ACS ES&T Engineering
·
2026
·
IF 6.3
Zhenyu Gu,Jianhai Lu,Huimin Xu,Yemin Zhao,Shan Gao,Qiguang Dai,Xiaole Weng,Zhongbiao Wu
A novel Fe-doped ZSM-5 nanosphere catalyst was synthesized via a complex-assisted dynamic two-stage hydrothermal method using Na2EDTA as a chelating agent, followed by calcination under an inert atmosphere. The resulting material (Fe-ZSM-5EDTA-Ar) featured a hierarchical spherical architecture assembled from nanorods, possessing a high surface area (up to 511 m2/g), hierarchical porosity, and uniform dispersion of Fe species within the zeolite framework. Structural and spectroscopic analyses confirmed the successful isomorphous substitution of Fe2+/Fe3+ with a high proportion into the framework of ZSM-5, which concurrently enhanced structural stability and effectively suppressed iron leaching. Fe-ZSM-5EDTA-Ar demonstrated exceptional efficacy in the heterogeneous Fenton degradation of chlorobenzene (CB) employing H2O2 as the oxidant. This catalyst uniquely integrated high adsorption affinity with outstanding catalytic activity, resulting in complete dechlorination elimination of the target pollutant under optimized reaction conditions. Quenching experiments and electron paramagnetic resonance (EPR) collectively demonstrated that hydroxyl radicals were the dominant reactive oxygen species, driving the degradation process. Furthermore, Fe-ZSM-5EDTA-Ar also exhibited excellent recyclability in multiple cycles with negligible activity and iron loss. This work provides a robust synthesis strategy for designing stable and efficient zeolite-based Fenton catalysts for the remediation of chlorinated organic wastewater.
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高影响因子
MOLECULES
·
2026
·Vol. 31
·期 17
·3084
·
IF 5.1
Shuyi Wu,Yanji Shi,Qihao Zheng,Jianle Yuan,Yilin Xiang,Yining Jiang,Jiaxing Zhang,Ajuan Zhou,Xinwen Guo
Low-cost synthesis of ZSM-5 zeolite is critical for its large-scale industrial application. Herein, a seed-assisted low-template hydrothermal route was employed to fabricate ZSM-5 zeolites. The regulatory effects of gradient crystallization temperatures on the crystallization kinetics, morphology, pore structure and acid properties of ZSM-5 were systematically investigated, and the structure–activity relationship linking temperature-driven evolution and catalytic behavior in benzene alkylation with methanol was established. The results reveal that increasing the crystallization temperature shortens the amorphous induction period, facilitates framework aluminum (Al) incorporation and increases the concentration of Brønsted acid sites. Meanwhile, crystallization temperature modulates the specific surface area and intercrystalline mesopore volume, thereby tuning the accessibility of acid sites and the mass transfer efficiency of reactants and products. The sample synthesized at a moderate temperature of 170 °C achieves an optimal balance between textural properties and acid concentration. Benefiting from its large specific surface area, abundant intercrystalline mesopores and high Brønsted acid concentration, the catalyst affords a benzene conversion of 69.1% and a methanol utilization of 79.1%, and maintains stable operation over 135 h on stream. The temperature-dependent regulation insights uncovered in this work facilitate low-cost synthesis of ZSM-5 and rational design of high-performance catalysts for aromatic alkylation.
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PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·Vol. 65
·期 33
·17553-17569
·
IF 3.9
Shi Ketao,Tang Ningjing,Xu Zhen,Zhu Youbing,Gong Ruidi,Jiao Nianming,Wang Hui
Bifunctional dehydrogenation-cracking
metal/zeolite catalysts
are
promising for the production of light olefins from alkanes, but their
activation commonly relies on high-temperature calcination. This conventional
activation can induce metal migration and aggregation, damage the
zeolite framework, reduce micropore accessibility, and alter the acid-site
distribution, thereby compromising the dehydrogenation-cracking synergy.
Herein, ion-exchanged Ag/ZSM-5 catalysts were activated by dielectric
barrier discharge (DBD) plasma as a mild alternative to thermal calcination
for nitrate removal and Ag-site reconstruction. Plasma activation
could effectively remove nitrate precursors while better preserving
the crystallinity, micropore accessibility, and acidity of ZSM-5.
