Chem Catalysis
·
2024
·
IF 11.5
Bin Chen,Shui Yang,Longmei Shang,Yiling Wu,Youting Wang,Jian Tian,Jiale Huang,Xiaodong Zhang,Qingbiao Li,Guowu Zhan
Biomass resources can be converted to biochemicals via the catalytic pyrolysis process, but conventional catalysts often suffer from severe deactivation due to coke formation. Here, a ternary Ni/bio-Z5 catalyst was constructed by integrating ZSM-5 and Ni components on a porous bio-SiO2 platform derived from rice husk. The Ni/bio-Z5 achieved 76% aromatic selectivity for the catalytic pyrolysis of soybean oil, corresponding to a space-time yield as high as 154.8 garom · h−1 · gcata−1. It is confirmed that the bio-SiO2 platform shortened the surface diffusion path of aromatics by co-diffusion, which then inhibited coke formation and significantly improved the catalyst stability. Moreover, the atomically dispersed Ni on ZSM-5 effectively promotes the aromatization of C2=-C6= by enhancing adsorption and acting as an oligomerization center for isoalkyl carbenium ions. The coupling of deoxygenation and aromatization reactions promotes the enhancement of aromatic selectivity through the formation of methyl-substituted cyclopentenone that can be readily converted to aromatics.
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Journal of Water Process Engineering
·
2024
·
IF 6.3
Jing Li,Suxia Ma,Nuo Xu
The pursuit of carbon peaking and carbon neutrality goals necessitates flexible operation and deep peaking of coal-fired units, thus placing heightened demands on nitrogen oxide (NO X ) emission control. Fly ash, a solid waste rich in silicon (Si) and aluminum (Al), should be fully leveraged, and the high-value synthesis of zeolite represents a viable utilization method. In this context, fly ash-based zeolite was prepared as a catalyst to facilitate the generation of active oxides from H 2 O 2 , combined with alkali solution absorption, to achieve efficient denitrification. This approach effectively transforms ‘waste to pollution’ mitigation. The optimal synthesis conditions for FA-ZSM-5 zeolite were established using the alkali fusion hydrothermal synthesis method, with fly ash as the raw material. The specified conditions were NaOH/FA = 1.2, SiO 2 /Al 2 O 3 = 40, H 2 O/Al 2 O 3 = 1325, TPAOH/Al 2 O 3 = 10, ZSM-5-seed addition of 5 %, and a hydrothermal temperature and time of 140 °C for 24 h. Experimental parameters were meticulously investigated to ascertain their impact on nitric oxide (NO) removal efficiency. The highest removal efficiency was achieved under specific conditions: a reaction temperature of 140 °C, an H 2 O 2 concentration of 6 %, a catalyst dose of 0.3 g, an NO concentration of 600 mg/m 3 , and an SO 2 concentration of 1000 mg/m 3 . Finally, analysis of the catalytic oxidation mechanism revealed that H 2 O 2 , when catalyzed by FA-ZSM-5 zeolite, generates ·OH radicals with strong oxidizing properties, thereby facilitating the oxidative removal of NO.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Xiangfei Ding,Youbing Zhu,Ketao Shi,Zhen Xu,Jian Chen,Zengxi Li,Hui Wang
ZSM-5 zeolite is extensively employed for hydrocarbons cracking to generate light olefins, and its acidity is closely related to the activity and product distribution. In this work, Al-Sn bimetallic ZSM-5 was prepared via a “one-pot” route. Characterizations, including XRD, UV–Vis, XPS, revealed that Sn species were mainly embedded into the zeolite framework as tetrahedral Sn (IV). Moreover, the Sn atoms promoted the formation of Lewis acid sites and reduced the Brønsted acid amount, which effectively inhibited occurrence of side reactions ( e.g. , aromatization, hydrogen transfer) and improved the selectivity of light olefins in n-hexane cracking. Light olefins yield over HZ5[100,200] (Si/Al = 100, Si/Sn = 200) reached 33.4 % due to the appropriate acid property, in comparison with only 15.4 % for HZ5[50,∞] (Si/Al = 50, Si/Sn=∞) containing system. Through optimization of reaction conditions, better catalytic performance (n-hexane conversion of 91.6 % and light olefins yield of 37.6 %) was obtained over HZ5[100,200] under 575 °C with WHSV of 2 h −1 .
