JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Shu-Ting Hu,Yue-Lun Wang,Qing-Gang Wang,Han-Bing Gao,Wen-Jie Gu,Wei-Hua Zhao,Yun-Peng Zhao,Jing-Pei Cao,Lin-Jun Zhu
The introduction of in situ hydrogen donors to obtain a high H/C eff ratio is an effective way to upgrade coal pyrolysis volatiles to light aromatics. In this study, the influence of different in-situ hydrogen suppliers in catalytic reforming of coal pyrolysis vapors was explored. The abilities of active hydrogen donation were greatly corresponded to structures of hydrogen donors. Isopropanol showed the best catalytic performance due to the release of a large amount of active α-H as a result of negative inductive effect of hydroxyl. Whereas tertbutanol showed the poorest catalytic performance owing to the lack of α-H. Meanwhile, the effect of in-situ hydrogen production via steam reforming with different alcohols on light aromatic yields was investigated. The highest BTEXN yield was obtained under in-situ hydrogen production from isopropanol steam reforming. Two circumstances of hydrogen supply were further compared. Relatively higher BTEXN yield was presented in the reaction of methanol steam reforming than that of using methanol solely. However, higher BTEXN yield was contrarily obtained from sole isopropanol as a hydrogen donor despite lower H 2 production was gained compared to the case of isopropanol steam reforming. The fact was probably ascribed that high electron-withdrawing effect of hydroxyl for isopropanol promoted the cleavage of α-C-H bond and favored the transfer of active hydrogen to reactants over acid sites.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Nengcui Zhang,Yimin Zhang,Feng Wu,Ziyan Liu,Xinyu Xu,Qiang Li,Yi Mei,Yun Zu
Phosphorus (P)-doping H-ZSM-5 zeolites, which is crucial for industrial applications, aim to adjust both acidity and framework stability while optimizing product distribution in heterogeneous catalysis. Nonetheless, current phosphating methods often suffer from inadequate phosphorus dispersion and unclear interfacial interactions with framework aluminum (Al). In this work, P-doping ZSM-5 zeolites were successfully one-step prepared by using tributylphosphine served as an organophosphorus precursor, assisting by density functional theory calculations. On account of this, a stable interface of tetracoordinated-phosphorus and framework Al was fabricated uniformly. Such an interfacial structure not only made more framework Al sit in the straight/sinusoidal channels, but also remodeled Brønsted acid sites and reinforced its acidity. Under comparable conditions, methanol-to-propylene (MTP) evaluations indicated that the high-silica PZ-75 zeolite catalyst displayed an appreciable catalytic lifetime (30 h) and a higher C 3 H 6 selectivity (52.4 %). Additionally, in-situ Fourier transform infrared spectroscopy further revealed that this exceptional MTP performance was attributable to the predominant olefinic pathway and lower hydrogen transfer ability. These results provide valuable information for cognizing phosphorus-zeolite chemistry and creating high-performance MTP catalytic materials.
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JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Lei Chen,Wenjie Yao,Xu Chen,Gang Yang
The Cu-Ce modified SAPO-34/ZSM-5 (S-Z) composite molecular sieve catalysts were synthesized via a stepwise crystallization process using triethylamine (TEA) and tetraethylammonium hydroxide (TEAOH) as dual templates. This method significantly reduces the crystallization time from 24 hours to 12 hours. The incorporation of metal ions alters the structure and acid strength of the molecular sieves, thereby decreasing the rate of coke formation during the reaction, which in turn extends the catalyst's lifetime. Experimental results demonstrated that the catalyst's lifetime increased progressively with the addition of Ce. In the methanol-to-olefin reaction, the catalytic lifetime of the S-Z/Cu 0.05 -Ce 0.05 samples reached 1440 mins, approximately 480 mins longer than that of the S-Z samples, while maintaining a selectivity for low-carbon olefins at around 89.6%.
