ENERGY & FUELS
·
2019
·
IF 3.021
Zhen-Yi Du,Bin-Bin Zhang,Ting-Sheng Chen,Yuli Betancur,Wen-Ying Li
Isobutanol derived from biomass can serve as a potential renewable candidate for the production of light olefins and aromatics, which are the building blocks to manufacture fuels and chemicals in the petrochemical industry. Dependent upon the product requirements, the product selectivity toward olefins or aromatics can be tuned by adjusting the reaction conditions and the properties of HZSM-5 catalysts. On bare HZSM-5, mild conditions (low temperature, low space time, and low acidity) favored the production of olefins and harsh conditions (high temperature, high space time, and high acidity) were more likely to produce aromatics. Ga was impregnated onto HZSM-5 to enhance the production of aromatics. Unexpectedly, Ga introduction only induced the intertransformation between olefins and aromatics without significantly impacting the selectivity of low-value paraffins. The exchanged Ga sites functioning together with Brønsted acid were identified as active Ga species and strengthened the direct dehydrogenation of C6–C8 olefins. The in situ-generated water from isobutanol dehydration affected the formation of Ga species. This resulted in different promotional effects of Ga on the transformation of isobutanol and isobutene. The reaction pathways were developed on the basis of the catalyst evaluation results, in tandem with an in situ diffuse reflectance infrared Fourier transform spectroscopy study on the intermediates formed during isobutanol transformation. Selectivity of olefins and aromatics from isobutanol transformation can be tuned by adjusting reaction conditions and properties of HZSM-5 catalysts.
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
Nanomaterials
·
2025
·Vol. 15
·期 10
·751
·
IF 4.3
Jian Li,Laizhi Sun,Derun Hua,Xinning Lu,Dandan Yang,Zhiying Wu
Gallium-modified Zeolite Socony Mobil-5 (ZSM-5) zeolites were synthesized using wetness impregnation and hydrothermal synthesis methods. The structural and acidic properties of the zeolites were characterized through an analytical instrument, which demonstrated that Gallium-modified HZSM-5 zeolites retain the Mobil five instructure (MFI) framework structure, but exhibit a reduction in Brønsted acid sites and a decrease in micropore size. The catalytic performance of these zeolites in the pyrolysis of cellulose biomass and polyethylene was tested. Compared with HZSM-5, Ga-modified HZSM-5 zeolites considerably increased monoaromatic yields while reducing alkanes production. In particular, gallium-impregnated HZSM-5 increased the monoaromatic yield from 37.6% for ZSM-5 to 43.2%, while hydrothermal synthesized Ga-HMFI reduced polyaromatic and alkane yields from 6.6% and 24.6% for HZSM-5 to 2.9% and 11.4%, respectively. These results indicated that Ga-modified HZSM-5 zeolites can improve the synergy between cellulose-derived oxygenates and polyethylene-derived olefins, enhancing the yield of petrochemical hydrocarbons compared to that predicted by theoretical calculations.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiaxing Song,Jun Wang,Xudong Du,Yuhan Pan,Jingyuan Sima,Youqi Zhu,Qunxing Huang
Non-thermal plasma (NTP)-assisted catalytic pyrolysis is a promising technology for producing benzene, toluene, ethylbenzene, and xylene (BTEX) from mixed waste plastics. A primary challenge in this approach is the need to achieve a high selectivity for the target products. To address this challenge, this study focused on the preparation of Ga-modified zeolites. The results showed that Ga loading was effective in increasing BTEX yields for the zeolites of USY, β, and HZSM-5 by 7.49%, 4.72%, and 8.63%, respectively. Among these zeolites, HZSM-5-Ga-N 2 was the most suitable for catalyzing the NTP-assisted pyrolysis reaction to produce BTEX hydrocarbons, with a maximum selectivity of 63.19% and a maximum yield of 31.84%. This was because the pore of HZSM-5 matched the ring size of BTEX, and NTP improved the distribution of Ga 2 O 3 active sites, allowing more acidic active sites to participate in the catalytic reaction. This work provides an applicable solution to increase the selectivity and yield of BTEX from NTP-assisted pyrolysis of mixed waste plastics with Ga-loading catalysts.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2017
·
IF 4.636
Wenwu Zhou,Qing Zhang,Yasong Zhou,Qiang Wei,Lin Du,Sijia Ding,Shujiao Jiang,Yanan Zhang
USY zeolites have been modified by incorporation of gallium, phosphorus and a combination of gallium and phosphorus by wetness impregnation method using gallium nitrate and ammounium phosphate diabasic, and the corresponding NiMo supported hydrodesulfurization (HDS) catalysts have been prepared for HDS of an inferior FCC diesel. The individual physical-chemical properties of the modified USY zeolites and the series NiMo supported catalysts were characterized using XRD, N 2 -adsorption-desorption(BET), NH 3 -TPD, Py-FTIR, H 2 -TPR, HRTEM and XPS methods, and their catalytic performances for an inferior FCC diesel HDS were assessed. The results show that both gallium and phosphorus modification can modulate the acid property of USY zeolite and weaken the interaction between the active metal and the supports, thus enhancing the degree of sulfidation and the dispersion of Mo species that are beneficial for the HDS of highly refractory organosulfur compounds. The highest HDS and HDN efficiencies of 99.7% and 99.6%, respectively, were observed over the catalyst containing the PGaUSY zeolite. More importantly, gallium modification of the USY zeolite promotes the hydrodesulfurization of all organosulfur compounds, and especially 4,6-DMDBT, in the FCC diesel and phosphorus modification of the USY zeolite promotes the hydrodesulfurization of most organosulfur compounds except for 4,6-DMDBT in the FCC diesel.
