Nature Communications
·
2021
·Vol. 12
·期 1
·1-10
·
IF 14.919
Wei Hongqiu,Lei Ming,Zhang Ping,Leng Jinsong,Zheng Zijian,Yu You
3D-printing tough conductive hydrogels (TCHs) with complex structures is still a challenging task in related fields due to their inherent contrasting multinetworks, uncontrollable and slow polymerization of conductive components. Here we report an orthogonal photochemistry-assisted printing (OPAP) strategy to make 3D TCHs in one-pot via the combination of rational visible-light-chemistry design and reliable extrusion printing technique. This orthogonal chemistry is rapid, controllable, and simultaneously achieve the photopolymerization of EDOT and phenol-coupling reaction, leading to the construction of tough hydrogels in a short time ( t gel ~30 s). As-prepared TCHs are tough, conductive, stretchable, and anti-freezing. This template-free 3D printing can process TCHs to arbitrary structures during the fabrication process. To further demonstrate the merits of this simple OPAP strategy and TCHs, 3D-printed TCHs hydrogel arrays and helical lines, as proofs-of-concept, are made to assemble high-performance pressure sensors and a temperature-responsive actuator. It is anticipated that this one-pot rapid, controllable OPAP strategy opens new horizons to tough hydrogels.
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Journal of Coatings Technology and Research
·
2021
·Vol. 18
·期 4
·989-998
·
IF 2.382
Xu Liangfeng,Wang Zhaofei,Yang Gongwen,Zhang Guobing,Wei Haibing,Fang Huagao,Ding Yunsheng
Traditional waterborne polyurethane (WPU) has poor water resistance because of the incorporation of permanent hydrophilic groups, such as carboxyl group or ammonium salt, into polymer chains. Therefore, developing WPU with excellent water resistance and mechanical properties is highly desirable for industrial applications. In this study, CO 2 -triggered hydrophobic/hydrophilic switchable waterborne polyurethane–acrylate (WPUA) containing methyl methacrylate (MMA) units were designed and synthesized. The molecular structure, hydrophobic/hydrophilic switchable behavior, water resistance, and mechanical properties were systematically investigated and characterized. The WPUA with 10 wt% MMA exhibited a low water uptake (2.15 wt%) and linear swelling ratio (0.17 L%), as well as a high tensile strength (16.7 MPa) and modulus (85.9 MPa), which were much higher than those of the pristine WPU. This study indicated that the CO 2 -triggered WPUA dispersed stably as latex particles in water and possessed excellent water resistance and mechanical properties after the film formation.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 5
·1-8
·
IF 5.833
Sun Ying,Lin Tianran,Zeng Cuihong,Jiang Gaoyan,Zhang Xuanhan,Ye Fanggui,Zhao Shulin
A self-correcting fluorescent assay of tyrosinase (TYR) was developed by utilization of Fe-MIL-88B-NH 2 as a peroxidase-like nanozyme and a capture probe. Fe-MIL-88B-NH 2 nanozyme was selected as an electron donor, and the oxidization product (dopamine- o -quinone) acts as an energy acceptor. First, TYR catalyzes the oxidation of tyramine hydrochloride to dopamine and then to dopamine- o -quinone. Second, Fe-MIL-88B-NH 2 with intrinsic peroxidase-like activity decomposes H 2 O 2 to produce ·OH radicals, which further accelerate the oxidation of dopamine to dopamine- o -quinone. Excessive H 2 O 2 and ·OH radicals reduce the interferences from ascorbic acid at the same time providing a self-correcting ability. Dopamine- o -quinone reacts with -NH 2 groups on the ligand of Fe-MIL-88B-NH 2 through Michael reaction which results in fluorescence quenching. Under 365-nm excitation, the fluorescence emission intensity at 452 nm gradually decreased with increasing TYR concentration varying from 0 to 10 U mL −1 . The linear range is from 1 to 5 U mL −1 and the detection limit is 0.05679 U mL −1 . This self-correcting fluorescent assay of tyrosinase exhibits good sensitivity and selectivity which is also successfully applied for tyrosinase inhibitor detection. Graphical abstract
Schematic representation of fluorescent assay for tyrosinase determination based on Fe-MIL-88B-NH 2 nanozyme. A self-correcting fluorescent assay for tyrosinase was developed based on the Fe-MIL-88B-NH 2 nanozyme.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 5
·1-10
·
IF 5.833
Gu Ying,Hu Yuanling,Zhang Fuyuan,Yi Lunzhao,Shang Ying,Ren Dabing,Ge Zhenhua
