CHEMOSPHERE
·
2020
·
IF 5.778
Xingtao Zuo,Cheng Qian,Senlin Ma,Juan Xiong
Sulfonamides (SAs) in the aquatic environment are a serious threat to human health, environmental ecology and water reuse . Natural organic matter and SAs are known to compete for adsorption sites on adsorbent. SAs adsorption by high silica ZSM-5 (HSZSM-5) affected by humic monomers remains unclear. The impact of representative humic monomers (HMs) (caffeic acid (CA) and vanillin (VNL)) on the sorption of SAs by HSZSM-5 at different pH was evaluated for the first time. Fourier transform infrared and X-ray photoelectron spectroscopy were used to obtain the group transformations. The presence of HM did not change the main adsorption mechanism of SAs on pristine and loaded HSZSM-5 (pH-dependent and hydrophobic interaction). Lewis acid-base electron interaction , π-π electron donor-acceptor (EDA), and H-bonding had a positive contribution to the adsorption of SAs by HSZSM-5 after HM coating. However, HM coating and competition reduced the adsorption capacity of HSZSM-5 towards SAs. In co-introduction system of HM and SAs, the reaction between C O in HM and N–H in SAs resulted in SAs and HM co-adsorbed on HSZSM-5. Meanwhile, CA concentration <20 mg/L was in favor of SMX adsorption. The findings give an insight into the interactions among HM and SAs in high silica zeolites adsorption system, thereby improving SAs removal in actual water.
研究领域:
环境科学
·
水处理工程
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DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2020
·
IF 4.794
Xiaowei Fang,Ze Wang,Wenli Song,Songgeng Li
In this paper the aldol condensation of furfural (C5) with acetone (C3) over Ca/ZSM-5 was studied with lower dosages of water and acetone as compared to previous studies. It was observed that the formation of CaO over the catalyst is critical to catalyst activity and that the reaction may not occur without water. Although higher quantity of water was favorable for the formation of 4-(2-Furyl)-3-buten-2-one (C8), it was inhibitive for the formation of 1,5-bis-(2-furanyl)-1,4-pentadien-3-one (C13). Highest yields of C8 (38.4 mol%) and C13 (60.2 mol%) were obtained with C3-to-C5 mole ratio of 0.8:1, and water content of 29.7 wt%. The deactivated catalyst was further regenerated by re-loading CaO. An intrinsic kinetic model was established whereby the reaction was first-order dependent on the concentration of each reactant. The formation of 4-(2-furyl)-4‑hydroxy‑butan-2-one (C8-OH), and the C8-OH-to-C8 dehydration were essential steps. The reaction of C8-OH with C5 owned the highest activation energy (41.9 kJ/mol), this step was more sensitive to reaction temperature than those of other steps.
研究领域:
化学工程
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催化化学
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产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Tao Pan,Sida Ge,Mengnan Yu,Yana Ju,Ran Zhang,Pei Wu,Kuanyu Zhou,Zhijie Wu
Zn modified ZSM-5 zeolite supported Ni bifunctional catalysts were prepared by in-situ hydrothermal synthesis (Zn-Ni-ZSM-5), co-impregnation method (Zn-Ni/ZSM-5) as well as combining in-situ hydrothermal synthesis of Zn-ZSM-5 and sequential impregnation of Ni (Ni/Zn-ZSM-5) and used for the selective converting olefin to aromatics applicable for FCC gasoline hydro-upgrading. The Lewis (L) acid sites generated by ZnOH + species and hydrogenation active sites from Ni 0 species were varied with preparation method, in which their locations at the external surface or micropores of zeolite changed the acid properties of catalysts. Comparing to the Zn-Ni/ZSM-5 from the co-impregnation method, direct in-situ hydrothermal method could incorporate Zn and Ni species within zeolite, which makes the strong interaction between the metal species and the framework Al to form medium-strong L acids (ZnOH + /NiOH + ). This leads to the decrease of ratio of Brønsted acid sites to L acid sites (B/L) from 0.40 to 0.12 and the difficulty in reducing of Ni cations to Ni 0 from 57% to 30% Ni 0 percent. Ni/Zn-ZSM-5 sample prepared by incorporating Zn species into micropores and sequential depositing Ni species at the external surface of zeolite possesses a low B/L ratio similar to Zn-Ni-ZSM-5 (0.20 versus 0.12) but a much higher Ni 0 percent (52% versus 30%). Zn-Ni-ZSM-5 shows closer intimacy between Zn and Ni species comparing to Zn-Ni/ZSM-5 and Ni/Zn-ZSM-5. For the 1-hexene aromatization, the formed iso -alkene at acid sites was quickly saturated to iso -alkanes by the adjacent Ni 0 particles over Ni-Zn-ZSM-5 catalyst in hydrogen steam. However, the location of aromatization active sites (ZnOH + , L acid sites) in micropores and hydrogenation active sites (Ni 0 species) on external surface of Ni/Zn-ZSM-5 makes the tandem conversion of n-alkene → iso -alkene → aromatics, rather than the n-alkene → iso -alkene → iso -alkane. Thus, Zn-Ni-ZSM-5 with close intimacy of ZnOH + and Ni 0 particles shows a high iso -alkane selectivity (27.9% iC 4 + ), while Ni/Zn-ZSM-5 exhibits a high aromatics selectivity (39.6 %) in the conversion of 1-hexene in hydrogen steam. Similar results have also found in the conversion of n-heptane. Here, the control of the intimacy of Zn and Ni in ZSM-5 zeolites has been realized to be a good protocol to adjust the selective conversion of olefins/alkanes to aromatics versus iso -alkanes.