pH-responsive Properties Research Articles

PH-induced fluorescent active sodium alginate-based ionically conjugated and REDOX responsive multi-functional microgels for the anticancer drug delivery

A sodium alginate (Alg) based REDOX (reduction and oxidation)-responsive and fluorescent active microgel was prepared via water in oil (w/o) mini-emulsion polymerization technique. Here, we initially synthesized sodium alginate-based disulfide cross linked microgels and after that those microgels were tagged with rhodamine amine derivative (RhB-NH2) by ionic interaction to get the pH-responsive fluorescent property. Functionalized microgels were characterized using 1H NMR, FTIR, DLS, HRTEM, FESEM, UV–vis, and fluorescence spectroscopy analyses. Presence of the REDOX-responsive disulfide-containing crosslinkers in the microgels enhances the release of doxorubicin (DOX), an anti-cancer drug in the reducing environment of the cancer-cells (simulated). Existence of the rhodamine-amine derivative in the microgels triggers the pH-dependent fluorescence property by showing fluorescence emission at 560–580 nm at pH 5.5 (cancer cell pH). The cytotoxicity of the biopolymer based microgel was assessed over both cancerous HeLa (IC50 100 µg/mL) and non-cancerous MDCK (IC50 200 µg/mL) cells by MTT assay which showed the synthesized microgel is non-toxic whereas DOX-loaded microgels showed significant toxicity. FACS and cell uptake (in vitro) analyses were conducted to understand the cell apoptosis cycle and behavior of the cancer cells in presence of the DOX-loaded microgels. This pH-responsive fluorescent active alginate-based biomaterial could be a promising material for the anti-cancer drug delivery and other medical fields.

Enhancing camptothecin loading and release control through physical surface modification of organosilica nanoparticles with polyethylene glycol

The surface modification of nanoparticles holds the potential to enhance the loading capacity of drug molecules and regulate their release, making it possible to exploit the differences between tumor and normal cells. To this end, the surfaces of tetrasulfide-based phenylene-containing biodegradable periodic mesoporous organosilica (BPMO) nanoparticles (designated P4S) are modified herein with a hydrophilic and biocompatible polyethylene glycol (PEG) polymer. The PEG coating is optimized by adjusting the PEG concentration during synthesis, thus resulting in a significant increase in the nanoparticle stability. Furthermore, PEG modification enhances the nanoparticles' camptothecin (CPT) loading capacity. Drug release assessments under physical and acidic pH conditions demonstrate the pH-responsive properties of the P4S nanoparticles upon PEG functionalization, which results in increased drug release at low pH, along with enhanced cellular uptake potential. Notably, the cytotoxicity of CPT against HepG2 cancer cells is significantly improved when loaded into the P4S-PEG nanoparticles. These findings reveal the efficacy of PEG surface modification of the drug-delivery material in augmenting the activity of CPT, with promising prospects for clinical applications.

ZIF-8-mediated block copolymer micelles and its application in drug delivery

Block copolymer micelles have been widely used in drug delivery. Great efforts have been made to optimize the function of block copolymer micelles and further enhance their bioavailability. We propose a means of embedding ZIF-8 in block copolymer micelles to regulate its stability for improving the drug release kinetics. The block copolymer poly (2-(diisopropyl amino-ethyl methacrylate)-block-poly (vinylimidazole-co-poly (ethylene glycol) methyl methacrylate) (PDPA18-b-P(Vim18-co-P(EG)5MA21) (PDPV) bearing imidazole moiety was synthesized through reversible addition-cracking chain transfer (RAFT) polymerization. PDPV can self-assemble into micelles in aqueous solution and then be loaded with doxorubicin (DOX) to obtain DOX@PDPV, followed by Zn coordination to anchor ZIF-8 to the PVim moiety in DOX@PDPV to obtain the final drug delivery system DOX@PDPV@ZIF-8 hybrids. The DOX@PDPV@ZIF-8 hybrids can avoid the influence of the critical micelle concentration (CMC) on it, which was further prevent the premature leakage of DOX under physiological conditions. Furthermore, the pH-responsive properties of PDPA and ZIF-8 facilitated enabled the effective release of DOX in weakly acidic tumor environments. In vitro studies also confirmed that DOX@PDPV@ZIF-8 improved DOX accumulation in cells, leading to the inhibition of cancer cell growth. Therefore, the integrated design provided a promising strategy to regulate the stability of block copolymer micelles, improve drug release kinetics, and ultimately inhibit the growth of cancer cell.

