Charged Poly Research Articles

Molecular Thermodynamics of Complex Coacervate Systems. Part I: Modeling of Polyelectrolyte Solutions using pePC-SAFT.

Rigorous molecular modeling of polyelectrolyte solutions is complicated by several intrinsic challenges of those systems, such as the strong charge correlation and the complex cocktail of short-range and long-range interactions, which span over a broad length scale. On the other hand, there is an increasing interest in understanding and designing polyelectrolyte systems in biology, life science, medicine, and (bio)chemical engineering. Thermodynamics of polyelectrolyte solutions is rather underexplored, and the difficulties in describing polyelectrolytes at the molecular level as well as the lack and the uncertainty of experimental data might have hindered the development of accurate thermodynamic models for polyelectrolytes. In this work, the main phenomena of counterion condensation, complex formation and coacervate formation are discussed and considered for the further development of polyelectrolyte PC-SAFT (pePC-SAFT) as modeling framework in this work. The new development was then validated using experimental osmotic coefficients of aqueous polyelectrolyte solutions. Finally, liquid-liquid phase separation (LLPS) of complex coacervate systems (aqueous solutions containing oppositely charged polyions) were modeled with pePC-SAFT, and the results were in very good agreement with literature data.

Multifunctional composite phase change material with electrostatic self-assembly structure based on carboxylated multi-walled carbon nanotubes

The need for improved thermal regulation in electronic devices and solar thermal energy storage, prompted by the energy crisis, has expedited the advancement of phase change materials (PCMs). Carboxylated multi-walled carbon nanotubes (MWCNT-COOH) were produced by introducing carboxyl functional groups onto MWCNTs utilizing a concentrated acid treatment. The novel composite was engineered through an electrostatic self-assembly process between the negatively charged MWCNT-COOH and the positively charged Poly dimethyl diallyl ammonium chloride (PDDA) solution, filling the structure with the PCM polyethylene glycol (PEG) and incorporating the (magnesium hydrate) Mg(OH)2 to enhance the material's flame resistance at high temperatures. The thermal conductivity of the obtained composites improved significantly from 0.25 W/m·K to 1.183 W/m·K, while maintaining an enthalpy of phase transition of phase change of 135.1 J/g. Owing to the capillary effect of the closely packed MWCNT-COOH tubular structure, the composite material exhibited excellent high-temperature shape retention ability. Additionally, the composite demonstrated high absorption with an absorbance reaching 1.18 L/(g·cm) and composite materials can convert up to 86.8 % of light energy into heat energy.

High rate capability and ultra‐long cycling life: Electrochemical synthesis of PEDOT based electrode material doped with AMPS and its supercapacitor application

AbstractPoly(3,4‐ethylene dioxythiophene) (PEDOT) is a conducting polymer that can be used in flexible bioelectronic devices. The electrode/electrolyte interface interaction is one of the most important factors in improving the electrochemical performance of energy storage materials, and these polymers are often combined with a negatively charged poly(styrene sulfonate) (PSS) chain to improve their interaction with alkali metal cations such as sodium and potassium. In this work, we performed a one‐step electrochemical synthesis of PEDOT on carbon fabric using the molecule 2‐acrylamido‐2‐methyl‐1‐propane sulfonic acid (AMPS) to create highly effective materials for supercapacitor electrodes. The electrode had a significant increase in capacitance value, measured 16.4 times higher than that of the PEDOT electrode. The 2‐electrode system exhibited a specific capacitance value of 495.2 F g−1 at a scan rate of 5 mV s−1. It exhibited a high operating voltage of 2.3 V in aqueous electrolyte system. It showed a significant energy density of 109.0 Wh kg−1 when operating at 6.1 kW kg−1 power density and 85.2 Wh kg−1 when operating at 30.6 kW kg−1 power density. Recent findings reveal that the capacitance retention performance value of the device increased significantly to 113.9% after 25,000 cycles in 3.0 M NaCl aqueous electrolyte, demonstrating its outstanding long‐term durability. Thus, the creation of the synthesized supercapacitor electrode is a significant advance in the study of conducting polymers, which often have a limited lifetime in real‐world electronic applications.

