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ACS Applied Bio Materials · 2020 · IF 0

Design of pH-Responsive Dissociable Nanosystem Based on Carbon Dots with Enhanced Anti-biofilm Property and Excellent Biocompatibility

Peili Li,Shuai Liu,Gaoke Zhang,Xu Yang,Weiwei Cao,Xuedong Gong,Xiaodong Xing

Bacterial biofilm poses a serious threat to human health, leading to increased and prolonged bacterial infections. How to solve the problem of eliminating biofilms effectively and rapidly while being nontoxic to normal cells is still a challenge. Here, we design a pH-sensitive anti-biofilm nanosystem formed by self-assembly between negatively charged carboxyl groups of poly(ethylene glycol_-COOH-polyethylenimine-2,3-dimethylmaleic anhydride (PPD) and positively charged amines on the surface of carbon dots derived from the ashes of calcined l-lysine powder (CDLys) (PPD@CDLys for short). The outmost copolymer could make PPD@CDLys facilely diffuse into the dense biofilm and reverse to be positively charged via hydrolysis, which lead to the acid-triggered disassembly of the nanosystem. After hydrolyzation, PPD would turn into a biocidal cationic polymer, which is prone to attaching on bacteria inside the biofilm and efficiently killing them. In addition, the released CDLys could induce intracellular reactive oxygen species (ROS) across the whole biofilm to degrade the matrix of extracellular polymer substances and kill resident bacteria deep into the biofilm. Finally, the prepared nanosystem effectively inhibits the formation of Staphylococcus aureus biofilm and rapidly destroys the mature biofilm by the synergy antibacterial effects of the cation and ROS. We also evaluate the biocompatibility of the nanocomposites. The results show that PPD@CQDLys has no toxicity to L929 and 3T3 cells and exhibits a zero hemolytic rate even when the concentration is up to 2000 μg/mL. The outstanding biocompatibility coupled with rapid anti-biofilm ability of the nanosystem presents an opportunity for it to be utilized as an effective pH-responsive and targetable anti-biofilm agent for controlling bacterial infections.

研究领域: 生物医学工程 · 材料科学 · 微生物学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

pH-Gated Switch of LCST-UCST Phase Transition of Hydrogels

Jiaqing He,Qiang Zhou,Zhiqing Ge,Shunfeng Jiang,Jiahe Li,Wei Feng,Haiyang Yang

Temperature-responsive hydrogels including lower critical solution temperature (LCST)- and upper critical solution temperature (UCST)-type hydrogels are attractive in various fields. However, the swift switch between LCST and UCST stimuli-responsive behaviors remains intriguing and challenging. Here is reported a kind of hydrogel with pH-gated LCST and UCST response behaviors. This is achieved using the hydrogen bonding between carboxylic acid groups of poly(acrylic acid- co -acrylamide) and hydroxyl groups of hydroxypropyl cellulose (HPC). The poly(acrylic acid- co -acrylamide)-HPC (PACA-HPC) hydrogels exhibit pH-gated reversible LCST-UCST phase transition behavior. When the transparent PACA-HPC hydrogel is placed in an acid bath, the COO − groups get protonated, rapidly forming hydrogen bonds with HPC to render a light-scattering state making the hydrogel opaque. Furthermore, the opaque hydrogel exhibits UCST phase transition behavior at 20–45 °C. When the opaque PCAC-HPC hydrogel is placed in an alkaline environment, hydrogen-bonded complexes gradually dissociate as the COOH groups are deprotonated to form a homogeneous transparent state. The transparent hydrogel exhibits LCST phase transition behavior at 20–45° C. Therefore, is shown the hydrogen bonding strategy to fabricate hydrogels with tunable LCST and UCST responses. With this pH-gated hydrogel with switchable LCST/UCST responsive behaviors, are demonstrated its applications in smart windows and information encryption.

CAS / MDL: 9004-64-2
研究领域: 材料科学 · 化学工程 · 生物医学工程
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LANGMUIR · 2010 · IF 3.898

pH-Responsive Chitosan-Mediated Graphene Dispersions

Ming Fang,Jiang Long,Weifeng Zhao,Liwei Wang,Guohua Chen

Homogeneous aqueous suspensions of graphene have been prepared by chemical reduction of graphene oxide in the presence of chitosan. The graphene sheets in thus prepared suspensions can be switched reversibly between a well dispersed and a more aggregated state with pH as a stimulus.

