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SURFACE & COATINGS TECHNOLOGY · 2023 · IF 5.4

Fabrication of fluorine-free pH-responsive functionalized mesh via thiol-ene click chemistry for oil-water separation

Meng Zhu,Yucheng Liu,Ahmad Rahimpour,Yong Liu,Mohtada Sadrzadeh

pH-responsive materials with switchable wettability provide a novel strategy for oil-water separation applications. The thiol-ene click chemistry method was used to fabricate pH-responsive stainless-steel meshes (SSM) by grafting long-chain alkanes with carboxyl ( COOH) and methyl ( CH 3 ) groups onto the SSM surface. The pH-responsive SSM showed excellent separation efficiency (>97 %) in both superhydrophobic and superhydrophilic states, which was unaffected by the presence of NaCl in the mixed solution. The pH-responsive SSM demonstrated a fast response within 3 s and a wide pH range after pre-wetting in an alkaline solution (pH spike) due to the presence of long carbon chains containing COOH and CH 3 groups. Moreover, the mesh underwent antifouling, ultraviolet light (UV) resistance, and mechanical resistance tests, showing excellent durability and stability. The water contact angle (WCA) remained higher than 130° after 24 h of UV exposure and six rounds of wear experiments. Furthermore, the oil-water separation efficiency remained above 98.4 % after 20 cycles. The in-depth investigations conducted in this study will provide valuable insights into developing pH-responsive membranes to meet diverse demands, such as water rejection or oil rejection under complex conditions.

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Small · 2023 ·Vol. 19 ·期 52 ·2305343 · IF 13.3

Scalable Synthesis of Ir Cluster Anchored on Porous Hollow Carbon Nanobowls for Enhancing pH-Universal Hydrogen Evolution

Yingxiu Zhao,Qiyan Sun,Xinyuan Zhou,Zhiyao Duan,Chuanfang Zhang,Guang-Rui Xu,Dianxing Ju,Lei Wang

Design high-loading with superior activity and high atomic efficiency has consistently been a new frontier of heterogeneous catalysis while challenging in synthetic technology. In this work, a universal solid-state strategy is proposed for large scalable production of high-loading Ir clusters on porous hollow carbon nanobowls (Ir CSs/PHCNBs). The strong electronic interaction between metallic Ir cluster and C on PHCNBs leads to electron redistribution, which significantly improves the electron transfer rate on the interface. The obtained Ir CSs/PHCNBs only require overpotentials of 35, 34, and 37 mV for the hydrogen evolution reaction (HER) with stable outputting of 10 mA cm −2 under acidic, alkaline, and neutral conditions, respectively, which exceeds the state-of-the-art HER electrocatalysts. Meanwhile, the Tafel slopes of Ir CSs/PHCNBs for the HER process are 23.07, 48.76, and 28.95 mV dec −1 , greatly lower than that of PHCNBs (152.73, 227.96, and 140.29 mV dec −1 ) and commercial Pt/C (20%) (36.33, 66.10, and 36.61 mV dec −1 ). These results provide a new strategy for the universal synthesis of clusters catalysts and insight into understanding the interface effects between clusters and carbon substrate, facilitating the industrial application of hydrogen production.

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Small · 2023 ·Vol. 19 ·期 48 ·2304258 · IF 13.3

CDs Regulated Sulfur-Based Flexible Electrode with Range pH Values for Efficient and Durable Hydrogen Evolution Reaction

Weiju Hao,Rikai Liang,Shiheng Liang,Bonan Liu,Yunlong Qian,Ding-Kun Ji,Guisheng Li

How to mildly structure a high intrinsic activity and stable catalytic electrode to realize long-term catalytic water splitting to produce hydrogen at a wide range of pH values at industrial high current is a challenge. Herein, this work creatively proposes to prepare industrial-grade catalytic electrodes with high efficiency and stability at high current density through carbon quantum dots (CDs) modification nickel sulfide on hydrophilic flexible filter paper via one-step mild chemical plating (denoted as CDs-Ni 3 S 2 @HFP). The intrinsic activity and surface area, electron transfer ability, and corrosion resistance of Ni 3 S 2 material are increased due to the regulation, homogenous, and high concentration doping of CDs. The overpotential of the flexible catalytic electrode is only 30, 35, and 87 mV in 1 m KOH, simulated seawater (1 m KOH + 0.5 m NaCl), and neutral electrolyte (0.5 m PBS) at a current density of 10 mA cm −2 . More attractively, the CDs-Ni 3 S 2 @HFP electrode achieves over 500 h of efficient and stable catalysis at industrial high current density (500 mA cm −2 ). Due to the advantages of mild, universal, and large-area preparation of catalytic materials, this work provides technical support for flexible catalytic electrodes in efficient catalysis toward water splitting, energy storage, and device preparation.

