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Preparation of Chemically Recyclable Poly(ether-alt-ester) by the Ring Opening polymerization of Cyclic Monomers Synthesized by Coupling Glycolide and Epoxides

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Chinese Journal of polymer Science 2024年第2期42卷 168-175,I0006页

作者： Feng Ren Zhuang-Zhuang Liang Ming-Xin Niu Chen-Yang Hu Xuan Pang Key Laboratory of polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China School of Applied Chemistry and engineering University of Science and Technology of ChinaHefei230026China

Polyester and polyether are two key oxygenated polymers, and completely alternative sequence of poly(ester-alt-ether) could efficiently combine the advantages(including flexibility, degradability, etc.) of both segments. Currently, despite their copolymers could be synthesized from one-pot mixture of cyclic esters and epoxides, perfectly alternative microstructure is very challenging to realize and typically restricted to certain monomer pairs. Moving forward, synthesizing poly(ester-alt-ether) from commercially available and largescale monomers would be a significant advance. For example, successfully commercialized poly(glycolic acid)(PGA), which is not easily soluble in polymers due to its high crystallinity and is brittle and difficult to control the degradation cycle, would encounter a new paradigm if engineered into poly(ester-altether). In this work, starting from the design of monomer with hybrid structures, we successfully synthesized a series of 1,4-dioxan-2-one containing different substituents based on glycolide(GA) and epoxides using commercially available Salen-Cr(III) and PPNCl catalytic *** new monomers underwent ring-opening polymerization(ROP) to form a series of poly(ester-alt-ether) with perfectly alternating glycolic acid and propylene glycol repeat units under catalytic system of thiourea/base. The poly(ester-alt-ether) have significantly lower glass-transition temperature than PGA. Additionally, the poly(ester-alt-ether) can be chemically recovered to monomer using Sn(Oct)2 or 1,8-diazabicyclo[5.4.0]undecane-7-ene(DBU) as a catalyst in solution, thus establishing a closed-loop life cycle. From monomers derived from GA and epoxides, this work furnishes a novel strategy for the synthesis of poly(ester-alt-ether) with chemical recyclability.

关键词： Polyester Polyether Alternative copolymer Ring-opening polymerization

Chain Dynamics Heterogeneity in Plasticized Poly(vinyl butyral)(PVB) as Elucidated by Solid-State NMR

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Chinese Journal of polymer Science 2024年第1期42卷 113-124,I0010页

作者： Jing Lv Xu Chen Zi-Shuo Wu Ya-Hui Li Wei Chen National Synchrotron Radiation Laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer FilmCAS Key Laboratory of Soft Matter ChemistryUniversity of Scienceand Technology of ChinaHefei 230026China

The chain dynamics heterogeneity of the poly(vinyl butyral)(PVB) plasticized by triethylene glycol bis(2-ethylhexa noate)(TEG-EH) was investigated by various solid-state NMR *** plasticized PVB shows two domains in distinct molecular dynamics differences,namely,rigid and soft domains,where the latter is the plasticizer-rich *** time domain low field NMR was first used to investigate the dynamics heterogeneity of the plasticized PVB,and the results show the decreasing activated energy of components in the soft domain of plasticized PVB(E_a=20.2 kJ/mol) as compared with that of the pristine one(E_a=24.3 kJ/mol).Detailed dynamics heterogeneity was obtained by high-field NMR with site-specific *** quadrupole-echo ~2H-NMR was adopted to elucidate the dynamics heterogeneity of the vinyl alcohol(VA) units,where only the hydroxyl group of VA is *** ~1H-^(13)C WISE NMR spectra show that there is not much difference in the mobility of the VB unit in PVB with and without plasticizer,whereas the glass transition temperature differed by approximately 53℃.This is further supported by Torchia's T_1 relaxation *** origin of such an unusual phenomenon is attributed to the critical role of the remaining VA(~22%) in the soft domain,where the VA units locally aggregate through hydrogen ***,the existence of a mobility gradient in the VB unit has been ***,the mobility difference for VB with different stereo-geometry(meso or racemic conformation) is observed for the first *** indicates the importance of modulating the ratio of meso over racemic VB for controlling the macroscopic perfo rmance of PVB.

