JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
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IF 6.2
Hengshuo Gu,Ting Zhao,Jian Li,Yufei Gu,Hucheng Ge,Yuke Liu,Fuwei Li,Zhixia Li,Hongfei Lin,Jiangfei Cao
Hierarchical ZSM-5 (Z-40) was synthesized via a simple two-step hydrothermal crystallization without using any organic template. Low-density polyethylene (LDPE) as hydrogen donor was added into the catalytic pyrolysis of cellulose to enhance deoxygenation and the formation of BTX (benzene, toluene, xylene). Cellulose and LDPE showed the strongest synergistic effect at a feed ratio of 1, and the obtained experimental BTX yield (22.9 %) was 52.7 % higher than the theoretical yield (15 %). Co-catalytic pyrolysis (CCP) of two polymers followed similar cracking behavior to CCP of their pyrolysis vapor model compounds (furfural and n -octane), mainly including pyrolysis, catalytic cracking of pyrolysis fragments in external surface and hydrocarbons pool reactions of small cracking fragments in the internal micropores of zeolite. Z-40 showed better catalytic performance than the commercial ZSM-5 (higher BTX yield and less coke deposition) due to the appropriate acidic properties and distinctive pore structure. The optimal condition for CCP of cellulose/LDPE was temperature at 550 °C, feed ratio at 1:1 and catalyst/feed ratio at 2:1, and the achieved BTX yield reached 24.5 % with high BTX selectivity of 86.7 %. This work provided a cost-effective method for synthesis of ZSM-5 and production of high value-added BTX via a green non-oil route.
研究领域:
化学工程
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能源科学
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DOI
高影响因子
ENERGY CONVERSION AND MANAGEMENT
·
2024
·
IF 9.9
Yang Zhang,Jun Zhao,Lei Zhang,Yong Chen,Wangjing Ma
The recycling and processing of plastic waste to promote resource sustainability has emerged as a global concern. Selectivily upcycling polyolefins into valuable monocyclic aromatic hydrocarbons (MAHs) is a promising strategy to promote a circular economy but limited by low yield and selectivity. In this study, one-step microwave-triggered tandem pyrolysis coupling ZSM-5 catalytic reforming technology was explored, which is efficient for selectively transforming plastic into benzene, toluene, ethylbenzene, and xylene (BTEX) riched oil products. Pyrolysis and catalytic processes were achieved by mixing plastic and ZSM-5 with graphite, respectively, and placing them in the bottom and top layers of the reactor. Results indicate the mass ratio of plastic or ZSM-5 to graphite and microwave irradiation power would influence the selectivity and yield of MAHs. After careful investigation, the optimum reaction conditions are deemed to be 600 W, and the mass ratio of LDPE and ZSM-5 to graphite is 3:1 and 1:1, respectively, and delightful selectivity and yield of MAHs of 82.06% and 28.12 wt% are obtained under the above conditions. More importantly, the BTEX accounted for a significant amount in the MAHs with the selectivity and yield of 70.53% and 24.17 wt%, demonstrating a strong ability to produce high-value BTEX, which is attributed to the ZSM-5 providing a sufficient active site for reforming the pyrolysis vapors and promote the formation of BTEX by cracking, aromatization and Diels-Alder reactions. Additionally, gas products are rich in C 2 H 4 , C 3 H 6 and C 4 H 8 olefin monomers accounting for around 60% of the gas products, which also manifest high value. Besides, the ZSM-5 can be stabilized by exceeding three successive cycles, and this strategy is also suitable for the catalytic upcycling of PP and mixed plastics to produce MAHs selectively. Therefore, this one-step microwave-triggered tandem pyrolysis coupling ZSM-5 catalytic reforming technology provides a potential waste resource utilization method to convert plastic waste into high-value petrochemical products.
