COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Boliang Li,Yigang Liu,Binfei Li,Junhao Zhang,Jiqian Wang,Yongming Chai,Jun Nan,Xianwei Fu,Zhaomin Li
The high activation temperature of catalysts and the difficulty of their dispersion in the formation are the main obstacles preventing the widespread application of catalytic hydrothermal cracking technology for heavy oil development. However, the "dual in-situ" strategy, which involves the in-situ generation of catalysts to achieve in-situ upgrading of heavy oil, holds promise as an ideal solution to overcome these challenges. Herein, a catalyst precursor suitable for the "dual in-situ" strategy was synthesized, and targeted decomposition experiments were conducted in both steam and oil-water environments typical of heavy oil thermal recovery. Additionally, oil displacement experiments in porous media were carried out, revealing the advantages and characteristics of this innovative oil displacement method in terms of heat transfer efficiency, oil displacement dynamics, and upgrading effects. The results showed that the final decomposition products of the synthesized cetyltrimethyl ammonium heptamolybdate in both steam and oil-water environments were catalytically active MoS 2 . In the oil-water environment, due to solvent and interfacial effects, MoS 3 could be converted to MoS 2 at 180–200°C, which was about 130°C lower than in a nitrogen or steam atmosphere, fully meeting the conditions for integration with heavy oil thermal recovery. Furthermore, the presence of organic groups significantly enhanced the adsorption properties of the MoS 2 generated from cetyltrimethyl ammonium heptamolybdate, with specific surface area and pore volume increasing by 110 m²/g and 0.04 cm³ /g, respectively. In the oil displacement experiments, the oil recovery after using cetyltrimethyl ammonium heptamolybdate increased by 10.3 % compared to steam flooding, and by 3.8 % compared to the direct injection of MoS 2 NPs. The in-situ generation of the catalyst resulted in reduced agglomeration and deposition, leading to significantly improved mobility and sweep efficiency. Consequently, this approach not only enhanced the upgrading and production of heavy oil but also greatly extended the durability of the effect.
研究领域:
石油工程
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Science of Advanced Materials
·
2020
·Vol. 12
·期 2
·304-311
·
IF 1.117
Xu Gaofeng,Jia Chengxinzhuo,Shi Zhengjun,Liang Ruijuan,Wu Chunhua,Liu Hu,Yan Chao,Fan Jincheng,Hou Hua,Ding Tao,Guo Zhanhu
The ex-situ catalytic cracking of camelina oil using nickel loaded MCM-41 as catalyst at 450 °C in fixed bed reactor was studied. Results revealed that the yield, selectivity and chemical composition of the liquid products was improved by nickel loaded MCM-41 without affecting
the crystalline structure of MCM-41. Moreover, the loaded nickel onto MCM-41 facilitated the cyclization, alkylation, aromatization, deoxygenation, isomerization and cracking reactions.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2022
·
IF 8.129
Huiyan Zhang,Chenjun Yang,Yujie Tao,Min Chen,Rui Xiao
The unstable oxygenates of raw bio-oil limit its high-value utilization, which renders the refinement process necessary. Catalytic cracking is one of the promising refining methods and HZSM-5 was found to be an effective catalyst. To investigate the reaction mechanism of catalytic cracking of the oxygenated components in bio-oil, guaiacol and acetic acid, are employed for the catalytic conversion over HZSM-5 and metal modified zeolite Zn/HZSM-5 in a self-designed micro-reactor. Herein, the mechanism of pyrolysis and catalytic cracking was calculated by density functional theory (DFT). For guaiacol, the selectivity of salicylaldehyde decreased from 57.41% to 41.84% and 40.31% over HZSM-5 and Zn/HZSM-5, respectively. In the catalytic cracking over Zn/HZSM-5, the yield of aromatic hydrocarbon increased. More specifically, benzene appeared in the liquid product. For acetic acid, the removal of the oxy-functional group was further promoted by Zn/HZSM-5, the as-formed ketene intermediate continues to react with zeolite catalysts, generating acetyl cation, and finally formed CO and ethylene. Zn/HZSM-5 has a better effect on promoting the reaction of ketene and methoxide since the energy barrier of the rate-determining step in this reaction decreased from 163.27 kJ/mol to 151.19 kJ/mol. Demethoxylation and dehydration were considered to be favored by Lewis acid sites.
