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    28 August 2021, Volume 21 Issue 8
    Cover and Contents
    The Chinese Journal of Process Engineering. 2021, 21(8):  0. 
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    Micro-Nano Bubbles
    Research progress of continuous generation of microbubbles by microdispersion
    Bingqi XIE Caijin ZHOU Xiaoting HUANG Xiangdong MA Jisong ZHANG
    The Chinese Journal of Process Engineering. 2021, 21(8):  865-876.  DOI: 10.12034/j.issn.1009-606X.220341
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    Microbubbles have been drawn more attentions due to their widely applications. At present, the preparation methods of microbubbles mainly include ultrasonic, electrolytic process, dissolved air flotation and microdispersion. Compared with traditional methods of microbubble generation, the microchannel technology has the advantages of high production efficiency, good controllability, excellent flexibility, which has been applied to produce the monodisperse microbubbles and drops. And the microchannels devices with different structures, such as co-flowing microfluidic, flow focusing, T-microchannel and venturi devices are an all-around introduced in this paper. In the process of gas-liquid membrane dispersion, the microbubbles size is affected by many factors, such as liquid flow velocity, liquid surface tension, liquid viscosity, the pore size, porosity, pore structure of membrane and gas flow velocity. So far, the mechanism of microbubbles formation is complicated, which is still not clear. Moreover, it is also critical important to rapidly and accurately measure the size and distribution of microbubbles due to the wide application of microbubbles. Traditionally, the size and distribution of microbubbles are measured by probes and laser particle analyzer, which is efficient and easy accessibility. However, the insertion of probes will affect the flow filed and the mechanism of lase particle analyzer is not clear. With the rapid development of digital image recognition technology, combination of high-speed camera and digital image recognition technology provides an effective, visual and accurate online microbubbles recognition method to measure microbubbles size. Furthermore, the application of deep learning technology in the recognition of microbubbles has drawn more attentions. In this work, the commonly characterization methods of microbubble size are summarized. In addition, the advantages and disadvantages of different methods of preparation microbubbles are also expounded and the current research status of microchannel method and gas-liquid membrane dispersion method are mainly introduced. On this basis, the future research directions of microbubbles prepared by microdispersion are prospected.
    Direct numerical simulation of mass transfer process of single free rising microbubbles under the influence of surface active materials
    Chengxiang LI Yizhou CUI Xiaogang SHI Jinsen GAO Xingying LAN
    The Chinese Journal of Process Engineering. 2021, 21(8):  877-886.  DOI: 10.12034/j.issn.1009-606X.220240
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    The international organization for standardization (ISO) has defined bubbles with the diameter between 1~100 μm as microbubbles in 2017. According to the above definition and the fact that microbubbles are easily affected by surface active materials, the mass transfer rate of single free rising microbubbles with various diameters under the influence of surface active materials was studied by direct numerical simulation. It was found that the velocity and mass transfer rate of the microbubbles were in good agreement with the theoretical results of creeping flow recommended by Clift et al. The adsorption of surface active materials on the surface of microbubble reduced the liquid-side mass transfer coefficient. However, for microbubbles that were greatly affected by surface active materials, the liquid-side mass transfer coefficient increased with the decrease of bubble size, which was different from the trend of clean microbubbles that decreased first and then increased. Therefore, in the application where the effect of surface active materials cannot be excluded, further reduction of the initial size of microbubbles can not only increase the specific surface area of the gas phase but also further increase the liquid-side mass transfer coefficient of the bubble, and the mass transfer capacity can be further enhanced.
