Table of Content

28 March 2022, Volume 22 Issue 3

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Contents

Cover and contents

The Chinese Journal of Process Engineering. 2022, 22(3):  0. 

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Reviews

Review of heat treatment process for spent lithium-ion batteries: from the perspective of pollutant migration and transformation

Hanlin HUANG Chunwei LIU Shaojie YAO Zhi SUN

The Chinese Journal of Process Engineering. 2022, 22(3):  285-303.  DOI: 10.12034/j.issn.1009-606X.221070

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Spent lithium-ion batteries have the dual properties of mineral resources and environmental pollution, they are not only rich in key metals with high external dependence in China, but also contain toxic and harmful substances such as heavy metals and organic pollutants. Efficient recycling of spent lithium-ion batteries is the key to ensure the sustainable development of strategic emerging industries such as electric vehicles. Lithium-ion batteries have various categories associated with complex structures and different organic compounds. Conventional pyrometallurgical and hydrometallurgical processes are likely to produce secondary environmental hazards, which affects the subsequent efficient recycling of metals. Heat treatment has attracted extensive attention in the industry in recent years, since it helps effective recovery of valuable metal resources. Heat treatment technology enjoys many advantages, such as little secondary pollution, attainable equipment, readily scaling up and low costs. Associated with the heat treatment method, the pollution control at the very beginning of recycling spent lithium-ion batteries can not only realize clean production, but also strengthen the subsequent in-depth treatment. Based on the current situation and strategic needs of the industry, this work focused on the generation, migration and transformation of pollutants in the pretreatment of spent lithium-ion batteries. The technical advantages of heat treatment were compared and summarized in the aspects of impurity removal and pollution prevention and control. Meanwhile, the heat treatment processes of spent lithium-ion batteries were systematically classified, and the material transformation mechanism under different heat treatment conditions was summarized.

Synthesis and application of viologen-based electrochromic material

Gaofeng ZHAO Weizhen ZHAO Xiaomin LIU

The Chinese Journal of Process Engineering. 2022, 22(3):  304-317.  DOI: 10.12034/j.issn.1009-606X.221132

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Viologen is a kind of compound with remarkable optical contrast, high coloring efficiency, unique redox stability. It's easy to be used for molecular design and large-area fabrication of devices. Due to its unique properties, viologen electrochromic materials have been widely used in military camouflage, screen display, information storage, intelligent dimming windows and other fields, and become one of the research hotspots. With the rapid development of smart materials, scientific researchers have gradually deepened their research on viologen-based electrochromic materials (including small molecule viologen derivatives, conjugated polymer functional viologen and viologen-based organic/inorganic composite material). In this review, the progresses of viologen electrochromic materials in recent years are reviewed, focusing on the synthesis and application of viologen, the application of ionic liquids or polyionic liquids in the field of viologen electrochromic, as well as the research status of enterprises and research institutions at home and abroad. The existing problems and potential applications of viologen electrochromic materials in the future are discussed from the perspective of industrial application.

Research Paper

Multi-GPUs simulation of turbulent square duct flow in lattice Boltzmann method

Tao HU Xing XIANG Wei GE Limin WANG

The Chinese Journal of Process Engineering. 2022, 22(3):  318-328.  DOI: 10.12034/j.issn.1009-606X.221118

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Compute unified device architecture (CUDA) and message-passing-interface (MPI) were used to implement the lattice Boltzmann method (LBM) multi-GPUs parallel algorithm on supercomputing system Mole-8.5E. The accuracy and effectiveness of the multi-GPUs parallel LBM algorithm was verified by the three-dimensional lid-driven cavity flow. Using this parallel algorithm, large-scale simulations of fully developed turbulent square duct flows with Reynolds numbers Reτ of 300, 600, and 1200 were carried out. Numerical results showed that when the grid size was less than the viscous sublayer, Δ+<5, the statistical error of the transfer characteristics near the wall was low, and the simulation accuracy met the need of engineering application. Meanwhile, when Reτ was 300 and 600, the simulation results at different grid sizes Δ+ showed that the LBM had a weak grid-dependent in the statistics of turbulence characteristics in the square duct central area, and when Reτ was 600, the averaged errors of the mean streamwise velocity predicted by LBM at Δ+=1.667, 3.750, and 6.250 compared with direct numerical simulation (DNS) were 1.357%, 2.994%, and 4.766%, respectively. The characteristics of turbulent square duct flow were studied when Reτ was 300, 600, and 1200, and the corresponding grid size Δ+ was 0.833, 1.667, and 3.333, respectively. The secondary flows were successfully captured, and the predicted mean streamwise velocity, pulsating root-mean-square (rms) velocity and other trends and results were consistent with the literature, which further verified the reliability of the single relaxation time (SRT) LBM, and the numerical results also provided a reference for understanding the turbulence characteristics of turbulent square duct flow at high Reτ. The simulation of turbulent square duct flow verified the potential of the SRT LBM multi-GPUs parallel algorithm in ultra-large-scale grid computing, and laid the foundation for further realization of the larger-scale numerical simulation required in practical engineering.