研究领域:
化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Petroleum Science
·
2025
·
IF 6.1
Chi Li,Ji-Xiang Guo,Li Wang,Wen-Long Zhang,Peng-Cheng Xue,Chen-Hao Gao
China possesses abundant heavy oil resources, yet faces challenges such as high viscosity, underdeveloped production technologies, and elevated development cost. Although the in-situ catalytic viscosity-reduction technology can address certain technical, environmental, and cost problems during the extraction process, the catalysts often suffer from poor stability and low catalytic efficiency. In this study, a green and simple room-temperature stirring method was employed to synthesize a class of highly efficient and stable 2D MOF catalysts, which possess the capability to conduct in-situ catalytic pyrolysis of heavy oil and reduce the viscosity. Under the condition of 160 °C, a catalyst concentration of 0.5 wt%, and a hydrogen donor (tetralin) concentration of 2 wt%, the viscosity-reduction rate of Fe-MOF is as high as 89.09%, and it can decrease the asphaltene content by 8.42%. In addition, through the structural identification and analysis of crude oil asphaltenes, the causes for the high viscosity of heavy oil are explained at the molecular level. Through the analysis of catalytic products and molecular dynamics simulation, the catalytic mechanism is studied. It is discovered that Fe-MOF can interact with heavy oil macromolecules via coordination and pore-channel effects, facilitating their cracking and dispersal. Furthermore, synergistic interactions between Fe-MOF and the hydrogen donor facilitates hydrogenation reactions and enhances the viscosity-reducing effect. This study provides a novel strategy for boosting heavy oil recovery and underscores the potential of 2D MOFs in catalytic pyrolysis applications.
研究领域:
石油工程
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Yang Xu,Yudi Zhao,Xuan Guo,Yunming Fang
Co-processing of bio-oil and petroleum-derived feed in a fluid catalytic cracking process of a refinery is considered to be one of the most potential bio-liquid fuel preparation technologies. The detailed qualitative and quantitative analysis of the oxygenates in the co-cracking products facilitates optimization of the subsequent processing. In this study, an in-depth characterization of trace oxygenates from home-made co-processing liquid products in a fluid catalytic cracking (FCC) pilot plant unit at different bio-oil water-soluble phase (BOWS)/vacuum gas oil (VGO) mass blending ratios (0/100, 10/90, 20/80) at different reaction temperature (500 and 525 °C) was performed with quantitative and qualitative comprehensive two-dimensional gas chromatography–mass spectrometry (GC × GC–MS). An internal standard method with the internal standard 1,1,3,3-tetramethoxypropane was used to quantify trace oxygenates, which was selected from the qualitative analysis of the co-processing liquid products. The results showed that the contents of phenols and benzofurans in the liquid products from co-processing were low and the addition of BOWS was beneficial to improve the co-processing conversion, reduce the coke yield, but reduce the gas products and gasoline yield. The deoxygenation of catalytic cracking for oxygenates also weakened with the increase of bio-oil addition. The increase of reaction temperature can strengthen the deoxygenation of catalytic cracking, but the excessively high temperature can strengthen the thermal cracking reaction and reduce the gasoline yield.
研究领域:
能源化学
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分析化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2019
·
IF 3.021
Run Zou,Jun Xu,Sebastian Kuffner,Julian Becker,Tao Li,Xiang Guan,Xiaowan Zhang,Li Li,Martien A. Cohen Stuart,Xuhong Guo
Catalytic aquathermolysis in situ upgrading and reducing the viscosity of heavy oil in the reservoir remarkably enhances the recovery and is considered as a promising technology. However, the low catalytic efficiency and inferior dispersity in both water and oil limit its applications. In the present work, spherical polymer brush nanocatalysts were synthesized, in which nano-TiO2 is the core and poly(vinyl imidazole) (PVI)-loading nickel cations are polymer brushes. The chemical characteristics, polymer-grafting content, nickel-loading content, and morphology of as-prepared catalysts were characterized by infrared (IR) spectroscopy, thermogravimetric analysis, inductively coupled plasma optical emission spectrometry, scanning electron microscopy, and transmission electron microscopy. The polymerization degree of PVI was analyzed by proton nuclear magnetic resonance (1H NMR) spectra. The effects of the nickel-loading content, catalytic conditions, and hydrogen donor on the viscosity of heavy oil were studied. The results show that the heavy oil is catalytically cracked by the synthesized catalysts, which leads to the reduction of oil viscosity. The viscosity reduction is enhanced by the increase of the nickel-loading content, catalytic temperature, dosage of catalyst, and hydrogen donor. The rheological behaviors in terms of flow curve, thixotropy, viscoelasticity, and time dependence of cracked oil were studied. To explore the cracking mechanism, the four compositions of heavy oil before and after aquathermolysis were compared. The extracted asphaltenes and resins were further analyzed by elemental analysis, 1H NMR spectra, and IR spectroscopy. The organic compounds in reacted water were characterized by gas chromatography–mass spectrometry. It is found that the content of light saturates is much increased after aquathermolysis, along with the distinct decrease of resins. From the structure change of resins, such as the decrease of hydrogen/carbon and methylene/methyl ratios and increase of aromaticity and aromaticity condensation, the increased light saturates are due to the dissociation of alkyl side chains in resins. In addition, the aromaticity and aromaticity condensation in asphaltenes are found decreased, which is because of the fragmentation and depolymerization of large aromatics. Meanwhile, the loss of oxygen in both asphaltenes and resins is connected with the phenols found in the reacted water, indicating the breakage of the C–O bond and heteroaromatic ring-open reaction in both asphaltenes and resins during aquathermolysis.