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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高影响因子
JOURNAL OF CHEMICAL SCIENCES
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2026
·Vol. 138
·期 4
·118
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IF 1.8
Xu Guohao
A Ga-substituted ZSM-5 zeolite was successfully synthesized via a hydrothermal synthesis method, and its catalytic performance and physicochemical properties in propane aromatization were systematically investigated. Comprehensive characterizations including XRD, SEM, ICP-AES, IR, NH 3 -TPD, XPS, N 2 adsorption-desorption and TG analyses revealed that Ga species exhibited the lower tendency to incorporate into the ZSM-5 zeolite framework compared to Al species. The gallium-doped aluminosilicate (GaAlZ5), possessing the largest specific surface area and highest acid content, demonstrated a superior aromatic selectivity of 85.6% and propane conversion of 66.1%, which exceeded those of gallosilicate (GaSiZ5) by 22.5% and 5.6%, respectively. Moreover, the intergranular mesopores in GaAlZ5 enhanced the mass-transfer rate of aromatics, effectively suppressed the formation of coke precursors, and endowed the catalyst with excellent long-term stability as well as regeneration stability. This work provides a facile synthesis strategy and systematic theoretical support for the design of high-stability and high-selectivity Ga-based zeolite catalysts for propane aromatization. Graphical abstract This graphical abstract illustrates the bifunctional tandem pathway of propane aromatization, where propane is activated to propylene via dehydrogenation over Ga-based Lewis acid sites, followed by aromatization under the synergy of Brønsted and Lewis acid sites. This work reports a Ga-modified ZSM-5 zeolite (GaAlZ5) with optimized acid properties and pore structure, which delivers 66.1% propane conversion and 85.6% aromatics selectivity with excellent recyclability, providing a facile approach for light alkane valorization.
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高影响因子
JOURNAL OF MATERIALS RESEARCH
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2022
·Vol. 37
·期 2
·543-553
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IF 2.909
Jia Yanfei,Wei Jianwen,Yuan Yuan,Geng Linlin,Chen Siqi,Liao Lei
A stable and effective amine-modified adsorbent for CO 2 capture was prepared with the impregnation method using the ZSM-5/SBA-16 (ZS) as support and the tetraethylenepentamine (TEPA) as modifier. The CO 2 adsorption performance was investigated by thermal gravimetric analysis (TGA) in mixed gases (15% CO 2 and 85% N 2 ) at 30–90 °C. At 60 °C, the ZS displayed the highest CO 2 adsorption capacity of 2.80 mmol g −1 at 60% TEPA loading. The adsorption kinetics analysis showed that the adsorption process of amine-modified ZS was dominated by both physical and chemical adsorptions. After five cycles of adsorption/desorption, ZS-T-60 kept better stability with the equilibrium adsorption capacity of the composite material was 2.486 mmol g −1 , which was 11.1% lower than the original adsorption capacity. The composite material ZS showed good CO 2 capture ability, indicating the promising future of these adsorbents for CO 2 adsorption from actual flue gas after desulfurization. Graphical abstract
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Xiuli Shao,Siqi Wang,Youhui Zhou,Xuan Zhang,Haizhou Tian,Zheng Wang,Zhong-Yong Yuan,Huanting Wang
The ZSM-5 zeolite nanosheets are highly desired materials for catalytic reactions and membrane separation . Their synthesis depends on specially designed complex surfactants ; however, the high-cost limits their large-scale industrial production. Herein, the tailored synthesis of coffin-shaped multilamellar ZSM-5 composed of orderly stacked 2D nanosheets is carried out using cetyltrimethylammonium bromide (CTAB) as a structure-directing agent (SDA) in the presence of silicalite-1 seed sol. The morphology and b -axis thickness of nanosheets is controlled by adjusting the amount of silicalite-1 seed sol, CTAB/TEOS ratio, SiO 2 /Al 2 O 3 ratio, and synthesis time. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) analysis indicate that the hydrophobic tail of CTAB acts as an inhibitor, effectively preventing the continuous growth along b -direction with an average thickness of 20–100 nm. This work highlights the role of silicalite-1 seed sol and CTAB in the orderly stacked sheets growth process. This crystallization strategy opens a facile and inexpensive approach for multilamellar ZSM-5 zeolite fabrication with 2D-nanosheets structures, and their practical applications in catalytic conversions of bulky molecules.
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高影响因子
RSC Advances
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2020
·Vol. 10
·期 50
·29618-29626
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IF 3.119
Yanming Jia,Qinghua Shi,Junwen Wang,Chuanmin Ding,Kan Zhang
Hierarchical nano-ZSM-5 zeolites (Z5-X) with different grain sizes were synthesized by varying amounts of 3-glycidoxypropyltrimethoxysilane (KH-560) in the hydrothermal synthesis strategy. Moreover, the conventional ZSM-5zeolite(Z5), which was prepared without KH-560, was used as the reference sample. The crystalline phases, morphologies, porous characteristics, Si/Al molar ratios and acidic properties of all fresh catalysts were characterized using the X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR), scanning electron microscopy (SEM), N2 adsorption–desorption, inductively coupled plasma atomic emission spectroscopy (ICP) and temperature programmed desorption of ammonia (NH3-TPD) techniques. Results show that the grain size and strong acid amount of zeolite decreased with the increasing amount of KH-560. The micropore surface areas and the corresponding volume of Z5-X changed less compared with Z5. Consequently, the high shape-selectivity of zeolite was preserved well under the addition of KH-560. However, the mesopore surface areas and the corresponding volume increased significantly with the increasing amount of KH-560. Benefiting from the abundant hierarchical structure, the Z5-X catalysts exhibited a larger coke capacity than the Z5 catalyst. The coke depositions of all the deactivated catalysts were characterized by the thermogravimetric technique (TG), and the results are indicative of the decreased average rate of coke deposition with an increasing amount of KH-560, which could result from the gradually reduced strong acid amount and the nano-sized crystallites. The catalytic performance of methanol-to-aromatics (MTA) indicates that the Z5-0.12 catalyst exhibited higher catalytic activity and selectivity of BTX as the reaction was prolonged, which could result from the synergistic effect among the proper strong acid amount, the smaller zeolite grain size, and the abundant hierarchical structure.