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Crystals
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2020
·Vol. 10
·期 9
·781
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IF 2.404
Qintong Huang,Rui Li,Guangying Fu,Jiuxing Jiang
ZSM-5 zeolites are commonly used as a heterogeneous catalyst for reactions. Four ZSM-5 catalysts (with various crystallite sizes and a similar ratio of Si/Al) and their ball-milling/surface-poisoning derivates were used to convert L-lactic acid to L, L-lactide. The reaction products were analyzed by three independent analytical methods (i.e., Proton nuclear magnetic resonance (1H NMR), high-pressure liquid chromatography (HPLC), and chiral gas chromatography (GC)) for determining the L, L-lactide yield and L-lactic acid conversion. A clear size effect, i.e., smaller catalysts providing better performance, was observed. Further ball-milling/surface-poisoning experiments suggested that the size effect of the ZSM-5 catalysts originated from the diffusion-controlled nature of the reaction under the investigated conditions.Keywords:ZSM-5 zeolites;L,L-lactide;size effect;diffusion control
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2016
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IF 3.652
Bo Zhang,Guiwei Tan,Zhaoping Zhong,Roger Ruan
In order to minimize coke yield and improve hydrocarbon production during microwave-assisted catalytic fast pyrolysis of spent edible mushroom substrate, ZSM-5 zeolite catalyst is modified with pre-coking treatment, chemical vapor deposition of SiO 2 , and ethylene diamine tetraacetie acid (EDTA) chemical modification method, respectively (labeled PC-ZSM-5, SiO 2 -ZSM-5 and EDTA-ZSM-5). Experimental results show that all the modification methods result in a loss of external acid sites of ZSM-5. Among the three modified catalysts, the maximum oil fraction yield and the minimum coke yield are obtained with SiO 2 -ZSM-5. The relative content of hydrocarbons in oil fraction increases in the following order: SiO 2 -ZSM-5 > EDTA-ZSM-5 > PC-ZSM-5 > original ZSM-5. Moreover, SiO 2 -ZSM-5 shows the highest relative contents of toluene and xylene, whereas original ZSM-5 produces the lowest ones. Besides, the selectivity of benzene in aromatics follows the order of original ZSM-5 > EDTA-ZSM-5 > PC-ZSM-5 > SiO 2 -ZSM-5, while the selectivity of toluene + xylene presents the opposite trend.
研究领域:
能源与环境科学
·
材料科学
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Shihe Zhang,Shuo Li,Yijun Tian,Chengna Dai,Ruinian Xu,Biaohua Chen
Cr-Zr/ZSM-5 converts PE at 280 °C to BTX and SAF with 93% selectivity. • Self-supplied H from BTX formation saturates C 9 -C 16 to SAF without external H 2 . • Zr doping lowers dehydrogenation barrier and boosts electron transfer. The catalytic conversion of polyethylene (PE) into a C 6 -C 8 BTX-rich fraction and a C 9 -C 16 SAF-range hydrocarbon fraction provides a potential route for plastic-carbon valorization, where “SAF-range” refers to the aviation-fuel-relevant carbon-number range rather than to specification-compliant finished SAF. However, many reported PE-upcycling routes require elevated temperatures, external H 2 , noble-metal catalysts, or high catalyst-to-feed ratios. Herein, we report a rationally engineered bifunctional Cr-Zr/ZSM-5 catalyst that converts PE at 280 °C and 0.5 MPa into targeted products with a liquid yield of 62 wt% and approximately 90% selectivity within the BTX-rich C 6 -C 8 fraction and SAF-range C 9 -C 16 hydrocarbons. Combined characterization, pyridine-adsorbed FTIR, online mass spectrometry, in situ FTIR, product analysis, and model-surface DFT calculations support a proposed bifunctional reaction network. A proposed reaction network is constructed, in which initial conversion may involve thermal and surface-assisted fragmentation at accessible external/near-external regions. Cr-Zr oxide-related species may subsequently facilitate adsorption, C-H activation, dehydrogenation, and olefin-intermediate formation. The resulting smaller olefinic intermediates can then undergo Brønsted-acid-initiated secondary conversion within the MFI channels, while product formation is accompanied by dynamic, competitive internal hydrogen redistribution without external H 2 . This work bridges atomic-scale engineering with catalytic function, providing a scalable, mechanism-guided platform for plastic waste valorization and establishing a fundamental mechanistic framework for the rational design of tandem catalytic systems in waste-to-fuel conversion. Download: Download high-res image (206KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Zhongbiao Wu
Pt@Cu-ZSM-5@CuO x catalyst was constructed for the catalytic oxidation of acetonitrile (AN), which achieved a complete mineralization rate and more than 95 % N 2 selectivity within 300–450 °C. Characterization results revealed that the satisfactory synergistic action of hydrolysis and oxidation pathways was well achieved. The NO x release from CN oxidation reaction on out-layer CuO x species and NH x species over-oxidation over Pt sites could be eliminated by NH 3 from CN hydrolysis reaction on Cu ions via internal selective catalytic reduction mechanism. The deep oxidation of carbon-containing intermediates (such as CO etc.) during CN decomposition over Cu species effectively occurred over Pt site. The encapsulation of Pt inner ZSM-5 zeolite not only strengthened low-temperature mineralization rate compared to Cu/ZSM-5 sample, but also inhibited NO x release caused by over-oxidation of AN at an elevated temperature with co-impregnation of Pt species over Cu/ZSM-5. This work provided a viable strategy for designing catalysts to effective abatement of NVOCs.