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Clean Energy
·
2025
·
IF 3.7
Jiang Zhenhua,Xia Wei,Zhang Yanli,Wang Xinrui,Dong Mingyuan,Chen Kun,Liu Dong,Lu Baowang
This study aims to compare the catalytic performance of ZSM-5 and SAPO-34 zeolite catalysts in the conversion of ethanol. Through experiments conducted at different temperatures (773 K and 673 K), it was found that SAPO-34 initially exhibits superior propylene selectivity compared to ZSM-5. However, the propylene yield on SAPO-34 gradually decreases, while the ethylene yield increases with time on stream. density functional theory calculations were employed for the investigation of reaction mechanism. The results indicate that the SAPO-34 catalyst surface favors propylene desorption, which beneficial for its initial high propylene selectivity. Nevertheless, the smaller pore structure of SAPO-34 limits the effective diffusion of products, leading to product accumulation within the pores and potentially causing catalyst coking and deactivation. By combining the experimental results with theoretical calculation, this study not only explored the selectivity difference between SAPO-34 and H-ZSM-5 in ethanol conversion reaction, but also revealed the influence of different molecular sieve catalyst structures on product distribution and catalyst stability.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Le Xu,Peng Guo,Jie Xu,Boxiong Shen,Zhong Zhao
TiO 2 has been widely studied in photocatalytic VOCs oxidation but its photocatalytic activity is still unsatisfied due to poor visible light absorption, serious charge recombination and weak toluene adsorption . Herein, a composite catalyst (TiO 2 /ZSM-5) was constructed between TiO 2 and hierarchical ZSM-5 by ball milling for photocatalytic toluene oxidation. The optimal composite catalyst exhibited the toluene degradation efficiency of 91.08 %, which was 2.7 and 1.3 times than those of TiO 2 and TiO 2 /commercial ZSM-5. It showed that the strong interaction between TiO 2 and hierarchical ZSM-5 was established via the formation of Ti-O-Si bond, which decreased the band gap from 3.08 to 0.55 eV when compared with TiO 2 and was helpful for the enhanced charge separation. In addition, the mesoporous volume of hierarchical ZSM-5 was regulated by a dual-template method, making the mesoporous volume increased from 0.23 to 0.38 cm −3 g −1 when compared with TiO 2 /commercial ZSM-5, which improved the toluene adsorption capacity from 0.12 to 0.16 cm −3 g −1 . DFT calculation further indicated that the energy barrier of toluene oxidation and ring-opening reaction was reduced in the presence of hierarchical ZSM-5. This work provided a new catalyst design method to improve the photocatalytic activity by the synergy action of TiO 2 and ZSM-5.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zhen-Qiang Yu,Yao-Xin Xiao,Dong Liang,Che Zhao,Zhen Huang,Gang-Qi Cheng,Rui Shan,Hao-Ran Yuan,Yong Chen
The chemical upgrade of the waste polyester coating on the surface of aluminum cans to value-added products can not only decrease the release of toxic substances, but also improve the quality of aluminum in the recycling process. In this study, different types of zeolite molecular sieve catalysts loaded with Ni, Mo and Co were synthesized, and utilized in the rapid catalytic pyrolysis of polyester coating. Among them, the Ni/ZSM-5 achieved the maximum aromatic compounds yield of 68.43 % at 600 ℃. A series of characterization results demonstrated that the embedding of transition metals (like Ni) could promote the cyclization and aromatization of products through deoxidation and dehydrogenation reactions by changing the pore structure and increasing total acid content (Brønsted and Lewis acids) of the ZSM-5 molecular sieve. Meanwhile, the thermodynamics of polyester coating during catalytic pyrolysis was studied by thermogravimetric method. The average activation energy of Ni/ZSM-5 catalytic pyrolysis of polyester coating is 238.65 kJ/mol. Furthermore, even after being reused for over 5 cycles, the catalyst can still maintain a relatively high yield of aromatic compounds (exceeding 60 %). Finally, the mechanism for aromatic compounds formation from Ni-modified ZSM-5 in-situ catalyzed polyester coating pyrolysis was proposed. This work provided useful ideas for the subsequent treatment of solid wastes.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2025
·
IF 7.7
Shenghui Xia,Chen Chen,Jinhong Liu,Yu Zhang,Hui Zhang,Thomas Thundat,Ajit Khosla
Nitrogen dioxide (NO 2 ) is a highly toxic air pollutant that endangers human health, environmental sustainability, and ecosystems. To address this issue, we designed an inorganic heterogeneous interface by integrating ZSM-5 molecular sieves with MXene via a facile synthesis route. This unique architecture synergizes the dual cross-channel framework of ZSM-5 and the high electrical conductivity and abundant surface functional groups of MXene. This combination greatly enhances electron transfer kinetics, interfacial NO 2 adsorption, and gas sensing properties. The optimized MXene/ZSM-5 nanocomposite achieves an ultra-low NO 2 detection limit of 1 ppm. Its response is 79.78 % higher than that of original MXene. The nanocomposite also exhibits excellent stability and significant anti-interference properties. Correlation studies confirm consistent performance across humidity and atmospheric conditions. Density functional theory (DFT) calculations elucidated the charge transfer pathways and adsorption mechanisms at the atomic level that enhance sensitivity. By pioneering the MXene/ZSM-5 interface and systematically investigating its gas interaction kinetics, this work provides fundamental insights for designing next-generation MXene-based gas sensors.
