RSC Advances
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2024
·Vol. 14
·期 13
·8709-8717
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IF 3.9
Jiang-Tao Ma,Teng-Fei Meng,Zi-Yun Chen,Yu-Jun Zhu,Cheng Lian,Peng Wang,Ding-Hua Liu,Yu-Pei Zhao
This work investigates the influence of catalyst HZSM-5 on the isomerization of 2,5-dichlorotoluene (2,5-DCT) to produce 2,4-dichlorotoluene (2,4-DCT). We observe that hydrothermal treatment leads to a decrease in total acidity and Brønsted/Lewis ratio of HZSM-5 while generating new secondary pores. These characteristics result in excellent selectivity for post-hydrothermal modified HZSM-5 in the isomerization reaction from 2,5-DCT to 2,4-DCT. Under atmospheric pressure at 350 °C, unmodified HZSM-5 achieves a selectivity of 66.4% for producing 2,4-DCT, however after hydrothermal modification the selectivity increases to 78.7%. Density Functional Theory (DFT) calculations explore the thermodynamic aspects of adsorption between the HZSM-5 surface and 2,4-DCT. The kinetic perspective investigates the mechanism involving proton attack on the methyl group of 2,5-DCT followed by rearrangement leading to formation of 2,4-DCT during isomerization. The consistency between simulation and experimental results provides evidence for the feasibility of isomerizing 2,5-DCT to 2,4-DCT. This work fills the gap in the low value-added product 2,5-DCT isomer conversion, indicating its significant practical application potential and provides a valuable reference and guidelines for industrial research in this field.
研究领域:
化学工程
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催化科学
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材料科学
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PubMed
高影响因子
BIORESOURCE TECHNOLOGY
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2014
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IF 5.039
Haiyan Zhang,Xuejun Liu,Meizhen Lu,Xinyue Hu,Leigang Lu,Xiaoning Tian,Jianbing Ji
In this work, the role of Brønsted acid for furfural production in biomass pyrolysis on supported sulfates catalysts was investigated. The introduction of Brønsted acid was shown to improve the degradation of polysaccharides to intermediates for furfural, which did not work well when only Lewis acids were used in the process. Experimental results showed that CuSO 4 /HZSM-5 catalyst exhibited the best performance for furfural (28% yield), which was much higher than individual HZSM-5 (5%) and CuSO 4 (6%). The optimum reaction conditions called for the mass ratio of CuSO 4 /HZSM-5 to be 0.4 and the catalyst/biomass mass ratio to be 0.5. The recycled catalyst exhibited low productivity (9%). Analysis of the catalysts by Py-IR revealed that the CuSO 4 /HZSM-5 owned a stronger Brønsted acid intensity than HZSM-5 or the recycled CuSO 4 /HZSM-5. Therefore, the existence of Brønsted acid is necessary to achieve a more productive degradation of biomass for furfural.
研究领域:
化学工程
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催化
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可再生能源
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PubMed
高影响因子
JACS Au
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2024
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IF 8.5
Jieyi Liu,Nan Wang,Sibao Liu,Guozhu Liu
The chemical upcycling of plastic wastes by converting them into valuable fuels and chemicals represents a sustainable approach as opposed to landfilling and incineration. However, it encounters challenges in dealing with mixed plastic wastes due to their complex composition and sorting/cleaning costs. Here, we present a one-pot hydrodeoxygenation (HDO) method for converting mixed plastic wastes containing poly(ethylene terephthalate) (PET), polycarbonate (PC), and poly(phenylene oxide) (PPO) into sustainable naphthenes under mild reaction conditions. To facilitate this process, we developed a cost-effective, contaminant-tolerant, and reusable Ni/HZSM-5 bifunctional catalyst through an ethylene glycol-assisted impregnation method. The metallic Ni site plays a pivotal role in catalyzing C–O and C–C cleavages as well as hydrogenation reactions, while the acidic site of HZSM-5 facilitates dehydration and isomerization reactions. The collaboration between metal and acid dual sites on Ni/HZSM-5 enabled efficient HDO of a wide range of substrates, including bottles, textile fibers, pellets, sheets, CDs/DVDs, and plastics without cleaning or pigments removal and even their various mixtures, into naphthenes with a high yield up to 99% at 250 °C and 4 MPa H2 within 4–6 h. Furthermore, the metal-acid balance of the Ni/HZSM-5 catalyst is crucial for determining both HDO activity and product distribution. This proposed one-pot HDO process utilizing earth-abundant metal catalysts provides a promising avenue toward practical valorization of mixed plastic wastes.
