MICROPOROUS AND MESOPOROUS MATERIALS
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2023
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IF 5.2
Hongmei Yang,Menglu Xu,Lili Zhang,Weiwei Fang,E. Liu,Huaxin Zhang
A benzotrizole-based hyper-crosslinked polymer (HCP) was employed to load cobalt and prepare a novel metal-containing nitrogen-doped carbon catalyst for the selective hydrogenation of quinoline . The high porosity, large surface area and nitrogen-containing monomer of HCP made a positive contribution to metal loading. Owing to the excellent thermostability of HCP, the original porous texture of HCP was partially reserved during pyrolysis , which resulted in highly dispersive Co species in the N-doped carbon material. The remaining mesopores in Co@CN catalyst during thermal decomposition provided available diffusion channels for substrates, which facilitated their full contact with catalytic active sites and their effective conversion. The prepared Co@CN catalyst achieved a conversion rate of 100% and a selectivity of 100% in the hydrogenation of quinoline into 1, 2, 3, 4-tetra-hydroquinoline in water at 100 °C under 3 MPa H 2 . The as-synthesized catalyst had good reuse performance, exhibiting >95% conversion rate and >99% selectivity even after 12 cycles. Moreover, the catalyst could also be applied to the selective hydrogenation of a serial of quinoline derivatives. The study provided a useful strategy for constructing metal-doped carbon materials which might be applicable for other metals and other reactions.
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JOURNAL OF MOLECULAR STRUCTURE
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2023
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IF 3.8
Yuxiu Fu,Xiaoli Song,Yaming Pang,Yinan Zheng,Liguo Gao
In this paper, a green solvent [BMIM] [PF 6 ] ionic liquid was selected for the extraction and separation of quinoline from simulated wash oil. The effects of extraction temperature, extraction time, and solvent oil ratio on the extraction of quinoline from wash oil were studied. The optimal process parameters were obtained by changing single factor conditions and optimizing the experiment using response surface methodology. When the temperature is 71 ℃, the time is 60 min, and the solvent oil ratio is 3:5, the extraction efficiency can reach 67%. The ionic liquids were recovered and their properties were investigated by infrared spectroscopy. The mechanism of quinoline extraction by ionic liquids was analyzed using infrared spectroscopy and GROMACS kinetic simulation calculations.
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CARBOHYDRATE RESEARCH
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2022
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IF 2.975
Huifang Ren,Xiao-Yang Yue,Wen-Sheng Dong
We propose a new approach for the synergistically catalytic conversion of cellulose to levulinic acid (LA) in water by SO 3 H-functionalized ionic liquid (SFIL) and lanthanide chloride (LnCl 3 ). Compared with using 1-methyl-3-(3-sulfopropyl)imidazolium chloride ([MIMPS]Cl) only, the LA yield using [MIMPS]Cl and ErCl 3 increased by 14.4% and 13.6% at 50 mol% of IL and 30 mol% of IL, respectively. Moreover, the combined [MIMPS]Cl and ErCl 3 system can tolerate high concentrations of substrates and maintain high activity at eleven runs. We also investigated the effects of the cation structure of ionic liquids (alkyl chain length, hydroxyl groups on the side chains, and aromatic properties) on LA production. The observations can provide useful information for designing efficient ionic liquid catalysts for biomass utilization.
