MICROPOROUS AND MESOPOROUS MATERIALS
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2025
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IF 4.7
Zhan Liu,Jia-Min Lyu,Chun-Mu Guo,Zhi-Yi Hu,Ming-Hui Sun,Li-Hua Chen,Bao-Lian Su
Hierarchically porous zeolites, combining the intrinsic microporous catalytic properties and the enhanced meso-/macroporous access and transport, exhibit excellent performances in many highly efficient catalytic processes. The acidity and porosity are two key factors affecting the catalytic conversion, selectivity and lifetime. It is necessary to construct such hierarchically porous zeolite catalysts with adjustable acid active sites and pore properties in a wide range to meet the specific catalytic requirements. Herein, an ordered interconnected hierarchical ZSM-5 single crystal catalyst composed by zeolite sphere units stacking in face-centered cubic (FCC) arrangement has been used as the theoretical model to research the corresponding material properties on the enhancement of specific catalytic process. Specifically, the properties of acid sites and meso-/macropores can be accurately adjusted by facilely changing the SiO 2 /Al 2 O 3 molar ratio (100–1000) and the sphere unit size (180–580 nm), respectively. As a result, the benzyl alcohol liquid-phase catalytic ability markedly improved thanks to the optimized acidity and meso-/macropore size. The larger meso-/macropore size shows higher benzyl alcohol conversion, while the higher SiO 2 /Al 2 O 3 molar ratio exhibits higher alkylation product selectivity. This work illustrate that the targeted catalytic process can be effectively enhanced by adjusting the acidity and porosity within such ordered hierarchical ZSM-5 single crystal system.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yu Zhou,Ning Li,Caiping Ma,Xiaohua Shen,Xiaofeng Li,Baojun Wang,Lixia Ling
Ga-ZSM-5 zeolite has excellent performance for methanol to aromatics (MTA) reactions, but introducing Ga metal into ZSM-5 zeolite leads to a complex acid species. The present study investigated the effect of Ga metal content on the acid amount and MTA reaction products in the hydrothermal synthesis of Ga-ZSM-5 zeolite. Lewis acid mainly formed at a Ga/Al ratio below 2.0, and at a Ga/Al ratio higher than 2.0, framework Ga species formed, increasing Brønsted acid content. Ga 2.0 -ZSM-5 zeolite exhibited the lowest B/L acid ratio (0.48), excellent BTX selectivity (40.26%), and the highest H 2 selectivity (8.93%). This finding indicates the most pronounced synergistic hydrogenation of Brønsted and Lewis acids. Ga 3.0 -ZSM-5 produced more xylene with more Brønsted acid compared to Ga 1.0 -ZSM-5, although they both had the same B/L acid ratio. The alterations in acidic species at different content of Ga metal appear to be conducive to the regulation of acidity in Ga-ZSM-5 zeolites.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Qichao Lu,Jie Li,Chen Liang,Lei Liu,Jinxiang Dong
Under the dual pressures of oil depletion and low-carbon transition, Fischer-Tropsch synthesis (FTS) technology offers a viable option for producing high value-added lower (C 2 -C 4 ) hydrocarbons from non-oil sources. However, conventional Fe-based catalysts often suffer from deactivation due to carbon deposition and sintering. Here, we report a unique Fe-ZSM-5 catalyst synthesized by doping Fe into ZSM-5, which demonstrates excellent FTS catalytic performance. During high-temperature template removal, Fe species migrated from the zeolite framework to form highly dispersed FeO x clusters (∼2 nm). Upon treatment by syngas, these FeO x clusters aggregate to form uniformly small-sized Fe 5 C 2 @C core-shell particles distributed on ZSM-5 support. The