Microstructure, mechanical, tribological, and oxidizing properties of AlCrSiN/AlCrVN/AlCrNbN multilayer coatings with different modulated thicknesses
作者:
Mei, Fangsheng;Zhang, Zhijian;Yu, Yang;Lin, Xiaoliang;Gao, Jiangxiong;...
期刊:
Ceramics International ,2022年48(22):32973-32985 ISSN:0272-8842
通讯作者:
Mei, Fangsheng(mfs_sheng@xtu.edu.cn);Zhijian, Zhang(zhangzhijian_cn@126.com)
作者机构:
[Lin, Jianguo; Mei, Fangsheng] Xiangtan Univ, Sch Mat Sci & Engn, Xiangtan 411105, Peoples R China.;[Zhang, Zhijian] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421001, Hunan, Peoples R China.;[Yu, Yang; Gao, Jiangxiong; Lin, Xiaoliang] Zhuzhou Huarui Precis Cutting Tools Co Ltd, Zhuzhou 412000, Peoples R China.;[Yuan, Tiechui] Cent South Univ, Powder Met Res Inst, Changsha 410083, Peoples R China.
通讯机构:
[Fangsheng Mei] S;[Zhang Zhijian] C;School of Materials Science and Engineering, Xiangtan University, Xiangtan, 411105, PR China<&wdkj&>College of Chemistry and Materials Science, Hengyang Normal University, Hengyang, Hunan, 421001, PR China
关键词:
AlCrSiN;AlCrVN;AlCrNbN multilayer coatings;Modulated thickness;Mechanical properties;Elemental diffusion;Wear resistance;Oxidation resistance
摘要:
Multilayer structure design is one of the most promising methods for improving the comprehensive performance of AlCrN-based hard coatings applied to cutting tools. In this study, four types of AlCrSiN/AlCrVN/AlCrNbN multilayer coatings, with different modulated thicknesses, were deposited to investigate their microstructure, mechanical, tribological, and oxidizing properties. All multilayer coatings exhibited grain growth along the crystallographic plane of (200) with a NaCl-type face-centered cubic (FCC) structure. The results show that, as the modulation thickness decreases from ∼35 nm to ∼10 nm, (1) the grain refinement effect is increasingly evident; (2) all multilayer coatings show a hardness of >30 GPa and an elastic modulus of >300 GPa. Both the ability to resist elastic strain to failure and the plastic deformation of multilayer coatings increase. In addition, their resistance to cracking reduces; (3) the wear rates of these multilayer coatings reduce successively from 1.78 × 10−16 m3 N−1 m−1 to 7.7 × 10−17 m3 N−1 m−1. This is attributed to an increase in self-lubricating VOx and a decrease in adhesives from the counterparts; (4) the best high-temperature oxidation resistance was obtained for the multilayer coating with a modulated thickness of ∼15 nm. © 2022 Elsevier Ltd and Techna Group S.r.l.
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英文
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Fluorescent porous organic cage with good water solubility for ratiometric sensing of gold(III) ion in aqueous solution
作者:
Dai, Cong* ;Gu, Biao;Tang, Si-Ping;Deng, Pei-Hong;Liu, Bo
期刊:
Analytica Chimica Acta ,2022年1192:339376 ISSN:0003-2670
通讯作者:
Dai, Cong
作者机构:
[Liu, Bo; Dai, Cong; Gu, Biao; Tang, Si-Ping; Deng, Pei-Hong] Hengyang Normal Univ, Coll Chem & Mat Sci, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421001, Peoples R China.
通讯机构:
[Dai, Cong] H;Hengyang Normal Univ, Coll Chem & Mat Sci, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421001, Peoples R China.