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PubMed
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JOURNAL OF CATALYSIS
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2022
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IF 8.047
Feiying Tang,Guangji Zhang,Liqiang Wang,Jianhan Huang,You-Nian Liu
Engineering unsymmetrical coordination is an efficient strategy for improving the performance of carbon supported single-atom catalysts for diverse applications. However, the exploration of this strategy to prepare carbon supported single-atom catalysts for hydrogenation reaction is still in infancy, especially for hydrogenation of quinolines. Herein, we report a protein-metal-ion-network strategy for preparation of single-atom cobalt supported on hierarchically porous carbon (SA-Co/NSPC). SA-Co/NSPC features unsymmetrically N/S-coordinated metal center, i.e., Co 1 –N 3 S 1 . Moreover, the carbon matrices possess an ultra-thin two-dimensional morphology and hierarchically porous structures. SA-Co/NSPC catalyst with Co 1 –N 3 S 1 active site exhibits excellent catalytic performance for hydrogenation of N-heterocycles. The DFT calculation results show that the site of Co 1 –N 3 S 1 reveals a significant electron redistribution in comparison to the Co 1 –N 4 , leading to a lower H* diffusion barrier and quinoline hydrogenation reaction barrier. SA-Co/NSPC catalyst combined with the unique hierarchically porous structure and high active Co 1 –N 3 S 1 owns extraordinary catalytic performance for hydrogenation of quinolines.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Bihan Sun,Houfen Li,Qian Wei,Shuai Xue,Aijuan Zhou,Xiuping Yue
Quinoline is a kind of organic pollutant difficult to be biodegraded, for which the photocatalysis technology is a commonly used removal method, but the degradation performance still needs to be improved. In this work, the WO 3 -CuFe 2 O 4 Z-scheme system was constructed, and the persulfate (PS)-assisted photocatalytic degradation of quinoline with WO 3 -CuFe 2 O 4 by adding persulfate in the photocatalytic systems was studied. The effects of different systems and key parameters such as catalyst dosage, PS concentration and initial pH value on the degradation efficiency of quinoline were investigated. With the addition of persulfate, the degradation efficiency of quinoline increased from 24.3% to 100% in 150 min, under the condition of [PS] = 3 mmol/L, [catalyst] = 3 g/L, temperature = 25 ± 2 °C, and pH = 9. And the WO 3 -CuFe 2 O 4 catalyst showed excellent reusability according to the result of 5-cycle repeated experiment. The possible degradation mechanism was studied by the quenching test and the identification of intermediates and products, which indicated the degradation of quinoline in WO 3 -CuFe 2 O 4 /VIS/PS system was realized via denitrification, dehydrogenation, hydroxylation and ring breaking processes.
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ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Xinlei Ding,Yun Chen,Junping Nan,Hengwei Dai,Yuling Wang,Guangmei Bai,Wenge Qiu
N-doped nestlike carbon nanosheets (NCNs-Nx) were prepared successfully by a two-step strategy, namely, the in situ self-assembly hydrothermal synthesis using glucose as the carbon source in the presence of magnesium nitrate and sodium carbonate and the controlled nitrogen doping carbonization using urea as the nitrogen source. The performance of the corresponding Pd/NCNs-Nx catalysts was investigated for the selective hydrogenation of quinolines. The characterization of transmission electron microscopy, nitrogen sorption isotherm measurement, powder X-ray diffraction, X-ray photoelectron spectra, temperature-programmed desorption of pyridine and benzene, and the pyridine adsorption experiments showed that the very high catalytic activities and selectivity of the Pd/NCNs-Nx catalysts were related with the high Pd dispersion and the electronic structure of Pd species as well as the adsorption capacity and the adsorption type of quinoline molecule on the catalyst surface.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Wenjin Sun,Ruizhen Li,Weifeng Liu,Xuguang Liu
Quinoline, as a refractory and toxic organic pollutant in coking wastewater, causes great harm to the environment and human health even in trace amount. To realize the selective and sensitive detection of quinoline in coking wastewater, a novel molecularly imprinted fluorescent nanopomegranate with carbon dots (CDs) as seeds and fluorescence source (CD-MIP) was prepared, using quinoline as the template, and N-(β-aminoethyl)-γ-aminopropyl trimethoxysilane (KH792) as the monomer. The preparation and detection conditions of CD-MIP were systematically optimized. The structure and detection performance of CD-MIP were investigated in detail. The resulting CD-MIP exhibits excellent photoluminescence performance, high detection sensitivity, good selectivity and reproducibility towards quinoline. Under the optimized conditions, the fluorescence intensity of CD-MIP shows a satisfying linearity with quinoline concentration in the range of 20–200 mg/L with a detection limit of 6.7 mg/L. Owing to the existence of imprinted cavities that highly match with quinoline, a high imprinting factor (3.46) for CD-MIP was obtained. In addition, CD-MIP represents a greater affinity towards quinoline than towards other analogues, as well as an outstanding anti-interference capability. For trace analysis in real coking wastewater, CD-MIP also gives satisfactory results. Therefore, CD-MIP shows promising application in the selective detection of trace quinoline in wastewater.
