APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Bingjie Ding,Yongjun Jiang,Beibei Xu,Sheng Dai,Honghui Gong,Xiuge Zhao,Yefeng Yao,Pengfei An,Zhenshan Hou
This work demonstrated a facile methodology to construct single Nb site catalysts with merely 0.63 wt% Nb by employing α-hydroxy carboxylic acid-functionalized cotton fiber as green and sustainable supporting material. The as-synthesized catalysts have been characterized thoroughly and exhibited a superior catalytic activity for selective oxidation of aniline into azoxybenzene with nearly 100% utilization efficiency of H 2 O 2 under mild and green conditions. Notably, it demonstrated the highest TOF (4806 h −1 ) among the currently reported heterogeneous catalysts. Moreover, the catalyst has steadily been operated under continuous-flow conditions, which afforded significant benefits compared to batch processes as reported in these transformations. The activity test and catalyst characterization indicated that the atomically dispersed Nb-peroxo coordination centers were actually catalytic sites. Especially, the α-hydroxy carboxylic acid groups on cotton fiber played an important role in coordinating/stabilizing single Nb site. Moreover, 1 H MAS NMR spectra verified that there exists an acid-base interaction between arylamines and free α-hydroxy carboxylic acid groups covalently grafted on cotton fiber, which was favorable for adsorption and activation of the substrates. Mechanism studies indicated that the azoxy derivatives were produced through condensation step between N-phenylhydroxylamine and nitrosobenzene rather than direct oxidation of azobenzene . The work provides an economical and environmentally friendly approach to construct single–site catalysts for the oxidation catalysis.
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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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RSC Advances
·
2022
·Vol. 13
·期 1
·499-505
·
IF 4.036
Rong Wang,Jiamin Luo
Rapid and accurate identification of bacteria is essential to ensure food safety and prevent pathogenic bacterial infection. In this study, a highly efficient method was established for accurately identifying bacterial species by applying Ag NP-filter paper based Surface enhanced Raman spectroscopy (SERS) analysis and Partial Least Squares-Discriminant Analysis (PLS-DA) statistical methods. The flexible Ag NP filter paper substrate with high sensitivity and uniformity was prepared by a facile and low-cost silver mirror reaction at room temperature, which exhibited desirable SERS activity in bacteria detection. Furthermore, PLS-DA was successfully employed to distinguish SERS spectra from S. aureus CMCC 26003, E. faecalis ATCC29212 and L. monocytogenes ATCC 19115 with a sensitivity of 93.3–100%, specificity of 96.7–97%, and overall predicting accuracy of 95.8%. This exploratory study demonstrates that a Ag NP-filter paper based SERS sensor coupled with PLS-DA has great potential for rapid and effective detection and identification of bacteria.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Dian Dai,Mingxiang Qv,Dongyang Liu,Chunming Tang,Wei Wang,Qirui Wu,Zhihong Yin,Liandong Zhu
Magnetic harvesting of microalgae depends on the interface interactions between microalgal cells and flocculants, and thus it is important to find a reasonable evaluation method understand these interface interactions. In this effort, we discussed the formation mechanism and pH regulation of microalgae magnetic harvesting via magnetic chitosan (Fe 3 O 4 @SiO 2 -CS) synthesized by a micro-emulsion method. The flocculation performances and mechanisms during the harvesting of microalgae by the novel flocculant were evaluated. The synthesis process and structure were determined by XRD, FT-IR, SEM and XPS, and the results indicated that Fe 3 O 4 @SiO 2 -CS was successfully prepared. The collection efficiency of 96.52 % was achieved for Chlorella vulgaris within 3 min using Fe 3 O 4 @SiO 2 -CS with the Fe 3 O 4 @SiO 2 and CS mass ratio of 1:3 under pH 1.0. Moreover, this study introduced the two-dimension fractal dimension and extended Derjaguin-Landau-Verwey-Overbeek (E-DLVO) model to evaluate the harvesting performances and mechanisms of Fe 3 O 4 @SiO 2 -CS. Experimental results showed that a strong electrostatic interaction was formed under acidic conditions between Fe 3 O 4 @SiO 2 -CS and microalgae cells with D 2 = 1.82 (fractal dimension value). The hydrophobic tryptophan-like amino acid was observed in the slime-extracellular polymeric substances (S-EPS) secreted by microalgae. S-EPS was found to be a significant substance to promote harvesting performance when the system was neutral or alkaline. This work provides deeper insights into microalgae harvesting by Fe 3 O 4 @SiO 2 -CS as well as reasonable mechanisms to illustrate the interaction of Fe 3 O 4 @SiO 2 -CS and microalgae under different pH values.