Preparation and design of intelligent multi-response PTMC/PVP composite nanofibrous dressing to promote wound closure and its applications in diabetic wounds

The healing process of diabetic wounds is characterized by a slow and arduous progression, making it challenging to achieve wound closure and complete healing through self-contraction, as observed in normal wounds. In this study, an intelligent multi-responsive composite of polytrimethylene carbonate (PTMC)/polyvinylpyrrolidone (PVP) nanofibrous dressing (C-PPZS) loaded with simvastatin-loaded ZIF-8 nanoparticles (ZIF-8@SIM NPs) was fabricated via electrospinning technology. The dressing exhibited liquid-triggered and temperature-controlled shrinkage characteristics, as well as pH-responsive drug release properties. When subjected to a temperature of 37 ℃ for 60 min, the area shrinkage rate of PPZS in PBS was determined to be 78.36 ± 1.14 %, and C-PPZS also reduced the area of isolated mouse skin defects to 38.01 ± 2.33 % of its original size. Furthermore, in vitro studies demonstrated that C-PPZS exhibited favorable biocompatibility and proangiogenic properties, along with significant inhibitory effects against S. aureus and E. coli. In vivo experiments conducted on diabetic mice revealed that C-PPZS facilitated wound closure and healing, attenuated scar formation, stimulated collagen fiber deposition, and promoted vascular regeneration. In conclusion, C-PPZS has great potential as an advanced dressing for the treatment of chronic wounds.

WITHDRAWN: Folic acid Grafted, cell-penetrating peptide conjugated pH-sensitive hydrophobically modified Glycol chitosan nanoparticles for drug delivery in breast cancer

Nanocarriers are an outcome of the fast development of nanotechnology; however, delivering drugs to tumor sites effectively is still a major difficulty. A pH-responsive drug carrier with good cell penetration and targeting ability was developed to release the drug exactly to the cancer site and overcome these limitations.The drug carrier FA-TAT-HGCNPs/PTX, which is pH-responsive, uses folic acid (FA) and TAT peptide to deliver paclitaxel (PTX) for target folate-receptor-overexpressing breast cancer cells. 2-(diisopropylamino) ethyl methacrylate was connected to glycol chitosan (GC) to form HGCNPs. Then TAT and HGCNPs were conjugated and FA was grafted onto the HGCNPs’ hydroxyl group. Physicochemical characterizations of FA-TAT-HGCNPs was also evaluated. The maximum DLE and EE values of the FA-TAT-HGCNPs at pH 8.0 were 74.0 ± 2.22 % and 93.7 ± 2.8 %, respectively. FA-TAT-HGCNPs, for instance, showed stability during long-term storage and lyophilization while exhibiting pH-responsive dissociation properties. The synthesized drug carrier was characterized by FTIR, XRD, SEM, HRTEM, DLS, and Zeta analysis. MTT assay exhibited the high anticancer activity of the FA-TAT-HGCNPs/PTX against the MCF-7 cells, whereas drug-free ones are highly biocompatible. The pharmacokinetic results showed twice the bioavailability of FA-TAT-HGCNPs/PTX compared to HGCNPs/PTX. Unlike FA-HGCNPs/PTX, CLSM analysis showed that FA-TAT-HGCNPs/PTX had a significantly more efficient intracellular uptake in MCF-7 cells. These data have shown the transmembrane ability of TATpeptide,the targeting effects of folate decoration, and the synergistic interaction between them.According to these findings, PTX-loaded FA-TAT-HGCNPs offer a potentially effective nanoscale drug delivery system for the treatment of breast cancer.

Cur@ZIF-8@BA nanomaterials with pH-responsive and photodynamic therapy properties promotes antimicrobial activity.

