Catalysis Science & Technology
·
2024
·
IF 4.4
Renjie Deng,Huajie Liu,Haishuai Cui,Yao Tian,Hai Yang
In this work, we have developed a green method for the preparation of para-nitrotoluene through the catalytic nitration of toluene with nitrogen dioxide (NO2) under the promotion of dioxygen (O2). The experimental results reveal that the dealumination of Hβ zeolite has a significant effect on the catalysis of the developed NO2–O2–acetic anhydride (Ac2O) system, in which the conversion of toluene is 78.1% and the selectivity to para-nitrotoluene is 71.8%. Furthermore, the nature of different dealuminated catalysts was investigated by nitrogen adsorption–desorption analysis, X-ray diffraction (XRD), Fourier-transform infrared (FT-IR), thermal gravimetric analysis (TGA), inductively coupled plasma (ICP), ammonia temperature-programmed desorption (NH3-TPD), pyridine adsorbed Fourier-transform infrared (Py-FT-IR), scanning electron microscopy (SEM) and 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR) techniques. The results of characterization indicate that the structure of the Hβ zeolite still remains and that of Al species in the extra-framework is preferentially removed after acid treatment. Based on the combined results of catalytic characterization and DFT calculation, a feasible reaction mechanism of improved para-selectivity in toluene nitration was suggested for the NO2–O2–Ac2O system.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 48
·e03981
·
IF 2
Huajie Liu,Hao Fan,Cao Botao,Tingying Guo,Fangfang Zhao,Yong Wang,Renjie Deng
In this study, we have successfully developed an environmentally benign methodology for synthesizing para -nitrotoluene ( p -NT) via catalytic nitration of toluene using nitrogen dioxide (NO 2 ) as the nitrating agent, with molecular oxygen (O 2 ) serving as an efficient promoter in the reaction system. The experimental results demonstrate that the Hβ zeolite-supported Lewis acid catalyst (AlCl 3 ) exhibits remarkable catalytic performance in the developed NO 2 –O 2 –Ac 2 O system, achieving a toluene conversion of 78.5% with a p -NT selectivity of 62.5%. To elucidate the structure–activity relationship, the physicochemical properties of various catalysts were systematically characterized using multiple analytical techniques, including nitrogen physisorption (BET), x-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), temperature-programmed desorption of ammonia (NH 3 -TPD), and scanning electron microscopy (SEM). On the basis of comprehensive catalytic characterization and density-functional theory (DFT) calculations, we propose a plausible reaction mechanism that accounts for the enhanced para -selectivity in the toluene nitration process within the NO 2 –O 2 –Ac 2 O catalytic system.
研究领域:
催化化学
·
绿色化学
·
有机合成
·
材料科学
·
环境化学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Nan Li,Zhi Wang,Jixiao Wang
Carbonic anhydrase (CA)-inspired membranes for CO 2 separation were constructed by introducing hydroxypropyl-β-cyclodextrins (Hβ-CDs) into the polyamide networks, which were formed via interfacial polymerization reactions between trimesoyl chloride and tertiary amino-containing monomers . Hydrophobic inner cavities of Hβ-CDs with the hydrophilic exterior can be used to simulate the hydrophobic pockets of CA enzymes. Hydrophilic and hydrophobic regions were constructed via introducing Hβ-CDs into membranes, while the transport of nonpolar CO 2 molecules and polar components (H 2 O and HCO 3 − ) in CO 2 hydration reactions could be enhanced. Meanwhile, tertiary amino groups in biomimetic membranes can act as the base catalysts for CO 2 hydration reactions, which were deemed as carriers for facilitated transport membranes. Biomimetic membranes containing Hβ-CDs and tertiary amino groups exhibited outstanding CO 2 permeance of 2792 GPU and CO 2 /N 2 selectivity of 171 at 0.15 MPa, showing the potentials for low-pressure CO 2 capture. Particularly, CO 2 transport mechanisms were also analyzed for biomimetic facilitated-transport membranes, which can supply new visions for developing novel membrane materials for CO 2 separation.
