Molar Composition Research Articles

Synergized enzyme-ultrasound-assisted aqueous two-phase extraction and antioxidant activity validation of polysaccharides from tobacco waste

A powerful and innovative technique was developed to efficiently extract and refine polysaccharides from tobacco waste. This was achieved through a combination of enzyme and ultrasound-assisted extraction assisted aqueous two-phase extraction (EUAATPE). The formation of an aqueous two-phase system (ATPS) using various salts and ethanol was investigated. ATPS of 18.0 % (NH4)2SO4 (w/w) and 25.0 % ethanol (w/w) was chosen due to its favorable selection extraction ability and high recovery of 93.68 ± 0.40 %. By utilizing both single-factor experiments and response surface method (RSM), the key factors involved in the EUAATPE process were optimized. The optimal conditions were as follows: ultrasonic power 180 W, ultrasonic time 9 min, cellulase concentration 2.0 %, pectinase concentration 1.0 %, extraction temperature 50 °C, extraction time 1.5 h, and liquid-to-solid ratio 30:1 (g/g). Under the optimal conditions, the extraction yield of polysaccharides was 6.72 ± 0.11 (mg/g), and the purity of the polysaccharides from the bottom phase was 78.73 ± 3.17 %. EUAATPE resulted in a significant enhancement in the extraction yield and purity of polysaccharides from tobacco waste compared to traditional methods such as hot water extraction (HWE), ultrasound-assisted extraction (UAE) and enzyme-assisted extraction (EAE). Polysaccharides of tobacco waste obtained from various methods had analogous monosaccharide compositions, different molar ratio compositions and surface structure characteristics. Moreover, all polysaccharides exhibited a certain extent antioxidant activities and polysaccharides from the bottom phase (PBP) extracted by EUAATPE showed superior antioxidant activity. Hence, EUAATPE, being an innovative and eco-friendly extraction technique, presents a productive substitute for extracting and refining polysaccharides from discarded tobacco resources.

Impact of Molar Composition on the Functional Properties of Glutinous Rice Starch-Chitosan Blend: Natural-Based Active Coating for Extending Mango Shelf Life.

This study investigates natural-based blends of glutinous rice starch (GRS) and chitosan (CS), varying their molar composition (0:100, 30:70, 50:50, 70:30, and 100:0) to explore their interaction dynamics. Our findings illustrate the versatility of these blends in solution and film forms, offering applications across diverse fields. Our objective is to understand their impact on coatings designed to extend the post-harvest shelf life of mangoes. Results reveal that increasing chitosan content in GRS/CS blends enhances mechanical strength, hydrophobicity, and resistance to Colletotrichum gloeosporioides infection, a common cause of mango anthracnose. These properties overcome limitations of GRS films. Advanced techniques, including FTIR analysis and stereo imaging, confirmed robust interaction between GRS/CS blend films and mango cuticles, improving coverage with higher chitosan content. This comprehensive coverage reduces mango dehydration and respiration, thereby preserving quality and extending shelf life. Coating with a GRS/CS blend containing at least 50% chitosan effectively prevents disease progression and maintains quality over a 10-day storage period, while uncoated mangoes fail to meet quality standards within 2 days. Moreover, increasing the starch proportion in GRS/CS blends enhances film density, optical properties, and reduces reliance on acidic solvents, thereby minimizing undesirable changes in product aroma and taste.

Phase behavior of supercritical CO2 + nonionic ethoxylated surfactants + methanol: Experimental data and modeling with PC-SAFT equation of state

The use of surfactants for oil and gas purposes has been explored and extensively applied. However, such systems' thermodynamic and predictability behavior still needs further investigation. This work aims to describe the phase behavior of the systems composed of nonionic ethoxylated surfactants (nonylphenyl ethoxylated surfactants—IGEPAL CO-630 and CO-720) + carbon dioxide (CO2) with additional methanol in wide ranges of temperature (T = 313 to 413 K), pressure (P = 0.8 to 54.8 MPa), and CO2 molar compositions (up to 90.0 %). It was observed for all systems studied that CO2 solubility was inversely proportional to temperature and the number of ethoxylated units for pure surfactants. The addition of methanol greatly increases the overall CO2 solubility. The thermodynamic modeling through the PC-SAFT equation of state was also evaluated. Bubble pressure deviations of 13.63 % and 13.49 % were obtained for pure IGEPAL CO-630 and IGEPAL CO-720 + CO2, respectively, and 12.63 % for the ternary system (IGEPAL CO-720 + methanol + CO2). A new set of binary interaction parameters was also provided for IGEPAL CO-630 and IGEPAL CO-720 + CO2.

