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NPG Asia Materials · 2016 ·Vol. 8 ·期 12 ·e335 · IF 8.772

The pH-switchable agglomeration and dispersion behavior of fluorescent Ag nanoclusters and its applications in urea and glucose biosensing

Dong Jiang Xue,Gao Zhong Feng,Zhang Ying,Li Bang Lin,Zhang Wei,Lei Jing Lei,Li Nian Bing,Luo Hong Qun

Water-soluble fluorescent Ag nanoclusters (Ag NCs) with distinct pH-switchable agglomeration and spectral signal responses are prepared using a facile etching method. Increased and decreased pH cause the Ag NCs to switch between agglomeration and dispersion, accompanied by decreases in and recoveries of fluorescence intensity and absorbance. The pH switchable behavior of the Ag NCs is attributed to carboxyl groups on the nanocluster surface that are rich in the citrate and amido functional groups of ligands (glutathione), creating an easily formed, weak molecular interaction among Ag NCs (for example, hydrogen bonding) and maintaining a balance in the colloidal solution, whereas a change in pH will disrupt the balance, leading to the reversible agglomeration of Ag NCs and the switchable spectral signal response. In addition, because urea and glucose can change the pH of a solution by producing NH 3 and gluconic acid in enzyme-catalyzed reactions, the pH-switchable behavior of the Ag NCs is used to develop them as an optical probe to establish a regenerated biosensing platform for the sensitive and selective detection of urea and glucose, and the test results are satisfactory.

研究领域: 生物化学 · 分析化学 · 纳米材料科学
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Soft Matter · 2019 ·Vol. 15 ·期 27 ·5529-5536 · IF 3.399

pH-Switchable IFT variations and emulsions based on the dynamic noncovalent surfactant/salt assembly at the water/oil interface

Han Jia,Xu Leng,Peng Lian,Yugui Han,Qiuxia Wang,Shaoyan Wang,Tunan Sun,Yipu Liang,Pan Huang,Kaihe Lv

Additional HCl can facilely control the dynamic noncovalent interaction between anionic surfactant sodium dodecyl benzene sulfonate (SDBS) and additional organic matter, 4,4′-oxydianiline (ODA), at the water/oil interface. At low HCl concentration (ODA/HCl molar ratio (r) = 1 : 1.5, [ODA] = 250 mg L−1), the ODA+ ions effectively enhanced the SDBS ability to reduce the water/oil interfacial tension (IFT) by about two orders of magnitude, while the (SDBS)2/ODA2+ gemini-like surfactants could be constructed at a relatively high HCl concentration (r = 1 : 4, [ODA] = 250 mg L−1), which could largely reduce the IFT to 1.19 × 10−3 mN m−1. Molecular simulation was employed to explore the interfacial activity of ODAn+ (ODA+/ODA2+) ions and the SDBS/ODAn+ interaction. The control experiments used another three surfactants to verify the proposed model. The pH-switchable gradual protonation of amino groups in ODA molecules determined the SDBS/ODA interfacial assembly, which was responsible for the reversal of IFT variations and the related emulsion behaviors.

研究领域: 化学 · 界面科学 · 胶体与表面化学
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FUEL · 2018 · IF 4.908

pH-switchable and CO2-switchable viscoelastic fluids based on a pseudo-hydrophobically associating water-soluble polymer

Haiyang Tian,Hongping Quan,Zhiyu Huang,Silong Jiang

The non-hydrophobically associating water-soluble polymer (DPAM) of acrylamide (AM) and dimethylamino propyl methacrylamide (DMAPMA) was synthesized. Then pH-switchable and CO 2 ‑switchable viscoelastic liquids based on DPAM and anionic surfactant sodium dodecyl sulfate (SDS)(referred to as DPAM-SDS) were developed. When minor HCl aqueous solution was added into the DPAM and SDS aqueous mixture or CO 2 was bubbled into it, the tertiary amine groups of DPAM were protonated to form quaternary ammonium groups, some of which in the same quaternary ammonium groups of DPAM “bridged” some SDS through noncovalent electrostatic attraction, behaving like a pseudo-hydrophobically associating water-soluble polymer and forming viscoelastic fluids as checked through environmental scanning electron microscope(ESEM) and rheology. Upon removing of CO 2 or back of pH by minor NaOH aqueous solution, the quaternary ammonium species of DPAM were deprotonated back to tertiary amine groups, separating the pseudo-hydrophobically associating water-soluble polymer back to DPAM and SDS molecules, which resulted in forming low-viscosity water solution. The switchable viscoelastic conversion can be repeated.