Electrochemical detection of sulfite using gold nanoparticles decorated poly[2-(methacryloyloxy) ethyl] trimethylammonium chloride: kinetic and mechanistic studies

Abstract Given the widespread use of sulfites in various industries and their potential environmental and health impacts, accurate and efficient detection is crucial. The deployment of positively charged poly [2-(methacryloyloxy) ethyl] trimethylammonium chloride (PMTC) decorated with gold nanoparticles (AuNPs) offers a novel approach, enhancing sensitivity and specificity in the electrochemical detection of negatively charged sulfite ions (SO32-). A sensor for detecting SO32- was developed using PMTC decorated with AuNPs on a glassy carbon electrode (GCE). Transmission electron microscopy (TEM) was employed to examine the structural morphology of the composite material, and the formation of AuNPs was confirmed through ultraviolet-visible spectroscopy. Zeta potential analysis affirmed the positive charge of the PMTC composite, highlighting its effective coordination with the negatively charged SO32-. The surface conductivity of the modified GCE was studied using electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). Kinetic analyses, focusing on scan rate and pH dependencies, elucidated the SO32- oxidation dynamics and the interaction between the positively charged PMTC and negatively charged SO32-. Quantitative evaluation was performed using the current-time (I-t) technique, achieving a limit of detection of 0.41 ± 0.003 µM (S/N = 3) within a linear range of 6.66 µM to 1020 µM. The modified electrode demonstrated remarkable stability, repeatability, and resistance to common interferents. Real sample analysis using laboratory tap water with a fixed SO32- concentration exhibited excellent recovery. The oxidation of SO32- on the AuNPs-PMTC-GCE proceeded via first-order kinetics and followed a stepwise pathway facilitated by the charge interactions.

Two Methods Based on Integral Equation Approaches in Analyzing Polyelectrolyte Solutions: Macrophase Separation.

To understand the phase behaviors of polyelectrolyte solutions, we provide two analytical methods to formulate a molecular equation of state for a system of fully charged polyanions (PAs) and polycations (PCs) in a monomeric neutral component, based on integral equation theories. The mixture is treated in a primitive and restricted manner. The first method utilizes Blum's approach to charged hard spheres, incorporating the chain connectivity contribution by charged spheres via Stell's cavity function method. The second method employs Wertheim's multi-density Ornstein-Zernike treatment of charged hard spheres with Baxter's adhesive potential. The pressures derived from these methods are compared to available molecular dynamics simulations data for a solution of PAs and monomeric counterions as a limiting case. Two-phase equilibrium for the system is calculated using both methods to evaluate the relative strength of phase segregation that leads to complex coacervation. Additionally, the scaling exponents for a selected solution near its critical point are examined.

EFFECT OF CHITOSAN CONCENTRATION ON PHYSICAL CHARACTERISTICS OF EXTRACT ETHANOLIC OF BAY LEAF (Syzygium polyanthum) NANOPARTICLE PREPARED BY CROSS-LINKING METHODS

Chitosan is a natural cationic polysaccharide that could form bonds with negatively charged polyanions like sodium tripolyphosphate (STPP) as a crosslinker. One of the important factors to develop nanoparticles is the concentration of polymer. The increased polymer concentration will increase the viscosity of the solution formed, and the size of the nanoparticles created will increase. However, if the amount of polymer is too small, the particles formed are smaller, and aggregation could be formed. In this study, the ethanolic extract of bay leaf (Syzygium polyanthum) was used as a drug that has a potent anti-dyslipidemia effect by lowering cholesterol and triglyceride levels. Studies on the ethanolic extract of a bay leaf as an anti-dyslipidemia are still limited. The objective of this research was an investigate effect of the chitosan concentration used 0.6 mg/ml (F1); 1mg/ml (F2); and 1.4 mg/ml (F3) on the physical characteristics of ethanolic extract of bay leaf (Syzygium polyanthum) nanoparticles (NSPs) prepared by cross-linking methods. The result of particle size evaluation showed that the particle size was 665.1 nm ± 14.71 (F1); 180.1 nm ± 0.5; and 221.35 nm ± 1.91 (F3), while the polydispersity index F1, F2, and F3 were 0.773 ± 0.152; 0.220 ± 0.016; and 0.212 ± 0.024 respectively. The results of this study found F2 was the most optimal chitosan concentration with particle size under 200 nm, and polydispersity index under 0.5 with positive ζ-potential value. In conclusion, chitosan concentration showed has an effect on the physical characteristics of the nanoparticles.

Emulsion Stabilized by Biocompatible and Stimuli-Responsive Poly(N-vinylcaprolactam)-Based Microgels: Effects of Electrostatic Repulsion and Deformability on Emulsion Stability.

