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Polymer Chemistry · 2013 ·Vol. 4 ·期 12 ·3545-3553 · IF 5.231

Folate-conjugated poly(N-(2-hydroxypropyl)methacrylamide-co-methacrylic acid) nanohydrogels with pH/redox dual-stimuli response for controlled drug release

Yuan-Jia Pan,Dian Li,Sha Jin,Chuan Wei,Ke-Yi Wu,Jia Guo,Chang-Chun Wang

Folate-conjugated poly(N-(2-hydroxypropyl)methacrylamide-co-methacrylic acid) nanohydrogels were facilely prepared via distillation–precipitation polymerization and subsequent folate modification. Due to the nanohydrogels being crosslinked with disulphide bonds, they could be easily degraded into short polymer chains in the presence of glutathione, which will be beneficial for easily discharging the nanohydrogels from the body. Doxorubicin (DOX), a clinical anti-cancer drug, was efficiently loaded in the nanohydrogels (up to 39.3 wt%) by the electrostatic interactions between the amine group in doxorubicin (DOX) and the carboxyl groups in the nanohydrogels at neutral conditions. The cumulative release profile of the DOX-loaded nanohydrogels showed a relatively low level of drug release (23 wt% in 48 h) at pH 7.4 and a quick release (over 95 wt% in 2 h) at pH 5.0 with reducing environment, exhibiting pH/redox dual-stimuli-responsive drug release. The dose-dependent cytotoxicity of the drug-loaded nanohydrogels was studied by the CCK-8 assay. The nanohydrogels possess many favourable merits of drug carriers, such as excellent biocompatibility, high drug loading capacity, minimal drug release under an extracellular condition, rapid drug release in response to the intracellular level of pH and reducing environment, and folate-mediated endocytosis, which endow them as great candidates for targeted delivery of anti-cancer drugs.

研究领域: 药剂学 · 生物材料学 · 肿瘤学
✓ 已验证 DOI 高影响因子
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JOURNAL OF CONTROLLED RELEASE · 2025 · IF 11.5

Multifunctional microfluidic-directed polymer/hydrogel fabrics towards pH-responsive drug delivery, wound monitoring and wearable sensing

Xiang-Yun Du,Yin-Jian Song,Chen Du,Ji-Dong Liu

Delayed skin wound healing caused by bacterial infection and persistent oxidative stress has been considered as a frequently encountered clinical problem that significantly affects patients' health. However, the real-time monitoring and on-demand treatment of non-healing wounds remain a great challenge. Herein, a feasible strategy is developed to core-shell polymer/hydrogel microfibers by integrating microfluidic spinning with shear-flow-induced coating technology. The fabricated self-healing microfibers are facilely assembled into nonwoven fabrics through reversible physical interactions. The core polycaprolactone (PCL) acting as a skeleton endows fabrics with structural and mechanical robustness (4.67 MPa), while the hydrogel shell brings functional diversity including great flexibility, self-healing, self-adhesion and pH-responsive swelling capability. By introducing epigallocatechin gallate (EGCG) in core PCL phase, the remarkable reactive oxygen species (ROS) cleaning capacity (93.8 % for 0.5 h) and antibacterial activity against E. coli (98.7 %) and S. aureus (99.6 %) are achieved. Particularly, the pH-regulated drug release of fabric in a prolonged form is achieved owing to the reversibly swelling/shrinking behavior of hydrogel shell with the changed environmental pH, which is expected to realize on-demand drug delivery and treatment of wound. Additionally, the pH-responsive curcumin-loaded mesoporous microparticles are incorporated into hydrogel shell, aiming to visually real-time detect pH level in a high-efficiency and reversible manner. Moreover, the fabric can serve as a flexible wearable sensor for precisely monitoring motions of patients. This strategy explores a feasible solution to diligently tracking wound pH and movements, along with inhibiting wound infection, substantiating a great foundation for application in personalized, intelligent and precise theranostic wound dressings.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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RSC Advances · 2016 ·Vol. 6 ·期 115 ·114714-114721 · IF 3.289

Highly efficient alginate sodium encapsulated chlorpyrifos/copper(II) Schiff base mesoporous silica sustained release system with pH and ion response for pesticide delivery