confinement effect of the inter-crystalline structure effectively prevents the sintering of Fe 5 C 2 . The smaller Fe 5 C 2 particles exhibit controlled CO dissociation, reducing the concentration of activated carbon species (C*), and the carbon shells (∼6.5 nm) limit the departure of C*, effectively suppressing carbon deposition. This unique structure enables stable catalytic activity for over 100 hours with maintained product selectivity. The Fe-ZSM-5 catalyst achieved a C 2 -C 4 hydrocarbons selectivity of 54.52 %, nearing the 56 % theoretical limit of the Anderson-Schulz-Flory (ASF) distribution. Additionally, the hydrophobic carbon shell prevents excessive oxidation of Fe 5 C 2 , reducing CO 2 selectivity by ∼56 % compared to conventional Fe/ZSM-5 catalysts, significantly enhancing atomic utilization efficiency and aligning with the principles of green development.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jingkai Hu,Huaxin Lin,Zhuowei Cheng,Jianmeng Chen,Ruiqi Zhu,Dongzhi Chen,Zhaoyang Lu
Volatile organic compounds (VOCs), particularly toluene, pose significant environmental and health challenges. This study addresses the limitations of ZSM-5 zeolite in humid environments by integrating Si/Al ratio optimization with hydrophobic modification via layered double hydroxide (LDH) coatings. H-ZSM-5 zeolites with Si/Al ratios of 25, 85, and 300 were synthesized using hydrothermal methods, revealing that higher Si/Al ratios enhance specific surface area (387.67 m 2 /g for Si/Al = 300) and mesopore volume (66.4 %). However, humidity reduced the adsorption capacity (e.g., ZSM-5(300) decreased from 85.37 ± 3.60 to 65.76 ± 2.26 mg/g at 80 % RH). To mitigate moisture interference, three LDH-coated composites were fabricated: self-assembled (ZZ-300@LDH), co-precipitated (GC-300@LDH), and sol-gel-derived (RN-300@LDH). Among these, GC-300@LDH exhibited superior hydrophobicity (water contact angle: 53°) and a hierarchical pore structure (mesopore volume: 0.3688 cm 3 /g), achieving a toluene adsorption capacity of 94.43 ± 1.43 mg/g under 80 % RH—43.6 % higher than ZSM-5(300). The dual adsorption sites and enhanced surface roughness contribute to prolonged breakthrough time (6.6 ± 0.3 min) and stable regeneration over five cycles. Comparative analysis with industrial zeolites highlights GC-300@LDH's potential for integration into zeolite rotor-RTO systems, offering a scalable solution for humid industrial VOC treatment.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Nai-Yu Yao,Jing-Pei Cao,Shi-Jie Cai,Chen-Xu Chen,Xiao-Yan Zhao,Xin-Bo Pang,Min Xu,You Lu,Xiao-Bo Feng,Tungalagtamir Bold
ZSM-5 is an effective catalyst for the catalytic reforming of volatiles from lignite. An increased density of acidic sites significantly enhances catalytic activity. However, its inherent microporous structure and abundant external surface acids lead to issues including catalyst deactivation. In this work, a nondiscriminatory etching method using NH4F was employed to simultaneously remove Si and Al species from highly acidic zeolites. This process introduces mesopores while reducing external surface acidity, maintains high crystallinity, and preserves the total acid content essentially unchanged. The mesoporous surface area of HZ5-6.5 reaches 129 m2/g. This significantly enhances the mass transfer efficiency of volatile component molecules within the zeolite, effectively improving the accessibility of active sites. Furthermore, compared to the parent zeolite, the modified HZ5-6.5 exhibits a 50% reduction in acidic sites on its crystal surface while maintaining essentially unchanged total acidity. Concurrently, light aromatic yields increase, while coke deposition decreases by 40%.