研究领域: 材料科学 · 生物医学工程
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CHINESE JOURNAL OF CHEMICAL PHYSICS · 2020 ·Vol. 33 ·期 5 ·540-546 · IF 1.067

Ultrafast infrared spectroscopic study of microscopic structural dynamics in pH stimulus-responsive hydrogels

Hong Jian,Zhou De-xia,Hao Hong-xing,Zhao Min,Bian Hong-tao

Hydrogels show versatile properties and are of great interest in the fields of bioelectronics and tissue engineering. Understanding the dynamics of the water molecules trapped in the three-dimensional polymeric networks of the hydrogels is crucial to elucidate their mechanical and swelling properties at the molecular level. In this report, the poly(DMAEMA-co-AA) hydrogels were synthesized and characterized by the macroscopic swelling measurements under different pH conditions. Furthermore, the microscopic structural dynamics of pH stimulus-responsive hydrogels were studied using FTIR and ultrafast IR spectroscopies from the viewpoint of the SCN − anionic solute as the local vibrational reporter. Ultrafast IR spectroscopic measurements showed the time constants of the vibrational population decay of SCN − were increased from 14±1 ps to 20±1 ps when the pH of the hydrogels varied from 2.0 to 12.0. Rotational anisotropy measurements further revealed that the rotation of SCN − anionic probe was restricted by the three-dimensional network formed in the hydrogels and the rotation of SCN − anionic probe cannot decay to zero especially at the pH of 7.0. These results are expected to provide a molecular-level understanding of the microscopic structure of the cross-linked polymeric network in the pH stimulus-responsive hydrogels.

研究领域: 生物材料学 · 分子动力学
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STRUCTURE · 2024 · IF 4.4

Structural insights into the unique pH-responsive characteristics of the anti-TIGIT therapeutic antibody Ociperlimab

Jian Sun,Xiangxiang Zhang,Liu Xue,Liang Cheng,Jing Zhang,Xin Chen,Zhirong Shen,Kang Li,Lai Wang,Chichi Huang,Jing Song

TIGIT is mainly expressed on T cells and is an inhibitory checkpoint receptor that binds to its ligand PVR in the tumor microenvironment. Anti-TIGIT monoclonal antibodies (mAbs) such as Ociperlimab and Tiragolumab block the TIGIT-PVR interaction and are in clinical development. However, the molecular blockade mechanism of these mAbs remains elusive. Here, we report the crystal structures of TIGIT in complex with Ociperlimab_Fab and Tiragolumab_Fab revealing that both mAbs bind TIGIT with a large steric clash with PVR. Furthermore, several critical epitopic residues are identified. Interestingly, the binding affinity of Ociperlimab toward TIGIT increases approximately 17-fold when lowering the pH from 7.4 to 6.0. Our structure shows a strong electrostatic interaction between ASP103 HCDR3 and HIS76 TIGIT explaining the pH-responsive mechanism of Ociperlimab. In contrast, Tiragolumab does not show an acidic pH-dependent binding enhancement. Our results provide valuable information that could help to improve the efficacy of therapeutic antibodies for cancer treatment.

研究领域: 免疫学 · 结构生物学 · 肿瘤学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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TALANTA · 2020 · IF 5.339

pH-responsive copper-cluster-based dual-emission ratiometric fluorescent probe for imaging of bacterial metabolism

Shanliang Song,Yue Zhao,Yang Li,Xudong Yang,Dong Wang,Zhuoqi Wen,Minghui Yang,Quan Lin

The profiling of bacterial metabolism is of great significance in practical applications. Therefore, the development of ultrasensitive and highly selective probe for bacterial metabolism detection and imaging is extremely desirable. Herein, a novel dual-emission pH-response bacterial metabolism detection and imaging probe is successfully developed. This probe consists of large-sized and easily separated SiO 2 microspheres , copper nanoclusters (Cu NCs) with red emission, and carbon dots (CDs) with blue emission through in-situ self-assembly. In this system, the fluorescence of Cu NCs is sensitive to pH change due to their obvious aggregation-induced emission enhancement (AIEE) property, while the blue fluorescence of CDs remained almost stable. Therefore, red fluorescence and blue fluorescence are compounded with different fluorescence intensity at different pH values, and their fluorescence ratio is also different. By observation of composite fluorescence color, the visual colorimetric pH detection can be realized with the change of pH value of 0.2 units. Utilizing this system, we are able to detect bacterial metabolism with high signal-to-noise ratio, and it can also be used for bacterial metabolic imaging. Therefore, the pH-responsive Cu NCs-based dual-emission ratiometric fluorescent probe we constructed can provide new ideas for bacterial detection, antimicrobial sterilization, and biological imaging.