Antimicrobial photodynamic therapy (aPDT) has emerged as a highly promising strategy for non-antibiotic treatment of infections due to its unique advantages in efficient bactericidal action and reduction of drug resistance. The natural photosensitizing properties of curcumin (Cur) are widely acknowledged; however, its limited bioavailability has impeded its practical application. In this study, we developed a nanomaterial called Cur@ZIF-8@BA by encapsulating Cur within ZIF-8 and modifying the surface with boric acid (BA). The Cur@ZIF-8@BA exhibits pH-responsive properties and enhances bacterial binding, thereby effectively promoting photodynamic therapy. Moreover, its antibacterial activity against E. coli, Staphylococcus aureus and A. baumannii is significantly increased in the presence of light compared to a dark environment. The mechanism behind this may be that BA increases the affinity of Cur@ZIF-8@BA towards bacteria, and making released Zn2+ and BA from the nanomaterial increase bacterial cell membrane permeability. This facilitates efficient delivery of Cur into bacterial cells, resulting in generation of abundant reactive oxygen species (ROS) and subsequent bactericidal activity. In conclusion, our prepared Cur@ZIF-8@BA holds great promise as a photodynamically mediated antimicrobial strategy.

Preparation of self-healing and pH-responsive nanofiltration membranes with improved anti-fouling property for salt/dye separation

Nanofiltration (NF) membranes can inevitably suffer from external damage in the practical application process, causing the loss of their original function and performances. In this work, the β-CD-DX-S were synthesized for the first time through one-step polymerization of SBMA, DMAEMA and double bond functionalized β-CD. Subsequently, the membrane was successfully fabricated via interfacial polymerization using the constructed β-CD-DX-S as aqueous phase monomer alone. The prepared β-CD-DX-S/PES membrane exhibits novel self-healing performance attributing to the host-guest interaction between DMAEMA and β-CD. The membranes also possess excellent pH-responsive property attributing to the protonation and deprotonation behavior under different pH environments of dimethylamine unit in DMAEMA. The grafted DMAEMA and SBMA enhanced the hydrophilic property of membrane, reducing electrostatic adsorption of pollutants on the surface of membrane. The hydrophobic binding site inside the cavity of β-CD can accommodate dimethylamino group in the DMAEMA which could be regulate the spatial structure of β-CD-based materials, strengthening salt/dye selectivity of membrane. The results indicated that the prepared β-CD-DX-S/PES membranes possess good potential for NF applications.

Fabrication of dual responsive microcapsules based on starch with enhanced foliar adhesion and photostability for improving control efficacy and reducing environmental risks

Stimuli-responsive controlled release formulations offer a promising avenue for enhancing effective utilization and mitigating environmental risks of pesticides. Herein, pH and enzyme-responsive pesticide microcapsules (AVE@CPS-Fe-TA) were constructed by encapsulating carboxylated porous starch (CPS) loaded with avermectin (AVE) within tannic acid-iron complexes (Fe-TA) to improve the insecticidal efficacy and reduce toxicity to non-targets of AVE. The results showed that the loading content of AVE in the modified starch-based microcapsules could be precisely adjusted by the enzymatic hydrolysis time of starch. The prepared AVE@CPS-Fe-TA had pH and α-amylase dual responsive release properties and exhibited superior photostability, and its photolysis half-life was extended by 15.57-fold compared to AVE technical. Additionally, the leaf retention rate of AVE@CPS-Fe-TA after being rinsed by simulated rainwater was 6.08 times higher than that of commercial formulation AVE EC. In greenhouse insecticidal activity experiment, AVE@CPS-Fe-TA demonstrated a high control efficacy against Ostrinia furnacalis and had a prolonged effective duration. Moreover, AVE@CPS-Fe-TA significantly reduced the acute toxicity of AVE to zebrafish and promoted the growth of maize seedlings. Therefore, this work would provide eco-friendly stimuli-responsive microcapsules of pesticides for improving the efficiency of utilization and reducing environmental risks.

The Role of Nanoparticle Morphology on Enhancing Delivery of Budesonide for Treatment of Inflammatory Bowel Disease.