    Microbubble enhanced Fe2+ oxidation in phosphoric acid solution
    Yaru WANG Yeqing LÜ Shaona WANG Hao DU
    The Chinese Journal of Process Engineering. 2021, 21(8):  877-894.  DOI: 10.12034/j.issn.1009-606X.220248
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    n order to realize the efficient separation of Fe2+ in acidic media, hydrogen peroxide oxidation method is often used in industry to transform Fe2+ into Fe3+ with lower solubility to realize the precipitation of iron. Due to the low utilization rate of hydrogen peroxide and poor economy, it is urgent to develop a new Fe2+ low-cost and high-efficiency oxidation method. Based on the principle that reactive oxygen species can be generated during the microbubbles bursting, the microbubble enhanced Fe2+ oxidation technology had been developed in this study. The effect of the aeration head aperture, reaction temperature, and acid concentration on the oxidation efficiencies of Fe2+ and ?OH production were studied. The oxidation efficiency of Fe2+ can reach to 99% within 30 min under the optimized conditions (90℃, 30wt% H3PO4, 0.22 μm aeration head aperture). The oxidation effect of microbubble enhanced technology was comparable to the current H2O2 oxidation, and greatly reduced the economic cost of the process. Moreover, the mechanism of Fe2+ oxidation enhanced by microbubbles was studied in this work, and the main reactive oxygen species generated by microbubbles bursting were determined to be hydroxyl radicals, and the influences of aeration head aperture, reaction temperature and acid concentration on the generation of hydroxyl radicals were studied, so as to obtain the regulation rules of hydroxyl radicals in acidic media.
    Reviews
    Preparation of hierarchical porous carbon and its application in supercapacitors
    Ying CUI Wei LIU Saijun XIAO
    The Chinese Journal of Process Engineering. 2021, 21(8):  895-904.  DOI: 10.12034/j.issn.1009-606X.220187
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    The rapid development of the global economy inevitably caused the rapid consumption of fossil resources and serious environmental pollution problems. Thus, the clean production and effective storage of sustainable energy have become one of the urgent problems to be solved. Among the new developed energy sources, solar energy, wind energy, and water energy are considered to be the most promising green energy sources, but the storage and conversion technologies of these energy sources limit their larger-scale applications. In recent years, supercapacitors have attracted great attention in electrochemical energy storage devices due to their outstanding characteristics such as high power density, ultra-fast charge and discharge characteristic and high stability. The energy storage performance of supercapacitors is mainly dependent on the electrode materials. Among the current developed electrode materials, porous carbon materials received more attention because of their excellent electrical conductivity, well-developed pore characteristics, and adjustable morphology structures. Traditional carbon materials are always developed into microporous materials to have a large specific surface area, but this kind of porous carbon also have some unavoidable deficiencies, such as low pores utilization, clogged pores, and large resistance. In order to avoid the defects of single-pore carbon materials in the application process, many researchers are working on the development of hierarchical porous carbon materials with micropores, mesopores and macropores. In this review, the several advanced synthetic strategies of hierarchical porous carbon materials were present in detail through analyzing relevant domestic and foreign literatures. The corresponding formation mechanisms, advantages, challenges and prospects of each method were briefly introduced, and the methods for improving capacitance performance of hierarchical porous carbon material were also summarized. This provides fundamental insight and offers important guidelines for the future design of hierarchical porous carbon and its application in energy storage.
    Research progress on synthesis and industrialization of fatty primary amines
    Jiasheng PAN Yaofeng WANG Shuangshuang MA Rui SUN Yuting TONG Qida DING Rui ZHANG
    The Chinese Journal of Process Engineering. 2021, 21(8):  905-917.  DOI: 10.12034/j.issn.1009-606X.220235
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    Organic amines have a wide range of applications in chemical, pharmaceutical, life science and other fields. They can be used as raw materials for dyes, daily necessities, antibiotics, alkaloids, and clinical medicines. Among different amine compounds, primary amine is the most basic structural unit. Its application is also the most widely used in amine compounds. With the rapid development of economic and social as well as the improvement of people's quality of life, the market demand for primary amines, especially fatty primary amines, is increasing day by day. The synthesis and industrial preparation of fatty primary amines has become an important field. After decades of development, though the production technology of fatty primary amines has achieved great results, there are still some problems such as harsh reaction conditions, insufficient catalyst performance, serious pollution, complicated processes, etc. This work takes the industrial production and hot preparation methods of fatty primary amines as the research object, summarizes the process of preparing fatty primary amines in industry (including alkylation of organic halides with ammonia, reductive amination of alcohol, hydrogenation reduction of nitrile, direct amination of olefin, amination of carboxylic acid, etc.) and illustrates the practical application of each preparation method in industry production. It also analyzes and compares the advantages and disadvantages of each production method. Inferior, the current research hotspot-the method of preparing fatty primary amines by reductive amination of carbonyl compounds is described, and the potential and challenges of the preparation method in future industrial applications are pointed out.