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CATALYSIS TODAY
·
2023
·
IF 5.3
Yong Yang,Hualei Hu,Qianquan Fang,Guowen Lu,Hongli He,Hui Chen,Chunlin Chen,Jian Zhang
The highly-efficient conversion of 5-hydroxymethylfurfural (HMF) to 2,5-bis(propoxymethyl)furan was achieved via the one-pot route, which were performed by the combination of supported copper catalyst and hierarchical pore ZSM-5 zeolite. Among the supported copper catalyst, the Cu/Al 2 O 3 catalyst exhibited the excellent activity and selectivity in the hydrogenation of HMF, obtaining a 98.7% yield of BHMF at 100 °C for 6 h under 2.5 MPa of H 2 . The reason might be attributed to that the highly dispersed copper particles and relatively weaker acid sites, which improved the hydrogenation activity of catalyst and suppressed the occurrence of side reaction. In the one-pot synthesis of BPMF, the Cu/Al 2 O 3 catalyst and HP-ZSM-5 zeolite were responsible for HMF hydrogenation and BHMF etherification , respectively, and the competition between them is negligible. This work provides a simple route to produce furanic diether from HMF.
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FUEL
·
2023
·
IF 7.4
Yuting Jin,Yanhong Quan,Yan Li,Jinxian Zhao,Jun Ren
A series of chainlike ZSM-5 supported Cu catalysts with the addition of citric acid (CA) was conveniently prepared using a complexation-impregnation method and employed in the methanol dehydrogenation to methyl formate (MF). The catalytic performance of Cu x /CZ5 first increased and then decreased with increasing CA/Cu ratio, reached 35.0% methanol conversion and 88.3% MF selectivity for Cu1.8/CZ5, significantly higher than that of Cu/CZ5. The superior catalytic performance might be principally explained by the higher Cu 0 concentration combined with abundant Brønsted acid sites, which are responsible for methanol conversion and MF selectivity, respectively. This work provides new insights into the synergy between Cu 0 species and surface acidity of Cu x /CZ5 catalysts for methanol dehydrogenation and offers a feasible and effective strategy for enhancement of the catalytic performance of copper-based catalysts.
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BIORESOURCE TECHNOLOGY
·
2021
·
IF 9.642
Jingyuan Shang,Guangbin Fu,Zhenping Cai,Xiang Feng,Yongxiao Tuo,Xin Zhou,Hao Yan,Chong Peng,Xin Jin,Yibin Liu,Xiaobo Chen,Chaohe Yang,De Chen
Valorization of biomass to olefin or aromatics harbours tremendous practical value due to growing concerns about sustainable production of chemicals. Herein, the olefin or aromatics yields of ex-situ catalytic pyrolysis of pine can be regulated by impregnating Sn on hollow-structured ZSM-5 (M-ZSM-5) and microporous ZSM-5 catalysts in fixed-bed reactor, respectively. Results showed that Sn/ZSM-5 catalyst simultaneously increased medium acidic sites and maintained strong acidic sites, which obtained the maximum carbon yield of aromatics (33.77%) due to enhanced cracking and deoxygenation reactions. In addition, Sn boosted alkylation between olefin and aromatics, generating more alkylbenzene. In contrast, Sn/M-ZSM-5 catalyst produced the highest olefins carbon yield (12.39%) because the reduction of strong acidic sites and microporous volume inhibited the olefin aromatization. Moreover, olefins were easier to desorb from Sn/M-ZSM-5 due to the enhanced mass transfer ability, which weakened the alkylation reactions. The synergistic effect harbours great significance to manipulate the distribution of products.