Inflammatory bowel disease (IBD) is a chronic and recurrent inflammatory disease that affects the gastrointestinal tract. The major hurdles impeding IBD treatment are the low targeting efficiency and short retention time of drugs in IBD sites. Nanoparticles with specific shapes have demonstrated the ability to improve mucus retention and cellular uptake. Herein, mesoporous silica nanoparticles (MSNs) with various morphologies were used to deliver budesonide (BUD) for the treatment of IBD. The therapeutic efficacy is strongly dependent on their shapes. The system comprises different shapes of MSNs as carriers for budesonide (BUD), along with Eudragit S100 as the enteric release shell. The encapsulation of Eudragit S100 not only improved the stability of MSNs-BUD in the gastrointestinal tract but also conferred pH-responsive drug release properties. Then, MSNs efficiently deliver BUD to the colon site, and the special shape of MSNs plays a critical role in enhancing their permeability and retention in the mucus layer. Among them, dendritic MSNs (MSND) effectively reduced myeloperoxidase (MPO) activity and levels of inflammatory cytokines in the colon due to long retention time and rapid release in IBD sites, thereby enhancing the therapeutic efficacy against colitis. Given the special shapes of MSNs and pH-responsivity of Eudragit S100, BUD loaded in the voids of MSND (E@MSNs-BUD) could penetrate the mucous layer and be accurately delivered to the colon with minor side effects. This system is expected to complement current treatment strategies for the IBD.

Recycling scale inhibitor wastes into pH-responsive complexes to treat wastewater produced from spent lithium-ion battery disposal

A large amount of organophosphorus-containing wastewater is produced in spent lithium-ion battery disposal. Forward osmosis (FO) offers unique advantages in purifying this kind of wastewater if suitable draw solutes – the core of FO technology, are available. Herein we synthesize several pH-sensitive zinc complexes, namely ZnATMP-iNa (i = 0, 1, 2, 3, 4), from ZnSO4 and amino tris(methylene phosphonic acid) (ATMP) obtained from scale inhibitor wastes for organophosphorus-containing wastewater remediation. Among these ZnATMP-iNa, ZnATMP-3Na best meets the standards of an ideal draw solute. This makes ZnATMP-3Na outperform other reported draw solutes. 0.6 M ZnATMP-3Na produces a water flux of 12.7 LMH, 136 % higher than that of NaCl and a solute loss of 0.015 g/L, lower than that of NH4HCO3 (0.83 g/L). In organophosphorus-containing wastewater treatment, ZnATMP-3Na has higher water recovery efficiency (8.3 LMH) and sustainability than NaCl and NH4HCO3, and is sufficient to handle large quantities of wastewater. Remarkably, the pH-responsive property allows ZnATMP-3Na to be readily recovered through pH-control and reused in FO. The ionic property, expanded cage-like structure and easy-recycling make ZnATMP-3Na achieve sustainable FO separation and superior to other draw solutes. This study provides inspiration for draw solute design from wastes and extends FO application to organophosphorus-containing wastewater remediation.

Biofilms from poly-vinyl alcohol/palmyra root sprout with Boswellia serrata, carbon dots and anthocyanin for sensing the freshness of sardine fish

One of the main issues that customers worldwide have is food adulteration. In commercial packages, freshness cannot always be determined visually. Here, we propose sensitive films for use in food packaging that could alter colour to indicate a change in freshness. Hybrid, multifunctional, and eco-friendly films were prepared from polyvinyl alcohol/palmyra root sprout (PVA/PRS), fused with soy protein isolate carbon dot (CD), Boswellia serrata (BS), and Clitoriaternatea anthocyanin (CTE). The films showed pH sensitivity, antioxidant, and UV barrier properties. By creating hydrogen bonds between PRS and the other fillers, adding these substances makes PVA less crystallized. These interactions were verified by infrared Fourier-transform analysis. When compared to PVA, PRS films had significantly lower moisture content and swelling ratios. The UV-blocking capabilities of the films were greatly improved by the addition of CD, BS, and CTE without compromising their mechanical, thermal, or water vapor barrier properties. The composite film PVA/PRS/CD/BS/CTE exhibited a maximum tensile strength value of 69.47 ± 1.49 MPa. The CT extract provides the film with superior antioxidant properties. The colorimetric films PVA/PRS/CTE and PVA/PRS/CD/BS/CTE showed distinct pH-responsive colour-change properties as well as good colour stability. The colorimetric films were used to test the freshness of sardine fish, and they revealed unique colour changes that indicated whether the fish sample was spoiled or not.

