EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2018
·Vol. 2019
·期 1
·51-58
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IF 2.507
Hangle Guo,Tongguang Ge,Jian Lv,Changlin Du,Jian Zhou,Zhicheng Liu,Zile Hua
Graphical A facile and eco-friendly mesoporogen-free steam-assisted crystallization strategy has been developed for the synthesis of hierarchically structured ZSM-5 zeolites with superior MTP catalytic performance, and a new “in situ alkali etching-hydrothermal restoring“ mechanism is discussed. A series of hierarchically structured ZSM-5 zeolites (ZSM-5 HSZs) with a Si/Al ratio of about 200 have been successfully synthesized in the absence of additional mesoporous agents. XRD, N 2 sorption isotherms, SEM, TEM and NH 3 -TPD results showed that the obtained HSZs materials possess high crystallinity, interconnected micro/mesoporous structures and similar total acid amounts. Meanwhile, in the methanol-to-propylene (MTP) reaction, compared to the microporous counterpart, all synthesized ZSM-5 HSZs demonstrated superior performance benefitting from their hierarchical porous structures. Interestingly, 27 Al MAS NMR and Py-FTIR results confirmed the inter-transformation of framework and extra-framework Al species with the extension of materials crystallization duration and consequently the variation of materials surface acidity. As a result, the optimized catalyst achieved the highest initial propylene selectivity of 54.4 % and the longest catalyst lifetime ( t 90 ) of 175 h under the weight hourly space velocity (WHSV) of 1.0 g g –1 h –1 . Moreover, a new “in situ alkali etching-hydrothermal restoring“ mechanism has been proposed to elucidate the structural evolution of here reported high-silica ZSM-5 HSZs during the synthesis.
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Biomass Conversion and Biorefinery
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2025
·
IF 4.1
Mubashir Tayyaba,Farrukh Aftab,Hassan Najam Ul,Mahmood Rashid,Nasir Zonaira,Tahir Mudassir Hussain
This study investigates the effectiveness of a two-stage process aimed at achieving sustainable aromatic production through the co-pyrolysis of biomass and plastic, followed by catalytic reforming utilizing an Fe-modified ZSM-5 catalyst. To characterize the thermal decomposition behavior and monitor the progression of volatile compounds during the co-pyrolysis process, we employed thermogravimetric analysis (TGA) in conjunction with Fourier transform infrared (FTIR) spectroscopy and gas chromatography-mass spectrometry (GC–MS). Additionally, we conducted a compositional analysis of the resultant bio-oil. This study demonstrates that the co-pyrolysis process, employing a catalyst-to-feedstock ratio of 1:1 with the 10Fe/ZSM-5 catalyst (10 wt.% Fe loading), significantly increases the yield of aromatic hydrocarbons to 67.38%. This yield is markedly higher compared to the aromatic hydrocarbon yield of 55.37% obtained from catalytic pyrolysis of biomass alone. Moreover, these findings highlight the potential of this integrated methodology as a promising pathway for transforming waste materials into value-added chemicals, thereby improving bio-oil quality through the enrichment of aromatic compounds.
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FUEL
·
2025
·
IF 7.5
Huiyu Liu,Ying Qiu,Rui Shan,Jun Zhang,Haoran Yuan,Yong Chen
Catalytic fast pyrolysis (CFP) using bimetallic modified ZSM-5 enables efficient upcycling of polyethylene (PE). The present study demonstrates that alkaline sites significantly enhanced the mass transfer capacity of catalysts through generating fragmented structures, thus contributing to the selective regulation of thermal decomposition behavior of PE. Specifically, CuZn/ZSM-5 reduced decomposition temperature range by > 100 °C via enhanced chain-cracking and product transport. The synergistic effects of Cu 0 and alkaline sites derived from Zn species facilitated the cleavage of C–C bonds under a high heating rate, thereby accelerating the formation of olefin intermediates as well as promoting the aromatization within ZSM-5 channels. CuZn/ZSM-5 optimally combined highly dispersed metal sites, abundant strong alkaline sites, moderate acidic sites, and reinforced diffusion capacity, boosting low-temperature aromatics selectivity by 29.7 %, particularly for monocyclic aromatic hydrocarbons (MAHs). Despite the highest alkalinity of CuMg/ZSM-5, the permanent loss of weak alkaline sites at high temperatures resulted in weak capacity for aromatization. In addition, the plausible pathway for fast pyrolysis of PE into aromatics over CuZn/ZSM-5 was proposed.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2024
·Vol. 50
·期 7
·3033-3052
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IF 2.8
Huang Guihua,Yang Zizhen,Li Sijia,Wang Zhengwei,Xu Jundong,Zheng Shuqin
