Chemistry of Heterocyclic Compounds
·
2021
·Vol. 57
·期 7
·806-816
·
IF 1.277
An Xiaoying,Gao Lei,Wang Mingliang,Wu Haitao,Wang Lanzhi
Novel, efficient and environmentally friendly approaches have been developed for the synthesis of 1,5-benzodiazepine-2,3-dicarboxylates by one-pot three-component domino reactions in the presence of a catalytic amount of γ-Fe 2 O 3 @SiO 2 /Ce(OTf) 3 in EtOH at ambient temperature. A total of 32 2,5-dihydro-1 H -1,5-benzodiazepine-2,3-dicarboxylates and 2-methyl-2,3-dihydro-1 H -1,5-benzodiazepine-2,3-dicarboxylates with enamine or imine structure of the heterocycle, respectively, were obtained in good yields by reacting substituted 1,2-phenylenediamine, β-carbonyl esters, and ethyl glyoxylate or ethyl pyruvate. One-pot reactions were successfully realized to form one new cycle and four new bonds (one C–C, two C–N, one C=C or two C–C, one C–N, one C=N). Furthermore, plausible mechanisms for the formation of 1,5-benzodiazepine-2,3-dicarboxylates have been proposed. The salient features of this reaction include short reaction time, mild reaction conditions, moderate to excellent yields, recyclability of the catalyst, and wide substrate scope.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 33
·15963-15974
·
IF 3.553
Wu Yanyan,Li Ying,Lü Zhe,Xu Lingling,Wei Bo
Developing efficient and durable oxygen evolution reaction (OER) electrocatalysts with non-noble elements is particularly urgent for electrochemical water splitting. Herein, we report heterostructural Ni 3 S 2 –Fe 5 Ni 4 S 8 hybrids directly grown on redox-NiFe foams (denoted as NFS/rNF) as excellent pre-catalysts for OER in 1 M KOH media. The electrochemical performance can be tuned by amount of sulfur source, and the optimized electrode only needs low overpotentials of 199 mV and 240 mV to attain 10 mA cm −2 and 100 mA cm −2 , respectively. Moreover, the overpotential is further reduced to 231 mV to deliver 100 mA cm −2 after multi-cyclic voltammogram scans, due to the exposure of abundant in situ generated Ni(Fe)OOH species. Excellent stability with continuous 40 h operation is also demonstrated. Our study provides a new strategy for direct synthesis of self-standing integrated hybrid electrodes for efficient and durable water oxidation.
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Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 4
·470-482
·
IF 4.5
Wang Yitong,Zhang Yue,Wang Li
Amino-functionalized zirconia was synthesized by the co-condensation method using zirconium butanol and 3-aminopropyltriethoxy silane for the simultaneous removal of various impurities from aqueous 30% H 2 O 2 solution. The results of Fourier transform infrared (FTIR) and Zeta potential showed that the content of N in amino-functionalized zirconia increased with the added amount of 3-aminopropyltriethoxy silane. Accordingly, the removal efficiency of total oxidizable carbon, phosphate and metallic ions from the H 2 O 2 solution increased. The adsorbent with an N content of 1.62% exhibited superior adsorption performance. The removal efficiency of 82.7% for total oxidizable carbon, 34.2% for phosphate, 87.1% for Fe 3+ , 83.2% for Al 3+ , 55.1% for Ca 2+ and 66.6% for Mg 2+ , with a total adsorption capacity of 119.6 mg·g −1 , could be achieved. The studies conducted using simulated solutions showed that the adsorption process of phosphate on amino-functionalized zirconia is endothermic and spontaneous, and the behaviors could be well described by the pseudo-second-order model and Langmuir model with a maximum adsorption capacity of 186.7 mg·g −1 . The characterizations of the spent adsorbents by Zeta potential, FTIR and X-ray photoelectron spectroscopy revealed that the adsorption mechanism of phosphate is predominantly electrostatic attraction by the protonated functional groups and complementary ligand exchange with zirconium hydroxyl groups.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-13
·
IF 14.919
Wu Junru,Wang Xianshu,Liu Qi,Wang Shuwei,Zhou Dong,Kang Feiyu,Shanmukaraj Devaraj,Armand Michel,Rojo Teofilo,Li Baohua,Wang Guoxiu
The current Li-based battery technology is limited in terms of energy contents. Therefore, several approaches are considered to improve the energy density of these energy storage devices. Here, we report the combination of a heteroatom-based gel polymer electrolyte with a hybrid cathode comprising of a Li-rich oxide active material and graphite conductive agent to produce a high-energy “shuttle-relay” Li metal battery, where additional capacity is generated from the electrolyte’s anion shuttling at high voltages. The gel polymer electrolyte, prepared via in situ polymerization in an all-fluorinated electrolyte, shows adequate ionic conductivity (around 2 mS cm −1 at 25 °C), oxidation stability (up to 5.5 V vs Li/Li + ), compatibility with Li metal and safety aspects (i.e., non-flammability). The polymeric electrolyte allows for a reversible insertion of hexafluorophosphate anions into the conductive graphite (i.e., dual-ion mechanism) after the removal of Li ions from Li-rich oxide (i.e., rocking-chair mechanism).