Chen Huayao,Lin Yueshun,Zhou Hongjun,Zhou Xinhua,Gong Sheng,Xu Hua

Salicylaldehyde modified mesoporous silica (SA–MCM-41) was prepared through a co-condensation method. Through the bridge effect from copper ion, the chlorpyrifos (CH) was supported on copper(II)/Schiff base mesoporous silica (Cu–MCM-41). And then CH–Cu–MCM-41 was encapsulated by alginate sodium (ALG) to form a highly efficient sustained-release system (ALG–CH–Cu–MCM-41). The sustained-release performance of ALG–CH–Cu–MCM-41 at different pH values and different NaCl concentrations was investigated. The as-synthesized system showed significant pH responsiveness. Under the condition of pH ≤ 7, the release rate of chlorpyrifos decreased with pH increasing. Meanwhile, its release rate under weak base conditions was slightly larger than under weak acid conditions. The sustained release curves of ALG–CH–Cu–MCM-41 were consistent with the sustained release curves of CH–Cu–MCM-41 but with a smaller release rate because of the block effect from ALG. Meanwhile, the drug release rate of the sustained release system was also affected by ion concentration. Their sustained-release curves could be described by the Korsmeyer–Peppas equation.

研究领域: 农药科学 · 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry B · 2021 ·Vol. 9 ·期 42 ·8871-8881 · IF 6.331

Double pH-sensitive nanotheranostics of polypeptide nanoparticle encapsulated BODIPY with both NIR activated fluorescence and enhanced photodynamic therapy

Huiping Dang,Quan Cheng,Youliang Tian,Changchang Teng,Kai Xie,Lifeng Yan

To achieve accurate fluorescence imaging-guided cancer therapy, intelligent systems with specific responsiveness to the tumor microenvironment need to be designed. Here, we have achieved both enhanced NIR fluorescence and photodynamic therapy by introducing a dimethylamino functional group in BODIPY dyes, which can be used as a pH sensor under acidic conditions by coordinating with the proton. At pH 7.4, the fluorescence is quenched due to the photo-induced electron transfer (PET) process. After the photosensitizer is protonated in tumor cell lysosomes (pH 4.0–5.5), the PET process is inhibited and the fluorophore emission capacity is restored (fluorescence enhancement up to 10-fold), resulting in near-infrared fluorescence with the OFF/ON transition inside the tumor and enhanced singlet oxygen production for lysosome targeting capability. Due to the substitution of heavy atom iodine, the compound has a high singlet oxygen quantum yield of 81.8% in dichloromethane. In addition, using a pH-sensitive amphiphilic polypeptide (POEGMA23-PE9) as a carrier to wrap the photosensitizer BDPI can release enough drug in the acidic environment (pH 5.5–6.5) of intracellular endosomes/lysosomes, which is conducive to more adequate interactions of the photosensitizer with H+ and more effective enhancement of fluorescence emission and 1O2 production, achieving precise fluorescence imaging capability and extremely low background toxicity.

研究领域: 生物医学工程 · 癌症研究 · 材料科学 · 分子影像
✓ 已验证 DOI PubMed 高影响因子
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Acta Biomaterialia · 2020 · IF 7.242

pH-responsive silk fibroin-based CuO/Ag micro/nano coating endows polyetheretherketone with synergistic antibacterial ability, osteogenesis, and angiogenesis

Jianglong Yan,Dandan Xia,Wenhao Zhou,Yangyang Li,Pan Xiong,Qiyao Li,Pei Wang,Ming Li,Yufeng Zheng,Yan Cheng

Polyetheretherketone has been widely used for bone defect repair, whereas failures may happen due to implant loosening and infection. Thus, PEEK implant with multi-function (osteogenesis, angiogenesis , and bacteria-killing) is essential to solve this problem. Herein, copper oxide microspheres (µCuO) decorated with silver nanoparticles (nAg) were constructed on porous PEEK surface via silk fibroin . In vitro studies highlighted the pH controlled release ability of this coating. It liberated a high dose of Cu 2+ and Ag + at low pH environment (pH 5.0), leading to 99.99% killing of planktonic bacteria and complete eradication of sessile bacteria, avoiding biofilm formation. Under physiological environment (pH 7.4), a lower amount of leaked metal ions induced promoted ALP production, collagen secretion, and calcium deposition, as well as NO production, which indicated potentiated osteogenesis and angiogenesis. In vivo results displayed the highest new bone volume around, and the appearance of new bone inside porous structure of, PEEK implant with this coating in rabbit tibia, signified the abilities of this coating to promote bone regeneration and osseointegration . Our study established solid support for implants with this coating to be a successful bone defect repair solution. Statement of Significance In this study, CuO/Ag micro/nano particles were incorporated into the porous surface of PEEK through polydopamine and silk fibroin layers. The design of this coating conferred pH-controlled release behavior to Cu 2+ and Ag + . High dose of metal ions were released at pH 5.0, which presented synergistic antibacterial ability and killed 99.99% of planktonic bacteria. Low concentration of metal ions were controlled by this coating at physiological environment, which potentiated osteodifferentiation of Ad-MSC in vitro and led to complete integration of implant with bone tissue in vivo .