In-situ crystallization was used to prepare the composite molecular sieve ZSM-5/MOR (Z/M) successfully, and FeLa-ZSM-5/MOR (FeLa-Z/M) was obtained by loading Fe and La on the surface of the composite molecular sieve by hydrothermal method. The composite molecular sieve combined the water absorption of mordenite (MOR) and the mass transfer performance of ZSM-5, and effectively improved the surface area and porous structure. This zeolite improved the dispersion performance of active sites in Z/M and reduced mutual aggregation between particles, which was conducive to catalytic efficiency. The addition of La increases the number of oxygen vacancies, according to XRD, TEM, XPS, UV-DRS, and other data analyses. Because doping of La stretched the Fe–O bond, reduced the oxygen vacancies’ formation energy, and promoted oxygen vacancies’ formation, which was an essential reason for Fe 3+ reduction and Fe 3 O 4 formation. The addition of La also had a highly dispersed effect on Fe. Under the optimal conditions, with a FeLa mass ratio of 1:1, FeLa-Z/M at 25 mg, H 2 O 2 at 0.5 ml, and a pH of 3, the degradation rate of IC was found to be 97.8% and 99.5% in 5 min and 10 min respectively. Analysis of the reaction indicated that the catalyst followed a first-order reaction kinetic. Free radical quenching experiments confirmed that the main free radicals in the FeLa-Z/M Fenton-like system were hydroxyl radicals (·OH), suggesting a possible catalytic mechanism. Furthermore, the synthesized FeLa-Z/M catalyst exhibited superior performance compared to other methods of IC removal, demonstrating high reusability and efficient degradation even after multiple uses. Graphical abstract
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SOLID STATE SCIENCES
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2025
·
IF 3.3
Yanlin Wang,Hao Liu,Haoyu Liu,Hong Yuan
A series of nanosized ZSM-5 (SNZSM-5) zeolites has been synthesized by the seed-assisted method using silicalite-1 as seeds. Catalytic cracking of oleic acid to produce light olefins and light aromatics using SNZSM-5 as the catalyst was performed using a laboratory-scale fixed-bed reactor. The effects of the crystallization time and Si/Al molar ratio on the morphology and multilamellar structure of SNZSM-5 were studied to reveal how these properties affect the catalytic performance. Scanning electron microscopy, transmission electron microscopy, X-ray diffraction, temperature-programmed desorption of ammonia, and N 2 physisorption and desorption were performed to characterize the morphological features, acidities, and pore structures of the SNZSM-5 nanozeolites. Compared with conventional ZSM-5 zeolite, the SNZSM-5 nanozeolites possessed smaller particle diameters (90–450 nm), and they thus contained more intercrystalline voids. The Brunauer–Emmett–Teller surface areas (211–309 m 2 g −1 ) and mesopore volumes (0.08–0.27 cm 3 g −1 ) were both higher than those of ZSM-5 zeolite. Moreover, owing to the larger specific surface areas of the nanocrystals, more acidic sites can be exposed. Therefore, the SNZSM-5 nanozeolites showed higher catalytic activity and stability than conventional ZSM-5. The catalytic activity could be sustained for up to 35 h. Under the conditions of a reaction temperature of 500 °C, an oleic acid flow rate of 0.04 mL min −1 , and a nitrogen flow rate of 30 mL min −1 , the SNZSM-5 nanozeolite prepared with a Si/Al molar ratio of 16 showed the highest catalytic activity, producing up to 67 % yield of light olefins and showing 14.5 % selectivity for light aromatics.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Lei Wu,Kun Zhang,Qiuyan Ye,Yingjie Lv,Jiaqiao Li,Xiaoyan Guo,Yongnan Chen,Yiming Chen
Titanium alloys exhibit excellent mechanical properties, good corrosion resistance and biocompatibility, making they widely used in medical field. Nevertheless, their practical application is frequently constrained by bacterial infection and corrosion issues in physiological environments. To overcome these challenges, this study proposes a novel multifunctional strategy involving the incorporation of Ag + -loaded ZSM-5 zeolites into a micro-arc oxidated (MAO) coating on the surface of titanium alloy to fabricate Ag/ZSM-5@MAO-Ti composite coating. The microstructure, mechanical properties, and functional characteristics of the coating were systematically characterized. Analysis confirmed that Ag/ZSM-5 were evenly dispersed within the MAO coating while preserving the crystal structure intact. By leveraging the mechanical interlocking effect, the particles were securely retained within the micropores of the MAO layer after in-situ hydrothermal secondary growth. The composite coating exhibited exceptional adhesion to the titanium alloy substrate, with an average bond strength of 64 N. Owing to the inherent hydrophilicity of zeolites, the composite coating demonstrated significantly enhanced hydrophilicity with a contact angle of 12.9±0.7°. Antimicrobial tests results revealed that the coating achieved an inhibition rate of more than 99.99% against Escherichia coli (E. coli), and the sustained release of Ag⁺ ensures long-term antimicrobial efficacy. Furthermore, the composite coating displayed superior corrosion resistance in phosphate buffer solution (PBS). In summary, the Ag/ZSM-5 modified MAO coating substantially enhances the antimicrobial properties and corrosion resistance of titanium alloy, offering a promising strategy for the development of advanced medical devices.