A glucose (Glu) sensor was designed by introducing synthetic cyclic peptides (CPs) as recognition receptors and Au nanoparticles assisted graphitic carbon nitride (AuNPs/g-C 3 N 4 ) for electrochemiluminescence (ECL) enhancement. The synthetic CP receptor (cyclo-[−CNDNHCRDNDC−]) with natural active center of Glu binding protein can mimic the interactions between Glu and Glu binding protein to specifically capture Glu. The AuNPs were reduced on g-C 3 N 4 and formed a new nanohybrid that can be applied as an ECL emitter. The AuNPs/g-C 3 N 4 effectively ameliorated the ECL response of bare g-C 3 N 4 . The ECL enhancement mechanism was theoretically speculated through computer simulation. Glu quantification was conducted by recording ECL shifts induced by the binding of Glu to CPs. The linear detection range of the fabricated CPs-based ECL sensor was 1 to 100 mmol L −1 , and the detection limit (LOD) was 0.57 nmol L −1 (S / N = 3). The CP-based ECL sensor also showed good specificity, repeatability, stability, and favorable recoveries in sample analysis. This work offer a promising analytical method for Glu assay in clinical diagnostics and bioprocess monitoring. Graphical abstract
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 15
·3847-3859
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IF 4.157
Xiao Jing,Liu Zhang,Li Chunxiang,Wang Jinglun,Huang Haowen,Yi Qingfeng,Deng Keqin,Li Xiaofang
Graphdiyne (GDY) adsorbed DNA probes have been used as a fluorescent sensing platform, but topics including DNA adsorption affinities, DNA probe displacement, and fluorescence quenching ability were rarely researched. Herein, the adsorption affinity of single-stranded DNA (ssDNA) and double-stranded DNA (dsDNA) on a tremella-like GDY was tuned by modulating the surface chemistry of GDY. The fluorescence quenching ability of GDY with different oxidation degrees was compared. The nonspecific displacement of DNA probes on GDY was studied. Under the same concentrations, GDY with low oxidation degree exhibited stronger adsorption affinity and higher adsorption capacity to both ssDNA and dsDNA than highly oxidized GDY. DNA adsorbed on low-oxidized GDY was more resistant to displacement by other DNAs. Protein showed strong interaction with different GDY and could displace DNA probes on GDY. Based on these findings, an ideal GDY with proper oxidation degree, exhibiting high surface affinity for ssDNA and low affinity for dsDNA, was used as scavenger of redundant ssDNA fluorescent probe in an enzyme-assisted amplification system for sensitive ochratoxin (OTA) detection. This study has enhanced our fundamental understanding of DNA adsorption by GDY. It also provided a rational way to apply GDY for fluorescence sensing in a complicated system. Graphical abstract
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Nanoscale Research Letters
·
2021
·Vol. 16
·期 1
·1-12
·
IF 4.703
Shu Mengjun,Gao Feng,Zeng Min,Yu Chulang,Wang Xue,Huang Renhua,Yang Jianhua,Su Yanjie,Hu Nantao,Zhou Zhihua,Liu Ke,Yang Zhi,Tan Hongtao,Xu Lin
To achieve better antitumour efficacy, it is urgent to improve anticancer drug delivery efficiency in targeting cancer cells. In this work, chitosan-functionalized graphene oxide (ChrGO) nanosheets were fabricated via microwave-assisted reduction, which were employed to the intracellular delivery nanosystem for anticancer drug agent in breast cancer cells. Drug loading and release research indicated that adriamycin can be efficiently loaded on and released from the ChrGO nanosheets. Less drug release during delivery and better biocompatibility of ChrGO/adriamycin significantly improve its safety and therapeutic efficacy in HER2-overexpressing BT-474 cells. Furthermore, ChrGO/adriamycin in combination with trastuzumab exhibited synergistic antitumour activity in BT-474 cells, which demonstrated superior therapeutic efficacy compared with each drug alone. Cells treated with trastuzumab (5 μg/mL) or equivalent ChrGO/adriamycin (5 μg/mL) each elicited 54.5% and 59.5% cell death, respectively, while the combination treatment with trastuzumab and ChrGO/adriamycin resulted in a dramatic 88.5% cell death. The dual-targeted therapy displayed higher apoptosis, indicating superior therapeutic efficacy due to the presence of different mechanisms of action. The combined treatment of ChrGO/adriamycin and trastuzumab in BT-474 cells induced cell cycle arrest and apoptosis, which ultimately led to the death of augmented cancer cells. This work has provided a facile microwave-assisted fabrication of ChrGO as a controlled and targeted intracellular drug delivery nanosystem, which is expected to be a novel promising therapy for treating HER2-overexpressing breast cancer cells.