关键词:
Gold(III) ion;Porous organic cage;Ratiometric fluorescent sensing;Water solubility
摘要:
Fluorescent porous organic cage with good water solubility is of great interest but still challenging for its fluorescent sensing application. Poor water solubility and single signal of most previous probes are unfavorable for the monitoring of Au3+ generated from the potential dissociation of gold nanoparticles in environmental and biological samples. Here we report a water-soluble porous organic cage as a ratiometric fluorescent probe for Au3+ in aqueous solution. The prepared porous organic cage with good water solubility showed specific redox interaction with Au3+ in pH 5, leading to the change of dual emission at 420 and 484 nm. Based on the change of fluorescence ratio, a simple ratiometric sensing method for Au3+ from the dissociation of gold nanoparticles in aqueous solution was developed. The proposed method gave a calibration function of F484/F420 = 0.0370[Au3+] + 0.5689 (where F484/F420 is the intensity ratio of fluorescence at 484 nm to that at 420 nm; [Au3+] in μM) (R2 = 0.9975) in the concentration range of 1–60 μM, the limit of detection (3s) of 8 nM, and the relative standard deviation of 0.26% for 10 replicate detections of 50 μM Au3+. The recoveries of spiked Au3+ in domestic wastewater and human serum samples ranged from 94.66% to 105.61%. © 2021
语种:
英文
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One-pot microwave-assisted synthesis of dialkytin 2-[(4-methylbenzoyl) hydrazono]-3-phenylpropanoic acid complexes and their anticarcinoma activities and DNA-binding properties
作者:
Jiang, Wu-Jiu* ;Tan, Yu-Xing;Peng, Yi-Yuan*
期刊:
Applied Organometallic Chemistry ,2022年36(3):e6562- ISSN:0268-2605
通讯作者:
Jiang, Wu-Jiu;Peng, Yi-Yuan
作者机构:
[Jiang, WJ; Peng, Yi-Yuan; Jiang, Wu-Jiu; Tan, Yu-Xing] Jiangxi Normal Univ, Key Lab Funct Small Organ Mol, Key Lab Green Chem, Coll Chem & Chem Engn,Minist Educ, Nanchang 330022, Jiangxi, Peoples R China.;[Jiang, Wu-Jiu; Tan, Yu-Xing] Hengyang Normal Univ, Coll Chem & Mat Sci,Univ Hunan Prov, Hunan Prov Engn Res Ctr Monitoring & Treatment He, Key Lab Funct Organometall Mat,Key Lab Funct Met, Hengyang, Hunan, Peoples R China.
通讯机构:
[Jiang, WJ; Peng, YY] J;Jiangxi Normal Univ, Key Lab Funct Small Organ Mol, Key Lab Green Chem, Coll Chem & Chem Engn,Minist Educ, Nanchang 330022, Jiangxi, Peoples R China.
关键词:
biological activity;crystal structure;microwave-assisted synthesis;one-pot;organotin
摘要:
Under microwave irradiation, five organotin complexes were produced through the reaction of 4-methylbenzhydrazide, sodium phenylpyruvate and corresponding dialkyltin. Fourier transform infrared spectroscopy; 1H, 13C and 119Sn nuclear magnetic resonance spectroscopy; high-resolution mass spectrometry; X-ray crystallography and thermogravimetric analysis (TGA) were performed to characterise the synthesised complexes. The in vitro antitumour activity for the complexes involved was assessed using the MTT assay on the human carcinoma cells of HepG2, NCI-H460 and MCF7. 2-Oxo-3-pheny propionic acid p-methyl benzoylhydrazone dibutyltin, C5, exhibited an intensive anticarcinoma activity. Cell apoptosis revealed that C5 mediated the cell apoptosis of HepG2 cells. DNA binding in C5 was investigated through UV-visible absorption spectrometry and viscosity measurement. Molecular docking was performed for predicting C5-DNA binding, which revealed C5 could be implanted into the DNA double helix. © 2022 John Wiley & Sons, Ltd.