CAS / MDL: 2997-92-4
研究领域: 化学工程 · 材料科学
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Nanoscale · 2017 ·Vol. 9 ·期 40 ·15673-15684 · IF 7.367

Nanodiamonds as pH-switchable oxidation and reduction catalysts with enzyme-like activities for immunoassay and antioxidant applications

T. M. Chen,X. M. Tian,L. Huang,J. Xiao,G. W. Yang

Nanodiamonds (NDs) have recently become a focus of interest from the viewpoints of both science and technology. Their intriguing properties make them suitable as biologically active substrates, in biosensor applications as well as diagnostic and therapeutic biomedical imaging probes. Here, we demonstrate that NDs, as oxidation and reduction catalysts, possess intrinsic enzyme mimetic properties of oxidase, peroxidase and catalase, and these behaviors can be switched by modulating the pH value. NDs not only catalyze the reduction of oxygen (O2) and hydrogen peroxide (H2O2) at acidic pH, but also catalyze the dismutation decomposition of H2O2 to produce O2 at alkaline pH. It was proposed that the molecular mechanism of their peroxidase-like activity is electron-transfer acceleration, the source of which is likely derived from oxygen containing functional groups on their surface. Based on the color reaction, a nanodiamond-based enzyme linked immunosorbent assay (ELISA) was established for the detection of immunoglobulin G (IgG). Surprisingly, NDs display an excellent antioxidant activity due to the protective effect against H2O2-induced cellular oxidative damage. These findings make NDs a promising enzyme mimetic candidate and expand their applications in biocatalysis, bioassays and nano-biomedicine.

研究领域: 材料科学 · 生物技术 · 生物化学 · 纳米技术
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Nanoscale · 2018 ·Vol. 10 ·期 14 ·6660-6670 · IF 7.233

Room temperature synthesis of pH-switchable polyaniline quantum dots as a turn-on fluorescent probe for acidic biotarget labeling

Yanfeng Liu,Yin Ding,Huilin Gou,Xin Huang,Guiyang Zhang,Qi Zhang,Yunzhong Liu,Zhen Meng,Kai Xi,Xudong Jia

The synthesis of well-defined light-element-derived quantum dots (LEQDs) with advanced optical properties under mild conditions is highly desirable yet challenging. Here, a polyaniline (PANI) structure is introduced into carbon-rich LEQDs to yield well-defined, fluorescent polyaniline quantum dots (PAQDs), PAQD24, through a one-pot room temperature reaction. The mild synthetic conditions effectively minimize the defects introduced during the conventional synthesis and endow PAQD24 with desirable optical properties, including a narrow emission band (full width at half maximum = 55 nm), an optimal quantum yield of 32.5% and two-photon fluorescence. Furthermore, the bandgap of PAQD24 is highly sensitive toward pH variations in the near-neutral region, due to the proton doping and dedoping of the PANI structure. Such unique properties together with its fine bio-compatibility enable the application of this material as a turn-on fluorescent probe for the labeling of acidic biotargets from sub-cellular to organ levels, providing potential applications in diagnosis and surgery guidance for certain diseases.