Adipose Stem Cell Response to Borophosphate Bioactive Glass

Silicate and borate bioactive glasses have been reported to create alkaline conditions by rapidly releasing ions when reacting in aqueous solution. At certain levels, this alkaline solution can negatively affect cell viability. Adding phosphate ions to the glass composition can control the degradation rate of bioactive glasses and create a neutral pH environment. This study evaluated a series of borophosphate bioactive glasses (BPBGs) with nominal molar compositions 16Na2O-24CaO-xB2O3-(60-x)P2O5, where x = 0, 40, or 60. The phosphate (X0) glass (PBG) produced an acidic solution when dissolved in water; the borate (X60) glass (BBG) produced an alkaline solution, and the BPBG glass produced a pH-neutral solution. These three glasses were evaluated using adipose stem cells (ASCs), a cell population known for their therapeutic abilities. The effects of each glass on the pH of cell culture, ions released during degradation, and on ASC functions, including viability, migration, angiogenic ability, differentiation, and protein secretions, were evaluated. The X40 BPBG created a physiologically neutral pH in cell culture media after 24 h. The X0 phosphate glass promoted ASC migration, while the highly alkaline X60 borate increased the angiogenic ability of ASCs. These results indicate that BPBG can be used safely in cell culture studies and customized for specific biomedical applications.

Dual-template synthesis of SFO-type aluminophosphate with enhanced water-sorption-driven cooling performance

Water-based adsorption chillers (ADC) driven by low-grade thermal energy are environment-friendly alternatives to the traditional compression ones to realize the net zero carbon target. Aluminophosphates molecular sieve (AlPOs) is an excellent material for water-based adsorption applications. However, AlPOs suffers from relatively high cost attributed to the extensive use of expensive structure direct agents (SDAs). This study employed a dual-template method, using cheap organic amine as a dual-template, to synthesize low-cost and excellent adsorbent AlPOs with SFO topology (AlPO-SFO). AlPO-SFO synthesized with dual templates shows high crystallinity, large micropore volume, excellent water uptake, and low regeneration temperature. AlPO-SFO guided by 4-dimethylaminopyridine (4-DMAPy) and diethanolamine (DEOA) molar composition of 0.4 and 0.1 exhibits large microporous volume (0.30 ml g−1), high water uptake (0.26 g g−1 at P/P0 = 0.25) and low regeneration temperature (65 °C). Importantly, this AlPO-SFO exhibits a high coefficient of performance (COP) of 0.89 for cooling at a low driven temperature of 64 °C. The additive amine providing alkaline medium ensures the practical synthesis of AlPO-SFO when expensive 4-DMAPy decreases, endowing the 42 % reduction of the raw material cost. The results provide a cheaper synthesis route of AlPO-SFO, which is conducive to its large-scale production as a distinguished adsorbent for adsorption chillers.

Barrier Properties of Biodegradable Aliphatic–Aromatic Copolyesters (PBXT Series)

AbstractIn this study, a series of biodegradable poly(butylene alkylene carboxylate‐co‐terephthalate) copolymers with varying methylene numbers in the alkylene units (0, 2, 4, and 8) are synthesized. These copolymers, namely, poly(butylene oxalate‐co‐terephthalate) (PBOT), poly(butylene succinate‐co‐terephthalate) (PBST), poly(butylene adipate‐co‐terephthalate) (PBAT), and poly(butylene sebacate‐co‐terephthalate) (PBSeT), are prepared with nearly identical structural and molar compositions. The objective of this study is to comprehensively examine the impact of alkylene unit length on the barrier properties of the materials, delving into aspects such as crystallinity, free volume, molecular chain mobility, as well as adsorption and diffusion of gases within the materials. The findings indicate a decrease in crystallinity from 17.2% for PBOT to 10.2% for PBSeT as the alkylene chain length increases, while maintaining the same chemical composition. Concurrently, the fractional free volume increases from 0.9% to 2.6%, and the melt flow activation energy decreases from 106.6 to 52.1 kJ mol−1. Importantly, theoretical calculations are performed, demonstrating that the predominant site for gas adsorption and diffusion is within the material's free volume. These combined observations indicate a gradual decrease in barrier properties as the number of methylene groups increases.

