Table of Content
  
15 March 2024, Volume 32 Issue 3
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    Reviews & Prospects
  • Han Qiao, Tan Zhihe, Gao Yujian, Wang Wei, Zhang Chao
    2024, 32(3): 1-8. DOI:10.3969/j.issn.1008-1143.2024.03.001
    Abstract ( ) Download PDF ( ) HTML ( )   Knowledge map   Save

    Producing of 1,3-butadiene from ethanol can replace and replenish the petroleum production route to relieve the pressure caused by the consumption of petroleum resources.The production mechanism of 1,3-butadiene from ethanol was introduced,and the research progress on one-step and two-step methods was discussed respectively.Meanwhile,the existing problems in the process of ethanol preparation of 1,3-butadiene were summarized,and the feasible research direction was put forward.

  • Shu Jie, Mao Qingguo, Bai Peng, Wu Pingping, Yan Zifeng
    2024, 32(3): 9-19. DOI:10.3969/j.issn.1008-1143.2024.03.002
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    C4 olefin is widely applied as a basic chemical raw stock in the petrochemical and polymer industries for the synthesis of special fuels,rubber,plastics,etc.Conversion of low-carbon alkanes to C4 olefins not only effectively alleviates the shortage of low-carbon olefins in China,but also greatly increases the added value of low-carbon alkanes.This paper reviews the current status and research progress on butane catalytic dehydrogenation technology both domestically and internationally in recent years.The mechanism of n-butane dehydrogenation reaction,the effects of catalyst active components,supports,and additives on catalytic dehydrogenation performance and the reasons for deactivation of dehydrogenation catalysts are summarized.The research prospects of butane dehydrogenation process and catalysts are prospected.

  • Wang Liming, Sun Shan, Li Zhilin, Jin Xiaojie, Zhao Yuting, Yu Xiaoxiao, Liu Jichen
    2024, 32(3): 20-28. DOI:10.3969/j.issn.1008-1143.2024.03.003
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    The pollutants discharged by human life and production into offshore waters threaten the ecological environment and human health.The control of heavy metal pollution is the key and difficult point of environmental problems.Traditional technology has limitations such as low efficiency,high cost and many by-products.Photocatalysis is a new catalytic oxidation and efficient clean technology and uses light as energy source,which is widely used in the treatment of various pollutants in water.Due to its excellent adaptability in environmental remediation,photocatalysis can be used in the treatment of heavy metals.The status of heavy metal pollution in marine or other water bodies and its effects on human health were systematically reviewed.Compared with other treatment technologies,the reaction principle and advantages of photocatalysis in the treatment of heavy metal pollutants in seawater were analyzed and explored.The latest progress and effect of different catalysts on the removal of heavy metals from water were summarized,and some suggestions on the existing problems of photocatalysis of heavy metals were put forward in order to provide scientific guidance and theoretical basis for the detection and risk control of marine heavy metal pollution by photocatalysis.

  • Yang Fan, Wang Yiming, Zhu Hanying, Jiang Xu, Shi Xiaobo
    2024, 32(3): 29-34. DOI:10.3969/j.issn.1008-1143.2024.03.004
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    TS-1 is a unique heterogeneous catalyst for selective oxidation in liquid phase with tetrahedral coordination Ti4+ ions in a high crystalline zeolite framework.The TS-1/H2O2 green reaction system has made a considerable breakthrough.The catalytic performance of TS-1 zeolite is related to its topological structure,crystal morphology,framework Ti content and reaction microenvironment.At present,the growing demand for macromolecular oxidation catalysts in petrochemical industry and fine chemical industry has set off a wave of research on the development of novel TS-1 with significantly improved catalytic performance.The research progress and catalytic application of TS-1 in recent years are reviewed in this paper.