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DOI
PubMed
高影响因子
ADVANCES IN POLYMER TECHNOLOGY
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2020
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IF 1.539
Yunlong Liu,Jie Guo,Zhuobing Xiao,Dazhao Peng,Ke Song
Separation and purification of active components from biomass by inorganic materials during the pretreatment process of hydrothermal conversion are studied in this work. The batch experiment results show that an initial solution pH of 6 favors chelerythrine adsorption, and the optimum adsorbent dosage is 2.0 g. The adsorption mechanism of ZSM-5 for chelerythrine is investigated by adsorption kinetics, isotherm adsorption models, and thermodynamics analysis. The results show that the kinetics data fit the pseudo-second-order model well (R2 = 0.9991), and the intraparticle diffusion model has 3 diffusion stages, preliminarily indicating that chemisorption plays a major role in the adsorption process, and the sorption mechanism includes intraparticle, external, and boundary diffusion. The adsorption isotherms agree well with the Langmuir model, indicating the occurrence of monolayer molecular adsorption during the adsorption process. Meanwhile, the maximum adsorption capacity is 2.327, 2.072, and 1.877 mg/g at different temperatures (288 K, 298 K, and 308 K), respectively. The thermodynamic data demonstrate that the adsorption process is exothermic and spontaneous in nature. These observed results clearly confirm that ZSM-5 has potential superior properties for the enrichment and purification of alkaloids during the pretreatment of biomass.
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DOI
高影响因子
SOLID STATE SCIENCES
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2017
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IF 1.811
Yisong Wang,Tao Du,Yanli Song,Shuai Che,Xin Fang,Lifeng Zhou
ZSM-5 type zeolite with mesoporous structure was prepared and then amine-functionalized with tetraethylenepentamine (TEPA) by wet impregnation method to form a series of CO 2 adsorbents (ZTx). The structural properties of ZSM-5 and ZTx were characterized by XRD , FTIR , TGA/DTG, nitrogen adsorption/desorption, SEM and EDX techniques. The adsorption capacity of the adsorbents with different amine loading was measured at a temperature from 40 to 100 °C and the adsorption capacity of ZT7 was 1.80 mmol/g at 100 °C. The adsorption process and mechanism were studied by fitting the experimental data used the three adsorption kinetic models, and a complex physical and chemical mixing process was produced as the amine entered the surface and pore size of the zeolite. The high adsorption selectivity at 10% CO 2 concentration and the stability of the five adsorption desorption cycles indicated that ZT7 is a suitable and promising CO 2 adsorbent for the purification of industrial flue gas .
