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
·
催化化学
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DOI
高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 2
·55
·
IF 2.4
Yu Yang,Song Xuefeng,Su Wenli,Jing Wenjiang,Fan Yu
To meet aviation decarbonization targets, efficient catalysts for bio-jet fuel are needed. Hydrodeoxygenation (HDO) is an indispensable step in converting lipid feedstocks to jet-range hydrocarbons, which critically depends on the pore architecture, acidity distribution and metal dispersion of the catalysts. In this work, a layered SAPO-11 (LS) molecular sieve was synthesized using the polyamine surfactant (C 22 H 45 -N(CH 3 )-C 6 H 12 -N(CH 3 ) 2 ) as a micro-mesopore-directing agent. Ni species were introduced to obtain a series of Ni x /LS catalysts with the Ni loadings of x wt% ( x = 3.0, 6.0, and 9.0), in which Ni 6 /LS exhibited the best HDO performance. Using methyl laurate (ML) as a model feedstock, at the optimized conditions of 360 °C, 2.0 MPa and a weight hourly space velocity (WHSV) of 6.0 h − 1 , the Ni 6 /LS catalyst had the 99.6% conversion of ML with the 97.3% selectivity toward C 11 -C 12 alkanes, surpassing the conventional Ni 6 /microporous SAPO-11 (Ni 6 /MS) catalyst and the literature-reported catalysts. The superior lipid HDO performance of Ni 6 /LS was attributed that the layered architecture of LS provided a larger specific surface area and more mesoporous channels than MS, greatly promoting the high dispersion of Ni species. Graphical
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高影响因子
ENERGY & FUELS
·
2012
·
IF 2.721
Hualiang Zuo,Qiying Liu,Tiejun Wang,Longlong Ma,Qi Zhang,Qing Zhang
Catalytic hydrodeoxygenation (HDO) of vegetable oils to renewable alkane-type biofuels has attracted more and more concern in recent years. However, the presently used catalysts were mainly focused on the sulfided CoMo and NiMo catalysts, which inevitably posed sulfur contamination in final products. Therefore, exploring nonsulfured catalyst for this processing is of fundamental importance, but it is still an open challenge. In this paper, we prepared the sulfur free Ni supported on SiO2, γ-Al2O3, SAPO-11, HZSM-5, and HY by incipient wetness impregnation and tested the catalytic performance in HDO of methyl palmitate. Alkanes with long carbon chains were mainly produced with two possibly parallel approaches: hydrogenation of hexadecanal to hexadecanol, followed by dehydration/hydrogenation to C16 alkane and decarbonylaton/decarboxylation of hexadecanoic acid to C15 alkane. The acidity of catalysts significantly influenced their catalytic performance, and the Ni/SAPO-11 catalysts with weak and medium acidity showed superior properties to the other catalysts due to the synergistic effect of metal Ni and acidic support. The maximum yield of 93% for C15+ alkanes was observed over 7 wt % Ni/SAPO-11 under the mild reaction conditions of 493 K and 2 MPa, indicating its promising application in this reaction.
研究领域:
催化化学
·
可再生能源
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DOI
高影响因子
RSC Advances
·
2025
·Vol. 15
·期 18
·14235-14245
·
IF 4.6
Tong Su,Daguo Wu,Xinghua Zhang,Qi Zhang,Lungang Chen,Xiuzheng Zhuang,Longlong Ma
Biomass is an important renewable resource in nature, and cellulose is a crucial component within it. The chemically directed conversion of cellulose into ethylene glycol offers a green alternative to traditional petroleum-based production methods. In this study, a multifunctional Ni–WOx/SAPO-11 catalyst was designed. By optimizing the processing parameters of catalysts and the reaction conditions of them, it was demonstrated that this catalyst could efficiently catalyze cellulose into alcohol products through a series of tandem reactions such as hydrolysis, retro-aldol condensation, and hydrogenation under relatively mild conditions. The yield of ethylene glycol climbed from 4% (at 180 °C) to 66.6% (at 240 °C) with the increase of reaction temperature. Characterization (XPS, TEM, TPD/TPR) revealed that a reduction temperature of 500 °C maximized Brønsted acidity and W5+/W6+ ratios, enhancing C–C cleavage efficiency. Further increases in the reduction temperature would weaken the Brønsted acid on the surface of SAPO-11, but its surface area would also increase (mainly in the form of mesopores). The uniformly dispersed elemental tungsten could form new acidic sites on the catalyst surface; in combination with active Ni0, this high-temperature reduced catalyst could achieve the direct hydrogenolysis of cellulose to produce ethylene glycol, benefiting the efficient utilization of lignocellulosic biomass in the future.