研究领域:
化学工程
·
材料科学
·
环境科学
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DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 109
·107239-107245
·
IF 3.289
Yuanyuan Wang,Hua Song,Xinglong Sun
Fe2O3 (x)/Hβ catalysts with different Fe2O3 loadings (x) were successfully prepared and characterized by XRD, SEM, TEM, ICP, BET, NH3-TPD and Py-IR. With selective alkylation of toluene with tert-butyl alcohol to produce 4-tert-butyltoluene as a probe reaction, the effects of the different Fe2O3 loadings on channel structures, acidity and catalytic performance over Hβ were studied. The results showed that modification of Hβ with Fe2O3 could adjust pore structures and decrease the total acidity, especially the strong acidity of Hβ. The parent Hβ exhibited the highest toluene conversion of 58.4% with the lowest PTBT selectivity of 67.3%. The low para-selectivity over parent Hβ could be attributed to the low shape-selective action of 12-ring portals of Hβ and the isomerization of the formed PTBT to MTBT. Upon loading of Fe2O3, the toluene conversion of Fe2O3 (x)/Hβ catalysts decreased slightly, but the PTBT selectivity increased significantly. A toluene conversion of 54.7% with PTBT selectivity of 81.5% was observed over Fe2O3 (20%)/Hβ at 190 °C after 4 h. The narrowed pores after loading the Fe2O3 were beneficial to increasing the selectivity to PTBT, since PTBT with a lower kinetic diameter (0.58 nm) can diffuse through the narrowed pores of Fe2O3 (x)/Hβ more easily than MTBT (0.65 nm). In addition, the decrease in number of strong acid sites and deactivation of acid sites on the surface are beneficial to increasing the selectivity to PTBT by suppressing further isomerization of the formed PTBT on acid sites.
研究领域:
催化化学
·
材料化学
·
化学工程
·
有机反应工程
·
多相催化
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Jinyu Huang,Zhuoqian Li,Jingyi Yang,Zhikun Peng,Qiaoyun Liu,Zhongyi Liu
Bifunctional Pd/Hβ catalysts with uniformly distributed palladium nanoparticles (Pd NPs) were successfully synthesized by a facile methanol-mediated weakly capping growth approach (WCGA). A series of Pd/Hβ catalysts with different metal loadings and Si/Al ratios were used for benzene hydroalkylation, and the identification of metal/acid matching balance over bifunctional Pd/Hβ toward benzene hydroalkylation performance was investigated. The obtained characterization and catalytic activity test results demonstrated that the weak acid site and Lewis acid site have greatly affected the benzene conversion, and the strong acid site as well as Brønsted acid site had more of an effect on the alkylation process. The best hydroalkylation performance was achieved by tuning the acid/metal molar ratio at 22.4 μmol of H+/μmol of exposed Pd with a high cyclohexylbenzene (CHB) selectivity of 51.7% at a benzene conversion of 63.4%, which is the best CHB yield currently obtained for all we know. In addition, the stability of Pd/Hβ catalysts was tested and compared with that prepared by the incipient wetness impregnation (IWI) method, which showed good stability, and no obvious particle aggregation was found. This work provides guidance for exploring the construction of bifunctional catalysts and the balance of metal/acid sites.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
Fuels
·
2025
·Vol. 6
·期 4
·89
·
IF 2.8
Zhibing Shen,Ruiyuan Tang,Shengrong Liang,Juntao Zhang,Leyuan Li,Shangli Zhang
The conversion of polycyclic aromatic hydrocarbons (PAHs) to monocyclic aromatic hydrocarbons holds significant importance in the petrochemical and coal chemical industries, as it enables the production of high-value-added chemicals. In this study, we investigated the methane-assisted hydroconversion of PAHs to monocyclic aromatic hydrocarbons with methyl side chains over Zn-based catalysts from Hβ zeolites treated with citric acid (CA) at different concentrations. The CA-modified Hβ catalysts were characterized using X-ray diffraction (XRD), N2adsorption–desorption, pyridine–Fourier transform infrared spectroscopy (Py-FTIR), and ammonia temperature-programmed desorption (NH3-TPD). The results show that low CA concentrations facilitate the removal of amorphous aluminum from the zeolite framework, thereby increasing the specific surface area, pore volume, and pore diameter of the Zn/Hβ catalyst, as well as improving its Lewis/Brønsted (L/B) acid ratio. In contrast, excessive CA treatment causes the undesirable removal of framework aluminum and leads to structural collapse in the mesoporous regions formed at the interfaces between certain crystal aggregates. This, in turn, has a negative impact on the catalyst’s specific surface area, pore volume, pore size distribution, total acidity, and L/B ratio. Experimental data further indicate that the optimal Zn/Hβ catalyst, prepared using Hβ treated with 0.08 M CA, achieves a naphthalene conversion rate of up to 99% and a benzene–toluene–xylene (BTX) selectivity of 60% in the liquid product over a 10 h reaction period. These findings confirm that CA treatment not only enhances the catalytic activity of Zn/Hβ but also significantly improves its operational stability. This work provides new insights into the rational design of catalysts for the efficient conversion of PAHs to monocyclic aromatic hydrocarbons and the utilization of methane resources.
