ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Chao Miao,Kaixuan Shang,Lixing Liang,Shumei Chen,Jing Ouyang
In this work, a Ni-based catalyst supported on a core–shell structure catalytic carrier material (Ni/ZSM-5@MCM-41) based on kaolinite tailings is reported, which exhibits excellent CO2 methanation performance at atmospheric pressure. At 400 °C, CO2 conversion and CH4 selectivity reach 80 and 97% with the space velocity of 12,000 mL gcat–1 h–1, respectively, and it can maintain good stability during the 80 h stability test. Compared with traditional Ni/ZSM-5 and Ni/MCM-41 catalysts, Ni/ZSM-5@MCM-41 has more substantial confinement effects on the active components, and the active components are more evenly dispersed on surface of the carrier. In addition, it is confirmed by the in situ diffuse reflectance infrared Fourier transform spectroscopy technique that CO2 methanation over the Ni/ZSM-5@MCM-41 catalyst follows the path of formate and CO as intermediates.
研究领域:
催化
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Mengxue Song,Chonghao Qiu,Pengfei Ma,Jiawei Zhong,Zhuohan Zhang,Weiping Fang,Wenjing Song,Jianqiang Fan,Weikun Lai
Reductive etherification is an attractive and practical strategy to convert bio-platform compounds into valuable chemicals. In directed synthesis of furfuryl ethers, reductive etherification of bioderived furfurals is still challenging due to the complexity of catalytic reaction . Herein, reductive etherification of furfural with alcohol was investigated over Ni/ZSM-5 catalyst, which found that Si/Al ratios in ZSM-5 played an important role on the catalytic performance. For Ni/ZSM-5 with Si/Al ratio of 50, 80.9% yield of furfuryl ether at 90.8% conversion of furfural was achieved under the condition of 2 MPa H 2 and 180 °C for 3 h in isopropanol. The catalyst exhibited superior stability and recyclability during the consecutive cycle run. Catalysts characterization demonstrated that both acidic properties and furfural adsorption were influenced by the Si/Al ratios in Ni/ZSM-5, which correlated to the reaction route and catalytic performance. Lewis acid sites enhanced furfural hydrogenation into furfuryl alcohol, while Brønsted acid sites on ZSM-5 effectively catalyzed sequential etherification of furfuryl alcohol to furfuryl ether. Under optimization conditions, various furfuryl ethers could be obtained with yields above 80% over Ni/ZSM-5 catalyst in different primary alcohols, demonstrating the general versatility of the approach. Our findings offered opportunities to develop an efficient furfuryl ethers synthesis method .
研究领域:
催化化学
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能源化学
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
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IF 6.7
Zekun Guan,Guangxun Sun,Chao Feng,Junxi Li,Minmin Wang,Mengdi Guo,Bin Liu,Yuan Pan,Chenguang Liu,Yongming Chai,Yunqi Liu
The production of cleaner gasoline requires reducing sulfur and olefin content in fluid catalytic cracking (FCC) gasoline. Herein, Ni/ZSM-5@Ni/ZnO catalysts were synthesized by uniformly coating Ni/ZnO on the surface of Ni/ZSM-5 by electrostatic induced crystallization strategy for FCC gasoline desulfurization-aromatization tandem reactions. The desulfurization activity of Ni/ZSM-5@Ni/ZnO has superior desulfurization activity due to the smaller size of ZnO, higher O vacancy content, and more uniform dispersion of Ni and ZnO relative to the physically mixed Ni/ZSM-5-Ni/ZnO. In addition, coating Ni/ZnO on the surface of Ni/ZSM-5 can reduce the Brønsted acid content of Ni/ZSM-5, increase the Lewis/Brønsted acid value of the catalyst, which inhibits the excessive cracking of FCC gasoline, and improves the liquid yield and aromatics selectivity. After 8 h of reaction, the desulfurization rate, aromatics generation rate and olefin conversion rate of Ni/ZSM-5@Ni/ZnO were 85.58 %, 25.22 % and 49.08 % respectively, which were higher than those of physically mixed Ni/ZSM-5-Ni/ZnO catalysts by 25.34 %, 15.95, and 12.98 %, respectively. Meanwhile, the unique structure of Ni/ZSM-5@Ni/ZnO reduces carbon deposition and delays catalyst deactivation. Density functional theory calculations show that Ni/ZSM-5@Ni/ZnO was more favorable for thiophene desulfurization and has a better ability to adsorb and activate H 2 . This study provides a new idea for the development of catalysts for clean gasoline production.