研究领域: 材料科学 · 纳米技术 · 生物医学工程 · 分析化学
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2021 · IF 5.268

Insight into the mechanism and formation process of bioinspired poly(amino acid)/polyphenol capsules engineered with fast pH switchable permeability

Shaoyin Wei,Daozhen Zhou,Jianghui Qin,Bo Peng,Xingjie Zan

Capsules have hollow cores and closed wall structures, and they have attracted considerable interest due to their wide applications and significance in life science. The engineering process of bioinspired capsules and related applications have earned heavy concerns. However, the mechanism of capsule formation is often ignored. Herein, based on polyornithine (POR) and tannic acid (TA), two facile strategies to engineer bioinspired capsules were proposed, and the formation mechanisms were deeply explored. We found that the oxidized state of TA had a profound influence not on the thickness or permeability of the formed capsule but on the mechanism and generation process. Compared to TA/POR capsules produced from TA without oxidization ( TA/POR), capsules produced from TA with preoxidization ( o TA/POR) had thicker shells with higher impermeability. The dominant construction mode in the shells of TA/POR capsules was electrostatic interactions but became Schiff base bonds in o TA/POR capsules. The permeability of o TA/POR displayed pH reversibility and strong pH dependence, with 100% permeability at lower pH and 100% impermeability at pH 7, completing loading/releasing kinetics in minutes at pH 4. We believe these findings contribute to knowledge of bioinspired capsules from engineering processes and formation mechanisms, extending their applications in various fields, such as in drug delivery, artificial cells, and sensors.

研究领域: 材料科学 · 化学 · 生物技术 · 药学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

pH-Switchable Antimicrobial Supramolecular Hydrogels for Synergistically Eliminating Biofilm and Promoting Wound Healing

Huimin Chen,Jing Cheng,Xixi Cai,Jinzhi Han,Xu Chen,Lijun You,Caihua Xiong,Shaoyun Wang

Biofilm infection will cause chronic inflammation and hinder the normal healing process of wound. Here, based on the self-assembly of three designed amphiphilic pentapeptides named EK, GG, and DR, pH-switchable antibacterial hydrogels with amphiphilic fiber network are used for the eradication of biofilms and the rescue of delayed healing in infected wounds. These pentapeptides-based hydrogels exhibit an acidic pH-switchable antimicrobial effect and are biocompatible at neutral pH. Additionally, supramolecular nanofiber networks with physical cross-linking with thermosensitive polymers (PNIPAm) and loaded antibacterial oregano oil are further developed. In vitro experiments indicate that the antimicrobial activity of hydrogels comes from the disassembly of acidic pH-dependent nanofiber network and activated release of pentapeptides and oregano oil, which achieves synergistic biofilm eradication. Remarkably, DR-based supramolecular hydrogel improves the healing efficiency of the full-thickness wound of skin in vivo, which is manifested by increased wound closure rate, reduced inflammatory response, faster angiogenesis, and collagen deposition in the wound, exhibiting great potential as wound dressing. The proposed synergistic strategy of inhibiting biofilm formation and activating healing may provide an efficient method for the treatment of clinically infected wounds.

CAS / MDL: 25316-40-9 8007-11-2
研究领域: 材料科学 · 生物材料 · 药学 · 伤口愈合 · 感染控制
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2023 · IF 5.2

Synthesis of Mn-Prussian blue analogues with multi-enzyme activity and related application for alcohol detection

Yihang Qian,Yuan Chen,Guowei Yang

Manganese-contained Prussian blue analogues (Mn-PBAs) have a rigid and open 3D framework and adjustable redox potential , coupled with nontoxic nature, they could be effectively applied in various medicinal and biomedical fields. In this study, we reported the nanozyme activity of Mn-PBA nanoparticles . It was found that Mn-PBA nanoparticles possess peroxidase (POD)-, urate oxidase (UOD)- and catalase (CAT)-like enzymes, and this multi-enzyme activity is pH-switchable. The working mechanism of Mn-PBA nanoparticles mimicking peroxidase to oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of hydrogen peroxide (H 2 O 2 ) was pursued. In this process, Mn-PBA nanoparticles accelerate the decomposition of H 2 O 2 into •OH, so that •OH catalyzes the oxidation of TMB. Based on the color reaction and the cascade reaction , we constructed a platform that utilizes Mn-PBA nanoparticles to detect alcohol concentration. This platform has a wide detection range and high detection accuracy, as well as excellent detection specificity. For example, 25 μM-2.5 mM concentration of alcohol can be measured accurately with a good linearity overall, and the limit of detection of the alcohol concentration can reach low to 3.17 μM. These studies prove that the application of Mn-PBA nanoparticles in biomedicine and detection has bright prospects.