研究领域: 生物医学工程 · 材料科学 · 组织工程
✓ 已验证 DOI PubMed 高影响因子
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Science of Advanced Materials · 2016 ·Vol. 8 ·期 10 ·1901-1907 · IF 1.812

Temperature and pH Dual-Responsive Polyhedral Oligomeric Silsesquioxane/Poly[2-(dimethyl amino)-ethyl methacrylate]-bPoly(N-isopropylacrylamide) Hybrid Materials Synthesized via RAFT Polymerization and Thiol-Ene Reaction: Potential Candidates for Absorption of Organic Dyes

Yang Zhenglong,Liu Xinyan,Xu Xiaoli,Chen Sai,Li Feng,Zhu Xingyi,Du Yuchuan

The temperature and pH dual-responsive polyhedral oligomeric silsesquioxane/poly[2-(dimethylamino)-ethyl methacrylate]-b-poly(N-isopropylacrylamide) hybrid materials (POSS/PDMAEMA-b-PNIPAM) were synthesized via combination of reversible addition-fragmentation chain transfer (RAFT) polymerization and thiol-ene "Click Chemistry." Their structures and self-assembly behaviors were characterized by 1HNMR, TEM, UV-vis absorbance and DLS measurements. POSS/PDMAEMA-b-PNIPAM could self-assemble into thermo- and pH-sensitive micelles with the POSS heads forming as a core and the PDMAEMA-b-PNIPAM chains as a corona. Hydrophobic dyes could be encapsulated in the micelles, so it can be used to absorb dyes. It was found that POSS/PDMAEMA-b-PNIPAM aqueous solution (5 mg/mL, 2 mL) could rapidly remove 98% of methyl red and 90% of diphenylthiocarbazone in petroleum ether with the initial concentrations of 50 mg/L (2 mL). In view of the good adsorption efficiency of POSS/PDMAEMA-b-PNIPAM hybrid materials, they will be a potential candidate for absorption of organic dyes.

研究领域: 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Asian Journal of Pharmaceutical Sciences · 2021 · IF 6.598

pH-sensitive micelles self-assembled from star-shaped TPGS copolymers with ortho ester linkages for enhanced MDR reversal and chemotherapy

Yong Xu,Shi Wang,Longshun Yang,Yuhang Dong,Yafang Zhang,Guoqing Yan,Rupei Tang

TPGS approved by FDA can be used as a P-gp inhibitor to effectively reverse multi-drug resistance (MDR) and as an anticancer agent for synergistic antitumor effects. However, the comparatively high critical micelle concentration (CMC), low drug loading (DL) and poor tumor target limit its further clinical application. To overcome these drawbacks, the pH-sensitive star-shaped TPGS copolymers were successfully constructed via using pentaerythritol as the initial materials, ortho esters as the pH-triggered linkages and TPGS active-ester as the terminated MDR material. The amphiphilic star-shaped TPGS copolymers could self-assemble into free and doxorubicin (DOX)-loaded micelles at neutral aqueous solutions. The micelles exhibited the lower CMC (8.2 × 10 −5  mg/ml), higher DL (10.8%) and long-term storage and circulation stability, and showed enhanced cellular uptake, apoptosis, cytotoxicity, and growth inhibition for in vitro MCF-7/ADR and/or MCF-7/ADR multicellular spheroids and in vivo MCF-7/ADR tumors via efficiently targeted drug release at tumoral intracellular pH (5.0), MDR reversal of TPGS, and synergistic effect of DOX and TPGS. Therefore, the pH-sensitive micelles self-assembled from star-shaped TPGS copolymers with ortho ester linkages are potentially useful to clinically transform for enhanced MDR cancer treatment.