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MICROCHIMICA ACTA
·
2015
·Vol. 183
·期 2
·625-631
·
IF 3.741
Ding Caiping,Yan Yinghan,Xiang Dongshan,Zhang Cuiling,Xian Yuezhong
Greigite magnetic nanoparticles (Fe 3 S 4 -MNPs) were prepared and reveal a peroxidase-like activity. Kinetic studies revealed a pseudo-enzymatic activity that is much higher than that of other magnetic nanomaterial-based enzyme mimetics. This finding was exploited to design a photometric enzymatic glucose assay based on the formation of H 2 O 2 during enzymatic oxidation of glucose by glucose oxidase, and the formation of a blue product from an enzyme substrate that is catalytically oxidized by H 2 O 2 in the presence of Fe 3 S 4 -MNPs. Glucose can be detected in the 2 to 100 μM concentration range, and the low detection limit is 0.16 μM. The method was applied to quantify glucose in human serum. In our perception, this enzyme mimetic has a large potential in that it may be used in other oxidase based assays, but also in ELISAs.
Fe 3 S 4 magnetic nanoparticles (MNPs) are shown to act as peroxidase mimetics and this was used to design a glucose oxidase (GOx) based glucose assay where the H 2 O 2 formed during oxidation of glucose oxidizes tetramethylbenzidine (TMB) to give a blue product which can be quantified by photometry.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Dong Hongzheng,Pan Xiangyu,Gong Yuancai,Xue Mengfan,Wang Pin,Ho-Kimura SocMan,Yao Yingfang,Xin Hao,Luo Wenjun,Zou Zhigang
In the past decades, a band alignment theory has become a basis for designing different high-performance semiconductor devices, such as photocatalysis, photoelectrocatalysis, photoelectrostorage and third-generation photovoltaics. Recently, a faradaic junction model (coupled electron and ion transfer) has been proposed to explain charge transfer phenomena in these semiconductor heterojunctions. However, the classic band alignment theory cannot explain coupled electron and ion transfer processes because it only regulates electron transfer. Therefore, it is very significant to explore a suitable design concept for regulating coupled electron and ion transfer in order to improve the performance of semiconductor heterojunctions. Herein, we propose a potential window alignment theory for regulating ion transfer and remarkably improving the photoelectrocatalytic performance of a MoS 2 /Cd-Cu 2 ZnSnS 4 heterojunction photocathode. Moreover, we find that a faradaic potential window, rather than the band position of the intermediate layer, is a criterion for identifying interface charge transfer direction. This finding can offer different perspectives for designing high-performance semiconductor heterojunctions with suitable potential windows for solar energy conversion and storage.