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TALANTA
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2022
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IF 6.556
Mingxing Liu,Rongrong Jiang,Meie Zheng,Mengjiao Li,Qingjie Yu,Hongda Zhu,Huiling Guo,Hongmei Sun
A sensitive unlabeled ratiometric biosensor was developed to the detection of cardiac troponin I (cTnI). This biosensor was established by using the glassy carbon electrode coated with graphene oxide to form a platform bonded with N, Zn co-doped graphene quantum dots (N, Zn-GQDs). The N, Zn-GQDs was successfully prepared as the raw materials of graphite powder and characterized. Antibodies of cTnI were bonded to the surface of N, Zn-GQDs as the nanoprobe by amide bonds. The signals of electrochemiluminescence (ECL) and differential pulse voltammetry (DPV) were exposed to decrease in the presence of cTnI, which caused the signal substance to move farther away from the electrode. It was found that the immune complex layer attenuated the intensity of ECL and DPV which could be used as the good overall signal for determining concentration of cTnI. The ratiometric biosensor had a good response to cTnI with the detection limit is 4.59 pg L −1 in the concentration range of 10–10 6 pg L −1 . The developed method was evaluated for the detection of cTnI in human serum, and the obtained results were consistent compared to the reference values obtained by hospital standard enzyme linked immunoassay (ELISA) with 9.09%–11.1% of RSD. Our findings suggested that this ratiometric biosensor could be used to the detection of cTnI in human serum with lower cost and higher sensitivity, it also might be better potential application prospect based on N, Zn-GQDs to detect other biomarkers.
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PubMed
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Molecular Catalysis
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2022
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IF 5.089
Kuan Wang,Zhe Cao,Junlei Wang,Zhen-Hong He,Dan Wang,Rong-Rong Zhang,Weitao Wang,Yang Yang,Zhao-Tie Liu
The development of non-precious metal catalysts in heterogeneous catalytic processes is of great importance to the hydrogenation of quinolines for both theoretical and industrial applications. Herein, an effective non-precious metal catalyst, 58% Fe 4 Ni 6 Cu 5 /MCM-41, was developed to catalyze the hydrogenation of quinolines under the green and mild conditions, which can achieve 97.5% conversion and exceeding 98% selectivity to tetrahydroquinoline in solvent-free at low temperature of 50 °C. Moreover, the acceptable results of the reusability and gram scale-up experiments proved an industrial application potential of the as-prepared catalyst. Meanwhile, in cyclohexane system, 58% Fe 4 Ni 6 Cu 5 /MCM-41 catalyst can further realize a higher activity of the hydrogenation at a lower temperature of 40 °C, achieving 98.2% conversion and 98% selectivity to tetrahydroquinoline. The existence of Fe-Ni and Ni-Cu alloys in Fe 4 Ni 6 Cu 5 /MCM-41 catalyst was demonstrated by TEM, XRD, XPS, H 2 -TPD, and Raman spectroscopy. And, Fe-Ni and Ni-Cu alloys can be well dispersed onto MCM-41 molecular sieves. For Fe 4 Ni 6 Cu 5 /MCM-41 catalyst, quinoline molecules can be adsorbed by Fe 3+ species on the surface of Fe-Ni alloy through the coordination, while hydrogen molecules can be adsorbed and activated by Ni-Cu alloy. Under the synergism of Fe-Ni and Ni-Cu alloys, the highly effective and selective hydrogenation of quinolines was achieved at low temperature and in solvent-free system. The present approach offers a prospective idea for building non-precious metal catalysts to realize the effective hydrogenation of N-heterocyclic compounds under mild conditions.
