FUEL
·
2025
·
IF 7.5
Lifang Cao,Pu Wang,Yuhan Tang,Hong Liu,Jiasheng Wang
Amorphous ZSM-5 was facilely synthesized by simply tuning the aqua ammonia amount and used as support of Mo-V-O for aerobic oxidation desulfurization. It was found that both geometric and electronic effects help to enhance the catalytic performance. Geometrically, the amorphous ZSM-5 could better disperse the metals due to its higher specific area. Electronically, the amorphous ZSM-5 could enable V to enrich electrons availing for oxygen activation to superoxide radical thanks to its low work function. The superoxide radical combines with Mo to form peroxide and then oxidize the sulfur-containing substrates. 100% desulfurization can be realized at 80°C for model oil with sulfur content of 500 ppm over the amorphous ZSM-5 supported Mo-V-O catalyst. This study provides inspiration for designing efficient catalysts for aerobic oxidation desulfurization.
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Caijin Zhou,Chun Shen,Kaiyue Ji,Jiabin Yin,Le Du
Aimed at efficient production of 5-hydroxymethylfurfural (HMF) in a green and sustainable way, dehydrogenation of fructose was enhanced by liquid–liquid extraction in a membrane dispersion microreactor. On account of the high mass-transfer rate resulted from dripping flow, the obtained HMF was readily extracted from the aqueous phase to the organic phase, effectively preventing the sequence side reaction and leading to high HMF selectivity. Enhanced by efficient extraction, the reaction duration decreased from 60 min in a traditional stirred reactor to 4 min in the microreactor, leading to an increase in the space-time yield by 3 orders of magnitude. The effects of total volume flow rate, droplet size, and phase ratio relating to extraction efficiency and HMF yield were systematically investigated. The highest extraction efficiency of nearly 100% coupled with the HMF yield of 93.0% was achieved at the phase ratio of 2 with volume flow rate of 600 mL/h. Overall, this work not only delineates an efficient strategy for synthesizing HMF but also opens a new avenue for reaction systems with subsequent side reaction, which suffer from low selectivity of the intermediates due to the in-line separation bottleneck under conditions of limited mass transfer.
研究领域:
化学工程
·
绿色化学
✓ 已验证
DOI
高影响因子
COMPOSITES PART B-ENGINEERING
·
2018
·
IF 4.92
Lei Wang,Libo Zhang,Hongyi Li,Yubo Ma,Ronghui Zhang
A mesoporous SBA-15 supported sulfonic acid catalyst (SBA-15-SO 3 H) was successfully prepared and used for the selective conversion of fructose to 5-hydroxymethylfurfural (HMF). Up to 96% of HMF selectivity with 100% fructose conversion was obtained under mild conditions (120 °C, 60 min, DMSO as solvent). Solvent effect, reaction time, reaction temperature and fructose-to-catalysts mass ratio have been investigated. The SBA-15-SO 3 H solid acid catalyst can be separated from the reaction mixture after reaction and reused by simple centrifugalization, and 100% fructose conversion with 95% HMF yield could be retained. Further, reaction activation energy of 56.4 kJ/mol has been fitted with kinetic analysis , which means that the dehydration of fructose into HMF is relative easier over SBA-15-SO 3 H catalyst in this work. Besides, X-ray diffraction (XRD), Fourier Transform Infrared Spectroscopy (FTIR) and scanning electron microscopy (SEM) measurements reveal that the –SO 3 H grafting on the SBA-15 surface have no obvious influence on its mesoporous structure even after five catalytic cycles, and acid site measurements demonstrate that there was no significant loss of acid site concentration, indicating high catalytic stability. This fruit give a useful reference to chemical engineering and materials, besides future energy and smart city.
研究领域:
化学工程
·
材料科学
·
能源领域
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Yonghou Xiao,Qiangqiang Xue,Kerun Zhu,Gaohong He
High-efficiency adsorbents are essential for ultradeep desulfurization through selective adsorption, which features low energy consumption without causing secondary pollution. Aluminum oxide is always added as a binder to form physically bound pellets, which weakens the adsorptive desulfurization performance. In this work, a novel micro–mesoporous binderless ZSM-5 (BL-ZSM-5) was successfully prepared through in situ crystallization, which could efficiently remove thiophene from model fuel. Desulfurization ability was investigated by static and fixed bed adsorption. The breakthrough adsorption capacity of thiophene on BL-ZSM-5 reaches 0.38 mg/g, which is twice as high as that of ZSM-5 with alumina binders (Al-ZSM-5). The improvement is attributed to the conversion of alumina into molecular sieves, which could increase the adsorption sites and provide appropriate mesoporous channels for thiophene transfer. The thermal stability of BL-ZSM-5 is superior to that of Al-ZSM-5. The adsorption performance of BL-ZSM-5 is maintained well after 6 cycles of regeneration. The results demonstrate that the attractive prospect of BL-ZSM-5 in highly efficient desulfurization of transport fuels through selective adsorption.