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Nanoscale Research Letters
·
2017
·Vol. 12
·期 1
·1-7
·
IF 2.833
Zhai Haifa,Qi Jingjing,Zhang Xiang,Li Hongjing,Yang Liping,Hu Chunjie,Liu Hairui,Yang Jien
Hollow structure LiNb 3 O 8 photocatalysts were prepared by a hydrothermal method assisting sintering process. The particles’ aggregation to form hollow structures with obvious cavities can be attributed to the Li element volatilization during calcination process. All the LiNb 3 O 8 powders show high photocatalytic efficiency of degradation of methylene blue (MB), especially for the sample calcined at 700 °C (LNO700), with only 3 h to completely decompose MB. The photo-degradation of MB follows the pseudo-first-order kinetics, and the obtained first-order rate is 0.97/h. The larger degradation rate of LNO700 can be attributed to its hollow structure which provides a larger specific surface area and more active sites to degrade the MB molecules. The cycling test of photo-degradation and adsorption of MB over LNO700 powder indicates that the hollow structure of the LiNb 3 O 8 photocatalyst is stable and the LiNb 3 O 8 photocatalyst is an efficient photocatalyst with good reusability, confirmed by the XRD and X-ray photoelectron spectroscopy tests before and after photo-degradation of MB.
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CHROMATOGRAPHIA
·
2019
·Vol. 82
·期 7
·1017-1027
·
IF 1.552
Huang Xueqian,Liu Minzhuo,Liu Xiong,Liu Qi,Chen Xiaoqing
In this work, by adopting polyethyleneimine functionalized multi-walled carbon nanotubes as the absorbent, a solid phase extraction based method for fast and selective screening of carboxylic acid compounds was developed. The structure and morphology of the polyethyleneimine functionalized multi-walled carbon nanotubes were confirmed via scanning electron micrograph, transmission electron microscopy, Fourier transform infrared spectra and X-ray photoelectron spectroscopy. And the proposed approach was successfully applied to screen carboxylic compounds from the crude extract of Perilla frutescens . As a result, seven polyhydric compounds with carboxyl including caffeic acid, luteolin-7- O -diglucuronide, apigenin-7- O -diglucuronide, sagerinic acid, scutellarein-7- O -glucuronide, rosmarinic acid, and apigenin-7- O -glucuronide were favorably screened out from compounds without carboxyl group. Similar screening results were also obtained via generalizing the method to the crude extract of Chrysanthemum . This strategy could serve as a rapid and efficient pathway for preliminary screening of certain types of compounds from complex natural products.
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EUROPEAN JOURNAL OF DRUG METABOLISM AND PHARMACOKINETICS
·
2023
·Vol. 48
·期 5
·595-614
·
IF 1.9
Han Yiran,Wen Tiantian,Wang Jia,Shi Jinmiao,Zhu Yongqiang
Background and Objectives Rearranged during transfection (RET) is a transmembrane receptor tyrosine kinase that plays a crucial role in tumorigenesis. FHND5071, a potent and selective RET kinase inhibitor, could exert antitumor effects by inhibiting RET autophosphorylation. The present work aims to profile the pharmacokinetics of FHND5071 in in vivo and in vitro experiments as a ground work for further clinical research. Methods The absorption, distribution, metabolism, and excretion properties of FHND5071 were examined, along with metabolite production and cytochrome P450 (CYP) phenotyping assay. Additionally, plasma protein binding and pharmacokinetics in mice were investigated. Results Microsomal stability assay corroborated moderate to high clearance of FHND5071, and the use of UPLC-Q-TOF-MS identified a total of six metabolites and suggested a possible metabolic pathway involving oxidation, demethylation, and N-dealkylation. Primary contributors to the CYP-mediated metabolism of FHND5071 were found to be CYP2C8 and CYP3A4, and FHND5071 displayed low permeability and acted as a substrate for the P-glycoprotein (P-gp). FHND5071 had a moderate to high binding in plasma and exhibited a moderate absorption degree (absolute bioavailability > 60%) The distribution of FHND5071 in mouse tissues was rapid (mostly peaking at 1–4 h) and wide (detectable in almost all tissues and organs), with the highest exposure in the spleen. A small fraction of FHND5071 was excreted via the urine and feces, and a presumed metabolic pathway involving 20 metabolites in mice is proposed. Conclusion Pharmacokinetic characteristics of FHND5071 were systemically profiled, which may lay the foundation for further clinical development as a drug candidate. Graphical Abstract