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Guohua Li,Xianjin Qi,Nina Yang,Xiaoxu Duan,Aimin Zhang
Molecular sieves have also been used for arsenic adsorption in recent years because of their special structure. In order to solve the problem of arsenic pollution in drinking water and/or industrial wastewater , ZSM-5/Fe adsorbent was prepared by loading iron on ZSM-5 molecular sieve. It is also used as an excellent adsorbent for removing arsenic and other heavy metal ions from industrial wastewater. At room temperature, the concentration of arsenic was reduced from 100 mg/L to 0.006 mg/L after the solution pH was adjusted to the range of weak acid to weak base (4–10) and 0.5 g of ZSM-5/Fe adsorbent was added for reacting 2 h. The adsorption capacity reached 40.00 mg/g, the adsorption efficiency reached 99.99%, reaching the national standard of drinking water. Adsorption thermodynamics, kinetics and isotherms showed that the adsorption mechanism of arsenic is heterogeneous nucleation adsorption (including electrostatic attraction and chemical precipitation). Moreover, ZSM-5/Fe adsorbent can adjust pH spontaneously by using non-skeleton Si–Al phase to achieve effective adsorption from weak acid to weak base. At the same time, ZSM-5/Fe adsorbent showed good reusability and stability in five cycles. This study provides an important idea for the application of ZSM-5 molecular sieve in many fields and the efficient removal of arsenic from drinking water and industrial wastewater.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Applied Sciences-Basel
·
2022
·Vol. 12
·期 8
·3769
·
IF 2.838
Wei Ma,Dong Ye,Haining Wang
Herein, a series of Co-Fe mixed oxide modified ZSM-5 adsorbents were synthesized using the ultrasonic-assisted impregnation method for the capture of elemental mercury. In comparison with other samples, Co4Fe1-ZSM-5 produced a relatively better performance, with the removal efficiency of around 96.6% Hg0and the adsorption capacity of around 901.63 ug/mg Hg0achieved at 120 °C. The interaction between CoOxand FeOximproved the reducibility of oxygen species, thus promoting the oxidation of Hg0. Among a variety of other gas components, O2and NO exerted a positive effect on Hg0, which improved its removal to a certain extent. By contrast, SO2caused an adverse effect on the capture of Hg0, which could be reversed to some degree by the introduction of 5% O2. After five cycles, the mercury removal efficiency of Co4Fe1-ZSM-5 remained above 90%, suggesting excellent recyclability. Finally, XPS analysis was conducted to reveal that Mars–Maessen mechanisms are dominant in the process of mercury adsorption.Keywords:Hg0adsorption;ZSM-5;cobalt oxide;iron oxide;regeneration
研究领域:
环境科学
·
化学工程
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DOI
高影响因子
Clean Energy
·
2025
·
IF 3.7
Jiang Zhenhua,Xia Wei,Zhang Yanli,Wang Xinrui,Dong Mingyuan,Chen Kun,Liu Dong,Lu Baowang
This study aims to compare the catalytic performance of ZSM-5 and SAPO-34 zeolite catalysts in the conversion of ethanol. Through experiments conducted at different temperatures (773 K and 673 K), it was found that SAPO-34 initially exhibits superior propylene selectivity compared to ZSM-5. However, the propylene yield on SAPO-34 gradually decreases, while the ethylene yield increases with time on stream. density functional theory calculations were employed for the investigation of reaction mechanism. The results indicate that the SAPO-34 catalyst surface favors propylene desorption, which beneficial for its initial high propylene selectivity. Nevertheless, the smaller pore structure of SAPO-34 limits the effective diffusion of products, leading to product accumulation within the pores and potentially causing catalyst coking and deactivation. By combining the experimental results with theoretical calculation, this study not only explored the selectivity difference between SAPO-34 and H-ZSM-5 in ethanol conversion reaction, but also revealed the influence of different molecular sieve catalyst structures on product distribution and catalyst stability.