Numerical simulation and operating parameter optimization of three-stage piston pusher centrifuge

Liqun ZHOU Zhiming WANG Zhennan WANG Yuping LI Zhizhong HUANG

The Chinese Journal of Process Engineering. 2022, 22(3):  329-337.  DOI: 10.12034/j.issn.1009-606X.221078

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In response to the need for improvement of the new three-stage piston pusher centrifuge such as the gradual increase in production capacity, the diversification of raw materials and the optimization of the centrifuge structure, the vital influence of operating parameters on the erosion phenomenon and separation efficiency in the drum during the separation process has been confirmed. The simulation software's pre-processing parameters were concluded based on the raw materials' experimental sampling and the corresponding piston pusher centrifuge provided by the manufacturer, starting from the material's particle size. The three-stage piston pusher centrifuge was modeled in three dimensions, using discrete phase and continuous phase. The solid-liquid separation process was simulated by the combined method and the dense discrete particle model (DDPM) was used to simulate the erosion process. Finally, the data was analyzed in combination with experiments to obtain the size and rules of the erosion of each structure by the particles during the separation process and the new equipment's optimal operating parameters. It was concluded that when the particle size dm of sodium chloride particles was between 0.070 mm and 0.200 mm, as the particle size increased, the solid phase's erosion inside the centrifuge drum became greater. Using prototype experiments and CFD numerical simulation combined with response surface analysis, the interactive influence of each factor of the response model was evident. The influencing factors from high to low were drum's rotating speed, feed concentration, and push frequency for the separation rate. For the erosion rate, the influencing factors from high to low were the drum's rotating speed and the feed concentration. Considering higher separation rate and lower erosion rate as evaluation indicators, the optimal value obtained as push frequency of 40 times/min, drum's rotating speed of 1431 r/min, and feed concentration of 60%. Compared with the experimental data, the simulation error was within the acceptable range.

Dispersion characteristics of droplets in the Q-type static mixer

Huibo MENG Jianbao WANG Yanfang YU Zongyong WANG Jianhua WU

The Chinese Journal of Process Engineering. 2022, 22(3):  338-346.  DOI: 10.12034/j.issn.1009-606X.221104

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Static mixer is widely used in the process industry due to their advantages of compact structure, excellent intensification performance and continuous production. The enhancement mechanism of multiphase flow and dispersion mixing in Q-type static mixer (QSM) are not adequate, which restricts its application in green production of fine chemicals and green production of active pharmaceutical ingredient. The computational fluid dynamics (CFD) coupled with the population balance equation are used to simulate the flow and dispersion performance of droplets in the QSM. The discrete interval number of droplet size in the class method (CM) is set as 16 groups. The numerical simulation result in the classical helical static mixer has a good agreement with the experimental results. The dispersive mixing performance of different medium in RL-90-QSM are studied under Re=8000~24000. The effects of dynamic viscosity, interfacial tension, and phase volume fraction on the Sauter mean diameter (d32) are analyzed, respectively. The Q-type elements have good functions of splitting, recombination, and stretching. At higher Reynolds number and lower phase volume fraction, the average d32 values at different cross section obviously decrease in the first group of elements and then gradually decrease with the increase of mixing time. They become stable after z/l=10. The decreasing ratio of d32 at z/l=11.5 of benzene, toluene, cyclohexane and silicone oil 50 relative to the inlet droplet diameter (2.50 mm) are in the range of 78%~95%, 80%~96%, 73%~94% and 82%~96%, respectively. RL-90-QSM has the advantage of high efficiency and universality for dispersion mixing for the medium with different physical properties. The dispersion performance of droplets in liquid-liquid two phase flow with different continuous phase viscosities and discrete phase viscosities is similar. Compared with dynamic viscosity of discrete phase, the interfacial tension has much more influence on the final mixing result. As far as the restrained aggregation be concerned, the breakup performance of droplets is still predominant at dispersed phase volume fraction no more than 5%.

