Performance Evaluation of Thermal Insulation Materials from Sheep's Wool and Hemp Fibres.

In the current work, the performance properties of natural-fibre-based thermal insulation materials were examined. For this purpose, three different compositions of natural fibres were prepared: pure sheep wool (SW), wool and industrial hemp (SW/HF) fibres, and pure industrial hemp (HF) fibres. Low-melt bicomponent polylactide (PLA) fibres were used as a binding material. For specimens prepared from natural fibres, the dependence of the thermal conductivity, the tensile strength along and across the direction of product formation, and the short-term water absorption on the density of the specimens and the flammability parameters were determined. In addition, to reduce the water absorption and flammability, the specimens were coated with hydrophobic agents and flame retardants. The obtained research results were also statistically processed. The analysis of the results showed that the thermal conductivity of natural-fibre-based thermal insulation materials varied within the range of 0.0333 ÷ 0.0438 W/(m·K), the tensile strength varied from 2.5 to 130 kPa, the short-term water absorption varied from 0.5 to 8.5 kg/m2, and the water vapour diffusion resistance factor varied from 2.537 to 2.667. It was additionally determined that all the studied products were flammable. The water absorption and flammability values were significantly reduced by the use of hydrophobic agents and flame retardants.

Biodegradable Polyurethane Derived from Hydroxylated Polylactide with Superior Mechanical Properties.

Developing biodegradable polyurethane (PU) materials as an alternative to non-degradable petroleum-based PU is a crucial and challenging task. This study utilized lactide as the starting material to synthesize polylactide polyols (PLA-OH). PLA-based polyurethanes (PLA-PUs) were successfully synthesized by introducing PLA-OH into the PU molecular chain. A higher content of PLA-OH in the soft segments resulted in a substantial improvement in the mechanical attributes of the PLA-PUs. This study found that the addition of PLA-OH content significantly improved the tensile stress of the PU from 5.35 MPa to 37.15 MPa and increased the maximum elongation to 820.8%. Additionally, the modulus and toughness of the resulting PLA-PU were also significantly improved with increasing PLA-OH content. Specifically, the PLA-PU with 40% PLA-OH exhibited a high modulus of 33.45 MPa and a toughness of 147.18 MJ m-3. PLA-PU films can be degraded to carbon dioxide and water after 6 months in the soil. This highlights the potential of synthesizing PLA-PU using biomass-renewable polylactide, which is important in green and sustainable chemistry.

Influence of Processing Parameters on Mechanical Properties and Degree of Crystallization of Polylactide.

This work attempts to assess the influence of process parameters on the change of mechanical properties and the degree of crystallinity of polylactide (PLA). PLA is a biodegradable material that has been widely used in various areas-from packaging, through medicine, to 3D printing, where it is used to produce prototypes. The method of processing is important, because the technological process and its parameters have a significant impact on the quality of the finished product. Their appropriate selection depends on quality and mechanical properties. The process parameters have an impact on the structure of PLA, specifically on the share of the crystalline phase, which is also important from the point of view of the functional properties of the finished product. This work assessed the impact of the technological parameters of the injection process on the final properties of the obtained samples. The obtained results of static tensile strength, hardness and differential scanning calorimetry (DSC) analysis confirm that changing these parameters affects the material properties.

Regulating the proinflammatory response to composite biomaterials by targeting immunometabolism.

Composite biomaterials comprising polylactide (PLA) and hydroxyapatite (HA) are applied in bone, cartilage and dental regenerative medicine, where HA confers osteoconductive properties. However, after surgical implantation, adverse immune responses to these composites can occur, which have been attributed to size and morphology of HA particles. Approaches to effectively modulate these adverse immune responses have not been described. PLA degradation products have been shown to alter immune cell metabolism (immunometabolism), which drives the inflammatory response. Accordingly, to modulate the inflammatory response to composite biomaterials, inhibitors were incorporated into composites comprised of amorphous PLA (aPLA) and HA (aPLA + HA) to regulate glycolytic flux. Inhibition at specific steps in glycolysis reduced proinflammatory (CD86+CD206-) and increased pro-regenerative (CD206+) immune cell populations around implanted aPLA + HA. Notably, neutrophil and dendritic cell (DC) numbers along with proinflammatory monocyte and macrophage populations were decreased, and Arginase 1 expression among DCs was increased. Targeting immunometabolism to control the proinflammatory response to biomaterial composites, thereby creating a pro-regenerative microenvironment, is a significant advance in tissue engineering where immunomodulation enhances osseointegration and angiogenesis, which could lead to improved bone regeneration.