Microgels have been widely used for stabilizing emulsions due to their softness and stimulus responsiveness. Although ultrastable emulsions have been prepared by microgel nanoparticles, the role of electrostatic interactions on emulsion stability is still a controversial topic and further investigation of the effect of microgel deformability is required. In the present study, neutral poly(N-vinylcaprolactam) (PVCL) and charged poly(N-vinylcaprolactam)-co-methacrylic acid (P(VCL-co-MAA)) microgels were synthesized and further used as emulsifiers to stabilizing emulsion. The P(VCL-co-MAA) microgel has a swelling ratio larger than that of the PVCL microgel in water. The nanomechanical properties of the microgels in water were characterized by atomic force microscopy with using the tip of different radii. The result reveals that the P(VCL-co-MAA) microgel is more deformable than the PVCL counterpart. Stability tests of the emulsions showed that below the volume phase transition temperature (VPTT) of the microgels, both microgel types can stabilize the emulsions under various conditions. Unexpectedly, most of the emulsions still remain stable above the VPTT. Further increasing the temperature to 60 °C, P(VCL-co-MAA) microgel emulsions remained stable at a pH value above the pKa of MAA while the emulsion was unstable below the pKa. However, phase separation occurs in PVCL microgel-stabilized emulsions at 60 °C. These results demonstrate that electrostatic repulsion and deformability of the microgels can enhance the emulsion stability, providing insights into the rational design and preparation of ultrastable Pickering emulsions.

Enzyme‐Responsive Polyion Complex Nanoparticles of Cationic Antimicrobials for Activatable Antibacterial Therapy

AbstractA self‐assembled “caging” strategy is presented for the safe delivery of potent cationic antimicrobials that suffer from non‐specific toxicity for the effective treatment of in vivo systemic bacterial infection. The key development here is a new block copolymer consisting of a poly(ethylene glycol) (PEG) stealth block and an anionic and lipase‐degradable block of poly(ɛ‐caprolactone) (PCL) and phosphonic acid‐bearing methacrylate copolymer, synthesized by hybrid copolymerization of methacrylate and cyclic esters. The anionic blocks electrostatically interact with cationic antimicrobials to form neutrally charged polyion complexes with the PEG blocks on the surface. The PCL component imparts the nanocomplex with biodegradability by bacterial secretory lipase. In the proof‐of‐concept study, cationic polyimidazolium that shows excellent antibacterial activity but severe toxicity is packaged by the block copolymer into nanocomplexes, which are stable in complex environments of high salt and protein concentrations and released the antimicrobials upon degradation of the copolymer by bacteria‐secreted lipase. The “caging” formulation of polyimidazolium eliminated its toxicity and led to highly effective bactericidal performance comparable to free polyimidazolium. This caging strategy does not require sophisticated chemical modification of cationic antimicrobials, offering a broadly applicable formulation strategy to overcome their common toxicity issue that has become a primary translational barrier.

Dynamic Ion Gels from the Complex Coacervation of Oppositely Charged Poly(ionic liquid)s.

A cationic poly(ionic liquid) (PIL) with pendent butyl imidazolium cations and free bis(trifluoromethylsulfonyl)imide (TFSI) anions and an anionic PIL with pendent TFSI anions and free 1-butyl-3-methylimidazolium cations are synthesized by postpolymerization chemical modification and reversible addition-fragmentation chain-transfer radical copolymerization, respectively. Upon mixing solutions of these two PILs in acetone with stoichiometric amounts of ion pairs, ionic exchanges induce coacervation and, after solvent evaporation, lead to the formation of a dynamic ion gel (DIG) and the concomitant release of free [1-methyl-3-butyl imidazolium]TFSI ionic liquid (IL). A comparison of thermal (Tg), ion conducting (σDC), and viscoelastic (elastic moduli (G')) properties for DIGs and their parent polyelectrolytes, as well as extracted and IL-doped DIGs, demonstrates the formation of ionic cross-links and the ability to easily produce polymer electrolytes with enhanced ionic conductivity (σDC up to 4.5 × 10-5 S cm-1 at 30 °C) and higher elastic moduli (G' up to 4 kPa at 25 °C and 1 rad s-1), making them highly desirable in many electrochemical applications, including supercapacitors, soft robotics, electrochromic devices, sensors, and solar cells.