研究领域:
化学工程
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环境科学
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材料科学
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DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
·
IF 3.5
Dongyang Liu,Liang Zhao,Yuen Bai,Jianxin Zhang,Jingjing Wang,Jiaojiao Wang,Haifeng Li,Jinsen Gao,Chunming Xu
Hierarchical HZSM-5 with integrated micro–mesopore structure is promising for boosting light olefin yield in light paraffin catalytic cracking, yet conventional alkali etching creates disordered large mesopores and rough crystal surfaces that degrade light olefin selectivity. Herein, this work adopts NaHCO 3 –TPAOH composite alkali treatment and pos-surface silanization treatment were used to regulate the micro-mesopore spatial distribution of hierarchical HZSM-5, for investigating the re-distribute of the hierarchical HZSM-5 and the effects of pore structure and its spatial arrangement on product selectivity. It was found TPA + in composite alkali system possesses large steric hindrance, which inhibits excessive local OH - corrosion, and avoids the formation of irregular large defective mesopores. On the optimized catalyst, the selectivity of light olefins is elevated by 8.7%. After surface silanization of zeolite, precisely passivates external acidic sites without blocking internal micropore channels, concentrating mesopores inside the zeolite framework. This structure greatly promotes the monomolecular cracking pathway of alkanes and achieves an improvement in ethylene production. This study clarifies the regulatory mechanism of spatially differentiated mesopores in HZSM-5 catalysts on the n-hexane catalytic pyrolysis reaction and their modulation effect on light olefin selectivity. It deepens the fundamental understanding of the structure-performance correlation of hierarchical porous zeolites and provides reliable guidance for the rational design and targeted fabrication of high-efficiency pyrolysis catalysts. Download: Download high-res image (254KB) Download: Download full-size image
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高影响因子
RENEWABLE ENERGY
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2025
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IF 9.1
Liqiang Zhang,Ningmin Zhu,Yuxiang Liu,Honglei Shi,Yiya Wang,Ruiqi Liu,Riyi Lin
A two-stage co-pyrolysis approach was developed for the efficient utilization of marine waste plastics and biomass, with a focus on the influence of biomass components. HZSM-5 was modified with Cu via wet impregnation and applied in the catalytic co-pyrolysis of Enteromorpha and polypropylene under varying catalyst-to-feedstock ratios. The Cu/HZSM-5 catalyst was characterized using X-ray diffraction (XRD), N 2 adsorption, and scanning electron microscopy (SEM). The results showed that Cu modification preserved the HZSM-5 framework while increasing pore size, enhancing catalytic cracking efficiency. Thermogravimetric and kinetic analyses revealed that Cu/HZSM-5 lowered the pyrolysis temperature, reduced residues, improved synergy, and decreased activation energy without altering the reaction mechanism. The catalyst significantly reduced oxygenated compounds and enhanced the formation of aromatic hydrocarbons in the oil products, reaching a maximum aromatic content of 90.20 % at a 6:5 catalyst-to-feedstock ratio in the second stage. Under the same conditions, hydrogen production in the gas phase also peaked at 47.91 %. Increased catalyst dosage decreased carbon and hydrogen content in the char while raising oxygen and nitrogen levels, with a higher H/C ratio mitigating char aromatization and densification. A reaction mechanism for Enteromorpha and polypropylene over Cu/HZSM-5 was proposed. This study provides insights into the catalytic co-pyrolysis of marine waste plastics and biomass with complex compositions.
研究领域:
化学工程
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环境科学
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材料科学
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高影响因子
FUEL PROCESSING TECHNOLOGY
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2012
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IF 2.945
Chao Duan,Xin Zhang,Rui Zhou,Yuan Hua,Li Zhang,Jie Chen
HZSM-5/SAPO-34 catalysts were prepared by physical mixture (named as ZS(m)-MM-n) and hydrothermal synthesis (named as ZS(m)-HS-n), respectively. Ethanol to propylene over these as-prepared catalysts was investigated under different reaction conditions. In addition, the physicochemical properties of these catalysts were characterized by AAS , XRD , N2 isothermal adsorption–desorption, SEM , NH3-TPD and TPO . The catalytic reactivity of HZSM-5/SAPO-34 catalyst was strongly dependent on its preparation method and composition as well as the reaction conditions. ZS(25)-MM-4 (HZSM-5/SAPO-34 = 4, weight ratio; HZSM-5 with Si/Al2 = 25 molar ratio) in isothermal fixed-bed reactor showed the highest propylene yield of ca. 34.5% among these catalysts and the poor catalytic stability. The use of nonisothermal fixed-bed reactor with the temperature configuration (2) significantly improved the catalytic stability of ZS(25)-MM-4. Synergetic effect of HZSM-5 with SAPO-34 occurred in HZSM-5/SAPO-34 catalyst, which modified its properties and catalytic reactivity. The concentration and the strength distribution of acid sites were closely relative to the catalytic reactivity of HZSM-5/SAPO-34 catalyst. For achieving the high yield of propylene, it was necessary that HZSM-5/SAPO-34 catalyst had the moderate concentration and strength distribution of acid sites.