More importantly, it suppressed Ag migration and aggregation, increased
the fraction of highly dispersed Ag + species associated
with exchange sites, and promoted a more favorable Brønsted/Lewis
acid balance. As a result, the plasma-activated Ag/ZSM-5 catalysts
exhibited enhanced catalytic performance in n -hexane
cracking, with higher selectivity to light olefins. At a low Ag loading,
the plasma-activated catalyst delivered a light-olefin selectivity
of 50.7% after 6 h of reaction, higher than those of the calcined
counterpart (46.8%) and parent ZSM-5 (34.7%). Meanwhile, it showed
slower deactivation during the 6 h fixed-bed reaction, together with
lower tendencies toward hydrogen transfer, aromatics formation, and
coke deposition.
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Molecular Catalysis
·
2021
·
IF 5.062
Jiarong Li,Zhe Liu,Guangfa Hu,Ruimin Gao,Ronglan Zhang,Jianshe Zhao
A series of hybrid catalyst PMoW@HKUST-1@ZSM-5-MCM-41 was prepared in which H 3 PMo 6 W 6 O 40 were supported in the pore of micro/mesoporous materials ZSM-5-MCM-41 and HKUST-1 by one-pot method. Five types of ZSM-5-MCM-41 were prepared and corresponding ODS catalysts PMOW@HKUST-1@ZSM-5-MCM-41 were synthesized. The prepared catalysts were characterized and the most efficient catalyst was selected by XRD, FT-IR, UV–vis, N 2 adsorption-desorption, SEM, TEM. The removal of DBT reached 98.13 % by using PMoW@HKUST-1@ZSM-5-MCM-41−2 under 60 °C with molecular oxygen as oxidant after 150 min. After desulfurization, the catalyst can be simply recovered and reused 7 times with an unnoticeable decrease in catalytic activity, indicating the successful combination of heteropolyacids and micro/mesoporous materials for desulfurization.
研究领域:
化学工程
·
催化材料
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高影响因子
Catalysts
·
2026
·Vol. 16
·期 3
·
IF 4.5
Yao He,Jie Zhang,Renhua Huang,Nanxin Li,Yunwu Zheng
CO2-assisted catalytic pyrolysis presents a viable and promising approach to addressing plastic waste pollution and mitigating climate change. However, the effects of the metal–catalyst combination mode and the spatial distance between metal–acid sites on catalytic performance remain unclear. In this study, the reaction behaviors of the configurations, Fe3O4and ZSM-5 in tandem catalysis (Fe3O4&HZ), their physical mixture (Fe3O4-HZ), and Fe-loaded ZSM-5 (Fe/HZ), were compared in polypropylene pyrolysis under a CO2atmosphere. The aromatic contents followed this order: Fe/HZ > Fe3O4-HZ > Fe3O4&HZ > ZSM-5 > Fe3O4. Specifically, Fe/HZ with the highest degree of metal–zeolite proximity achieved an aromatic content of 66.1%, significantly higher than the 34.2% obtained with Fe3O4&HZ, demonstrating that closer metal–acid proximity promoted aromatic formation. Moreover, Fe/HZ significantly reduced coke deposition. Based on characterization results from XRD, SEM, TEM, XPS, and NH3-TPD, the enhanced spatial proximity between metal and acid sites strengthened the functional synergy between iron-based redox sites and zeolitic Brønsted acid sites. This synergy facilitated the reverse water–gas shift reaction of CO2, which consumed hydrogen generated during aromatization and shifted the reaction equilibrium toward enhanced aromatic production. These findings would offer theoretical and strategic insights into the optimization of CO2-assisted catalytic pyrolysis systems for the sustainable upcycling of plastic waste.
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Surfaces and Interfaces
·
2022
·
IF 6.137
Weiquan Li,Die Hu,Ke Yin,Chenglong Yu,Bichun Huang
A series of hierarchical Ru-Ce/H-ZSM-5 were designed and synthesized using the sol-gel method, and they were applied as catalysts for the catalytic combustion of chlorobenzene. The pore diameter of the catalyst was adjusted using an amount of sodium alginate (SA). Among all of the catalysts synthesized, the 0.8 wt.%Ru-10 wt.%Ce/H-ZSM-5 catalyst with a crystallization recipe of 1SiO 2 : 0.02Al 2 O 3 : 0.15TPAOH: 0.04SA: 40H 2 O (named RCZA-0.04) exhibited the optimal catalytic activity, with the 90% conversion of chlorobenzene at 247 °C. In addition, the RCZA-0.04 catalyst maintained superb stability during a long-term reaction at 325 °C. The results of characterizations demonstrated that RCZA-0.04 possessed the largest mesoporous volume, which reduced the diffusion resistance of chlorobenzene and increased the dispersion of the active components, thereby enhancing the catalytic activities. Moreover, the RCZA-0.04 catalyst possessed a low Brønsted/Lewis ratio, which was conducive to the adsorption of chlorobenzene and the cleavage of the C Cl bond.
