Reaction Chemistry & Engineering
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2021
·Vol. 7
·期 3
·699-710
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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
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DOI
高影响因子
RSC Advances
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2025
·Vol. 15
·期 18
·14235-14245
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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
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可再生能源
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产品关联
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Meiqiu Hu,Xiaolong Liu,Hong Yuan,Jingye Ma
An in situ encapsulation process was used to prepare ordered worm-like mesoporous Pt@SAPO-11 catalysts with different Pt loadings. Transmission electron microscopy images showed that Pt nanoparticles encapsulated within the SAPO-11 support mesopores were uniformly distributed and highly dispersed and had a narrow particle size distribution of 2–7 nm. Scanning electron microscopy indicated that increasing the Pt loading from 0.6 to 1.6 wt % did not significantly change the crystalline morphology of the catalyst, although the crystallinity decreased slightly. The specific surface area and average pore diameter of the Pt@SAPO-11 were in the ranges of 72–116 m2/g and 8.1–9.5 nm, respectively, which are determined by the Brunauer–Emmett–Teller method and Barrett–Joyner–Halenda method, respectively. The NH3 thermal-programmed desorption established that increasing the Pt loading gradually decreased the total NH3 desorption and that a loading of 1.2 wt % produced the highest concentration of medium-strong acid sites (6.2 cm3/g STP). X-ray photoelectron spectroscopy and H2 temperature-programmed reduction showed that a Pt loading of 1.2 wt % gave the strongest interaction between Pt nanoparticles and the SAPO-11 support. The Pt@SAPO-11 catalysts were used for the preparation of C8–C17 alkanes by decarboxylation of oleic acid. Employing a reaction temperature of 340 °C, a CO2 atmosphere, a Pt loading on the catalyst of 1.2 wt %, and a reaction time of 4 h, 100% oleic acid conversion was obtained together with an 80% yield of C8–C17 alkanes.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 3
·1-11
·
IF 2.4
Wen Chenglong,Liu Kang,Lu Yi,Wu Xintian,Li Shuning,Lu Mohong,Zhu Jie,Li Mingshi,Song Chunshan,Lu Xiaosong
Ni/SAPO-11 catalysts with highly dispersed Ni (TA-Ni/SA-11) were prepared using tartaric acid as a dispersant. The effect of the tartaric acid content on the physiochemical properties of the TA-Ni/SA-11 catalysts and their n-heptane hydroisomerization performance were investigated. TA-Ni/SA-11 exhibits smaller Ni particles and more Ni active sites in comparison to conventional Ni/SAPO-11 prepared via the impregnation method due to the interaction between tartaric acid and Ni 2+ . As the molar ratio of tartaric acid and Ni 2+ (n TA /n Ni ) increases, the number of Ni active sites in TA-Ni/SA-11 rises, while the surface area and relative crystallinity decrease because of the dealumination of SAPO-11. When n TA /n Ni is 0.75, 0.75TA-Ni/SA-11 presents the highest n-heptane conversion of 82.4% and isomer selectivity of 90.5%, as well as the lowest cracking selectivity of 9.0% at 380 °C, 1.5 MPa, 2 h − 1 , and a volume ratio of H 2 to n-heptane of 400 among these catalysts. Graphical
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 15
·3679-3691
·
IF 7.779
Lei Fan,Lianming Zhao,Yuchao Lv,Tinghu Wang,Yupeng Tian,Jianye Fu,Xinmei Liu
The synthesis of highly-dispersed non-noble metal based catalysts and their application in hydrogenation/dehydrogenation still remain challenging. Therefore, it is of great importance to protect metals from aggregation in both calcination and reduction processes. In this research, density functional theory (DFT) calculations were used to elucidate the stabilization effect of ionic liquid [Bmim][BF4] on Ni in the reduction process, showing that [Bmim][BF4] could efficiently inhibit Ni aggregation on the support. By further analysis combined with theoretical calculations, we found that the degree of metal dispersion before reduction directly determines the effect of [Bmim][BF4]. Guided by the DFT results, the method of co-assisted preparation of Ni/SAPO-11 using [Bmim][BF4] and lysine was adopted. Lysine forms a coordination compound with nickel oxides. The steric hindrance generated by the Ni–lysine complex can effectively inhibit the aggregation of nickel oxides during the calcination process. The DFT calculations revealed that during the reduction process, [BF4−] plays a dominant role in stabilization and electronic modulation by directly interacting with Ni on the support. The combination effects of [Bmim][BF4] and lysine effectively inhibit metal aggregation, leading to ultra-small nickel particles with a mean size of 4.4 nm over the obtained catalyst. Furthermore, the presence of [Bmim][BF4] also tunes the electronic state of Ni species. Using hexane isomerization as a probe reaction, the result indicates the excellent catalytic activity of the obtained catalyst (≈93.7% isomer selectivity at 63.5% conversion), much superior to that of Ni/SAPO-11 obtained from the traditional impregnation route (≈75.8% isomer selectivity at 64.6% conversion). This work provides a new method for the preparation of highly effective non-noble metal supported catalysts.