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高影响因子
Chem
·
2022
·
IF 25.832
Bo Wu,Tiejun Lin,Zhengxing Lu,Xing Yu,Min Huang,Ruoou Yang,Caiqi Wang,Chen Tian,Jiong Li,Yuhan Sun,Liangshu Zhong
Summary The direct conversion of methane to C2 oxygenates with high selectivity under mild conditions has attracted wide attention but still remains a great challenge. Herein, we report the conversion of methane to acetic acid (CH 3 COOH) with ultrahigh selectivity for oxygenated products by the direct coupling of CH 4 , CO, and H 2 O 2 over ZSM-5-supported Fe binuclear sites under 30°C. The unexpected ultrahigh selectivity toward CH 3 COOH was attributed to the unique Fe binuclear site structure of [Fe(III)–( μ O) 2 –Fe(III)–(OH) 2 ], which was evidenced by advanced spectroscopic techniques and density functional theory (DFT) calculations. It was suggested that the lower energy barriers for the direct coupling of methyl radicals (·CH 3 ) and adsorbed CO∗ and OH∗ species to form CH 3 COOH, compared with the oxidation of CH 4 by OH∗ to form CH 3 OH, benefited the CH 3 COOH formation.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
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2019
·Vol. 91
·期 1
·54-62
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IF 1.986
Deng Senlin,Zhang Xubin,Lv Guojun,Zhai Yi,Yang Zebin,Zhu Yongqiang,Li Haichao,Wang Fumin
Fe-doped zeolites with Mobil Five (MFI) structure have been widely used as heterogeneous Fenton catalysts to eliminate dyes from wastewater. However, the influence of carriers on degradation efficiency has not been reported yet. In this work, we have prepared three Fe-doped zeolite catalysts, FeS-1, FeZSM-5, and FeTS-1, with silicalite-1 (S-1), zeolite socony mobil-5 (ZSM-5), and titanium silicalite-1 (TS-1) as carriers, respectively. Characterizations, such as X-ray diffraction (XRD), scanning electron microscopy, energy-disperse X-ray spectroscopy, Fourier transform infrared spectroscopy, ultraviolet-visible diffuse reflection spectroscopy (UV–Vis DRS), X-ray fluorescence spectrometer, zeta potential, and N 2 adsorption/desorption isotherms, were used to investigate the morphologies and physicochemical properties of the synthesized materials. The catalytic performances of all zeolite catalysts were evaluated in the degradation experiments. The results depicted that the degradation efficiency of FeZSM-5 was higher than that of FeS-1 and FeTS-1 owing to its higher hydrophilic property, larger external specific surface area, and more negative zeta potential value. Therefore, the ZSM-5 could be a more suitable solid matrix for heterogeneous Fenton reactions than S-1 and TS-1.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Yuxia Zhu,Yuze Zu,Wei Xu,Yinghui Sun,Ying Li,Jie Bai
Coal gangue, the primary solid waste generated during coal mining, is mainly composed of silicon and aluminum oxide. Achieving its high-value utilization is crucial for resource recycling and sustainable development. In this study, we developed a method to synthesize ZSM-5 zeolite (ZSM-5-CG) using coal gangue as the sole silica–alumina source. The synthesis process, crystal growth mechanism, and catalytic performance of the resulting zeolites were systematically investigated. Compared with ZSM-5 prepared from commercial raw materials (ZSM-5-C), the coal gangue-derived synthesis required a significantly lower amount of template due to the favorable interaction between gangue-derived species and the template. Although crystallization in both systems follows the “solid–liquid phase transformation” mechanism, coal gangue, as a natural mineral source, exhibits significant differences in Si and Al coordination environment compared to commercial inorganic raw materials. These differences alter the dissolution and migration behaviors of Si and Al species in the mother liquor, leading to a synchronous release of these components during crystallization. As a result, nucleation and crystal growth processes happen more slowly, yielding a lower overall growth rate than that observed in systems derived from commercial raw materials. The obtained ZSM-5-CG was further applied in CO2 cycloaddition and methanation reactions, exhibiting catalytic activity comparable to that of ZSM-5-C, owing to its abundance of acid sites and large surface area. A cost analysis revealed that the total production cost of ZSM-5-CG was 29.7% lower than that of ZSM-5-C. This work provides a novel and economically viable route for the high-value utilization of coal gangue and highlights the potential of ZSM-5-CG in CO2 catalytic conversion.
研究领域:
材料科学
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催化化学
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环境化学
·
可持续工程
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高影响因子
Materials Chemistry Frontiers
·
2026
·
IF 8.1
Jiayu Yu,Di Pan,Ke Du,Wei Chen,Jian Zhou,Yi Tang,Yahong Zhang
Passivation of external surface acid sites in zeolites is a widely used strategy to enhance catalytic stability and to mitigate undesired non-shape-selective reactions. However, synthesizing zeolites with a uniform and thickness-controllable Si-zoned shell in a true one-pot manner remains highly challenging. Here, we develop an ethanol-mediated one-pot route to synthesize surface Si-zoned ZSM-5 zeolites. Ethanol establishes a favorable synthesis environment that promotes a classical, layer-by-layer crystallization pathway and enables the near-quantitative utilization of aluminosilicate species during the initial crystallization stage. This complete consumption of framework-forming species allows soluble silicate species to be subsequently added directly into the mother liquor, where they are selectively incorporated onto the preformed ZSM-5 crystals to build a thickness-tunable silica-rich shell. Notably, bulk and surface analyses together with bulky-probe reactions confirm that the silica-rich shell is structurally continuous and catalytically inert. This ethanol-assisted strategy offers a facile, high-yield, and scalable one-pot platform for engineering surface compositions in zeolites. The resulting surface Si-zoned ZSM-5 offers a versatile basis for the design of catalysts with improved stability and shape-selectivity.
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高影响因子
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