GREEN CHEMISTRY
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2025
·Vol. 27
·期 6
·1838-1857
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IF 9.2
Li Yang,Bonan Liu,Yingying Zhao,Zijian Zhang,Hanyu Wu,Minyi He,Chao Tang,Jun Zhao,Yu Fan,Wangjing Ma
Modern chemists dream of a low-temperature bioethanol dehydration to ethylene process promoted by biomaterial-based catalysts, which would be without doubt an energy-saving, sustainable achievement in green chemistry. However, limitations on catalytic activity and competition from exothermic side reactions have always been an insurmountable gap. Herein, a microwave-assisted pathway employing biochar-based catalysts was designed to effectively dehydrate ethanol into ethylene at temperatures lower than 100 °C. Either biochar (BC) or phosphoric acid-modified derivate (HBC) was synthesized from bamboo powder through a simple one-step decomposition. ZSM-5/MOR composite zeolite was further introduced to form HBC-2-ZSM-5/MOR hybrid catalysts, which could effectively prevent the formation of diethyl-ether and enhance the production of ethylene. With a microwave input power and reaction temperature as low as 10 W and 82 °C, ethanol (WHSV = 2 h−1) could be completely converted on the HBC-2-ZSM-5/MOR (1.5) catalyst with almost 100% ethylene selectivity. Similar results were obtained in the conversion of bioethanol (model), Chinese liquor and beer, pointing to the wide applicability of this strategy. Investigation of the potential mechanism found that weak acidity, special structure and P-modification characteristics can effectively inhibit the formation of diethyl ether by-products, oligomerization and the coking process, which is conducive to promoting the selective conversion of ethanol to ethylene. This work has blazed another trail for low-temperature ethanol to ethylene by combining the advantage of microwave heating with precise tailoring of biochar-based catalysts, all for a better future life with green chemistry.
研究领域:
绿色化学
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催化材料科学
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CRYSTAL GROWTH & DESIGN
·
2017
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IF 4.055
Meng Pan,Jiajun Zheng,Yujian Liu,Qinglan Kong,Huiping Tian,Ruifeng Li
Hollow zeolite microspheres have attracted considerable interest due to their unique properties and great potential applications. In this work, we report a simple and cost-effective approach for constructing hollow zeolite microspheres based on a biomass-derived template, i.e., carboxymethylcellulose sodium (CMC). As an example, a hollow ZSM-5 microsphere with a hollow core smaller than 1 μm in diameter and a complete crystal shell is synthesized. This approach overcomes most of the limitations associated with the existing methods, such as complex operations and costly spherical templates. By studying the growth process in detail, a possible formation mechanism is proposed. The crystallization of the hollow zeolite microsphere is through a “surface to core” process, in which the interaction between the CMC and the zeolite gel and the decomposition of the polymer network play the critical roles.
研究领域:
材料科学
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化学工程
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JOURNAL OF POROUS MATERIALS
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2026
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IF 3.2
Guo Hanxu,Fu Sen,Yuan Hong
Hierarchical zeolites can provide multidimensional spatial networks, thereby holding significant potential as catalysts for BTX production from biomass pyrolysis. In this study, nano-ZSM-5 zeolite (Z X-X ) with a hierarchical pore structure was synthesized using glycine as a growth inhibitor. Due to the exceptional ability of Ni to cleave C–C and C–H bonds, Ni modification was performed on the Z 30-0.2 catalyst. The effects of glycine and Ni loading on the morphology and pore structure of the zeolites were systematically investigated using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and N 2 adsorption–desorption. The results demonstrated that the particle size of 10 wt% Ni-Z 30-0.2 zeolite ranged from 200 to 300 nm, with a BET surface area of 314 m 2 /g and abundant mesopores. The NH 3 -TPD results showed that the acid amount of 10 wt% Ni-Z 30-0.2 was 0.72 mmol/g. The prepared zeolite was employed in a fixed-bed reactor to catalyze the pyrolysis of oleic acid for the production of benzene, toluene, and xylene (BTX). The introduction of metal Ni significantly enhanced the BTX yield. At 500 ℃, the average BTX yield achieved with the 10 wt% Ni-Z 30-0.2 catalyst was 19.4 wt%, which was higher than that of the zeolite without Ni loading.