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MOLECULES
·
2022
·Vol. 27
·期 23
·8455
·
IF 4.927
Hongping Xu,Junhong Ling,Han Zhao,Xinyi Xu,Xiao-kun Ouyang,Xiaoyong Song
Chemotherapy is a common method for tumor treatment. However, the non-specific distribution of chemotherapeutic drugs causes the death of normal cells. Nanocarriers, particularly mesoporous carriers, can be modified to achieve targeted and controlled drug release. In this study, mesoporous polydopamine (MPDA) was used as a carrier for the antitumor drug doxorubicin (DOX). To enhance the release efficiency of DOX in the tumor microenvironment, which contains high concentrations of glutathione (GSH), we used N,N-bis(acryloyl)cysteamine as a cross-linking agent to encapsulate the surface of MPDA with fucoidan (FU), producing MPDA-DOX@FU-SS. MPDA-DOX@FU-SS was characterized via transmission electron microscopy, thermogravimetric analysis, and X-ray photoelectron spectroscopy (XPS), and its antitumor efficacy in vitro was investigated. The optimal conditions for the preparation of MPDA were identified as pH 12 and 20 °C, and the optimal MPDA-to-FU ratio was 2:1. The DOX release rate reached 47.77% in an in vitro solution containing 10 mM GSH at pH 5.2. When combined with photothermal therapy, MPDA-DOX@FU-SS significantly inhibited the growth of HCT-116 cells. In conclusion, MPDA-DOX@FU-SS may serve as a novel, highly effective tumor suppressor that can achieve targeted drug release in the tumor microenvironment.Keywords:mesoporous polydopamine;antitumor;nanomedicine;photothermal synergistic chemotherapy
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ACS Omega
·
2022
·
IF 4.132
Xiaolu Xiong,Chengwang Guo,Gengyang Yan,Bingxin Han,Zan Wu,Yueqian Chen,Shiqi Xu,Peng Shao,Hong Song,Xiyan Xu,Junfeng Han
Water quality guarantee in remote areas necessitates the development of portable, sensitive, fast, cost-effective, and easy-to-use water quality detection methods. The current work reports on a microfluidic paper-based analytical device (μPAD) integrated with a smartphone app for the simultaneous detection of cross-type water quality parameters including pH, Cu(II), Ni(II), Fe(III), and nitrite. The shapes, baking time, amount, and ratios of reaction reagent mixtures of wax μPAD were optimized to improve the color uniformity and intensity effectively. An easy-to-use smartphone app was established for recording, analyzing, and directly reading the colorimetric signals and target concentrations on μPAD. The results showed that under the optimum conditions, the current analytical platform has reached the detection limits of 0.4, 1.9, 2.9, and 1.1 ppm for nitrite, Cu(II), Ni(II), and Fe(III), respectively, and the liner ranges are 2.3–90 ppm (nitrite), 3.8–400 ppm (Cu(II)), 2.9–1000 ppm (Ni(II)), 2.8–500 ppm (Fe(III)), and 5–9 (pH). The proposed portable smartphone-app integrated μPAD detection system was successfully applied to real industrial wastewater and river water quality monitoring. The proposed method has great potential for field water quality detection.
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TALANTA
·
2022
·
IF 6.556
Qiu-Shun Li,Yan Yang,Yong-Dong Du,Lei Cai,Yao-Hong Ma,Jun-Hui Yang,Mingyu Li,Qing-Jun Meng,Qing-Ai Liu,Wen-Fei Dong
Long period fiber gratings (LPFGs) have special advantages in the detection of salt concentrations due to small volume, corrosion resistance and immunity to electromagnetic interference. However, it is very difficult to distinguish low-concentration salt solutions with usual LPFGs owing to the poor sensitivity. In this paper, the detection capability of the LPFG to low-concentration salt solutions was significantly improved by assembling salt-containing poly (diallyldimethylammonium chloride) (PDDA) and salt-containing poly (sodium- p -styrenesulfonate) (PSS). Experimental results showed that, the responsive wavelength range of the LPFG was remarkably broadened in low-concentration salt solutions after assembling nanofilms . The suitable detection range of the PDDA/PSS films coated LPFG for salt concentrations was 0–3%. In such a range, the average refractive index sensitivity and the average salinity sensitivity of the LPFG was as high as 29545.9 nm/RIU and 52.2 nm/% respectively. Compared with the LPFG without nanofilms, the discrimination ability of the PDDA/PSS films coated LPFG to 0–3% salt solutions increased by 568 times. The analysis demonstrated that PDDA and salt in the assembly solutions played a pivotal role in the above effects. The proposed sensor has extensive application prospects in the monitoring of salt concentration in many fields such as seawater , food processing, fermentation process , etc.