  • Catalyst Preparation & Research
  • Yan Jiangmei, Fang Lili, Zhang Peng, Wang Zhaowen, Li Yuefeng, Zhang Zhixiang
    2024, 32(3): 35-40. DOI:10.3969/j.issn.1008-1143.2024.03.005
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    Activated carbon (AC) was modified with hydrogen peroxide and used as supports for preparation of Pd/C catalysts.The characterization results revealed that the AC textural structure and surface properties were selectively modified via different temperature treatments,and the surface functional groups of the supports could affect the dispersion and chemical states of Pd nanoparticles.Compared with other treatment temperatures,the surface of AC treated at 250 ℃ contained more acidic oxygen-containing groups,and the as-prepared Pd/C showed the highest dispersion.In Suzuki coupling reaction for the synthesis of 4’-chloro-2-nitrobiphenyl,an intermediate of boscalid,the activity of the Pd/C was significantly improved,and the reaction yield was increased.The acidic oxygen-containing group provided an effective anchor sites for the dispersion of palladium nanoparticles on the surface of AC,promoted the electron transfer between the support and palladium nanoparticles,and formed relatively electron-deficient Pd nanoparticles,thus improving the activity of Pd/C catalyst.

  • Ma Huanhuan, Chang Liangliang, Cao Baoyue, Wang Tongtong, Du Leixi
    2024, 32(3): 41-45. DOI:10.3969/j.issn.1008-1143.2024.03.006
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    Multi-flaw MoS2 nanosheets were synthesized by a hydrothermal method through controlling the molar ratio of Mo and S.The morphologies and structures of the samples were characterized by SEM and XRD,and the piezoelectric catalytic performance of the sample was evaluated using norfloxacin as the target pollutant.The results showed that compared with flaw-free MoS2,multi-flaw MoS2 nanosheets exhibited excellent piezocatalytic ability.The degradation efficiency of Flaw MoS2 (1∶5) nanosheets for norfloxacin can reach 99.69% in 11 min under ultrasonic irradiation,and the degradation rate constant is 6.78 min-1. The superior piezocatalytic performance of multi-flaw MoS2 nanosheets was mainly attributed to the highly efficient separation of electron-hole pairs caused by the strain-induced piezoelectric field.Active species trapping experiments demonstrated that the hydroxyl radicals (·OH) were the major reactive oxygen species for degradation of norfloxacin.In addition,the ultrafast degradation efficiency of multi-flaw MoS2 nanosheets could be used for practical environmental remediation applications.

  • Zhao Caiyun, Feng Shengdan, Li Ping
    2024, 32(3): 46-52. DOI:10.3969/j.issn.1008-1143.2024.03.007
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    The production of zeolite with excellent catalytic performance using low-cost feedstock has been a focus of academic and industrial attention.Synthesis of zeolite using industrial waste residue not only makes resource utilization of waste residue,but also alleviates the environmental problems caused by waste residue dumping.Here,ZSM-5 zeolite are successfully prepared by hydrothermal method using NaOH pretreated fly ash as aluminum source and part of the silicon sources.ZSM-5 zeolite synthesis did not require the introduction of NaOH to modulate the alkalinity,but required the introduction of an appropriate amount of silica sol as silicon source and tetrapropylammonium bromide (TPABr) as template agent.The effect of temperature,time,template and water were studied using orthogonal experiments of 9 factors 4 levels.ZSM-5 zeolite with long strips of (35-40) μm in length was synthesized under the optimized condition of crystallization time of 60 h,crystallization temperature of 190 ℃,TPABr dosage of 4.5 g,and water dosage of 18 mL.In ethanol and acetic acid esterification to ethyl acetate,a conversion of up to 62% and a yield of 55% over the as-synthesize catalyst were obtained at 130 ℃,90 min,acid to alcohol ratio of 1∶3,and catalyst dosage of 5%.