语种:
英文
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Synthesis and characterization of Al (III)-Zn (II) heterometallic complex and the application in ring-opening polymerization of cyclohexene oxide
作者:
Mu, Debao;Feng, Chunping;Li, Wenyi;Yuan, Dan;Yao, Yingming
期刊:
Applied Organometallic Chemistry ,2022年36(9):e6796- ISSN:0268-2605
通讯作者:
Yuan, Dan(yuandan@suda.edu.cn);Yao, Yingming(yaoym@suda.edu.cn);Li, Wenyi(757189515@qq.com)
作者机构:
[Feng, Chunping; Yuan, Dan; Yao, Yingming; Mu, Debao] Soochow Univ, Key Lab Organ Synth Jiangsu Prov, Coll Chem Chem Engn & Mat Sci, Dushu Lake Campus, Suzhou 215123, Peoples R China.;[Li, Wenyi] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang, Peoples R China.
通讯机构:
[Wenyi Li] C;[Dan Yuan; Yingming Yao] K;Key Laboratory of Organic Synthesis of Jiangsu Province, College of Chemistry, Chemical Engineering & Materials Science, Dushu Lake Campus, Soochow University, Suzhou, P. R. China<&wdkj&>College of Chemistry and Materials Science, Hengyang Normal University, Hengyang, P. R. China
关键词:
cyclohexene oxide;heterometallic complex;ring-opening polymerization
摘要:
Four aluminum, zinc, and aluminum/zinc heterometallic complexes 1–4 stabilized by o-phenylenediamine bridged poly (phenolato) ligands were synthesized and characterized. It was found that the reaction sequence has significant influence on the formation of the Al-Zn heterometallic complex AlZnL1Me (4), which was prepared through successive complexation of poly (phenol) with ZnEt2 and AlMe3. The catalytic behaviors of complexes 1–4 for the ring-opening polymerization of cyclohexene oxide (CHO) were investigated, and the heterometallic complex 4 showed significantly enhanced activity (TOF up to 410 min−1). Kinetic study was conducted; the activation energy (Ea) for formation of PCHO using 4 was determined to be 58.0 ± 6.5 kJ mol−1. © 2022 John Wiley & Sons, Ltd.
语种:
英文
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Engineering shell thickness of pyridinic-N rich hollow carbon nanospheres for stable and high energy density potassium ion hybrid capacitors
作者:
Wang, Deping;He, Yongqiang;Liu, Hongbo;Xia, Xiaohong
期刊:
Electrochimica Acta ,2022年428:140931 ISSN:0013-4686
通讯作者:
Xia, Xiaohong(xxh@hnu.edu.cn)
作者机构:
[Wang, Deping] Hengyang Normal Univ, Coll Chem & Mat Sci, Key Lab Funct Organometall Mat, Hengyang 421008, Hunan, Peoples R China.;[He, Yongqiang; Xia, Xiaohong; Liu, Hongbo] Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China.;[Xia, Xiaohong] Hunan Univ, Hunan Joint Int Lab Adv Mat & Technol Clean Energy, Changsha 410082, Hunan, Peoples R China.
通讯机构:
[Xiaohong Xia] C;College of Material Science and Engineering, Hunan University, Changsha, Hunan 410082, PR China<&wdkj&>Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy, Hunan University, Changsha, Hunan 410082, PR China
关键词:
Hollow carbon nanospheres;Shell size;Pyridinic-N;Energy density;Potassium-ion hybrid capacitors
摘要:
Potassium-ion hybrid capacitors (PIHCs) are candidate devices for large-scale electricity storage due to their attractive combination of high energy density of batteries and high power capacity of supercapacitors. But the much larger ionic size and higher mass of K+ in comparison to that of Li+and Na+ make it difficult to identify a high capacity and rate capability anode material. Here we fabricate pyridinic-N rich hollow carbon nanospheres (NHCNs) with tunable shell size by a facile core-shell polymerization and carbonization method. By simply regulating the shell thickness, we can control the carbon nanospheres with appropriate surface area and defects/functional groups level, which are critical in determining their potassium storage capability. Due to the high nitrogen content (8.56 at.%), optimal porosity and shell size (∼20 nm), the NHCNs-420 exhibits a dominant surface-control behavior of a high capacity of 197.5 mAh g−1 at a high rate of 5 A g−1 and long-term stability of 280.3 mAh g−1 over 2500 cycles at 1 A g−1, which compares favorably with most previously reported carbon-based electrodes. Moreover, the kinetics matched NHCNs-420//porous carbon PIHC device combines high energy and power density, demonstrating the promise of using NHCNs for potassium-ion storage. © 2022 Elsevier Ltd
语种:
英文
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Co7Fe3Nanoparticles Confined in N-Doped Carbon Nanocubes for Highly Efficient, Rechargeable Zinc-Air Batteries
作者:
Tu, Teng-Xiu;Zhou, Xiao;Zhang, Peng-Fang;Tan, Liang;Xu, Zhi-Feng;...