研究领域:
催化化学
·
石油化工
·
煤化工
·
材料科学
·
多相催化
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产品关联
DOI
高影响因子
APPLIED ENERGY
·
2019
·
IF 8.426
Xiaowen Zhang,Yufei Huang,Hongxia Gao,Xiao Luo,Zhiwu Liang,Paitoon Tontiwachwuthikul
The extensive energy penalty of CO 2 -loaded solution regeneration is one of the most crucial challenges facing industrial application of amine-based CO 2 capture technology. Here, to decrease the energy requirement, the regeneration behaviors of the rich 5 M monoethanolamine (MEA) and 3 M MEA-2.5 M N-methyl-diethanolamine (MDEA)−0.5 M piperazine (PZ) tri-solvent blended amines (tri-blend) with four different solid acid catalysts (H-mordenite, Hβ, HZSM-5 and Al 2 O 3 ) were studied at 98 °C. For the catalyst-free tests, the results revealed that the tri-blend hugely enhanced the CO 2 desorption kinetics and reduced the relative energy consumption compared to 5 M MEA. Based on the results of 13 C NMR, the multiple proton transfer paths and abundant bicarbonate ions in the tri-blend contribute to the improved regeneration performance. Additionally, the use of catalyst further improved the CO 2 desorption activity of the tri-blend. The combination of Hβ and tri-blend presented the best regeneration performance, increasing the desorption performance by 1360.8%, and reducing the relative energy requirement by 66.1% compared with the blank run of MEA. In addition, a plausible catalytic mechanism of solvent regeneration over the solid acid catalyst in the tri-blend was suggested. The superior catalytic performance of Hβ resulted from the large mesoporous surface area, larger number of Brϕnsted acid sites and prominent total acid sites. Furthermore, Hβ displayed excellent stability and had no adverse influence on the CO 2 absorption activity. Results herein manifest that the combination of tri-blend amines with high-efficiency catalyst is exceptional strategy for tremendously decreasing the energy consumption of amine-based CO 2 capture processes, ultimately making this technology more technically and economically feasible.
研究领域:
化学工程
·
环境科学
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DOI
高影响因子
RARE METALS
·
2025
·Vol. 44
·期 4
·2379-2392
·
IF 11
Na Guo-Quan,Cui Wen-Gang,Shi Hang-Yan,Li Zheng-Long,Gao Fan,Wang Xing-Qiang,Wang Ke,Gao Yong,Yang Ya-Xiong,Shen Zi-Chao,Pan Hong-Ge
High-capacity LiBH 4 is a promising solid hydrogen storage material. However, the large electron cloud density between the B-H bonds in LiBH 4 induces high dehydrogenation temperatures and sluggish dehydrogenation kinetics. To solve the above problems, it is proposed to enhance the hydrogen storage properties of LiBH 4 through the synergistic effect of Brønsted and Lewis acid in Hβ zeolite. Composite hydrogen storage systems with different mass ratios were prepared by simple ball-milling. At a LiBH 4 -to-Hβ mass ratio of 6:4, the 6LiBH 4 -4Hβ system released hydrogen at 190 °C and achieved a hydrogen release capacity of 7.0 wt% H 2 upon heating to 400 °C. More importantly, the hydrogen release capacity of the system reached 6.02 wt% at 350 °C under isothermal conditions after 100 min and 7.2 wt% at 400 °C under isothermal conditions after 80 min, whereas the pristine LiBH 4 only achieved 2.2 wt%. The improvement in hydrogen storage performance of the system was mainly attributed to two factors: (i) Lewis acid sites with acceptable electrons in the Hβ weaken the electron density of B–H bonds in LiBH 4 , and (ii) the H + proton from the Brønsted acid sites and H − of LiBH 4 undergo a H + + H − = H 2 reaction. Theoretical calculations revealed that the Lewis and Brønsted acid sites in the Hβ zeolite are conducive to the weakening of B – H bonds and that storage charge transfer occurs near the Lewis acid sites. The present work provides new insights into improving the hydrogen storage performance of LiBH 4 by weakening the B–H bonds in the LiBH 4 .
研究领域:
能源存储
·
催化
·
材料科学
·
无机化学
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产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Hao Li,Huimin Liu,Chiliu Cai,Haiyong Wang,Youwang Huang,Song Li,Bin Yang,Chenguang Wang,Yuhe Liao,Longlong Ma
Nowadays, 2-methylfuran is urgently needed especially in pharmaceutical manufacture. However, the direct synthesis of 2-methylfuran via the efficient dehydration and hydrogenation of xylose usually requires a multistep reaction. Herein, a route of tandem conversion xylose to 2-methylfuran was developed. The xylose was firstly converted into furfural by Hβ zeolite, followed by the catalysis of furfural to 2-methylfuran over 0.5NiCu/C. Compared with two-step reaction, cascade strategy applied xylose conversion improved the 2-methylfuran yield rate by 41.5%. In general, this work expanded the application of tandem method for the enhancement of xylose effective conversion and provided a new biomass utilization technology.