Experimental assessment of reverse water gas shift integrated with chemical looping for low-carbon fuels

Chemical looping integrated with reverse water gas (CL-RWGS) shift is presented in this study using Cu-based oxygen carrier (OC) supported on Al2O3 has been used to convert the CO2 and H2 mixture stream into a syngas stream with a tailored H2 to CO ratio and relevant conditions. The results demonstrated consistent breakthrough curves during redox cycles, confirming the chemical stability of the material. In 10 consecutive cycles at 600 °C and 1 bar, bed temperatures increased by 184 °C and 132 °C across the bed during oxidation and reduction stages respectively. The cooling effects during RWGS showed a decline in solid temperatures demonstrating the effectiveness of the heat removal strategy while attaining a CO2-to-CO conversion close >48%. The outlet gas maintains a H2/CO ratio above 2, confirming the material's dual role as OC and catalyst. During complete CL-RWGS cycles, varying temperature from 500 °C to 600 °C at a constant H2/CO2 molar ratio (1.3) and pressure (1 bar) reduces the H2/CO molar ratio from 3.14 to 2.35, respectively with a remarkable continuous CO2-to-CO conversion > 40%. The decrease in H2/CO molar ratio with the increase in temperature is consistent with the expected results of equilibrium limited conditions. Additionally, in CL-RWGS cycles, pressure insignificantly affects product molar composition. The study showed the capability of Cu material in converting CO2 into syngas through the CL-RWGS technique.

Determination of the individual block lengths of the block copolymers of Poly(trimethylene carbonate) by liquid chromatography at critical conditions

Amphiphilic block copolymers based on poly(trimethylene carbonate) (PTMC) have gained significant attention for biomedical applications owing to their unique degradation characteristics. Ring-opening polymerization (ROP) is the most widely employed method for polymerization of cyclic carbonates, especially for trimethylene carbonate (TMC). Herein, di- and tri-block copolymers of PTMC are synthesized by ROP of TMC using poly(ethylene glycol) monomethyl ether (MeO-PEG) or poly(ethylene glycol) (PEG) as a macro-initiator, respectively. The synthesized products are characterized by size-exclusion chromatography (SEC) and nuclear magnetic resonance spectroscopy (1H NMR) for their molar mass and chemical composition, respectively. However, these techniques are inconclusive about several pertinent aspects of the block copolymers, such as individual block length and unwanted homopolymer content. To address these limitations, liquid chromatography at critical conditions of both PEG and PTMC are employed. Chromatographic critical conditions for PTMC are reported for the first time in the current study. The analysis protocol successfully reveals the individual block lengths of both blocks of the block copolymers, along with the quantification of the unwanted homopolymers in the samples. The individual block lengths and the presence of homopolymers significantly affect the self-assembly capability and drug-loading capacity of amphiphilic block copolymers. Thus, the study divulges important information crucial for the development of structure-property correlations, which is essential for optimizing the performance of these block copolymers in biomedical applications.

Tg, Density and X-ray Diffraction of Zinc-doped Bioactive Glasses with Molar Formulation: 20.15[(2.038+x)SiO2-(1.457-x)Na2O]-2.6P2O5-26.905CaO-0.045ZnO System

In the present work, glasses with molar composition 20.15[(2.038+x)SiO2-(1.457-x)Na2O]-2.6P2O5-26.905CaO-0.045ZnO were studied in order to contribute to the application of thermal analysis methods to the characterization of zinc-doped bioactive glasses. The aim is to provide answers to the expectations of practitioners before in vitro or in vivo tests on the physicochemical properties of these zinc doped bioactive glasses. Samples were produced by high temperature melting followed by quenching. The samples were characterized by X-Ray Diffraction (XRD), Differential Scanning Calorimetry (DSC) and pycnometry. The results show that the samples are amorphous, and the values for vitreous transition temperature and density are of the same order of magnitude as those for the system without addition of ZnO. Consequently, it appears that the addition of 0.045 % mol of ZnO to the base glass does not significantly alter the physicochemical and structural properties of the glass.