研究领域:
催化化学
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石油加工工程
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Xiaocui Wei,Yanan Liu,Yang Cao,Jin Li,Xianghao Meng,Zhao Zhang,Zhongyi Jiang
The catalytic pyrolysis of biomass is a sustainable approach for biofuel production, contributing to replacing fossil resources with renewable resources . The ZSM-5 zeolite remains an attractive catalyst in the catalytic pyrolysis of biomass, and how to reduce the product diffusion resistance and regulate the surface acidity of ZSM-5 should be explored more deeply. Herein, a hierarchical gallium-modified ZSM-5@SBA-15 catalyst is fabricated through coating a mesoporous layered SBA-15 shell on a hollow ZSM-5 core with gallium modified on the surface, which is effective for increasing hydrocarbon production during the catalytic pyrolysis of biomass process. The synergistic effect of hollowness, mesoporosity, and activity in the hierarchical gallium-modified ZSM-5@SBA-15 catalysts is found to affect the yield and quality of bio-oil. Accordingly, the hierarchical gallium-modified ZSM-5@SBA-15 catalyst with 11 wt% Ga loading exhibits a superior deoxygenation ability, and the relative content of hydrocarbons in bio-oil reach to 49.76 area% which is much higher than that of ZSM-5 (35.30 area%). Furthermore, a possible catalytic pyrolysis mechanism of biomass was also proposed to clarify the potential application of hierarchical gallium-modified ZSM-5@SBA-15 catalysts.
研究领域:
能源科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Yiheng Wu,Yangping Lv,Ruipu Wang,Lixia Bao,Zhongdong Zhang,Dejun Shi,Anlv Zhang,Yaoyuan Zhang,Qi Liu,Qin Wu,Daxin Shi,Kangcheng Chen,Guiyuan Jiang,Hansheng Li
The aromatization of light alkane is an important process for increasing the aromatic production and utilization efficiency of light alkane resources simultaneously. Herein, Ga-modified HZSM-5 catalysts were prepared and investigated by a series of characterization techniques such as X-ray diffraction, nuclear magnetic resonance spectroscopy, transmission electron microscopy, N2 adsorption–desorption, and NH3 temperature-programmed desorption to study their physicochemical properties. The catalytic performance in propane aromatization was also tested. Importantly, the structure–activity relationship, reaction pathway, and coke formation mechanism in propane aromatization were systematically explored. It was found that different Ga introduction methods would affect the amounts of Brønsted and Lewis acid sites, and Ga-HZSM-5 prepared by the hydrothermal method exhibited higher amounts of Brønsted and Lewis acid sites but a lower B/L ratio. As a result, Ga-HZSM-5 showed higher propane conversion and benzene, toluene, and xylene yield compared with that of Ga2O3/HZSM-5. The propane aromatization reaction pathway indicated that propane dehydrogenation to propene was a crucial step for aromatic formation. The increase of the Lewis acid density in Ga-HZSM-5 can effectively improve the dehydrogenation rate and promote the aromatization reaction. Furthermore, the formation of coke species was studied by thermogravimetry–mass spectrometry and Raman approaches, the results of which indicated that the graphitization degree of coke formed over spent Ga-HZSM-5 is lower, resulting in enhanced anticoking stability.
研究领域:
催化
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化学工程
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 39
·9369-9382
·
IF 5.317
Wenwu Zhou,Yasong Zhou,Qiang Wei,Lin Du,Sijia Ding,Shujiao Jiang,Yanan Zhang,Qing Zhang
Graphical Desulfurization : The effects of gallium modified HUSY zeolite acidic co-supports on the hydrodesulfurization (HDS) activity and isomerization selectivity of highly refractory organosulfur compounds such as 4,6-dimethyldibenzothiophene have been investigated. The effects of metal-modified acidic co-supports on the hydrodesulfurization (HDS) activity and isomerization selectivity of highly refractory organosulfur compounds such as 4,6-dimethyldibenzothiophene have been investigated. Y zeolite crystals with high Si/Al ratios and small crystallite sizes were successfully synthesized by a new hydrothermal synthesis approach. The synthesized Y zeolite crystals were ion-exchanged and stabilized. The prepared samples were then modified with different gallium contents using an impregnation method to adjust their acidity properties, and these modified samples were used as co-supports for NiMo sulfide HDS catalysts. The catalyst containing 10 wt.% zeolite Y modified by 2 wt.% gallium (NiMo/2GaY-ASA-A) exhibited the highest HDS activity, with 4,6-dimethyldibenzothiophene (4,6-DMDBT) conversion nearly double the rate of the catalyst without zeolite at 563 K, 4.0 MPa and liquid hourly space velocity (LHSV) of 40 h −1 . NiMo/2GaY-ASA-A also exhibited superior isomerization ability, with 3,4′-DMBP, 4,4′DMBP, and 3,6-DMDBT as the main products, indicating that the isomerization pathway was the main reaction route over NiMo/2GaY-ASA-A. The superior catalytic performance is related to the synergistic effect of the proper amount of medium and strong Brønsted acid sites. The compounds 3,6-DMDBT and 3,7-DMDBT (isomers of 4,6-DMDBT) and 3,4,6-TMDBT and tetra-methyl-DBT (transmethyl products) were detected simultaneously in the HDS product of 4,6-DMDBT for the first time over NiMo/GaY-ASA-A catalysts. Finally, a new reaction network over NiMo/2GaY-ASA-A was proposed.
研究领域:
催化化学
·
材料科学
·
能源化工
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）