研究领域:
生物质能
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催化化学
·
可再生能源
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yuxiang Liu,Yuchao Lyu,Baojie Wang,Yi Wang,Xinmei Liu,Mark J. Rood,Zhen Liu,Zifeng Yan
It is important to develop new promoters of fluid catalytic cracking (FCC) catalyst to increase iso-paraffin yield and avoid the decrease of research octane number (RON) caused by olefin saturation in gasoline hydrofining. SAPO-11 and LaAPO-11 molecular sieves were used as promoters to FCC catalyst to increase gasoline RON and were tested in the cracking reaction of n-dodecane on FCC conditions. LaAPO-11 molecular sieve has less and weaker acidity than SAPO-11 molecular sieve. LaAPO-11’s metallic sites polarize the C H bonds to form carbenium ions for isomerization reaction and weak acid sites make less contributions to the cracking of iso-paraffin. LaAPO-11 promoter increases the yield of iso-paraffin (C 5-9 ) from 6.4% to 10.2%. Besides that, a high yield of arene (2.0%) is caused by the dehydrogenation activity of LaAPO-11 promoter. The new contributions of this paper are the synthesis of a hydrothermal stable LaAPO-11 molecular sieve with isomerization activity and proposing the reaction routes of iso-paraffin. These new contributions are important for developing more effective RON promoters of FCC catalyst.
研究领域:
化学工程
·
催化材料科学
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DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2020
·Vol. 27
·期 5
·1455-1466
·
IF 2.183
Yuan Zhishuai,Cheng Yuchun,Ma Shoutao,Jiang Zhen,Zhou Yisi,Wang Yingjun,Zhang Wei,Suo Yanhua
A new method called Instant Exactness Synthesis (IES), which was applied to prepare SAPO-11 molecular sieve, was introduced innovatively. The metal–acid bifunctional Ni/SAPO-11-IES catalyst with a Ni content of 4% was prepared by the impregnation method. Ni/SAPO-11-H catalyst was prepared as a comparative sample through the traditional hydrothermal method. In addition, the growth mechanism was used to explain the excellent performance of catalyst prepared by IES method in detail. The structure of Ni/SAPO-11-IES was confirmed via XRD and TEM characterization. The pore structure of the molecular sieve was determined by nitrogen adsorption and desorption. 29 Si MAS NMR measurement was used to illustrate multiple silicon environment which supported the excellent acidity in NH 3 -TPD measurement. Furthermore, the favourable dispersibility of Ni species was proved by the mapping of the elements and EDS. Benefiting from the superior performance of materials, Ni/SAPO-11-IES catalyst exhibited a higher catalytic performance for n-heptane hydroisomerization with n-heptane conversion of 82% and isoheptane selectivity of 86%, respectively, compared with other catalysts in the same system. The study also provides new ideas for the preparation of molecular sieve materials.
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Hao Qin,Nengjie Feng,Quan Lv,Hui Wan,Guofeng Guan
Single atomic catalysts (SAC) isolated in zeolite have been reported for hydroisomerization of n-alkanes. However, it is widely found that metal species located outside zeolite crystals have beneficial effects on catalytic performance, rather than inside zeolite. Herein, we introduce cerium oxide as a binder to anchor Pt single atoms on the catalyst surface . Pt species were atomically dispersed on catalyst surface certified by AC HAADF-STEM and XAS. Pt 1 @CeO x /SAPO-11 not only shows significant activity but also effectively inhibits the selectivity of cracking or hydrogenolysis . The turnover frequency value of 0.05%Pt 1 @CeO x/ SAPO-11 reaches 9511 h −1 , 13 times higher than reported catalyst prepared with the space-confined strategy. Reaction mechanisms have been proposed to explain the different effects of platinum status and location on the reaction. Platinum single atoms located outside the catalyst crystal are speculated more favourable to this reaction. Conceptually, catalytic efficiency of this reaction can be improved by dispersing the active sites to reduce the local concentration of the product of a reversible step in an intermediate reaction. An appropriate loading of 0.05 wt% is needed to achieve the high efficiency of the metal and acid sites simultaneously.