Development of receptor-targeted and pH-responsive zeolitic imidazole framework-90 nanoplatform for anti-ovarian cancer

The covalent functionalization of the zeolitic imidazolate framework (ZIF) is rapidly progressing and is being exploited as a nanoplatform for antitumor drug delivery to improve tumor targeting and drug release. Here, a novel nanoplatform strategy was developed by encapsulating Carboplatin (CBP) in ZIF-90 nanospheres (NPs) to obtain CBP@ZIF-90 NPs and then, modifying folate-terminated methoxypoly(ethylene glycol) (FA-PEG-NH2) on the aldehyde group of ZIF-90 to form CBP@ZIF-90-NPF NPs with acid-sensitive Schiff base bond. The research results indicate that the yield of ZIF-90 was 72.77 ± 0.27 %, and the encapsulation efficiency and the loading content of CBP@ZIF-90 were 45.22 ± 0.49 % and 24.65 ± 0.34 %, respectively. The size of CBP@ZIF-90-NPF was 107.7 ± 1.7 nm in monodispersity with a single crystalline dodecahedral structure. Furthermore, the in vitro release behavior study revealed the sustained-release and the pH-responsive dissociation properties of the NPs. Only 6.84 % of CBP was released from the nanocarrier under physiological pH conditions for 48 h, while the release from the tumor microenvironment was 92.89 %. In addition, the cellular uptake result clearly showed that most of the FA-PEG-NH2 modified NPs exhibited specific selectivity in tumor cell nuclei. Finally, the cell counting kit-8 (CCK8) assay based on human ovarian cancer cell line (OVCAR-3) and human normal ovarian epithelial (IOSE-80) cell line obviously indicated that the ZIF-90 NPs had good biocompatibility and minimal cytotoxicity, as well as the high inhibition efficiency of the CBP@ZIF-90-NPF NPs meant that a much higher amount of CBP was transferred into the folate receptor (FR)-overexpressed ovarian cancer cells via FR mediated endocytosis. These results suggest that ZIF-90-NPF NPs could be an ideal targeted drug delivery vehicle for CBP, serving as a promising strategy for ovarian cancer treatment.

Polyphenol-based photothermal nanoparticles with sprayable capability for self-regulation of microenvironment to accelerate diabetic wound healing

Current treatments for diabetic wounds have some curative effect, but the process is complicated and lack user-friendly wound dressings. Nanozymes have gained significant attention for wound healing due to their striking merits. Herein, we have developed a novel sprayable tannin acid-cobalt coordination nanozyme (TACo) for diabetic wound healing. TACo nanozyme offers a convenient and efficient methods by spraying directly onto wounds surface, reducing infection risk by avoiding direct contact. Notably, its antioxidant properties contribute to scavenging the reactive oxygen species (ROS), alleviating oxidative stress and inflammation of wound microenvironment. Additionally, TACo nanozyme could promote cell survival and multiplication, which is crucial for the wound healing process. Importantly, TACo nanozyme facilitates angiogenesis by enhancing cell viability, migration, and tube formation. The unique coordination between metal and phenolic components confers pH-responsive cobalt ion and TA release properties, avoiding secondary damage during the wound cleaning. This unique composition seamlessly integrates photothermal antibacterial therapy, inflammatory microenvironment management, supporting for angiogenesis, and effective promotion of extracellular matrix production sequentially by harnessing the acidic pH environment of diabetic wounds. In conclusion, the development of a sprayable TACo nanozyme presents a promising therapeutic approach for the treatment of diabetic wounds, addressing the complexities of current treatments and providing a user-friendly application method.

Construction and evaluation of biomass-modified mesoporous silica nanoparticles as enzyme-responsive and pH-Responsive drug carriers for the controlled release of quercetin

This study constructed a biomass-modified mesoporous silica nanoparticle with enzyme-responsive and pH-responsive properties. The nanoparticles were used to evaluate the loading and release capacities of quercetin (QU). The multifunctional nanoparticles (MSN@CMCS-HA) were constructed by using hyaluronic acid (HA) and carboxymethyl chitosan (CMCS) as shells and mesoporous silica nanoparticles (MSN) as cores. The carrier's structure and properties were evaluated utilizing zeta, FTIR, TGA, XPS, XRD, BET, SEM, and TEM. The drug adsorption test revealed that the maximum equilibrium adsorption capacity of MSN@CMCS-HA for QU was 314.4 mg/g. In vitro drug release demonstrated that, under the influence of hyaluronidase (100 μg/mL) and pH of 5, the high drug release rate (63.73 %) was achieved. In addition, hemolysis and CCK8 tests confirmed the high biocompatibility of MSN@CMCS-HA. Consequently, MSN@CMCS-HA exhibited promising potential as an enzyme-responsive and pH-responsive drug carrier.