Open- and Closed-Loop Recycling: Highly Active Zinc Bisguanidine Polymerization Catalyst for the Depolymerization of Polyesters.

In this study, the aliphatic N,N-bisguanidine zinc complex [Zn(DMEG2ch)2](OTf)2·THF is introduced as a promising candidate for the chemical recycling of (bio)polyesters. This catalyst is highly active in the ring-opening polymerization (ROP) of lactide (LA) and ε­caprolactone (CL). The combination of polymerization and depolymerization activity creates new pathways towards a sustainable circular economy. The catalytic activity of [Zn(DMEG2ch)2](OTf)2·THF for the chemical recycling of polylactide (PLA) via alcoholysis was investigated by detailed kinetic and thermodynamic studies. It is shown that various high value-added alkyl lactates can be obtained efficiently under mild reaction conditions. Catalyst recycling was successfully tested using ethanol for the degradation of PLA. In addition, LA can be recovered directly from PLA, enabling either open- or closed-loop recycling. Selective PLA degradation from mixtures with polyethylene terephthalate (PET) and polymer blends are presented. For the first time, a cascade recycling reaction of a PLA/polycaprolactone (PCL) blend is tested with a zinc-based bisguanidine catalyst, whereby PLA is degraded selectively at first and subsequent modification of the reaction conditions leads to efficient degradation of the remaining PCL. The highly active, universally applicable benign zinc catalyst allows the implementation of a circular plastics economy and thus the reduction of plastic pollution in the environment.

The Influence of Environmental Factors on the Degradation of PLA/Diatomaceous Earth Composites.

In the present study, tests were carried out on composite samples on a polylactide matrix containing 25% by weight of mineral filler in the form of diatomaceous earth, base, and silanized with GPTMOS (3-glycidoxypropyltrimethoxysilane), OTES (n-octyltriethoxysilane), and MTMOS (methyltrimethoxysilane) silanes. The addition of two types of waxes, synthetic polyamide wax and natural beeswax, were used as a factor to increase the rheological properties of the composites. The obtained samples were characterized in terms of the effect of filler silanization on the degradation rate of the composites. The tests were conducted under different conditioning conditions, i.e., after exposure to strong UV radiation for 250 and 500 h, and under natural sunlight for 21 days. The conditioning carried out under natural conditions showed that the modified samples exhibit up to twice the degradation rate of pure polylactide. The addition of synthetic wax to the composites increases the tendency to agglomerate diatomaceous earth, while natural wax has a positive effect on filler dispersion. For composites modified with GPTMOS and OTES silanes, it was noted that the addition of natural wax inhibited the degree of surface degradation, compared to the addition of synthetic wax, while the addition of MTMOS silane caused the opposite effect and samples with natural wax degraded more strongly. It was shown that, despite the high degree of surface degradation, the process does not occur significantly deep into the composite and stops at a certain depth.

Comparison of Polylactide-Based Active Films Containing Berberine and Quercetin as Systems for Maintaining the Quality and Safety of Blueberries.

Polymeric thin films based on polylactide with an addition of poly(ethylene glycol) as a plasticizer and flavonoids in the form of quercetin and berberine were subjected to tests that were particularly relevant from the point of view of contact with food. A comparative analysis of the effect of individual flavonoids on the antioxidative properties of tested films and blueberry storage was carried out. The influence of active compounds on the water vapor permeability, as well as UV protection, of the obtained materials was investigated. Also, the specific migration of individual flavonoids from obtained materials to food simulants in the form of acetic acid and ethyl alcohol was determined. The crucial point of this study is the storage of blueberries. The obtained results indicate that the selection of packaging, containing individual active compounds, depends on the purpose and requirements that the packaging must meet for particular types of food.

In-situ self-reinforcement of amorphous polylactide (PLA) through induced crystallites network and its highly ductile and toughened PLA/poly(butylene adipate-co-terephthalate) (PBAT) blends.