Experimental investigation of the CO2+SiCl4 mixture as innovative working fluid for power cycles: Bubble points and liquid density measurements

Supercritical CO2 is recognized as a promising working fluid for next-generation of high temperature power cycles. Nevertheless, the use of CO2 mixtures with heavier dopants is emerging as a promising alternative to supercritical CO2 cycles in the recent years for air-cooled systems in hot environments. Accordingly, this work presents an experimental campaign to assess the thermodynamic behaviour of the CO2+SiCl4 mixture to be used as working fluid for high-temperature applications, conducted in the laboratories of CTP Mines Paris PSL. At first, bubble conditions of the mixture are measured in a variable volume cell (PVT technique), then liquid densities are measured with a vibrating tube densimeter, for molar composition in the range between 70 % and 90 % of CO2. The Peng Robinson EoS was fine-tuned on the bubble points obtained, resulting in a satisfactory accuracy level. Finally, a non-conventional methodology has been developed to measure bubble points with the vibrating tube densimeter, whose results are consistent with the VLE data obtained with the standard PVT technique. Thermodynamic analysis in next-generation concentrated solar power plant, at 700 °C turbine inlet, confirms the mixture overcomes 50 % thermal efficiency, providing +4.2 % net electrical output over pure supercritical CO2 at equal thermal power from the solar field.

Study of optical, structural and radiation shielding properties of (55 − x)TeO2–20ZnO–25B2O3–xEr2O3 glass matrix

Abstract Erbium doped zinc boro-tellurite (EZBT) glass samples with molar composition of (55 − x)TeO2–20ZnO–25B2O3–xEr2O3 (x = 0.0, 0.5, 1.0, 1.5 and 2.0 mol.%) were prepared by a conventional melt quenching technique. The prepared samples were characterised using X-ray diffraction, Fourier transform infrared spectroscopy and ultraviolet–visible spectroscopy techniques to investigate the structural, optical and dielectric properties. To study the radiation shielding capabilities, the parameters such as mass attenuation coefficient (μ m), half-value layer (HVL), effective atomic number (Z eff) etc., were evaluated using WinXCom software. Judd–Ofelt analysis was carried out to determine the intensity of electronic transitions and other radiative transition parameters within the 4f shell of erbium ions. The μ m values in a range of (108.5–0.03) cm2 g−1 for energy range (0.01–10) MeV were obtained for 2.0 mol.% erbium-doped tellurite glass matrix. The μ m and HVL values were also compared with conventionally used ordinary concrete and specific lead borate glass at certain energies. The detailed investigation of this current EZBT glass matrix is very useful in the specific optical and radiation shielding applications of this EZBT glass.

Crystalline / glass nanoscale chemical separation induced by femtosecond laser pulses in aluminosilicate glass

An aluminosilicate glass with a molar composition of 60%Al2O3–40%SiO2 fabricated by the aerodynamic levitation technique was irradiated in volume using an infrared femtosecond laser. Optical retardance was observed and measured upon a wide range of varying laser parameters including pulse energy, repetition rate, pulse duration, writing speed, and laser polarization. A similar analysis was performed in silica glass (Suprasil CG) taken as a reference. We measured retardance values as high as 100 nm in the aluminosilicate glass, which is approximately 2x higher than previously investigated aluminosilicate glasses. Raman spectroscopy and electron microscopy techniques revealed the presence of an orientable lamellar structure, commonly referred to as nanogratings, composed of alternate SiO2-enriched amorphous layers with Al2O3-enriched ones. The latter are essentially crystallized in a 3Al2O3:2SiO2 Mullite phase. This internal structuring, the first one in a congruent glass, brings additional insights into the mechanisms leading to nanogratings formation, and may be proved useful for future glass-based functional optical devices with very large thermal stability.

Processing and cytocompatibility of Cu-doped and undoped fluoride-containing bioactive glasses

Sintered or additive-manufactured bioactive glass (BG) scaffolds are highly interesting for bone replacement applications. However, crystallization often limits the high-temperature processability of bioactive glasses (BGs). Thus, the BG composition must combine high bioactivity and processability. In this study, three BGs with nominal molar (%) compositions 54.6SiO2-1.7P2O3-22.1CaO-6.0Na2O-7.9K2O-7.7MgO (13–93), 44.8SiO2-2.5P2O3-36.5CaO-6.6Na2O-6.6K2O-3.0CaF2 (F3) and 44.8SiO2-2.5P2O3-35.5CaO-6.6Na2O-6.6K2O-3.0CaF2-1.0CuO (F3–Cu) were investigated. The dissolution and ion release kinetics were investigated on milled glass powder and crystallized particles (500–600 μm). All glasses showed the precipitation of hydroxyapatite (HAp) crystals after 7 days of immersion in simulated body fluid. No significant differences in ion release from glass and crystalline samples were detected. The influence of surface roughness on cytocompatibility and growth of pre-osteoblast cells (MC3T3-E1) was investigated on sintered and polished BG pellets. Results showed that sintered BG pellets were cytocompatible, and cells were seen to be well attached and spread on the surface after 5 days of incubation. The results showed an inverse relation of cell viability with the surface roughness of pellets, and cells were seen to attach and spread along the direction of scratches.