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PubMed
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RENEWABLE ENERGY
·
2021
·
IF 8.001
Nishu,Chong Li,Meiyun Chai,Md. Maksudur Rahman,Yingkai Li,Manobendro Sarker,Ronghou Liu
Hemicellulose was extracted from rice straw, and catalyst ZSM-5 was modified by NaOH and Ni over alkaline treatment and wet impregnation method, respectively. To investigate the effects of modified ZSM-5 on selectivity of aromatic hydrocarbons, catalytic pyrolysis of hemicellulose was studied via Py-GC/MS. Significant effect has been reported for product selectivity and composition over the modified catalysts. All the modified catalysts showed better aromatic selectivity than parent ZSM-5 (P-ZSM-5). Notably, alkali modified ZSM-5 with 0.4 M concentration of NaOH (0.4 M ZSM-5) showed 36% selectivity towards aromatics with the share of benzene, toluene, and xylene (58%) and share of polyaromatics (15%) compared to others. Meanwhile, 8 wt% Ni-ZSM-5 showed the highest selectivity of aromatic hydrocarbons of 54% where the share of benzene, toluene, and xylene was 70%. This research revealed that metal modified ZSM-5 significantly influences the aromatics yield, which is essential for the production of liquid fuels and chemicals.
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JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Xu Zhao,Fuxin Yang,Wentao Li,Houzhang Tan,Lijuan Gao,Yanhao Jiao
With the urbanization and population growth, the disposal of plastic waste has become a significant challenge, as the traditional methods often result in pollution and resource wastage. Pyrolysis technology offers a sustainable solution by converting the waste plastics into valuable gas or liquid fuels. The co-pyrolysis of plastics and biomass is an effective approach for synergistically managing these two types of solid waste. The polyethylene (PE) and salix psammophila (SP) was used to investigate the gas production characteristics and polycyclic aromatic hydrocarbons (PAHs) formation during the co-pyrolysis. Additionally, Cu/ZSM-5, Co/ZSM-5, and Ni/ZSM-5 catalysts were employed to investigate the effects of different metal-loaded catalysts on the co-pyrolysis process. The results indicate that, with the increase of the pyrolysis temperature, the yield of gas-phase products gradually increases, solid residue decreases, and liquid-phase products initially increase before declining, reaching their maximum at 500 °C. The synergistic effect promotes the formation of C 2 H m (C 2 H 2 , C 2 H 4 , C 2 H 6 ) and CH 4 , leading to the increase of the gas-phase product yields compared to the individual pyrolysis. The addition of catalysts further enhances the gas production: Cu/ZSM-5 boosts H 2 yield, Co/ZSM-5 shows selectivity for CH 4 and C 2 H m , and Ni/ZSM-5 exhibits better selectivity for CO and H 2 . Under the various pyrolysis conditions, aromatic compounds and aliphatic hydrocarbons consistently dominate the liquid-phase products. With the increase of the pyrolysis temperature, the proportion of aliphatic hydrocarbons decreases, while the proportion of aromatic compounds increases. The addition of catalysts reduces the proportions of both aliphatic and aromatic compounds. PAHs generation is temperature-dependent, significantly increasing at 700 °C. At the low pyrolysis temperatures, the co-pyrolysis reduces PAHs yield, but at high temperatures, PAHs formation increases. The addition of catalysts decreases PAHs yield and toxicity equivalency. Cu/ZSM-5 promotes the cracking of two-ring PAHs, reducing two-ring PAHs yield. Co and Ni catalysts enhance the selective aromatization of small hydrocarbon molecules, forming low-ring PAHs and limiting PAHs aggregation. Overall, Ni/ZSM-5 demonstrates the best performance in enhancing gas production and reducing PAHs emissions, followed by Co/ZSM-5 and Cu/ZSM-5.
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