研究领域: 生物化学 · 微生物学 · 生物成像
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Nanoscale · 2016 ·Vol. 8 ·期 17 ·9318-9327 · IF 7.76

Hierarchical design of a polymeric nanovehicle for efficient tumor regression and imaging

Jinxia An,Qianqian Guo,Peng Zhang,Andrew Sinclair,Yu Zhao,Xinge Zhang,Kan Wu,Fang Sun,Hsiang-Chieh Hung,Chaoxing Li,Shaoyi Jiang

Effective delivery of therapeutics to disease sites significantly contributes to drug efficacy, toxicity and clearance. Here we designed a hierarchical polymeric nanoparticle structure for anti-cancer chemotherapy delivery by utilizing state-of-the-art polymer chemistry and co-assembly techniques. This novel structural design combines the most desired merits for drug delivery in a single particle, including a long in vivo circulation time, inhibited non-specific cell uptake, enhanced tumor cell internalization, pH-controlled drug release and simultaneous imaging. This co-assembled nanoparticle showed exceptional stability in complex biological media. Benefiting from the synergistic effects of zwitterionic and multivalent galactose polymers, drug-loaded nanoparticles were selectively internalized by cancer cells rather than normal tissue cells. In addition, the pH-responsive core retained their cargo within their polymeric coating through hydrophobic interaction and released it under slightly acidic conditions. In vivo pharmacokinetic studies in mice showed minimal uptake of nanoparticles by the mononuclear phagocyte system and excellent blood circulation half-lives of 14.4 h. As a result, tumor growth was completely inhibited and no damage was observed for normal organ tissues. This newly developed drug nanovehicle has great potential in cancer therapy, and the hierarchical design principle should provide valuable information for the development of the next generation of drug delivery systems.

研究领域: 药剂学 · 肿瘤学 · 生物材料科学
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LANGMUIR · 2015 · IF 4.457

Preparation of Novel Porphyrin Nanomaterials Based on the pH-Responsive Shape Evolution of Porphyrin Microspheres

Wenbo Zhang,Lingbo Xing,Haisheng Wang,Xiujun Liu,Yaqing Feng,Changyou Gao

The shapes and properties of self-assembled materials can be adjusted easily using environmental stimuli. Yet, the stimulus-triggered shape evolution of organic microspheres in aqueous solution has rarely been reported so far. Here, a novel type of poly(allylamine hydrochloride)-g-porphyrin microspheres (PAH-g-Por MPs) was prepared by a Schiff base reaction between 2-formyl-5,10,15,20-tetraphenylporphyrin (Por-CHO) and PAH doped in 3.5-μm CaCO3 microparticles, followed by template removal. The PAH-g-Por MPs had an average diameter of 2.5 μm and could be transformed into one-dimensional nanorods (NRs) and wormlike nanostructures (WSs) after being incubated for different times in pH 1–4 HCl solutions. The rate and degree of hydrolysis had a significant effect on the formation and morphologies of the nanorods. The NRs@pH1, NRs@pH2, and NRs@pH3 were all composed of the released Por-CHO and the unhydrolyzed PAH-g-Por because of the incomplete hydrolysis of the Schiff base. However, the WSs@pH4 were formed by a pure physical shape transformation, because they had the same composition as the PAH-g-Por MPs and the Schiff base bonds were not hydrolyzed. The self-assembled NRs and WSs exhibited good colloidal stability and could emit stable red fluorescence over a relatively long period of time.

CAS / MDL: 109-97-7
研究领域: 材料科学 · 化学
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NANOTECHNOLOGY · 2022 ·Vol. 33 ·期 26 ·265002 · IF 3.953

Highly luminescent pH-responsive carbon quantum dots for cell imaging

Xiaohui Fan,Yang Wang,Bo Li,Chang Shen,Zhengguang Sun,Yuan Zhan,Yuhong Zhang

Carbon quantum dots (CDs) have attracted tremendous interest owing to their idiosyncratic functions and wide-ranging applications. However, it remains a great challenge to empolder an integrated CDs combining high luminescence, biocompatibility and luminescence color tunability for bioimaging via simple approach. In this work, pH-responsive carbon quantum dots (Si-CDs) with high luminescence (quantum yield = 74.8%) were fabricated by one-step hydrothermal method using (3-mercaptopropyl) triethoxysilane (KH-580) as modifier for the first time. The optical properties of the as-prepared Si-CDs can be controlled from obvious green–blue–violet transformation by altering the pH. More importantly, the change is reversible and repeatable. In addition, the Si-CDs have good biocompatibility and chemically inert in vitro cell system simulation. Such non-toxic, environmental friendly, low-cost, inert CDs materials are promising candidates for biomedical and pH-sensitive sensors.