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Polymers
·
2022
·Vol. 14
·期 22
·4888
·
IF 4.967
Jia Qu,Hongpu Huang,Qiang Yang,Wei Gong,Meilan Li,Liangliang Chang,Baoyue Cao,Guochun Zhang,Chunsheng Zhou
Water pollution is a worldwide problem that requires urgent attention and prevention and exceeding use of heavy-metal ions is one of the most harmful factors, which poses a serious threat to human health and the ecological environment. In this work, a magnetic oxidized micro/mesoporous carbon (MOMMC) was prepared for the easy separation of Cu(II) and Pb(II) from water. The dual-template method was used to prepare micro/mesoporous carbon using sucrose as the carbon source, silica nanoparticles formed by tetraethyl orthosilicate as the microporous templates, and triblock copolymer F127 as the mesoporous template. MOMMC was obtained by oxidation using potassium persulfate and then magnetized through in situ synthesis of Fe3O4nanoparticles. FTIR, TG-DSC, XRD, TEM, SEM, nitrogen adsorption–desorption isotherms, zeta potential, and VSM were used to confirm the synthetic process, structure, and basic properties of MOMMC. The high-saturation magnetization (59.6 emu·g−1) of MOMMC indicated its easy and fast separation from water by an external magnetic field. Kinetics studies showed that the adsorption of Cu(II) and Pb(II) on MOMMC fit the pseudo-second-order model well. Isotherm studies showed that the adsorption behavior of Cu(II) was better described by the Langmuir model, and the adsorption behavior of Pb(II) was better described by both Langmuir and Redlich–Peterson models. MOMMC obtained efficient adsorption for Cu(II) and Pb(II) with the large adsorption capacity of 877.19 and 943.40 mg·g−1according to the Langmuir adsorption isotherm equation, and a better selectivity for Pb(II) was observed in competitive adsorption. MOMMC still possessed a large adsorption capacity for Cu(II) and Pb(II) after three adsorption–desorption cycles. These findings show that MOMMC represents an excellent adsorption material for the efficient removal of heavy-metal ions.Keywords:magnetic mesoporous carbon;adsorption;copper;lead;adsorption kinetics;adsorption isotherms;selectivity
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Enmin Zong,Runfang Fan,Hao Hua,Jiayao Yang,Shengtao Jiang,Jinfeng Dai,Xiaohuan Liu,Pingan Song
It has been always attractive to design a sustainable bio-derived adsorbent based on industrial waste lignin for removing organic dyes from water. However, existing adsorbent strategies often lead to the difficulties in adsorbent separation and recycling. Herein, we report a novel magnetically recyclable bio-adsorbent of Mg(OH) 2 /Fe 3 O 4 /PEI functionalized enzymatic lignin (EL) composite (EL-PEI@Fe 3 O 4 -Mg) for removing Congo red (CR) by Mannish reaction and hydrolysis-precipitation. The Mg(OH) 2 and PEI functionalized EL on the surface act as active sites for the removal of CR, while the Fe 3 O 4 allows for the easy separation under the help of a magnet. As-obtained EL-PEI@Fe 3 O 4 -Mg forms flower-like spheres and has a relatively lager surface area of 24.8 m 2 g −1 which is 6 times that of EL. The EL-PEI@Fe 3 O 4 -Mg exhibits a relatively high CR adsorption capacity of 74.7 mg g −1 which is 15 times that of EL when initial concentration is around 100 mg L −1 . And it can be easily separated from water by applying an external magnetic field. Moreover, EL-PEI@Fe 3 O 4 -Mg shows an excellent anti-interference capability according to the results of pH values and salt ions influences. Importantly, EL-PEI@Fe 3 O 4 -Mg possesses a good reusability and a removal efficiency of 92 % for CR remains after five consecutive cycles. It is illustrated that electrostatic attraction, π-π interaction and hydrogen binding are primary mechanisms for the removal of CR onto EL-PEI@Fe 3 O 4 -Mg. This work provides a novel sustainable strategy for the development of highly efficient, easy separable, recyclability bio-derived adsorbents for removing organic dyes, boosting the efficient utilization of industrial waste lignin.