研究领域:
化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 103
·101365-101371
·
IF 3.289
Guang Xiong,Jinpeng Yin,Jiaxu Liu,Xiyan Liu,Zhendong Guo,Liping Liu
Nano-sized ZSM-5 aggregates with interparticle mesopores was synthesized by an aerosol-assisted method. The amorphous aluminosilicate powder was used as a precursor, which was obtained by an aerosol process from an aqueous solution of the silicon and aluminium sources. The amorphous powder was crystallized in an autoclave with the structure-directing agent tetrapropylammonium hydroxide. No extra water was added in this step. The synthesis was performed in an extremely dense system, hence the amount of both template and waste water can be significantly reduced. The formation of the nanocrystalline MFI zeolite is mainly based on the liquid phase transformation in a supersaturation system. The nano-sized ZSM-5 aggregates were composed of nanocrystals with a size of 50–100 nm. Compared with the ZSM-5 zeolite synthesized by a conventional hydrothermal method, the nano-sized ZSM-5 aggregates exhibits a higher BET surface area, external surface area, and total pore volume and better Al species distribution. This nanocrystalline ZSM-5 zeolite shows a higher catalytic activity and stability in catalytic cracking of 1,3,5-triisopropylbenzene.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
·
IF 3.171
Xing Zhang,Jingfeng Wu,Junhao Chen,Liang Lu,Lingjun Zhu,Shurong Wang
The catalytic cracking of bio-oil is important to produce aromatic hydrocarbons , which can partially replace gasoline or diesel to greatly reduce carbon emissions from transportation. To further promote the formation of aromatic hydrocarbons, this work studied the effects of the preparation method and the acid strength of Ga 2 O 3 /HZSM-5 on catalytic cracking of the bio-oil distilled fraction systematically. The preparation method of Ga 2 O 3 /HZSM-5 had an important effect on its catalytic activity: the Ga 2 O 3 /HZSM-5 prepared by physical mixing showed the low dispersion of active phases and poor pore structure, resulting in its insufficient activity and severe coke deposition; the Ga 2 O 3 /HZSM-5 prepared by precipitation exhibited the higher activity, while many polycyclic aromatic hydrocarbons unfavorable for the subsequent utilization were in the oil phase; the Ga 2 O 3 /HZSM-5 prepared by impregnation showed the highest activity and 35.5% (mass) selectivity of the oil phase, including 80.3% monocyclic aromatic hydrocarbons and 12.0% polycyclic aromatic hydrocarbons. The Brønsted acidity of Ga 2 O 3 /HZSM-5 decreased with Si/Al ratio, leading to the decline in reactant conversion, oil phase selectivity and quality. Meanwhile, the polymerization between monocyclic aromatic hydrocarbons and oxygenates was promoted to produce many polycyclic aromatic hydrocarbons and even coke, causing catalyst deactivation .
