Table of Content

10 February 2024, Volume 45 Issue 2

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Cover and Content of Chemical Journal of Chinese Universities Vol.45 No.2(2024)

2024, 45(2):  1-6. 

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Review

Advantages and Research Progress of Metal-organic Framework in Supercapacitors

LU Chunyu, JING Yuan, WEI Xiaofei, YAO Shiwei, WANG Zhifei, WANG Shubin, DAI Fangna

2024, 45(2):  20230450.  doi:10.7503/cjcu20230450

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Metal-organic framework（MOF） plays an important role in gas separation， energy storage， catalysis and other fields due to its excellent surface area， numerous active sites， adjustable pore size range and flexible framework structure. In recent years， the use of MOF materials with high surface area， permanent pores and inherent redox active sites as electrode materials for supercapacitors has attracted close attention from researchers. This paper starts with the application research of MOF in the field of supercapacitors， introduces the effects of their properties and structures on the electrochemical properties of supercapacitors emphatically， and elaborates the research progress of MOF property regulation and structure design. First of all， the conductivity of MOF is a key performance that affects the energy density and power density of supercapacitors， and the special structure of the material directly affects the conductivity. Secondly， the abundant active sites and adjustable pore size of MOF create conditions for its improvement of electrical conductivity. In addition， the structural stability of MOF is closely related to the cycling performance of supercapacitors. The construction of stable structure is an important prerequisite for enhancing the cycling performance of supercapacitors. Finally， the future research of MOF in the field of supercapacitors is prospected. The structure regulation is still an important research direction in this field.



Article: Inorganic Chemistry

Construction of a Eu-MOF Material with Fe³⁺ and Nitro-aromatic Explosives Fluorescence Detection Performance

JI Chao, LI Wen, ZHANG Lirong, HUA Jia, LIU Yunling

2024, 45(2):  20230455.  doi:10.7503/cjcu20230455

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Massive release of metal cations and nitro-aromatic explosives causes a serious threat to the environment and human health， and their efficient detection is of great research significance and challenge. Metal-organic frameworks（MOFs） are considered as a promising fluorescence sensing detection platform. A Eu-MOF material， ［（CH₃）₂NH₂］₂［Eu₆（μ₃-OH）₈（EDDC）₆］·8DMA·3MeOH·6H₂O［JLU-MOF128， H₂EDDC=（E）-4，4′-（ethene-1，2-diyl）-dibenzoic acid］， with fcu topology， was synthesized under solvothermal conditions. The structure and composition of JLU-MOF128 were characterized by single crystal X-ray diffraction， powder X-ray diffraction， X-ray photoelectron spectroscopy， infrared spectroscopy， elemental analysis and thermogravimetric analysis. Owing to the introduction of the fluorescent H₂EDDC ligand， JLU-MOF128 exhibits significant fluorescence properties. The metal cations and nitro-aromatic compounds detection results indicate that JLU-MOF128 is an ideal multi-induction fluorescence sensor with good fluorescence detection performance for Fe³⁺， 2，4，6-trinitrophenol（TNP）， and 2，4-dinitrophenol（2，4-DNP） in N，N-dimethylformamide（DMF）， with K_sv values of 2.09×10⁴， 8.49×10⁴ and 5.75×10⁴ L/mol， and detection limits of 5.99， 1.51 and 1.93 μmol/L， respectively.



Analytical Chemistry

MOFs-based Microfluidic Chips for Real-time Online Determination of Multiple Heavy Metal Ions

CHEN Xiaoping, WANG Xutan, LIU Ning, WANG Qingxiang, NI Jiancong, YANG Weiqiang, LIN Zhenyu

2024, 45(2):  20230395.  doi:10.7503/cjcu20230395

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This study combines the accumulation effects of rich microporous ZIF-8 metal-organic framework（MOF） and the electrochemical technology for the metal ions， and the controllable ability of microfluidic devices for the flowing of solution， to construct a new type of sensor to achieve high-throughput， real-time and rapid detection of multiple metal ion contaminations in the environment. The developed ZIF-8-Nafion/ITO-based microfluidic electrochemical sensors have a good linear relationship for Cd²⁺， Pb²⁺ and Hg²⁺ ions in the concentration range of 0.1—100 μmol/L with the detection limit of 0.055， 0.0025 and 0.0016 μmol/L， respectively（S/N=3）. The microfluidic chips require less sample volume which reduces energy consumption； at the same time， the microfluidic devices made up of polydimethylsiloxane are also expected to realize the function of flexible electrodes， which is important for the integrated and automatic detection of biological and environmental samples using portable and flexible electro- chemical devices.