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JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY
·
2022
·Vol. 38
·期 1
·156-165
·
IF 4.351
Xiuhong Liao,Wen Zhang,Tao Yang,Zhaochu Hu,Tao Luo,Xianli Zeng,Lian Zhou
Rare earth elements (REEs) in porewater can be useful proxies in the studies of marine geochemistry. The main challenges for the determination of REEs in porewater samples from marine sediments lie in three aspects—low concentration, high salinity, and limited sample sizes (usually only a few millilitres). In this study, a method based on laser ablation (LA) solution sampling ICP-MS for REEs analysis of small volumes (2–4 mL) of porewater is established. With the help of matrix removal and REEs preconcentration from natural liquids by a miniaturized Fe(OH)3 co-precipitation method, a high enrichment factor (10–20 fold) was achieved with only 2 mL of the original liquid, which was preconcentrated to be as small as 100–200 μL. Ultratrace (sub-pg mL−1) analysis was realized through the use of high laser ablation pulse frequency (up to 250 Hz) and based on the high transport efficiency of aerosol particles by the LA system. Due to the almost “dry” ICP condition generated by LA and nitrogen addition (5 mL min−1) to the plasma, the CeO+/Ce+ ratio was reduced to approximately 0.05%, and the total yields of BaO+ and BaOH+ ions were reduced to 0.003%, which means that the potential biases induced by oxide and hydroxide interferences could be negligible. Method validation was achieved through the analysis of the seawater reference material NASS-7 and a spike recovery test with quantitative recoveries of 94–101% for REEs. The application results of porewater samples characterized by no or slight Ce anomalies together with significantly positive Eu anomalies may be indicative of highly reducing and neutral to basic pH conditions. Reagents consumed by the LA-ICP-MS method were significantly reduced, making it a more environment-friendly method. Moreover, the simplicity in sample preparation and lack of need for special reagents or devices give the proposed method great potential for wide applications in the determination of REEs in natural water samples.
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Current Research in Food Science
·
2022
·
IF 6.269
Simeng Shao,Weiyin Xu,Zhaoyang Xie,Mengyuan Li,Jingli Zhao,Xinxin Yang,Peng Yu,Hongmei Yang
Despite the widely recognized importance of ginseng carbohydrates, their structural analysis is still challenging due to structural complexity. This study presents the first ion mobility-mass spectrometry (IM-MS) combined with 1-phenyl-3-methyl-5-pyrazolone (PMP) labeling and multivariate data analysis for profiling carbohydrates in the seven ginseng products. 11 carbohydrates were tentatively annotated, including 5 first found in ginseng, and three of them were solely detected in black ginseng (BG) samples, speculated as monosaccharides bearing various groups based on MS 2 analysis. Furthermore, 3D profiles of carbohydrates in IM-MS of the samples showed good discrimination between the varieties of ginseng which were classified into two groups utilizing carbohydrate contents by PLS-DA. The big difference between BG and the others may be ascribed to the repeated heating and steaming process for preparation of BG products. Our findings may provide insights into the differences in bioactivity of different ginseng varieties for future research and show a valuable methodology for discovering unknown carbohydrates.
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MOLECULES
·
2022
·Vol. 27
·期 22
·7947
·
IF 4.927
Qingmei Sun,Yawen Hong,Zhaoxu Yang,Peixia He,Chao Chen,Jincheng Wang,Qinjie Weng
Pyrroloquinoline quinone (PQQ) is a powerful antioxidant coenzyme existing in diet, benefiting growth, development, cognition function, and the repair of damaged organs. However, a method for detecting PQQ in vivo was rarely described, limiting the research on the bioanalysis and metabolic properties of PQQ. In this study, a novel, simple, and efficient ultra-high performance liquid chromatography/tandem mass spectrometry (UPLC-MS/MS) method was developed and validated to quantify the concentration of PQQ in rat plasma. Detection through mass spectrometry was operated by multiple reaction monitoring (MRM) in negative electrospray ionization mode with ion transitionsm/z328.99→197.05 for PQQ andm/z280.04→195.04 for the internal standard. The calibration curves were linear up to 10,000 ng/mL, with a lower limit of quantitation of 10 ng/mL. Inter-run and intra-run precision ranged from 1.79% to 10.73% and accuracy ranged from −7.73% to 7.30%. The method was successfully applied to a toxicokinetic study in Sprague–Dawley rats after the oral administration of PQQ disodium salt at doses of 250 mg/kg, 500 mg/kg, and 1000 mg/kg. The toxicokinetic parameters were subsequently analyzed, which may provide valuable references for the toxicokinetic properties and safety evaluation of PQQ.Keywords:PQQ disodium salt;UPLC-MS/MS;toxicokinetic;rat plasma
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