Breeding of ε-poly-L-lysine high yield strain by ARTP and fermentation condition optimization

Zuwei XU Lihao JI Wenxiu TANG Liang GUO Xiulai CHEN Jia LIU Liming LIU

The Chinese Journal of Process Engineering. 2022, 22(3):  347-356.  DOI: 10.12034/j.issn.1009-606X.221100

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ε-poly-L-lysine (ε-PL) is a natural homo-polymer of microbial origin, consisting of 25~35 L-lysine monomers, which is mainly produced by aerobic microbial fermentation and secreted to extracellular accumulation. Due to its wide antimicrobial spectrum and high safety, ε-PL has been successfully used as a food preservative. Besides, as a safe and green biopolymer, it has also been extensively applied in biomedical, chemical, and many other fields. Unfortunately, the efficient microbial production of ε-PL has reached a bottleneck owing to the limitations of low productivity, long fermentation period and unstable fermentation process, which can not satisfy the demand of industrialized production and brought obstacles to its popularity. To tackle these issues, S. albulus FMME-545RX with high tolerance to rifamycin was firstly screened and obtained by atmospheric and room temperature plasmas (ARTP) mutagenesis combined with ribosomal engineering, which could produce 2.44 g/L of ε-PL, with an increase of 105% in comparison with that of the parent strain S. albulus FMME-545. Then, a series of fermentation optimization strategies, including carbon sources regulation, pH control and dissolved oxygen (DO) regulation, were employed in increasing the production of ε-PL. The final results demonstrated that the mixed carbon source of glucose and sucrose fermentation was helpful to improve the metabolic intensity of bacteria; the addition of sodium citrate in the fermentation process can effectively improve the ability of the bacteria to resist the acidic environment; the optimum pH and DO values for product synthesis were 3.80 and 30%, respectively. Finally, under the controlled fed-batch fermentation, the production, productivity, and dry cell weight (DCW) of ε-PL reached up to 53.0 g/L, 6.63 g/(L?d), and 0.88 g/g, respectively, which were 130%, 131%, and 118% higher than those of the parent strain S. albulus FMME-545. Taken together, this study shows great potential for industrial production of ε-PL and the strategies described here also pave the way to the production of other value-added chemicals.

Microstructure changes of saline?alkali soil influenced by fly ash-based soil conditioner

Shaowen DONG Shuhua MA Mo CHU Xiaohui WANG Yuejiao WANG Chenxu LIU Fenglan HAN

The Chinese Journal of Process Engineering. 2022, 22(3):  357-365.  DOI: 10.12034/j.issn.1009-606X.220371

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The field test results have shown that the physical and chemical properties of saline-alkali soil can be significantly improved by adding fly ash-based soil conditioner. However, at present, the improving mechanism of fly ash-based soil conditioner is not clear, and the structural change law of soil particles is not understood. So this work took the typical saline-alkali soil in the Yinbei area of Ningxia Hui Autonomous Region as the research object, studying the microstructure of saline-alkali soil particles under the action of fly ash-based soil conditioner by X-ray diffraction (XRD), infrared spectroscopy (FTIR), specific surface automatic physical adsorption instrument (BET) and scanning electron microscope (SEM). The results showed that the main components of soil minerals did not change, but a new crystal phase calcite was found in the soil after the fly ash-based soil conditioner was added and the pH value of the soil was greatly reduced from 9.01 to 7.66. The infrared absorption of the soil with fly ash-based soil conditioner changed little, but the absorption peaks of Si-O-Si and organic matters were slightly enhanced. The soil microstructure changed greatly with the increase of the conditioner addition since the small soil particles began to aggregate and the soil porosity gradually increased. Taking the 2.5wt% group as an example, its porosity was up to a level of 21.30% after 15 days and 25.29% after 30 days, which was about twice that of the blank control group. The specific surface area of soil particles increased slightly from the initial value of 23.06 m2/g to 25.55 m2/g after 30 days. The above results proved that fly ash-based soil conditioner could not only alleviate the problem of land salinization, but also realized the large-scale consumption of fly ash solid waste.