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CELLULOSE
·
2021
·Vol. 28
·期 6
·3409-3421
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IF 5.044
Chen Weixiang,Chen Bo,Lv Rixin,Wu Milian,Zhou Jie,Lu Beili,Huang Biao,Lu Qilin,Tang Lirong
Natural cellulose nanocrystals (CNCs) possess outstanding properties, such as biodegradability, hydrophilicity, large specific surface areas, and are low in cost. A highly stable and sensitive humidity sensor based on a quartz crystal microbalance (QCM) was prepared using CNCs as the sensing film. To investigate the impact of CNCs loading on the sensor performance, a series of humidity-sensitive performance tests, including linearity, response and recovery times, repeatability, hysteresis characteristics, selectivity, and long-term stability tests, was conducted. The experimental results indicated that the humidity sensor with CNCs loading of 2 μg (QCM-2) exhibited excellent logarithmic linearity, high sensitivity (32.35 Hz/% relative humidity (RH)), excellent reversible behavior, and long-term stability at a RH of 11–84%. The contact angle of QCM-2 was 12.5°, revealing its suitable hydrophilicity. Thus, we demonstrate that CNCs are great prospects for potential application in humidity sensors with high performance and low cost. Graphic abstract
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CELLULOSE
·
2021
·Vol. 28
·期 18
·11429-11450
·
IF 5.044
Zhao Yali,Lu Wenxi,Shen Shangzhu,Wei Li
The hydrogel wound dressings are mostly sheet-like and do not possess adhesive properties, so it is often difficult for them to adhere well to the skin tissues and fit completely with the irregularly shaped wounds or deep wounds, thereby affecting their therapeutic effects. Herein, the chitosan derivative-based mussel-inspired hydrogels have been developed to overcome these obstacles. Specifically, the principle of adhesion of marine mussel was imitated to synthesize catechol-modified chitosan (CMC), which was potentially used as the raw material to prepare the mussel-inspired hydrogels, that can contribute to the excellent adhesive property and make the hydrogels adhere well to the wound sites. The o-diphenyl groups in CMC could be easily oxidized to form o-diquinone to further form a covalent binding with amino groups (–NH2), or can directly form coordination binding with Fe 3+ .This strong covalent and coordination binding causes the hydrogels to possess a complex spatial structure, which facilitates the hydrogels to display good swelling properties, drug loading and release properties. Furthermore, the total saponins of Panax notoginseng were loaded in the hydrogels and the therapeutic effects of drug-loaded hydrogel were investigated in the model of full-thickness skin injury in mice. The wound healing rate was observed to be as high as 92.5% without exhibiting any scarring. Overall, our findings provided a novel strategy for the preparation of hydrogels for therapeutic applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2021
·Vol. 29
·期 12
·17866-17877
·
IF 4.223
Gao Yu-Qiong,Zhou Jin-Qiang,Ning Han,Rao Yan-Yan,Gao Nai-Yun
In this study, electrochemically activated peroxymonosulfate (EC/PMS) with a sacrificial iron electrode was used for the removal of chloramphenicol (CAP) from water. Compared to electrolysis alone, peroxymonosulfate (PMS) alone, and Fe 2+ /PMS, EC/PMS significantly enhanced the CAP degradation. Various parameters, such as the applied current, electrolyte concentration, and PMS dose, were investigated to optimize the process. In addition, acidic conditions facilitated the CAP degradation. The presence of Cl − slightly enhanced the CAP degradation, while both HCO 3 − and NO 3 − exhibited an inhibitory effect on the CAP degradation. The floccules were also analyzed after the reaction by XPS and XRD. Quenching experiments indicated that both sulfate radicals (SO 4 ●− ) and hydroxyl radicals (•OH) were responsible for the CAP degradation. In addition, the degradation products were identified by LC/TOF/MS, and the degradation pathways were proposed accordingly. These results indicated that EC/PMS is a promising treatment process for the remediation of water polluted by CAP.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2021
·Vol. 23
·期 10
·1-15
·
IF 2.253
Guo Zhengqiang,Liu Zheng,Liu Wangyu,Tang Aimin,Chen Wenjin,Luo Shijie