Organic Chemistry

Synthesis of Dihydro-1，3-benzoxazine Compounds via Catalytic Cycloaddition of ortho-Hydroxyphenyl-substituted para-Quinone Methides and Ketimines

SUN Yidan, LI Xin

2024, 45(2):  20230473.  doi:10.7503/cjcu20230473

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The ［4+2］ cycloaddition reaction between ortho-hydroxyphenyl-substituted para-quinone methides and ketimines was carried out in a phosphoric acid catalytic system. A wide range of dihydro-1，3-benzoxazine derivatives were obtained with good yields and excellent diastereoselectivities. When the catalytic amount of B（C₆F₅）₃ was added to the reaction system， the yield of the product was maintained and the diastereoselectivity was flipped.



Design， Synthesis and Antifungal Activities of Novel Succinate Dehydrogenase Inhibitors Bearing a Pyrazolyl Acetamide Scaffold

WANG Xiaobin, DONG Xue, WANG Ruiying, ZHANG Juan, WANG Mengqi, ZHANG Zongqun, YANG Tingyu, XU Menghan

2024, 45(2):  20230444.  doi:10.7503/cjcu20230444

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Aiming to search for novel fungicide candidates， a series of novel pyrazolyl acetamides potentially targeting fungal succinate dehydrogenase（SDH） were constructed by flexibly reinventing the dualistic amide linkage that emerges in the structure of pyrazole-4-carboxamide fungicides. The diphenylether-containing pyrazole-4- acetamide（6l） featuring broad-spectrum antifungal effects was screened via a mycelium growth rate method. The above molecule exhibited the conspicuous inhibitory effect against Rhizoctonia solani， Fusarium graminearum and Botrytis cinerea at 50 μg/mL， with the inhibitory rates that were slightly better than that of hymexazol. Strikingly， the median effective concentration（EC₅₀） of compound 6l against R. solani was estimated as 19.92 μg/mL that is better than that of hymexazol（76.74 μg/mL） and fluopyram（40.36 μg/mL）. The bioactive evaluations against SDH indicated that a fungal SDH was the potential target of compound 6l for inhibiting R. solani. Subsequently， molecular docking studies implied that the diphenylether unit emerging in the structure of compound 6l could multiply interact with the pivotal residues locating at SDH protein pockets， which plays a critical role in guaranteeing the antifungal effect of diphenylether-containing pyrazole-4-acetamides. The above researches indicated that the diphenylether- containing pyrazole-4-acetamides exhibit obviously inhibitory effects against phytopathogenic fungi， and could be further optimized for developing novel fungicide candidates that could effectively control phytopathogenic fungi.



Physical Chemistry

Preparation of MnO_δ Catalysts and Their Catalytic Performance for Combustion of Diesel Exhaust Soot Particles

ZHOU Shengran, PENG Chao, GAO Siyu, YU Di, ZHANG Chunlei, WANG Lanyi, FAN Xiaoqiang, YU Xuehua, ZHAO Zhen

2024, 45(2):  20230447.  doi:10.7503/cjcu20230447

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Based on the excellent redox performance of manganese oxide（MnO _x ） catalysts， a series of layered MnO _δ catalysts were prepared by hydrothermal method in this paper. The physicochemical properties of as-prepared catalysts were characterized by XRD， Raman， SEM， TEM， N₂ adsorption-desorption， H₂-TPR， O₂-TPD and so on. The effects of hydrothermal reaction temperature， calcination temperature， and raw material composition on the crystal structure， morphology， and redox performance of the catalyst were studied. In addition， the as-prepared catalysts were applied in catalytic combustion of diesel exhaust soot particles. The results showed that the MnO _δ -t₁₂ catalyst exhibits the best catalytic activity when the hydrothermal reaction time was 12 h， the calcination temperature was 550 ℃， and the presence of KOH and K₂CO₃ in the raw materials. The corresponding temperature values of T₁₀， T₅₀ and T₉₀ for soot combustion are 274， 321 and 354 ℃， respectively.