关键词： Poly(vinyl butyral) Dynamics heterogeneity Plasticizer Solid state NMR

Light-responsive Self-Immolative L-glutamic Acid-based Polyester Nanoparticles for Controlled Drug Release via Passerini Three-Component polymerization

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Chinese Journal of polymer Science 2024年第5期42卷 570-578,I0005页

作者： Xiao-Fei Sun Xu Zhang Shu-Ping Song Ya-Qun Yao Yan Zhang Cheng-Liang Wang Jing-Jiang Sun Qing-Fu Wang Key Laboratory of Rubber-plastics Ministry of EducationSchool of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao266042China Qingdao Research Academy of Environmental Science Qingdao266012China

L-glutamic acid(LA)is a bio-based,non-toxic,environmentally friendly material derived from *** present study reports the application of Passerini three-component polymerization(P-3CP)for the straightforward preparation of LA-based light-responsive polyesters(PLTDs)under mild *** with molar masses up to 8500 g/mol and high yields exceeding 90%are *** chemical structures and light-responsive self-immolative behavior of PLTDs are comprehensively characterized by employing ultraviolet-visible(UV-Vis)spectroscopy,size exclusion chromatography(SEC),nuclear magnetic resonance(NMR)spectroscopy,and liquid chromatography mass spectrometry(LC-MS).Meanwhile,monodisperse PLTD-based doxorubicin-loaded nanoparticles(PLTD-DOX-NP)(size=193 nm,PDI=0.018)are formulated by nanoprecipitation *** light-induced depolymerization,the PLTD-DOX-NP undergoes rapid decomposition,resulting in a burst release of 80%cargo within 13 ***,according to biological toxicity tests,the PLTD-NP possesses adequate biosafety,both before and after ***,the incorporation of P-3CP with biorenewable LA-based monomer adheres to the principles of green chemistry,significantly simplifying the synthetic pathway of light-responsive polymers.

关键词： L-glutamic acid Passerini three-component polymerization Light-responsive Polyester Nanoparticles

Bilayer Compounded Polytetrafluoroethylene Membrane for Enhanced Oil-Water Emulsion Separation

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Chinese Journal of polymer Science 2024年第6期42卷 838-850页

作者： Yu-Liang Yang Tai-Ran Zhang Yan-Ting Han Shao-Yun Guo Qin-Gong Rong Jia-Bin Shen State Key Laboratory of polymer Materials engineering Polymer Research Institute of Sichuan UniversitySichuan Provincial Engineering Laboratory of Plastic/Rubber Complex Processing TechnologyChengdu610065China West China Hospital/West China School of Nursing Sichuan UniversityChengdu610041China Shandong Senrong New Materials Co. Ltd.Zibo256401China

In order to achieve efficient and durable oil-water emulsion separation,the membranes possessing high separation efficiency and mechanical strength attract extensive attention and are in great *** present study,a kind of polytetrafluoroethylene(PTFE)-based bilayer membrane was fabricated by electrospinning fibrous PTFE(fPTFE)on an expanded PTFE(ePTFE)*** morphological observation revealed that the fibrous structure of the fPTFE layer could be tailored by controlling the formulation of spinning *** addition of appropriate polyoxyethylene(PEO)would make the fibers in the fPTFE layer finer and more *** a result,the compounded membrane exhibited a small pore size of approximately 1.25µm and a substantial porosity nearing 80%.This led to super-hydrophobicity,characterized by a high water contact angle(WCA)of 149.8°,and facilitated rapid oil *** water-in-oil emulsion separation experiment further confirmed that the compounded membrane not only had a high separation efficiency closing 100%,but such an outstanding separation capacity could be largely retained,either through multiple cycles of use or through strong acid(pH=1),strong alkali(pH=12),or high-temperature(100°C)***,the mechanical behavior of the bilayer membrane was basically contributed by that of each layer in terms of their volume *** significantly,the poor creep resistance of fPTFE layer was suppressed by compounding with ePTFE ***,this study has laid the groundwork for a novel approach to create PTFE-based compounded membranes with exceptional overall characteristics,showing promise for applications in the realm of emulsion separation.

关键词： ePTFE Electrospinning membrane Bilayer compounding Emulsion separation

A robust viscoelastic surfactant tolerating 20% HCl up to 150℃ for oil well stimulation

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Petroleum Science 2024年第3期21卷 1865-1874页

作者： Ji Wang Ning Qi Hong-Yao Yin Yu-Jun Feng polymer Research Institute State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065SichuanPR.China Tianfu Yongxing Laboratory New Theory and Technology of CO_(2) Capture Research CenterChengdu610065SichuanPR China School of Petroleum engineering China University of Petroleum(East China)Qingdao266580ShandongPR China

