DALTON TRANSACTIONS
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2025
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IF 3.3
Xue-Qing Xu,Shen Yu,Xing-Yu Yue,Zhan Liu,Jia-Min Lyu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
Phenol is an important intermediate for high value chemicals. Current phenol production via a three-step cumene process causes severe energy-waste and environmental problems. The conversion of benzene to phenol under mild condition can be achieved by oxidation with Cu-based zeolites. However, conventional microporous zeolite suffers from severe diffusion limitation, especially when bulky molecules are involved, such as benzene. In this work, we used a hierarchically macro-meso-microporous ZSM-5 single crystal (Hier-ZSM-5) as substrate for Cu species (Cu@Hier-ZSM-5). Irregular morphology of opal-like Hier-ZSM-5 exhibits abundant surface Si-OH groups and provides a platform for stabilizing Cu2+ sites. Meanwhile, hierarchical porosity provides significantly improved diffusion ability of bulky molecules. As a result, excellent selective oxidation performance of benzene was obtained with the Cu@Hier-ZSM-5, achieving a conversion of 77% and a phenol selectivity of 73%, which is 1.5 times and 2 times of these obtained with a catalyst based on a microporous ZSM-5, respectively. Species of CuOOH were identified as an important intermediate for benzene oxidation. This hierarchical zeolite system with a synergistic effect of site anchoring and molecular diffusion presents an excellent platform for catalyst design.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Jiaze Chen,Huijie Xie,Yusen Chen,Dong Guo,Binjie Li,Xuanxuan Sun,Volodymyr Turkevych,Caixia Li,Dehong Chen,Lei Wang,Bin Li
Fenton-like degradation based on iron catalyst have been developed to remove organic pollutants from wastewater. However, iron-based catalysts still face challenges of poor accessibility and stability of active sites. Here, we report a facile and green method for the preparation of Fe x Cu (1-x) @HZSM-5 catalyst using ethylenediamine as an organic ligand to stabilize metal species via a combination of solid-state grinding and steam-assisted crystallization methods without organic templates. Due to the confinement of zeolite ZSM-5 framework and synergistic effect of Fe and Cu bimetals, the optimized Fe 0.8 Cu 0.2 @HZSM-5 catalyst exhibits excellent activity and reusability in the Fenton-like degradation of methylene blue at the neutral condition. Our strategy for fabricating bimetal@zeolite can bring about new thoughts for the preparation of iron-based catalyst with high efficiency for Fenton-like degradation.
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Waste and Biomass Valorization
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2024
·
IF 2.6
Luo Bo,Liu Huiyu,Shan Rui,Zhang Jun,Yuan Haoran,Chen Yong
Purpose This work aims to investigate the thermal behavior and kinetic characteristics of polyethylene (PE) pyrolysis over Cu/Ce modified ZSM-5. The influences of metal types, particles size of active center and interaction of Cu–Ce species on products distribution are elucidated. Methods Metal-modified ZSM-5 catalysts were prepared by negative pressure impregnation method. Catalytic fast pyrolysis and thermogravimetric experiments were conducted using Py–GC/MS and TG/MS for the qualitative and quantitative analysis of pyrolysis products. Results Morphology characterization indicated the interaction of Cu–Ce species facilitated the regulation of active center size into a nanoparticle scale. The final products were restricted to a carbon number of less than 9 over CuCe/ZSM-5. Cu–Ce modification increased the aliphatic content from 58.5 to 76.1%. Kinetic analysis revealed a remarkable reduction in activation energies during both the intermediate and final stages, where an average decrease of 30% was achieved. Conclusion The synergistic effects of Cu 0 and CeO x facilitated the formation of more short chain olefins by enhancing C–C bonds cleavage activity. Undesired polycyclic aromatic hydrocarbons (PAHs) were avoided by the optimal steric hindrance of CuCe/ZSM-5. Graphical Abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Huiyu Liu,Chengyu Li,Rui Shan,Jun Zhang,Haoran Yuan,Yong Chen
