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.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Leilei Zhou,Liyan Zhang,Jingrong Li,Tingting Xiao,Peikai Luo,Xinluona Su,Haiyang Cheng,Fengyu Zhao
The hydrodeoxygenation of fatty acids and esters is a critical pathway to produce biofuels. We report an efficient RuRe/ZSM-5(18) catalyst for hydrodeoxygenation of methyl laurate, the selectivity of n -C 12 H 26 reached up to 95.2 % at complete conversion under the reaction conditions of 200 °C, 3 MPa H 2 , 3 h. The contribution of ReO x and acid sites was discussed from the perspective of dynamics and thermodynamics. ReO x was available for the adsorption of substrate and intermediates, the acidity from ReO x species and ZSM-5 are conducive to the cleavage of C O bond. The synergistic effects of ReO x and Brønsted acid sites induced Ru 0 species to be electron-deficient, which preferred to adsorb aldehyde group in a linear adsorption configuration and facilitated for the hydrogenation of the aldehyde intermediate to alcohol, followed by dehydration to produce hydrocarbons. Thus, RuRe/ZSM-5(18) catalyst presented superior activity and chemoselectivity in the hydrodeoxygenation of methyl laurate as well as a series of fatty acids and esters without loss in carbon numbers in reactant.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Ketao Shi,Youbing Zhu,Zhen Xu,Nianming Jiao,Hui Wang
The metal coordination state and the corresponding acid property of zeolite closely relate to its catalytic performance. In this study, DBD-plasma (dielectric barrier discharge-plasma), a low-temperature and energy-efficient external activation method, was proposed to activate the NH4+-type ZSM-5 zeolite and to regulate the Al coordination. It was found that DBD treatment could efficiently decompose NH4+ species at 115 °C, far below that required for calcination (550 °C). Characterizations, including X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), 27Al magic angle spinning nuclear magnetic resonance (27Al MAS NMR), and pyridine-adsorption infrared spectroscopy (Py-IR), revealed that DBD-plasma treatment could inhibit zeolite framework destruction and retain more framework Al and mesoporous structure, thus improving the stability and enhancing the amount of medium-strong Brønsted acid sites. In n-hexane cracking, DBD-activated zeolite exhibited improved conversion and C2–C4 olefin selectivity due to the enhanced monomolecular cracking pathway induced by increased Brønsted acidity, while reducing aromatics and coke formation by suppressing side reactions. This paper presents an alternative method that is more energy-efficient, highly effective, and capable of regulating the metal coordination and acidity of ZSM-5 zeolite.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yihua Yue,Jian Tian,Jiechao Ma,Shui Yang,Wen Li,Jiale Huang,Qingbiao Li,Guowu Zhan
Herein, Ga-ZnZrO x &ZSM-5 bifunctional catalysts were designed for CO 2 thermal hydrogenation to aromatics, particularly, aiming to enhance the selectivity of high-value BTX ( i.e. , benzene, toluene, and xylene). It was evident that the exterior surface properties and acidity of ZSM-5 can be effectively tailored by in-situ silicon deposition originating from the rice husk template. Catalytic performance assessments demonstrate an optimized catalyst achieving 88.1 % aromatics selectivity (exclusive CO) in a single pass, with a notable 45.2 % BTX selectivity within total aromatics and a low CO selectivity of 23.6 %. This superior performance is attributed to the in-situ silicon deposition on ZSM-5 during one-pot synthesis and the optimized spacing between Ga-ZnZrO x and ZSM-5 facilitated by the rice husk platform. Furthermore, in-situ DRIFTS analysis identifies key reaction intermediates. This study offers an effective strategy for tuning zeolite acidity using rice husks, while modulating metal oxide-zeolite proximity on the bio-SiO 2 platform, thus boosting CO 2 conversion to aromatics.
✓ 已验证
产品关联
DOI
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
·
2025
·
IF 6.6
Guoying Fu,Lei Cai,Peihang He,Yan Wang,Yingqi Zhang,Enxue Xie,Liang Li,Zedong Zhang,Guoqiang Wu
A series of Candida antarctica lipase B (CALB) catalysts immobilized on two-dimensional planar ZSM-5 zeolite (denoted as x CAL/ZSM-5-P) were developed for the efficient and green esterification of capric acid (CA) and glycerol (Gly) to synthesize medium-chain glycerides (MCGs). Comprehensive characterizations, including X-ray diffraction, Fourier-transform infrared, scanning electron microscopy, transmission electron microscopy, N 2 physisorption, and thermogravimetric analysis, confirmed the successful immobilization and uniform dispersion of lipase of CALB on ZSM-5-P via sulfhydryl modification. The framework structure of ZSM-5-P remained structurally intact after immobilization. The CAL/ZSM-5-P catalysts exhibited outstanding catalytic performance in the esterification reaction. Notably, the 9CAL/ZSM-5-P catalyst achieved the highest CA conversion of 66.94 %, with nearly 100 % selectivity toward MCGs—substantially outperforming bare ZSM-5-P (without immobilized lipase), which showed only 0.19 % conversion. Additionally, 9CAL/ZSM-5-P demonstrated excellent catalytic stability and chemical robustness. A possible mechanism for the CALB/ZSM-5-P-catalyzed esterification of CA to MCGs was also proposed. This approach provides both theoretical insight and practical guidance for developing MCGs as food emulsifiers and functional oils via heterogeneous catalytic esterification using immobilized lipase in the food industry.
