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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

A biomimetic PLLA/MXene piezoelectric hydrogel promotes jawbone regeneration via mitochondrial autophagy-dependent Immunometabolic reprogramming

Shuaishuai Zhang,Chen Du,Xinnan Teng,Hui Wang,Runlong Pan,Junrong Li,Min Zhang,Qian Zhang

To address the issue of lacking tissue specificity in existing piezoelectric materials for bone repair, this study developed for the first time a biomimetic PLLA/MXene piezoelectric conductive hydrogel based on the tissue-specific piezoelectric coefficient of jawbone (∼7.53 pC/N). By incorporating MXene and applying polarization treatment, the piezoelectric performance of the hydrogel was precisely matched to that of natural jawbone, while its electrical conductivity was significantly enhanced. Under ultrasound stimulation, the hydrogel generates localized electrical signals, effectively driving macrophage polarization toward the pro-healing M2 phenotype. This remodeling of the immune microenvironment further synergistically enhances the osteogenic differentiation of bone marrow mesenchymal stem cells and the angiogenic activity of human umbilical vein endothelial cells. Animal experiments confirmed that the hydrogel significantly promotes bone regeneration and collagen mineralization in rat jawbone defect areas. Mechanistically, its immunomodulatory function stems from regulating macrophage polarization by enhancing mitophagy and oxidative phosphorylation. This study provides a novel and tissue-specific intelligent biomaterial strategy for precise jawbone defect repair.

CAS / MDL: 920-66-1
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Journal of Materials Chemistry B · 2026 · IF 6.2

Poly(γ-glutamic acid)-thickened PLLA microspheres with enhanced biocompatibility and efficacy in aged mice

Dan-Qi Ren,Hui-Zhen Peng,Yue Zhang,Yue Yue,Yu Chen,Yun-Li Zhao,Ming-Long Yuan,Xiao-Dong Luo

Poly(L-lactic acid) (PLLA) microspheres are widely used in aesthetic and regenerative medicine to promote collagen remodeling, but their efficacy and long-term safety lack sufficient experimental data. In this study, a poly(γ-glutamic acid)-thickened PLLA microsphere formulation (PLLA–γ-PGA) was developed, and its biocompatibility and efficacy were evaluated in an aged mice model induced by subcutaneous injection of D-galactose combined with UV irradiation. As a result, PLLA–γ-PGA significantly enhanced dermal fibroblast activation, promoted sustained tissue remodeling and elicited milder inflammatory responses without observable adverse effects, outperforming marketed hyaluronic acid (HA) fillers and PLLA–carboxymethyl cellulose sodium (PLLA–CMC) formulations. These findings present PLLA–γ-PGA as a safe and efficacious regenerative material, providing robust preclinical evidence to support its translational potential for long-term skin rejuvenation.

CAS / MDL: 25322-68-3 301-10-0
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INDUSTRIAL CROPS AND PRODUCTS · 2026 · IF 6.4

Epoxy-functionalized cellulose nanocrystals for simultaneous compatibilization and 3D printability enhancement in PLLA/PBAT blends

Xinqi Zhang,Taixiang Zhang,Ying Song,Xia Gao,Hao Wu,Jianming Zhang

A novel reactive compatibilizer was developed by grafting P(VAc-co-GMA) copolymers onto CNCs. • The copolymer-grafted CNCs effectively compatibilized the immiscible PLA/PBAT blends. • The resulting composite exhibited improved melt strength and processability, which directly translated to superior FDM printability. Cellulose nanocrystals (CNCs) hold great potential as nanofiller compatibilizers for immiscible poly( L -lactic acid) (PLLA) and poly(butylene adipate-co-terephthalate) (PBAT) blends. However, a key challenge remains the precise engineering of CNC surface chemistry to achieve strong interfacial interactions and selective localization. In this study, a novel multifunctional compatibilizer was developed based on CNCs grafted with a poly(vinyl acetate-co-glycidyl methacrylate) (P(VAc-co-GMA)) copolymer. The PVAc segments ensure thermodynamic compatibility within the PLLA matrix, while the epoxy groups from GMA offer reactive sites for in-situ interfacial compatibilization. By tuning the comonomer ratio, the surface energy of the grafted CNCs was tailored to match that of PLLA, promoting excellent dispersion during melt processing. The modified CNCs effectively compatibilized the PLLA/PBAT blend, reducing the PBAT domain size from 3.27 µm to 2.00 µm. Moreover, covalent bonds formed between the polymers and CNCs enhanced the melt strength and complex viscosity of blends. Furthermore, the improved processability was directly reflected in the printability. The compatibilized blend exhibited excellent performance in fused deposition modeling (FDM), producing parts with improved dimensional accuracy and interlayer adhesion. Overall, this work offers a facile and effective strategy for designing reactive CNC-based additives that enable simultaneous compatibilization and performance enhancement of PLLA/PBAT blends, facilitating their application in sustainable manufacturing and advanced 3D printing.