CAS / MDL: 14459-95-1 54827-17-7
研究领域: 纳米技术 · 生物化学 · 生物医学工程 · 分析化学
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ADVANCED MATERIALS · 2025 · IF 26.8

Lattice-Reconstructed Ru-Clusters on FeOOH-Based Self-Adaptive Artificial Peroxisome with Programmed ROS Regulation for Infectious and Inflammatory Chronic Wounds

Heng Yang,Xiaoke Jia,Ting Wang,Jiangge Li,Wei Geng,Mohsen Adeli,Tian Ma,Yang Gao,Chong Cheng,Weifeng Zhao

Chronic refractory wounds present substantial clinical difficulties, owing to their complex wound microenvironments featuring bacterial colonization, sustained inflammation, and deficient angiogenesis. Existing treatment options often fall short of concurrently overcoming these interconnected obstacles, underscoring the demand for integrated therapeutic platforms that combine antimicrobial, anti-inflammatory, and pro-angiogenic properties. Drawing inspiration from natural peroxisomes, a lattice-reconstructed Ru-clusters are designed on FeOOH-based self-adaptive artificial peroxisome with programmed reactive oxygen species (ROS) regulation for infectious and inflammatory chronic wounds. Within this architecture, electron-rich Ru clusters and hole-rich FeOOH domains establish an efficient electron-transfer network. Density functional theory calculations demonstrate that this distinctive electronic structure lowers reaction energy barriers, enabling pH-switchable ROS-catalytic behaviors. Under acidic wound pH, LR-RuC@FeOOH catalyzes ROS generation to disrupt bacterial metabolism and eliminate infections, while under neutral conditions, it efficiently scavenges ROS to alleviate oxidative stress and support tissue repair, enabling a logically sequenced therapeutic progression from infection control to inflammation resolution. In vivo experiments using diabetic foot ulcers confirmed that LR-RuC@FeOOH significantly enhanced bacterial clearance, attenuated inflammatory responses, stimulated neovascularization, and accelerated wound closure. These results position LR-RuC@FeOOH as an artificial peroxisome with stage-specific therapies and promising translational potential for the treatment of refractory diabetic wounds and other infection-related pathologies.

研究领域: 生物医学工程 · 伤口愈合 · 纳米医学 · 活性氧调控 · 抗菌治疗 · 炎症性疾病
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

pH-Switchable Pickering Interfacial Biocatalysis: One-Pot Enzymatic Synthesis of Phytosterol Esters with Low-Value Rice Bran Oil

Tao Yang,Yufei Zhang,Liujia Xu,Hao Zhu,Juntao Zhang,Zheng Guo,Fenghong Huang,Mingming Zheng

Herein, a pH-switchable Pickering interfacial biocatalysis (PIB) system is proposed and applied to a solvent-free biphasic biocatalysis. The oil-in-water emulsion was stabilized by amine-functionalized hollow mesoporous silica nanospheres (HMSS-N), which is functioned as emulsifiers of PIB and carriers of lipase AYS. The smart emulsifiers exhibited switch of the surface wettability behaviors in response to abrupt changes of pH. Under the optimality conditions, the immobilized lipase loading amount, activity, and expressed activity were 174.1 mg g–1, 9073 U g–1, and 52.1 U g–1 protein, respectively, at pH 6. Based on it, the hydrolysis of rice bran oil and esterification with phytosterols to produce phytosterol esters (PEs) were successfully performed. Compared with the conventional free enzyme one-phase system, the PIB system displays a higher reaction efficiency (catalytic efficiency value 6.88 mmol g–1 h–1, 20-fold enhancement). In addition, the system maintains 95% residual activity after 10 reaction cycles with 38.3 g products/g biocatalyst average productivity, complying with the requirements of industry-accepted standards. In each cycle, the demulsification is realized simply by in situ pH regulation. Therefore, this paper provides a powerful and green platform for oil–fat modification and stimuli-responsive interfacial biocatalysis with the advantages of a high efficiency, sustainability, a solvent-free process, and multi-recyclability.