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
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Yingna Li,Muhammad Sajjad Ahmad,Mudassir Hussain Tahir,Maryam Bashir,Arif Muhammad Khan,Rana Muhammad Irfan,Imran Riaz Malik,Boxiong Shen
This study investigates the selective production of aromatics through the co-pyrolysis of cabbage waste and plastics followed by catalytic reforming with Ni-modified ZSM-5. Co-pyrolysis significantly improves the inflection point (a parameter for determining thermal stability) to 251.3 °C from 232.7 °C. This process also enhances the relative yield of olefins and phenols , which are precursors for aromatic production to 25.46 and 17.23 respectively, up from 13.87 to 12.05. Furthermore, catalytic pyrolysis elevates the relative yield of aromatics to 53.4, as confirmed by Thermogravimetric Analysis (TGA) and Thermogravimetric-Fourier Transform Infrared Spectroscopy (TG-FTIR) analyses. GC-MS confirms the enhanced formation of valuable chemical precursors via co-pyrolysis such as phenols and olefines to 18.67 % and 22.13 % leading to a 63.81 % selective yield of aromatics in the final oil with 10Ni/ZSM-5. Ni modification of ZSM-5 is influential in decreasing PAH formation (7.26 % from 20.37 %), indicating that this two-step process is an effective method for transforming waste into high-quality bio-oil with enriched aromatic content.
研究领域:
环境科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Chem Catalysis
·
2024
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IF 11.5
Bin Chen,Shui Yang,Longmei Shang,Yiling Wu,Youting Wang,Jian Tian,Jiale Huang,Xiaodong Zhang,Qingbiao Li,Guowu Zhan
Biomass resources can be converted to biochemicals via the catalytic pyrolysis process, but conventional catalysts often suffer from severe deactivation due to coke formation. Here, a ternary Ni/bio-Z5 catalyst was constructed by integrating ZSM-5 and Ni components on a porous bio-SiO2 platform derived from rice husk. The Ni/bio-Z5 achieved 76% aromatic selectivity for the catalytic pyrolysis of soybean oil, corresponding to a space-time yield as high as 154.8 garom · h−1 · gcata−1. It is confirmed that the bio-SiO2 platform shortened the surface diffusion path of aromatics by co-diffusion, which then inhibited coke formation and significantly improved the catalyst stability. Moreover, the atomically dispersed Ni on ZSM-5 effectively promotes the aromatization of C2=-C6= by enhancing adsorption and acting as an oligomerization center for isoalkyl carbenium ions. The coupling of deoxygenation and aromatization reactions promotes the enhancement of aromatic selectivity through the formation of methyl-substituted cyclopentenone that can be readily converted to aromatics.
研究领域:
能源与环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Processes
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2022
·Vol. 10
·期 10
·1970
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IF 3.352
Xuan Zhou,Hongling Pan,Shuixiang Xie,Guotao Li,Zhicai Du,Xiang Wang,Yan Luo
The aim of this research is to design and synthesize an efficient catalyst to enhance high value-added products, such as aromatic hydrocarbons and phenols, from the catalytic fast pyrolysis (CFP) of different types of forestry and agricultural residues. All three biomasses (rape straw, wheat straw, and bamboo powder) had no aromatic production via thermal pyrolysis alone; however, the aromatic selectivity and monocyclic aromatic selectivity were largely enhanced using ZSM-5, with suitable silica-alumina ratios and Ni loadings. Specifically, for rape straw, the optimum catalyst was 15 wt.% Ni/ZSM-5 (silica-aluminum ratios = 85), and the selectivity of aromatic hydrocarbons was achieved at 39%, of which 71% were monocyclic aromatic hydrocarbons. For wheat straw, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was 67%, of which 55% were monocyclic aromatic hydrocarbons. For bamboo powder, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was achieved at 21%, of which 80% were monocyclic aromatic hydrocarbons. Meanwhile, biomass types have significant effects on the pyrolyzed product distribution due to their different components. Cellulose and hemicellulose promoted the production of aromatic hydrocarbons, while lignin enhanced the production of phenols. The promotion of phenol by Ni was better and more efficient than that by the molecular sieve.Keywords:catalytic fast pyrolysis;forestry and agricultural residues;Ni/ZSM-5;aromatic hydrocarbons;phenols;Py-GC/MS