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2019
·Vol. 189
·期 3
·960-971
·
IF 2.14
Wang Mengjun,Zhu Mengde,Wang Yu,Fan Zichun,Wu Shining,Zhang Xiaobo,Tong Zhiwei
In this paper, we synthesized HNbMoO 6 /C composite through the calcination of octylamine-intercalated HNbMoO 6 precursor. The resulting HNbMoO 6 /C composite showed some new phases of MoO 2 , MoO 3 , NbO 2 , Nb 2 O 5 , and carbon, which was fully confirmed via powder X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and X-ray photoelectron spectroscopy (XPS) technologies. Besides, the HNbMoO 6 /C hybrid was coated on glass carbon electrode to construct an electrochemical sensor for sensitive determination of clenbuterol. The electrochemical behaviors of clenbuterol on the prepared electrode were tested by cyclic voltammetry (CV) and differential pulse voltammetry (DPV) analysis. The results showed that the intercalated carbon can act as active sites to accelerate electron transfer. In addition, more exposed surface areas of the HNbMoO 6 /C composite will facilitate the electrolyte to permeate. The oxidation peak current of clenbuterol was linearly related to its concentration in the range of 1.04 × 10 −5 to 7.51 × 10 −4 mol L −1 , and the determination limit was calculated to be 3.03 × 10 −6 mol L −1 (S/N = 3). This sensor exhibits excellent stability, reproducibility, specificity, and good recoveries when applied to monitor clenbuterol in real samples.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2022
·Vol. 33
·期 8
·5750-5762
·
IF 2.779
Ling Chen,Yimin Dai,Qi Lu,Chengqian Fang,Zhiheng Wang,Yaqi Li,Ling Cai,Bo Liu,Yue-fei Zhang,Yan Li,Li Wan
A new environmental-friendly magnetic cellulosic adsorbent MnFe 2 O 4 @Cel-g-p(AA-DMC) was easily synthesized via natural cellulose and easy-recovered magnetic particles MnFe 2 O 4 . Magnetic cellulose composites were characterized by SEM, TEM, XPS, XRD, BET, VSM, TGA and FTIR. The effect of pH, contact time and PMS dosage on adsorption was investigated. Besides, the adsorption kinetic model was well-fitted to the pseudo-second-order model, and the adsorption isotherm were matched with the Frenudlich isotherm model. The MnFe 2 O 4 @Cel-g-p(AA-DMC) posseses the excellent stability, reusability and superior superparamagnetic behavior and its possible adsorption mechanism for the adsorption of CR was proposed.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Tang Mengyao,Dong Shuai,Wang Jiawei,Cheng Liwei,Zhu Qiaonan,Li Yanmei,Yang Xiuyi,Guo Lin,Wang Hua
In contrast to conventional batteries, anode-free configurations can extend cell-level energy densities closer to the theoretical limit. However, realizing alkali metal plating/stripping on a bare current collector with high reversibility is challenging, especially at low temperature, as an unstable solid-electrolyte interphase and uncontrolled dendrite growth occur more easily. Here, a low-temperature anode-free potassium (K) metal non-aqueous battery is reported. By introducing Si-O-based additives, namely polydimethylsiloxane, in a weak-solvation low-concentration electrolyte of 0.4 M potassium hexafluorophosphate in 1,2-dimethoxyethane, the in situ formed potassiophilic interface enables uniform K deposition, and offers K||Cu cells with an average K plating/stripping Coulombic efficiency of 99.80% at −40 °C. Consequently, anode-free Cu||prepotassiated 3,4,9,10-perylene-tetracarboxylicacid-dianhydride full batteries achieve stable cycling with a high specific energy of 152 Wh kg −1 based on the total mass of the negative and positive electrodes at 0.2 C (26 mA g −1 ) charge/discharge and −40 °C.
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