INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
·
IF 4.326
Wenhui Li,Jiaxing Zhang,Xiao Jiang,Minchen Mu,Anfeng Zhang,Chunshan Song,Xinwen Guo
Carbon dioxide (CO2) hydrogenation to gasoline through the methanol-mediate route using the metal oxide/ZSM-5 tandem catalyst has attracted considerable attention to reduce the pernicious effect of CO2 on global climate change and to reduce our dependence on fossil fuels. The C5+ molecules are preferred to pass through the straight channels of ZSM-5 zeolite, where side reactions may occur on the acid sites and the catalyst is deactivated due to pore blockage. Thus, the thickness of ZSM-5 along the straight channel, namely the b-axis direction, is crucial to manipulating the product distribution and catalyst lifetime. Here, HZSM-5 nanosheets with different thicknesses (2 nm to 2 μm) along the b-axis were synthesized controllably and composited with In2O3/ZrO2 as tandem catalysts for CO2 hydrogenation to gasoline. In2O3–ZrO2/HZSM-5 with a thickness of 20 nm shows the highest selectivity toward C5+ hydrocarbons under isoconversional conditions and no deactivation after 150 h of reaction with less carbon deposition compared with the 2 μm one. Comparative activity tests and characterization results demonstrate that an appropriate length of straight channels can benefit the production of C5+ hydrocarbons through the polymerization of short-chain molecules while preventing the cracking of long-chain hydrocarbons on acid sites. Adding an appropriate loading of Co into tandem catalysts with optimal composition gives rise to further enhancement in CO2 conversion by 10%, and a slight increase in C5+ selectivity. This can be attributed to the Co-induced hydrogen spillover from metallic Co to support ZrO2, facilitating the formation of the key intermediate and its subsequent hydrogenation steps. This study provides insights into designing effective and anti-carbon deposition tandem catalysts for CO2-to-gasoline by manipulating the channel length–resident time–acidity relationship and the promoter effect.
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Yang Huang,Tianyi Gao,Chong Sun,Tingting Han,Mingwu Zang,Daoying Wang,Weimin Xu
In this study, an electrochemical platform based on a novel ternary nanocomposite of advantageously united gold nanoparticles , polypyrrole and graphitic carbon nitride (Au-PPy@ g- C 3 N 4 ) for detection of guanosine-5’-monophosphate (GMP) was designed. Owing to the π-π stacking interaction between the ring structures of the nucleobases in GMP and the hexagonal cells original from g -C 3 N 4 in Au-PPy@ g- C 3 N 4 , the irreversible oxidation of GMP occurred with the potential of 1.08 V (vs. SCE) in phosphate buffer solution (PBS). Under the optimized conditions, the peak currents were linear with the concentration of GMP ranging from 0.05 to 200 μg•mL −1 with a detection limit of 0.028 μg•mL −1 (S/N=3). Meanwhile, the Au-PPy@ g- C 3 N 4 /APTES/GCE sensor exhibited good stability, high reproducibility and acceptable anti-interference ability. Importantly, the results of the detection of GMP with the proposed sensor were well consistent with the data determined by high performance liquid chromatography (HPLC), indicating a promising platform for evaluation of soup quality.
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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.
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PubMed
高影响因子
ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yu Wang,Juanjuan Wang,Ming Guan,Parashuram Kallem,Hongdeng Qiu,Jia Chen
In this work, Fe/Ni bimetallic nitrogen-doped porous graphene (Fe/Ni-NPG) nanomaterials with rich pores, strong magnetism and good reusability were successfully prepared by one-step combustion and can be used as magnetic solid phase extraction (MSPE) adsorbents for the determination of 5-nitroimidazoles (5-NDZs) in environmental water samples. The dispersion and active sites of the materials were increased by the introduction of nitrogen. The adsorption behavior of Fe/Ni-NPG for 5-NDZs was investigated, which corresponds to the quasi-second-order kinetics and Langmuir adsorption model. The π-π electron donor-acceptor interaction (π-π EDA), hydrogen bond and electrostatic interaction between Fe/Ni-NPG and 5-NDZs are the main factors that help to obtain excellent adsorption properties. Several important conditions of MSPE are systematically optimized. Under the optimal MSPE conditions, the linear range of DMZ was 0.6–500 μg/L, the linear range of TNZ and ONZ was 0.7–500 μg/L, and the correlation coefficient R 2 ≥ 0.9991. The limit of detection was 0.18–0.2 μg/L, the limit of quantification was 0.6–0.7 μg/L, and the RSDs of intraday and interday precision were 1.58%–4.66% and 3.77–9.69%, respectively. In the three spiked actual environmental water samples, the recovery was 78.05%–107.05% (RSDs<7.82%). The results show that this method based on Fe/Ni-NPG provides an accurate and reliable way to detect 5-NDZs in environmental water.