Viscoelastic surfactants(VES)are often used as viscous diverters in acidizing stimulation to prolong the acid consumption time and maximize zonal coverage of the acid for improving well ***,the ceiling temperature of commercial VES cannot exceed 120℃in practical use because of the poor thermal stability and fragile molecular structure,hindering their implementation in hightemperature oil reservoirs,i.e.,≥150℃.Here we synthesized a novel C22-tailed diamine,N-erucaminopropyl-N,N-dimethylamine(EDPA),and examined comparatively its rheological behavior,assemblies morphology and molecular stability in 20 wt%HCl with a commercial VES,erucyl dimethyl amidopropyl betaine(EDAB).The feasibility of EDPA for acidizing stimulation was assessed by acid etching of carbonate rock with its HCl solution at 150℃.Rheological results showed that the 2.5 wt%EDPA—20 wt%HCl solution maintains stable viscosity of 90 m Pa s at 150℃for 60 min,while that of 2.0 wt%EDAB HCl solution is just 1 m Pa s under identical conditions.1H NMR spectra and cryo-TEM observations revealed that the chemical structure and self-assembled architectures of EDPA remained intact in such context,but the EDAB suffered from degradation due to the hydrolysis of the amide group,accounting for the poor heat-resistance and *** reaction rate of 2.5 wt%EDPA HCl solution with carbonate rock was one order of magnitude lower than that of 20 wt%HCl solution at 150℃,underpinning the potential of EDPA to be used in the high-temperature reservoirs *** work improved the thermal tolerance of VES in highly concentrated HCl solution,paving a feasible way for the acidization of high-temperature reservoir environments(~150℃).

关键词： Viscoelastic surfactants Thermal stability Self-diverting acid Wormlike micelles Acidizing stimulation

Lightweight,Strong and High Heat-Resistant Poly(lactide acid)Foams via Microcellular Injection Molding with Self-Assembly Nucleating Agent

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Chinese Journal of polymer Science 2024年第6期42卷 739-750页

作者： Xiao-Hu Bing Wen-Yu Ma Ming-Hui Wu Peng Gao Xiao Zhou Hai-Bin Luo Long Wang Wen-Ge Zheng School of materials Science and engineering Shanghai UniversityShanghai200444China Ningbo Key Lab of polymer Materials Ningbo Institute of Material Technology and EngineeringChinese Academy of SciencesNingbo315201China University of Chinese Academy of Sciences Beijing100049China

Poly(lactide acid)(PLA)foams have shown considerable promise as eco-friendly alternatives to nondegradable plastic foams,such as polystyrene(PS)***,PLA foam typically suffers from low heat-resistance and poor cellular structure stemming from its inherent slow crystallization rate and low melt *** this study,a high-performance PLA foam with well-defined cell morphology,exceptional strength and enhanced heat-resistance was successfully fabricated via a core-back microcellular injection molding(MIM)*** scanning calorimetry(DSC)results revealed that the added hydrazine-based nucleating agent(HNA)significantly increased the crystallization temperature and accelerated the crystallization process of ***,the addition of a 1.5 wt%of HNA led to a significant reduction in PLA’s cell size,from 43.5µm to 2.87µm,and a remarkable increase in cell density,from 1.08×10^(7)cells/cm^(3)to 2.15×10^(10)cells/cm^(3).This enhancement resulted in a final crystallinity of approximately 55.7%for the PLA blend foam,a marked improvement compared to the pure PLA ***,at 1.5 wt%HNA concentration,the tensile strength and tensile toughness of PLA blend foams demonstrated remarkable improvements of 136%and 463%,***,the Vicat softening temperature of PLA blend foam increased significantly to 134.8°C,whereas the pure PLA foam exhibited only about 59.7℃.These findings underscore the potential for the preparation of lightweight injection-molded PLA foam with enhanced toughness and heat-resistance,which offers a viable approach for the production of high-performance PLA foams suitable for large-scale applications.

关键词： Poly(lactide acid) Nucleating agent Microcellular injection molding Heat-resistance Toughness

Study on frictional behavior of SiC_(f)/SiC composite clad tube clamping condition under nuclear irradiation

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Friction 2024年第5期12卷 919-938页

作者： Chenglong XIAO Liangliang SHEN Tianqi ZHU Jianbo TANG Ximing XIE Xinyu FAN Jian XU Zhiying REN School of Mechanical engineering Zhejiang University of TechnologyHangzhou310023China engineering Laboratory of Advanced Energy Materials Ningbo Institute of Material Technology and EngineeringChinese Academy of SciencesNingbo315201China State Key Laboratory of Fine Chemicals Liaoning High-Performance Polymer Engineering Research CenterSchool of Chemical EngineeringDalian University of TechnologyDalian116024China School of Mechanical engineering and Automation Fuzhou UniversityFuzhou350116China School of Computer Science and technology Shandong UniversityQingdao266237China Aviation Industry Corporation of China Ltd.Beijing100028China