研究领域:
化学工程
·
环境科学
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2018
·
IF 3.525
Wenjin Xu,Guangxu Zhang,Hanwei Chen,Guomeng Zhang,Yang Han,Yichuan Chang,Peng Gong
Two series of Mn/beta and Mn/ZSM-5 catalysts were prepared to study the influence of how different Mn precursors, introduced to the respective parent zeolites by wet impregnation, affected the selective catalytic reduction (SCR) of NO by NH 3 across a low reaction temperature window of 50–350 °C. In this study, the catalysts were characterized using N 2 adsorption/desorption, X-ray diffraction, X-ray fluorescence, H 2 temperature-programmed reduction, NH 3 temperature-programmed desorption and X-ray photoelectron spectroscopy. As the manganese chloride precursor only partially decomposed this primarily resulted in the formation of MnCl 2 in addition to the presence of low levels of crystalline Mn 3 O 4 , which resulted in poor catalytic performance. However, the manganese nitrate precursor formed crystalline MnO 2 as the major phase in addition to a minor presence of unconverted Mn-nitrate. Furthermore, manganese acetate resulted principally in a mixture of amorphous Mn 2 O 3 and MnO 2 , and crystalline Mn 3 O 4 . From all the catalysts screened, the test performance data showed Mn/beta-Ac to exhibit the highest NO conversion (97.5%) at 240 °C, which remained >90% across a temperature window of 220–350 °C. The excellent catalytic performance was ascribed to the enrichment of highly dispersed MnO x (Mn 2 O 3 and MnO 2 ) species that act as the active phase in the NH 3 -SCR process. Furthermore, together with a suitable amount of weakly acidic centers, higher concentration of surface manganese and a greater presence of surface labile oxygen groups, SCR performance was collectively enhanced at low temperature.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jiayu Feng,Fei Wang,Chi Wang,Kai Li,Xin Sun,Ping Ning
In this study, an NH3 plasma-treated Cu/HZSM-5 sorbent was introduced to simultaneously remove H2S and PH3 in low-temperature and low-oxygen environments. The effects of the Cu loading amounts, modification methods, and plasma-treatment conditions on the adsorption–oxidation performance of the sorbents were investigated. From the performance test results, the sorbent treated by NH3 plasma with the specific energy input (SEI, electrical input energy to the unit volume of gas) value of 1 J·mL–1 (Cu/HZSM-5-[S1]) was identified as having the highest breakthrough capacities of 108.9 mg S·g–1 and 150.9 mg P·g–1 among all of the materials tested. After three times of regeneration, the sorbent can still maintain the ideal performance. The results of Fourier transform infrared (FT-IR) spectroscopy and CO2 temperature-programmed desorption (CO2-TPD) indicated that the NH3 plasma treatment can introduce amino groups (functional groups) onto the sorbent surface, which greatly increases the number and strength of the basic sites on the sorbent surface. Results of N2 adsorption/desorption isotherms and scanning electron microscopy–energy dispersive spectroscopy (SEM–EDS) showed that the morphology of the sorbent changed after the plasma treatment, which exposed more active sites (copper species). In situ IR spectra showed that the amino groups are continuously consumed during the reaction process, indicating that these amino groups can help sorbents to capture gas molecules. Moreover, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses indicated that CuO is the main active species and the consumption of CuO and accumulation of the reaction products on the surface and inner pores of the sorbent are the primary reasons for the deactivation of the sorbent.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Fei Wang,Jing Ren,Yunliang Cai,Long Sun,Chuanling Chen,Shuai Liang,Xingmao Jiang
