolysis gas was performed over red mud-based oxides. The maximum yield of ketones in the catalytic conversion of bagasse pyrolysis gas over original red mud was 18.66% at 420 °C. To promote the oxidability of red mud and obtain a higher yield of ketones, the effect of metal oxides (CeO 2 , MnO 2 , TiO 2 , CaO, ZrO 2 ) loading and loading amount of CeO 2 on red mud on ketonization of bagasse pyrolysis gas were studied. The highest yield of ketones of 27.86% was obtained over red mud-based oxides with 40 wt% CeO 2 loading. The oxidability of the catalyst was enhanced greatly by the high loading of CeO 2 , leading to the peroxidation of acetone as the side reaction. To control the oxidability and cut costs, bimetallic oxides were loaded on red mud. The yield of ketones reached 30.12% over the composite red mud catalyst with the loading of 20 wt% CeO 2 and 20 wt% MnO 2 . The rough coating of MnO 2 on the surface of red mud was beneficial to the loading of CeO 2 , resulting in smaller and more uniform grains. This study provides the efficient utilization of red mud and biomass as solid wastes for high-valued chemicals and fuels.
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Analytical Methods
·
2021
·Vol. 13
·期 26
·2989-2996
·
IF 2.896
Yiwen Cao,Shenjie Zhu,Lin Zhang,Qun Cui,Haiyan Wang
Aiming at the difficulty in qualitative and quantitative analysis of trace compositions in food preservative propionic acid, the trace compositions and the key components influencing the total aldehyde content in propionic acid were analyzed by gas chromatography-mass spectrometry (GC-MS), high performance liquid chromatography (HPLC) and gas chromatography (GC) in this paper. The results show that the food preservative propionic acid contains 18 trace compositions. The main compositions affecting the total aldehyde content in propionic acid are acetaldehyde, propionaldehyde, 1-cyclopropyl-1-propanone and 2-methyl-2-pentenal, which account for ∼90% of the total aldehyde content in propionic acid. The total aldehyde content in propionic acid can be quickly determined by iodometric titration. However, the impurity compositions, solution oxygen content and pH value of propionic acid may affect the stability of NaHSO3, which lead to a higher titration value of the aldehyde content. The total aldehyde contents in propionic acid determined by GC (148.535–337.890 mg L−1) and HPLC (157.730–335.780 mg L−1) are close and reliable with a relative deviation of 0.31–3.00%. The volatile low-carbon aldehydes and ketones including formaldehyde, acetaldehyde and acetone have a weak response and a high detection limit in GC. The derivation conditions of all aldehydes and ketones in propionic acid should affect the determination results of HPLC. It provides the basic data for quality improvement and ultra-deep purification of food-grade propionic acid.
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TALANTA
·
2020
·
IF 5.339
Xue Li,Yuan-Yuan Cui,Cheng-Xiong Yang
Microporous organic networks (MONs) have shown great promise in separation science recently. Exploring novel, simple and convenient strategy to fabricate MONs coated capillary columns for gas chromatography (GC) still remains challenging but desirable for the development of MONs in chromatographic separation. To extend the potential application of MONs in separation science and to further develop novel method for the fabrication of MONs-based capillary columns, here we demonstrate a novel covalent coupling strategy to fabricate uniform MONs bonded capillary columns for GC separation of position isomers and hydrocarbons. The bare capillary column was firstly modified with (3-bromopropyl)trimethoxysilane to provide bromine sites for coupling with alkynyl monomers . The amino- and hydroxyl-functionalized MONs (MON-NH 2 and MON-OH) were then directly grown onto the inner wall of the brominated capillary columns via the covalent coupling between bromine and alkynyl groups. The uniform MON-NH 2 and MON-OH bonded capillary columns were obtained and showed good resolution for GC separation of dichlorobenzene , chlorotoluene, bromotoluene, and propylbenzene position isomers and many other hydrocarbons including linear alkanes, alkylbenzenes , pinene isomers, cyclohexane and benzene, ketones and aldehydes. The MONs bonded capillary columns also owned good lifetime and precision for dichlorobenzene isomers with the relative standard deviations (RSDs) of 0.2–0.3%, 1.2–2.1%, and 1.7–2.5% for retention time, peak height and peak area, respectively. In addition, the fabricated MON-NH 2 and MON-OH bonded capillary columns offered better resolution than commercial InertCap-1, InertCap-5, InertCap-1701 and InertCap-WAX capillary columns for the separation of chlorotoluene and bromotoluene position isomers. These results revealed the feasibility of covalent coupling strategy to fabricate MONs-based stationary phases in GC, highlighting the potential of MONs in separation science.