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高影响因子
FUEL
·
2023
·
IF 7.4
Xiao-Yan Zhao,Xue-Yu Ren,Yan-Jun Wang,Jing-Pei Cao,Zi-Meng He,Nai-Yu Yao,Hong-Cun Bai,Hou-Luo Cong
Direct conversion of lignite into light aromatics via catalytic fast pyrolysis is a great challenge because of severe catalyst deactivation and low aromatics yield. The tandem catalysis (1Zn@MCM-41 and ZSM-5) system was employed to promote the conversion of thermally-derived volatiles of lignite into aromatics at 600 °C. The mesoporous Zn-incorporated MCM-41 (xZn@MCM-41) with different doping amount of Zn was prepared with a one-pot hydrothermal procedure. The structure and the dispersion of Zn species of 1Zn@MCM-41 were systematically studied with XRD, SEM, BET, NH 3 -TPD and so on. The presence of 1Zn@MCM-41 significantly expands the lifetime of the microporous ZSM-5. Meanwhile, the yield of aromatics, especially benzene, is also increased to some extent. The content of the long-chain hydrocarbons and the phenolic compounds are decreased significantly after being cracked by the mesoporous 1Zn@MCM-41. More small molecules are able to contact with the active sites located in the micropores of ZSM-5 with the presence of Zn@MCM-41. In addition, the ZSM-5 in the tandem catalysts system presents an excellent stability. Therefore, this meso -microporous tandem catalysis system promotes the preferential cracking of macromolecular compounds, the cracked small molecules generated from which then contact with ZSM-5 to produce aromatics. This work provides a new perspective for the gradient catalyzing lignite-derived volatiles over a tandem catalysis system.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yuen Bai,Dongyang Liu,Liang Zhao,Jinsen Gao,Chunming Xu,Haitao Pang,Xuhui Gao
The influences of different B (Brønsted) acid site concentrations and the ratio of L (Lewis)/B (Brønsted) on the cracking pathways and product distributions in hexane cracking reactions as a model component of naphtha were investigated. The sodium-modified ZSM-5 catalysts were prepared by the wet impregnation method, and the Si–OH–Al groups of ZSM-5 were broken in the post-treatment process, resulting in a decrease in the number of strong B acid sites (SBAS) and an increase in the number of strong L acid sites (SLAS). The correlations between the n-hexane catalytic cracking reaction pathways and the catalyst acid properties were established. The reduced SBAS inhibits secondary reactions of light olefins such as hydrogen transfer, oligomerization, cyclization, and aromatization, while the increased SLAS and the ratio of SLAS/SBAS promoted the β scission reactions that significantly improved the yields of light olefins. Consequently, the appropriate SBAS and SLAS/SBAS ratios are desirable for the production of ethylene and propylene. The optimal SBAS concentration and SLAS/SBAS ratio ranged from 4.44 to 6.69 μmol/g and 9.18–11.86 for maximum ethylene and propylene yields of 16.14% and 14.63% in hexane catalytic pyrolysis reactions, respectively. Furthermore, the optimally prepared catalysts illustrated superior reactivities and catalytic stabilities in naphtha catalytic pyrolysis reactions under industrial conditions.