High dispersed palladium nanoparticles with the size of about 3.8 nm confined within ZSM-5 zeolite catalyst (Pd/ZSM-5-IS) was successfully synthesized by in situ synthesis method based on azeotropic distillation assisted fabrication. Liquid phase selective hydrogenation of p -nitrophenol (PNP) to p -aminophenol (PAP) was chosen as model reactions to evaluate the catalytic behavior of the Pd/ZSM-5 catalysts. Thiophene and 4,6-dimethyldibenzothiophene were used as poisons to test their anti-poisoning ability. Pd/ZSM-5-IS catalyst exhibited higher catalytic activity in hydrogenation of PNP to PAP than sample prepared by impregnation method (Pd/ZSM-5-IM), which was mainly attributed to entering of Pd nanoparticles into the intracrystalline mesovoids of the ZSM-5 support for in situ method efficiently prevent active sites from loss and aggregation. In addition, Pd/ZSM-5-IS catalyst not only maintained high activity for five consecutive runs, but also showed high sulfur tolerance for the hydrogenation reactions. This simple and versatile method also can be extended to cover many kinds of other supported catalysts for broad applications in many other catalytic reactions in the future.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2022
·Vol. 29
·期 14
·e202203095
·
IF 5.02
Zihan Zhou,Xingwen Wang,Junjie Li,Yu Gao,Rui Yu,Rongli Jiang
Graphical A green and efficient strategy for synthesizing phosphorus modified ZSM-5 zeolite is proposed by grinding phosphorus source, silicon source and aluminum source with the solvent-free conditions. Phosphorus-modified ZSM-5 zeolites exhibited higher light olefin selectivity and longer catalytic lifetime (33 h) in methanol to olefin reaction when the weight hourly space velocity was 4 h −1 . The traditional hydrothermal synthesis strategy of ZSM-5 zeolite is energy-consumption accompanying by pollution issues. Herein, phosphorus-modified layered ZSM-5 zeolites (PZ) were obtained by one-pot synthesis under solvent-free conditions. The synthesized samples were fully characterized by XRD, SEM, BET, NH 3 -TPD and FTIR. The effect of phosphorus addition on the morphology and catalytic activity of ZSM-5 was investigated. The results showed that phosphorus-modified ZSM-5 zeolites exhibited higher light olefin (ethylene and propylene) selectivity (above 50 %) and longer catalytic lifetime (33 h) in methanol to olefin (MTO) reaction when the weight hourly space velocity was 4 h −1 . Phosphorus-modified ZSM-5 zeolite synthesized by in situ solvent-free method, which not only reduced the discharge of sewage but also showed a simple method to realize the introduction of phosphorous species, which provided a new idea for phosphorus modification of ZSM-5 zeolite.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Runze Jin,Ke Ma,Zhongshun Chen,Zhongqiang Tang,Haobin Hu,Jiaofei Wang,Zhuangzhuang Zhang,Chengyi Dai,Xiaoxun Ma
The selectivity of methanol conversion to aromatics on Zn/ZSM-5 is often limited, mainly because the hydrogen removed during the process combines with low-carbon olefin intermediates to regenerate alkanes and reduce the effective utilization of carbon atoms. Herein, CO 2 is added to the methanol aromatization reaction as a receptor that consumes hydrogen in situ, which reduces the hydrogen transfer reaction and improves the selectivity of aromatics. It is proposed that aromatic selectivity under CO 2 atmosphere is determined by the chemical state of Zn species. Specifically, ZnO converts CO 2 and consumes hydrogen, and ZnOH + promotes methanol aromatization. Under the same conditions, aromatic selectivity of 3ZnZ18-IM under CO 2 atmosphere can reach 85.2 %, which is much higher than that of 71.4 % under N 2 atmosphere. This study provides a new strategy for methanol to aromatics (MTA) reaction, which has a positive impact on solving the energy and environmental problems in the production of aromatics.