期刊:
ACS SUSTAINABLE CHEMISTRY & ENGINEERING ,2022年10(27):8694-8703 ISSN:2168-0485
通讯作者:
Wu, Yi-jin(wuyj313978@163.com);Zheng, Jian-zhong(zhengjianzhong49@163.com)
作者机构:
[Tu, Teng-Xiu; Zhou, Xiao; Tan, Liang; Xu, Zhi-Feng; Liu, Meng-Qin; Li, Wen-Yi; Wu, Yi-Jin] Hunan Engineering Research Center for Monitoring and Treatment of Heavy Metals Pollution in the Upper Reaches of XiangJiang River, Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, College of Chemistry and Material Science, Hengyang Normal University, Hengyang;421001, China;[Zheng, Jian-Zhong] School of Environmental Science and Engineering, Nanjing Tech University, Nanjing;211816, China;[Zhang, Peng-Fang] Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, School of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng
通讯机构:
[Yi-jin Wu] H;[Jian-zhong Zheng] S;Hunan Engineering Research Center for monitoring and treatment of heavy metals pollution in the upper reaches of XiangJiang River, Key Laboratory of Functional Metal−Organic Compounds of Hunan Province, College of Chemistry and Material Science, Hengyang Normal University, Hengyang 421001, People’s Republic of China<&wdkj&>School of Environmental Science and Engineering, Nanjing Tech University, Nanjing 211816, People’s Republic of China
关键词:
Bimetallic active component;M-Nxspecies;Metal nanoparticles;Oxygen-based bifunctional electrocatalyst;Rechargeable zinc-air battery
摘要:
Active component management and microengineering of metal nanoparticles are significant challenges for efficient M/N/C electrocatalysts, as a crucial electrode material for reversible zinc-air batteries, because of the lack of a multifunctional structural strategy in the electrocatalytic preparation process. Here, a convenient, one-step pyrolysis method was introduced into the preparation process of a difunctional electrocatalyst, an Fe-, Co-, and N-codoped carbon-based cube hybrid (Co7Fe3/CFNC) with abundant active components, including metallic Co7Fe3nanoparticles and Fe/Co-Nxspecies. The as-constructed Co7Fe3/CFNC demonstrates impressive activity/stability for ORR/OER. Moreover, practical zinc-air battery building with Co7Fe3/CFNC electrocatalysts reveals a superior cycling stability for 224 h. Our work could educate a new applicable branch for designing multifunctional catalysts and regulating their active sites to apply the energy and environment. © 2022 American Chemical Society. All rights reserved.
语种:
英文
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Li-CO2/O2 battery operating at ultra-low overpotential and low O2 content on Pt/CNT catalyst
作者:
Zhang, Peng-Fang;Sheng, Tian;Zhou, Yao;Wu, Yi-Jin;Xiang, Cheng-Cheng;...
期刊:
Chemical Engineering Journal ,2022年448:137541 ISSN:1385-8947
通讯作者:
Li, Jun-Tao(jtli@xmu.edu.cn)
作者机构:
[Zhou, Yao; Li, Jun-Tao; Sun, Shi-Gang; Zhang, Peng-Fang] Xiamen Univ, Coll Energy, Xiamen 361005, Peoples R China.;[Lin, Jin-Xia; Li, Yu-Yang; Huang, Ling; Xiang, Cheng-Cheng; Sun, Shi-Gang] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China.;[Zhang, Peng-Fang] Liaocheng Univ, Sch Chem & Chem Engn, Shandong Prov Key Lab Chem Energy Storage & Novel, Liaocheng 252000, Peoples R China.;[Sheng, Tian] Anhui Normal Univ, Coll Chem & Mat Sci, Wuhu 241000, Peoples R China.;[Wu, Yi-Jin] Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organometall Mat, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.