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CATALYSIS TODAY
·
2022
·
IF 6.562
Bin Kang,Ming Li,Zhaoying Di,Xiaonan Guo,Ying Wei,Jingbo Jia,Runduo Zhang
Series of ZSM-5 zeolites with diverse contents and locations of Al pairs were synthesized, and Co 2+ ions were subsequently anchored at the Al pairs of ZSM-5 zeolites by wet ion-exchange with H protons. The Co-ZSM-5 sample derived from the mixtures of AlCl 3 and TEOS of Si/Al=30.3 showed the best de N 2 O performance. Analysis on Co (Ⅱ) ion exchange capacity demonstrated the content of Al pairs followed the sequence: AlCl 3 (0.84) > Al(NO 3 ) 3 (0.73) > aluminum isopropoxide (0.65) and TEOS (0.84) > silicic acid (0.57). More Al pairs coordinated with protons or cobalt ions were essentially associated with better performances for N 2 O catalytic dissociation. Moreover, Si source had a significant effect on the location of Al pairs determined by UV–vis–DRS of bare Co (Ⅱ), Al pairs of ZSM-5 zeolite synthesized from TEOS were enriched in the sinusoidal channel (γ site), whereas those synthesized from silicic acid were concentrated in the channel intersections (6-MRs β site). The theoretical calculation revealed that the O 2 desorption at γ-site Co 2+ of ZSM-5 zeolite required to overcome less energy barrier (23.8 kcal/mol) than that at β-site one.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2026
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IF 3.9
Xin-Bo Pang,Jing-Pei Cao,Nai-Yu Yao,Jing-Ping Zhao,Tian-Long Liu,Shi-Jie Cai,Xiao-Yan Zhao,Tungalagtamir Bold
Catalytic pyrolysis as an important pathway for the production of sustainable chemicals and fuels from biomass. However, it is still a huge challenge to significantly improve the yield of light aromatics by adjusting the structure of ZSM-5 zeolite and to fully understand its catalytic mechanism. Here, the directional preparation of ZSM-5 nanosheets with controllable b-axis thickness was achieved by controlling the amount of silicalite-1 added during the hydrothermal synthesis process. Characterization results demonstrate that the reduction in b-axis thickness greatly enhances the mass transfer process of the zeolite while enhancing the accessibility of acidic sites, thereby promoting the catalytic conversion of biomass pyrolysis volatiles to aromatic. The yield of light aromatic hydrocarbons in bio-oil is substantial increased, the bio-oil of 20-NCZ5 had the highest aromatic content with a yield of 97.1% and a yield of 135 mg/g, achieving efficient catalytic upgrading of bio-oil. Highly b-axis-oriented ZSM-5 nanosheets provide a new approach for efficient biomass utilization. Furthermore, this zeolite holds promise for broader applications in the catalytic conversion of various energy sources.
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CATALYSIS TODAY
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2026
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IF 5.1
Wenjing Bao,Yulian He,Xiaonan Guo,Chao Feng,Shanshan Liu,Xing Fan,Peng Liang,Runduo Zhang
The directional design of efficient catalysts for volatile organic compounds (VOCs) abatement remains effective yet challenging. Here, 3 wt% Co 3 O 4 catalysts supported on ZSM-5, Beta, MCM-41, and HY supports were constructed to elucidate the pronounced influence of pore confinement on catalyst redox behavior and catalytic activity. The micropore channels of ZSM-5 stabilizes appropriately sized CoO x clusters and enriches surface Co 3+ , thereby promoting low-temperature Co 3+ /Co 2+ cycling and lattice-oxygen migration, which endows Co 3 O 4 /ZSM-5 with superior performance in propane total oxidation. The T 50 of Co 3 O 4 /ZSM-5 catalyst is 260 ℃, which is 20 ℃ and 100 ℃ lower than those of Co 3 O 4 /Beta and Co 3 O 4 /MCM-41, respectively; it also exhibits E a of 37.6 kJ·mol -1 , specific surface activity at 260 ℃ of 21×10 -8 mol·m -2 ·s -1 , and TOF of 1.2×10 -2 s -1 , together with excellent water resistance and stability. By contrast, the wide mesopores of MCM-41 induce Co 3 O 4 agglomeration, while the overly strong confinement exerted by HY and Beta supports over-stabilizes Co 2+ and tightly bound lattice oxygen, both unfavorable for oxidation. DFT calculations further confirm that Co 3 O 4 confined in ZSM-5 exhibits the strongest O 2 activation and the lowest barriers for O 2 dissociation, CO oxidation, and the initial O-insertion/H-abstraction/C-C bond cleavage steps in propane. Overall, this work offers a new avenue for designing efficient, water-tolerant catalysts for propane oxidation.