Crystallites of a semicrystalline polylactide (cPLA) were induced in an amorphous PLA (aPLA) and its blends with poly(butylene adipate-co-terephthalate) (PBAT) to achieve in-situ self-reinforced PLA based structures. The approach involved the melt blending of cPLA as a minor phase with aPLA and its blends with PBAT at processing temperatures below the crystal melting peak of cPLA. An injection molding (IM) process was first adopted to obtain self-reinforced PLA (SR-PLA) structures at aPLA/cPLA weight ratios of 100/0, 95/5, 90/10, 85/15, and 80/20. IM barrel and mold temperatures revealed crucial impacts on preserving the cPLA crystallites and thereby enhancing the final mechanical performance of SR-PLA (i.e., aPLA/cPLA) samples. SR-PLA samples at various aPLA/cPLA weight ratios of 100/0, 90/10, 80/20, and 70/30 were then melt blended with PBAT to produce SR-PLA/PBAT at a given ratio of 85/15. These blends were first prepared in an internal melt mixer (MM) to evaluate the rheological properties. The rheological analysis confirmed the significance of cPLA reinforcing efficiency within SR-PLA and its corresponding blends with PBAT. Similar SR-PLA/PBAT blends were also prepared using the IM process to explore their thermal and mechanical characteristics. The effect of cPLA concentrations in blends was distinctive, leading to significant enhancements in stain at break and toughness values. This was due to the increased crystallite network within the matrix, further refining PBAT droplets. Morphological analysis of the melt-processed blends through MM and IM also revealed that the PBAT droplets were further refined when the IM process was applied. The induced shear during the molding could have further elongated the cPLA crystallites towards a fiberlike structure, which could additionally cause the matrix viscosity to increase and refine the PBAT droplets.

Bilayer Scaffolds of PLLA/PCL/CAB Ternary Blend Films and Curcumin-Incorporated PLGA Electrospun Nanofibers: The Effects of Polymer Compositions and Solvents on Morphology and Molecular Interactions.

Tissue engineering scaffolds have been dedicated to regenerating damaged tissue by serving as host biomaterials for cell adhesion, growth, differentiation, and proliferation to develop new tissue. In this work, the design and fabrication of a biodegradable bilayer scaffold consisting of a ternary PLLA/PCL/CAB blend film layer and a PLGA/curcumin (CC) electrospun fiber layer were studied and discussed in terms of surface morphology, tensile mechanical properties, and molecular interactions. Three different compositions of PLLA/PCL/CAB-60/15/25 (TBF1), 75/10/15 (TBF2), and 85/5/10 (TBF3)-were fabricated using the solvent casting method. The electrospun fibers of PLGA/CC were fabricated using chloroform (CF) and dimethylformamide (DMF) co-solvents in 50:50 and 60:40 volume ratios. Spherical patterns of varying sizes were observed on the surfaces of all blend films-TBF1 (17-21 µm) > TBF2 (5-9 µm) > TBF3 (1-5 µm)-caused by heterogeneous surfaces inducing bubble nucleation. The TBF1, TBF2, and TBF3 films showed tensile elongation at break values of approximately 170%, 94%, and 43%, respectively. The PLGA/CC electrospun fibers fabricated using 50:50 CF:DMF had diameters ranging from 100 to 400 nm, which were larger than those of the PLGA fibers (50-200 nm). In contrast, the PLGA/CC electrospun fibers fabricated using 60:40 CF:DMF had diameters mostly ranging from 200 to 700 nm, which were larger than those of PLGA fibers (200-500 nm). Molecular interactions via hydrogen bonding were observed between PLGA and CC. The surface morphology of the bilayer scaffold demonstrated adhesion between these two solid surfaces resembling "thread stitches" promoted by hydrophobic interactions, hydrogen bonding, and surface roughness.

Tuning the Structure-Property Relationships in Binary and Ternary Blends of PLA/PBAT/PHBH.

While the brittle polylactide (PLA) has a high durability among bioplastics, poly(3-hydroxybutyrate-co-3-hydroxyhexanoate) (PHBH) with certain ductility exhibits facile compostability. The addition of polybutylene adipate terephthalate (PBAT) may also be used to improve the ductility and toughness of brittle bioplastics. Binary and ternary blends of PLA/PBAT/PHBH based on either PLA or PHBH as the matrix have been manufactured using a twin-screw extruder. The melt rheological, mechanical, and morphological properties of the processed samples were examined. Binary blends of PLA/PHBH show superior strength, with the PLA75/PHBH25 blend exhibiting a tensile strength of 35.2 ± 3.0 MPa, which may be attributed to miscible-like morphology. In contrast, blends of PLA with PBAT demonstrate low strength, with the PLA50/PBAT50 blend exhibits a tensile strength of 9.5 ± 2.0 MPa due to the presence of large droplets in the matrix. PBAT-containing blends exhibit lower impact strengths compared to PHBH-containing blends. For instance, a PLA75/PBAT25 blend displays an impact strength of 1.76 ± 0.1 kJ/m2, whereas the PHBH75/PBAT25 blend displays an impact strength of 2.61 ± 0.3 kJ/m2, which may be attributed to uniformly dispersed PBAT droplets.