CAS / MDL: 106-91-2 108-05-4
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN MEDICINE · 2026 ·Vol. 37 ·期 1 ·32 · IF 4.5

Enhancing bone repair ability of 3D-printed PLLA scaffolds via N-methyl-2-pyrrolidone etching

Yuanzheng Wang,Qilin Jiang,Xin Huang,Shaohong Wu,Jinlong Li,Jian Cao,Zhongxing Liu

The development of bone repair scaffolds has long been a research hotspot in tissue engineering. Owing to its unique capability for personalized customization of scaffold geometry and microstructure, 3D printing technology has been extensively adopted for fabricating bone repair scaffolds. Poly-L-lactic acid (PLLA), endowed with favorable biodegradability, excellent biocompatibility, and reliable in vivo safety, is widely used as a matrix material for 3D printed bone repair scaffolds. PLLA is a bioinert polymer characterized by inferior cell adhesion and osteogenic differentiation capabilities. To mitigate this bioinertness limitation, the present study employed N-methylpyrrolidone (NMP) etching to modify the surface of 3D-printed PLLA bone repair scaffolds. Following NMP etching for 1–24 h, the originally smooth scaffold surface evolved into a hierarchical, petal-like gradient microstructure, accompanied by a marked increase in surface roughness. Correspondingly, the hydrophilicity of the treated scaffolds was also enhanced. Differential scanning calorimetry (DSC) and X-ray diffraction (XRD) analyses further confirmed that the crystallinity of PLLA in the scaffolds was significantly enhanced. Concomitantly, the modified scaffolds exhibited a marked improvement in adsorption capacity for green fluorescent protein (GFP), while the adhesion and proliferation of MC3T3-E1 on their surface were also significantly promoted. In vivo animal experiments demonstrated that the NMP-etched scaffolds could accelerate the process of bone defect repair. Collectively, surface modification of 3D-printed PLLA bone scaffolds via NMP etching enables precise modulation of their physicochemical properties, thereby effectively mitigating the inherent bioinertness limitation of PLLA scaffolds. Graphical

CAS / MDL: 872-50-4
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2026 · IF 5.4

Co-loaded CNT having adjustable Co2+/Co3+ ratio endows PLLA bone scaffold with ROS-scavenging

Feng Yang,Mengling Jiang,Linfeng Fan,Hao Pan,Pei Feng

Co-loaded CNT with high Co 2+ content of 61.07% exhibited enhanced nanozyme activity. • P2 possessed a safe Co-ion release content far below the threshold of 20 ppm. • P2 exhibited good well-rounded properties and excellent anti-inflammatory activity. Excessive reactive oxygen specie (ROS) is not conducive to bone repair, which is prone to generate during the initial hematoma inflammatory phase following poly( L -lactic acid) (PLLA) bone scaffold implantation and the potential inflammation caused by its acidic degradation products. This study proposed introducing cobalt (Co)-based nanozyme into the PLLA scaffold, and focused on improving the dispersion between nanozyme and the PLLA matrix as well as enhancing the activity of nanozyme itself for efficiently scavenging ROS. The Co was loaded on the surface of carbon nanotube (CNT) for achieving uniform dispersion, and then calcined under different atmospheres for enhancing nanozyme activity via regulating the Co 2+ /Co 3+ ratio and optimizing the electronic structure. It was found that the nanozyme that was calcined in an N 2 atmosphere followed by phosphorylation exhibited a superior ROS-scavenging ability, which was attributed to its high Co 2+ content of 61.07% that facilitating the redox cycling and the optimization of its electronic structure by P doping. As a result, the composite scaffold (P2) at a nanozyme loading of 2 wt% possessed superior intracellular ROS-scavenging ability and downregulation of key inflammatory cytokines compared to the pure PLLA scaffold. It also possessed good cytocompatibility for cell adhesion and proliferation, and exhibited upregulated expression of the pro-angiogenic VEGF factor. Download: Download high-res image (228KB) Download: Download full-size image Co-based nanozyme was engineered by promoting dispersion and optimizing the Co 2+ /Co 3+ ratio for highly efficient SOD and CAT, and was used to endow the PLLA bone scaffold with good ROS-scavenging and cytocompatibility.

