CHEMOSPHERE
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2017
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IF 4.208
Xiaoxue Pan,Liqing Yan,Ruijuan Qu,Zunyao Wang
The goals of this study were to bring forward new data and insights into the effect of activation methods, operational variables and reaction pathways during sulfate radicals-based oxidation of benzophenone-3 (BP-3) in aqueous solution. Heat, transition metal ions (Fe 2+ , Cu 2+ , Co 2+ ), UV and visible light irradiation were used to activate persulfate (PS) to degrade BP-3. The results showed that these three activation methods can remarkably enhance BP-3 removal efficiency. Under the conditions of [BP-3] 0 : [PS] 0 = 1: 500, pH = 7.0, and 40 °C, complete removal of BP-3 (1.31 μM) was observed in 3 h. In the pH range of 3.0–9.0, the degradation of BP-3 decreased with increasing pH. Increasing the PS dosage accelerated the reaction, while the presence of humic acid (HA) significantly inhibited the efficiency of BP-3 removal. Based on electron paramagnetic resonance (EPR) and radical quenching studies, sulfate and hydroxyl radicals contributed to the oxidation process. According to the evolution of BP-3 and its 7 by-products, as well as frontier electron densities (FED) calculation, two routes were proposed involving hydroxylation, demethylation and direct oxidation. On the whole, this work is a unique contribution to the systematic elucidation of BP-3 removal by PS.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Jiarong Li,Shude Liu,Yuanzhao Xie,Fengluan Jiang,Xinyu Huang,Jianfeng Xia,Limin Wu,Yonghui Deng
Core–shell magnetic polymer microspheres with porous organic shells are highly desired for adsorption, separation, delivery/immobilization of guest objects in catalysis, and drug release. Herein, an amphiphilic block copolymer-directed interfacial assembly and polymerization strategy was reported to synthesize magnetic mesoporous 3-aminophenol–formaldehyde resin (MMAPF) microspheres. The uniform MMAPF microspheres exhibit well-defined core–shell structures, controllable porous shell thickness, high magnetization, and superparamagnetic properties. The abundant hydroxyl and amino groups in the porous shell offer the exceptional capability for stable immobilization of ultrafine Au nanoparticles, which can serve as a magnetically recoverable heterogeneous catalyst for catalyzing the hydrogenation of 4-nitrophenol with a fast reaction rate constant (0.59 min−1) and conversion rate (99%) at room temperature and good recycling stability.
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ANALYTICAL CHEMISTRY
·
2025
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IF 6.7
Qing-Nan Li,Yun-Xi Cui,Zhi-Qi Dai,Zhi-Li Yao,Man-Ying Li,Qi-Liang Cai,De-Ming Kong
The CRISPR/Cas12a system has emerged as a powerful tool in biosensing due to its unique trans-cleavage activity. This study conducted an in-depth investigation of the modulatory capabilities of this system, particularly focusing on the 5′-end modifications of the activator strand, and found that introducing a hairpin structure (HP) at the 5′-end of the activator strand, which was designed based on the RESET effect, can effectively suppress the activator strand’s ability to activate the trans-cleavage activity of the CRISPR/Cas12a system. This suppression is independent of the HP’s relation to the activator strand and the type of linker used (DNA, RNA or peptide). Detaching the HP from the activator strand restores the system’s activity. These findings enrich the development of CRISPR/Cas12a-based biosensors, and expand their application beyond DNA-based target detection to peptide sequence-based target recognition. Based on this discovery, we constructed a sensitive biosensor for caspase-3 (Casp-3), a key executor in apoptosis, by linking the HP to the activator strand with a peptide linker containing a Casp-3 recognition site. The proposed biosensor has been validated for its sensitivity and specificity in detecting Casp-3, as well as for monitoring drug-induced apoptosis through the imaging of Casp-3 in living cells, providing a valuable tool for studying the apoptotic process, screening drugs, assessing drug efficacy, and evaluating treatment outcomes. This strategy also shows promise for detecting other peptide-based targets, broadening the horizons for early disease biomarker detection and timely therapeutic interventions.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Yongfeng Liu,Yupeng Ying,Qingyu Xie,Zhaoju Gao,Xiuwen Shao,Min Zhou,Wei Pei,Xiaosheng Tang,Yusong Tu
Mixed-halide CsPb(Br/Cl)3 perovskite quantum dots (PeQDs) have attracted extensive attention in light-emitting diodes (LEDs), but their low photoluminescent efficiency and especially poor stability impede their practical applications. Here, we employ bifunctional didodecyldimethylammonium thiocyanide (DDASCN) with a pseudohalogen SCN– and branched DDA+ to obtain blue-emitting CsPbBr2Cl PeQDs. DDASCN significantly boosts the photoluminescence quantum yield to 92% by inhibiting nonradiative recombination. Importantly, DDASCN PeQDs show excellent stabilities against air, UV light, heat, and polar solvents. These improved performances were explained by density functional theory calculation, which shows that SCN– fills the Cl– vacancy by simultaneously binding with undercoordinated Pb2+ and Cs+, while DDA+ connects undercoordinated Br– and lies parallel to the PeQD core, leading to efficient passivation and a strong binding capacity. Finally, we achieved high-performance white LEDs by integrating our PeQDs, resulting in a color-rendering index of 92.9, a color gamut of 119.61%, and chromaticity coordinates of (0.33, 0.33). This provides an effective method to obtain efficient and stable CsPb(Br/Cl)3 PeQDs for practical applications.