A biomass phosphonamide enables biodegradable polylactide with favorable flame retardancy and rapid crystallization.

PLA is widely known as biodegradable plastics whose further application in fields such as automotive and architectural is still constrained by its flammability and unsatisfactory crystallization properties. To address the aforementioned concerns, a novel biomass phosphonamide PDPA was synthesized with chemical structure confirmed by FTIR, NMR and elemental analysis tests. Immediately thereafter, PLA/PDPA composites were prepared by melting blending, with a focus on flame retardancy, crystallization properties and flame-retardant mechanism. As expected, PDPA efficiently enhanced both the flame retardancy and crystallization properties of PLA. Specifically, the PLA/4.0PDPA obtained UL-94 V-0 grade and the LOI value increased to 28.6 % with only 4 wt% PDPA added, which comes down to the superior free radical capture and dilution effect of PDPA in the vapor phase and the melting droplet effect. More appealingly, the crystallinity of PLA/4.0PDPA was significantly enhanced to 43.4 % from 2.5 % of PLA, and the shortest t1/2 was 4 mins in the isothermal crystallization process due to the excellent heterogeneous nucleation of PDPA. Moreover, PLA/PDPA composites maintain almost the same mechanical performance as pure PLA. In brief, this work provides a green strategy for the preparation of PLA composites with excellent comprehensive performance and shows great potential in engineering materials.

Development of functionalized poly(lactide) films with chitosan via SI-SARA ATRP as scaffolds for neuronal cell growth.

Polylactic acid (PLA), a polymer derived from renewable resources, is gaining increasing attention in the development of biomedical devices due to its cost-effectiveness, low immunogenicity, and biodegradability. However, its inherent hydrophobicity remains a problem, leading to poor cell adhesion features. On this basis, the aim of this work was to develop a method for functionalizing the surface of PLA films with a biopolymer, chitosan (CH), which was proved to be a material with intrinsic cell adhesive properties, but whose mechanical properties are insufficient to be used alone. The combination of the two polymers, PLA as a bulk scaffold and CH as a coating, could be a promising combination to develop a scaffold for cell growth. The modification of PLA films involved several steps: aminolysis followed by bromination to graft amino and then bromide groups, poly(glycidyl methacrylate) (PGMA) grafting by surface-initiated supplemental activator and reducing agent atom transfer radical polymerization (SI-SARA ATRP) and finally the CH grafting. To prove the effective adhesive properties, conjugated and non-conjugated films were tested in vitro as substrates for neuronal cell growth using differentiated neurons from human induced pluripotent stem cells. The results demonstrated enhanced cell growth in the presence of CH.

Complete sequence randomness of lactate-based copolymers (LAHBs) with varied lactate monomer fractions employing a series of propionyl-CoA transferases.

Previously, we biosynthesized an evolved version of a bio-based polylactide (PLA) on microbial platforms using our engineered lactate-polymerizing enzyme (LPE). This lactate (LA)-based copolyester, LAHB, has advantages over PLA, including improved flexibility and biodegradability, and its properties can be regulated through the LA fraction. To expand the LA-incorporation capacity and improve polymer properties, in the state of in vivo LAHB production, propionyl-CoA transferases (PCTs) that exhibited enhanced production of LA-CoA than the conventional PCTs were selected. Here, the present study has demonstrated that the LA fraction of LAHB could be altered using various PCTs. Enhanced PCT performance was achieved by balancing polymer production and cell growth. Both events are governed by the use of acetyl-CoA, a commonly shared key metabolite. This could be attributed to the different reactivities of individual PCTs towards acetyl-CoA, which serves both as a CoA donor and a leading compound in the TCA cycle. Interestingly, we found complete sequence randomness in the LAHB copolymers, independent of the LA fraction. The mechanism of LA fraction-independent sequence randomness is discussed. This new PCT-based strategy synergistically combines with the evolution of LPE to advance the LAHB project, and enables us to perform advanced applications other than LAHB production utilizing CoA-linked substrates.