研究领域:
催化化学
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材料科学
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理论计算
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产品关联
DOI
高影响因子
Petroleum Science
·
2022
·
IF 4.757
Wei-Long Zhan,Yu-Chao Lyu,Xin-Mei Liu,Lei Fan,Fu-Rang Li,Ye Yang
The Ni/SAPO-11 catalyst used for n-hexane hydroisomerization was prepared via a novel two-step crystallization strategy. It involves introduction of nickel salt into the pre-crystalized system of SAPO-11 by grinding followed by a second crystallization step. No extra solvent is introduced during the whole synthesis procedure which reduces waste liquid emissions significantly. More importantly, interaction between nickel and support is effectively regulated by the novel method to achieve a well dispersed nickel species and inhibit formation of inert nickel spinel simultaneously. Chemical environments of framework Si are tuned to enhance surface acidity of the Ni/SAPO-11 catalyst. It also shows smaller particle size which favors fast diffusion of reactants and products. Insights into the two-step crystallization indicate that accumulation of SAPO-11 precursors in the pre-crystallization stage, pH regulation by nickel salt and structural directing effect of Ni 2+ during the second crystallization period account for the rapid crystal growth and smaller particle size of the Ni/SAPO-11 catalyst. All the unique features endow the Ni/SAPO-11 catalyst higher activity and isomers selectivity than the Pt/SAPO-11 catalyst in n-hexane hydroisomerization.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 38
·18070-18081
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IF 3.591
Xiaolong Liu,Jingye Ma,Hong Yuan
A series of mesoporous Pt@SAPO-11 catalysts with different Pt loadings were prepared using an in situ encapsulation process. These materials exhibited good topological structures and high Brunauer–Emmett–Teller (BET) surface areas (132–166 m2 g−1). Transmission electron microscopy images showed that the Pt nanoparticles in this material were in the 5–8 nm size range and were highly dispersed on the inner surfaces of the SAPO-11 support. N2-BET analyses demonstrated that the samples had mesoporous structures with average pore sizes of 7.3–8.5 nm. Characterization of the 1.0 wt% Pt@SAPO-11 catalyst by X-ray photoelectron spectroscopy and H2-temperature programmed reduction indicated strong interactions between the Pt nanoparticles and the carrier. This material was used to promote oleic acid decarboxylation under CO2 and gave a C8–C17 alkane yield of 80.8% after 4 h at 340 °C. After five repeated uses, the catalyst still gave a yield of 77.6%.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2022
·Vol. 97
·期 8
·2055-2067
·
IF 3.709
Xiaolong Liu,Jingye Ma,Minxin Wang,Hong Yuan
BACKGROUND A series of mesoporous Pt@KIT−6/SAPO−11 catalysts with SiO 2 :Al 2 O 3 molar ratios of 0.3, 0.4, or 0.5 and Pt loadings of 0.4, 0.8, or 1.2 wt% were prepared via an in situ encapsulation process using a PEO − PPO − PEO triblock copolymer (EO 20 PO 70 EO 20 , P123) as the mes. China 750001 oporous template and KIT−6 molecular sieves as the silicon source. RESULTS These catalysts were characterized by transmission electron microscopy (TEM), specific surface area analysis, and pyridine–infrared spectroscopy (Py − IR). The results showed that Pt nanoparticles with particle sizes of 3–7 nm were uniformly dispersed on the supports. These materials also exhibited good mesoporous structures with specific surface areas of 138–197 m 2 /g and average pore sizes of 7.1–9.9 nm. The specimens having a SiO 2 :Al 2 O 3 molar ratio of 0.4 also showed an orderly strip−shaped pore structure. The Py − IR results indicated that the catalysts had both Brønsted acid and Lewis acid sites, with total acid contents in the range of 77.8–131.1 μmol/g. CONCLUSION The decarboxylation of oleic acid using these materials under CO 2 was examined. The catalyst with a SiO 2 :Al 2 O 3 molar ratio of 0.4 and a Pt loading of 0.8 exhibited the best catalytic performance and a C8 − C17 alkanes yield as high as 85.1% at 340 °C by using a catalyst−to−oil mass ratio of 1:10 and a reaction time of 5 h. This performance was attributed to the ordered mesoporous structure of this catalyst along with its high surface area (173 m 2 /g), good crystallinity (92.8%), suitable acid content (98.6 μmol/g), and abundant Pt metal active sites. © 2022 Society of Chemical Industry (SCI).