Solvent Effect on the Catalytic Performance of Cinnamaldehyde Hydrogenation over Pt/MIL-100（Fe）

CAI Jiani, LIU Yingya, SUN Zhichao, WANG Yao, WANG Anjie

2024, 45(2):  20230442.  doi:10.7503/cjcu20230442

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This study employs an environmentally-friendly method to synthesize MIL-100（Fe）， and utilizes a double-solvent impregnation approach to confine Pt nanoparticles within the pores of MIL-100（Fe）， subsequent to acidification with HCl and reduction with formaldehyde， a bifunctional catalyst， Pt/MIL-100（Fe）， featuring hydrogenation and Lewis acid centers， is prepared. The catalytic performance is evaluated using the selective hydrogenation of cinnamaldehyde（CAL） as a probe reaction. Under optimal conditions（60 ℃， 1 MPa H₂）， the conversion of CAL reaches 88.3% in 2 h， with a cinnamyl alcohol（COL） selectivity of 84.9%. By comparing the reaction performance of Pt/MIL-100 catalysts with Cr， Al and Fe metal centers， it is revealed that the Fe center favors for the hydrogenation of C=O bonds in both CAL to COL and furfural to furfuryl alcohol. The impact of water content in the reaction system on the selective hydrogenation of CAL is extensively studied. Characterization and static adsorption experiments indicate that removal of free water from the pores of Pt/MIL-100（Fe） facilitates direct enrichment of CAL in the channels， leading to an enhanced conversion. Additionally， removal of coordinated water from the Fe cluster promotes the adsorption of the C=O group of CAL， resulting in an improved selectivity toward COL. After five catalytic cycles under optimal conditions， Pt/MIL-100（Fe） maintains the catalytic performance. Results of powder X-ray diffraction （XRD）， transmission electron microscopy （TEM）， and low-temperature nitrogen adsorption characterization confirm the stability of the catalyst structure after reaction.



Effect of Service Environment of Proton Exchange Membrane Fuel Cell on the Corrosion Behaviors of TA1

JIA Linhan, YANG Daijun, MING Pingwen, MIN Junying, LENG Yu

2024, 45(2):  20230436.  doi:10.7503/cjcu20230436

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In this study， TA1 was selected as the experimental material to investigate the impacts of operating environment（temperatures， pH， gas atmospheres） and operating conditions（potentials and test duration） on its corrosion behavior using the techniques such as potentiodynamic， potentiostatic， electrochemical impedance spectroscopy（EIS）， and working conditions tests. The surface morphology and properties of the TA1 under different durations of working condition test were analyzed by optical microscopy（OM）， energy dispersive X-ray spectroscopy（EDX）， X-ray photoelectron spectroscopy（XPS）， interfacial contact resistance（ICR）， contact angle， and surface roughness measurement techniques. The results show that the operating environment and operating conditions all impact the corrosion resistance of TA1. After working conditions tests of 10 h， the accumulated oxide layer on the surface of TA1 improves its corrosion resistance， decreasing corrosion current density from 2.62 μA/cm² to 0.94 μA/cm². Whereas the conductivity and hydrophobicity of TA1 are significantly reduced， as evidenced by the increase in interfacial contact resistance（ICR） value from 31.75 mΩ·cm² to 333.17 mΩ·cm² compared to commercially available carbon paper and the decrease in contact angle from 86.28° to 68.04°.