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 45
·17441-17453
·
IF 4.569
Yuewen Shao,Mingzhu Guo,Mengjiao Fan,Kai Sun,Guoming Gao,Chao Li,Félix Mérimé Bkangmo Kontchouo,Lijun Zhang,Shu Zhang,Xun Hu
One-pot conversion of furfural, a biomass-derived platform chemical, to gamma-valerolactone (GVL), a fuel additive and green solvent, involves multiple steps of hydrogenation. Among these reactions, the deep hydrogenation of the furan ring in furfural interrupts GVL formation over Ni or Co-based catalysts. In this study, a method of alloying Ni and Co with Fe over a ZSM-5 support was proposed for tackling excessive activity of the catalyst for hydrogenation. The results indicated that the formation of binary NiFe and CoFe alloys in Ni–Co–Fe/ZSM-5 enhanced the dispersion of metallic species, reduction of metal oxides, formation of more Lewis acidic sites, and the adsorption of the C–O functionality of the furan ring, while lowering the capability for adsorption/activation of H2 and the adsorption of the CC group of the furan ring. These factors together reduced the activity for the hydrogenation of the furan ring in furfural, but enhanced the hydrogenation of the CO in ethyl levulinate (EL). The kinetic study confirmed that the hydrogenation of EL was the rate-determining step. The coordination of the dual alloys, NiFe and CoFe, in the bifunctional Ni–Co–Fe/ZSM-5 catalyst rendered superior activity for selective one-pot conversion of furfural to GVL with a yield of 85.7%.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2022
·
IF 0
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Qingji Ying,Zhongbiao Wu
Cerium-modified Cu/ZSM-5 catalysts were employed for the selective catalytic combustion of acetonitrile. It was obtained that cerium addition effectively improved the mineralization rate of acetonitrile and nitrogen selectivity as well. The optimal Cu5Ce8/ZSM-5 sample exhibited 100% mineralization rate and higher than 95% nitrogen selectivity within 325–500 °C. The strong interaction between Cu and Ce species was induced in a core–shell-like structure of Cu–Ce/ZSM-5 samples, where the Cu–Ce/ZSM-5 core was wrapped with a Cu–Ce mixed oxide layer. The external mixed oxides exhibited enhanced reducibility and increased active oxygen species. In situ diffuse reflectance infrared Fourier transform spectroscopy and density functional theory simulations revealed that surface cerium species strengthened the hydrolysis reaction path of acetonitrile as ceria could effectively promote the dissociation of water and the hydrolysis of cyano groups, thereby generating a sufficient amount of NHx species. As a result, the NOx from acetonitrile overoxidation would be eliminated through internal selectivity catalytic reduction over the Cu–Ce/ZSM-5 core.
✓ 已验证
产品关联
DOI
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yi Zhai,Xubin Zhang,Fumin Wang,Guojun Lv,Tao Jiang,Yuzhou Wu,Mengyue Li,Mengyao Li,Qing Zhang,Yongkui Liu
Development of economic strategy to synthesize hollow zeolite with widely tunable Si/Al ratios providing variable acidity is of great significance in industry. Here, a one-step and low-cost strategy without mesoporogen was successfully developed to synthesize single-crystal hollow ZSM-5 containing mesopores/macropores, with variable Si/Al ratios of about 14–∞ and 114–∞ at critical TPA+/SiO2 ratios of 0.05–0.1 and 0.05, respectively. This is the first time the usage of a large amount of TPAOH was avoided while breaking the traditional limitation of Si/Al ratio (25–50). The component of synthesis system and crystallization temperature acting as the vital roles in hollow structure has been confirmed by a series of characterization. Moreover, according to the investigation of the evolution process, a novel racing crystallization mechanism based on the competition relationship between surface crystallization and the internal dissolution rate was proposed for the first time. The racing crystallization mechanism and internal nonprotective aluminum become the crucial factors for synthesis. The prepared hollow ZSM-5 zeolites exhibit superior catalytic performance in the different acidity-catalyzed condensation involving large molecules between benzaldehyde and n-butyl alcohol as well as 2-hydroxyacetophenone, which is mainly attributed to the property acidity, more accessible active Al sites on the surface, and shorter diffusion path. By calculating, the effectiveness factor (η) of hollow zeolite is close to 1, further confirming its better mass transfer ability. The strategy has also been successfully extended to the synthesis of high-amount Fe-doped, Ga-doped, and B-doped hollow silicate-1.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Qitong Cheng,Benxian Shen,Jichang Liu,Hui Sun,Di Wu,Lei Jiang,Peikun Yan,Xin Pu,Suhui Ou,Jigang Zhao
