CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yuan-Ju Tang,Kai Cheng,Lin-Fang Tan,Xiao-Ting Xie,Bin Zhang,Wen-Ming Su,Yuan-Di Zhao,Qiu-Ran Xu
The construction of solid nanochannel-based biosensor with submicron pore size has great significance to the analysis of biomolecule with high sensitivity and low detection limit. In this paper, a submicrochannel heterogeneous membrane with asymmetric geometry is prepared as the base by combining thermo-crosslinked hydrophobic conducting polymer and porous anodic aluminium oxide channel (AAO) with submicron pore size (269 nm). After the polydopamine-Au multilayer assembly, a large number of Au nanoparticles with adjustable size (∼10 and 89 nm) and density are in situ generated and fixed on the inner wall of AAO. Then 4-mercapto phenylboric acid with high density is grafted through Au-S bond to construct the submicrochannel heterogeneous membrane with the characteristic of ion current rectification in response to pH and saccharide. Benefit from the blocking effect of hydrophobic conducting polymer and the multilayer assembly of polydopamine-Au, the current of background response by the membrane device is effectively reduced, the ion current rectification strength can be effectively regulated in the range of pH 3–9, and the response to ultra-low glucose concentration without enzyme is achieved in the linear range of 1 pM-0.1 μM. A universal substrate platform is provided for the construction of solid nanochannel-based biosensor with submicron pore size.
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POLYMER
·
2023
·
IF 4.6
Ke Wang,Liru An,Ganghui Lu,Jialu Zhang,Zilong Wang,Meiyu Si,Guiyan Liu,Yongfei Zeng
A series of novel thermo/pH/CO 2 -triple responsive homopolymers were synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. These homopolymers contain ethoxy groups , and the end substituents are pyrrolidine , piperidine , N -methylpiperazine, morpholine and thiomorpholine , respectively. The effects of different heterocyclic substituents on the responsiveness of temperature, pH and CO 2 were studied. For temperature-response, it was found that the lower critical solution temperature (LCST)-type cloud point (CP) temperature decreased as the number of carbon atoms increases, while the solubility of the polymers changed greatly with the introduction of oxygen, nitrogen and sulfur atoms. And the CP of the polymers can be adjusted by molecular weight , concentration and salt. Furthermore, some of these polymers present upper critical solution temperature (UCST) behavior in alcohols. For pH-response, the initial pH of the polymer solution is different, their critical pH changed accordingly, and is affected by temperature; in addition, changing the pH of solution can also affect the CP. For CO 2 -response, all of the polymers were completely soluble after pumping with CO 2 , and their LCST behavior recovered after N 2 was pumped in, but there was a gap with the initial CP. The study of these properties reveals the influence of different heterocyclic substituents on the responsiveness of polymers, which is of great significance for understanding the stimulation response properties of polymers and provides ideas for the design of new stimuli-responsive polymers.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Yafang Liu,Ming Yi,Yan Wang
Membrane fabricated with a method of ingenious simplicity to be equipped with antibacterial function is the key to address the biofouling issue in separation applications. Herein, we proposed an innovative approach to armor abundant antibiotics on the membrane with minimal loss of the active functional groups of the antibiotics. Boronate ester-based membrane was first fabricated with non-solvent induced phase separation (NIPS) method. A loose nanofiltration (LNF) membrane with unique trinity structure was then constructed through the cross-linking between boronate ester complexes and trimesoyl chloride (TMC) on the top layer. Due to the pH responsive and dynamic nature of boronate ester complexes, boronic acid groups can be released under acidic conditions, acting as binding sites for diol-bearing antibiotics. This not only allows the sufficient anchoring of antibiotics (here kanamycin (KM) was chosen as model antibiotics), but also minimizes the consumption of active groups of KM molecules. The resultant membrane delivers excellent biocidal effect against both Gram-negative and positive bacteria, while also exhibiting superior water permeance of 134.86 ± 5.62 L m −2 h −1 bar −1 . This work reveals the great potential of boronate esters complexes for the development of high-flux antibacterial membranes.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Qianjin Li,Meng Wang,Yu Jin,Yongling Lu,Shuqing Xiong,Mengdi Wang,Jianhong Xu,Chenhong Wei,Jianlin Li