Superhydrophobic stereocomplex-type polylactide/ultra-fine glass fibers aerogel for passive daytime radiative cooling.

Passive daytime radiative cooling (PDRC) technology offers a green and sustainable strategy for cooling, eliminating the need for external energy sources through its exceptional efficiency in heat radiation and sunlight reflection. Despite its benefits, the widespread usage of non-biodegradable PDRC materials has unfortunately caused environmental pollution and resource wastage. Furthermore, the effectiveness of outdoor PDRC materials can be significantly diminished by rainfall. In this work, a superhydrophobic composite aerogel composed of stereocomplex-type polylactide and ultra-fine glass fiber has been successfully developed through simple physical blending and freeze-drying, which exhibits low thermal conductivity (36.26 mW m-1 K-1) and superhydrophobicity (water contact angle up to 150°). Additionally, its high solar reflectance (91.68 %) and strong infrared emissivity (93.95 %) enable it to effectively lower surface temperatures during daytime, resulting in a cooling effect of approximately 3.8 °C below the ambient temperature during the midday heat of summer, with a cooling power of 68 W/m2. This aerogel offers an environmentally friendly and sustainable approach for the utilization of radiative refrigeration materials, paving the way for environmental protection and sustainable development.

Electrospun Polylactide-Poly(ε-Caprolactone) Fibers: Structure Characterization and Segmental Dynamic Response.

Electrospun ultrathin fibers based on binary compositions of polylactide (PLA) and poly(ε-caprolactone) (PCL) with the various content from the polymer ratio from 0/100 to 100/0 have been explored. Combining thermal (DSC) and spectropy (ESR) techniques, the effect of biopolymer content on the characteristics of the crystal structure of PLA and PCL and the rotative diffusion of the stable TEMPO radical in the intercrystallite areas of PLA/PCL compositions was shown. It was revealed that after PLA and PCL blending, significant changes in the degree of crystallinity of PLA, PCL segment mobility, sorption of the Tempo probe, as well as its activation energy of rotation in the intercrystalline areas of PLA/PCL fibers, were evaluated. The characteristic region of biopolymers' composition from 50/50 to 30/70% PLA/PCL blend ratio was found, where the inversion transition of PLA from dispersive medium to dispersive phase where an inversion transition is assumed when the continuous medium of the PLA transforms into a discrete phase. The performed studies made it possible, firstly, to carry out a detailed study of the effect of the system component ratio on the structural and dynamic characteristics of the PLA/PCL film material at the molecular level.

Effect of Bentonite on the Electrical Properties of a Polylactide-Based Nanocomposite.

In this paper, a novel polylactide-based nanocomposite with the addition of bentonite as a filler, Fusabond, and glycerine as a compatibilizer and plasticizer, were prepared and investigated. Four samples with different contents of bentonite (1, 5, 10, and 15 wt.%), as well as three samples without fillers, were prepared with an easily scalable method: melt blending. The electrical properties of all prepared samples were investigated with broadband dielectric spectroscopy in the frequency range between 0.1 Hz and 1 MHz. Measurements were conducted at nine temperatures between 293.15 and 333.15 K (20 to 60 °C) with steps of 5 K. It was found that the increase in the content of bentonite in polylactide has a significant effect on the electrical properties of the prepared nanocomposites.

Understanding the Impact of Chain Mobility on Conformational Evolution and Kinetics of Mesophase Formation in Poly(ʟ-lactide) under Low-Pressure CO2.

Although the mesomorphic phase as an intermediate state has been introduced to understand polymer crystallization, the understanding of the mesomorphic phase is far from complete. Here, the effect of chain mobility on the mesophase structuring in melt-quenched poly(ʟ-lactide) (PLLA) treated in low-pressure CO2 at 1.6-2.0 MPa and 0 °C was investigated using infrared (IR) spectroscopy, differential scanning calorimetry (DSC), and atomic force microscopy (AFM). The IR and AFM results demonstrated that the final degree of order and the kinetics of structural evolution during the CO2-induced mesophase formation were critically dependent on the CO2 pressure. This was attributed to the distinct dynamics of conformational evolution (gg to gt conformer transition) due to the different CO2 pressures. The thermal behavior from the DSC results showed that CO2 pressure dominated both the scale and dynamics of the chain motion of PLLA. At a lower CO2 pressure of 1.6 MPa, smaller-scale segmental motion was not replaced by the larger-scale cooperative motion that occurred at a relatively higher CO2 pressure of 2 MPa, which was favorable for faster mesophase formation. Consequently, by inhibiting direct crystallization under limited mobility conditions, it was demonstrated that different chain mobility controlled by CO2 pressure and thus CO2 solubility impacted the dynamics of the mesophase formation of PLLA. The present results have implications for understanding the role of chain mobility in determining the intermediate structural phases in semicrystalline polymers.