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MICROPOROUS AND MESOPOROUS MATERIALS · 2023 · IF 5.2

Smart bifunctional covalent organic frameworks for water treatment: Reversible colorimetric pH detection and photocatalytic removal of pollutants

Zi-Wen Zhou,Zhe-Ning Wu,Chun-Xian Cai,Ru-De Lin,Xiao-Qi Yu,Kun Li,Na Wang

Covalent Organic Frameworks (COFs) with uniform aperture size, high surface area and tunable structure have been proposed as a potential material in water treatment. In this work, we utilized methoxy based covalent organic frameworks (COF–OMe) at room temperature as a dual-role smart material. For one thing, it can respond to the pH of solutions by visual, colorimetric change. Due to the protonation effect of methoxy groups in its pore skeleton, the fluorescent intensity of COF–OMe went down and the color changed from yellow to black as the pH decreased reversibly. For another, the abundant pores and ordered conjugated structure endowed it with a large surface area and light absorption ability. Therefore, the light-triggered oxidase-mimic porous COF–OMe can be applied in the synergistic removal of organic pollutants with synergistic physical absorption and light degradation. The outstanding and sensitive response to pH, great removal efficiency and dual function made it applied in water treatment with great potential, achieving killing two birds with one stone.

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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 44 ·21235-21244 · IF 3.925

Self-assembly of micelles with pH/ROS dual-responsiveness and mitochondrial targeting for potential anti-tumor applications

Huan Xu,Mingyue Yang,Yijing Du,Tian Gao,Yi Liu,Liwei Xiong,Na Peng

Nano-drug carriers have been widely used in chemotherapy to improve the efficacy of chemotherapeutic drugs. Polymer nano-carriers have greater potential for the enrichment of chemotherapeutic drugs at the target tumor site and controlled release. Herein, a series of amphiphilic copolymers (ITT) was synthesized via melt polymerization with a ROS-cleavable thioketal cross-linker, imidazole groups, and polyethylene glycol-conjugated triphenylphosphonium (PEG-TPP) segments; the actual proportions of the imidazole groups to the PEG-TPP segments were 5.2 : 1, 2.6 : 1, and 1.8 : 1, respectively. The amphiphilic copolymers could self-assemble into cationic micelles with hydrophobic imidazole groups as the core and hydrophilic PEG-TPP segments as the shell in deionized water. The cationic micelles with an average particle size of 124.6–187.3 nm showed a drug loading content (DLC) of 5.65–6.10%. In vitro release studies revealed the pH/ROS dual-responsiveness of the DOX-loaded ITT micelles, and the release behavior of DOX from the micelles strongly depended on the content of imidazole groups in the ITT micelles. Typically, the release of the encapsulated DOX was 27.2%, 30.0%, and 34.1% from DOX-loaded ITT-1 micelles in PBS (pH 6.5) containing 0, 100, and 500 μM H2O2, respectively. The release of the encapsulated DOX was 20.3%, 27.2%, and 42.5% from DOX-loaded ITT-1 micelles in PBS (pH 7.4), PBS (pH 6.5), and PBS (pH 5.0), respectively. The DOX-loaded micelles effectively inhibited the growth of 4T1 cells through being internalized into the 4T1 cells and releasing DOX into the mitochondria, with a cell viability of less than 65% when the DOX concentration was 2.5 μg mL−1. This work presents a novel mitochondria-targeting and pH/ROS-responsive polymer nanocarrier for potential chemotherapy applications.

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PEST MANAGEMENT SCIENCE · 2022 ·Vol. 79 ·期 3 ·969-979 · IF 4.462

Fabrication of a dual pH-responsive and photothermal microcapsule pesticide delivery system for controlled release of pesticides

Linhuai Li,Jun Cen,Lingling Huang,Ling Luo,Guangqi Jiang

BACKGROUND The development of stimulus-responsive and photothermally controlled-release microcapsule pesticide delivery systems is a promising solution to enhance the effective utilization and minimize the excessive use of pesticides in agriculture. RESULTS In this study, an AVM@CS@TA-Fe microcapsule pesticide delivery system was developed using avermectin as the model drug, chitosan and tannic acid as the wall materials, and tannic acid–Fe complex layer as the photothermal agent. The optical microscope, scanning electron microscope, transmission electron microscope, and Fourier-transform infrared spectroscope were used to characterize the prepared microcapsule. The slow-release, UV-shielding, photothermal performance, and nematicidal activity of the microcapsule were systematically investigated. The results showed that the system exhibited excellent pH-responsive and photothermal-sensitive performances. In addition, the UV-shielding performance of the delivery system was improved. The photothermal conversion efficiency ( η ) of the system under the irradiation of near-infrared (NIR) light was determined to be 14.18%. Moreover, the nematicidal activities of the system against pine wood nematode and Aphelenchoides besseyi were greatly increased under the irradiation of light-emitting diode (LED) simulated sunlight. CONCLUSION The release of the pesticide-active substances in such a pesticide delivery system could be effectively regulated with the irradiation of NIR light or LED-simulated sunlight. Thus, the developed pesticide delivery system may have broad application prospects in modern agriculture fields. © 2022 Society of Chemical Industry.