研究领域: 药学 · 纳米技术 · 癌症研究 · 药物递送系统
✓ 已验证 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Interface-confined multi-layered reaction centers between Ce-MOFs and Fe3O4@C for heterogeneous electro-Fenton at wide pH 3–9: Mediation of Ce3+/Ce4+ and oxygen vacancy

Pei Su,Xuedong Du,Yang Zheng,Wenyang Fu,Qizhan Zhang,Minghua Zhou

A bifunctional catalyst with Ce-based metal–organic frameworks deposited on carbon encapsulated Fe 3 O 4 particles (Ce-MOFs/Fe 3 O 4 @C) was prepared for heterogeneous electro-Fenton (EF), which exhibited high H 2 O 2 generation efficiency (over 90% selectivity and 80.7% current efficiency), high sulfamethazine (SMT) removal with very low electric energy consumption (7.65 kWh kg −1 SMT), and wider pH suitability to alkaline environment (pH 9). The highest content of oxygen vacancies (O V ), Ce 3+ and Fe 2+ was simultaneously exhibited when the Fe/Ce ratio in precursor was 2:1. Interface-confined between Ce-MOFs and Fe 3 O 4 @C and presence of O V promoted the O 2 adsorption for oxygen reduction reaction and O 2 ∙- generation, and electron transfer between Fe and Ce. Meanwhile, the presence of Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ simultaneously facilitated the sequential catalysis induced by H 2 O 2 to generate ∙ OH, and Ce 4+ could promote O 2 ∙- to generate 1 O 2 . This work provides new insight into the design and synthesis of Fe-based catalysts in EF with interface confinement and multi-layered reaction centers to improve the generation and the decomposition of H 2 O 2 at the same time at a low cathode potential.

研究领域: 环境科学 · 催化化学
✓ 已验证 DOI 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2025 · IF 2.5

pH-responsive color indicator film based on sodium carboxymethylcellulose and natural acid buffering matrix for real-time beef sub-freshness monitoring

Shouyan Zhu,Huimin Wu,Rongrong Ma,Xiaoying Wang,Qin Wu

The good water solubility and film-forming properties of sodium carboxymethylcellulose (CMC–Na) render it an excellent matrix for a pH-responsive color indicator film, but its basic character inhibits its direct application. Natural acids can be used to solve this problem, but the buffering system formed in these processes may decrease the sensitivity and improve the heterogeneous compound distribution of the film. Previous studies have tried to address this problem by adjusting the species and amounts of the acids. However, the underlying mechanism has not been comprehensively clarified. Herein, a CMC–Na and CaCl2 mixture was used as the matrix for a pH-responsive color indicator film, alizarin (AZ) was used as the pH indicator, cinnamaldehyde (CMA) was used as an ultraviolet (UV) shielding agent, and natural acids were used as pH-controlling agents. Three protic acids with distinct numbers of acidic protons and pKa, acetic acid (monoacid), tartaric acid (diacid) and citric acid (triacid), were compared to elucidate the effect of these properties on the matrix pH, dye dispersion, and film response. The results showed that tartaric acid can be a good candidate in solving the problem on a basic CMC–Na matrix owing to its good performance in adjusting the film color and the sensitive color response of the resulting film at pH 6.0–7.0. The hydrogen bonds, hydrophobic interactions and chelation reactions formed among the compounds improve the mechanical property and oxygen barrier performance of the film, which are also beneficial to the homogeneous distribution of AZ and CMA, leading to a uniform color response and good UV-shielding performance. This film displays excellent color response quality in beef sub-freshness detections, suggesting its high sensitivity in “point-of-care” detections of real meat samples via naked eyes.

✓ 已验证 产品关联 DOI 高影响因子
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Materials Chemistry Frontiers · 2020 ·Vol. 4 ·期 9 ·2635-2645 · IF 6.788

One-pot quaternization of dual-responsive poly(vinyl alcohol) with AIEgens for pH-switchable imaging and killing of bacteria

Jin Wang,Meng Gao,Zhong-Kai Cui,Yong-Guang Jia,Sa Liu,Kai-Feng Chen,Xiaohui Chen,Yiqing Zhang,Zhou Fang,Yunhua Chen,Kaojin Wang,Huatang Zhang,Lin Wang,Li Ren