  • Zhang Juntao, Yang Tingting, Tang Ruiyuan, Liu Kai, Luo Jianling, Zhang Yuyu
    2024, 32(3): 53-60. DOI:10.3969/j.issn.1008-1143.2024.03.008
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    The hydrogenation saturation of polycyclic aromatic hydrocarbons is conducive to environmental protection and promotes the high-quality utilization of coal tar.In this paper,the coal tar fraction rich in 2-4 ring polycyclic aromatic hydrocarbons at (210-360) ℃ was taken as the research object,and the hydrogenation saturated and zeolite catalysts were used as the double effect composite catalyst.The results indicate that the double effect coupling catalyst has the respective reaction characteristics and stable structure with less interaction between zeolite and hydrogenation saturated catalyst,which has catalytic hydrogenation activity between zeolite and hydrogenation saturated catalyst in polycyclic aromatic hydrocarbons.The active metal components Ni and Mo show stable and uniform distribution in the catalyst.The catalytic hydrogenation performance of difunctional coupling catalyst with the coupling ratio of 4∶6 for polycyclic aromatic hydrocarbons is better than other coupling ratio catalysts.Under the process conditions of reaction temperature 380 ℃,initial hydrogen pressure of 8.0 MPa,reaction time of 60 min,and the catalyst oil ratio of 5∶100,the hydrogenation performance of the catalyst is better.After multiple selective hydrogenation of distillate oil,the content of saturates significantly increases,while the content of resin and aromatics significantly decreases.

  • Kang Yu
    2024, 32(3): 61-67. DOI:10.3969/j.issn.1008-1143.2024.03.009
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    Kilograms of spherical clay mesoporous composites (sepiolite,diatomite and attapulgite) were synthesized by centrifugal spray dryer.X-ray diffraction structure analysis,specific surface area-pore size distribution,and TEM testing were conducted to verify mesoporous structure and highly ordered pores in the composites.SEM analysis results show that these three new materials have uniform sphericity and good dispersibility.The influence of atomizer rotation speed and reactant ratio on the particle shape of spherical clay mesoporous composites was also studied,and the best spray drying conditions were obtained.The composition,structure,and microscopic morphology of clay mesoporous composite polyethylene catalysts were investigated in the article.The test results indicate that the three types of clay mesoporous composite materials still maintain good microstructure and unique mesoporous material pore structure after loading polyethylene catalyst.The optimum conditions for the composites were entrance/exit temperature of 200 ℃/100 ℃,content of clay slurry of 30%,and atomizer rotation speed of 12 000 r·min-1.Three new materials were used as carriers to load polyethylene catalysts for high-pressure ethylene polymerization in small-scale experiments.The results showed that the activity of the three catalysts for ethylene polymerization[(4 000-4 300) gPE·(gcat·h)-1]was better than that of the current industrial carrier 955 silica gel loaded with the same metallocene for ethylene polymerization[(1 005 gPE·(gcat·h)-1).The important physical properties of polyethylene powder,including bulk density,melt index,average particle size D50,and crushing rate,are superior to those obtained from industrial 955 silica gel.

  • Fine Chemical Engineering & Catalysis
  • Shang Jianxuan, Yu Chun, Cui Louwei, Pan Liuyi, Wang Hongyan, Li Dong
    2024, 32(3): 68-74. DOI:10.3969/j.issn.1008-1143.2024.03.010
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    The selective hydrogenation of heavy aromatics in coal tar was carried out in a fixed-bed reactor,and the effects of reaction temperature and pressure on the saturation degree of heavy aromatics and the selectivity of monocyclic aromatics were studied.By comparing the four catalysts prepared,the Ni-Mo-P system catalyst with higher selectivity for monocyclic aromatic hydrocarbons was selected.The results of hydrogenation reaction of coal tar distillate shown that the saturation degree of polycyclic aromatic hydrocarbons (PAHs) was 84.2% and the selectivity of monocyclic aromatic hydrocarbons was 60.4% when the temperature was 360 ℃,the pressure was 6 MPa,the liquid hourly space velocity(LHSV) was 0.5 h-1 and the hydrogen-oil ratio was 800∶1.Compared with the distillate oil,the heavy aromatics in the dephenolized oil of coal tar obtained higher conversion and selectivity of monocyclic aromatics after selective hydrogenation.