Inflammatory microenvironment regulation and osteogenesis promotion by bone-targeting calcium and magnesium repletion nanoplatform for osteoporosis therapy

Osteoporosis is the most common bone metabolic disease that affects the health of middle-aged and elderly people, which is hallmarked by imbalanced bone remodeling and a deteriorating immune microenvironment. Magnesium and calcium are pivotal matrix components that participate in the bone formation process, especially in the immune microenvironment regulation and bone remodeling stages. Nevertheless, how to potently deliver magnesium and calcium to bone tissue remains a challenge. Here, we have constructed a multifunctional nanoplatform composed of calcium-based upconversion nanoparticles and magnesium organic frameworks (CM-NH2-PAA-Ald, denoted as CMPA), which features bone-targeting and pH-responsive properties, effectively regulating the inflammatory microenvironment and promoting the coordination of osteogenic functions for treating osteoporosis. The nanoplatform can efficaciously target bone tissue and gradually degrade in response to the acidic microenvironment of osteoporosis to release magnesium and calcium ions. This study validates that CMPA possessing favorable biocompatibility can suppress inflammation and facilitate osteogenesis to treat osteoporosis. Importantly, high-throughput sequencing results demonstrate that the nanoplatform exerts a good inflammatory regulation effect through inhibition of the nuclear factor kappa-B signaling pathway, thereby normalizing the osteoporotic microenvironment. This collaborative therapeutic strategy that focuses on improving bone microenvironment and promoting osteogenesis provides new insight for the treatment of metabolic diseases such as osteoporosis.

PH-Responsive Charge Convertible Hyperbranched Poly(ionic liquid) Nanoassembly with High Biocompatibility for Resistance-Free Antimicrobial Applications.

As a potential alternative to antibiotics, hyperbranched poly(ionic liquid)s (HPILs) have demonstrated significant potential in combating bacterial biofilms. However, their high cation density poses a high risk of toxicity, greatly limiting their in vivo applications. In this study, we constructed a biocompatible HPIL (HPIL-Glu) from a hyperbranched polyurea core with modified terminals featuring charge-convertible ionic liquids. These ionic liquid moieties consist of an ammonium-based cation and a gluconate (Glu) organic counter. HPIL-Glu could form a homogeneous nanoassembly in water and exhibited a pH-responsive charge conversion property. Under neutral conditions, Glu shielded the positively charged surface, minimizing the toxicity. In a mildly acidic environment, Glu protonation exposes cationic moieties to biofilm eradication. Comprehensive antimicrobial assessments demonstrate that HPIL-Glu effectively kills bacteria and promotes the healing of bacteria-infected chronic wounds. Furthermore, prolonged exposure to HPIL-Glu does not induce antimicrobial resistance.

Dynamic Schiff base linkage-based double-network hydrogels with injectable, self-healing, and pH-responsive properties for bacteria-infected wound healing

Dynamic Schiff base linkage-based double-network hydrogels with injectable, self-healing, and pH-responsive properties for bacteria-infected wound healing

Synthesis and Characterization of Multiple Stimuli-Responsive Fluorescent Polymer Hydrogels Based on Terpyridine and N-Isopropylacrylamide.