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JOURNAL OF CATALYSIS
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2018
·
IF 6.759
Meng Pan,Jiajun Zheng,Yujian Liu,Weiwei Ning,Huiping Tian,Ruifeng Li
The conversion of the heavy fractions of crude oil into transportation fuels and chemical feedstocks is still a severe challenge for fluid catalytic cracking (FCC) technology, in which geometrical parameters of the catalyst are of key importance to the accessibility for reactant and product molecules to travel through the pore space. Here a new core-shell zeolite catalyst with hierarchical pore network from macro- via meso- to micropores is developed by controlling overgrowth of another zeolite shell on the surface of a commercial Y-zeolite. The zeolite shell is a distinctive nano ZSM-5 crystals. The core-shell zeolite catalyst has a high thermal and hydrothermal stability because of high crystallinity, which can meet the industrial requirements. More importantly, the heavy oil can be cracked by the designed zeolite catalyst step-by-step into the required products. The meso- and macroporous shell facilitates pre-cracking the large molecules in heavy oil into moderate ones which can directly diffuse into the micropores of the Y-zeolite to be cracked selectively into the desired products. Both the pore structure network and acid sites distribution of the core-shell zeolite catalyst in the FCC processing are completely harmonious. As a practical example, the catalytic cracking of VGO heavy oil is actualized over the new catalyst. The results showed that the conversion of heavy oil and the yield of gasoline increased by 1.8 wt% and 8.9 wt% respectively, LPG decreased by 6.9 wt%, iso -paraffins and olefins in gasoline fraction increased by 5.21 wt% and 6.31 wt% respectively, aromatics decreased by 11.55 wt%, because of the graduated cracking in core-shell zeolite and returned isomerization in nano ZSM-5, compared with commercially industrial FCC catalyst.
研究领域:
化学工程
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催化材料
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石油加工
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Guoqing Chen,Zhongchen Ma,Wenli Gu,Pu Liu,Tian Lan,Yong Lu
The direct production of sustainable aviation fuel (SAF) through Fischer−Tropsch synthesis (FTS) has garnered significant interest within the energy and petrochemical sectors. However, attaining high SAF selectivity remains a critical hurdle, as the inherent maximum selectivity for the C 8 −C 16 hydrocarbon fraction in traditional FTS process hovers around 41%. Here, we report a promising bifunctional catalyst system for FTS to SAF, featuring cobalt nanoparticles (Co NPs) embedded within amorphous silica (Co@ x Si) integrated with ZSM-5 zeolite. The optimal catalyst system was identified by combining Co@ 3 Si derived from an APTES-infused ZIF-67 (with a 3:1 mass ratio of APTES to ZIF-67) with two mass fractions of a ZSM-5 (Co@ 3 Si& 2 Z5). This formulation achieved a 75.2% selectivity to C 8 −C 16 hydrocarbons with an iso-paraffins proportion of 24.3%, while effectively minimizing CH 4 formation to 6.3%. It also sustained a high CO conversion of 85.1% and was stable for at least 168 h. The Co@ 3 Si, leveraging its abundant active cobalt sites and distinctive confined structure, not only improved CO adsorption and activation but also extended the residence time of −CH x intermediates on the surface of Co NPs, thereby efficiently facilitating the formation of long-chain hydrocarbons. The ZSM-5 zeolite facilitated the selective catalytic cracking and isomerization of long-chain hydrocarbons, effectively converting them into SAF-range paraffins. The collaborative synergy between the two core components forms an efficient catalytic process akin to an assembly line, enabling the highly selective direct transformation of syngas into SAF.