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MATERIALS CHEMISTRY AND PHYSICS
·
2024
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IF 4.3
Hao Tian,Jie Ma,Bai Yang,Ran Li,Ronghai Yu
It is necessary to broaden absorption bandwidth, regulate applied frequency, reduce the weight and maintain strong absorption for magnetic microwave absorbing materials by constructing suitable material structures to satisfy the requirements for wide applications in various electromagnetic devices. In this work, well-structured amorphous-Co@Nd(BO 2 ) 3 /rGO nanocomposites have been fabricated using a selective chemical reduction in a mixed aqueous solution containing Co 2+ and Nd 3+ ions along with GO sheets reduced by NaBH 4 as the reductant, in which only Co 2+ and GO but no Nd 3+ ions were reduced. Very low coercivity of 0.4 Oe is achieved in amorphous-Co@Nd(BO 2 ) 3 /rGO nanocomposites due to amorphous Co@Nd(BO 2 ) 3 core-shell nanoparticles uniformly anchored on rGO sheets. These soft magnetic rGO-based nanocomposites exhibit high-frequency microwave absorption performance including a minimum reflection loss ( RL min ) value of −84.09 dB at 15.38 GHz for a 2.1 mm thickness at an applied frequency range (12.31–18 GHz) covering almost the entire Ku band. Moreover, a much wider absorption band of 7.24 GHz (10.67–17.89 GHz, RL ≤ −10 dB) with a 2.3 mm thickness along with a RL min value of −35.92 dB is also achieved. These rGO-based magnetic composites also show good structural stability , low density and easily controlled material compositions along with facile chemical fabrication suitable for mass production, which promises their latent use in high-performance microwave absorbing devices. Crystallization behavior of a new amorphous Nd(BO 2 ) 3 phase was also investigated.
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POLYMER
·
2012
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IF 3.438
Xu-Cheng Zhang,Xi Xiong,Jian Yu,Zhao-Xia Guo
Amine-functionalized thermoplastic polyurethane (TPU) electrospun fibers with controllable number of amine groups on fiber surfaces are prepared by co-electrospinning of TPU and 3-aminopropyltriethoxysilane (APS) in DMF/THF 4:6, followed by thermal treatment at 60 °C in a ventilated oven for 24 h. The morphology of the fibers was observed by Field Emission Scanning Electron Microscopy (FESEM), showing a decrease in average fiber diameter with increasing APS content, resulted from significantly increased solution conductivity. The amine groups are homogeneously distributed on the fiber surfaces, as revealed by energy dispersive X-ray spectroscopy (EDX) Si-mapping. Both the Si content measured by X-ray photoelectron spectroscopy (XPS) and NH 2 content obtained by chemical titration show an enrichment of APS condensate on the fiber surfaces, which is explained by the higher mobility of APS to TPU during electrospinning. Gold nanoparticles of 16 nm are homogeneously adsorbed on the amine-functionalized TPU fibers. A conductive gold layer with a surface resistivity of 0.3 Ω/sq is formed after electroless plating using the adsorbed gold nanoparticles as the seeds, demonstrating the usefulness of the amine groups in the preparation of TPU fibers with added functionalities.