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高影响因子
TOPICS IN CATALYSIS
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2026
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IF 3.7
Mu Yifang,Li Yanhong,Huang Aisheng
Direct synthesis of dimethyl ether (DME) from carbon dioxide (CO 2 ) hydrogenation by using bifunctional catalysts has attracted much attention in view of CO 2 conversion and utilization. However, direct CO 2 hydrogenation to DME is challenging due to kinetics and thermodynamic limitations, thus requiring the development of more effective bifunctional catalysts. In this work, metal-organic framework (MOF) Cu/Zn-BTC derived CuZnO catalyst is developed and combined with HZSM-5 for direct CO 2 hydrogenation to DME. The influence of Si/Al ratio of HZSM-5, mass ratio of CuZnO and HZSM-5, reaction temperature, reaction pressure and space velocity on the catalytic performances of the CuZnO/HZSM-5 bifunctional catalysts is systematically examined in a fixed-bed reactor. Attributing to a high activity of the Cu/Zn-BTC derived CuZnO catalyst for CO 2 hydrogenation to methanol, the CuZnO/HZSM-5 bifunctional catalysts display high CO 2 conversion and DME selectivity. Under a mild reaction condition (225 °C and 3.0 MPa), a high CO 2 conversion of 54.3% and DME selectivity of 79.5% are obtained for the bifunctional catalysts, which outperform the state-of-the-art catalysts for CO 2 hydrogenation to DME. Further, after 100 h of reaction, the bifunctional catalyst can still maintain a high CO 2 conversion rate (~ 52.6%) and DME selectivity (~ 77.3%), which suggests promising prospects for industrial applications.
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2026
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IF 6.9
Abrar Hussain,Ndumiso Vukile Mdlovu,Kuen-Song Lin,Chi-Jung Chang,Amin Hussain
Background The conversion of CO 2 into value-added fuels and chemicals remains one of the major challenges in catalysis and sustainable energy research. Developing efficient catalysts for CO₂ hydrogenation to methanol and dimethyl ether (DME) is essential for reducing greenhouse gas emissions and promoting carbon recycling. Methods In this work, a Zr-modified CuO–ZnO–Al₂O₃ (CZZA) catalyst was synthesized via a co-precipitation method for CO 2 hydrogenation. The catalyst systems “CZZA/HZSM-5-L” and “CZZA/com-HZSM-5” represent Zr-modified CZZA physically integrated with loofah-templated and commercial HZSM-5 (Si/Al = 25), respectively. A bio-HZSM-5 catalyst was also prepared using loofah sponge and rice husks as dual biotemplates to promote methanol dehydration into DME. The novelty lies in (i) the dual-biomass templating strategy (silica-rich rice husk vs. low-silica loofah) to achieve macro– meso –micro hierarchies while retaining MFI crystallinity, and (ii) Zr-promotion of the Cu–ZnO–Al₂O₃ matrix to enhance Cu⁺/Cu²⁺ and Cu–Zn interfacial sites, enabling efficient one-pass CO₂ → MeOH → DME conversion at 280 °C and 30 bar. Significant findings Zr incorporation significantly improved the structural and electronic properties of the CZZA catalyst, leading to enhanced surface area, active site dispersion, and CuO–ZnO interfacial synergy. Among all tested catalysts, the CZZA/HZSM-5-L bifunctional catalyst achieved the highest DME yield (13.2 %), DME selectivity (58.6 %), and CO₂ conversion (22.5 %) at 280 °C and 30 bar. An economic evaluation of 5- and 10-ton-per-day (TPD) DME production using refinery waste CO₂ showed payback periods of 2.98 and 2.44 years, respectively. Sensitivity analysis (±20 % variation in H 2 and DME prices) confirmed the payback remained below 4 years, demonstrating the technical and economic viability of the developed Power-to-DME process.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
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IF 3.8
Chenhao Wei,Di Gao,Guohao Zhang,Liang Zhao,Jinsen Gao,Chunming Xu
1-Hexene aromatization is a promising technology to convert excess olefin in FCC gasoline to high-value benzene (B), toluene (T), and xylene (X). Besides, the increasing market demand of xylene has put forward higher requirements for new generation of catalyst. For increasing xylene yield in 1-hexene aromatization, the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied. Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5, including NaOH treatment, Tetra-propylammonium hydroxide (TPAOH) treatment, and recrystallization. It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity, as a result of damage of micropores close to the catalyst surface. While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst. Besides, the state of loaded Zn was also affected by mesopores spatial distribution. On the optimized catalyst, the xylene selectivity was enhanced by 12.4% compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%. It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties. This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution, as well as their synergistic effect two on the improvement of xylene selectivity, which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.