    Flow & Transfer
    Multi-factor effects on and correlation of maximum spouting pressure drop in spout-fluid bed
    Shuang FU Dongxiang WANG Jianfeng YU Hai'an JIN
    The Chinese Journal of Process Engineering. 2021, 21(8):  918-925.  DOI: 10.12034/j.issn.1009-606X.220256
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    The maximum spouting pressure drop (Δpm) is one of the important parameters for the design and operation of the spout-fluid bed. Almost all the literature correlations for predicting the Δpm were developed from single-component particles or spherical particles, and hence were with some limitation in actual application. In view of this, with binary particle mixtures, single-component spherical particles and non-spherical particles as experimental materials, the Δpm was studied based on a rectangular spout-fluid bed with cross section of 200 mm×20 mm, height of 1600 mm and conical base angle of 60°. The results showed that the Δpm increased with the static bed height, particle density, particle sphericity and deposition component ratio, and decreased with the fluidized gas velocity. While with the increase in particle size or spout nozzle size, it went down firstly and then up with a minimum pressure drop. For non-spherical particles and binary particle mixtures, the variation of total pressure drop with superficial spouting gas velocities was found to be similar with that of single-component spherical particles, while the fluctuation range of total pressure drop was larger under the same conditions. Based on the 854 sets of measured data by experiments, a predicting correlation of the Δpm was proposed by dimensional analysis method, which was in good agreement with the measured data in this work and the experimental data in literature.
    Numerical simulation of the effect of magnetic fiber diameter on trapping Fe-based fine particles
    Zhongjian JIA Yongfa DIAO Li′an ZHANG Minghao CHU Henggen SHEN
    The Chinese Journal of Process Engineering. 2021, 21(8):  926-934.  DOI: 10.12034/j.issn.1009-606X.220241
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    In order to achieve ultra-low emissions of fine particles in the steel industry, magnetic fibers are proposed to improve the trapping efficiency of Fe-based fine particles. Based on CFD-DPM (Discrete Phase Model), the effect of traditional fiber and magnetic fiber diameter on the trapping efficiency of Fe-based fine particles and the filtration resistance of the fiber was studied. The results showed that there was no obvious difference in filtration resistance between magnetic fiber and traditional fiber. When the wind speed was 0.10 m/s, for fibers with a diameter in the range of 35~45 μm, the increase in diameter can significantly increase the filtration resistance. Traditional fibers had a low trapping efficiency for particles with a particle size of less than 2.5 μm. As the particle size increase, the trapping efficiency gradually increased. When the wind speed was in the range of 0.01~0.10 m/s, as the wind speed increased, the traditional fiber trapping efficiency decreased first and then increased. For the trapping efficiency of particles with a particle size of 4.5 μm, the traditional fiber diameter had an optimal range of 15~25 μm. For particles with a particle size of less than 2.5 μm, the increase in the diameter of the magnetic fiber had a relatively small effect on the improvement of the trapping efficiency. When the particle size was greater than 2.5 μm, increasing the fiber diameter can significantly improve the trapping efficiency. When the wind speed was in the range of 0.01~0.05 m/s, increasing the fiber diameter had a significant effect on improving the magnetic fiber trapping efficiency; when the wind speed was 0.08~0.10 m/s, the effect of the change in fiber diameter on the trapping efficiency was smaller. The quality factor of magnetic fiber decreased with the increase of fiber diameter. When the fiber diameter was in the range of 10~35 μm, the decreasing rate of the quality factor of increasing fiber diameter was small, and when the fiber diameter was in the range of 35~45 μm, the decreasing rate of quality factor was larger.