Static state synthesis of STT zeolite membranes for high-pressure H2/CH4 separation

STT zeolite membrane with seven-membered rings (7 MR) and nine-membered rings (9 MR) is an ideal alternative for the separation of hydrogen (H2) and methane (CH4). However, the successful synthesis is only possible in rotation conditions, which is difficult to achieve at an industrial scale. Herein we developed a static synthesis approach to prepare high-quality STT zeolite membranes. The precursor transformed in-situ from a liquid state to a semi-solid state to efficiently suppress the nucleation in the bulk gel. This did not affect the growth of the seed layer to form a continuous membrane. The water content was modulated between y = 44 and y = 124 in the molar composition of 1 SiO2: 0.2 TMAdaOH: y H2O. The precursor could be re-used one more time to reduce the total amount of chemical waste. The optimal H2 permeance and H2/CH4 mixture selectivity was up to 6.1 × 10−8 mol m−2 s−1 Pa−1 and 115 at atm pressure. The H2 permeation flux monotonically increased to 2.0 Nm3 m−2 h−1 under feed pressure up to 2.1 MPa. This paves the way for zeolite membranes to high-pressure H2 separation in practical applications.

In-situ approach to porous nitrogen-doped carbon nanosheets functionalized by Brønsted acidic ionic liquids for microwave-assisted upgrading fructose to 5-hydroxymethylfurfural

In the search for robust and recoverable supported Brønsted acidic ionic liquids (BAILs) catalysts for efficient upgrading bio-sugars to value-added chemicals, an in-situ strategy of supramolecular preorganization-thermal polycondensation is designed to fabricate porous ultrathin nitrogen-doped carbon nanosheets (NCNSs), and then BAILs-functionalized NCNSs catalysts are prepared via successive quaternary ammonization by sultones and anion exchange with Brønsted acids. By adjusting the molar composition of the starting monomers, the textural properties of NCNSs supports are tuned; and by functionalization with different sultones (1,3-propanesultone and 1,4-butanesultone) and organic (trifluoromethanesulfonic acid and p-toluenesulfonic acid) or inorganic (H2SO4 and H3PO4) acids, the surface hydrophobicity and Brønsted acid strength of the catalysts are regulated. The catalysts are applied in microwave-assisted upgrading fructose to 5-hydroxymethylfurfural, and influences of Brønsted acid nature, surface hydrophobicity and textural properties on the catalytic performance are explored. For the most active [C4SO3HN][OTf]-NCNSs-MA-3 catalyst with the advantages of superstrong Brønsted acidity, higher surface hydrophobicity and perfect porous ultrathin sheet-like nanostructure, the conversion of fructose and the yield of 5-hydroxymethylfurfural of 100% and 87.7% are achieved after microwave irradiation for 15 min, outperforming Amberlyst-15 resin and HY zeolite. The catalysts also demonstrate the robust catalytic reusability, and after five consecutive catalytic runs, the obvious activity loss hardly occurs, along with little acid sites leaching.

How Do Deep Eutectic Solvents Form Porous Liquids? The Example of Methyltriphenylphosphonium Bromide: Glycerol and ZIF-8.

Porous liquids are new materials that provide permanent porosity in the liquid phase through the dispersion of nanoporous solid particles in a bulky solvent. Herein, we aim at understanding how new sustainable solvents such as deep eutectic solvent (DES) can be used to form porous stable suspensions for the capture of gases of interest for sustainable chemistry. The properties of an ionic DES, methyltriphenylphosphonium bromide/glycerol in a 1:3 molar composition, and its behavior at the interface with a metal-organic framework (MOF), ZIF-8, are here investigated by polarizable molecular dynamics simulations. The structural and dynamic properties of the DES are analyzed in the bulk liquid and in the interfacial regions with the MOF, namely, in the accessible cavities exposed at the surface. The porosity of the suspension is maintained, and it is caused not only by the Coulomb cohesive energy between cations and anions, which prevents the small anions from entering the pores, but also by the glycerol molecules not penetrating the small aperture of the ZIF-8 structure. This was further verified by simulating a system composed of glycerol and ZIF-8. Simulations with CO2 show its partition between the DES and the MOF, with higher concentrations registered in the MOF cavities.