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
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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
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能源材料科学
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DOI
高影响因子
JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 29
·期 5
·1387-1398
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IF 2.523
Ma Jingye,Liu Xiaolong,Yuan Hong
This work employed dodecyl trimethyl ammonium bromide, sodium dodecyl benzene sulfonate (SDBS) or dodecyl dimethyl betaine (BS–12) along with a PEO–PPO–PEO (P123) block copolymer to obtain a dual template system for catalyst synthesis. Using Pt(NH 3 ) 4 (NO 3 ) 2 as the platinum source, a series of mesoporous Pt/SAPO–11 catalysts with different Pt loadings were prepared via an in situ synthesis and characterized by X-ray diffraction, specific surface area analysis, temperature programmed desorption, X-ray photoelectron spectroscopy and transmission electron microscopy. These catalysts each had a complete AEL model structure with pore diameters in the range of 8.1–10.9 nm and specific surface areas between 103 and 168 m 2 /g. At a Pt loading of 1.0 wt%, the Pt/SAPO–11–S synthesized with SDBS–P123 as the dual template showed the least Pt loss, the largest specific surface area (159 m 2 /g) and the smallest Pt particle size (6.1 nm). This material also exhibited the highest ratio of Pt metal to oxide, indicating that it contained more active metal sites. This catalyst was applied to the decarboxylation of oleic acid under CO 2 to prepare C8–C17 alkanes, the main component of biological aviation kerosene. At a reaction temperature of 340 °C and catalyst-to-oil mass ratio of 1:10, the yield of C8–C17 alkanes reached 80.6% after 6 h. This same catalyst provided a 73.8% yield after six reuses, demonstrating good stability.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2019
·
IF 2.584
Lili Geng,Jianjun Gong,Guilong Qiao,Songshou Ye,Jinbao Zheng,Nuowei Zhang,Binghui Chen
Pt(NH3)4(NO3)2, Pt(NH3)4(Ac)2, (NH4)2PtCl4, and H2PtCl6 were used to prepare Pt/SAPO-11 catalysts to investigate the effect of Pt precursors on the hydroisomerization of n-dodecane. The catalyst derived from Pt(NH3)4(NO3)2 displays the best hydroisomerization activity and selectivity among these precursors. The hydroisomerization conversion of n-dodecane is affected by the platinum particle size, platinum dispersion, the location of platinum, and the valence state of platinum. The selectivity of n-dodecane is determined by the number of Brønsted acid sites and Pt crystal planes. These conclusions are verified by combining transmission electron microscopy, high-resolution transmission electron microscopy, hydrogen temperature programmed reduction, NH3-temperature programmed desorption, and Py-IR studies. The catalyst prepared with Pt(NH3)4(NO3)2 as the precursor exhibits the smallest platinum particle size and the highest platinum dispersion. Most of the platinum particles are supported on the external surface of SAPO-11 with the Pt(111) crystal face. Such a catalyst also possesses a suitable number of Brønsted acid sites and then displays the best catalytic performance. Obviously, the use of various precursors for the Pt-based catalyst can significantly affect the performance of Pt/SAPO-11 for the hydroisomerization of n-dodecane.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Lei Fan,Yuchao Lyu,Jianye Fu,Yupeng Tian,Furang Li,Wenjing Zhang,Xinmei Liu
The prominent size effects of metal nanoparticles (NPs) are mainly reflected in the change of electronic and geometric properties, which may induce distinct catalytic performance of the catalyst. Herein, Ni/SAPO-11 bifunctional catalysts with controllable sizes of Ni NPs were synthesized to investigate the particle size effects in n-hexane hydroisomerization. The results show that decreasing Ni particle size from 11.7 to 5.3 nm increases the concentration of surface Ni atoms and the proportion of low-coordinated Ni sites (corner, step sites) by 1.7 and 1.5 times, respectively. The low-coordinated surface Ni atoms have rich dangling bonds and high surface energy, resulting in greatly improved H 2 adsorption and activation abilities. Moreover, an increased proportion of low-coordinated Ni sites within the Ni cluster shifts the d-band center upward, further enhancing the adsorption and activation of reactants. The intrinsic catalytic activity (turnover frequency) of 5.3 nm Ni NPs is ca. 2 times as much as that of the 11.7 nm ones. Besides, the smaller Ni NPs enhanced the metal–acid synergy, leading to a higher selectivity to isomers. This work provides deep insights into the metal particle size effects over the bifunctional Ni/SAPO-11 hydroisomerization catalysts and can be extended to various metal supported catalysts.
研究领域:
催化化学
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材料科学
✓ 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）