ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Yanping Feng,Lefeng Su,Zhaowenbin Zhang,Yanxin Chen,Muhammad Rizwan Younis,Dongmin Chen,Jinfeng Xu,Chenle Dong,Yumei Que,Chen Fan,Yiren Jiao,Hong Zhu,Jiang Chang,Zhihong Dong,Chen Yang
Nanozymes, emerging nanomaterials for wound healing, exhibit enzyme-like activity to modulate the levels of reactive oxygen species (ROS) at wound sites. Yet, the solo regulation of endogenous ROS by nanozymes often falls short, particularly in chronic refractory wounds with complex and variable pathological microenvironments. In this study, we report the development of a multifunctional wound dressing integrating a conventional alginate (Alg) hydrogel with a newly developed biodegradable copper hydrogen phosphate (CuP) nanozyme, which possesses good near-infrared (NIR) photothermal conversion capabilities, sustained Cu ion release ability, and pH-responsive peroxidase/catalase-mimetic catalytic activity. When examining acute infected wounds characterized by a low pH environment, the engineered Alg/CuP composite hydrogels demonstrated high bacterial eradication efficacy against both planktonic bacteria and biofilms, attributed to the combined action of catalytically generated hydroxyl radicals and the sustained release of Cu ions. In contrast, when applied to chronic diabetic wounds, which typically have a high pH environment, these composite hydrogels exhibit significant angiogenic performance. This is driven by the provision of catalytically generated dissolved oxygen and a beneficial supplement of Cu ions released from the degradable CuP nanozyme. Further, a mild thermal effect induced by NIR irradiation amplifies the catalytic activities and bioactivity of Cu ions, thereby enhancing the healing process of both infected and diabetic wounds. Our study validates that the synergistic integration of photothermal effects, catalytic activity, and released Cu ions can concurrently yield high antibacterial efficiency and tissue regenerative activity, rendering it highly promising for various clinical applications in wound healing.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Yaqi Zhang,Hongliang Wei,Bingya Hua,Chunwang Hu,Wenjing Zhang
Chitosan based hydrogels with multiple stimulus responses have broad application prospects in many fields. Considering the advantages of semi interpenetrating network (IPN) technology and the special temperature and ion responsiveness of polymers containing zwitterionic groups, a semi-IPN hydrogel was prepared through in situ free radical polymerization of N , N -dimethyl acrylamide and [2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide with polyethylene glycol dimethacrylate as a crosslinker and carboxymethyl chitosan as filler. The gel mass fraction and swelling ratio were measured, and the preparation conditions were optimized. The result indicated that the hydrogel possessed a unique thermo-/pH−/ ion-sensitive behavior. The swelling ratio increased with the increase of temperature and ion concentration, and showed a decreasing trend with the increase in pH. In addition, the hydrogel was stable when the stimuli changed. Adsorption behavior of the hydrogel to Eosin Y (EY) was systematically investigated. The adsorption process can be described well by the pseudo-second-order kinetic model and Langmuir isotherm model, indicating that it was a chemical adsorption. The experiments indicated that the hydrogel exhibited good antifouling and reusability features. Therefore, the semi-IPN hydrogel with antifouling properties and thermo-/pH−/ion-sensitivity can be easily manufactured is expected to find applications in water treatment fields.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 9
·2500-2513
·
IF 7.3
Chao Xue,Xiaoyun Yi,Yuebei Yang,Feng Jiang,Hua Yin,Zhi Dang
It has been widely believed that the adsorption mechanism of cadmium on iron (oxyhydr)oxide is solely the inner-sphere complexation based on extended X-ray absorption fine structure spectroscopy (EXAFS). However, these results were obtained at specific experiment settings (high ionic strength and high cadmium surface loading). In natural cadmium-polluted soil and water environments, such as acidic mineral drainage (AMD) areas, the pH/ionic strength is relatively low. Therefore, under practical conditions, the bonding pathway of cadmium could be different and may comprise other potential mechanisms. This work focuses on the proportion of different cadmium sorption pathways on goethite by employing a chemical extraction procedure. Cadmium is mostly adsorbed on goethite via electrostatic adsorption and inner-sphere complexation in a pH range of 5.5–7.5 under 10 mM ionic strength conditions. Through quantitative calculation, it is confirmed that the amount of Mg(NO3)2-extracted cadmium can refer to the content of electrostatically adsorbed cadmium. Two types of surface hydroxyls contributed differently to inner-sphere complexed Cd(II) at different pH values, and the emergence of surface-induced precipitates at higher pH could also be included in the retention mechanism. The behavior of electrostatically adsorbed cadmium and inner-sphere complexed Cd(II) was found to be different at different pH values when sulfate was introduced. Based on zeta potential and total reflectance Fourier transform infrared spectral analyses, sulfate would modify the surface charge of goethite, but, moreover, sulfate might form pseudo ion-group species with cadmium, which could influence the sorption pathway of cadmium.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2023