Selective Replacement of Cholesterol with Cationic Amphiphilic Drugs Enables the Design of Lipid Nanoparticles with Improved RNA Delivery.

The delivery of RNA across biological barriers can be achieved by encapsulation in lipid nanoparticles (LNPs). Cationic amphiphilic drugs (CADs) are pharmacologically diverse compounds with ionizable lipid-like features. In this work, we applied CADs as a fifth component of state-of-the-art LNPs via microfluidic mixing. Improved cytosolic delivery of both siRNA and mRNA was achieved by partly replacing the cholesterol fraction of LNPs with CADs. The LNPs could cross the mucus layer in a mucus-producing air-liquid interface model of human primary bronchial epithelial cells following nebulization. Moreover, CAD-LNPs demonstrated improved epithelial and endothelial targeting following intranasal administration in mice, without a marked pro-inflammatory signature. Importantly, quantification of the CAD-LNP molar composition, as demonstrated for nortriptyline, revealed a gradual leakage of the CAD from the formulation during LNP dialysis. Altogether, these data suggest that the addition of a CAD prior to the rapid mixing process might have an impact on the composition, structure, and performance of LNPs.

Intermolecular Interactions of Binary Mixtures Comprising 2‐Benzylaminoethanol with Alcohols (C1−C3) at Different Temperatures: Experiments and Modelling

AbstractThis manuscript represents the physical quantities comprising the densities, speed of sound and refractive indices for the binary mixtures involving [2‐Benzylaminoethanol (BAE) with methanol, ethanol, 1‐propanol, or 2‐propanol] over a molar composition (xBAE=0–1). The measurements were conducted with the use of Anton Paar densimeter (DSA 5000 M) operated at different temperatures, T=(293.15–323.15) K and at atmospheric pressure. The intermolecular interactions occurring between the prepared binary mixtures were interpreted by computing the excess properties including excess molar volumes ( ), isentropic compressibilities ( ), intermolecular free length ( ), specific acoustic impedance ( ), relative association ( , relaxation strength ( ), and Rao's molar sound function ( ). The Redlich‐Kister polynomial equation was utilized to fit the computed excess properties and PC‐SAFT EoS was utilized for modeling the measured densities. In addition, the Laplace mixing rule as well as the Nomoto's relation were utilized for the modeling of refractive indices and speed of sound, respectively. The experimental data was found in good agreement with the theoretical data for the measured properties.

Effects of Assisting Solvents on Purification Efficiency in the Layer Melt Crystallization of Glycerol.

The efficiency of layer melt crystallization for the selective separation of glycerol from a glycerol-diethylene glycol mixture containing 4 wt % of diethylene glycol was evaluated using solvent-free and solvent-aided approaches. The effect of 1-butanol and the binary solvent of 1-butanol and acetone with a total molar composition of 25 mol % on the crystal growth kinetics and the purity of the final product was studied at different undercooling degrees and crystallization yields. The melting point temperature of the mixtures was predicted by using the modified UNIFAC Dortmund model. The addition of both a single and binary solvents significantly increased the crystal growth rate and purity of the final product compared to crystallization from the solvent-free mixture. Additionally, higher crystal growth rates and product purity were observed in the binary solvent system compared to those in the single solvent system at the same degree of undercooling. The second stage of solvent-aided crystallization resulted in glycerol with a purity above 99.5 wt %, depending on the type of solvent used and the rate of crystal growth.

Multivariate Analysis of Cellular Uptake Characteristics for a (Co)polymer Particle Library.

Controlling cellular responses to nanoparticles so far is predominantly empirical, typically requiring multiple rounds of optimization of particulate carriers. In this study, a systematic model-assisted approach should lead to the identification of key parameters that account for particle properties and their cellular recognition. A copolymer particle library was synthesized by a combinatorial approach in soap free emulsion copolymerization of styrene and methyl methacrylate, leading to a broad compositional as well as constitutional spectrum. The proposed structure-property relationships could be elucidated by multivariate analysis of the obtained experimental data, including physicochemical characteristics such as molar composition, molecular weight, particle diameter, and particle charge as well as the cellular uptake pattern of nanoparticles. It was found that the main contributors for particle size were the polymers' molecular weight and the zeta potential, while particle uptake is mainly directed by the particles' composition. This knowledge and the reported model-assisted procedure to identify relevant parameters affecting particle engulfment of particulate carriers by nonphagocytic and phagocytic cells can be of high relevance for the rational design of pharmaceutical nanocarriers and assessment of biodistribution and nanotoxicity, respectively.