Aggregation of positively charged poly(methyl methacrylate) latex particles in the presence of trifluoromethanesulfonate anion

Abstract We investigated the unique aggregation behavior of 3 types of positively charged poly(methyl methacrylate) (PMMA) latex particles in the presence of a trifluoromethanesulfonate (triflate) anion. The particles were prepared based on surfactant-free emulsion polymerization using azo radical initiators. The triflate anion was strongly adsorbed to surfaces of positively charged PMMA latex particles, as confirmed by electrophoresis. Additionally, its presence significantly reduced the critical coagulation concentration of the cationic PMMA latex particles compared with other anions.

Poly(l-threonine-co-l-threonine Succinate) Thermogels for Sustained Release of Lixisenatide.

Negatively charged poly(l-Thr-co-l-Thr succinate) (PTTs) was developed as a new thermogel. Aqueous PTT solutions underwent thermogelation over a concentration range of 6.0-8.3 wt %. Dynamic light scattering, FTIR, 1H NMR, and COSY spectra revealed the partial strengthening of the β-sheet conformation and the dehydration of PTTs during the transition. Extendin-4 was released from the PTTs thermogel with a large initial burst release, whereas positively charged lixisenatide significantly reduced its initial burst release to 25%, and up to 77% of the dose was released from the gel over 14 days. In vivo study revealed a high plasma concentration of lixisenatide over 5 days and hypoglycemic efficacy was observed for type II diabetic rats over 7-10 days. The biocompatible PTTs were degraded by subcutaneous enzymes. This study thus demonstrates an effective strategy for reducing the initial burst release of protein drugs from thermogels with the introduction of electrostatic interactions between the drug and the thermogel.

Late-Stage Desulfurization Enables Rapid and Efficient Solid-Phase Synthesis of Cathepsin-Cleavable Linkers for Antibody-Drug Conjugates.

The synthesis of linker-payloads is a critical step in developing antibody-drug conjugates (ADCs), a rapidly advancing therapeutic approach in oncology. The conventional method for synthesizing cathepsin B-labile dipeptide linkers, which are commonly used in ADC development, involves the solution-phase assembly of cathepsin B-sensitive dipeptides, followed by the installation of self-immolative para-aminobenzyl carbonate to facilitate the attachment of potent cytotoxic payloads. However, this approach is often low yield and laborious, especially when extending the peptide chain with components like glutamic acid to improve mouse serum stability or charged amino acids or poly(ethylene glycol) moieties to enhance linker hydrophilicity. Here, we introduce a novel approach utilizing late-stage desulfurization chemistry, enabling safe, facile, and cost-effective access to the cathepsin B-cleavable linker, Val-Ala-PABC-MMAE, on resin for the first time.

Surface charge engineering for structural control of colloidal silica rod-decorated silica particles and their flexible integration into magnetic core–multishell structures

In this study, the effect of surface modification and the resulting surface charge of colloidal silica seeds on the growth of silica rods during an emulsion droplet-based process is investigated. Through electrostatic interactions between negatively charged poly(vinylpyrrolidone) (PVP) and seed surfaces, significant PVP adsorption occurs as the seed surfaces are modified with positively charged cationic substances and then aged with PVP. This surface charge-enhanced PVP adsorption promotes the anchoring of water emulsion droplets, serving as the starting point for the growth of silica rods on the seed surfaces and leading to a high yield of silica rod-decorated particles during emulsion droplet-based growth. The surface properties, including surface charge and hydrophobicity, can be further modified by applying different cationic modifiers, which influence the morphology, structural architecture, and yield of the final product. We further demonstrated the versatility of this approach by successfully generating silica rod-decorated magnetic core (Fe3O4)–multishell (silica/polystyrene/titania) particles. The findings of this study highlight the critical role of surface charge engineering in controlling the structure and morphology of silica rod-decorated silica particles as well as their integration into complex multicomponent systems.

PARP1 interacts with WDR5 to enhance target gene recognition and facilitate tumorigenesis

Poly (ADP-ribose) polymerase-1 (PARP1) is a nuclear protein that attaches negatively charged poly (ADP-ribose) (PAR) to itself and other target proteins. While its function in DNA damage repair is well established, its role in target chromatin recognition and regulation of gene expression remains to be better understood. This study showed that PARP1 interacts with SET1/MLL complexes by binding directly to WDR5. Notably, although PARP1 does not modulate WDR5 PARylation or the global level of H3K4 methylation, it exerts locus-specific effects on WDR5 binding and H3K4 methylation. Interestingly, PARP1 and WDR5 show extensive co-localization on chromatin, with WDR5 facilitating the recognition and expression of target genes regulated by PARP1. Furthermore, we demonstrated that inhibition of the WDR5 Win site impedes the interaction between PARP1 and WDR5, thereby inhibiting PARP1 from binding to target genes. Finally, the combined inhibition of the WDR5 Win site and PARP shows a profound inhibitory effect on the proliferation of cancer cells. These findings illuminate intricate mechanisms underlying chromatin recognition, gene transcription, and tumorigenesis, shedding light on previously unrecognized roles of PARP1 and WDR5 in these processes.