Analysis of pyrolysis and volatile products characteristics of Jatropha curcas shell

Baoping DING Huili LIU Fashe LI

The Chinese Journal of Process Engineering. 2022, 22(3):  366-375.  DOI: 10.12034/j.issn.1009-606X.221053

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The pyrolysis characteristics of the Jatropha curcas shell were investigated using thermogravimetric Fourier transform infrared spectrometry (TG-FTIR) and pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). The component information of pyrolysis products and the change of functional groups in organic compounds with temperature 300~800℃ were studied. The Coast-Redfern integral method was used to solve the kinetic parameters at different heating rates. The results showed that the pyrolysis process of the Jatropha curcas shell can be divided into four stages: drying (30~100℃), preheating (100~258℃), pyrolysis (258~420℃) and carbonization (420~900℃). With the increase of heating rate, the maximum mass loss rate of the Jatropha curcas shell increased, and the increase of heating rate promote the thermal decomposition rate of the Jatropha curcas shell. With the increase of pyrolysis temperature, the intensity of absorption peak changed obviously, and the intensity of absorption peak of CO2, aldehydes and ketones gradually decreased or even disappeared. The main gas products were CO, CO2, H2O, etc., and the main volatile organic products were phenol, carbonyl compounds, guaiacol, etc. When the pyrolysis temperature increased from 400℃ to 700℃, the peak area ratio of phenolic compounds increased from 35.94% to 59.59%, the peak area ratio of carbonyl compounds decreased from 36.90% to 11.87%. When the reaction order n=1, the maximum apparent activation energy (E) was 61.34 kJ/mol, and the fitting correlation coefficients of the three heating rates were all above 98%. When the reaction order n≠1 and the n value of the maximum correlation coefficient were selected as the reaction order, then n=0.2, the activation energy (E) was 47.64 kJ/mol, and the pre-exponential factor (A) was 0.83. The apparent activation energy decreased with the increase of heating rate, and the fitting correlation coefficient was above 97%.

Effect of CO₂ content in annealing atmosphere and heating time on billet oxidation

Weidong ZENG Cuijiao DING Fangqin DAI Yue GUO Luwei PAN Ping′an CHEN

The Chinese Journal of Process Engineering. 2022, 22(3):  376-384.  DOI: 10.12034/j.issn.1009-606X.220297

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Gas-fired heating continues to be the main heating method in the steel processing industry. In the reheating furnace before hot rolling, the annealing atmosphere can vary significantly because of the fluctuation of the calorific value of gas. When the calorific value of gas is low, the residence time of billet in the furnace will be prolonged, which will affect the production rhythm. For the above reasons, the oxidation of steel billet in reheating furnace is difficult to predict and control. To achieve quantitative understanding and prediction of steel oxidation in a reheating furnace, an experiment was conducted to study the oxidation behavior of steel billet in simulated atmospheres at the temperature of a soaking zone of the heating furnace. The results of steel oxidation in high purity nitrogen with selected CO2 content at 1523 K (1250℃) are obtained. The result shows that oxidation kinetics curves of samples in different CO2 content are divided into a linear phase and a parabolic phase. In the linear phase, the time and weight gains of the linear phase decrease with CO2 content increase. In the parabolic stage, the parabolic rate constant has a logarithmic relationship with CO2 content. The oxide film on the surface of the sample is divided into a loose compact layer and a loose layer. The compact layer is located on the outside of oxide film consisting of Fe3O4 and its reduction product FeO, while the loose layer is between compact layer and metal matrix and is mainly composed of FeO as well as a few proeutectoid Fe3O4 during cooling. There are voids and cracks inside of the loose layer, and the higher the CO2 content is, the more voids there are. Condensation of vacancy was believed to be responsible for the formation of voids, while increased CO2 content can promote the process. By observing the surface morphology, it can be inferred that FeO in the compact layer might be generated by the reduction of Fe3O4.