Kinetics of Methane Decomposition in the Catalytic Liquid Metal Reactor for Hydrogen Production

LIAO Jiashu, LIU Jianxing, WANG Sishu, CHEN Bo, CHEN Jianjun, WEI Jianjun, YE Zongbiao, GOU Fujun

2024, 45(2):  20230421.  doi:10.7503/cjcu20230421

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Liquid metal catalytic pyrolysis of methane is an emerging technology for the efficient production of hydrogen without CO₂ emissions. In this paper， a numerical model for catalytic methane pyrolysis within a liquid metal cracking reactor was introduced. Experimental data from our in-house liquid metal hydrogen production platform align closely with the model's predictions， which demonstrated a strong correlation between experimental findings and model outcomes. The model was constructed by integrating the catalytic thermal decomposition of methane at the gas-liquid interface， the non-catalytic pyrolysis processes within bubbles， and the fluid dynamics during bubble ascent. This framework harmoniously combines the kinetics of catalytic and non-catalytic reactions with fluid dynamics. Our approach utilizes parameters such as gas volumetric， flow rate， pressure， gas composition temperature and the inherent properties of the liquid metal（density， viscosity， and surface tension） to forecast both bubble dimensions and gas content within the melt. The model accurately predicted the methane conversion under different temperatures， methane flow rates， and liquid metal heights during the catalytic methane pyrolysis experiment using liquid copper-bismuth alloy（Cu_0.45Bi_0.55）. In addition， the gas holdup， superficial gas velocity， and pressure distribution along the height of the liquid metal during the catalytic methane pyrolysis process were obtained. Closely matching experimental data with model predictions provides compelling evidence of the model's robustness and reliability. The proposed model would be useful for reactor optimization and high hydrogen scale-up.



Multi-stage Thermal Decomposition Mechanism of Energetic Plasticizer DNTN Triggered by Cleavage of the Nitrate Ester Bond

CAO Huawen, TANG Qiufan, QU Bei, HUO Huan, ZHENG Qilong, CAO Yilin, LI Jizhen

2024, 45(2):  20230398.  doi:10.7503/cjcu20230398

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2，3-Bis（hydroxymethyl）-2，3-dinitro-1，4-butanediol tetranitrate（DNTN） is energetic material， which is the densest nitrate. The unclear thermal decomposition mechanism of DNTN has seriously hindered its application in propellants. The thermal decomposition process of DNTN was investigated by a combination of reactive force field molecular dynamics（ReaxFF MD） simulation， solid-phase in situ infrared spectroscopy（in situ IR） and TG-DSC- FTIR-MS simultaneous techniques， and the gas and solid products of the thermal decomposition were analysed， the thermal decomposition mechanism was elucidated. The results showed that the decomposition of DNTN was revealed that the process occurred in three stages. During the first stage from 127 ℃ to 147 ℃， the O—N bond in DNTN was partially broken， releasing a minor amount of NO₂ gas. In the second stage， between 147 ℃ and 220 ℃， DNTN underwent rapid decomposition， removing the nitro groups and decomposing the quaternary carbon skeleton， accompanied by the formation and cleavage of the microcyclic structure， releasing a large amount of gases such as NO₂ and CO₂， and at the same time emitting a large amount of heat. The third stage， taking place within the temperature range of 240—350 ℃， involved the high temperature pyrolysis of the remaining solid product of DNTN， which resulted in a limited release of CO₂ gas， and above 300 ℃， the remaining solid phase material would further react to result in the production of cyano. In this paper， the thermal decomposition mechanism of DNTN was illustrated from a multistage perspective， which had important guiding significance for its application in propellants and the follow-up research on stability mechanism.