    CFD-PBM numerical simulation on the breakup and coalescence process of dispersed phase droplet in Kenics static mixer
    Zongyong WANG Liang WANG Huibo MENG
    The Chinese Journal of Process Engineering. 2021, 21(8):  935-943.  DOI: 10.12034/j.issn.1009-606X.220202
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    CFD-PBM coupling method was used to numerically simulate the breakup and coalescence process of dispersed phase oil droplets in Kenics static mixer. The discrete method was used to solve the population balance model, aggregation kernel and breakage kernel adopt Luo model and turbulent model respectively. A mixture-multiphase model and a realizable k-ε turbulence model were also used. First, by comparing three different initial particle sizes, the influence of initial particle size of the droplet difference on the results was excluded, and the accuracy of the simulation results was verified by comparing with the experimental data. Secondly, the influence of parameters such as Reynolds number, element numbers and element aspect ratio on the particle size of the droplet was analyzed, and the evolution rule of the particle size of the droplet was revealed during the flow of dispersed phase in Kenics static mixer. The results showed that the particle size of the droplet at the outlet of the static mixer decreased with the increase of Reynolds number, and then the critical trend appeared. The particle size of the droplet decreased faster at the first few elements position of the static mixer. The higher the Reynolds number was, the shorter the flow distance required for oil droplets to break to achieve a stable particle size. The number of elements had a significant effect on particle size only at low Reynolds number. At the same Reynolds number, the smaller the aspect ratio was, the smaller the outlet the particle size of the droplet was, and the shorter the flow distance was required to achieve stability. It can be seen from the contour diagram that the change of rotation direction of elements and fluid separation action were the important reasons for droplet breakage. In addition, this can also explain why the smaller the aspect ratio was, the better the emulsification effect was.
    Process & Technology
    Characteristics of silicon-based substances effect on hot-metal dephosphorization process
    Guobin SUN Xiaodong XIANG
    The Chinese Journal of Process Engineering. 2021, 21(8):  944-950.  DOI: 10.12034/j.issn.1009-606X.220183
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    In the context of increasing domestic demand for hot-metal dephosphorization and advocating the utilization of solid waste, it is of great practical value to understand the effect of silicon impurities on the hot-metal dephosphorization when industrial solid waste is used to prepare dephosphorizer. Therefore, in order to explore the effect of silicon-based substances on dephosphorization efficiency, the dephosphorization experiments were carried out by using ferrosilicon and SiO2 to prepare hot-metals containing different mass fraction of silicon and dephosphorizers containing different mass fraction of SiO2. Meanwhile, to further understand the characteristics of hot-metal dephosphorization when different silicon-based substances were used as initial conditions in the slag-iron system, under the condition of ensuring the same molar amount of silicon-based substances, the dephosphorization experiments were carried out by selecting different silicon-based substances involved in desiliconization process as an additive to hot-metal or dephosphorizer, including ferrosilicon, SiO2 and CaSiO3, and the overall mass transfer coefficient of phosphorus in the three experiments was calculated by theoretical derivation and curve fitting. The results had shown that under the conditions of temperature 1400℃ and initial hot-metal phosphorus content of 0.3wt%, when the initial hot-metal silicon content was 0.4wt%, the highest dephosphorization efficiency can be obtained. The effect of initial SiO2 content in the dephosphorizer on dephosphorization efficiency can be ignored. In addition, under the condition that the molar amounts of silicon, SiO2 and CaSiO3 were the same, a higher overall mass transfer coefficient of phosphorus can be obtained in the hot-metal dephosphorization by using the dephosphorizer containing CaSiO3.
    Impurity removal and hydrothermal heterogeneous cryogenic rapid oxidation of semi-dry desulfurization ash from iron ore sintering flue gas
    Rufei WEI Yulong ZHU Di ZHOU Yifan WANG Hongming LONG
    The Chinese Journal of Process Engineering. 2021, 21(8):  951-958.  DOI: 10.12034/j.issn.1009-606X.220223
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    The semi-dry desulfurization ash of iron ore sintering flue gas cannot be effectively utilized because it contains a lot of unstable calcium sulfite. Oxidation modification of desulfurization ash is an important means to realize its large-scale or high-value utilization. The results show that the calcium carbonate in the desulfurization ash is the main factor limiting its oxidation modification. Calcium carbonate and calcium sulfite cover each other, which reduces the specific surface area of calcium sulfite oxidation reaction and limits its oxidation rate. Two weak acids, L(+)-ascorbic acid and glacial acetic acid, were used to remove calcium carbonate. Glacial acetic acid with a concentration of 0.4 g/g could increase the content of calcium sulfite to 81.17% with the maximum increase of 69.71%. The effect of different factors on the oxidation rate of calcium sulfite in desulfurization ash was studied by subcritical hydrothermal heterogeneous oxidation method. The results showed that the oxidation rate of calcium sulfite was significantly increased after removing impurities. The oxidation rate of calcium sulfite can be increased by increasing the initial pressure, the reaction temperature and time, and reducing the solid-liquid ratio. When the reaction temperature was 140℃, the reaction time was 30 min, the initial pressure was 2 MPa, the initial solid-liquid ratio was 1:30 and the rotating speed was 300 r/min, the oxidation rate of calcium sulfite was 98.72%, while the oxidation rate of desulfurized ash without impurity removal was only 78.77% at 180℃(other conditions were the same). In this work, the desulfurization ash was oxidized rapidly at low temperature. From the micro morphology point of view, compared with the desulfurized ash without impurity removal, the calcium sulfite after impurity removal was easier to grow along the radial direction, which had preliminary conditions for the preparation of calcium sulfate whiskers with a large aspect ratio, which was of great significance for the preparation of calcium sulfate whiskers.