A series of stimuli-responsive fluorescent hydrogels were successfully synthesized via micelle radical copolymerization of hydrophilic acrylamide (AM), hydrophobic chromophore terpyridine-based monomer (TPY), and N-isopropylacrylamide (NIPAM). These hydrogels presented blue emissions (423-440 nm) under room temperature, which is caused by the π-π* transition of the conjugated structures. Once the ambient temperature was increased to 55 °C, the fluorescence color changed from blue (430 nm) to pink (575 nm) within 10 min, subsequently to yellow (535 nm), and eventually back to pink. The thermal-responsive properties are attributed to the transition of the TPY units from unimer to dimer aggregation via the intermolecular charge transfer complex at high temperatures. The hydrogels showed pH-responsive properties. The emission peak of the hydrogel exhibited a blue shift of ~54 nm from neuter conditions to acidic conditions, while a 6 nm red shift to an alkaline environment was observed. The hydrogels demonstrated an obvious change in fluorescence intensity and wavelength upon adding different metal ions, which is caused by the coordination between the terpyridine units incorporated on the backbones and the metal ions. As a consequence, the hydrogels presented a sharp quenching fluorescence interaction with Fe2+, Fe3+, Cu2+, Hg2+, Ni2+, and Co2+, while it exhibited an enhanced fluorescence intensity interaction with Sn2+, Cd2+, and Zn2+. The microstructural, mechanical, and rheological properties of these luminescent hydrogels have been systematically investigated.

Stability and release mechanism of double emulsification (W1/O/W2) for biodegradable pH-responsive polyhydroxybutyrate/cellulose acetate phthalate microbeads loaded with the water-soluble bioactive compound niacinamide

Microbeads of biodegradable polyhydroxybutyrate (PHB) offer environmental benefits and economic competitiveness. The aim of this study was to encapsulate a water-soluble bioactive compound, niacinamide (NIA), in a pH-responsive natural matrix composed of PHB and cellulose acetate phthalate (CAP) by double emulsification (W1/O/W2) to improve the encapsulation efficiency (%EE) and loading capacity (%LC). PHB was produced in-house by Escherichia coli JM109 pUC19-23119phaCABA-04 without the inducing agent isopropyl β-D-1-thiogalactopyranoside (IPTG). The influences of PHB and polyvinyl alcohol (PVA) concentrations, stirring rate, PHB/CAP ratio and initial NIA concentration on the properties of NIA-loaded pH-responsive microbeads were studied. The NIA-loaded pH-responsive PHB/CAP microbeads exhibited a spherical core-shell structure. The average size of the NIA-loaded pH-responsive microbeads was 1243.3 ± 11.5 μm. The EE and LC were 33.3 ± 0.5 % and 28.5 ± 0.4 %, respectively. The release profiles of NIA showed pH-responsive properties, as 94.2 ± 3.5 % of NIA was released at pH 5.5, whereas 99.3 ± 2.4 % of NIA was released at pH 7.0. The NIA-loaded pH-responsive PHB/CAP microbeads were stable for >90 days at 4 °C under darkness, with NIA remaining at 73.65 ± 1.86 %. A cytotoxicity assay in PSVK1 cells confirmed that the NIA-loaded pH-responsive PHB/CAP microbeads were nontoxic at concentrations lower than 31.3 μg/mL, in accordance with ISO 10993-5.

Ion and Molecular Sieving With Ultrathin Polydopamine Nanomembranes.

In contrast to biological cell membranes, it is still a major challenge for synthetic membranes to efficiently separate ions and small molecules due to their similar sizes in the sub-nanometer range. Inspired by biological ion channels with their unique channel wall chemistry that facilitates ion sieving by ion-channel interactions, the first free-standing, ultrathin (10-17nm) nanomembranes composed entirely of polydopamine (PDA) are reported here as ion and molecular sieves. These nanomembranes are obtained via an easily scalable electropolymerization strategy and provide nanochannels with various amine and phenolic hydroxyl groups that offer a favorable chemical environment for ion-channel electrostatic and hydrogen bond interactions. They exhibit remarkable selectivity for monovalent ions over multivalent ions and larger species with K+/Mg2+ of ≈4.2, K+/[Fe(CN)6]3- of ≈10.3, and K+/Rhodamine B of ≈273.0 in a pressure-driven process, as well as cyclic reversible pH-responsive gating properties. Infrared spectra reveal hydrogen bond formation between hydrated multivalent ions and PDA, which prevents the transport of multivalent ions and facilitates high selectivity. Chemically rich, free-standing, and pH-responsive PDA nanomembranes with specific interaction sites are proposed as customizable high-performance sieves for a wide range of challenging separation requirements.