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Materials Today Chemistry
·
2026
·
IF 7.4
Guohao Xu
A facile desilication-recrystallization strategy is developed to fabricate b-axis oriented hollow nanosheet ZSM-5 zeolites. • Optimal catalyst achieves 94.4% propane conversion, 8.2% methane conversion and 80.1% aromatic selectivity in MPC reaction. • The catalyst exhibits a 100 h catalytic lifetime (10-fold that of commercial ZSM-5) with excellent regeneration stability. • In-situ IR and DFT calculations reveal the synergistic mechanism of methane-propane co-aromatization. A nanosheet ZSM-5 (∼100 nm thick) was synthesized via a facile desilication-recrystallization approach using silicalite-1 as a precursor for methane and propane co-aromatization (MPC). The Si/Al feed ratio was tuned by varying NaAlO 2 dosage to direct the structural evolution of the zeolite. The acid strength and acid amount gradually increased with decreasing the Si/Al ratio from 100 to 25. Under the suitable Si/Al ratio of 50, the resulting Zn-bZSM-5(50) catalyst possessed the proper acidity and the largest average pore diameter of 6.16 nm, which endowed it with optimal catalytic performance: achieving 94.4% propane conversion, 8.2% methane conversion, 80.1% total aromatics selectivity, and an extended catalytic lifetime of 100 h. Additionally, the catalyst displayed outstanding regeneration stability, with no significant decline in reactant conversion and aromatics selectivity after five consecutive reaction-regeneration cycles. The exceptional stability originated from the chemical anchoring of Zn species as isolated [ZnOH] + sites within the framework, which effectively suppressed Zn volatilization. In-situ infrared spectroscopy analysis revealed that the presence of methane, combined with the acidity and Zn species, promoted the formation of adsorbed reaction intermediates, thereby improving the reaction performance. Control experiments with varied feed compositions further confirmed the synergistic effect between methane and propane. Density functional theory (DFT) calculations demonstrated that the co-aromatization of methane and propane was more thermodynamically favorable for the conversion of methane, corroborating the experimental observations. These findings establish a rational design strategy for developing nanosheet ZSM-5 zeolites with the superior performance and a long lifetime for MPC reaction. Download: Download high-res image (269KB) Download: Download full-size image
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MICROPOROUS AND MESOPOROUS MATERIALS
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2026
·
IF 4.5
Rui Feng,Runxi Zhang,Dejun Shi,Hongyue Yu,Kebin Chi,Peng Peng,Xinlong Yan,Shijian Lu
Seed type controls the physiochemical properties of template-free DGC ZSM-5. • S1 seeding affords mesoporous nanocrystallite aggregates with moderate acidity. • S2 seeding favors Al occupation at straight and intersecting channels. • S2-derived catalyst achieves 94.1% conversion with >90% stability after 36 h. • S1-derived catalyst exhibits ultralow coking rate (0.056 h −1 ) and coke content (∼2.2 wt%). The template-free dry gel conversion (DGC) synthesis of zeolites typically suffers from poor crystallinity and limited structural tunability. In this study, we demonstrated that these limitations can be effectively overcome through a seed-assisted DGC strategy, employing colloidal S1, self-synthesized S2, and commercial ZSM-5 as seeds to direct ZSM-5 crystallization. Comprehensive characterization revealed that seed type critically influences crystallite size, mesoporosity, framework silica-to-alumina ratio (SAR), aluminum siting, and the distribution of Brønsted and Lewis acid sites. Specifically, S1 seeding afforded nanocrystallite aggregates with abundant mesopores, moderate acidity, and the highest SAR (106). S2 seeding resulted in intermediate crystallite dimensions, preferential Al occupation at straight and intersecting channels, and the highest Brønsted/Lewis ratio (6.1). In contrast, the seed-free system yielded dense, large-block crystallites with a lower SAR (65). In n-hexane cracking at 550 °C, the S2-derived catalyst (S2-DG-Z5) achieved the highest initial conversion (94.1%) and light olefin selectivity, while maintaining >90% conversion after 36 h, whereas the seed-free counterpart (DG-Z5) dropped from 90% to <80%. Meanwhile, the S1-derived catalyst (S1-DG-Z5) exhibited the lowest coking rate (0.056 h −1 ) and coke content (∼2.2 wt%), attributable to its moderate acidity, nanocrystallite morphology, and mesoporosity, which synergistically suppress coking and enhance mass transport. Collectively, these findings establish seed type as a pivotal parameter for tuning Al siting and acidity in template-free DG-synthesized ZSM-5, and highlight this seed-assisted route as an effective strategy for producing high-crystallinity, stable zeolite catalysts for hydrocarbon cracking. Download: Download high-res image (288KB) Download: Download full-size image
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Yidan Ouyang,Yongxuan Wang,Jingjing Kou,Junhui Cai,Ruijie Jin,Zehong Chen,Ruilan Xu,Zhengbao Wang,Yong Peng
Efficient adsorptive removal of dyes from aqueous solutions by solid porous materials depends on the number of adsorption sites and rapid mass transfer in the pore channel networks. In this work, alkaline coetching on conventional bulky ZSM-5 zeolite by tetrapropylammonium hydroxide and sodium metaaluminate was developed to produce hierarchical ZSM-5 zeolites with a hollow structure. The synergistic etching effect was systematically investigated by adjusting the etchant amount and etching conditions. The dissolution-protection reconciled etching mechanism was demonstrated, and a map illustrating the synergistic relationship was proposed. The etched zeolite exhibited a hierarchical pore structure with a high mesopore volume of 0.68 cm3 g–1 and a large pore size centered around 30 nm, which are beneficial for the mass transfer of large dye molecules. Besides, it had more silanol groups and a lower Si/Al ratio (11–15) with evenly distributed Al element, thus significantly increasing the active adsorption sites. The hierarchical hollow ZSM-5 zeolites presented a great adsorption capacity of 120.95 mg g–1 for methylene blue at a pH of 12 and a high rhodamine B uptake (23.84 mg g–1 under specified conditions). The synergistic etching method is expected to finely manipulate the microstructure of zeolite materials, which would expand their applications in many fields, such as adsorption and catalysis.