·
IF 4.7
Liang Yang,Yao Wang,Yijia Liang,Haibin Deng,Jun Wang,Yuhao Dai,Fuyou Guo,Hong Zhou,Shili Li,Wei Ding
Ralstonia solanacearum ( R. solanacearum ) is one of the most devastating pathogens in terms of losses in agricultural production. Bentonite (Bent) is a promising synergistic agent used in development of effective and environmentally friendly pesticides against plant disease. However, the synergistic mechanism of Bent nanoclays with benzothiazolinone (BIT) against R. solanacearum is unknown. In this work, acid-functionalized porous Bent and cetyltrimethylammonium bromide (CTAB) were employed as the core nanoclays, and BIT was loaded into the clay to form BIT-loaded CT-Bent (BIT@CT-Bent) for the control of bacterial wilt disease. BIT@CT-Bent exhibited pH-responsive release behavior that fit the Fickian diffusion model, rapidly releasing BIT in an acidic environment (pH = 5.5). The antibacterial effect of BIT@CT-Bent was approximately 4 times greater than that of the commercial product BIT, and its biotoxicity was much lower than that of BIT under the same conditions. Interestingly, R. solanacearum attracted BIT@CT-Bent into the nanocomposites and induced cytoplasmic leakage and changes in membrane permeability, indicating an efficient and synergistic bactericidal effect that rapidly reduced bacterial density. In addition, BIT@CT-Bent significantly inhibited R. solanacearum biofilm formation and swimming activity, by suppressing the expression of phcA , solR and vsrC . Indeed, exogenous application of BIT@CT-Bent significantly suppressed the virulence of R. solanacearum on tobacco plants, with control effect of 75.48%, 72.08% and 66.08% at 9, 11 and 13 days after inoculation, respectively. This study highlights the potential of using BIT@CT-Bent as an effective, eco-friendly bactericide to control bacterial wilt diseases and for the development of sustainable crop protection strategies.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Yajun Hou,Shanshan Wang,Baojuan Deng,Yun Ma,Xing Long,Chengrong Qin,Chen Liang,Caoxing Huang,Shuangquan Yao
As an environmentally friendly lignocellulosic biomass separation technology, hydrothermal pretreatment (HP) has a strong application prospect. However, the low separation efficiency is a main factor limiting its application. In this study, the poplar components were separated using HP with ferric chloride and pH buffer (HFB). The optimal conditions were ferric chloride concentration of 0.10 M, reaction temperature of 150 °C, reaction time of 15 min and pH 1.9. The separation of hemicellulose was increased 34.03 % to 77.02 %. The pH buffering resulted in the highest cellulose and lignin retention yields compared to ferric chloride pretreatment (FC). The high efficiency separation of hemicellulose via HFB pretreatment inhibited the degradation of xylose . The hydrolysate was effectively reused for five times. The fiber crystallinity index reached 60.05 %, and the highest C/O ratio was obtained. The results provide theoretical support for improving the efficiency of HP and promoting its application.
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MATERIALS & DESIGN
·
2023
·
IF 8.4
Hao Xue,Fei Liu,Ze Wang,Delei Liu,Liang Zhou,Wenbo Su,Shichao Niu,Zhiwu Han,Luquan Ren
Responsive photonic crystals (PCs) with bio-inspired microstructures and tailorable functionalities are of critical importance for their potential applications in diverse fields such as biological detection, sensing, decoration, anti-counterfeiting, etc. However, limited by preparation technologies and design theories, it is still a challenge to accurately and uniformly deposit smart responsive materials on natural PC structures and achieve dual stimulus response. Herein, a simple and rapid in situ polymerization method is presented for preparing dual-responsive PCs with ultra-precise micro-/nanoscale hierarchical structures. Exposure of the reaction site by deacetylation of Morpho butterfly wings allows in situ polymerisation of poly ( N -isopropylacrylamide- co -acrylic acid) (P(NIPAAM- co -AAc)) on the surface of the natural photonic structure. The obtained P(NIPAAM- co -AAc) photonic crystals (P(NIPAAM- co -AAc)-PCs) exhibited a dual response to pH and temperature reversibility. In addition, the synergistic effect of the structures and materials on the optical response of the natural PCs is revealed. This work allows the combination of natural hierarchical PC structures with smart hydrogel to achieve an optical response to pH and temperature, thus opening up the channels for responsive PC to multiple stimulus responses.