    Influence of the dilution gas flow rate on SiO2 deposition on the powder surface during the fluidized vapor deposition
    Zhaoyang WU Zihan GAO Hui KONG Chen XIAN Jixiang JIA Xiangwei LIAO
    The Chinese Journal of Process Engineering. 2021, 21(8):  959-968.  DOI: 10.12034/j.issn.1009-606X.220257
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    Using Fe(Si) alloy particles as deposition basement materials and tetraethoxysilane as gas SiO2 precursor, Fe(Si)/SiO2 composite powders were synthesized under fluidized vapor deposition. The influence of Ar dilution gas flow rate on deposition process of SiO2 insulating medium, and the formation Ar dilution gas flow rate range of complete Fe(Si)/SiO2 core-shell heterostructure were investigated. The results showed that the microstructure of SiO2 insulating medium on the Fe(Si) particle base surface varied from submicron clusters to integrated films to porous films with the increasing of Ar dilution gas flow rate during a fluidized vapor deposition process, while the deposition rates SiO2 insulating medium first decreased, then increased and decreased again. The homogeneity of the SiO2 insulating medium was the best and the deposition rate was 0.069 nm/s when the Ar dilution gas was at a flow rate of 250 sccm. In addition, when reaction temperature, reaction time, gas SiO2 precursor content and carrier gas flow rate was 930 K, 60 min, 9 mL and 100 sccm respectively, the conversion from Fe(Si) alloy particles to complete Fe(Si)/SiO2 core-shell heterostructure particles during the fluidized vapor deposition occurred within the Ar dilution gas flow rate range from 200 sccm to 300 sccm. The results of the performance test indicated that the Fe(Si)/SiO2 core-shell heterostructure led to a substantial enhancement in the electrical resistivity of the particles and reduction in their saturation magnetization, but hardly affected the coercive force. Compare to Fe(Si) alloy particles, the Fe(Si)/SiO2 core-shell heterostructure particles exhibited much higher electrical resistivity. The varying trend of Fe(Si)/SiO2 core-shell heterostructure particles was consistent with the deposition rate of SiO2 insulating medium. The results in this study may provide a foundation for future kinetics investigations and the application of fluidized vapor deposition technology.
    Biochemical Engineering
    Study on humic acid-like components, molecular structure and physiological activity
    Bingkai SHANG Haitao MO Zhuowang FU Xiaoyong ZHANG
    The Chinese Journal of Process Engineering. 2021, 21(8):  969-975.  DOI: 10.12034/j.issn.1009-606X.220291
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    By means of methods of elemental analysis, FT-IR and solid 13C NMR, a comparative study on the component, elemental composition and molecular structure of humic acid-like substances prepared from four different raw materials and humic acids from mineral sources were carried out. Also the physiological activity of four humic acid-like substances was determined by seed germination experiment. The study results showed that the content of fulvic acid in the humic acid-like materials prepared from herbaceous plants (wheat straw and bamboo) was significantly higher than that from woody plants (pine and poplar). The molecular structure of humic acid-like materials was similar to that of mineral humic acid, because both of them had the characteristic functional groups of humic acid. Compared with mineral humic acids, the structures of humic acid-like materials were more complex, and the types and contents of functional groups were different. They have more aromatic structures and lower oxygen-containing functional groups. Also, humic acid-like materials from herbaceous plants had higher aromatization degree and lower molecular weight than those from woody plants. The results of wheat seed germination experiment showed that, when the concentration of the humic acid-like materials was 20~40 mg/L, it can obviously promote the germination of seeds. However the seed growth will be inhibited if the concentration was too high.