Enhanced Catalytic Activity of a de novo Enzyme in a Coacervate Phase

Biomolecular condensates are membraneless organelles that orchestrate various metabolic pathways in living cells. Understanding how these crowded structures regulate enzyme reactions remains yet challenging due to their dynamic and intricate nature. Coacervate microdroplets formed by associative liquid‐liquid phase separation of oppositely charged polyions have emerged as relevant condensate models to study enzyme catalysis. Enzyme reactions within these droplets show altered kinetics, influenced by factors such as enzyme and substrate partitioning, crowding, and interactions with coacervate components; it is often challenging to disentangle the contributions of each. Here, we investigate the peroxidase activity of a de novo enzyme within polysaccharide‐based coacervates. By comparing the reaction kinetics in buffer, in a suspension of coacervates and in the bulk coacervate phase collected after centrifugation of the droplets, we show that the coacervate phase significantly increases the enzyme catalytic efficiency. We demonstrate that the main origin of this enhanced activity lies in macromolecular crowding coupled to changes in the conformational dynamics of the enzyme within the coacervate environment. Altogether, these findings underline the crucial role of the coacervate matrix in enzyme catalysis, beyond simple partitioning effects. The observed boost in enzyme activity within the coacervate phase provides insights for designing biocatalytically active synthetic organelles.

Tuning physicomechanical properties of PEG-interpenetrated anionically modified semi-IPN cryogels functionalized with carboxylate groups

Anionically modified interpenetrated polymer network (semi-IPN) cryogels containing linear polyethylene glycol chains (PEG) were prepared via in situ synthesis and directed assembly of the negatively charged copolymer poly(acrylamide-co-sodium acrylate) (PAN) network template. The influence of reaction conditions; the concentration of linear PEG chains, and polymerization temperature on the elasticity and swelling of these IPNs was analyzed in detail. The interpenetrating structure of PEG chains and PAN host network have been confirmed by FTIR, TGA and XRD analysis. The equilibrium water content, oscillatory swelling/deswelling kinetics, and water transport mechanism were analyzed as a function of PEG content. The results showed that semi-IPN gels exhibited different swelling behavior as the reaction conditions varied. Addition of 13.9% (w/v) PEG resulted in a 25-fold increase in the swelling ratio of semi-IPN hydrogels. By performing compression tests on semi-IPN gels to determine the change of compression properties, the effective cross-linking density of semi-IPN PAN/PEG was expressed as a second-order polynomial depending on the amount of PEG. The swollen modulus of semi-IPN cryogels was much higher than that of semi-IPN hydrogels for all PEG concentrations. Semi-IPNs showed reversible on-off switching with remarkable sensitivity to external pH stimulus. Structural parameters, degree of swelling, volume fraction of cross-linked polymer in the swollen state, and diffusion coefficients due to pH-induced swelling of semi-IPN gels were determined. The presence of linear PEG chains in the structure promoted swelling by both increasing the swelling rate and significantly reducing the time required to reach the equilibrium-state. The swelling process was Fickian diffusion, and the diffusion coefficients for swelling of PEG-interpenetrated semi-IPNs increased with PEG content. The effectiveness of removing methylene blue (MB) dye from aqueous solutions by semi-IPNs was evaluated. Batch adsorption experiments were performed as a function of the gelation temperature, amount of PEG, contact time, and initial dye concentration. The adsorption isotherm and kinetics were described well by Langmuir isotherm model and pseudo-second-order model, respectively. Adsorption of MB was a multi-step process involving surface adsorption followed by intra-particle diffusion. Semi-IPN PAN/PEG cryogels prepared under cryocondition with high adsorption capacities and fast adsorption rates have been developed as new adsorbents effective in removing dyes and other toxic substances with higher mechanical strength in water and wastewater treatment.