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APPLIED CATALYSIS A-GENERAL
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2026
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IF 4.8
Leqing He,Changyue Shao,Ping Liu,Yingxia Li,Jiqin Zhu,Chongpin Huang
Conventional ZSM-5 zeolites face significant challenges in achieving high product selectivity and avoiding rapid catalyst deactivation due to coke deposition during the condensation of ethylenediamine (EDA) to triethylenediamine (TEDA). Based on the characteristic of ammonia generation during the synthesis of TEDA from EDA, this study treats ZSM-5 with high-temperature ammonia-steam to investigate its effect on the catalytic synthesis of TEDA. The results show that ZSM-5 sample treated with 5 wt% ammonia-steam at 600 ℃ exhibited higher crystallinity and more mesoporous structure. A large amount of framework aluminum in the catalyst was removed, resulting in significant decrease of acid strength and a high L/B ratio. The modified catalyst achieved complete EDA conversion during the reaction, with 64% TEDA selectivity—a 17% improvement over that of unmodified catalyst. It also exhibited a significant reduction in coke deposition from 6% to 2.3% and a 15-days continuous fixed-bed reaction test confirmed the high stability of the modified catalyst without noticeable deactivation. Compared to acid-base treated and metal ion treated ZSM-5, ammonia-steam treated ZSM-5 demonstrates superior selectivity and stability, and it has been verified that the TEDA yield is higher than that of TS-1. This study provides a novel strategy for designing efficient catalysts for amine cyclization reactions.
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FUEL
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2026
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IF 7.8
Tonggui Liu,Botian Hao,Guanyu Jiang,Donghai Xu,Haochuang Li,Xingshuo Zhang,Xin Ding,Lili Qian,Yang Guo,Shuzhong Wang
Hydrothermal liquefaction (HTL) was identified as a promising technology for the conversion of wet municipal sludge (MS) into liquid biofuel. However, the oil product (biocrude) derived from MS exhibited high O content and low higher heating value (HHV). These issues severely limited its application as a biofuel. In this study, a catalytic hydrogenation process was employed to upgrade the sludge biocrude. ZSM-5 zeolites were selected as catalysts. A series of alkali modification studies were conducted. Furthermore, the mechanism of catalytic hydrogenation upgrading was analyzed. The results indicated that the modified ZSM-5 (NaOH + TPAOH-ZSM-5), prepared via mixed organic and inorganic alkali modification, exhibited the best hydrogenation performance, with synergistic meso -microporous structures. This catalyst significantly enhanced the deoxygenation efficiency, increasing from 33.76% for ZSM-5 to 75.02%% for NaOH + TPAOH-ZSM-5 (300 °C, 40 min). Meanwhile, the hydrocarbons content in the upgraded biocrude exceeded 50%. Additionally, the content of heavy oil fraction (>C20) decreased from 83.68% to 13.66%. The study confirmed that the modification of the ZSM-5 pore structure facilitated the formation of mesopores. This structure allowed macromolecular substrates to enter the catalyst channels and participate in the reaction. Consequently, the catalytic hydrodeoxygenation effect on the biocrude was effectively enhanced. This work provided an experimental basis for the application of dual-alkali modified ZSM-5 in catalytic upgrading of sludge hydrothermal biocrude.
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JOURNAL OF CATALYSIS
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2026
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IF 6
Zhengxi Zou,Zhenke Xu,Weiming Hua,Yinghong Yue,Zi Gao
Catalytic ethane dehydrogenation to ethylene is an attractive route for ethylene production following the shale gas revolution. However, its industrial implementation remains challenging due to high costs and environmental concerns. Iron-based catalysts have been identified as promising alternatives, while their catalytic performance is significantly dependent on the coordination environment and oxidation state of the iron species. Herein, a series of Fe/ZSM-5 catalysts were synthesized via urea precipitation (FeZ-P) and incipient wetness impregnation (FeZ-I) methods to investigate the relationship between Fe species evolution and catalytic behavior during ethane dehydrogenation. The FeZ-P catalysts exhibited significantly enhanced activity compared with FeZ-I, which was attributed to the improved dispersion of iron species and their favorable transformation behavior under reaction conditions. Detailed characterizations of fresh and spent catalysts revealed that the initial Fe 2 O 3 species on FeZ-P surface possessed limited dehydrogenation activity but underwent reaction-induced reduction and carbonization, generating Fe 3 C with enhanced ethane dehydrogenation performance. In contrast, the Fe 2 O 3 bulks on FeZ-I exhibited slower transformation rates, resulting in inferior catalytic activity. Air oxidation treatment enabled partial regeneration of the catalyst by removing carbon deposits and modifying Fe species evolution. This study highlights the importance of regulating Fe species dispersion and dynamic reduction-carbonization behavior, through which catalytically active Fe 3 C can be generated for enhanced ethane dehydrogenation performance. These findings provide valuable insights into the rational design of efficient Fe-based catalysts for non-oxidative alkane dehydrogenation.