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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2019 ·Vol. 220 ·期 5 ·1800528 · IF 2.622

PLLA-Grafted Gelatin Amphiphilic Copolymer and Its Self-Assembled Nano Carrier for Anticancer Drug Delivery

Du Beibei,Fan Tiantang,Li Jiafeng,Gong Li,Zhang Qin,Ye Wuyou,Tai Hongyun,Wang Wenxin,Fan Zhongyong

A series of poly( l -lactide)-grafted gelatin (Gel-g-PLLA) copolymers are synthesized by coupling the amino groups of gelatin with different molar masses and the carboxyl endgroup of poly( l -lactide) in the presence of 1-ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride and N -hydroxysuccinimide. Fourier transform infrared and nuclear magnetic resonance ( 1 H NMR) data confirm the successful bonding between gelatin and PLLA. Self-assembled micelles of copolymers are prepared by using the direct dissolution method. The size and micellar morphology are determined from dynamic light scattering as well as transmission electron microscopy measurements. Meanwhile, in vitro drug release reveals that Gel-g-PLLA micelles show excellent sustained-release properties when used as the carrier of the anticancer drug paclitaxel. A burst release of about 70% is observed in the first 24 h. All these features, together with the outstanding biocompatibility, make Gel-g-PLLA micelles a promising drug carrier for cancer therapy.

研究领域: 高分子化学 · 纳米技术 · 药学 · 生物医学工程 · 肿瘤学
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Polymer Crystallization · 2018 ·Vol. 1 ·期 1 ·e10006 · IF 0

The crystallization and phase transition behaviors of asymmetric PLLA/PDLA blends: From the amorphous state

Liying Wang,Congshu Feng,Dongdong Zhou,Jun Shao,Haoqing Hou,Gao Li

The phase transition behaviors of melt-quenched asymmetric poly( l -lactide acid)/poly( d -lactide acid) (PLLA/PDLA) blends are investigated by the in-situ wide angle X-ray diffraction. Results indicate that the crystal structures and their transition of PLLA/PDLA specimens depend on the composition, molecular weight, and temperature. In the specimens with lower molecular weights (∼9 kg/mol), the poly(lactic acid) homocrystallites (HC), mesophase, and stereocomplex crystallites (SC) develop in specific blends. As the content of PDLA increases, the formation temperature of HC increases to a fixed value, while that temperature for SC reduces to a constant value, and the formation temperature of mesophase does not vary with composition. For the specimens with moderate molecular weights (∼30 kg/mol), the HC, modified HC, and SC develop in specific composition, the formation temperatures of both the HC are constant, and the formation of SC reduces to a fixed temperature. In the blends with molecular weight of ∼65 kg/mol, HC and SC develop, and the formation of HC does not vary, but that temperature for SC reduces slightly as more PDLA incorporated. After melting of HC, another enhancement of SC is observed in all the PLLA/PDLA specimens. The unique crystallization phenomena for these PLLA/PDLA specimens are analyzed.

CAS / MDL: 111-77-3 301-10-0
研究领域: 材料科学 · 高分子化学
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Polymers · 2020 ·Vol. 12 ·期 11 ·2482 · IF 3.426

Novel Temperature/Reduction Dual-Stimulus Responsive Triblock Copolymer [P(MEO2MA-co- OEGMA)-b-PLLA-SS-PLLA-b-P(MEO2MA-co-OEGMA)] via a Combination of ROP and ATRP: Synthesis, Characterization and Application of Self-Assembled Micelles