Here, fluorescent artificial antibodies for sensing ovalbumin in food were synthesized by molecular imprinting technique in a microfluidic reactor. A phenylboronic acid-functionalized silane was employed as the functional monomer to enable the polymer has pH-responsive property. Fluorescent molecularly imprinted polymers (FMIPs) could be produced continuously in a short time. Both fluorescein isothiocyanate (FITC) and rhodamine B isothiocyanate (RB)-based FMIPs can specifically recognize the target ovalbumin, particularly FITC-based FMIP, giving an imprinting factor of 2.5 and cross-reactivity factors of 2.7 (ovotransferrin), 2.8 (β-lactoglobulin) and 3.4 (bovine serum albumin), and was applied for the detection of ovalbumin in milk powder with recovery rates of 93–110%; moreover, the FMIP can be reused at least four times. Such FMIPs have promising future in replacing the fluorophore-labelled antibodies to fabricate fluorescent sensing devices or establish immunoassay methods, which have extra merits of low-cost, high stability and recyclability, easy to carry and store at ambient environments.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jieming Huang,Yuanwu Liu,Lirong Wang,Zhipeng Hou,Zhang Zhang,Xiaoming Zhang,Junming Liu
Hydrogen energy can be a promising alternative to fossil energy and can be applied to address the global energy challenge. However, the large overpotential and limited operation in the single electrolyte for hydrogen evolution reaction (HER) greatly hinder its practical applications. Herein, an efficient HER electrocatalyst demonstrated as MoO 2 -Mo 2 C-NC (NC is nitrogen-doped carbon) heterostructure applied in a wide pH, was in-situ constructed on carbon cloth (CC) by controlling coupling interactions of multicomponents. The strong coupling interactions in the heterostructure triggered the strain effect to induce C atoms to absorb H and promoted the establishment of a distinct synergy effect between Mo and C atoms, resulting in further electron configuration regulation. Besides, C defects and O vacancies of catalyst developed a rich H 3 O + environment in alkaline media, improving H-seizure of active sites. As expected, MoO 2 -Mo 2 C-NC@CC-950 °C achieved 10 mA·cm −2 only with 72 mV in 0.5 M H 2 SO 4 , 206 mV in 1 M phosphate buffer solution (PBS) and 79 mV in 1 M KOH, respectively, corresponding to the Tafel slopes of 56.42, 133.42 and 59.7 mV∙dec -1 . In addition, stability test in 1 M KOH performed at 100 mA∙cm −2 for 120 h exhibited ultrahigh durability in HER. The high-performance was attributed to the synergy of Mo and C atoms and the key roles of C defects and O vacancies, which were verified by the density functional theory (DFT) calculations. This work presents fresh possibilities for multicomponent modification and mechanism exploration in HER electrocatalysts.
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PROGRESS IN ORGANIC COATINGS
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2022
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IF 6.206
Guangyi Cai,Pengfei Hu,Xiangkang Cao,Junquan Chen,Xinxin Zhang,Zehua Dong
Self-inhibition ability is crucial to realize long-term anticorrosion performance of coatings. Here, we synthesized a kind of nanofiller made of Ce III -tannic metal-phenolic network wrapped carbon nanotubes (Ce III -TA-CNTs). Through incorporation of the nanofiller, the intelligent epoxy coating possessing excellent anti-permeability and pH-responsive self-inhibition performance was investigated in detail. The pH-responsive release activity of Ce 3+ ions from Ce III -TA-CNTs nanoparticles showed an increase trend in the acidic solution of pH = 7 down to 3, and increased first and then decreased in the alkaline solution of pH = 7 up to 11 by UV–vis spectroscopy. The cumulative release amount was above 90 % both at pH = 3 and pH = 9. In addition, the Ce III -TA-CNTs/EP composite coating system on aluminum alloy showed long-term excellent corrosion resistance proved by accelerated cyclic ageing tests. The coating resistance of EP composite coatings with 1.0 and 2.0 % Ce III -TA-CNTs loading could maintain above 10 7 Ω·cm 2 after 8 ageing cycles, which was higher than 1.0%CNTs/EP and pure EP coatings. Adhesion investigation indicated that the higher adhesion strengthen (6.7 MPa) and remarkable anti-peeling property were recorded for 1.0%Ce III -TA-CNTs/EP. Moreover, the scratched coating system loaded with Ce III -TA-CNTs researched by local electrochemical showed long-lasting self-inhibition and anti-diffusion properties with |Z| 10Hz value above 2 × 10 5 Ω·cm 2 , potential and current about −0.82 V and 10 −8 A·cm −2 respectively surrounding the scratched area after 28 days immersion. The results indicated that the synergistic corrosion resistance effect of Ce III -TA-CNTs came from the cross-linking barrier of CNTs, the active release of Ce 3+ inhibitor via pH variation and the rust conversion of tannic acid.