CAS / MDL: 10025-77-1 1401-55-4
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Quantification of adsorption mechanisms distribution of sulfamethoxazole onto biochar by competition relationship in a wide pH range

Yinxue Li,Hongru Shang,Yongna Cao,Chunhui Yang,Yujie Feng,Yanling Yu

This study aimed to investigate the degree of contribution of adsorption mechanisms of sulfamethoxazole (SMX) on corncob - derived biochar CC800 through competition experiments. The SMX adsorption was governed by diverse mechanisms under different pH, resulting in high pH dependent adsorption of SMX on biochar. The adsorption of SMX on CC800 in the presence of ions was evaluated, demonstrating that the ion exchange mechanism had a weak effect on the adsorption. The intense competitiveness of SMX structural analogs verified π + –π electron donor-acceptor (EDA) effect was the dominant adsorption mechanism of SMX on CC800 at low pH, and the negative charge-assisted hydrogen bond (CAHB) was critical to the adsorption at high pH. The adsorption mechanisms contribution of SMX on CC800 were further quantified. The SMX adsorption on CC800 was mainly controlled by 51% pore filling and 43% π + –π EDA effect in the acid region, 62% pore filling mechanism and 25% (−)CAHB mechanism in the alkalic region, and less than 5% of hydrophobic interaction and ion exchange. Consequently, the above mechanisms provided a theoretical basis for biochar application to remove sulfonamide antibiotics and other similar organic contaminants and targeted design of biochar products. Also, this quantification method can be extended to quantify the adsorption mechanisms between other antibiotics or organics and biochar adsorbent materials by selecting suitable adsorption competitors.

CAS / MDL: 92-70-6 723-46-6
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ChemNanoMat · 2022 ·Vol. 8 ·期 12 ·e202200424 · IF 3.82

FeOCl Nanodots and Doxorubicin Co-loaded Polymer Nanoparticles for Glutathione/pH-responsive Chemodynamic Therapy/Chemotherapy of Tumors

Lihui Yuwen,Yue Zhang,Huayu Xiao,Hang Xiao,Xiao Li,Wenjing Yang,Zhaoxia Yang,Heng Dong,Lianhui Wang

Graphical FeOCl nanodots were prepared by a ball-milling method and used as novel Fenton agents. Glutathione/pH dual-responsive polymer nanoparticles were synthesized by co-polymerization of acrylic acid and 3-methacrylamido dopamine with a cross-linker containing disulfide bonds, which can load FeOCl nanodots and doxorubicin to form a multifunctional nanoplatform for efficient chemodynamic therapy/chemotherapy. Chemodynamic therapy (CDT) based on the Fenton reaction has been considered as a promising solution for the treatment of tumors. However, the limited therapeutic efficacy and lack of responsive release of Fenton agents still hinder the further application of CDT. To this end, we designed a disulfide bond (−S−S−) cross-linked polymer nanoparticles (poly(AA-co-DMA), PAD) to load FeOCl nanodots (FeOCl NDs) and doxorubicin (DOX) with the surface coating of bovine serum albumin (BSA) to prepare glutathione (GSH)/pH-responsive PAD-FeOCl/DOX@BSA nanoparticles (PFDB). In the tumor microenvironment (TME) with abundant GSH and acidic pH, the −S−S− bond in PFDB can be reduced and the linkage between the polymer chains is broken down, which facilitates the controlled release of FeOCl NDs and DOX. Both in vitro and in vivo experimental results showed that PFDB can serve as a GSH/pH-responsive nanoagent for the effective killing of 4T1 tumor cells by combined CDT/chemotherapy. This study provides a promising TME-responsive nanoagent with dual therapeutic modes for the effective treatment of tumors.

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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY · 2022 · IF 5.062

pH/NIR-responsive nanocarriers based on mesoporous polydopamine encapsulated gold nanorods for drug delivery and thermo-chemotherapy