An alternative and promising route for the production of light olefins which realizes the objective of effective resource usage is the coupling conversion of n -hexane-methanol. The SAPO-34@ZSM-5 core-shell composite has been designed and fabricated by the steam-assisted crystallization (SAC) method for boosting the n -hexane-methanol synergies. SAC avoids the undesired phase transformation/dissolution of SAPO-34 caused by exposure to harsh basic conditions of the ZSM-5 precursor solution. In comparison with the nanosized ZSM-5 or physical mixture, the SAPO-34@ZSM-5 core-shell zeolite demonstrates a 32–38 wt% increase in the light olefin selectivity, a 28–67 wt% increase in the n -hexane conversion, and an 89–143% improvement in the catalyst lifetime under identical reaction conditions. With the aid of GC-MS analysis of carbonaceous deposits in spent catalysts, higher polymethylbenzenes concentration and lower polycyclic aromatic hydrocarbon (PHA) concentration are obtained from the extracted species of spent SAPO-34@ZSM-5 in comparison with that of other samples, which suggests the aromatic-based route to light olefins is enhanced and the carbonaceous deposition is slowed down. The core-shell configuration of the SAPO-34@ZSM-5 composite diminishes the diffusion rate of methanol towards the SAPO-34 core layer and increases the coupling of n -hexane derivatives with methanol in the hydrocarbon pool (HCP) route. The decreased number of acidic sites on the external surface of the SAPO-34 core layer may also be accounted for the inhibited carbon deposition.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 36
·22365-22375
·
IF 3.361
Guangbing Liang,Yanhong Li,Chun Yang,Xun Hu,Qingyin Li,Wenbo Zhao
In this work, industrial biomass power plant ash was used to synthesize the ZSM-5 zeolites for the first time with the original intention to turn value-added material into wealth, and then committed to adsorption performance testing. Typical chemical structure and morphology of ZSM-5 zeolite were identified by comprehensive technologies. Uniquely, it was found that there was a low pressure hysteresis loop which was caused by crossed 10-membered rings in the N2 adsorption–desorption isotherm. To investigate the adsorption performance for dyes, the zeolite samples were used to remove cationic (MB) and anionic (CR) dyes from aqueous. The results demonstrated that when it came to adsorbing MB, the isotherm was in line with the Redlich–Peterson model (R2 > 0.99), whereas it was matched up with the Sips model (R2 > 0.99) for adsorbing CR. Kinetic models were assigned to the pseudo-second order equation (R2 ≥ 0.99) along with remarkable intraparticle diffusion. In the end, thermodynamic parameters were ΔG0 < 0, and Ea > 0. Especially, adsorbing MB was ΔS0 > 0, and ΔH0 > 0, whilst adsorbing CR was ΔS0 < 0, and ΔH0 < 0, which indicates that electrostatic interaction plays a significant role in the whole process. All in all, this work might encourage novel attempts to dispose of industrial biomass ash.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
IF 3.649
Kai Qiao,Feng Zhou,Zheng Han,Jie Fu,Huixia Ma,Guang Wu
Two series of ZSM-5 catalysts with hierarchical porosity were hydrothermally synthesized by adding two types of organosilane reagents (OSA) into the medial synthesis system. The effects of the types and addition amounts of OSA on the pore characteristics, crystallinity, morphology and acidity of the ZSM-5 zeolites were studied by XRD , SEM, TEM , N 2 -adsorption, 27 Al MAS NMR and NH 3 -TPD. Mesopores were generated by introducing appropriate amounts of OSA. In addition, the catalytic performance of the hierarchical ZSM-5s were investigated for the catalytic fast pyrolysis (CFP) of cellulose . The increase in the mesoporosity leads to a reduced amount of coke. However, the highest yield of aromatics was obtained for the mesoporous sample with the greatest microporosity. Thus, the right balance between meso- and microporosity is critical for achieving high aromatic yields. In addition, the distribution of aromatic products is directly related to the microporosity.
✓ 已验证
产品关联
DOI
高影响因子
PETROLEUM CHEMISTRY
·
2017
·Vol. 57
·期 3
·209-214
·
IF 0.493
Liu G. L.,Wang Y. D.,Zhang R.,Liu H. Y.,Liu Z. C.,Meng X. H.
The catalytic cracking performance of light hydrocarbon model compounds (1-hexene, n -octane, i -octane, ethylcyclohexane and ethylbenzene) over a mesoporous catalyst based on ZSM-5 zeolite was analyzed and compared using a microscale apparatus with a fixed-bed reactor. The effects of reaction temperature and weight hourly space velocity (WHSV) on feed conversion and the yields of ethene and propene were investigated. The results showed that with increased reaction temperature, the conversion of model compounds increased monotonically, and that of 1-hexene was close to 100% above 660°C; the yield of ethene plus propene of n -octane, i -octane and ethylcyclohexane increased continuously, while that of 1-hexene and ethylbenzene passed through maximum. With increased WHSV, the yield of ethene plus propene of ethylbenzene increased continuously, and that of the other model compounds decreased continuously. Through comprehensive analysis of the data, it is indicated that 1-hexene exhibited the highest cracking performance, followed by n -octane and ethylcyclohexane, whereas i -octane and ethylbenzene exhibited the lowest.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）