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高影响因子
Processes
·
2022
·Vol. 10
·期 10
·1970
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IF 3.352
Xuan Zhou,Hongling Pan,Shuixiang Xie,Guotao Li,Zhicai Du,Xiang Wang,Yan Luo
The aim of this research is to design and synthesize an efficient catalyst to enhance high value-added products, such as aromatic hydrocarbons and phenols, from the catalytic fast pyrolysis (CFP) of different types of forestry and agricultural residues. All three biomasses (rape straw, wheat straw, and bamboo powder) had no aromatic production via thermal pyrolysis alone; however, the aromatic selectivity and monocyclic aromatic selectivity were largely enhanced using ZSM-5, with suitable silica-alumina ratios and Ni loadings. Specifically, for rape straw, the optimum catalyst was 15 wt.% Ni/ZSM-5 (silica-aluminum ratios = 85), and the selectivity of aromatic hydrocarbons was achieved at 39%, of which 71% were monocyclic aromatic hydrocarbons. For wheat straw, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was 67%, of which 55% were monocyclic aromatic hydrocarbons. For bamboo powder, the optimum catalyst was 10 wt.% Ni/ZSM-5 (silica-aluminum ratios = 18), and the selectivity of aromatic hydrocarbons was achieved at 21%, of which 80% were monocyclic aromatic hydrocarbons. Meanwhile, biomass types have significant effects on the pyrolyzed product distribution due to their different components. Cellulose and hemicellulose promoted the production of aromatic hydrocarbons, while lignin enhanced the production of phenols. The promotion of phenol by Ni was better and more efficient than that by the molecular sieve.Keywords:catalytic fast pyrolysis;forestry and agricultural residues;Ni/ZSM-5;aromatic hydrocarbons;phenols;Py-GC/MS
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Crystals
·
2022
·Vol. 12
·期 7
·948
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IF 2.67
Haolong Zhai,Xiaoping Cui,Yuping Gan
Taking the combustion tear gas mixture as the research object, the system formula was optimized by adding a different mass fraction of 5-amino-1H-tetrazole(5AT). TG-DSC, a thermocouple, and a laser smoke test system were used to characterize the characteristic combustion parameters such as combustion temperature and velocity, as well as the end-point effects such as smoke concentration and particle size. Starink’s method, the Flynn–Wall–Ozawa method, and the Coats–Redfern method were used to evaluate the pyrolysis kinetic parameters of the samples. The results show that when the mass fraction of 5-amino-1H-tetrazole in the system is 10%, the maximum combustion temperature of the sample decreases by nearly 70 °C and the smoke concentration increases by 12.81%. The kinetic study also found that with a different mass fraction of 5-amino-1H-tetrazole in the system, the main reaction model of the mixed agent in the first, third, and fourth stages of pyrolysis changed significantly, but for the second stage of sample pyrolysis, the main reaction model (the A4 model) showed a high degree of consistency, which can be considered as the thermal diffusion stage of the tear agent capsicum oleoresin (OC) (the temperature range is 220~350 °C), which is highly consistent with the results of the TG-DSC analysis. It was also confirmed that OC’s thermal diffusion is mainly concentrated in this stage. The results of this study show that adding an appropriate amount of the combustible agent 5-amino-1H-tetrazole to the combustion tear gas mixture can improve its combustion performance and smoking performance, which provides an important, new idea for the development of a new generation of safe, efficient, and environmentally friendly tear gas mixtures.Keywords:5-amino-1H-tetrazole;tear gas mixture;combustible agent;combustion pyrolysis characteristics;dynamics research
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FUEL PROCESSING TECHNOLOGY
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2022
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IF 8.129
Xiangbo Song,Yuhe Liao,Tingsen Liu,Dedu Yin,Haiyong Wang,Lungang Chen,Longlong Ma,Hongwei Yang,Leonid G. Voskressensky,Chenguang Wang
Synthesis of 5-hydroxymethylfurfural (HMF) from carbohydrate is one of vital step for bio-refinery development. In this work, a novel strategy was developed for catalytic conversion of fructose to HMF in 2-butanol. The inexpensive ionic liquids were used to adjust the acidity of biobased acid catalyst for enhancing the dehydration of fructose to HMF. The combination of 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) with oxalic acid afforded an excellent HMF yield of 97.1% at 98.7% fructose conversion under mild conditions of 100 °C and 60 min, owing to the enhanced dissociation ability of oxalic acid by [Bmim]Cl. A possible dissociation mechanism of oxalic acid induced by [Bmim]Cl was proposed based on control experiments and detailed analyses with NMR and FT-IR techniques. It involved that the [Bmim]Cl interacted with oxalic acid through hydrogen bond , which decreased the electron density of oxygen atom on hydroxyl group and weakened the O-H bond, thus making the hydrogen in the O-H group to easily dissociate in the form of H + . Moreover, the reusability of oxalic acid and [Bmim]Cl was demonstrated, and both could be reused up to six times without significant loss in activity
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 10
·1-9
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IF 3.061
Huangfu Fei,Li Wanrong,Yang Zhongqiang,You Jiang,Yang Po
This work aims to explore the bulk ring-opening metathesis copolymerization of dicyclopentadiene and 5-ethylidene-2-norbornene by modifying the comonomer feed ratios. Thorough studies showed that their performance can be enhanced by polymerization at elevated temperature and there was a little deviation of properties from mixing rules. That is, the copolymers properties depend on monomer composition and can be roughly predicted by empirical mixing rules. We believe this can help researchers design and prepare ROMP derived polydicyclopentadiene copolymers and apply them in more applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Haochen Qi,Chuang Xing,Weiguo Huang,Mingquan Li,Yujia Jiang,Xu Sun,Heyang Liu,Peng Lu,Jiangang Chen,Shuyao Chen
Fischer-Tropsch (FT) synthesis as a strongly exothermic reaction has diffusely manufactured clean fuels from syngas. However, it is difficult to obtain the concentrated product distributions. Here, we design ZSM-5 encapsulated cobalt particles on the thermal conductivity of the SiC matrix. The Co@NaZSM-5/SiC capsule catalyst with hierarchical structure is ingeniously assembled through a solvent-free synthesis route. Due to the joint functions of acidic zeolite , SiC thermal conductivity and macropores, the olefin selectivity enhances to 32.3% on the Co@NaZSM-5/SiC catalyst. Moreover, the ratio of O 5-11 /C 5-11 approaches 49.1% suggesting the elevated middle olefin proportion. The H + ion-exchanged Co@HZSM-5/SiC capsule catalyst shows a high isoparaffin selectivity of 27.3%, since the olefin isomerization reaction is accelerated over strong acid sites. Besides, Co 2 C phase is readily formed during the FT reaction, which is an activity center for olefin synthesis. The capsule catalyst with the proper acidity, thermal conductivity, and hierarchical structure is a promising prospect for tuning production distribution in FT reaction.