研究领域:
催化化学
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材料科学
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计算化学
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产品关联
DOI
高影响因子
Nanoscale
·
2021
·Vol. 14
·期 2
·250-262
·
IF 7.79
Jian Tian,Lixue Qi,Quan Zhang,Guowu Zhan,Daohua Sun,Qingbiao Li
Inspired by the alveolar configuration, an alveoli-like ZSM-5 and the corresponding platinum encapsulated nanocomposite (Pt@PZ5) were fabricated via a dual-template method and a controlled selective desilication–recrystallization strategy. The dimensions of the central cavity, interconnected zeolitic vesicles, and mesoporous shell could be tuned by adjusting the synthesis parameters, as verified by scanning electron microscopy, transmission electron microscopy, nitrogen physisorption investigations, X-ray photoelectron spectroscopy, and X-ray diffraction techniques. Thanks to these properties and merits, the alveoli-like Pt@PZ5 showed the highest catalytic performance with excellent stability, obtaining 100% benzene conversion at 180 °C. Adsorption experiments combined with a finite-element simulation study uncovered that the alveolar architecture could expedite the accumulation of reactants and boost mass transfer; the conversion of intermediates in the voids could be further facilitated, giving optimal catalytic performance. Additionally, the alveolar architecture is resistant to metal sintering (5–20 nm) and leaching, even after calcination at 850 °C for 360 min. This work provides an alveolar concept into the rational design of efficient catalysts for fundamental catalytic action.
研究领域:
材料科学
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催化化学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yaoyu Zhang,Yuxiong Wang,Yue Liu,Huimin Xu,Zhongbiao Wu
Aiming at the coexistence of pollutants in the actual industrial process, the catalytic oxidation of acetonitrile and ethyl acetate mixture on the Cu–Ce/ZSM–5 catalyst was studied. The mutual inhibition effect during catalytic removal of acetonitrile and ethyl acetate mixture was observed. Acetonitrile showed a more obvious inhibitory effect on the conversion of ethyl acetate, and the introduction of ethyl acetate reduced the N 2 selectivity of acetonitrile oxidation. The simulation results demonstrated acetonitrile could be preferentially adsorbed on Cu center of the catalyst surface, leading to significant inhibition of the initial conversion of ethyl acetate. In addition, the coexistence of ethyl acetate would weaken the hydrolysis of acetonitrile to generate carboxylic acid and –NH x species. As such, no enough adsorbed NH x species could be used to reduce the NO x produced by excessive oxidation of acetonitrile, resulting in a decreased in N 2 selectivity. This study could provide reference on the application of catalysts for cyanide–containing waste gas degradation.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Jun-Qing Ye,Pin-Xi Wang,Xin Rong,Qi-Da Ding,Jun-Feng Qian,Sheng-Chun Chen,Ming-Yang He,Qun Chen
Vinylsilane compounds are essential chemical feedstocks and intermediates in organic synthesis. A heterogeneous Cu-containing mesoporous ZSM-5 zeolite catalyst developed through an in-situ doping method can be used for preparing vinylsilane compounds via decarboxylative coupling with remarkable catalytic efficiency. The mesoporous structure along with the appropriate surface area and pore volume of the catalyst is likely to be responsible for facilitating mass transfer in the reaction process. Additionally, due to the suitable Brønsted and Lewis acid active sites, adsorption and activation of reactant molecules can be readily triggered to promote the generation of alkoxyl radicals, which is the crucial species to complete the catalytic cycle. Importantly, the transformation exhibits high efficiency, broad substrate scope, and good reusability for at least six cycles.