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DESALINATION
·
2023
·
IF 9.9
Yuyan Hai,Xin Wen,Rui Ma,Can He,Xue Yang,Rihua Xiong,Jingyun Chen,Qiaoyi Sun
An in-situ chemical cross-linking rejuvenation technique for reverse osmosis (RO) membranes was developed and investigated utilizing pH-responsive polymer with multiple carboxyl groups to improve the salt rejection and performance stability of end-of-life RO membranes. Polyacrylic acid (PAA) was used as a rejuvenating agent to cross-link with amino groups on the degraded RO membrane through EDC/NHS activated reaction. Indicated by ATR-FTIR, XPS , Zeta potential and SEM analyses, the covalent bonds between carboxyl groups and amino groups were generated on the PAA-rejuvenated membrane. The end-of-life RO membrane elements with an average NaCl rejection of 92.68 % could be recovered to 97.26 % by PAA rejuvenation. As a result of pH responsivity , PAA-rejuvenated membranes exhibit excellent rejection stability after continuous 12 cycles of alkali and acid alternate cleaning. The adjustable salt rejection and the durability of PAA-rejuvenated membrane elements were validated in real water tests for 185 days at a coal mine water treatment plant , indicating the practical application potentiality. The effects of initial end-of-life RO membrane condition on PAA rejuvenation are also provided.
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ACS Applied Bio Materials
·
2023
·
IF 4.7
Minghua Zhou,Beibei Tian,Yingcui Bu,Zhichao Wu,Jianhua Yu,Sen Wang,Xianshun Sun,Xiaojiao Zhu,Hongping Zhou
Considering the chemodynamic therapy and chemotherapy independent of external stimulus witnessing great advantage in the clinical translation, developing a smart nanoplatform that can realize enhanced chemo/chemodynamic synergistic therapy in the tumor microenvironment (TME) is of great significance. Herein, we highlight the enhanced pH-responsive chemo/chemodynamic synergistic cancer therapy based on in situ Cu2+ di-chelation. The alcohol-withdrawal drug disulfiram (DSF) and chemotherapeutic drug mitoxantrone (MTO) were embedded into PEGylated mesoporous CuO (denoted as PEG-CuO@DSF@MTO NPs). The acidic TME triggered the collapse of CuO and the concurrent release of Cu2+, DSF, and MTO. Then, the in situ complexation between Cu2+ and DSF, as well as the coordination between Cu2+ and MTO not only prominently enhanced the chemotherapeutic performance but also triggered the chemodynamic therapy. In vivo mouse model experiments demonstrated that the synergistic therapy can remarkably eliminate tumors. This study provides an interesting strategy to design intelligent nanosystems, which could proceed to clinical translations.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wen Guo,Dinglingge Cao,Weihan Rao,Tao Sun,Yiman Wei,Yang Wang,Lin Yu,Jiandong Ding
Local anesthetics are important for the treatment of postoperative pain. Since a single injection of the solution of a drug such as bupivacaine (BUP) works only for a few hours, it is much required to develop a long-term injectable formulation that maintains its efficacy for more than 1 day. Herein, an intelligent copolymer hydrogel loaded with BUP microcrystals was invented. The biodegradable block copolymer was synthesized by us and composed of a central hydrophilic poly(ethylene glycol) (PEG) block and two hydrophobic poly(lactide-co-glycolide) (PLGA) blocks. The aqueous system of the amphiphilic copolymer underwent a sol–gel transition between room temperature and body temperature and, thus, physically gelled after injection. Considering the decrease of solubility of BUP with the increase of pH and the internal acidic environment due to the hydrolysis of PLGA, calcium carbonate (CaCO3) powder was introduced as a pH regulator. Then, the internal pH was found to be nearly neutral and many BUP microcrystals were dispersed in the gel network. In this way, BUP had achieved a sustained release out of the thermogel. The maximum possible effect (MPE) in a rat sciatic nerve blockade model was used to describe the sensory blockade effect. In vivo analgesic effects evaluated with a hot plate experiment of rats demonstrated that the thermogel encapsulated with BUP microcrystal and CaCO3 powder significantly prolonged analgesia up to 44 h, the duration time with respect to 50% MPE. The intramuscularly injected implant exhibited biocompatibility in histological analyses. Besides, the untreated leg of the rats was not influenced by the treated leg, indicating no obvious systematic anesthesia of this hydrogel formulation. Such an intelligent and composite formulation represents a potential strategy for long-acting analgesia therapy.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 50