Facing the challenges posed by bacterial infection, the real-time detection of bacterial infection combined with antibacterial functions is urgently needed. Herein, we prepare thermo- and pH-responsive poly(vinyl alcohol) derivatives (PVA–TPE) bearing aggregation-induced emission luminogens of tetraphenylethene (TPE) and quaternary ammonium moieties through a facile one-pot quaternization with a tertiary amine method. Intrinsic fluorescence from TPE moieties and antibacterial functions from quaternary ammonium units can efficiently integrate the functions of “monitoring and killing of bacteria”. It is found that PVA–TPE can selectively image and kill Gram-positive bacteria at pH 7.4, while it switched to display enhanced broad-spectrum antimicrobial activity against both Gram-negative and -positive bacteria in an acidic environment (pH 5.5). Moreover, PVA–TPE exhibits low cytotoxicity on mammalian cells of L929, HepG2 and red blood cells. Furthermore, in vivo evaluations further confirmed that PVA–TPE has excellent antibacterial efficacy with no tissue damage. This study represents the first example of a pH-switchable integrated system for “monitoring and killing of bacteria” constructed through a facile one-pot quaternization method.

研究领域: 材料科学 · 生物材料 · 生物医学工程 · 微生物学
✓ 已验证 DOI 高影响因子
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International Journal of Nanomedicine · 2023 · IF 8

pH-triggered surface charge-switchable polymer micelles for the co-delivery of paclitaxel/disulfiram and overcoming multidrug resistance in cancer

Qiang Huo,Jianhua Zhu,Yimin Niu,Huihui Shi,Yaxiang Gong,Yang Li,Huihui Song,Yang Liu

Multidrug resistance (MDR) remains a major challenge for providing effective chemotherapy for many cancer patients. To address this issue, we report an intelligent polymer-based drug co-delivery system which could enhance and accelerate cellular uptake and reverse MDR. The nanodrug delivery systems were constructed by encapsulating disulfiram (DSF), a P-glyco-protein (P-gp) inhibitor, into the hydrophobic core of poly(ethylene glycol)-block-poly(l-lysine) (PEG-b-PLL) block copolymer micelles, as well as 2,3-dimethylmaleic anhydride (DMA) and paclitaxel (PTX) were grafted on the side chain of l-lysine simultaneously. The surface charge of the drug-loaded micelles represents as negative in plasma (pH 7.4), which is helpful to prolong the circulation time, and in a weak acid environment of tumor tissue (pH 6.5–6.8) it can be reversed to positive, which is in favor of their entering into the cancer cells. In addition, the carrier could release DSF and PTX successively inside cells. The results of in vitro studies show that, compared to the control group, the DSF and PTX co-loaded micelles with charge reversal exhibits more effective cellular uptake and significantly increased cytotoxicity of PTX to MCF-7/ADR cells which may be due to the inhibitory effect of DSF on the efflux function of P-gp. Accordingly, such a smart pH-sensitive nanosystem, in our opinion, possesses significant potential to achieve combinational drug delivery and overcome drug resistance in cancer therapy.

研究领域: 药剂学 · 纳米技术 · 肿瘤学 · 药物递送系统
✓ 已验证 DOI PubMed 高影响因子
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COLLOID AND POLYMER SCIENCE · 2015 ·Vol. 293 ·期 7 ·2035-2044 · IF 1.865

Preparation of pH-sensitive nanoparticles of poly (methacrylic acid) (PMAA)/poly (vinyl pyrrolidone) (PVP) by ATRP-template miniemulsion polymerization in the aqueous solution

Chen Guoxia,Liu Junxiu,Yang Yadong,Zhang Lijuan,Wu Min,Ni Henmei

Employing polymethacrylic acid (PMAA) as the template and N -vinyl pyrrolidone (N-VP) as monomer, the ATRP-template miniemulsion polymerization was carried out in the aqueous medium by using MBP/CuBr/bpy as initiator. The results were characterized by dynamic light scattering (DLS), transmission electron microscope (TEM), and gel permeation chromatography (GPC). It was observed that the stable particles exhibited amphoteric pH sensitivity, namely that in the range of pH 3.0 to 5.0, the particles precipitated, whereas beyond the range the particles were stable and swollen as pH varied. Moreover, the pH range was variable according to the molecular weight of PVP. The results of GPC indicated that the molecular weight of template polymer PMAA was duplicated by the daughter polymer PVP. Being noncross-linked, unlike the common microgels, the hydrodynamic diameter dramatically increased in a very narrow pH range, e.g., pH 5.5 –6 and 2.0–2.5. Finally, the nanoparticles of PMAA/PVP were applied for the controlled release of rifampicin (RFP) and doxorubicin (DOX).

研究领域: 材料科学 · 药学
✓ 已验证 DOI 高影响因子
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