CAS / MDL: 14814-09-6
研究领域: 生物医学 · 材料科学 · 光学
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ACS Applied Nano Materials · 2022 · IF 6.14

Curcumin/Zeolitic Imidazolate Framework-8 Nanoparticle-Integrated Microneedles for pH-Responsive Treatment of Skin Disorders

Seojin Jung,Seokhee Chang,Na-Eun Kim,Seong-O Choi,Yoon-Jae Song,Yue Yuan,Jooyoun Kim

A feasible strategy of on-demand drug delivery for the treatment of dermal inflammation under low-pH conditions is proposed, employing zeolitic imidazolate framework-8 (ZIF-8) as a pH-responsive nanoparticle and curcumin (CCM) as a model drug. To overcome the low bioavailability of topically treated drug, a microneedle (MN) form is used to incorporate CCM and ZIF-8. Taking advantage of the fact that ZIF-8 degrades under acidic conditions, CCM is embedded in porous ZIF-8 nanoparticles such that CCM is released when ZIF-8 comes into contact with an acidic dermal fluid at the inflammation site, and this CCM-encapsulated ZIF-8 (CCMZIF) is incorporated into water-dissolvable poly(vinyl pyrrolidone) MN. The ZIF-8 shows a high loading capacity (∼40.5%) of CCM through chemical bonding and physical adsorption. From in vitro tests with both a buffered solution and porcine skin, CCM from the CCMZIF MN is released in a higher amount at pH 5.0 than at pH 7.4, demonstrating the capability of the pH-responsive release of the drug when needed at inflammatory sites. The analytical investigation conducted here reveals that an acidic environment triggers the structural degradation of ZIF-8, allowing the release of the chemically bonded CCM. Cytotoxicity and stability tests demonstrate the good biocompatibility and bioavailability of ZIF-8. This study highlights the analytical discussion of the encapsulation and release mechanism of CCM in a ZIF-8-implemented MN drug delivery platform. The results demonstrate an advanced on-demand therapeutic strategy for skin disorder treatment.

研究领域: 药剂学 · 生物材料学 · 皮肤病学
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2016 ·Vol. 16 ·期 6 ·5689-5695 · IF 1.338

Effect of the Chain Density and Chain Length on the pH-Responsibility of Poly(acrylic acid) Grafted Cotton

Wu Jindan,Jiang Yuelin,Cai Guoqiang,Wang Zhengliao,He Ju,Wang Jiping

With the development of material science, pH-responsive fabric emerges as a novel material in recent years. Effect of chain density and chain length on the conformation transition of surfaceanchored polymers is a fundamental problem which relates to their functionality. In this work, poly(acrylic acid) (PAA) was grafted onto cotton fabrics through surface-initiated atom transfer radical polymerization (ATRP) technique. The chain length of PAA was modulated by monomer concentration, and the grafting density was regulated by the density of amino groups on the fabric surface. Contact angle analysis, IR measurement and water uptake observation were employed to study the pH-responsive behavior of the PAA modified cotton. Fabrics with polymers of a larger molecular weight and optimal grafting density exhibited better pH-responsibility. This study provided a structure-property fundamental understanding on the important parameters influencing the pH-responsibility of PAA modified cotton fabric.

研究领域: 材料科学 · 高分子化学
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ACS Biomaterials Science & Engineering · 2019 · IF 4.511

Polymer–Doxorubicin Prodrug with Biocompatibility, pH Response, and Main Chain Breakability Prepared by Catalyst-Free Click Reaction

Dian Li,Yue Song,Jinlin He,Mingzu Zhang,Peihong Ni

Click chemistry has increasing applications of the development of polymer materials and modification of drug carriers. The amino–yne click polymerization reacts quickly at room temperature without catalyst, and the enamine bond (-ena-) gained from the reaction is sensitive to acid and can be used to prepare stimulus-responsive polymeric prodrugs. Herein, we report an alkynyl-terminated polymer containing alternately distributed low molecular weight polyethylene glycol (PEG) and hexamethylenediamino (HMDA) linked by enamine bonds, abbreviated as A-P(PEG-alt-HMDA)-A, which was synthesized within 3 h at 35 °C without catalyst. The polymer was verified to have good water solubility, biocompatibility, and acid-sensitive fracturing. Then, a pH-responsive polymeric prodrug (DOX-ena-PPEG-ena-DOX) was further prepared through the amino–yne click reaction between the alkynyl groups of A-P(PEG-alt-HMDA)-A and the amino group of doxorubicin hydrochloride (DOX·HCl). The resulting prodrug can self-assemble into nanoparticles (NPs) in aqueous solution. The pH responsiveness of the prodrug NPs was demonstrated by a stability experiment of NPs and in vitro drug release behavior measurement. The accumulative release of doxorubicin (DOX) was tested with different pH media, which confirmed that the prodrug NPs could effectively dissociate and release drug under a weak acid microenvironment of lysosome/endosome. Subsequently, we investigated cell cytotoxicity and intracellular uptake of the prodrug. It turned out that the prodrug nanoparticles could be internalized into HeLa cells, release original DOX, and efficiently inhibit the proliferation of cancer cells. These results show that the pH-responsive DOX-ena-PPEG-ena-DOX has the potential for use in cancer therapy.

研究领域: 材料科学 · 药学 · 生物医学工程
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