Clinical study of antibacterial medical textiles containing polyhydroxyalkanoate oligomers for reduction of hospital-acquired infections.

INTRODUCTION: The prevention and control of hospital-acquired infections remain a significant challenge worldwide, as textiles used in hospital wards are highly involved in transmission processes. This paper reports a new antibacterial medical fabric used to prepare hospital pillowcases, bottom sheets and quilt covers for controlling and reducing hospital-acquired infections. METHOD: The medical fabric was composed of blended yarns of staple polyester (PET) and degradable poly(3-hydroxybutyrate co-3-hydroxyvalerate) (PHBV)/polylactic acid (PLA) fibres, which were coated with polylactide oligomers (PLAO), which are environmentally friendly and safe antimicrobial agents with excellent thermal stability in high-temperature laundry. A clinical trial was conducted, with emphasis on the bacterial species that were closely related to the infection cases in the study hospital. RESULT: After 7 days of use, 94% of PET/PHBV/PLA-PLAO fabric retained <20 colony-forming units/100 cm2 of the total bacterial amount, meeting hygiene and cleanliness standards. CONCLUSION: This study demonstrates the potential of fabrics containing polyhydroxyalkanoate oligomers as highly effective, safe and long-lasting antimicrobial medical textiles that can effectively reduce the incidence of hospital-acquired infections.

Microstructural and Hydrophilic Properties of Polylactide Polymer Samples with Various 3D Printing Patterns.

The aim of the work is to study the effect of the 3D printing process on the microstructural and hydrophilic properties of polylactic acid (PLA) samples with various model printing patterns obtained from the black filament PLA by sequentially applying polymer layers using the FDM (fused deposition modeling) method. X-ray phase analysis revealed the partial crystallization of PLA polymer chains in the printed samples, which occurs under thermal and mechanical action on the original amorphous PLA filament during 3D printing to varying degrees, depending on the geometry of the pattern and the morphology of its surface. At the same time, IR spectroscopy data indicate the preservation of all intrastructural chemical bonds of polylactide. Measured at the original installation, the values of the wetting edge angles on the surface of the printed samples are in the range φ = 50-60°, which is significantly less than the right angle. This indicates the hydrophilic properties of the whole sample's surface. At the same time, the influence of different geometries of model drawings in printed samples was found not only on the morphology of the sample's surface according to SEM data but also on its wettability.

Chitin nanocrystals-stabilized emulsion as template for fabricating injectable suspension containing polylactide hollow microspheres.

One of the promising applications of rod-like chitin nanocrystals (ChNCs) is the use as particle emulsifier to develop Pickering emulsions. We reported a ChNC-stabilized oil-in-water emulsion system, and developed a Pickering emulsion-templated method to prepare polylactide (PLA) hollow microspheres here. The results showed that both non-modified ChNCs and acetylated ChNCs could well emulsify the dichloromethane (DCM) solution of PLA-in-aqueous mannitol solution systems, forming very stable emulsions. At the same oil-to-water ratios and ChNC loadings, the emulsion stability was improved with increasing acetylation levels of ChNCs, accompanied by reduced size of droplets. Through the solvent evaporation, the PLA hollow microspheres were templated successfully, and the surface structure was also strongly dependent on the acetylation level of ChNCs. At a low level of acetylation, the single-hole or multi-hole surface structure formed, which was attributed to the out-diffusion of DCM caused by the solvent extraction and evaporation. These surface defects decreased with increased acetylation levels of ChNCs. Moreover, the aqueous suspension with as-obtained PLA microspheres revealed shear-thinning property and good biocompatibility, thereby had promising application as injectable fillers. This work can provide useful information around tuning surface structures of the Pickering emulsion-templated polymer hollow microspheres by regulating acetylation level of ChNCs.