Fei Song,Zhidan Wang,Wenli Gao,Yu Fu,Qingrong Wu,Shouxin Liu

Novel temperature/reduction dual stimulus-responsive triblock copolymers, poly [2-(2-methoxyethoxy) ethyl methacrylate-co-oligo (ethylene glycol) methacrylate]-b-(L-polylactic acid)-SS-b-(L-polylactic acid)-b-poly[2-(2-methoxyethoxy) ethyl methacrylate-co-oligo(ethylene glycol)methacrylate] [P(MEO2MA-co-OEGMA)-b-PLLA-SS-PLLA-b-P(MEO2MA-co-OEGMA)] (SPMO), were synthesized by ring opening polymerization (ROP) of L-lactide and 2,2’-dithio diethanol (SS-DOH), and random copolymerization of MEO2MA and OEGMA monomers via atom transfer radical polymerization (ATRP) technology. The chemical structures and compositions of the novel copolymers were demonstrated by proton nuclear magnetic resonance (1H NMR) and Fourier transform infrared spectroscopy (FTIR). The molecular weights of the novel copolymers were measured by size exclusive chromatography (SEC) and proved to have a relatively narrow molecular weight distribution coefficient (ÐM ≤ 1.50). The water solubility and transmittance of the novel copolymers were tested via visual observation and UV–Vis spectroscopy, which proved the SPMO had a good hydrophilicity and suitable low critical solution temperature (LCST). The critical micelle concentration (CMC) of the novel polymeric micelles were determined using surface tension method and fluorescent probe technology. The particle size and morphology of the novel polymeric micelles were characterized by dynamic light scattering (DLS) and transmission electron microscopy (TEM). The sol–gel transition behavior of the novel copolymers was studied via vial flip experiments. Finally, the hydrophobic anticancer drug doxorubicin (DOX) was used to study the in vitro release behavior of the novel drug-loaded micelles. The results show that the novel polymeric micelles are expected to become a favorable drug carrier. In addition, they exhibit reductive responsiveness to the small molecule reducing agent dithiothreitol (DTT) and temperature responsiveness with temperature changes.Keywords:temperature/reductive dual-stimulus responsiveness;block copolymers;amphiphilic;ring-opening polymerization;atom transfer radical polymerization

CAS / MDL: 26915-72-0 4511-42-6
研究领域: 高分子化学 · 药物递送系统 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Gambogic acid augments black phosphorus quantum dots (BPQDs)-based synergistic chemo-photothermal therapy through downregulating heat shock protein expression

Biao-Qi Chen,Ranjith Kumar Kankala,Yang Zhang,Shu-Ting Xiang,Han-Xiao Tang,Qi Wang,Da-Yun Yang,Shi-Bin Wang,Yu Shrike Zhang,Gang Liu,Ai-Zheng Chen

In an attempt to attain synergistic therapeutic benefits and address various intrinsic limitations of the highly efficient black phosphorus quantum dots (BPQDs), we fabricated poly( L -lactide)-poly(ethylene glycol)-poly( L -lactide) triblock copolymer (PLLA-PEG-PLLA)-based nanocomposites co-loaded with BPQDs and gambogic acid (GA) using the supercritical carbon dioxide (SC-CO 2 ) technology to achieve photoacoustic (PA) imaging-guided synergistic chemo-photothermal therapy. On the one hand, BPQDs displayed near-infrared (NIR)-induced hyperthermia through the high photothermal conversion efficiency. On the other hand, the NIR-responsive release of GA facilitated early apoptosis through specific binding to stress-induced overexpression of heat shock protein (HSP)-90 for combating thermoresistant tumor cells. GA significantly promoted the photothermal therapy (PTT) efficiency by enhancing both early and late apoptosis of BPQDs. Moreover, the encapsulation of BPQDs in the polymer significantly improved their chemical as well as photothermal stabilities. Our findings suggested that these nanocomposites fabricated using the eco-friendly supercritical fluid (SCF) technology provided good protection to the biodegradable BPQDs, offering a great potential towards cancer ablation through augmented synergistic effects.

研究领域: 癌症治疗 · 纳米技术 · 生物医学工程 · 材料科学 · 药学
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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

An ultrasound-activated PLLA@BaTiO3&SF Janus membrane enhances fracture healing via synergistic piezoelectricity and bioactivity

Qinghua Guo,Jiahao Cao,Zixian Yang,Wei Cao,Hongli Chen,Yidi Duan,Xu Wang,Zhen Gong,Xiaolin Liu,Shanshan Fu,Yibin Huang,Yafei Feng,Jing Wang,Weijia Wang,Wei Lei