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Catalysts
·
2025
·Vol. 15
·期 3
·277
·
IF 4
Yunhan Pu,Huajie Zhang,Yanjun Li,Chuan Yu,Xiaofei Song,Chen Yang,Mingli Fu
The conversion of methane (CH4) to methanol (CH3OH) under mild conditions remains a significant challenge in catalysis. In this study, we introduce a method to adjust the surface valence states of copper species in Cu-ZSM-5 catalysts by annealing under different atmospheres (N2, air, and H2). Among these, the 10% Cu-ZSM-5 catalyst calcined in H2showed outstanding performance, achieving a methanol productivity of 8.08 mmol/(gcat·h) and 91% selectivity at 70 °C and 3 MPa using H2O2as the oxidant. Comprehensive characterization revealed that H2annealing optimized the Cu surface to a lower valence state (predominantly Cu+), enhancing CH4adsorption and promoting H2O2activation to generate ·OH and ·CH3radicals, which drive selective CH3OH formation. In situ DRIFTS and radical trapping experiments further confirmed the critical role of Cu+in facilitating C-H bond cleavage and suppressing overoxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Yimin Zhang,Yun Zu,Ke Yan,Yuan Zhu,Yibin Luo,Enhui Xing,Qiang Li,Lijuan Song,Tan Li,Yi Mei,Xingtian Shu
In this work, a "bottom-up" strategy was proposed to one-step, in-situ synthesize P@ZSM-5 zeolites in a sodium-free system by elaborately self-designed tetrapropylphosphonium hydroxide as a new member of MFI-type zeolite organic templates inventory, and the interaction of phosphorus species with framework aluminum was investigated in detail. Multiple advanced characterizations confirm that the tetrahedrally-coordinated bidentate P IV -O 2 -Al IV structures are precisely customized and uniformly scattered in the zeolite channels. After experiencing harsh hydrothermal treatment (100 %H 2 O, 800 °C, 17 h), this new structure endows excellent hydrothermal stability of zeolite (crystallinity retention beyond 95 %) and reinforces its Brønsted acidity. Furthermore, methanol-to-propylene tests show that directly synthetic P@ZSM-5 zeolite performs extraordinarily long lifetime (180 h, WHSV = 1 h −1 ), enviable propylene selectivity (60.4 %) and propylene/ethylene ratio ( ca. 4.3) compared to the counterparts, which is benefited from encouragingly olefinic cycle pathway. These findings afford value-filled opportunities in novel catalyst production mode and understandings for phosphorus-zeolite chemistry . Synopsis -A "bottom-up" strategy was demonstrated to one-step, in-situ synthesize P@ZSM-5 zeolite in a sodium-free system by elaborately self-designed tetrapropylphosphonium hydroxide. The resultant P@ZSM-5 catalyst with hyperuniformly-stable bidentate P IV -O 2 -Al IV structures exhibited extraordinarily long lifetime (180 h) and enviable propylene selectivity (60.4 %).