The growing accumulation of waste polyethylene terephthalate (PET) has raised great concern about its effective upcycling. Catalytic fast pyrolysis is a promising method for selectively upcycling of waste PET into aromatics. However, the high temperature and poor mass transfer performance remain considerably challenging. In this research, a diffusion-enhanced hollow ZSM-5 catalyst with Ru modification was designed for low-temperature valorization of waste PET into aromatics. Ru species significantly enhanced the primary depolymerization of long-chain polymers by generating abundant Lewis acid sites, which markedly increased the aromatics content. Additionally, the mesopore-rich structure formed after Ru-modification improved diffusion capacity of products effectively. The existing of active Ru 0 species was beneficial to the hydro-upgrading of oxygen-containing intermediates, therefore monocyclic aromatic hydrocarbons (MAHs) content and hydrogen atom utilization increased to a great extent. More gratifyingly, the pyrolysis temperature for preparing aromatics from waste PET was obviously lowered, probably due to the synergistic effect of diffusion-enhanced structure and Ru modification. Ru/ZH exhibited higher aromatics yield of 46.4 wt% with selectivity of 95.3 % at 500 °C, resulting in a significant mass yield increase of 93.1 % compared to unmodified hollow ZSM-5 (24.0 wt%). Finally, the plausible pathway for PET-to-aromatics via catalytic fast pyrolysis over Ru/ZH was proposed.
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POWDER TECHNOLOGY
·
2025
·
IF 4.6
Yanting Zhou,Junchao Zhao,Tengfei Wang,Zhilei Yu,Yangyang Fu,Yong Jiang,Xudong Cheng,Heping Zhang
Despite the exceptional fire-suppressant capabilities of ultrafine dry powder fire extinguishing agents, additional work is essential to improve their overall fire-extinguishing performance. In this investigation, we explored the utility of Fe 3+ loaded ZSM-5 zeolite in enhancing the firefighting capabilities of ultrafine dry powder fire extinguishing agents. The loading of transition metal ions Fe 3+ onto the ZSM-5 zeolite was achieved through the ion solution exchange method. Interestingly, the loading of Fe element on Fe/ZSM-5 zeolite displayed a pattern of initial increase followed by decrease as the ion exchange time lengthened. Furthermore, the loading of Fe element on Fe/ZSM-5 zeolite was found to be influenced positively by the initial molar concentration of Fe 3+ and pH levels. Impressively, under specific working conditions, the prepared Fe/ZSM-5 zeolite demonstrated a substantial Fe element loading of 5.82 %. Incorporation of ZSM-5 zeolite resulted in a 10.01 % enhancement in the fire-extinguishing efficiency of the ultrafine dry powder compared to undoped samples. Moreover, the incorporation of Fe/ZSM-5 zeolite has resulted in an enhancement of fire extinguishing efficiency by 20.45 % (S3), 24.20 % (S4), and 29.04 % (S5) in comparison to S1. These findings contribute to the understanding that the incorporation of Fe/ZSM-5 zeolite significantly enhances the fire extinguishing performance of ultrafine dry powder fire extinguishing agents, with extinguishing efficiency improving with increased Fe element loading.
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ACS Catalysis
·
2020
·
IF 12.35
Xiaoli Yang,Ruifeng Wang,Jia Yang,Weixin Qian,Yaru Zhang,Xuning Li,Yanqiang Huang,Tao Zhang,De Chen
Direct conversion of syngas into aromatics with tandem catalysts containing Fe-based Fischer–Tropsch synthesis (FTS) catalysts and zeolites has been attracting significant attention because of the great cost-efficiency. However, the interaction role between two active species and reaction paths are still unclear. We report here that a high yield of aromatics was achieved by serial reactions directly from syngas on a Na-Fe-ZrO2/ZSM-5 tandem catalyst. Results point out significant impacts of zeolite in the catalytic system on performance including activity and selectivity. The role of the zeolite on reaction pathways about both CO conversion and aromatic formation has been systematically investigated by steady-state isotopic transient kinetic analysis and designed experiments. The presence of zeolite in the catalytic system promotes the CO hydrogenation rate by means of improving the iron carburization degree, possibly because of the enhanced CO adsorption and the formation of surface intermediates. It also enhances selectivity to aromatics by coupling CO to participate in the olefin transformation on ZSM-5. In addition, the formation rate of aromatics is proportional to the number of Lewis acidic sites, suggesting the dehydroaromatization route as the main mechanism of olefin aromatization. These findings provide some insights into the effect of ZSM-5 on reaction paths over the FTS catalyst–zeolite tandem catalyst system.