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高影响因子
FUEL
·
2025
·
IF 7.5
Hucheng Ge,Yufei Gu,Feifei Liu,Yanmei Huang,Yuke Liu,Silin Wu,Yunshuang Hu,Zhixia Li,Hongfei Lin
The core–shell structured MCM-22/ZSM-5 zeolite (MZCS50) was synthesized through a combination of hydrothermal crystallization (to form the MCM-22 core) and steam-assisted crystallization (to form the ZSM-5 shell). The MCM-22 core exhibited lamellar cake-like shape with a diameter of 3 ∼ 4 µm, while the ZSM-5 shell consisted of aggregated nanoparticles. MZCS50 possessed a high specific surface area, a micropore-mesopore coexisting structure, and was Brønsted acid-dominant material. MZCS50 was used as a catalyst for the cracking of low-density polyethylene (LDPE) to produce BTEX (benzene, toluene, ethylbenzene and xylenes). The results showed that 550 °C was the optimal temperature for LDPE cracking. The maximum liquid yield achieved was 23.4 %, with selectivities to BTEX, xylenes and p -xylene of 79.8 %, 43.2 %, and 21.3 %, respectively. Repeated cracking experiments demonstrated that MZCS50 exhibited good stability and superior catalytic performance in converting toluene to xylenes and further transforming xylene isomers into p -xylene. These results indicate that the core–shell structured MZCS50 is a promising catalyst for converting plastic wastes into valuable p -xylene.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Haiwei Xu,Linghao Li,Jian Huang,Wei Wang,Siyu Yang,Haohao Gao,Suhui Chen,Haojian Zhang,Zile Hua
Hierarchically structured high-silica ZSM-5 nanozeolites with an average particle size of about 115 nm and abundant inter/intra-crystal mesopores were successfully synthesized via a new combination of dry-gel crystallization (DGC) and subsequent alkali-etching treatment. The alkali-etching process effectively introduced auxiliary intracrystal mesopores into the nanozeolite precursors, significantly increasing the specific surface area and total pore volume while maintaining appropriate surface acidity, which had been confirmed by comprehensive characterizations, e.g., XRD, N2 sorption isotherms, SEM, TEM, NMR, ICP-OES, and NH3-TPD. Benefiting from the developed three-dimensional interconnected micro/mesoporous structure, the resultant nanoZSM-5(200)_D catalyst exhibited superior performance in the methanol-to-propylene (MTP) reaction. It achieved 46% propylene selectivity and an exceptionally prolonged catalyst lifetime for 90% methanol conversion of 224 h (t90), which is approximately 3 times and 16 times that of the nanoZSM-5(200) precursor and purely microporous ZSM-5(200) counterpart, respectively. Additionally, the universality of the here-reported two-step procedure has also been proven, which offers a new choice for preparation of high-performance hierarchically structured zeolite catalysts.
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JOURNAL OF THE ENERGY INSTITUTE
·
2026
·
IF 6.5
Liqin Yang,Peng Lv,Jiaofei Wang,Xudong Song,Juntao Wei,Yonghui Bai,Weiguang Su,Guangsuo Yu
V 2 O 5 -modified hierarchical ZSM-5 catalysts were synthesized. • The catalysts enhanced deoxygenation during biomass pyrolysis. • The obtained bio-oil was enriched in aromatic hydrocarbons. • The bio-oil upgrading mechanism over the catalysts was elucidated. Biomass catalytic pyrolysis is a key technology for converting biomass into high-value bio-oil as a sustainable alternative to fossil resources. To address the limitations of conventional microporous zeolites, such as mass transfer constraints and insufficient deoxygenation capability during bio-oil upgrading, this study employed V 2 O 5 -modified hierarchical ZSM-5 zeolite as the catalyst and corn stover as the feedstock to investigate the catalytic upgrading process. A hierarchical ZSM-5 zeolite with intercrystalline mesopores was first prepared via a mechanical ball milling-recrystallization method, followed by V 2 O 5 loading using wet impregnation. The catalyst's structure and properties were systematically characterized. Fast catalytic pyrolysis experiments of corn stover showed that the Me 0.004 support possesses a well-defined hierarchical pore structure, which facilitates the diffusion and reaction of large molecules in bio-oil. The redox properties of V 2 O 5 promoted the catalytic deoxygenation of biomass macromolecules, yielding smaller molecular intermediates. These intermediates subsequently underwent a series of reactions, including Diels–Alder cyclization and dehydrogenative aromatization, leading to the formation of aromatic hydrocarbons (AHs) over the ZSM-5 catalyst. In particular, the V2/Me 0.004 catalyst achieved an aromatic hydrocarbon yield 1.94 times higher than that of conventional ZSM-5. Based on pyrolysis experiments with model compounds, possible reaction pathways for AHs formation from corn stover over the developed catalyst were proposed. This study provides a theoretical foundation and technical support for the production of high-value chemicals, contributing to the advancement of efficient biomass resource utilization. Download: Download high-res image (540KB) Download: Download full-size image
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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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高影响因子
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