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APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Ge Yang,Xi Yan,Yan Chen,Xiao-Jing Guo,Wan-Zhong Lang,Ya-Jun Guo
In recent years, Ga-based catalysts attract much attention in propane dehydrogenation (PDH) reaction due to environmental friendliness and low cost. Nevertheless, it is still challenging to obtain high selectivity of propylene under harsh reaction conditions. In this work, the supported catalysts (Ga- x Mg/ZSM-5) were prepared with the sequential impregnation method and applied in the PDH reaction. The results show that MgO as an additive reduces the acidity of the catalysts, promotes the dispersion of Ga 2 O 3 and improves the selectivity of propylene. As a result, the average particle size of the Ga/ZSM-5 catalyst is larger (4.5 nm), and the initial propylene selectivity is only 71.0 %. In contrast, the optimal Ga-0.7Mg/ZSM-5 catalyst shows the smallest particle size (2.4 nm) and the highest propylene selectivity of 90.8 %. In comparison with the previous GaO x catalysts in literatures, the Ga-0.7Mg/ZSM-5 catalyst exhibits a superior production rate of propylene ( r C 3 H 6 ) based on either catalyst weight or Ga 2 O 3 weight.
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高影响因子
FUEL
·
2022
·
IF 8.035
Fuwei Li,Xiaofeng Wang,Hengshuo Gu,Hongbing Fu,Asad Ali,Hongfei Lin,Zhixia Li
Minimizing the catalyst cost is critical to achieving long-term economic feasibility for obtaining bio-chemicals directly from biomass. In the present study, low cost ZSM-5 was synthesized via hydrothermal crystallization of the activated aluminosilicate gel without adding any organic ammonium templates and additional seed crystals . The activation process promoted the depolymerization of the silica-alumina species and the formation of active pasty gel containing nucleation precursors, consequently accelerating the subsequent crystallization reaction. The addition of eucalyptus sawdust (ES) in the synthesis process increased the BET (Brunauer-Emmett-Teller) surface area and acidity of the resultant zeolites . The ES-mediated ZSM-5 (AGZ-10) achieved a higher benzene, toluene, ethylbenzene and xylene (BTEX) carbon yield (18.9 %) from co-cracking of ES and waste plastics (WP) (ES/WP mass ratio at 1:1) at 500 °C and exhibited better synergistic effect and anti-coking ability compared to the commercial ZSM-5. The results provide an efficient synthetic strategy to produce low-cost zeolites, and a promising technique to effectively utilize biomass and plastic wastes.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Jian He,Huining Zhao,Xinru Hu,Zhiyong Fang,Jilin Wang,Rui Zhang,Guoyuan Zheng,Bing Zhou,Fei Long
In this study, a new type of 0-dimensional organic–inorganic hybrid perovskite single crystal (2-5-py)2MnBr4 was synthesized using 2-amino-5-methylpyridine (2-5-py) as the organic ligand. The crystal is a center-symmetric P-1 space group with a grain size of 20 mm, which belongs to the triclinic crystal system. It has a strong absorption of violet and blue light as well as excellent thermal stability. Its optical band gap is 2.38 eV, which is in good agreement with the theoretical band gap (2.39 eV) calculated by density functional theory. Under the excitation of a suitable light source, it can emit 526 nm pure bright green lights, which are confirmed by the main peaks to be almost in the green range with a full width at half maximum of 45 nm. As a result, the quantum efficiency and fluorescence lifetime reached a high level of 44.2% and 117 μs, respectively. Based on the good fluorescence performance of the crystal, a white LED with a color rendering index of 97 was finally successfully fabricated, realizing the leap from basic materials to optoelectronic devices.
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