研究领域:
催化
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化学工程
·
材料科学
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DOI
高影响因子
Petroleum Science
·
2021
·Vol. 18
·期 2
·654-666
·
IF 4.09
Wen Cheng-Long,Xu Jun-Dong,Wang Xue-Man,Fan Yu
To enhance the gasoline octane number, low-octane linear n-alkanes should be converted into their high-octane di-branched isomers via n-alkane hydroisomerization. Therefore, hierarchical SAPO-11-based catalysts are prepared by adding different contents of sodium dodecylbenzene sulfonate (SDBS), and they are applied in n -nonane hydroisomerization. When n (SDBS)/ n (SiO 2 ) is less than or equal to 0.125, the synthesized hierarchical molecular sieves are all pure SAPO-11, and as the SDBS content increases, the submicron particle size decreases, and the external surface area (ESA) increases. Additionally, these hierarchical SAPO-11 have smaller submicron particles and higher ESA values than conventional SAPO-11. When n (SDBS)/ n (SiO 2 ) is greater than 0.125, with increasing SDBS content ( n (SDBS)/ n (SiO 2 ) = 0.25), the synthesized SAPO-11 contains amorphous materials, which leads to a decline in the ESA; with the further increase in SDBS content ( n (SDBS)/ n (SiO 2 ) = 0.5), the products are all amorphous materials. These results indicate that in the case of n (SDBS)/ n (SiO 2 ) = 0.125, the synthesized SAPO-11 molecular sieve (S–S 3 ) has the most external Brønsted acid centers and the highest ESA of these SAPO-11, and these advantages favor generation of the di-branched isomers in hydrocarbon hydroisomerization. Among these Pt/SAPO-11 catalysts, Pt/S–S 3 displays the highest selectivity to entire isomers (83.4%), the highest selectivity to di-branched isomers (28.1%) and the minimum hydrocracking selectivity (15.7%) in n -nonane hydroisomerization.
研究领域:
催化化学
·
石油化工
·
材料科学
·
多相催化
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DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2024
·
IF 5.2
Hao Qin,Hui Wan,Guofeng Guan
Hydroisomerization of n-alkanes plays an important role in fuel and lubricants processing. Bifunctional catalysts with ultralow platinum loading have recently been reported successively for hydroisomerisation. Herein, the catalysts were prepared successfully with different methods to improve the catalytic performance. The conversion of 0.01%Pt1@CeOx/SAPO-11 prepared by co-calcination method (0.01%Pt1@CS-c) is 71.4%, 25% higher than the other prepared by precipitation method. The turnover frequency per active surface platinum site (TOFPt) of 0.01%Pt1@CS-c is as high as 13115 h –1 . Revealed by the X-ray photoelectron spectroscopy (XPS) results, the quality of phase boundary/intersurface between ceria and zeolite is found significantly different. The conjunction quality of phase boundary directly affects the spillover rate of intermediate species, which further leads to an apparent activity difference. In addition, the possible role of ceria in the reaction is discussed, rather than just as a carrier for the active metal atoms.