Study on mechanism and process of oxidation of methacrolein catalyzed by phosphomolybdovanadic acid

Shenglin ZHANG Jiayuan YU Lei WANG Ruiyi YAN Chunshan LI

The Chinese Journal of Process Engineering. 2022, 22(3):  385-392.  DOI: 10.12034/j.issn.1009-606X.221067

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As an important chemical raw material, methacrylic acid (MAA) is often used in the production of coatings, adhesives, ion exchange resins, etc. Among the production routes of MAA, the oxidation route of isobutene is a research hotspot. In this route, the first step is to produce methacrolein (MAL) by oxidation of isobutene, and then to produce MAA by catalytic oxidation of MAL with heteropoly acid catalyst. Keggin type heteropoly acid catalyst has been successfully applied in this route. In this work, phosphomolybdovanadic acid was took as an example to analyze the adsorption and reaction process of MAL on heteropoly acid catalyst. The results of in-situ FT-IR showed that the ester intermediate adsorbed on the bridging oxygen of heteropoly acid catalyst was important. After MAL adsorption, the ester intermediate was formed and further oxidized to carboxyl intermediate or carbon oxides. The mechanism of catalytic oxidation of MAL over heteropolyacid catalysts was further proposed based on the above conclusions. The reaction process was analyzed at different temperatures. The characteristic peak of vanadium oxide compound in the secondary structure of the catalyst was observed when the reaction temperature rose to 310℃, and the peak was enhanced with the increase of temperature. Referring the results of catalyst evaluation, the conversion of the reaction increased significantly when the vanadium oxide compound transferred to the second structure, indicating that it was the active site in the reaction. It was considered that the migration of vanadium oxide compound from primary structure to secondary structure was the key reason for the significant improvement of catalytic performance. By reduction with H2, the migration of vanadium oxide compound was promoted, and the conversion of MAL and the yield of MAA were further improved. After reduction at 250℃ for 3 h, the catalyst had the highest activity, and the yield of MAA increased from 17.3% to 27.2%.

Catalytic carbonylation of hexanediamine with diethyl carbonate to synthesis hexamethylene dicarbamate

Xitao YUAN Kelin HUANG Liguo WANG Peng HE Yan CAO Shuang XU Jiaqiang CHEN Huiquan LI

The Chinese Journal of Process Engineering. 2022, 22(3):  393-402.  DOI: 10.12034/j.issn.1009-606X.220438

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Hexamethylene dicarbamate (HDI) is an important aliphatic isocyanate are often used in aerospace, aviation, and polymer materials. Compared with aromatic isocyanates, HDI does not contain a benzene ring and has a symmetrical carbon chain skeleton, which makes it light stable and highly decorated. Studies have shown that the non-phosgene method can be used to prepare HDI through the thermal decomposition of the key intermediate hexamethylene dicarbamate. In this work, 1,6-hexanediamine (HDA) and diethyl carbonate (DEC) are used to synthesis hexamethylene dicarbamate ethyl ester (HDEC) under the catalysis of manganese acetate anhydrous. The structure and purity of the self-made HDEC standard sample are determined by FT-IR, 1H-NMR and TG, and a quantitative analysis method is established. Furthermore, qualitative analysis of the main and side products of the reaction is carried out by GC-MS, and the reaction pathway is inferred. At the same time, the reaction parameters are optimized and the reaction mechanism is speculated. The results show that the reaction is achieved in two steps. First, HDA reacts with DEC to form a monosubstituted 1-(6-amino)-hexamethylene monocarbamate (HMEC) intermediate, the process is that manganese acetate attacks -NH2 at one end of HDA to form reactive intermediate I [H2N(CH2)6NHCOCH3], and reactive intermediate I reacts with DEC to form HMEC. Second, HMEC further reacts with DEC to form HDEC target product, the process is that manganese acetate attacks -NH2 at the end of HMEC to form reactive intermediate II [CH3CH2COONH(CH2)6NHCOCH3], and reactive intermediate (II) reacts with DEC to form HDEC. The CH3COOCH2CH3 reacts with Mn(OH)2 to form manganese acetate catalyst in the reaction process. In addition, DEC reacts with HDA and HMEC to form urea by-products during the reaction. Under the optimum reaction conditions, the molar ratio of DEC to HDA is 3.5:1, the reaction temperature is 120℃, the amount of anhydrous manganese acetate catalyst is 15% of HAD initial amount, the reaction time is 5 h and the rotating speed is 400 r/min, the conversion of HDA is 100% and the yield of HDEC is 89.6%.