Zehua Han,Minjie Gao,Zhihua Wang,Lichao Peng,Yanbao Zhao,Lei Sun

Gold nanorods (AuNRs) have potential application value in the field of cancer therapy. However, the poor stability, high dark toxicity, insufficient drug-carrying capacity and photothermal conversion efficiency have limited its practical applications. In this study, we encapsulated AuNRs in mesoporous polydopamine (mPDA) shells. The mPDA has exceptional adhesion, excellent biocompatibility , large specific surface area and favorable photothermal properties, making [email protected] an ideal photothermal composite and drug delivery carrier. [email protected] can generate heat under near-infrared (NIR) laser irradiation, which disrupts the intermolecular forces and hydrogen bonds between PDA shell and drug, showing a photothermal enhanced drug release. Furthermore, by using polyethyleneimine (PEI) to seal the pore channels of mPDA, the pH-/NIR-responsive nanocarrier of [email protected] @PEI was fabricated, which shows a high drug loading capacities for DOX to 121.7 mg/g. What's more, by combination of chemotherapy and photothermal therapy , the [email protected] @PEI nanocarrier exhibits significant anticancer effect in vitro . In a word, this carrier demonstrated high drug capacity, excellent photothermal conversion efficiency (55.7%) and pH/NIR stimulation-responsive delivery performance, and promising to become a nanoplatform for multifunctional cancer therapy in the future.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Luminescent composite organohydrogels with Fe3+, pH, and glucose-dependent shape memory behavior accompanied with diverse fluorescence variation

Yanqin Wang,Yu Zhu,Xuehui Zhang,Fengbo Zhu,Yi-Xian Qin,Weiyi Chen,Qiang Zheng

It is quite urgent to develop a smart and high through-put confidential information storage, protection, and display platform based on the fluorescent hydrogels that could exhibit diverse fluorescent variation behavior during each stimulus-based shape memory and recovery process. Herein, it proposed an effective approach to develop a novel fluorescent composite gel with Fe 3+ , pH, and glucose-dependent diversity fluorescence variation and shape memory behavior. For this composite gel system, based on the reversible coordination interactions between Fe 3+ and carboxylic acid groups of carboxymethyl cellulose (CMC), boric acid groups of carbon dots (CDs), and hydroxyl groups of PVA , it can stabilize and memorize the temporary shapes under the stimulus of Fe 3+ and pH, respectively. Meanwhile, the fluorescence of the CDs within the gels can also exhibit diversity variation behaviors during each shape recovery process. Furthermore, the compositions of the composite gel were optimized to realize relatively high efficiency of shape recovery and fluorescence variation under each type of stimulus. In summary, this study presented a universal strategy for multi-shape memory hydrogels with diverse fluorescence variation properties which exhibited prominent prospective in the field of information encryption with high-level security.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Development of pH-responsive konjac glucomannan/pullulan films incorporated with acai berry extract to monitor fish freshness

Guoyu Cao,Nitong Bu,Taotao Zeng,Runzhi Sun,Ruojun Mu,Jie Pang,Lin Wang

In this work, konjac glucomannan (KGM)-based film reinforced with pullulan (PL) and acai berry extract (ABE) was developed by solvent casting method. The as-prepared films performed pH-sensitive properties, which can be potentially applied for fish freshness detection. Rheology , Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), scanning electron microscopy (SEM) were used to characterize chemical structure and morphology of ABE-loaded KGM/PL (KP) films (KP-ABE). FT-IR spectrum indicated that hydrogen bond dominated the formation of KP-ABE films. Adding PL contributed to enhanced mechanical properties of KGM film with increased tensile strength (TS) from 21.25 to 50.27 MPa and elongation at break (EAB) from 10.64 to 19.19 %. Incorporating ABE upgraded flexibility, UV-shielding, thermostability , water barrier (decreased Water vapor permeability (WVP) from 2.07 to 1.67 g·mm/m 2 ·day kPa), antioxidant, and antibacterial ability of KP films, but weakened TS. In addition, KP-ABE films can reflect fish freshness in real time through color variability. Therefore, KP-ABE films exhibited potential applications in intelligent food packaging materials.

CAS / MDL: 1898-66-4 9057-02-7
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

One-pot self-assembly fabrication of chitosan coated hollow sphere for pH/ glutathione dual responsive drug delivery

Jiagen Li,Yaqi Li,Zhanqiong Zhong,Xiaohong Fu,Zhonghui Li

Chitosan-coated poly (methacrylic acid) (PMAA) hollow spheres with 64 ± 3% drug loading capacity and low drug leakage (7 ± 2%, 54 h) were prepared through a novel one-pot two-step self-assembly process. Site-specific doxorubicin (DOX) loading and chitosan coating were achieved by electrostatic interaction to fulfill efficient drug loading and well-controlled drug release behavior. In vitro drug release profile revealed the pH and glutathione (GSH) dual responsive fast triggered drug release behavior, reaching 62 ± 3% during the first 10 h. And completely drug release could be achieved in 54 h. The high drug content and sensitive tumor microenvironment responsibility lead to similar anti-cancer efficiency with free doxorubicin in in vitro MTT assay . This self-assembly guided one-pot two-step fabrication process was proved to be an effective and convenient way to prepare the well-defined multi-layer structure and might be further employed in fabricating high-performance drug delivery systems.

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