Ultrasound-activated PLLA@BaTiO 3 &SF Janus membrane for non-invasive fracture therapy • Optimal piezoelectricity achieved by 20 wt% BaTiO 3 doping in PLLA • Hydrophilic and ROS-scavenging SF interface favoring BMSCs adhesion • Enhanced fracture healing via ITGB1-dependent signaling activation Fracture nonunion remains a significant clinical problem, largely due to insufficient mechanistic insight and effective treatments. Piezoelectric materials including polylactic acid (PLA) and barium titanate (BaTiO 3 ), facilitate bone regeneration through electrical stimulation, but their clinical application is constrained by undefined optimal ratio for achieving maximum electrical energy output and concerns regarding biological toxicity. To overcome these drawbacks, we designed a Janus membrane inspired by asymmetric material architecture, featuring a piezoelectric outer layer of poly (L-lactic acid) (PLLA) doped with BaTiO 3 and an inner silk fibroin (SF) layer. Our findings indicate that PLLA containing 20 wt% BaTiO 3 yields optimal electrical output under ultrasound stimulation, while the SF layer provided a hydrophilic and antioxidant interface for bone marrow-derived mesenchymal stem cells (BMSCs). The results showed that PLLA@BaTiO 3 &SF Janus membrane significantly enhanced BMSCs adhesion, proliferation, and osteogenic differentiation, thereby accelerating fracture repair in a mouse femoral fracture model. Mechanistically, ultrasound-activated piezoelectric stimulation triggered PI3K-Akt, MAPK, and TGF-β signaling pathways in an integrin β1 (ITGB1)-dependent manner. Overall, the PLLA@BaTiO 3 &SF Janus membrane integrates noninvasive activation, tunable piezoelectricity and excellent biocompatibility to achieve robust bone regeneration, offering a promising therapeutic strategy for reducing fracture nonunion and improving the quality of life for patients. Design and biomedical applications of a Janus membrane consisting of a piezoelectric PLLA-BaTiO3 outer layer and an SF-based inner layer. This design ultimately effectively enhances the pro-repair behaviors of bone marrow stromal cells (BMSCs) and accelerates bone regeneration. Download: Download high-res image (277KB) Download: Download full-size image

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CARBOHYDRATE POLYMERS · 2012 · IF 3.628

One-pot synthesis of chitosan-g-(PEO-PLLA-PEO) via “click” chemistry and “SET-NRC” reaction

Ke Zhang,Pengyu Zhuang,Zhengke Wang,Youliang Li,Zhiqiang Jiang,Qiaoling Hu,Minying Liu,Qingxiang Zhao

For the development of biocompatible and degradable biomaterials, a kind of well-defined graft copolymer consisting of chitosan back-bone and amphiphilic PEO-PLLA-PEO branch chains was synthesized by Cu(0) catalyzed one-pot strategy combining “click” chemistry and single electron transfer-nitroxide radical coupling (SET-NRC) reaction. First, the precursors of 6-azide- N -phthaloyl-chitosan, TEMPO-PEO-alkyne and mPEO-PLLA-Br were designed and produced. Then, the one-pot coupling reactions between these precursors were performed in the presence of nanosized Cu and PMDETA. The efficiencies of the coupling reactions were greater than 90% determined by the FTIR and ESR spectra. The structure of graft copolymer with 43% of the grafting ratio was confirmed by the spectral analysis. This work provided a route to prepare chitosan graft copolymer.

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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Efficient continuous waste PLLA degradation via stearyl alcohol-mediated transesterification catalyzed by tin(II) octadecyl alkoxide

Yankai Zhang,Chenxi Zhu,Haoyi Wang,Yunbiao Qi,Ping Sun,Quanxing Zhang,Wei Jiang

The chemical recycling of waste poly(L-lactic acid) (PLLA) into its monomer, L-lactide, offers a promising strategy for establishing a circular economy for PLLA-based polymers. However, conventional approaches typically require high reaction temperatures and suffer from significant side reactions, thereby hindering the efficient recycling of waste PLLA. In this study, we present a low-temperature, continuous depolymerization process for waste PLLA, catalyzed by stearyl alcohol (StOH) and stannous octanoate (Sn(Oct) 2 ) at a mild temperature of 165 °C. This system achieves an L-lactide yield of 99.31 % and purity of 98.02 % (ee = 99.73 %). Characterization of the reaction mechanism, supported by density functional theory (DFT) calculations, reveals that StOH displaces the octanoate ligands in Sn(Oct)₂ to form tin(II) octadecyl alkoxide. This nucleophilic species interacts with the carbonyl groups of PLLA, promoting chain scission via ligand-assisted attack. The mechanism reduces the energy barrier for backbiting reactions, thereby enhancing the rate of L-lactide formation. This method exhibits strong practical viability, achieving a 97 % yield from real-world PLLA waste and selectively degrading PLLA in mixed plastic streams to enable efficient separation. Furthermore, a simplified continuous processing system was developed, demonstrating stable and sustained PLLA degradation. This work provides an innovative and scalable strategy for sustainable PLLA chemical recycling under mild conditions.

CAS / MDL: 661-19-8 57-11-4
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