First-principles study of thermodynamic properties of lightweight dual-phase high-entropy alloy Al₂₀Li₂₀Mg₁₀Sc₂₀Ti₃₀

Wei WANG Jin YANG Ning DING Xiaotao CHEN Biyu TANG

The Chinese Journal of Process Engineering. 2022, 22(3):  403-412.  DOI: 10.12034/j.issn.1009-606X.221086

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High-entropy alloys (HEAs) have attracted plenty of attention over the past decade due to their excellent properties. Compared with face-centered cubic (FCC) or body-centered cubic (BCC) structure, hexagonal close-packed (HCP) structure is rarely found in the single-phase random solid solution of HEAs, and most existing HCP HEAs are composed of rare earth (RE) elements. As a novel HEA, Al20Li20Mg10Sc20Ti30 possess two phases including FCC and HCP phase. And the RE elements in Al20Li20Mg10Sc20Ti30 are only one (Sc), showing that it may open up a new way for the design of less-RE HCP HEAs. Moreover, the advantage of low density about 2.67 g/cm3 indicates the tremendous potential of it in aeronautics and prosthetic devices, etc. In this work, the structure stability and thermal properties of face-centered cubic (FCC) and hexagonal close-packed (HCP) Al20Li20Mg10Sc20Ti30 HEAs are studied from density functional theory in which the chemical disorder of completely random solid solution are treated using the special quasi-random structure (SQS). The theoretical lattice constants for both structures are in good agreement with experimental measurements, and HCP phase has better compressibility resistance due to slightly higher bulk modulus. Both HCP and FCC structures are thermodynamic metastable due to slightly positive formation enthalpies and the chemical bond in HCP is more covalent due to its broader pseudogap. Applying Debye-Grüneisen model, thermal properties of HCP and FCC Al20Li20Mg10Sc20Ti30 are studied under different temperatures. Results show that the bulk modulus of both phases decline gently as temperature increases, and bulk modulus of HCP phase is usually larger. By comparison, FCC phase possesses lager volumetric thermal expansion coefficient. Specifically, temperature dependence of thermal entropy for both phases, including vibrational and electronic contribution, is investigated in details, finding that the HCP has a larger entropy than FCC at investigated temperature range, and the entropies of both phases originate predominantly from the vibrational contribution.

The influence of the structure of the interfacial compatibilizer on the interfacial state and performance of the PLA/PP blends

Bingyu FAN Xinliang CHEN Li YANG Shang GAO Yongjian XIE Zhenfeng WANG Ping WANG Jin LIU

The Chinese Journal of Process Engineering. 2022, 22(3):  413-420.  DOI: 10.12034/j.issn.1009-606X.221087

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Maleic anhydride grafted ethylene-octene copolymer (POE-g-MAH) and glycidyl methacrylate grafted ethylene-octene copolymer (POE-g-GMA) were introduced into the polylactic acid (PLA)/polypropylene (PP) blends to prepare different structures and performance blended materials (PLA/PP/POE-g-MAH, PLA/PP/POE-g-GMA). The effects of compatibilizers with different structures on the regulation behavior of interface state and performance of PLA/PP blends were investigated by the torque rheometer, DSC, SEM, flat rheometer and electronic universal testing machine, etc. The results showed that both POE-g-MAH and POE-g-GMA could improve the interface morphology of PLA and PP, but compared with POE-g-GMA, the interface catalytic efficiency of POE-g-MAH was higher, which could induce PLA and PP more compatible, and catalyzed the formation of micro cross-linking structure at the interface between PLA and PP, which enhance the interfacial interaction between PLA and PP, and finally improved the mechanical properties of the material. When 4wt% POE-g-MAH was introduced, the tensile strength of the PLA/PP/POE-g-MAH blend reached 29.7 MPa, and the elongation at break increased to 39.3%, which was 8 times higher than that of PLA/PP sample. Also, the impact strength of the samples enhanced with the increase of the content of POE-g-MAH, and when its addition amount was 6wt%, the impact strength of the material reached 30.1 kJ/m2, which had a good balance of rigidity and toughness.