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高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 3
·80
·
IF 2.5
Li Xincheng,Huang Pengpeng,Fan Mingming,Zhang Pingbo
Isostearic acid, a bio-based and environmentally friendly chemical, has attracted considerable attention because of its high value as an oleic acid derivative. The synthesis of isostearic acid via oleic acid isomerization over commercial H-ZSM-5 zeolites is limited by low yield and acid value, mainly due to diffusion constraints. To address this issue, a hierarchical-pore H-ZSM-5 zeolite (Meso-5) was synthesized using Silicalite-1(S-1) as a seed crystal to enhance diffusion and catalytic performance. The catalyst was comprehensively characterized by XRD, SEM, BET, TGA, FT-IR, and Py-FTIR. Meso-5 efficiently catalyzed the isomerization of oleic acid, attributed to its abundant Brønsted and Lewis acid sites whose synergistic interaction significantly promoted the formation of branched-chain products. The catalyst delivered a selectivity of 87.3% with a 71.1% yield in the first run, and even after five reuse cycles it maintained 82.1% selectivity with a 55.6% yield. Evidently, the hierarchical pore structure of the catalyst significantly facilitated the diffusion of oleic acid molecules and their isomerized intermediates, thereby enhancing the overall catalytic activity. The resulting isostearic acid was purified via a simple recrystallization procedure to a purity of 83.4% and an acid value of 186.7 mg KOH/g, both meeting the standards of commercial isostearic acid. These findings provide a robust basis for further catalyst optimization and scale-up toward industrial isostearic acid production. Graphical A tandem catalytic route combining ZSM-5-driven isomerization with Ni/C-catalyzed hydrogenation enabled the efficient conversion of oleic acid to isostearic acid. The hierarchical H-ZSM-5 structure enhanced branched-chain formation, ensuring high selectivity and yield toward the desired product
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SURFACE & COATINGS TECHNOLOGY
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2022
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IF 4.865
Juan Du,Zhaolin Wang,Ziming Wei,Jiawei Yao,Haipeng Song
This paper investigated the preparation of new environmental, pH stimulation response nanocontainer enhanced, self-healing, and efficient anti-corrosion coating for aluminum alloy protection. Silane/Ce-ZSM-5 coating with improved morphology was successfully synthesized on aluminum alloy surface, through the new proposed “hydrothermal crystallization - ion exchange - self-assembled seed growth - hot pressing” technology, in which ZSM-5 molecular sieve was served as pH stimulation response nanocontainer. The corrosion resistance and self-healing ability of the coating in 3.5 wt% NaCl solution were further investigated by the combined analysis of SEM, EIS, LEIS , ICP-MS characterization and 3D microscopic observation. The experimental results showed that the prepared silane-Ce-ZSM-5 coatings exhibited excellent corrosion protection and self-healing ability, which was attributed to the pH stimulation release of corrosion inhibitor Ce 3+ when the coatings were damaged. The ZSM-5 zeolites generated Ce(OH) 3 or CeO 2 precipitates to gradually fill the aluminum alloy defects, thus forming a dense protective layer and inhibiting the corrosion activity.
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