Study on Reverse Polarization of Proton Exchange Membrane Fuel Cell Stack Caused by Anode Starvation

DONG Wenya, PAN Jianxin, GUO Wei

2024, 45(2):  20230397.  doi:10.7503/cjcu20230397

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At present， the study of proton exchange membrane fuel cell（PEMFC） reversal was mainly completed through a single cell， and the reversal process didn’t consider the influence of adjacent cells， which was not completely the same as the actual situation of the stack. This paper analyzed the anode starvation reverse polarity of PEMFC stack composed of 5 single cells under water flooding and gas shortage conditions by controlling testing conditions such as humidity and excess coefficient. The results show that under anode water flooding conditions， the voltage of the reverse polarity single cell slowly decreases to the electrolysis level table and then quickly recovers. The reason for performance recovery is that the pressure difference between the inlet and outlet of the water flooded single cell anode increases， causing liquid water to be discharged and hydrogen to enter again. Under the condition of gas shortage in the anode of the stack， the voltage of the reverse pole single cell exhibits a cyclic process of rapidly decreasing to the carbon corrosion platform and then rapidly recovering. The reason for the performance recovery is that the decrease in pressure difference between the anode inlet and outlet of the gas deficient single cell causes a new distribution of hydrogen gas in the stack. Due to the lack of gas， the voltage of the reverse polarity battery will decrease to the carbon corrosion platform， which will cause irreversible damage to the battery performance.



Preparation of Non-noble Metal Catalytic Electrode Ni/C@CF and Its Green Fenton Performance

CHENG Shiyu, YANG Ling, BAO Ruiyu, CHEN Chen, CUI Mengmeng, ZHANG Guling, LI Hua

2024, 45(2):  20230382.  doi:10.7503/cjcu20230382

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The traditional Fenton process uses Fe²⁺ to catalyze H₂O₂ to produce strong oxidizing hydroxyl radical（^•OH）， which can efficiently oxidize and degrade organic matter. However， its operating pH range is narrow（pH： ca. 3）， the production of iron flocculation precipitation and other shortcomings limit its application and development. Atomic hydrogen H^*， as a single electron donor， can quickly transfer electrons to H₂O₂ to generate ^•OH， which is suitable for a wide range of pH values and does not produce iron sludge， and is an efficient green Fenton method. However， H^* atoms are more likely to combine with each other to form H₂， which is extremely unstable. Therefore， exploring suitable electrocatalysts plays a crucial role in the application of H^* green Fenton. In this paper， Ni/C@CF electrocatalytic material with high catalytic activity and stable performance was successfully prepared by liquid phase reduction method using carbon black as the carrier. The prepared Ni nanoparticles were uniformly dispersed on carbon black. Using this electrode material as the cathode， a green Fenton catalytic system is constructed， which can catalyze water molecules（H₂O） and hydrogen ions（H₃O⁺） to produce H^*， so that it can catalyze the decomposition of H₂O₂ to produce ^•OH， thus achieving the effect of degrading antibiotic pollutants. By adjusting the preparation method such as voltage， pH value of solution and the additional oxidation dose， the optimal reaction conditions of Ni/C catalyst degradation in this system were determined. In addition， Ni/C@CF composite material has good stability and can be recycled to realize rapid oxidation of green Fenton technology， which has many potential practical applications in wastewater treatment.



Polymer Chemistry

Synthesis and Physiological Properties of Cyclized Poly（ β -amino ester）s

YONG Haiyang, LI Zhili, GUO Rui, ZHOU Dezhong

2024, 45(2):  20230466.  doi:10.7503/cjcu20230466

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The topological structure of polymers has a significant impact on their properties. In this study， we synthesized cyclized poly（β-amino ester）s by adjusting the polymerization parameters and investigated their physiological properties. By utilizing trimethylolpropane triacrylate（TMPTA） and N-（3-Aminopropyl）morpholine（MPA） as monomers and varying their feed ratios and concentrations， two cyclized poly（β-amino ester）s were prepared through Michael addition reaction. The chemical composition， topological structure， and physiological properties of the cyclized poly（β-amino ester）s were characterized by gel permeation chromatography（GPC）， nuclear magnetic resonance spectroscopy（NMR）， and atomic force microscopy（AFM）. The results showed that an increase in cyclization led to enhanced DNA condensation ability， faster degradation profiles， stronger proton buffering capacity， and higher cytotoxicity. These findings provide valuable insights into the preparation and characterization of cyclized poly（β-amino ester）s， shedding light on the design of reliable gene delivery vectors.