Recently, hydrogels have attracted considerable interests due to their intrinsic flexibility and adjustable mechanical properties. However, the integration of high conductivity, enhanced mechanical performance, and plasticity into one single hydrogel is still challenging. In this work, TEMPO-oxidized cellulose nanofibers (TOCNF, diameter 20–50 nm, length \(\ge\) 1 um) are used as the efficient dispersant of multiwalled carbon nanotubes (MWCNTs, out diameter 5–15 nm, length 10–30 um). Conductive hydrogels are prepared through a simple one pot process and freeze–thaw cyclic method in combination with Fe 3+ ions and TOCNF-MWCNT dispersions in polyvinyl alcohol (PVA) hydrogels. The resulting hydrogels demonstrate high water content (~ 88.8%), mechanical properties (ultimate stress of 1.1 MPa, strain of 336%), and conductivity (0.57 S/m), which can be applied to the preparation of stress or strain sensors. The hydrogel-based resistance sensor is applied to human motion detection, showing a sensitivity of 1.876 kPa −1 with pressure lower than 16 kPa. Similarly, the hydrogel-based capacitive sensor can detect imperceptible pressure of 20 Pa. In addition, the hydrogels also reveal excellent plasticity. In conclusion, the conductive hydrogel possesses excellent comprehensive properties, providing inspiration and potential for the preparation and application of wearable strain sensors.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 8
·2293-2301
·
IF 3.186
Liu Xueping,Shi Shengbin,Yang Su,Gu Liuyu,Gao Lijing,Zhang Jin,Xiao Guomin
Using etherification to convert glycerol into biofuel additives is an effective way to solve the current problem of excess glycerol. In this study, a series of environmentally friendly (x)HPW/ZrO 2 catalysts were synthesized for the etherification of glycerol and tert-butyl alcohol (TBA). The internal microstructure and acidity analysis of the synthesized samples were derived from BET, XRD, Raman spectroscopy, FTIR, SEM, NH 3 -TPD and Py-FTIR. The results revealed that the synthesized catalysts retained the complete Keggin structure of phosphotungstic acid (HPW) which supported on it. The (15)HPW/ZrO 2 catalyst with suitable structure and acidity had an excellent catalytic effect on the etherification reaction. Driven by the (15)HPW/ZrO 2 catalyst, the optimal reaction conditions were determined from parameters of reaction temperature, time, molar rate of glycerol and TBA, and catalyst dosage. 93.2% glycerol conversion and 42.5% selectivity of multi-substituted tert-butyl glycerol ethers (DTBG + TTBG) were obtained under optimal conditions. In addition, even after a total of four consecutive reactions, (15)HPW/ZrO 2 catalyst still demonstrated relatively good catalytic activity. Graphic Abstract
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-10
·
IF 4.38
Chen Huanyu,Cai Ping,Feng Yue,Sun Zhanliang,Wang Yinwen,Chen Yue,Zhang Wei,Liu Nan,Zhou Zhijun
68 Ga-radiolabeled small molecules that specifically target prostate-specific membrane antigen (PSMA) have been extensively investigated, and some of these tracers have been used in the diagnosis of prostate cancer via 68 Ga-positron emission tomography ( 68 Ga-PET). Nevertheless, current 68 Ga-labeled radiotracers show only fair detection rates for metastatic prostate cancer lesions, especially those with lower levels of prostate specific antigen (PSA), which often occurs in the biochemical recurrence of prostate cancer. The goal of this study was to design and synthesize a new PSMA-targeted radiotracer, 68 Ga-SC691, with high affinity for prostate cancer cells and excellent pharmacokinetics. To this end, structural optimization was carried out on the bifunctional group, target motif, and linker while the high affinity targeting scaffold remained. To explore its potential in the clinic, a comparative study was further performed in vitro and in vivo between 68 Ga-SC691 and 68 Ga-PSMA-11, a clinically approved tracer for PSMA-positive prostate cancer. SC691 was radiolabeled to provide 68 Ga-SC691 in 99% radiolabeling yield under mild conditions. High uptake and a high internalization ratio into LNCaP cells were observed in in vitro studies. In vivo studies showed that 68 Ga-SC691 had favorable biodistribution properties and could specifically accumulate on PSMA-positive LNCaP xenografts visualized by micro-PET/CT. This radiotracer showed excellent PET imaging quality and comparable, if not higher, uptake in LNCaP xenografts than 68 Ga-PSMA-11.
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