研究领域:
化学工程
·
催化科学
·
能源与环境科学
✓ 已验证
DOI
高影响因子
Materials
·
2024
·Vol. 17
·期 6
·1440
·
IF 3.1
Yarong Bai,Chuhan Miao,Weilong Ouyang,Lang Wang,Haiqiang Wang,Zhongbiao Wu
Barium and iridium supported on Zeolite Socony Mobil-5 (ZSM-5) are efficient catalysts for the selective catalytic reduction of nitric oxide by carbon monoxide (CO-SCR), with enhanced cyclic stability. The introduction of Ba hindered the oxidation of metallic Ir active species and enabled Ir to maintain an active metallic state, thereby preventing a decrease in catalytic activity in the CO-SCR reaction. Moreover, the Ba modification increased the NO adsorption of the catalyst, further improving the catalytic activity. Owing to the better anti-oxidation ability of Ir0in IrBa0.2/ZSM-5(27) than in Ir/ZSM-5(27), IrBa0.2/ZSM-5(27) showed better stability than Ir/ZSM-5(27). Considering that all samples in the present study were tested to simulate actual flue gases (such as sintering flue gas and coke oven flue gas), NH3was introduced into the reaction system to serve as an extra reductant for NOx. The NOxconversion to N2(77.1%) was substantially improved using the NH3-CO-SCR system. The proposed catalysts and reaction systems are promising alternatives for treating flue gas, which contains considerable amounts of NOxand CO in oxygen-enriched environments.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Wenqian Song,Yuxin Wen,Guojun Kang,Wenqing Lv,Dekang Li,Haoquan Hu,Lijun Jin,Shijian Lu,Zhong Yan,Pengfei Liu
Amine-based solution absorption as the most promising and commercialized CO 2 capture method, attracted the increasing attention. However, its key lies in improving the CO 2 desorption performance while reducing the energy consumption in desorption. In this paper, HZSM-5 was dealuminated by sulfuric acid, further loaded by Fe 2 O 3 , Co 3 O 4 , NiO and ZnO via impregnation method and used in catalytic desorption of the blended amine solution of N-methyl-diethanolamine and piperazine. Results indicated that sulfuric acid leaching increased the number of acid sites and mesoporous surface area. When sulfuric acid reached 0.8 mol/L, the resultant catalyst (0.8H 2 SO 4 -HZ) improved the amount of the desorbed CO 2 by 10.26% and decreased the heat duty to 2128 kJ/mol CO 2 , with a reduction of 17.01% compared to non-catalytic system. The loading of metal oxides on 0.8H 2 SO 4 -HZ decreased surface area and changed acidity of catalysts. CO 2 desorption amount under catalysis of metal oxide modified M /0.8H 2 SO 4 -HZ followed the order of Fe/0.8H 2 SO 4 -HZ > Zn/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ, whereas the relative heat duty was in order of Zn/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Fe/0.8H 2 SO 4 -HZ. Fe/0.8H 2 SO 4 -HZ exhibited excellent catalytic performance, along with 12.82% increase in amount of CO 2 desorbed and reduction in heat duty to 2039 kJ/mol CO 2 , with a 20.49% decrease. Meanwhile, Fe/0.8H 2 SO 4 -HZ showed good stability after ten cycles and the addition of Fe/0.8H 2 SO 4 -HZ promoted CO 2 absorption. Suitable pore structure and abundant acid sites of the modified catalyst contributed to proton transfer and decomposition of carbamate. A possible mechanism for catalytic desorption over modified HZSM-5 was proposed. The work indicates that catalytic desorption by modified HZSM-5 catalyst is a promising way to decrease the energy consumption of amine solution regeneration.
研究领域:
化学工程
·
环境科学
·
能源化学
·
催化化学
·
气体分离
·
材料科学
·
工业催化
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Tinghu Wang,Yuzhi Li,Wenjing Zhang,Furang Li,Lei Fan,Jianye Fu,Xinmei Liu,Yuchao Lyu
Acidity of supports always plays a key role in the determination of dispersion and electron density of metal components and then the catalytic behavior of bifunctional catalysts for deoxygenation of biomass-based resources. Herein, Ni/ZSM-5 catalysts with various Si/Al ratios and acidity were synthesized, and the role of acid centers in the deoxygenation of methyl laurate (ML) was discussed. The decreasing Si/Al ratios promote dispersion of Ni due to the anchoring effect of framework Al to nickel species. It also increases the electron density of Ni, which not only benefits the activation of hydrogen but also curbs the cleavage of C–CHO bonds. All of these accelerate ML transformation and preferentially promote the hydrodeoxygenation (HDO) route instead of decarboxylation (DCO2) or decarbonylation ones. The metal centers play a key role in the hydrogenolysis of ML and the hydrogenation of resultant fatty acids, while the acid centers can facilitate these processes. Besides, suitable acidity of the catalyst would increase selectivity to target alkanes and isomerized ones for biojet fuels by enhancing the HDO routes. However, excessive acid centers favor cracking reactions, reducing the selectivity of target products. This work contributes a profound understanding of the role of acid centers in the deoxygenation of ML into biojet fuels and can be extended to other bifunctional deoxygenation catalysts.
研究领域:
催化化学
·
能源科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）