研究领域:
有机化学
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催化材料科学
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产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 9
·6664-6672
·
IF 3.201
Yao-Yi Xu,Xue-Ling Wei,Shuai Liang,Ya-Li Sun,Zi-Sheng Chao
Considering the reliable characteristics and the suitable silica alumina content of kaolin, a new way of synthesizing a ZSM-5/NaA hybrid zeolite membrane on 170 mm length ceramic tubes by employing kaolin as a modification layer using a hydrothermal synthesis process was presented for the first time in this work. Kaolin was filtrated on the surface of the support (not only the ceramic tube, but also the NaA membrane layer) as a modification layer not only promoting the interface interlinkage among the support, NaA membrane and ZSM-5 membrane layer, but also promoting the growth of zeolite membranes. The SEM and XRD results showed that compact and homogeneous NaA and ZSM-5 zeolite layers were both formed with the thicknesses being 7.06 μm and 6.14 μm, respectively, after modification with kaolin. The permeation separation experiments demonstrated that the performance of the ZSM-5/NaA hybrid membrane was better than that of the monolayer zeolite membrane with permselectivities of H2 over CO2, N2, CO and CH4 of 5.40, 4.65, 4.70 and 3.93, respectively, which were higher than the corresponding Knudsen diffusion coefficients. Above all, modifying the support with kaolin and then synthesizing the ZSM-5/NaA hybrid membrane could strengthen the performance of the zeolite membrane effectively, which provided a new approach for the synthesis of high performance zeolite membranes in the field of membrane separation.
研究领域:
材料科学
·
膜分离技术
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2013
·
IF 4.75
Huiyan Zhang,Mengmeng Luo,Rui Xiao,Shanshan Shao,Baosheng Jin,Guomin Xiao,Ming Zhao,Junyu Liang
Chemical liquid deposition (CLD) with KH550, TEOS and methyl silicone oil as the modifiers was used to modify ZSM-5 and deposit its external acid sites. The characteristics of modified catalysts were tested by catalytic conversion of biomass pyrolysis-derived compounds. The effects of different modifying conditions (deposited amount, temperature, and time) on the product yields and selectivities were investigated. The results show KH550 modified ZSM-5 (deposited amount of 4%, temperature of 20 °C and time of 6 h) produced the maximum yields of aromatics (24.5%) and olefins (16.5%), which are much higher than that obtained with original ZSM-5 catalyst (18.8% aromatics and 9.8% olefins). The coke yield decreased from 44.1% with original ZSM-5 to 26.7% with KH550 modified ZSM-5. The selectivities of low-molecule-weight hydrocarbons (ethylene and benzene) decreased, while that of higher molecule-weight hydrocarbons (propylene, butylene, toluene, and naphthalene) increased comparing with original ZSM-5.
研究领域:
催化转化
·
能源材料化学
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产品关联
DOI
PubMed
高影响因子
FUEL
·
2021
·
IF 6.609
Mingjie Liao,Xin Ning,Junwen Chen,Jiajun Zheng,Wenlin Li,Ruifeng Li
Zeolite is one kind of the solid acid catalysts for the oligomerization process but surfers from rapid deactivation. In this specific study, a series of mesoporous ZSM-5 catalysts have been synthesized and evaluated in the 1-hexene oligomerization. XRD, BET, SEM, TEM, 27 Al MAS NMR, 29 Si MAS NMR, NH 3 -TPD, Py-FTIR and TGA analysis were used to characterize the physicochemical properties of zeolites. The synthesized mesoporous zeolites were found to be more stable in the reaction and the initial activity increase significantly compared with the common ZSM-5 zeolite . Moreover, the catalytic activity of mesoporous ZSM-5 zeolite is found to be closely related to the number and the distribution of acid sites. The mesoporous ZSM-5 zeolites with the lower amount of acid sites, moderate strength of Brønsted acid sites inhibiting the cracking and coke products. High L/B ratio enhanced the dimers formation. The efficiency was further highlighted by a high space–time yield (STY) of 557 mg·g cat −1 h −1 in the average stage at 260 °C. Compared to conventional ZSM-5 catalyst, the synthesized catalyst displayed excellent resistance to coke deposit.
研究领域:
催化化学
·
材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）