·2305975
·
IF 19
Shaopeng Gan,Hui Li,Xu Zhu,Xilu Liu,Kangxing Wei,Lei Zhu,Baojun Wei,Xiaoming Luo,Jianqiang Zhang,Qingzhong Xue
The tunable wettability by pH-stimulus has great potential in liquid adhesion, transport, collection, and separation due to its rapid response and wide control range. However, achieving pH-regulated wettability on the selected region of material without acid–base contamination presents a distinct challenge for the existing methods. Here, a scalable conductive network membrane is prepared with switchable wettability by regulating interfacial pH. The generation and diffusion of interfacial pH on the selected region of the membrane are regulated through the confinement electrolysis process, which is adapted to both spatial arrangements of the conductive network and the electrical potential. By regulating the interfacial pH (>13), the wettability of the selected region can change from superhydrophobicity (Water contact angle = 150°) to superhydrophilicity/underwater superoleophobicity (Water contact angle = 0°) without additional reagent in 30 s under 15 V. Based on the switchable wettability and precise controllability, the prepared membrane can efficiently realize on-demand oil–water separation (>99%) and in situ extraction-back extraction. The membrane with switchable wettability is programable and free of acid–base contamination, which may have broad practical application potential in intelligent fluid-related systems.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
·
2023
·
IF 5
Fenglin Huang,Sisi Yang,Hao Wang,Peiwen Zhao,Bo Zhou,Bo Cheng,Siyan Dong,Jing Yang,Binbin Li,Xinyu Wang
Multi-functional drug-loaded microsphere system can overcome drug resistance and selectively transport drugs to tumor tissues, thus reducing the toxicity to normal tissues, and can achieve long-term effect through drug release, thus becoming a new way to treat tumor-related diseases. Poly (lactic-co-glycolic acid) PLGA/gelatin composite microspheres were prepared by an emulsion solvent evaporation technique. The microsphere shows that it has positive charge and pH response, which is more suitable for the weak acid environment of tumor and has certain targeting effect. At the same time, the scanning electron microscope showed that the surface was loose and rough, and the internal structure was porous, and the morphology was novel. In addition, UV spectrophotometer was used to test the drug loading rate and encapsulation efficiency of the microspheres. For smooth PLGA and PLGA/gelatin microspheres, the latter has better drug loading rate of 11.66% and encapsulation rate of 89.22%. The results showed that among pure paclitaxel , PLGA and PLGA/gelatin microspheres, the latter had the better than performance in the lethal rate of lung cancer cells and could achieve the goal of continuous lethal. Therefore, the preparation of porous drug-loaded microspheres in this study is pH responsive, and can achieve the goal of safe, targeted and efficient inhibition of cancer cell proliferation , and inspire the follow-up anti-cancer research.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 23
·7722-7731
·
IF 6.4
Xin Chen,Jianlong Ji,Yubo Peng,Zhipeng Gao,Min Zhao,Bin Tang,Ying Liu
With the advantages of miniaturization, simple device structure, and fast response, organic electrochemical transistors (OECTs) have become an emerging platform for developing wearable pH sensors for real-time human health monitoring. However, the application of devices is limited because they use water electrolytes. This paper proposed a feasible pH-sensitive OECT with a flexible BTB dye-embedded ion-gel dielectric layer. The real-time H+ detection performances of the devices, the effects of the BTB content in the ion-gel layer and gate voltages on the pH sensing capability, as well as the property–microstructure relationship of the ion-gel were investigated. The experimental results showed that the pH-sensitive OECT integrated with a 15 wt% BTB ion-gel layer exhibited outstanding H+ ion sensitivity and linear response properties at a gate voltage of −0.4 V. The pH-sensitive ion-gel modified OECT presented here provides a novel strategy for developing wearable pH sensors with high real-time monitoring characteristics.
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