研究领域:
催化化学
·
能源材料科学
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DOI
高影响因子
Petroleum Science
·
2026
·
IF 6.4
Xue-Feng Song,Xue-Man Wang,Yan Bing,Yu Fan
A novel polyacrylamide-assisted method for synthesizing the hierarchical SAPO-11-wrapped Ni catalyst was proposed. In this method, firstly, Ni 2+ ions from nickel salts were coordinated with nitrogen atoms in polyacrylamide (HPAM) to form a Ni 2+ -HPAM complex; then, Ni 2+ -HPAM was adsorbed on negative SAPO-11 crystals during the crystallization of SAPO-11, and Ni 2+ -HPAM was wrapped by SAPO-11 crystals with the growth of these crystals; finally, Ni 2+ -HPAM was transformed into NiO nanoparticles (about 2.5 nm) wrapped by SAPO-11 crystals after the HPAM was removed during calcination. This method obtained an in-situ Ni@SAPO-11 assembly with hierarchical pore structures and highly dispersed Ni metals. Compared with both Ni/SAPO-4.0 with the same Ni content synthesized by conventional impregnation and the Ni@SAC-4.0 in which Ni salt was introduced into SAPO-11 in situ without HPAM addition, the as-synthesized catalyst (Ni@SACH-4.0) exhibited a higher Ni dispersion with smaller Ni nanoparticles, and more mesopores and Brønsted (B) acid sites. Consequently, Ni@SACH-4.0 showed a higher C 10 isomer yield (78.2%) and a lower cracking selectivity (9.4%) than Ni/SAPO-4.0 and Ni@SAC-4.0.
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 4
·1770-1778
·
IF 3.591
Xia Jiang,Feng Long,Qiaolong Zhai,Jiaping Zhao,Peng Liu,Junming Xu
Soap stocks are by-products obtained during the refining process of vegetable oil, and are mainly feedstocks to produce acidified oil. In this work, an efficient process was developed to convert soap stock into a high-quality biofuel with low impurity content. A combination of acidification and catalytic cracking reactions employed as pretreatment was investigated to decrease the impurity content in the soap stock feedstock for obtaining a value-added biofuel. A high olefin content (approximately 47%) pyrolytic oil was obtained during the pretreatment. For further improvement of the cold flow properties, hydro-isomerization of pyrolytic oil for the formation of iso-alkanes over the Ce–Pt/SAPO-11and Ce–Pt/ZSM-5 catalysts was then carried out. The isomerization reaction temperature could be decreased to 320 °C because of the approximately 47% olefin content. The cold filter plugging point (CFPP) of the resulting product could be obtained at −11 °C, and the sulfur content could be decreased to lower than 10 ppm, which could meet the EN and ASTM specifications.
研究领域:
化学工程
·
生物能源
·
催化
·
可再生能源
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6.5
Fan Shao,Fengzhi Guo,Tianyu Bai,Rongrong Li,Shixuan Guo,Jinxiao Sun,Yasong Zhou,Wenbin Huang,Lu Gong,Gang Wang,Qiang Wei
Improving the performance of hydroisomerization catalysts for jet fuel production remains a considerable challenge, due to the difficulty in precisely controlling the balance between metal and acid functions. Although zinc modification offers a promising strategy to enhance the synergy, the underlying mechanistic understanding of Zn-induced framework repair and reconstruction remains unclear, blocking the rational design of bifunctional catalysts. In this work, A series of Zn-modified SAPO-11 zeolites with tunable ZnO/Al 2 O 3 ratios were synthesized via in-situ doping technique. Characterization results revealed that Zn substitution for Al altered the silicon incorporation environment. The formation of Si-O-Zn bonds (NH 3 adsorption energy = -0.99 eV) indicated weaker acidity than Si-O-Al bonds (−1.44 eV). At ZnO/Al 2 O 3 = 0.5% doping, isolated P-O-Zn bonds promoted the dispersion and dissolution of large silicon islands (Si(4Si)), increasing weak Brønsted acid sites. At higher Zn doping, the mechanism shifted inducing Si redistribution and forming medium-strong Brønsted acid sites. Namely, a dual role of Zn was identified as framework repair at low loading and framework reconstruction at high loading. The weakened and dispersed acidity enhanced Pt dispersion and reducibility, enabling Pt/(0.75ZnSAPO-11 + ASA) catalyst to deliver the highest iso-C 22 yield (30.9%) and selectivity (58.7%), with double-branched isomer yield (10.8%) and selectivity (20.6%). This work highlights the underlying mechanism of Zn modification in catalyst framework, and demonstrates its implications for enhancing the industrial application of Zn-modified catalysts in Fischer-Tropsch wax upgrading and jet fuel cold-flow performance.
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DOI
高影响因子
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