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JOURNAL OF MATERIALS SCIENCE
·
2024
·Vol. 59
·期 27
·12447-12463
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IF 3.5
Gong Yanan,Xue Pan,Wang Xinyi,Ma Shaoshuai,Xu Xinhua
Developing hydrogel actuators with excellent driving performance and extended lifespan remains challenging. Ti 3 C 2 T x MXene, as a two-dimensional nanomaterial with a unique layered structure, has attracted widespread attention in flexible hydrogel actuators for its excellent optical absorption properties and tunable surface functionality. However, MXene faces difficulties in dispersion and is prone to oxidation, which significantly hinders the development and use of MXene-based hydrogel actuators. In this study, we fabricated a near-infrared light-driven hydrogel actuator with rapid photo responsiveness and antioxidative properties by incorporating modified MXene with antioxidant characteristics and the pore-forming agent polyvinyl alcohol into the poly( N -isopropylacrylamide) (PNIPAM) hydrogel system. We functionalized MXene nanosheets with (3-aminopropyl)triethoxysilane (APTES), effectively enhancing antioxidative properties, preventing structural degradation caused by spontaneous oxidation, and improving surface properties. This enhanced the dispersion stability of MXene in the system and extended its lifespan from 7 days to over two weeks. The hydrophilic polyvinyl alcohol chains served as drainage channels during hydrogel contraction, imparting the hydrogel with rapid driving capabilities (127.1° s −1 ). Additionally, leveraging the fast response characteristics, we designed an octopus-inspired light-driven soft swimmer and gripper. This work provides novel insights into the application of intelligent responsive hydrogels in biomimetic and practical scenarios. Graphical abstract
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Methods and Applications in Fluorescence
·
2024
·Vol. 12
·期 2
·025001
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IF 2.4
Mingyu Gan,Rui Yao,Baoping Wang,Jiarong Li,Ning Wang,Martin M F Choi,Wei Bian
Dopamine (DA) is the most abundant catecholamine neurotransmitter in the brain and plays an extremely essential role in the physiological activities of the living organism. There is a critical need for accurately and efficiently detecting DA levels in organisms in order to reflect physiological states. Carbon nitride quantum dots (C3N4) were, in recent years, used enormously as electrochemical and fluorescence probes for the detection of metal ions, biomarkers and other environmental or food impurities due to their unique advantageous optical and electronic properties. 3-Aminophenylboronic acid (3-APBA) can specifically combine with DA through an aggregation effect, providing an effective DA detection method. In this work, 3-APBA modified carbon nitride quantum dots (3-APBA-CNQDs) were synthesized from urea and sodium citrate. The structure, chemical composition and optical properties of 3-APBA-CNQDs were investigated by XRD, TEM, UV–visible, and FT-IR spectroscopy. The addition of DA could induce fluorescence quenching of 3-APBA-CNQDs possibly through the inner filter effect (IFE). 3-APBA-CNQDs shows better selectivity and sensitivity to DA than other interfering substances. By optimizing the experiment conditions, good linearity was obtained at 0.10–51 μM DA with a low detection limit of 22.08 nM. More importantly, 3-APBA-CNQDs have been successfully applied for the detection of DA in human urine and blood samples as well as for bioimaging of intracellular DA. This study provides a promising novel method for the rapid detection of DA in real biological samples.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Hairui Fang,Jiawei Zhang,Eryang Shang,Hong Chen,Xiao Ma,Xingyu Kang,Huizhang Zhao,Yuxia Liu,Dong Wang
Metal oxides are widely used because of their simple structure, low price, and excellent gas-sensitive properties. But now, the metal oxide sensor faces two challenges. One is that when the detection limit of the sensor is low, it will be affected by a high concentration of gas and fail in practical applications. Second, the metal oxide sensor is susceptible to temperature changes, resulting in inaccurate measurement results. To address the above problems, the performance of metal oxides is enhanced through doping. Indium oxide doped with various levels of indium molybdate was prepared using a two-step hydrothermal method resulting in a composite material with an n-n heterostructure. The interaction formed by the n-n heterostructure enhances the redox reaction between NO 2 gas and the sensor, and the unique nano cluster structure provides more active sites for the sensor, significantly improving the gas performance of the sensor towards NO 2 . Sensors based on In 2 (MoO 4 ) 3 with a doping ratio of 4 % (the sample IM3) showed excellent gas sensitivity. The lower and upper detection limits of the sensor are 200 ppb (response is 1.46) and 150 ppm (response is 515.94), respectively. And the sensor has good resistance to ultra-high concentration (10000 ppm) nitrogen dioxide (NO 2 ) impact. In the range of 130–170°C, the temperature has a small and linear effect on the sensor response, which is very beneficial for temperature correction of gas sensors. The sensor prepared by In 2 (MoO 4 ) 3 doped In 2 O 3 composite material has a good potential for application in engineering practice.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2025