研究领域:
能源与环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Fuxiang Feng,Li Wang,Xiangwen Zhang,Qingfa Wang
Ultrathin Ni/ZSM-5 nanosheet catalysts with different acid concentrations, B/L (Brønsted/Lewis acid sites) ratios, and nanosheet thicknesses are designed for the hydroconversion of oleic acid into aviation-fuel-range alkanes (AFRAs). The role of acid concentration/distribution and nanosheet thickness was investigated. High acid concentration enhances the hydrodeoxygenation (HDO) reaction and intrinsic deoxygenation activity because of the synergistic effect between acid sites and metal sites. The selective cracking reaction can be enhanced by tailoring nanosheet thickness and acid distribution. The thin nanosheet favors isomerization, the selective cracking reaction, as well as the generation of central branched isomers. External acid sites dominate the primary cracking and central C–C cracking of the deoxygenated products, but internal acid sites promote the deeper cracking and terminal C–C cracking. Formation of aromatics is thoroughly suppressed at low reaction temperature (≤533 K). A high AFRA yield of 41.4% is achieved over the 3 nm nanosheet catalyst with Si/Al = 300 and B/L = 0.18.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
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IF 12.2
Bingyan Sun,Haifeng Xu,Tan Li,Wenjie Guan,Kaige Wang
Upcycling waste plastic into aromatics presents an attractive strategy to tackle both plastic pollution and energy challenges. However, previous studies often rely on high temperatures, precious metals, and have broad product distributions. In this study, we reported that a Ni/ZSM-5 bifunctional catalyst can directly convert polyethylene (PE) into methylated aromatics with high selectivity under mild conditions, while eliminating the requirement for hydrogen gas and solvents. The liquid yield could attain up to 70.3 %, and the aromatics yield could achieve up to 51.7 %. Over 78.4 % of the aromatics were methylated aromatics including toluene, xylene, and mesitylene. Polymer chains underwent dehydrogenation over Ni and the acid sites in ZSM-5, forming C C bonds. Certain of these bonds evolved into carbenium ions through the process of proton transfer at the acid sites. The optimization of Ni and acid sites enhanced the oligomerization, cyclization, and aromatization process. The extra mesopores created by Ni on the molecular sieve aid in the generation of aromatics. Furthermore, the Ni/ZSM-5 catalyst demonstrated the ability to convert typical commercial grades of PE plastic, such as gloves and bottles, into aromatics with a selectivity of up to 61.1 %. It offers an economically feasible and environmentally friendly upcycling avenue for the circular economy of plastics.
研究领域:
化学工程
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环境科学
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材料科学
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催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Fuxiang Feng,Xiaopo Niu,Li Wang,Xiangwen Zhang,Qingfa Wang
Ni/ZSM-5 nanosheet catalysts with different Si/Al ratios were modified by chemical liquid deposition (CLD) of tetraethoxysilane (TEOS) to tailor their acid spatial distribution. Their catalytic performance was evaluated with the hydroconversion of oleic acid to aviation-fuel-range-alkanes (AFRAs) at different reaction temperatures and H 2 pressures. The modified catalysts inherit the nanosheet structure with decreased external Brønsted acid concentration, especially the strong one. External Brønsted acid sites mainly favor the cracking of the deoxygenated products (C 17 /C 18 ). Internal Brønsted acid sites mainly enhance the isomerization of the linear AFRAs. And the catalytic activity of the external Brønsted acid sites was more sensitive to reaction temperature than that of the internal ones. The deoxygenation and cracking reactions were also more sensitive to H 2 pressure compared to the isomerization reaction. High AFRA selectivity of 51.4% as well as high iso/n -alkanes ratio of 1.7 were achieved at 250 °C and 10 bar over NS200(1).