研究领域: 生物技术 · 化学工程 · 环境科学 · 材料科学
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LANGMUIR · 2021 · IF 3.882

pH-Switchable Latexes Based on the Nonionic Amphiphilic Diblock Copolymer with a Chargeable End-Group on the Core-Forming Block

Jiazhou Jin,Shanshan Dai,Xiaojiang Li,Ya Liu,Hongsheng Lu

Reversible addition–fragmentation transfer (RAFT) dispersion polymerization of styrene was performed in an ethanol–water mixture using a Z-group carboxylated poly(N-acryloylmorpholine) (PNAM) macro-RAFT agent, and dialysis was performed against water to produce the PNAMx-PSy-COOH (PS = polystyrene) diblock copolymer latexes. This new formula is developed for the fabrication of pH-switchable copolymer latexes through an end-group response approach. The PNAM44-PS134-COOH latex is unstable at suitably low pH values (pH ≤ 4), and these aggregated spherical nanoparticles are redispersed successfully by adding base as determined by analysis of their dynamic light scattering (DLS) diameters and transmission electron microscopy (TEM) data. Negative zeta potential (−19.4 mV at 0.02% w/w) of the original latex indicated that carboxylic acid end-groups were anchored on the surface of the PS core via the polymerization-induced self-assembly (PISA) process and exposed to the solvent. Protonation of carboxylate groups reduces the degree of hydration of the PS core with a great impact on the free energy of the core/solvent interface, inducing the aggregation of PNAM44-PS134-COOH latex particles. A comparative experiment where the carboxylic acid end-group is designed on the PNAM stabilizer block proves that no pH-switchable behavior occurs in this case. Moreover, the vesicle-like nanoparticles composed of PNAM44-PS428-COOH copolymers have an apparently anionic character (zeta potential ≈ −33.5 mV at 0.02% w/w) and are still pH-switchable with a lower critical flocculation point (pH 2–3). More importantly, the latex composed of PNAM118-PS151-COOH diblock copolymers is insensitive to the solution pH.

研究领域: 聚合物化学 · 材料科学 · 纳米技术 · 胶体科学
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Advanced Materials Interfaces · 2020 ·Vol. 7 ·期 14 ·2000329 · IF 4.948

The Bioinspired Facile Method to Efficiently Generate Diverse Proteinosomes with pH Switchable Permeability

Jianghui Qin,Shaoyin Wei,Hongyan Xu,Liwen Wang,Pengyan Hao,Bo Peng,Yagang Zhang,Pengzhong Shi,Xingjie Zan

Proteinosome, characterized by an inner aqueous cavity wrapped by membrane with embedded protein, is one of the most attractive structures, has huge potential applications on drug delivery, tissue engineering, catalysis, synthetic biology, artificial cells, engineering of the biomachines, biosensors, and biodevices, etc. Here, inspired by polyphenol chemistry, a facile and universal method is presented to fabricate the diverse proteinosomes, with independence on the amino acid sequence, isoelectric points, molecular weight ( M w ), wettability, and functional domains of applied proteins. Besides, the materials employed here are green and cost-effective, and the method developed here is efficient and easily operated without any expensive equipments. The proteinosomes and the mechanism of generating proteinosomes are well characterized and analyzed by various techniques. The permeability of generated proteinosomes is underlined, which not only shows dependence on the applied proteins but also the M w of diffused molecules. In addition, the permeability can be reversibly switched on/off in 100% by environmental pH. Capitalizing the facility and university of this method, it is believed it paves the way of the proteinosomes to multiple potential applications, such as drug delivery, micro-/nanoreactors, tissue engineering, catalysis, biosensor, etc.

研究领域: 材料科学 · 纳米技术 · 生物技术 · 药学 · 生物医学工程 · 化学工程 · 合成生物学
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