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高影响因子
FUEL
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2023
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IF 7.4
Yujun Ma,Wenliang Wang,Yishuai Fu,Hui Miao,Jiale Huang,Sizhe Han,Yutong Chen
Improving the yield of the target product of monocyclic aromatic hydrocarbons plays an important role in increasing the economic competitiveness of biomass and waste plastics. In this study, a 3D SiC@HZSM-5@CoFe 2 O 4 multifunctional catalyst with high microwave absorptivity and excellent catalysis was successfully fabricated by a “coating-coating” method. Results showed that the obtained SiC@HZSM-5@CoFe 2 O 4 catalyst had a stable porous structure, abundant oxygen vacancy defects, high specific surface area, good dielectric loss performance, and magnetic loss performance. Encouragingly, co-pyrolysis of corncob (CC) and polystyrene (PS) revealed that the catalyst significantly promoted the synergistic effect and improved the selectivity of renewable gasoline-range aromatics (47.2 area %). In addition, finite element simulations indicated that the prepared catalyst with high microwave absorptivity could effectively accelerate the mass and heat transfer, thereby facilitating the cracking and conversion of pyrolysis vapors. This work provides an efficient method for the production of renewable gasoline-range aromatics from the mixture of biomass and waste plastics by microwave-assisted co-pyrolysis (MACP).
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Guoqiang Hou,Tingjun Fu,Xin Li,Qian Ma,Zhong Li
HZSM-5 catalysts with abundant silanol nests were fabricated by removing framework Al, which effectively promoted the selective alkylation of toluene with methanol by inhibiting the deep alkylation of aromatics to heavy aromatics and the conversion of methanol to light hydrocarbons. Correspondingly, the alkylation efficiency reached 65.3% at a toluene conversion of 31.3% over dealuminated HZSM-5, higher than the 55.2% efficiency and 28.0% conversion of parent zeolites, respectively. In situ DRIFTS and single-factor experimental clarified that toluene adsorption was enhanced and methanol to hydrocarbons was inhibited with the presence of silanol nests. Additionally, by increasing the crystal size of HZSM-5 with silanol nests from 2 to 5 µm, para-xylene selectivity was increased from 36.1% to 65.5% because of the enhanced diffusion barrier . The finding of the positive effect of the silanol nests on toluene alkylation can provide a solid fundamental basis for the rational design of catalysts.
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高影响因子
APPLIED CATALYSIS A-GENERAL
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2021
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IF 5.706
Xiaochao Xian,Mengjun He,Yakai Gao,Yi Bi,Yirong Chu,Jun Chen,Lichun Dong,Jin Wang,Shuo Zhao
Reducing the acid density and strength of HZSM-5 zeolite are typical strategies to inhibit coke deposition during catalytic cracking reactions. Herein, direct titration of HZSM-5/H 2 O suspension using dilute NaOH aqueous solution at room temperature was introduced to neutralize excessive Brønsted acid sites of HZSM-5 zeolite (Si/Al = 25). SEM, XRD, N 2 adsorption and n -propylamine temperature-programmed decomposition confirmed that simultaneous acid strength weakening and acid density reducing were achieved without obvious influence on crystalline or textural property. The evolution of the surface charge during the titration process tracked by Zeta-potential measurement reveals that the mechanism of such neutralization is: liquid phase neutralization between H + and OH − & solid phase ion exchange between Na + and H + . Supercritical catalytic cracking of n -dodecane over a series of partial neutralized HZSM-5 catalysts showed that moderate neutralization can enhance the conversion of n -dodecane by alleviating both the coke amount and harmfulness per unit mass of coke.
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高影响因子
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