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CHINESE JOURNAL OF CATALYSIS
·
2022
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IF 12.92
Qixian Xie,Dan Ren,Lichen Bai,Rile Ge,Wenhui Zhou,Lu Bai,Wei Xie,Junhu Wang,Michael Grätzel,Jingshan Luo
Nickel iron layered double hydroxide (NiFe LDH) is one of the best oxygen evolution reaction (OER) catalysts in alkaline electrolytes. However, it performs poorly in neutral electrolytes, and the detailed mechanism is still unclear. Herein, we introduce electrochemical measurements, operando surface enhanced Raman spectroscopy and operando 57 Fe Mössbauer spectroscopy to elucidate the mechanism of NiFe LDH for OER process in different pH electrolytes. Our results show that even though there exist Ni 3+ and Fe 4+ species, the NiFe LDH based electrocatalysts still show worse OER performance in neutral electrolytes than in alkaline conditions. Combining the electrochemical measurements with spectroscopic investigations, we demonstrated that the rate-determining step (RDS) of OER on NiFe LDH based electrocatalysts is from *O to *OOH in alkaline medium while *OH formation is the RDS in neutral conditions. Our work provides new insights into elucidating the OER mechanism in different pH electrolytes.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 3
·1214-1228
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IF 4.5
Qian Guowen,Wang Junzhe,Yang Liuyimei,Zeng Zhikui,Zhao Zhenyu,Peng Shuping,Shuai Cijun
The insufficient of H 2 O 2 restricts the efficacy of chemodynamic therapy in tumor microenvironment. Calcium peroxide (CaO 2 ) is expected to solve this problem due to its H 2 O 2 -evolving ability. However, it prematurely decomposes in the moist air or water before reaching tumor site. In this study, zeolitic imidazolate framework-67 (ZIF-67) was in-situ grown on the surface of CaO 2 to construct a pH-responsive CaO 2 @ZIF-67 system and then incorporated into poly-L-lactic acid (PLLA) to prepare PLLA/CaO 2 @ZIF-67 scaffold by selective laser sintering technology. On the one hand, ZIF-67 is used as a chemodynamic therapy agent due to the release of cobalt ions after degradation. On the other hand, ZIF-67 can serve as protective layers to prevent premature decomposition of CaO 2 due to its hydrophobic properties, and then CaO 2 is exposed and reacts with water to form H 2 O 2 after the pH-responsive degradation of ZIF-67 under tumor acidic microenvironment. Results showed that the PLLA/CaO 2 @ZIF-67 scaffold could sustainedly produce H 2 O 2 under acidic pH and achieve 84.64% antitumor ratio against MG-63 cells. In addition, the scaffold also promoted proliferation and osteogenic differentiation of mouse bone marrow mesenchymal stem cells due to the release of calcium ions. The prepared PLLA/CaO 2 @ZIF-67 scaffold with chemodynamic antitumor and osteogenic effects has great potential to treat tumorous bone defect.
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Polymers
·
2023
·Vol. 15
·期 3
·638
·
IF 5
Jia Tan,Jiaming Sun,Chunhui Ma,Sha Luo,Wei Li,Shouxin Liu
The global challenge of oil pollution calls for the efficient selective recovery of oil or organics from oil–water mixtures. A pH-responsive carbon foam (CF) made from liquefied larch sawdust (LLS) with switchable wettability was fabricated in this work. After grafted with poly 4-vinyl pyridine (P4vp), the CF obtained a switchable wettability surface, which allowed the CF to exhibit superhydrophilicity and superhydrophobicity at different pH levels, respectively. The results revealed that the pH-responsive CF possessed a three-dimensional (3D) spongy-like skeleton and porous structure with a diameter between 50 and 200 µm. Thus, the pH-responsive CF could absorb 15–35 g/g of oil/organics in a neutral aqueous solution at pH = 7 and desorb all the absorbate within 40 s after immersion in an aqueous solution at pH = 1. Moreover, only about 2.8% loss was observed for organic (chloroform) absorption and recovery after reusing up to 15 cycles, which indicated promising prospects in oil and organic recovery.Keywords:switchable wettability;wood materials;carbon foams;oil recovery;oil cleanup
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Materials Today Bio
·
2023
·
IF 8.2
Yifei Jiang,Qinghe Wu,Mengfei Hou,Wangxi Hai,Min Zhang,Biao Li,Chunfu Zhang