研究领域:
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Weicheng Xu,Bingxu Chen,Xueding Jiang,Feng Xu,Xin Chen,Limin Chen,Junliang Wu,Mingli Fu,Daiqi Ye
The effect of Ca modification on the Ni/ZSM-5 catalyst for efficient toluene oxidation was studied in a plasma-catalytic system. The Ni/ZSM-5 and Ca-Ni/ZSM-5 catalysts were prepared by a wet impregnation method and characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Fourier transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), Pyridine-FTIR spectroscopy and temperature programmed desorption of ammonia (NH 3 -TPD). Among the catalysts tested, the Ca-Ni/ZSM-5 sample showed the best potential for toluene conversion (90.2%) and CO 2 selectivity (70.7%). Pyridine-FTIR spectra and NH 3 -TPD results proved that the introduction of Ca and Ni onto ZSM-5 caused a decrease in the strong and weak acidic sites. In addition, gas chromatography/mass spectrometry (GC-MS) result showed that the Ca-Ni/ZSM-5 catalyst reduced the production of undesirable byproducts (such as p-nitrotoluene and methyl benzoate). Calcium in the Ni/ZSM-5 system influenced the acidity and other surface characteristic of the catalyst, as well as directly impacting the reactive plasma species and the intermediates. Finally, possible reaction mechanisms in the plasma catalysis of toluene were also proposed.
研究领域:
环境催化
·
大气污染控制
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材料化学
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表面科学
·
等离子体化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
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IF 7.2
Zhen-Qiang Yu,Yao-Xin Xiao,Dong Liang,Che Zhao,Zhen Huang,Gang-Qi Cheng,Rui Shan,Hao-Ran Yuan,Yong Chen
The chemical upgrade of the waste polyester coating on the surface of aluminum cans to value-added products can not only decrease the release of toxic substances, but also improve the quality of aluminum in the recycling process. In this study, different types of zeolite molecular sieve catalysts loaded with Ni, Mo and Co were synthesized, and utilized in the rapid catalytic pyrolysis of polyester coating. Among them, the Ni/ZSM-5 achieved the maximum aromatic compounds yield of 68.43 % at 600 ℃. A series of characterization results demonstrated that the embedding of transition metals (like Ni) could promote the cyclization and aromatization of products through deoxidation and dehydrogenation reactions by changing the pore structure and increasing total acid content (Brønsted and Lewis acids) of the ZSM-5 molecular sieve. Meanwhile, the thermodynamics of polyester coating during catalytic pyrolysis was studied by thermogravimetric method. The average activation energy of Ni/ZSM-5 catalytic pyrolysis of polyester coating is 238.65 kJ/mol. Furthermore, even after being reused for over 5 cycles, the catalyst can still maintain a relatively high yield of aromatic compounds (exceeding 60 %). Finally, the mechanism for aromatic compounds formation from Ni-modified ZSM-5 in-situ catalyzed polyester coating pyrolysis was proposed. This work provided useful ideas for the subsequent treatment of solid wastes.
研究领域:
环境科学
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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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Tinghu Wang,Yuzhi Li,Wenjing Zhang,Furang Li,Lei Fan,Jianye Fu,Xinmei Liu,Yuchao Lyu
Acidity of supports always plays a key role in the determination of dispersion and electron density of metal components and then the catalytic behavior of bifunctional catalysts for deoxygenation of biomass-based resources. Herein, Ni/ZSM-5 catalysts with various Si/Al ratios and acidity were synthesized, and the role of acid centers in the deoxygenation of methyl laurate (ML) was discussed. The decreasing Si/Al ratios promote dispersion of Ni due to the anchoring effect of framework Al to nickel species. It also increases the electron density of Ni, which not only benefits the activation of hydrogen but also curbs the cleavage of C–CHO bonds. All of these accelerate ML transformation and preferentially promote the hydrodeoxygenation (HDO) route instead of decarboxylation (DCO2) or decarbonylation ones. The metal centers play a key role in the hydrogenolysis of ML and the hydrogenation of resultant fatty acids, while the acid centers can facilitate these processes. Besides, suitable acidity of the catalyst would increase selectivity to target alkanes and isomerized ones for biojet fuels by enhancing the HDO routes. However, excessive acid centers favor cracking reactions, reducing the selectivity of target products. This work contributes a profound understanding of the role of acid centers in the deoxygenation of ML into biojet fuels and can be extended to other bifunctional deoxygenation catalysts.
研究领域:
催化化学
·
能源科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）