研究领域:
能源化学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2022
·
IF 3.428
Bo Meng,Shenyong Ren,Zhi Li,Weiyu Song,Qiaoxia Guo,Baojian Shen
Decreasing steam treating temperature of zeolite Y to prepare USY has great attraction for industrial production of FCC catalysts, which is often operated at high temperature thus leading to huge energy consumption. Heteroatoms in the framework of zeolite Y are easier to be removed under steam condition, but the introduction of heteroatoms often leads to the decrease of relative crystallinity of zeolite. When Ga 3+ is introduced into the framework of zeolite Y, high crystallinity is well maintained in this work. Interestingly [Al, Ga]-NaY can be treated at low steam temperature to form [Al, Ga]-USY with very good mesoporosity and high framework SiO 2 /Al 2 O 3 ratio. The sample [Al, Ga]-NaY-8 has a distinctive micropore size distribution at 0.92 nm which is much bigger than conventional microporous NaY. DFT study disclosed the reason of low temperature steam treatment. The catalytic cracking of 1,3,5-TIPB and n -octane showed that the catalyst [Al, Ga]-USY obtained at lower steam treating temperature presented good performance.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Reaction Chemistry & Engineering
·
2021
·Vol. 7
·期 3
·699-710
·
IF 4.239
Xia Jiang,Feng Long,Jiaping Zhao,Peng Liu,Jianchun Jiang,Junming Xu
Molecular structural modification was a critical step for the production of high-quality biofuel. In this study, it was found that catalytic cracking followed by product isomerization is an effective technology to convert waste oil into low CFPP and high-quality biofuel. The detailed catalyst characterization was conducted by X-ray diffraction (XRD), scanning electron microscopy (SEM), thermo-gravimetric analysis (TGA), NH3-temperature programmed desorption (NH3-TPD), H2-temperature programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), pyridine-adsorbed Fourier-transform infrared spectroscopy (Py-FTIR) and Fourier-transform infrared (FTIR) spectroscopy analysis. With the addition of Ce into the Ni/SAPO-11 catalyst, the occurrence of the hydro-cracking reaction was restrained efficiently, and (20 + 1)% NiCe/SAPO-11 was considered as the optimal catalyst for the hydro-isomerization study. Under the action of the bimetallic catalyst, the isomerization reaction could be carried out at low reaction temperature (340 °C) because of the high olefin content (approximately 43%) in pyrolytic oils. Comparison of physical and chemical properties for the hydro-isomerization of pyrolytic oil catalyzed over NiCe/SAPO-11 and Pt/SAPO-11 was conducted. For the two catalysts, the product fuel revealed excellent properties, which abided by the established EN and ASTM standards.
研究领域:
能源科学
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催化化学
✓ 已验证
DOI
高影响因子
Journal of Inorganic and Organometallic Polymers and Materials
·
2024
·
IF 3.9
Liu Hao,Wang Yanlin,Yuan Hong,Luo Wenbo
Nanoscale ZSM-5 zeolites (NZSM-5) having different crystal sizes and Si/tetrapropylammonium hydroxide (TPAOH) molar ratios were synthesized using a hydrothermal method. These materials were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and N 2 adsorption–desorption. The results showed that each zeolite was highly crystalline regardless of the Si/TPAOH ratio and that the Brunauer–Emmett–Teller surface areas were in the range of 329−392 m 2 /g. The random aggregation of these nanoparticles resulted in the formation of numerous intergranular mesopores. These NZSM-5 zeolites were applied to the catalytic cracking of oleic acid to prepare light olefins and light aromatics using a laboratory-scale fixed bed reactor. The zeolite having a Si/TPAOH ratio of 10/5 showed the best catalytic activity and provided light olefins yield of 55% and selectivity of BTX in liquid phase products of 18%, respectively, at 500 °C. The small crystal size and abundant intergranular mesopores in this specimen resulted in shorter diffusion paths and an increase in the external specific surface area that both inhibited coke deposition and ensured accessible acid sites. Graphical Abstract
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·Vol. 9
·期 1
·152-171
·
IF 5
Haoyu Liu,Wenbo Luo,Ke Wang,Yanlin Wang,Hong Yuan
The bolaform surfactant C6H13-N+(CH3)2-C6H12-N+(CH3)2-C6H12-O-C6H4-C6H4-O-C6H12-N+(CH3)2-C6H12-N+(CH3)2-C6H13 (BCPH-6-6-6) was synthesized and used to guide the synthesis of hierarchical ZSM-5 nanosheets (HZN) for use as zeolite catalysts. The number of acidic sites and the Al distribution in the zeolite pores were varied by changing the amounts of sodium sulfate and Al in the initial gel. The X-ray diffraction, Fourier transform infrared spectroscopy, scanning electronic microscopy, NH3 temperature programmed desorption, 27Al magic angle spinning nuclear magnetic resonance spectroscopy and N2 adsorption/desorption were used to characterize these materials. These zeolites each had a well-developed hierarchical system and specific surface areas as high as 631 m2 g−1, indicating that the BCPH-6-6-6 formed lamellar micelles based on π–π stacking. Interconnected hierarchical pore structures were retained after the templating agent was removed. The HZN sample exhibited a 90° rotational intergrowth structure and retained a large number of lamellae. The same material had a high concentration of acidic sites and contained Al in a tetrahedral coordination framework. The catalytic cracking of oleic acid using this zeolite gave light olefin yields up to 52.2% at 500 °C, exceeding the performance of conventional ZSM-5 (38.9%), and the catalyst remained active for up to 60 h. At 450 °C, the BTX selectivity of 6.72% obtained with this material also exceeded that from the conventional ZSM-5. These results were attributed to the connected hierarchical pores of the HZN, which promoted diffusion and provided higher carbon resistance.
研究领域:
材料科学
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催化化学
✓ 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）