Versatile cationic dual-layer hydrogel filtration system for sustainable solar steam generator

Our increasing water demand has been an ongoing critical challenge due to water usages in areas such as industrial, agriculture, and domestic household. Conventional water production faces challenges, such as high investment, energy consumption, and brine discharge that may be unsustainable in the future. Solar steam generation (SSG) has been recently proposed by many researchers due to their sustainable and green water production method. Here we demonstrated the use of simple manufacturing and low-cost dual-layer hydrogel (DLH) system containing a double network of positive charged poly-[2-(acryloyloxy)ethyl] trimethyl ammonium chloride (PAETAC) and polyvinyl alcohol (PVA) bottom layer for fast water transport, as well as a broad light absorbing and heat generating PVA/graphene oxide (GO) top layer for fast water evaporation. As a result, the DLH was able to generate a high 3.12 kg m−2 h−1 water evaporation with 92% efficiency under 1 sun (kW m−2) exposure. Furthermore, this DLH design allows for a safe and passive anti-salt and bacterial property due to PAETAC cationic chain, eliminating 99% salt and bacteria via Donnan repulsion and electrostatic interaction without the need of sunlight exposure.

A Dual Fluorescence Turn-On Sensor Array Formed by Poly(para-aryleneethynylene) and Aggregation-Induced Emission Fluorophores for Sensitive Multiplexed Bacterial Recognition.

Bacterial infections have emerged as the leading causes of mortality and morbidity worldwide. Herein, we developed a dual-channel fluorescence "turn-on" sensor array, comprising six electrostatic complexes formed from one negatively charged poly(para-aryleneethynylene) (PPE) and six positively charged aggregation-induced emission (AIE) fluorophores. The 6-element array enabled the simultaneous identification of 20 bacteria (OD600=0.005) within 30s (99.0 % accuracy), demonstrating significant advantages over the array constituted by the 7 separate elements that constitute the complexes. Meanwhile, the array realized different mixing ratios and quantitative detection of prevalent bacteria associated with urinary tract infection (UTI). It also excelled in distinguishing six simulated bacteria samples in artificial urine. Remarkably, the limit of detection for E. coli and E. faecalis was notably low, at 0.000295 and 0.000329 (OD600), respectively. Finally, optimized by diverse machine learning algorithms, the designed array achieved 96.7 % accuracy in differentiating UTI clinical samples from healthy individuals using a random forest model, demonstrating the great potential for medical diagnostic applications.

A Dual Fluorescence Turn‐On Sensor Array Formed by Poly(para‐aryleneethynylene) and Aggregation‐Induced Emission Fluorophores for Sensitive Multiplexed Bacterial Recognition

AbstractBacterial infections have emerged as the leading causes of mortality and morbidity worldwide. Herein, we developed a dual‐channel fluorescence “turn‐on” sensor array, comprising six electrostatic complexes formed from one negatively charged poly(para‐aryleneethynylene) (PPE) and six positively charged aggregation‐induced emission (AIE) fluorophores. The 6‐element array enabled the simultaneous identification of 20 bacteria (OD600=0.005) within 30s (99.0 % accuracy), demonstrating significant advantages over the array constituted by the 7 separate elements that constitute the complexes. Meanwhile, the array realized different mixing ratios and quantitative detection of prevalent bacteria associated with urinary tract infection (UTI). It also excelled in distinguishing six simulated bacteria samples in artificial urine. Remarkably, the limit of detection for E. coli and E. faecalis was notably low, at 0.000295 and 0.000329 (OD600), respectively. Finally, optimized by diverse machine learning algorithms, the designed array achieved 96.7 % accuracy in differentiating UTI clinical samples from healthy individuals using a random forest model, demonstrating the great potential for medical diagnostic applications.

Unraveling mechanisms of protein encapsulation and release in coacervates via molecular dynamics and machine learning.

Coacervates play a pivotal role in protein-based drug delivery research, yet their drug encapsulation and release mechanisms remain poorly understood. Here, we utilized the Martini model to investigate bovine serum albumin (BSA) protein encapsulation and release within polylysine/polyglutamate (PLys/PGlu) coacervates. Our findings emphasize the importance of ingredient addition sequence in coacervate formation and encapsulation rates, attributed to preference contact between oppositely charged proteins and poly(amino acid)s. Notably, coacervates composed of β-sheet poly(amino acid)s demonstrate greater BSA encapsulation efficiency due to their reduced entropy and flexibility. Furthermore, we examined the pH responsiveness of coacervates, shedding light on the dissolution process driven by Coulomb forces. By leveraging machine learning algorithms to analyze simulation results, our research advances the understanding of coacervate-based drug delivery systems, with the ultimate goal of optimizing therapeutic outcomes.