·Vol. 172
·期 3
·036504
·
IF 3.3
Ke Qu,Qianlan Li,Chao Liang,Jia Wei
In typical solid-contact potentiometric sensing, ion selective membranes (ISMs) play the role of recognizing the target analytes. A variety of solid-contact materials have been utilized to realize the ion-to-electron transduction. However, the ISMs show some drawbacks during practical application. Recent research efforts have been devoted to developing ISM-free potentiometric sensing. In this work, an ion-imprinted conducting poly (pyrrole-co-pyrrole-3-carboxylic acid) copolymer was investigated to achieve the ISM-free potentiometric sensing toward nitrate, an important anion to monitor in the environment. The copolymer-based electrochemical sensor afforded good potentiometric responses toward nitrate in a Nernstian manner, exhibiting superior or comparable sensing performances with existing ISM-based potentiometric sensors. Compared with polypyrrole homopolymer, the introduced carboxylate group in the side chain of the copolymer was likely to contribute to the redox activity, enabling better ion-to-electron transduction. More importantly, a unique self-doped effect was observed in the prepared poly (pyrrole-co-pyrrole-3-carboxylic acid), extending the working pH range of polypyrrole family and providing potential implications to develop electrochemical sensors when the environmental pH matters.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2024
·
IF 4.8
Yujing Du,Linjie Li,Xixuan Li,Jingxuan Tan,Yanjie Qin,Yongning Lv,Xuejia Zhai
DL-3-n-butylphthalide (NBP) is isolated from the seeds of Apium graveolens L., and has been recently used as a neuroprotective agent for acute ischemic stroke. The present study aimed to determine the efficacy and safety of the combined use of dual antiplatelet therapy (DAPT) and NBP for treating of acute ischemic stroke in rats and to explore the synergistic mechanism of this treatment strategy in rat middle cerebral artery occlusion models. The efficacy of DAPT combined with NBP was evaluated by determining neurological deficits, infarction status, and histological changes. Changes in body weight, blood glucose level, blood count, and serum biochemical parameters were detected to evaluate the safety. To explore the synergistic pharmacological mechanism, the mRNA expression and protein levels of key proteins in the pyroptosis–inflammatory pathway, and the pyroptosis ratio of microglias were examined. Compared with the administration of NBP or DAPT alone, combination of them significantly improved neurological deficits, reduced infarct area, and repaired tissue injury and inflammation after cerebral ischemia. No hepatorenal toxicity was observed. The mRNA expression and protein levels of key proteins in the pyroptosis–inflammation pathway, and the pyroptosis ratio of microglias were significantly downregulated in the combined administration group than in the monotherapy group. We demonstrated that the combined use of NBP and DAPT exhibits better efficacy and high safety and plays a synergistic role by inhibiting the pyroptosis–inflammation pathway in the brain tissues, particularly in microglial cells.
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JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Tianyang Hou,Yuangang Xu,Ze Xu,Xiaopeng Zhang,Ming Lu
The formation of non-metallic pentazolate salts from the combination of simple nitrogen-rich cations with cyclo -N 5 − is expected to be applied in propellants and explosives. In this work, a series of structurally similar cations ([NH 3 CH 3 ] + , [NH 2 (CH 3 ) 2 ] + , [NH(CH 3 ) 3 ] + , and [N(CH 3 ) 4 ] + ) were used to synthesize four cyclo -N 5 − containing energetic salts, and the contribution of crystal stacking mode, hydrogen bonding, C–H··· π and π -stacking interactions in the stabilization of cyclo -N 5 − salts has been investigated by geometrical and Hirshfeld surface analyses as well as theoretical calculations. All salts have been thoroughly characterized by single-crystal X-ray diffraction, infrared (IR), multinuclear NMR ( 1 H and 13 C) spectroscopy, and elemental analysis. The decomposition temperatures of all salts are higher than 75 °C, as measured by thermogravimetric (TG). These compounds all show low sensitivities (IS ≥ 35 J, FS > 360 N) measured by standard BAM methods. Their heats of formation and detonation performances were calculated using the Born–Haber energy cycle and K-J method (“Pilem” program), respectively. This study has great significance for future design and synthesis of cyclo -N 5 − containing energetic materials.
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