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FUEL
·
2022
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IF 8.035
Zidan Zou,Chun Chen,Zhi Hu,Yue Shen,Zhen Fu,Wenchao Li,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
Silica is one of the most referenced materials for the preparation of heterogeneous metal catalysts. However, silica spheres with smooth surfaces have difficulty encapsulating active metals due to their small surface area and the presence of only a handful of silicon hydroxyl groups on the surface. In this work, the silica sphere has been first consciously transformed into a hierarchical SiO 2 @silicate structure, and then the core–shell hetero-structured SiO 2 @Ni/SiO 2 catalyst can be tactfully obtained by reducing treatment. The core–shell catalyst is composed of a rigid core (SiO 2 ) and a rough shell (Ni NPs highly disperse on nanosheet SiO 2 ), which are carefully verified by X-ray diffraction (XRD), transmission electron microscope (TEM), field scanning electron microscope (FESEM), H 2 -TPR/TPD and X-ray photoelectron spectroscopy (XPS). The derived SiO 2 @Ni/SiO 2 catalyst can selectively hydrogenate vanillin in the aqueous phase at near-room temperature (40 ℃) and low hydrogen pressure (2 MPa H 2 ), and the conversion of vanillin can be up to 99%. The preparation method of the SiO 2 @Ni/SiO 2 catalyst is simple and can be amplified to a large scale at a low price, thus can be adopted to convert bio-derived unsaturated compounds in an economical and eco-friendly way.
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Arabian Journal of Chemistry
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2023
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IF 6
Lan Yi,Xiaoqin Wu,Shuguang Ouyang,Li Guo,Jialing Chen,Mario Gauthier,Wen-Ying Li
The extraction of indole from wash oil is of economic value and practical significance. In this study, deep eutectic solvents (DESs) are investigated to extract indole from wash oil. Initially, density functional theory calculations were used to explore the association of indole with aromatic compounds in wash oil, and the feasibility of indole extraction with a tetraethylammonium chloride/ p -toluenesulfonic acid (TEAC/2TsOH) DES. Then, the influence of the temperature, stirring time, DESs dose, initial indole concentration, and amount of water added were investigated, followed by discussions on the comparison with other extractants and the performance of extracting of indole from real wash oil. The results show that indole associates with aromatic compounds in wash oil through π−π interactions, but that a large electrostatic interaction energy of −52.8 kJ/mol between indole and the DESs is the main driving force for the extraction process. Under optimal conditions, TEAC/2TsOH extracts more than 63.5 ± 3% of indole from wash oil, and its extraction capacity is superior to other extractants.
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FUEL
·
2023
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IF 7.4
Wenbin Huang,Qiang Wei,Haoran Liu,Han Yang,Zhen Xu,Zhengyu Chen,Dongdong Chen,Yasong Zhou
The reason for high-difficulty nitrogen removal of aromatic N-heterocyclic compounds in petroleum fractions was investigated from the main thought of “NiWS property - Reaction behavior - DFT calculation”. The properties of the used catalyst were characterized by a series of techniques with the aim of providing the basis for model construction in the DFT calculations. The kinetic experiments in fixed-bed reactor revealed that although 1,2,3,4-tetrahydroquinoline (THQ1) and decahydroquinoline (DHQ), o-ethylaniline (OEA) exhibited relatively high yields in the HDN reaction of quinoline and indole respectively, they were all able to show high conversions and HDN rates when reacted as feedstocks alone. The study of product normalizations in the reaction system of the mixed feedstocks demonstrated that the difficulty of conversion of THQ1 and DHQ in quinoline HDN was mainly due to the inhibition effect of quinoline feedstock. While in the HDN of indole, the presence of the intermediate product OEA was the main factor for the low conversion of indole. This phenomenon of inhibition originating from within the molecular reaction network was proposed as N-N self-inhibition effect for the first time. The DFT calculations suggested that the inhibition of quinoline on THQ1 could be attributed to the adsorption advantage of quinoline, while the inhibition on DHQ was mainly due to the steric hindrance effect of DHQ itself. And the inhibition effect of OEA on indole can be mainly attributed to its greater nucleophilicity and stronger adsorption ability on the active sites compared with IND.
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