Excess Entropy of Janus Particles Immersed in Hydrogen Bonding Fluids

CHEN Qingqing, LI Jiangtao, HUANG Xinrong, GU Fang, WANG Haijun

2024, 45(2):  20230443.  doi:10.7503/cjcu20230443

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Rich aggregation states and phase behavior of Janus particles can be observed in various solvents because of its characterized features， which is closely related to its excess entropy in solution. For the mixture of Janus particles immersed in a hydrogen-bonding（HB） fluid， we presented the excess entropy of a Janus particle in the limit of dilute solution. This investigation was performed by means of the density functional theory for classical fluids. With the aid of local density profiles of HB fluid around the Janus particle under various conditions， the pair correlation functions were given and then were employed to calculate the excess entropy. Furthermore， the effect of interactions between Janus particle and HB fluid， bulk density of HB fluid， HB strength and HB functionality on the excess entropy was elucidated. An attempt was made to find the dependence of the excess entropy on these factors such that the driving force of the assembly of Janus particles can be quantitatively presented. As a result， it is expected that such an effort can provide useful clues to investigate aggregation of Janus particles.



Preparation and Application of CuBDC-NH₂/PmPD Mixed Matrix Membranes for Photothermal Conversion

TANG Haiyan, ZI Limeng, ZHANG Bing, FU Yu

2024, 45(2):  20230379.  doi:10.7503/cjcu20230379

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A kind of metal-organic framework（MOF）-based mixed matrix membranes（MMMs） with excellent photothermal conversion performance was prepared by a simple and efficient soft spray technique in this paper. A small amount of copper ions is uniformly sprayed on the surface of the mixed solution containing 2-aminoterephthalic acid （H₂BDC-NH₂）and m-phenylenediamine（mPD）， and the copper ions simultaneously initiate the self-assembly of MOFs and monomer polymerization to form a large-area CuBDC-NH₂/PmPD MMM with homogeneous MOF at the gas-liquid interface. This method not only is simple and efficient， but also can synthesize mixed matrix membranes with uniform MOF distribution in one step due to the dual action of copper ions. The MMMs obtained by this synchronous synthesis method has good integrity and shows excellent solar water evaporation capacity， which can be used for high-efficiency seawater desalination， and it’s expected to play a role in desalination of seawater.



Preparation of Stereocomplexed PLA Nanofibrous Membranes with High PM_2.5 Filtration Efficiency

SONG Xinyi, TANG Mengke, WANG Cunmin, ZHU Jintuo, HUANG Sheng, XU Huan, HE Xinjian

2024, 45(2):  20230352.  doi:10.7503/cjcu20230352

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Poly（lactic acid）（PLA） nanofibers have potential applications in the field of environmentally friendly filtration materials， but their intrinsic helical molecular chains conformation and low dielectric constant result in poor electret properties， easy decay of filtration performance（e.g.， decreased filtration efficiency， elevated pressure drop）， and short effective service life. The formation of highly electroactive stereocomplex crystals（SCs） was achieved by blending poly（L-lactic acid） （PLLA） and poly（D-lactic acid）（PDLA）， which was promoted by facilitating the polarization of oriented C=O dipoles induced by the high-voltage electrostatic field during electrospinning. The existence of SCs significantly increased the dielectric constant， electret effect and surface potential of the refined PLA nanofibers. The enhanced electroactivity of PLA nanofibrous membranes（NFMs） enabled significant increase of the PM_2.5 filtration efficiency to 96.32%（72.44% for pure PLLA）， while providing desirable pressure drops（85 L/min， 209.2 Pa）. More importantly， the filtration performance of the electroactive PLA NFMs showed weak relation to the airflow velocity（10—85 L/min）， compared to that of the pure PLLA. The excellent stability under increased airflow velocities allows great practical application potential in air filtration field. Moreover， the promotion of the electroactivity of PLA NFMs remarkably enhanced the triboelectricity and electrical signals as stimulated by respiratory vibrations， laying the theoretical foundation for human respiration-based physiological monitoring. This work reveals a new structuring strategy for expanding the application of electroactive PLA in the field of high-performance respiratory protection and intelligent physiological monitoring.