研究领域:
化学工程
·
催化化学
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CATALYSIS TODAY
·
2018
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IF 4.667
Mudassar Javed,Guihua Zhang,Weizhe Gao,Yingnan Cao,Peiyao Dai,Xuewei Ji,Chengxue Lu,Ruiqin Yang,Chuang Xing,Jian Sun
Zeolite supported Fischer-Tropsch (FT) catalysis has attracted extensive attentions in past few years. Capsule catalysts have unique characteristics of tuning product selectivity more precisely and enhancing stability of catalysts during reaction, which makes them to stand out of the crowed. Fe-based FT catalysts have been facing limitations for syngas conversion to hydrocarbons with their associated problems of high CO 2 selectivity and rapid catalyst deactivation. A series of ZSM-5 supported Fe-based microcapsule catalysts, composed of Fe/ZSM-5 core and silicalite-1 shell, was prepared and employed for direct synthesis of gasoline range hydrocarbons from syngas. Tuning silicalite-1 shell thickness significantly affected water-gas shift reaction with increasing hydrophobicity of catalyst surface, and greatly decreased CO 2 selectivity. The microcapsule catalysts significantly suppressed the CO 2 selectivity as compared with supported Fe-based catalyst. Moreover, all zeolite supported Fe-based catalysts, showed significantly high gasoline range hydrocarbons selectivity (about 60%). The proposed catalyst design suggests a promising approach to overcome high CO 2 selectivity challenge associated with Fe-based FT catalysts.
研究领域:
化学工程
·
催化材料
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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%.
研究领域:
催化化学
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能源化学
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材料科学
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化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.7
Weixiang Chen,Yuxiong Wang,Yaoyu Zhang,Yue Liu,Zhongbiao Wu
Ammonia (NH 3 ) has emerged as a promising zero‑carbon energy source for energy and transportation. However, its utilization leads to the emission of NH 3 , which contributes to PM 2.5 formation and disrupts the global nitrogen cycle. Selective catalytic oxidation (SCO) represents a mainstream technology for NH 3 treatment, yet achieving both sufficient activity and high N 2 selectivity across a broad temperature window remains challenging. Here, a core-shell Pt@Cu-ZSM-5 catalyst was employed for NH 3 catalytic abatement by encapsulating metallic Pt clusters (Pt 0 ) inside the channels of Cu ion-exchanged ZSM-5. The optimal sample achieved a complete NH 3 conversion below 250 °C and maintained over 92% N 2 selectivity from 250 to 500 °C due to the synergism between the Pt Cu dual sites. Mechanistic studies revealed that NH 3 oxidation preferentially occurred on Pt 0 sites with excellent redox capacity to produce N 2 O and NO x at relatively low and high temperatures, respectively. And the presence of Cu ions (Cu δ+ ) could efficiently both inhibit the formation of N 2 O on Pt 0 sites and reduce NO x emission, thereby improving the N 2 selectivity. At relatively low temperatures, NH 3 -solvated Cu + (NH 3 ) 2 could migrate to the adjacent Pt sites and reduce the adsorbed NO* species from NH 3 oxidation, damping the formation of N 2 O. At high temperatures, the NO and NO 2 emitted from Pt 0 sites could be reduced on Cu δ+ sites via a typical selective catalytic reduction. This study provides new insights into the rational design of bifunctional SCO catalysts and offers a comprehensive understanding of the synergistic effects in Pt Cu dual-site systems.