Silicon carbide fiber reinforced silicon carbide matrix(SiC_(f)/SiC)composite is the key cladding material of nuclear fuel,which determines the safety and reliability of nuclear fuel storage and *** replacement of its storage and transportation scenario needs to be completed by the manipulator,but the application of SiC_(f)/SiC wear,fracture,and nuclear leakage in the snatching process of brittle-flexible-rigid contact in the irradiation environment has been seriously restricted due to unclear understanding of the damage ***,the effects of irradiation dose and clamping load on the friction characteristics of the contact interface between SiC_(f)/SiC clad tube are studied in this paper,and the effects of irradiation parameters and clamping force on the static friction coefficient of the contact interface between the clad tube and flexible nitrile are *** on the Greenwood-Williamson tribological model,a numerical model of the shape and structure of the contact micro-convex at the micro-scale of the clamping interface is constructed by introducing the multi-surface integral,and finally verified by *** research results show that there is a unique“Irradiation suppression zone”under the clamping condition of SiC_(f)/SiC cladding tube under the nuclear irradiation environment,and the growth of static friction coefficient slows down until stagnates after irradiation reaches a certain extent(600 kGy),and there will be a decline when the irradiation dose continues to increase,among which the clamping force of 15.2 N within the irradiation interval of 1,000 kGy can meet the safety of nuclear environment *** results of this paper can provide an important theoretical basis and application guidance for the safe operation of SiC_(f)/SiC cladding tubes in the storage and transportation clamping process.

关键词： SiC_(f)/SiC Clad tube nuclear irradiation conditions Greenwood-Williamson tribological model multi-surface integral

An advanced 2D/3D g-C_(3)N_(4)/TiO_(2)@MnO_(2) multifunctional membrane for sunlight-driven sustainable water purification

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Nano Research 2024年第4期17卷 2368-2380页

作者： Fan Yu Chunjia Luo Xiaohan Niu Min Chao Pengfei Zhang Luke Yan polymer Materials&engineering Department School of Materials Science&EngineeringChang’an UniversityXi’an 710064China Key Laboratory of Road Construction technology and Equipment MOEChang’an UniversityXi’an 710064China School of Textile Science and engineering Xi’an Polytechnic UniversityXi’an 710064China

Graphitic carbon nitride(g-C_(3)N_(4))nanosheets have attracted widespread interest in the construction of advanced separation ***,dense stacking and a single functionality have limited the membrane ***,an advanced two-/three-dimensional(2D/3D)g-C_(3)N_(4)/TiO_(2)@MnO_(2) membrane is constructed by intercalating 3D TiO_(2)@MnO_(2) nanostructures into g-C_(3)N_(4) *** 3D flower-like nanostructures broaden the transport channels of the composite *** membrane can effectively separate five oil-in-water(O/W)emulsions,with a maximum flux of 3265.67±15.01 L·m^(-2)·h^(-1)·bar^(-1) and a maximum efficiency of 99.69%±0.45%for toluene-in-water emulsion(T/W).Meanwhile,the TiO_(2)@MnO_(2) acts as an excellent electron acceptor and provides positive spatial separation of electrons–holes(e^(-)–h^(+)).The formation of 2D/3D heterojunctions allows the material with wider light absorption and smaller bandgap(2.10 eV).These photoelectric properties give the membrane good degradation of three different pollutants,with about 100%degradation for methylene blue(MB)and malachite green(MG).The photocatalytic antibacterial efficiency of the membrane is also about 100%.After cyclic experiment,the membrane maintains its original separation and photocatalytic *** remarkable multifunctional and self-cleaning properties of the g-C_(3)N_(4) based membrane represent its potential value for complex wastewater treatment.

关键词： graphitic carbon nitride(g-C_(3)N_(4))based membrane three-dimensional(3D)nanostructures self-cleaning multifunction

Vacancy healing for stable perovskite solar cells via bifunctional potassium tartrate

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Journal of Energy Chemistry 2024年第1期88卷 64-70,I0002页

作者： Jing Dou Yue Ma Xiuxiu Niu Wentao Zhou Xueyuan Wei Jie Dou Zhenhua Cui Qizhen Song Tinglu Song Huanping Zhou Cheng Zhu Yang Bai Qi Chen Experimental Centre for Advanced Materials School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Key Laboratory for Theory and technology of Advanced Battery Materials Key Laboratory of Polymer Chemistry and Physics of Ministry of EducationBIC-ESATSchool of Materials Science and EngineeringPeking UniversityBeijing 100871China

Perovskite solar cell has gained widespread attention as a promising technology for renewable ***, their commercial viability has been hampered by their long-term stability and potential Pb leakage. Herein, we demonstrate a bifunctional passivator of the potassium tartrate(PT) to address both challenges. PT minimizes the Pb leakage in perovskites and also heals cationic vacancy defects, resulting in improved device performance and stability. Benefiting from PT modification, the power conversion efficiency(PCE) is improved to 23.26% and the Pb leakage in unencapsulated films is significantly reduced to 9.79 ppm. Furthermore, the corresponding device exhibits no significant decay in PCE after tracking at the maximum power point(MPP) for 2000 h under illumination(LED source, 100 mW cm^(-2)).

关键词： Perovskite Potassium tartrate Lead leakage Long-term stability