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高影响因子
Catalysts
·
2022
·Vol. 12
·期 3
·351
·
IF 4.501
Peng Wang,Xia Xiao,Yutong Pan,Zhen Zhao,Guiyuan Jiang,Zhongdong Zhang,Fanfang Meng,Yuming Li,Xiaoqiang Fan,Lian Kong,Zean Xie
The development of an effective strategy for synthesizing two-dimensional MFI zeolites has attracted more and more attention. Herein, nanosheet-stacked hierarchical ZSM-5 zeolite was obtained by a seed-assisted hydrothermal synthesis route using a small amount of [C18H37-N+(CH3)2-C6H12-N+(CH3)2-C6H12]Br2(C18-6-6Br2) as a zeolite structure-directing agent and triethylamine (TEA) as a zeolite growth modifier. By varying the molar ratio of C18-6-6Br2/TEA from 2.5/0 to 2.5/40, the morphologies and textural properties of the resultant HZ5-2.5/x catalysts were finely modulated. By increasing x from 5 to 40, the morphology of the HZ5-2.5/x changed from unilamellar assembly with narrowa–cplane to intertwined nanosheets with widea–cplane and multilamellar nanosheets with house-of-cards morphology. The thickness of these nanosheets was almost 8–10 nm. In addition, selectivity to light olefins reached 70.7% for the HZ5-2.5/10 catalyst, which was 6.6% higher than that for CZSM-5 (64.1%). Furthermore, the MFI zeolite nanosheets exhibited better anticoking stability within the 60 h reaction time compared to conventional ZSM-5 zeolite, which could be attributed to the short diffusion path and hierarchical porosity. This work will provide valuable insights into the rational design of novel zeolite catalysts for the efficient cracking of hydrocarbons.Keywords:ZSM-5;nanosheets;zeolite growth modifiers;catalytic cracking of n-octane;light olefins
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高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 13
·3348-3358
·
IF 7.779
He Han,Hong Yang,Anfeng Zhang,Limin Ren,Xiaowa Nie,Chaoqiu Chen,Min Liu,Chuan Shi,Chunshan Song,Xinwen Guo
This work aims to achieve high para-selectivity while maintaining catalytic stability for the alkylation of toluene with methanol to para-xylene over ZSM-5 catalysts under demanding reaction conditions. A high para-selectivity of greater than 97% is achieved by applying consecutive SiO2–P2O5–MgO (SPM) and SiO2 surface coatings on the surface of pristine ZSM-5. This surface modification passivates the external acid sites and at the same time narrows the pore openings of the ZSM-5 particles, which are both beneficial for the high para-selectivity. The catalytic stability of the surface modified catalysts is achieved by loading with metals including Pt, Ni and (Pt + Ni). This study shows that catalysts co-loaded with (Pt + Ni) exhibit superior catalytic stability, not only in pure H2 but also in a carrier gas containing a very low H2 fraction of 5% H2 and 95% Ar. This is because the co-existence of Pt and Ni effectively inhibits the formation of low-carbon olefins (the coke precursors) via the dehydrogenation of methanol to carbon oxides and the hydrogenation of olefins to paraffins. By studying the different locations of metal loading on the catalysts, this work also confirms that the most effective location of metal loading is on the external surface of the modified catalysts.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Guohao Xu,Xuedong Zhu
A core-shell structured Zn/SiO 2 @ZSM-5 catalyst was prepared by a hydrothermal coating method, and its physicochemical properties and catalytic performance in methane co-aromatization with propane were studied using a conventional solid catalyst (Zn/ZSM-5) as the comparison. Results revealed that methane was activated on Zn sites to form a large number of Zn methyl species and then incorporated during the aromatic formation process to promote the formation of aromatics. At a space velocity of 3600 mL g −1 h −1 and the reaction temperature of 550 ℃, the methane, propane conversion and the aromatics selectivity of Zn/SiO 2 @ZSM-5 catalyst were 7.9 %, 95.9 % and 88.1 %, respectively, which were higher than those of Zn/ZSM-5 catalyst by 2.8 %, 6.7 % and 6.8 %, respectively. The unique reaction pathway of core (Zn/SiO 2 , Zn sites)-shell (ZSM-5, acid sites) was mainly responsible for the superior performance in methane co-aromatization with propane. Meanwhile, the core-shell structured Zn/SiO 2 @ZSM-5 catalyst aroused the formation of distinct micro-macroporous system, which facilitated quick diffusion of desired products out of the intraframework channels and inhibited the formation of carbon deposits. These features of Zn/SiO 2 @ZSM-5 catalyst granted it superb diffusion ability and unique core-shell structure, which greatly enhanced the methane, propane conversion and aromatic selectivity together with a preeminent catalytic stability.
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高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2020
·
IF 3.35
Yue Zhou,Huiping Zhang,Ying Yan
CuO/ZSM-5/PSSF was synthesized by a combined wet lay-up papermaking, secondary growth and chemical vapor deposition (CVD) method for the catalytic oxidation of ethyl acetate in the fixed bed reactor. Ethanol and acetaldehyde are found during the oxidation and 3 wt% CuO/ZSM-5/PSSF catalyst exhibited the best performance with 90% conversion of 1500 ppm ethyl acetate at 254 °C with GHSV of 15,000 h −1 , and the CuO/ZSM-5/PSSF exhibits low byproducts selectivity compared to granular CuO/ZSM-5 catalyst. Furthermore, the 3 wt% CuO/ZSM-5/PSSF catalyst exhibits a high stability after being used at 262 °C for 48 h.
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