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CATALYSIS SURVEYS FROM ASIA
·
2021
·Vol. 26
·期 1
·35-45
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IF 3.106
Shan Shufeng,Tian Yiting,Chen Feifei,Wu Shikui,Zhou Rujin,Xie Ying,Li Ning,Zeng Xingye,Lin Cunhui,Yu Wei
NiMoS supported on ZSM-5 with different Si/Al ratio, crystallite size and pore structure was prepared by incipient impregnation method and applied in 1, 3, 5-trimethylbenzene (1, 3, 5-TMB) hydrodealkylation (HDAK). The physicochemical properties of samples were characterized by XRD, FTIR, SEM, N 2 adsorption–desorption, NH 3 -TPD, Py-FTIR, H 2 -TPR, HRTEM and TGA. It is demonstrated that for microporous NiMoS/ZSM-5, acid amount and crystallite size of HZSM-5 are key factors affecting HDAK performance. The larger acid amount and smaller crystallite size can promote the conversion of 1, 3, 5-TMB, especially the dealkylation reaction, resulting in higher BTX yield. Compared to NiMoZ-3, mesopores in micro-mesoporous NiMoAKZ-3 are beneficial to accessibility of 1, 3, 5-TMB to NiMoS and acid sites in close proximity, and the diffusion of reactant and product molecules inside pores, thus resulting in superior HDAK performance of NiMoAKZ-3. Moreover, the reaction network of 1, 3, 5-TMB HDAK was revealed according to product distribution. Graphic Abstract NiMoS supported on ZSM-5 was developed for heavy aromatic hydrodealkylation (HDAK). Acid amount and crystallite size of microporous ZSM-5 are key factors affecting 1,3,5-trimethylbenzene (1,3,5-TMB) HDAK. Mesopores inside ZSM-5 facilitate accessibility of 1,3,5-TMB to NiMoS and acid sites in close proximity and improve HDAK performance.
研究领域:
催化化学
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材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Yongyue Bai,Lei Ye,Yunxing Bai,Peng Zhou,Yongrui Wang,Ying Ouyang,Weixin Huang,Jichang Liu,Xingtian Shu,Wenjie Yang,Youhao Xu
Coconversion of hydrocarbons offers a sustainable and efficient route to high-value products while lowering the cost and energy demand for pure feedstock preparation. Here, we propose a cocracking process for alkanes and alkenes, and systematically investigate their interactions under mixed feed conditions through experiments and simulations. Introducing 0–40% alkanes into the alkene feed enhances conversion and maintains high selectivity for light olefins while suppressing methane and aromatics. At 20% alkane, the combined selectivity of ethylene and propylene reaches 69.8%, with an ethylene/methane ratio of 11.94. Validation experiments using cocracking of pentadiene and n-pentane with in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) show that dienes improve the product profile of alkane cracking and strengthen n-pentane adsorption on acidic zeolites, which favors alkene formation and suppresses methane and aromatics. Density functional theory (DFT) calculations further support that interactions between pentadiene and n-pentane facilitate a shift in the cracking pathway from a pentacoordinate to a tricoordinate carbocation mechanism, lowering the energy barrier. This work demonstrates a feasible strategy for the production of light olefins via hydrocarbon coconversion and advances mechanistic understanding of alkane–alkene cocracking.
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Journal of Physical Chemistry Letters
·
2026
·
IF 4.5
Liyuan Wang,Zhishun Feng,Shiji Li,Hongsheng Liu,Yanying Ren,Junfeng Gao,Lei Li
Silver nanoparticles hold great promise in biomedical and environmental applications, yet small and uniform Ag nanoclusters are hindered by easy aggregation, uncontrollable growth, and difficult recovery. Here we report a rapid and controllable ultrasmall (1–4.5 nm) Ag nanocluster by uniformly dispersed encapsulation in ZSM-5 channels using a microwave-assisted one-pot synthesis strategy. The ZSM-5 containing 1.21 wt % Ag nanoclusters exhibits a high Ag atomic utilization rate of 81.2%. The unique confinement structure effectively prevents Ag nanocluster overgrowth while conferring exceptional recyclability, maintaining over 99.9% bactericidal efficacy against Escherichia coli after three cycles. Performance testing reveals the material exhibits remarkable peroxidase-like activity (3.73 U/mg) and catalytic capability (methylene blue reduction rate constant of 0.167 min–1). This study offers a size-controllable approach for preparing high-performance, easily recoverable, and scalable Ag-based nanomaterials.
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