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E-POLYMERS
·
2020
·Vol. 20
·期 1
·214-225
·
IF 1.675
Wan-Xia Wu
A novel full bio-based ketone-containing aliphatic polyester was prepared by enzyme-catalyzed polycondensation of diethyl γ-ketopimelate (DEK) with 1,6-hexanediol (HDO) using immobilized lipase B from Candida antarctica (CALB). The influences of polymerization conditions such as temperature, time, enzyme amount, and solvent amount on the molecular weight of poly(hexamethylene γ-ketopimelate) (PHK) were investigated. New fully bio-based poly(hexamethylene γ-ketopimelate- co -hexamethylene adipate) (poly(HK- co -HA)) copolymers with narrow polydispersity and well-defined composition were synthesized by copolymerization of DEK, HDO, and diethyl adipate. The structures of PHK and poly(HK- co -HA) copolymers were characterized by nuclear magnetic resonance, and their thermal characterization was examined by thermogravimetric analysis and differential scanning calorimetry. The degradation of PHK and poly(HK- co -HA) copolymers was studied. The post-polymerization modification of these polyketoesters via oxime click chemistry was further demonstrated. Graphical
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FOOD CHEMISTRY
·
2019
·
IF 5.399
Hui Shen,Mingquan Huang,Mouming Zhao,Weizheng Sun
Typical ketone flavours (with variations in chain length, position and number of keto group, branched chain) were selected to investigate the effect of molecule structure of ketones on their interactions with myofibrillar proteins (MPs). Results showed that 2,3-pentanedione quenched the fluorescence of MPs more effectively than 2-pentanone and 3-pentanone due to the number of keto group. There was no significant difference between 5-methyl-2-hexanone and 2-heptanone, which was attributed to their similar molecular size and polarity. The quenching effect of homologous ketone flavours increased with carbon chain growth due to the higher hydrophobic interaction. Dynamic quenching played a major role in the fluorescence quenching process of MPs by 2-pentanone, 3-pentanone, 5-methyl-2-hexanone, 2-heptanone and 2-octanone. The α-helix content decreased gradually with the increase of ketones concentration. Results of GC/MS were in accordance with the fluorescence quenching analysis generally, whereas 2,3-pentanedione and 2-nonanone exhibited some differences due to their higher steric hindrance effects.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Zhao Yang,Wenhan Chen,Jinbao Zheng,Zhiqing Yang,Nuowei Zhang,Chuan-Jian Zhong,Bing Hui Chen
Carbon supported Pt-Ru nano-alloy with multiple reactive sites exhibits unprecedentedly efficient performance in acetone hydrogenation at room temperature. Catalytic properties can be controllably regulated and optimized via performing the specific annealing treatment for the catalyst. The essential correlation between the variations in catalyst’s annealing conditions and the resultant variation in catalytic properties has been explored and discussed as a structure-function relationship. The combination of Pt and Ru sites exhibits enhanced catalytic activity compared with monometallic ones. Larger PtRu alloy particle size favors the rapid C O hydrogenation and the improvement of catalytic selectivity to isopropanol. Isopropyl ether generation is related to the Pt defect sites on the surface, which can be blocked though the catalyst’s oxidation treatment . The presence of surface metal-oxide species is beneficial to the performance enhancement, resulting from the synergetic behavior between metal-oxide sites and metallic sites on respectively activating the reactants. Moreover, 3-pentanone is used as a probe molecule to verify the structure-function relationship of catalytic low-temperature C O hydrogenation on PtRu/C.
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ANALYST
·
2015
·Vol. 140
·期 9
·3107-3112
·
IF 4.107
Ye-Yu Wu,Cheng-Xiong Yang,Xiu-Ping Yan
The unique properties of metal–organic frameworks, such as diversity in structures and pore sizes, high surface area, shape selectivity and available to functionality make them as potential materials of the stationary phase for gas chromatography. Here we show an in situ growth approach to the fabrication of zeolite imidazolate framework-90 (ZIF-90) bonded capillary column for gas chromatography separation. ZIF-90 was directly grown onto the inner wall of the carboxyl modified capillary via the coordination between Zn(II) and carboxyl group. The fabricated ZIF-90 bonded capillary column acted as a weak polar stationary phase. It not only exhibits high capacity in the separation of linear molecules, but also offers excellent features for the separation of 2- and 3-substituted ketones.
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