研究领域:
化学工程
·
催化
·
生物质转化
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产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Zhensheng Shen,Gewei Zhang,Chengxiang Shi,Juncong Qu,Lun Pan,Zhenfeng Huang,Xiangwen Zhang,Ji-Jun Zou
Synthesis of fuels from lignin bio-oil feedstock significantly alleviates energy crises and environmental pollution. Phenol is the simplest model compound for lignin bio-oil feedstocks, and the synthesis of fuel precursors from phenol through alkylation has received increasing attention. Here we report a one-pot strategy for preparing polycyclic alkane high-density fuels from phenol and cyclohexanol over bifunctional Pt/Hβ catalyst by combining alkylation with following hydrodeoxygenation (HDO). The activity of different zeolites for catalyzing the alkylation of phenol and cyclohexanol was explored. It was found that the larger pore size of alkali treated Hβ would not limit the production of polycyclic compounds, and good acid content in a particular mesoporous specific surface area can speed up the reaction rate. The one-pot reaction conditions were then optimized. When the alkali treatment concentration is 0.2 mol/L, the metal loading is 0.2 wt%, and the molar ratio of phenol and cyclohexanol is 1:1, the highest conversion of phenol can reach more than 83 %. The selectivity of alkylphenol can reach more than 97 %, and the yield of bicyclic and tricyclic rings in the final product after HDO can reach 83.42 %. The bifunctional catalyst can also realize the coupling of other acid-catalyzed carbon growth reactions and metal-catalyzed HDO reactions, which allows the direct synthesis of fuel from lignin oil or other biomass compounds.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Bao Zien,Ren Xiaohong,Rong Zeming
The selective upgrading of lignin-derived compounds into
high-value
chemicals remains a critical challenge. In this study, a series of
Ni-based catalysts supported on Hβ zeolite and modified with
secondary metals (Zn, Fe, and Cu) were synthesized and systematically
evaluated for the catalytic conversion of 4-propylguaiacol in aqueous
phase under hydrogen-free conditions. Among the catalysts studied
at 220 ° C for 2 h, Ni/Hβ delivered a conversion of 36.1%
and a phenolic selectivity of 89.6%. By comparison, NiZn/Hβ
exhibited the highest catalytic activity, achieving a conversion of
82.9% with a selectivity of 96.5%, indicating the promotional effect
of Zn incorporation. NiFe/Hβ showed a moderate conversion of
45.5% but maintained a high phenolic selectivity of 97.6%. However,
NiCu/Hβ showed almost no catalytic activity, with a conversion
of only 2.0%. Structural characterization by XRD, XPS, N 2 physisorption, H 2 -TPR, SEM, and TEM revealed that the
introduction of Zn significantly improved the dispersion of Ni species
and reduced Ni crystallite size, thereby increasing the number of
accessible active sites. In contrast, Fe incorporation altered the
catalyst structure and reduced catalytic activity, while Cu addition
induced metal aggregation and markedly suppressed catalytic performance.
The results indicate that appropriate second-metal modification can
effectively regulate the metal dispersion, microstructure, and metal–support
interactions in Ni/Hβ catalysts, thereby influencing the hydrogen
activation ability and the cleavage of Ar–CO 3 bonds.
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DOI
高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Jiapeng Zhang,Wuyu Wang,Linfei Zhou,Xinghua Zhang,Longlong Ma
The synthesis of high-performance jet fuel from biomass presents a solution to energy crises and environmental pollution. This paper introduces a novel strategy for producing jet fuel with a high heat sink and low freezing point using bio-derived phenol and ethanol. The production route comprises two successive steps: the alkylation of phenol with ethanol, followed by hydrodeoxygenation (HDO), catalyzed by Hβ zeolite and Pt/C, respectively. The alkylation conditions were optimized at 260 °C for 8 h, achieving phenol conversion rates exceeding 95 % and yielding 88.7 % alkylphenol at a phenol to ethanol molar ratio of 1:3. The final HDO products consisted of 20.25 % monoethylcyclohexane, 44.87 % diethylcyclohexane, and 28.32 % triethylcyclohexane. These products demonstrated a heat sink capacity of 3.3 MJ/kg, a freezing point below −65 °C, a heat value of 45.4 MJ/kg, and a density of 0.82 g/cm 3 at 20 °C, surpassing the performance metrics of conventional JP-8 fuel. Kinetic studies on the alkylation revealed activation energies of 58.36 kJ/mol for O-alkylation and 122.07 kJ/mol for C-alkylation. The findings contribute to understanding the mechanisms of alkylation reactions between phenolic compounds and short chain alcohols. This work offers a straightforward and energy-efficient way to synthesize high-performance jet fuel from lignocellulosic derivatives, reducing processing energy consumption and enhancing feedstock utilization rates.
研究领域:
能源化学
·
催化
·
燃料科学
·
化学工程
·
生物质转化
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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）