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Petroleum Science
·
2025
·
IF 6.1
Chuan-Hao Zhang,Qi Dong,Fei Wang,Ning-Yue Lu,Feng Yu,Bin-Bin Fan,Rui-Feng Li
Deep hydrogenation of polycyclic aromatic hydrocarbons (PAHs) into jet fuel is an important strategy for the upgrading of light cycle oil (LCO). Zeolite-supported metal catalysts have exhibited good catalytic performance for hydrogenation of PAHs under relatively mild conditions. However, the impacts of acidity variations in zeolite supports, arising from the differences in framework Al (Al F ) distribution on the catalytic behavior of zeolite-supported metal catalysts in the deep hydrogenation of PAHs remains unclear. Herein, two series of mesoporous ZSM-5 samples, that is ZSM-5-E- x and ZSM-5-F- x , with the differences in Al F distribution but similar Si/Al ratios, were prepared in the crystallization system with or without NaOH. The results of NH 3 -TPD, Pyridine-IR, N 2 adsorption-desorption and SEM reveal that two series of HZSM-5 samples have similar acid density and acid strength, textural properties, morphology and particle size. However, the results of XPS, 27 Al MAS NMR, 2,6-Ditert-butylpyridine-IR, catalytic cracking of 1,3,5-triisopropylbenzene and the controlled reactions as well as DFT calculation indicate that the higher enrichment degree of Al F on the external surface and the suitable arrangement mode of Al F in ten-membered ring (10-MR) of HZSM-5-F- x compared to HZSM-5-E- x in case of the similar Si/Al ratios, result in Pt/HZSM-5-F- x exhibiting remarkably-improved deep hydrogenation performance of phenanthrene (PHE) compared to Pt/HZSM-5-E- x . Particularly, the selectivity to perhydrophenanthrene (PHP) over Pt/HZSM-5-F-50 can reach above 99.0% at a conversion of PHE (>99.0%). Furthermore, Pt/HZSM-5-F-50 exhibits well reusability. This work helps to clarify the impact of Al F distribution in ZSM-5 on catalytic hydrogenation performance for PAHs, providing valuable guidance for design and development of efficient catalysts for the hydrogenation of PAHs.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2025
·
IF 6.2
Yingna Li,Muhammad Sajjad Ahmad,Pei Gao,Yu Zhang,Mingtao Yang,Xiaolan Zhao,Boxiong Shen
This study examined the catalytic pyrolysis of melon seed shell (MSS) using vanadium tungsten modified ZSM-5 (V/W-ZSM-5) through combined experimental and theoretical methods. Thermogravimetric analysis (TGA) with model-free kinetics revealed that the catalyst lowered the activation energy by about 10 % (184–194 kJ mol⁻¹) compared with non-catalytic pyrolysis. Thermodynamic assessment showed reduced entropy (ΔS) values for conversion fractions below 0.7, indicating a more ordered and energy-efficient pathway. Product distribution from Py-GC/MS confirmed enhanced selectivity, with levoglucosan and furfural yields increasing nearly 5-folds and 3-folds, respectively. Density functional theory (DFT) clarified the mechanistic pathways: levoglucosan formed primarily via glucose dehydration, while furfural production followed xylose ring-opening and nucleophilic conversion. Collectively, these findings demonstrate that V/W-ZSM-5 not only improves selectivity toward high-value products but also reduces both kinetic and thermodynamic barriers, highlighting its potential for sustainable biomass valorization.
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Asia-Pacific Journal of Chemical Engineering
·
2025
·
IF 1.6
Shuai Yan,Xin Pu,Zhiyong Qi,Xiaoran Zhang,Xiaoyu Zhou,Xin Han,Lei Ye,Xinglong Qin,Jichang Liu
m -Cresol and p -cresol cannot be effectively separated using conventional distillation because of their proximate boiling temperatures. This study investigated the adsorption separation of cresol using the short b -axis ZSM-5 synthesized via a urea-assisted method. In contrast to the ellipsoidal HZSM-5, which was approximately 1 μm in length, the thickness of the sheet-like HZSM-5 decreased to 36 nm, resulting in an increase in total cresol adsorption capacity from 76 to 122 mg/g. Applying the CLD method, an increase in the TEOS:HZSM-5 ratio from 0 to 0.83 resulted in the increase in p -cresol adsorption capacity from 69 to 106 mg/g, while m -cresol adsorption capacity dropped from 53 to 12 mg/g. The adsorption selectivity significantly rose from 1.3 to 9.7. The adsorption kinetics and isotherms demonstrated that the process was exothermic for p -cresol and endothermic for m -cresol.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Feng Wang,Yimin Zhang,Xinyu Xu,Yunxiang Nie,Binbin He,Yi Mei,Yun Zu
Low-valuable utilization and a massive accumulation of yellow phosphorus slag (YPS) have caused severe pollution in surrounding environments. Among numerous implementation strategies, the conversion of YPS into phosphorus-containing zeolites represents a promising approach for high value-added utilization. Herein, we report that P-ZSM-5 zeolites were successfully prepared from acid-leaching YPS in one step using a hydrothermal synthesis method. The obtained P-ZSM-5 zeolites exhibited high crystallinity, uniform crystal size (200–400 nm), and a large BET surface area (>400 m2/g). Accordingly, a nonclassical crystallization mechanism of P-ZSM-5 zeolites from the YPS was proposed by multiple advanced characterizations. Importantly, the presence of phosphorus not only induced framework Al sited in the straight/sinusoidal channels and improved the hydrothermal stability of the zeolite framework but also enhanced the Brønsted acidity. Under comparable conditions, the as-prepared P-ZSM-5(75) zeolite catalyst with a higher ratio of Brønsted/Lewis acid sites in the methanol-to-propylene reaction exhibited a considerable catalytic lifetime (30 h, WHSV = 6 h–1), high propylene selectivity (55.1%), and a propylene-to-ethylene ratio of 5.9. The advancement in P-ZSM-5 zeolites paves a novel way for more effective YPS utilization and driving sustainability in phosphorus-based chemical production.
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