    Environment & Energy
    Separation of low-concentration copper ions via the joint effect of electro-sorption and electrodeposition
    Meiqing HU Wei JIN
    The Chinese Journal of Process Engineering. 2021, 21(8):  976-984.  DOI: 10.12034/j.issn.1009-606X.220188
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    Due to the significant importance in modern electronic devices and chemical products manufacture, considerable copper ions have been discharged into the global environment, which requires an effective way to remove and recover. Many conventional techniques have been explored, such as solvent extraction, ion exchange and precipitation. It has been demonstrated that electrodeposition is a promising way to recover copper ions as metallic products, however, it is difficult to directly use electrodeposition for copper recovery in acidic low-concentration copper-containing wastewater due to the performance of inefficient and time-consuming with low-quality products. To achieve efficient separation in the dilute wastewater system, a new stepwise method of electro-sorption and electrodeposition was proposed in this study. Initially, the ACF/CoS had been readily prepared as the low-cost and stable electrode, presenting excellent properties of a larger specific surface area of 33.2 m2/g and specific capacitance of 141.2 F/g at 5 mV/s. It can effectively recovery copper ions by electro-sorption method within 90 min, and the copper ion was concentrated from 30 mg/L to 500 mg/L after desorption and concentration process. Subsequently, it was connected to the turbulent reactor for enhanced electrodeposition, to overcome the bottlenecks of concentration polarization. The results showed that under the voltage of 0.25 V and the current density of 150 A/cm2, the recovery of copper ion can reach 99%, and the energy consumption was only 1.35×10?2 kW/h, which was 50% and 15% lower than the traditional electrodeposition and enhanced electrodeposition under the voltage of 0.40 V. Consequently, with the efforts of the effective electrode and improved mass transfer, the joint method of electro-sorption and electrodeposition exhibits a good prospect for the efficient treatment of low concentration metal wastewater and the recovery of low concentration metal ions.
    Optimization of CO2 absorption process parameters of blast furnace gas based on response surface methodology
    Jinxing ZHANG Yang ZHANG Zhijia HUANG Liping ZHU
    The Chinese Journal of Process Engineering. 2021, 21(8):  985-992.  DOI: 10.12034/j.issn.1009-606X.220245
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    In the practical engineering application of carbon capture and separation of blast furnace gas in steel plant, process parameter optimization is one of the effective ways to reduce the energy consumption of carbon capture system regeneration. In order to explore the influence of the interaction between the factors of carbon capture system on the regeneration energy consumption of regeneration tower, this work takes the blast furnace gas alcoholamine solution absorption CO2 capture system as the research object, combines Aspen Plus with response surface methodology (RSM) to study the lean liquid temperature, lean liquid load, and regeneration tower pressure on the carbon capture system regeneration energy consumption influences. The accuracy of the numerical model was verified by comparing with the experimental data in literature, on this basis, the Aspen Plus simulation data was used as a sample, and the regenerative energy consumption in the sample was used as the response value. The mathematical model was established using the response surface method to obtain the optimized parameter combination with the lowest regenerative energy consumption. The numerical simulation results showed that the lean liquid temperature, the lean liquid load, and the regeneration tower pressure all had significant effects on the regeneration energy consumption, and there was an obvious interaction effect between lean liquid load and regeneration tower pressure. The interaction between the lean liquid temperature and the lean liquid load and the lean liquid load and the pressure of the regeneration tower showed that the change of the lean liquid load and the pressure of the regeneration tower affected the energy consumption of regeneration. The response surface optimization obtained the best process parameters: the lean liquid temperature of 30℃, the lean liquid load of 0.24 mol/mol, the regeneration tower pressure of 1.80×105 Pa, regeneration energy consumption of 3.12 GJ/t, which was 28.4% lower than that of the benchmark experimental program.