  • Yu Mingquan, Zhang Hengchen, Yang Xuejiao, Yuan Renxu, Liu Yang, Fang Yanxiong
    2024, 32(3): 75-79. DOI:10.3969/j.issn.1008-1143.2024.03.011
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    The ring-opening metathesis polymer of norbornene-tetracyclododecene was synthesized by using the Ziegler-Natta catalyst with MoCl5 as the core,and a stable monomer conversion of 100% and gel fraction of 0% were achieved.The polymers were heterogeneously hydrogenated by using Al2O3 supported Ru metal catalyst and SiO2/Al2O3 supported Ni metal catalyst.A 100% hydrogenation efficiency could be achieved,and the catalyst could be completely separated from the polymer solution by simple filtration.The products of the two hydrogenation catalysts have different properties.The melt flow index of the hydrogenation product of Ni catalyst is more than 76 g·min-1 and the glass transition temperature is 126 ℃ when mass of total solids feeding is 10% of polymer weight,190 ℃,4 MPa pressure of initial hydrogen and 2 h of reaction time,while the melt flow index of the hydrogenation product of Ru catalyst is 10 g·min-1 and the glass transition temperature is 131 ℃ when mass of total solids feeding is 2% of polymer weight,180 ℃,4 MPa pressure of initial hydrogen and 2 h of reaction time.

  • Environmental Protection & Catalysis
  • Zhang Chenchen, Yu Qian, Yuan Shutang, Zhu Ling, Yang Lin, Chen Chen
    2024, 32(3): 80-85. DOI:10.3969/j.issn.1008-1143.2024.03.012
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    Artificial wetland (CW) and microbial fuel cell technology (MFC) are two potential environmental technologies that are used for water pollution control and renewable energy production.At present,most studies are mainly explored for high-end artificial wetlands-microbial fuel cells,and it is difficult to be used in the actual artificial wetland.Therefore,this article mainly takes vertical flow artificial wetlands as the research object to study the performance and water purification effect of composite vertical artificial wetland-microbial fuel cell coupling system.The results show that in the same vertical current CW-MFC system,the performance of electricity production has a certain relationship with the content of water pollutants;In the case of simulating natural water flow,protons and electrons generated by CW-MFC1 anode biological oxidation can migrate to CW-MFC2 cathode,and undergo oxidation-reduction reactions with its electron acceptors to generate voltage current.Its voltage is higher than a single vertical flow CW-MFC system.In the case of simulation,the CW-MFC system has a good removal effect on various water pollutants.Among them,the removal efficiency of phosphate and total phosphorus is 97.5% and 97.9%.The removal efficiency of ammonia nitrogen and total nitrogen is 86.4%and 66%,and the minimum removal efficiency of COD is 36.5%.It indicates that of water body pollutants are effectively removed in the composite vertical streaming CW-MFC system.

  • Lu Hui
    2024, 32(3): 86-92. DOI:10.3969/j.issn.1008-1143.2024.03.013
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    Bimetallic oxide Fe3O4/CuO catalytic materials loaded on nickel foam (NF) were prepared by electrodeposition synthesis and applied to the cathode of a two-compartment microbial fuel cell (MFC) for the electrochemical removal of chemical oxygen demand (COD),ammonia-nitrogen ($\mathrm{NH}_4^{+}$-N),and phosphorus (P) pollutants from wastewater.The Fe3O4/CuO-NF catalytic material prepared in this experiment was analyzed by electrochemical tests to have significant redox peaks and lower charge transfer resistance,showing higher catalytic activity.The maximum output voltage during the operation of the MFC system reaches 695 mV,and the maximum output power density reaches 576 mW·m-2.The experimental results show that the nickel foam-based bimetallic catalytic material coupled with microbial fuel cell system has efficient degradation performance for COD,$\mathrm{NH}_4^{+}$-N,and P,with removal efficiencies of 92.15%,95.46%,and 97.77%,respectively.It was shown that the Fe3O4/CuO-NF coupled MFC system not only has good performance in electricity production,but also excels in the treatment of organic wastewater.The method is more economical,lower energy consumption,higher efficiency,and has a promising application.