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MATERIALS LETTERS
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2023
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IF 3
Yuanyuan Tao,Wenhui Wei,Qianqian Gu,Xiaoping Jiang,Dongwei Li
The desilicated zeolite ZSM-5 (des-ZSM-5) based composite polymer electrolytes (CPEs) PZEw was fabricated via phase inversion processes and in-situ polymerization with polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) and liquid electrolyte 1 M lithium bis(trifluoromethanesulphonyl)imide (LiTFSI) in vinylene carbonate (VC) (VC@LiTFSI). Assisted by des-ZSM-5, PZEw possess excellent thermal stability, mechanical properties, high ionic conductivity (2.75 × 10 −4 S cm −1 , 25 °C), and enlarged electrochemical windows (4.94 v, vs. Li + /Li). Meanwhile lithium metal batteries (LMBs) LiFePO 4 (LFP)/PZEw/Li showed superior rate performance and long-time cycling stability.
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Molecular Catalysis
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2023
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IF 4.6
Quan Zhang,Wei Huang,Wenhao Cui,Xingzong Dong,Guangye Liu,Yunpeng Xu,Zhongmin Liu
The acidity and porosity of zeolite catalysts are crucial parameters affecting the catalytic performance. In this work, alkali treatment and metal species loading were used to modify the porosity and acidity of ZSM-5 zeolite to prepare an efficient catalyst for the 1,2-dichloroethane cracking reaction. After optimization, the highly active catalyst Zn (1%) /ZSM-5-120 was obtained, and 78% conversion of EDC and 99% selectivity toward VCM could be achieved under the conditions of 300 °C and 3.0 h −1 (WHSV). A detailed investigation was conducted on the effects of acidity, texture properties and metal species loaded on ZSM-5 zeolite on the 1,2-dichloroethane cracking reaction.
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Journal of the Taiwan Institute of Chemical Engineers
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2018
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IF 3.849
Yue Zhou,Huiping Zhang,Ying Yan
A series of CuO/ZSM-5 catalysts with different copper loadings were prepared by impregnation (IM) and chemical vapor deposition (CVD) methods, respectively. Their physicochemical properties were investigated by N 2 adsorption/desorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectronic spectra (XPS), temperature-programmed reduction by hydrogen (H 2 -TPR) and temperature-programmed desorption of NH 3 (NH 3 -TPD). The XRD and TEM results demonstrated that the crystallite size of the CuO prepared by CVD method was smaller than that by IM, and the XPS results illustrated that the copper specie was mostly in Cu 2+ state and Cu + co-existed. The performance of catalytic oxidation of ethyl acetate was conducted in the fixed-bed reactor based on CuO/ZSM-5 catalysts. The experimental results showed that the preparation method affected the catalytic activity of CuO/ZSM-5; the CVD catalysts exhibited a higher catalytic activity for ethyl acetate oxidation compared with the IM catalysts at the same copper loadings. Ethanol and acetaldehyde are observed to be the intermediate products in the combustion of ethyl acetate over the synthesized catalysts. The relative amounts of acetaldehyde and ethanol are determined by the selectivity of the catalyst toward acetaldehyde production from ethanol. Particularly, the 3 wt% CVD catalyst showed the best catalytic activity for ethyl acetate oxidation with 90% conversion of ethyl acetate at 235 °C, which was much lower than that of the 3 wt% IM catalyst (278 °C), meanwhile, the intermediate products of the 3 wt% CVD for ethyl acetate oxidation were completely oxidized into CO 2 and H 2 O at temperature as low as 288 °C.
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