The acidic microenvironment is one of the remarkable features of tumor and is also a reliable target for tumor theranostics. Ultrasmall gold nanoclusters (AuNCs) have good in vivo behaviors, such as non-retention in liver and spleen, renal clearance, and high tumor permeability, and held great potential for developing novel radiopharmaceuticals. Herein, we developed pH-sensitive ultrasmall gold nanoclusters by introducing quaternary ammonium group (TMA) or tertiary amine motifs (C6A) onto glutathione-coated AuNCs (TMA/GSH@AuNCs, C6A-GSH@AuNCs). Density functional theory simulation revealed that radiometal 89 Sr, 223 Ra, 44 Sc, 90 Y, 177 Lu, 89 Zr, 99m Tc, 188 Re, 106 Rh, 64 Cu, 68 Ga, and 113 Sn could stably dope into AuNCs. Both TMA/GSH@AuNCs and C6A-GSH@AuNCs could assemble into large clusters responding to mild acid condition, with C6A-GSH@AuNCs being more effective. To assess their performance for tumor detection and therapy, TMA/GSH@AuNCs and C6A-GSH@AuNCs were labeled with 68 Ga, 64 Cu, 89 Zr and 89 Sr, respectively. PET imaging of 4T1 tumor-bearing mice revealed TMA/GSH@AuNCs and C6A-GSH@AuNCs were mainly cleared through kidney, and C6A-GSH@AuNCs accumulated in tumors more efficiently. As a result, 89 Sr-labeled C6A-GSH@AuNCs eradicated both the primary tumors and their lung metastases. Therefore, our study suggested that GSH-coated AuNCs held great promise for developing novel radiopharmaceuticals that specifically target the tumor acidic microenvironment for tumor diagnosis and treatments.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2022
·
IF 5.999
Min Du,Jing Jin,Feng Zhou,Jiayue Chen,Wei Jiang
Antibacterial and hemostatic properties are essential for wound healing dressing. In this study, a new type of hydrogel composed of gelatin methacryloyl (GelMA) and hyaluronic acid-aldehyde (HA-CHO) is fabricated by photo-crosslinking and respectively loaded with a single drug gentamicin sulfate (GS), and two drugs of GS and lysozyme (LZM). The composite hydrogel of GelMA and HA-CHO is successfully synthesized by the aldehyde and Schiff base reactions. The structures and compositions of the hydrogels with and without drug loaded are characterized by FT-IR, 1 H NMR, and XPS. Furthermore, the microstructure and swelling behaviour of hydrogels prove that the content of HA-CHO has a significant role in the formation of hydrogels with dense porous structures and super absorbent. pH 7.4 and pH 5.0 conditions are used to evaluate the drug release behaviour of the obtained hydrogels. The released amount of GS of the drug-loaded hydrogels in the acidic buffer is more than that of the physiological environment because of the cleaved Schiff base bonds and the electrostatic interaction. Especially for the dual drug-loaded hydrogel GelMA/HA-CHO/GS/LZM, the released ratio of GS is elevated from 59 % in pH 7.4 buffer to about 78 % in pH 5.0 buffer within the first 6 h, which verifies the excellent pH-stimulus responsiveness. These endow the GS-LZM dual drug-loaded hydrogels with superior antibacterial efficiencies to that of the single GS drug-loaded hydrogels, no drug-loaded hydrogels, and SEBS control, especially in inhibiting S. aureus in a lower concentration of 10 6 CFU mL −1 , which can be attributed to the synergistic effect of LZM and GS. For S. aureus at 10 6 CFU mL −1 , the bacterial survival of GelMA/HA-CHO/GS/LZM is 1.1 %, which shows outstanding antibacterial effect . Hence, the drug-loaded hydrogels, especially the dual drug-loaded hydrogels with pH-responsive, antibacterial, and hemostatic properties have great potential as wound healing materials.
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MACROMOLECULAR RAPID COMMUNICATIONS
·
2023
·Vol. 44
·期 8
·2200928
·
IF 4.6
Xiaotong Wei,Jie Li,Zhirui Hu,Chen Wang,Zhiqiang Gao,Yang Cao,Jing Han,Yingchun Li
In recent years, hydrogels have attracted extensive attention in smart sensing owing to their biocompatibility and high elasticity. However, it is still a challenge to develop hydrogels with excellent multiple responsiveness for smart wearable sensors. In this paper, a facile synthesis of carbon quantum dots (CQDs)-doped cross-linked chitosan quaternary/carboxymethylcellulose hydrogels (CCCDs) is presented. Designing of dual network hydrogels decorated with CQDs provides abundant crosslinking and improves the mechanical properties of the hydrogels. The hydrogel-based strain sensor exhibits excellent sensitivity (gauge factor: 9.88), linearity ( R 2 : 0.97), stretchable ability (stress: 0.67 MPa; strain: 404%), good cyclicity, and durability. The luminescent properties are endowed by the CQDs further broaden the application of hydrogels for realizing flexible electronics. More interestingly, the strain sensor based on CCCDs hydrogel demonstrates photo responsiveness (Δ R / R 0 ≈20%) and pH responsiveness (pH range ≈4–7) performance. CCCDs hydrogels can be used for gesture recognition and light sensing switch. As a proof-of-concept, a smart wearable sensor is designed for monitoring human activities and detecting pH variation in human sweat during exercise. This study reveals new possibilities for further applications in wearable health monitoring.
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