通讯机构:
[Jun-Tao Li; Shi-Gang Sun] C;College of Energy, Xiamen University, Xiamen 361005, PR China<&wdkj&>State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, PR China<&wdkj&>College of Energy, Xiamen University, Xiamen 361005, PR China
关键词:
Contacting interface;Li-CO2/O2 battery;Localized growth mechanism;O2 content;Pt/CNT catalyst
摘要:
Li-CO2/O2 battery presents a promising solution to combine CO2 utilization and electrochemical energy storage. Herein, Pt nanoparticles (NPs) of 2.5 nm in mean size loaded uniformly on carbon nanotubes (Pt/CNT) were synthesized and served as cathodic catalysts. The Li-CO2/O2 battery with Pt/CNT catalyst were investigated in mixture gas of CO2 and O2 with O2 content varying from 0% to 20%. It has revealed that the Li-CO2/O2 (2% O2) battery, i.e., operating with 2% O2 content, displays a minimum overpotential of 0.31 V and a cycling stability of 127 cycles, which are significantly superior to the Li-CO2/O2 (20% O2) battery (0.51 V, 90 cycles) and the Li-CO2 battery (0% O2 content) (0.44 V, 110 cycles). Results of in-situ Fourier transform infrared (FTIR) spectroscopy have demonstrated the complete decomposition of Li2CO3 at 3.2 V in the Li-CO2/O2 (2% O2) battery. However, density function theory (DFT) calculations indicate that the decomposition energy barrier of Li2CO3 in Li-CO2/O2 (2% O2) battery is higher than that in Li-CO2 battery. SEM characterizations revealed a localized growth mechanism when O2 content is between 2% and 6% during the initial cycling, in which the Li2CO3 tends to form inside the Pt/CNT catalyst layer, rather than it distributes uniformly on both sides of the Pt/CNT catalyst layer with 0% or 20% O2 content. Such a growth mechanism ensures a better contacting interface between the Pt/CNT catalyst and Li2CO3, which plays a key role in optimal battery performance. © 2022 Elsevier B.V.
语种:
英文
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Hot corrosion behavior of Y3Al5O12/LaPO4 materials exposed to molten V2O5
作者:
Chen, Ting;Sun, Junbin;Song, Chenxi;Huang, Ling;Qi, Xiang;...
期刊:
Ceramics International ,2022年48(10):14856-14864 ISSN:0272-8842
通讯作者:
Sun, Junbin(jbsun2018@hynu.edu.cn);Lu, Weihong(123377836@qq.com);Chen, Xiaolong(Xiaolong.CHEN@jnu.edu.cn)
作者机构:
[Sun, Junbin; Lu, Weihong; Qi, Xiang; Xu, Zhifeng; Huang, Ling; Chen, Ting; Song, Chenxi; Wang, Juan] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.;[Sun, Junbin; Lu, Weihong; Xu, Zhifeng] Hengyang Normal Univ, Key Lab Organometall New Mat Hunan Prov, Hengyang 421008, Peoples R China.;[Sun, Junbin; Lu, Weihong; Xu, Zhifeng] Hengyang Normal Univ, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;[Sun, Junbin; Lu, Weihong; Xu, Zhifeng] Hengyang Normal Univ, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hengyang 421008, Peoples R China.;[Chen, Xiaolong] Jinan Univ, Inst Adv Wear & Corros Resistant & Funct Mat, Guangzhou 510632, Peoples R China.
通讯机构:
[Junbin Sun; Weihong Lu] C;College of Chemistry and Material Science, Hengyang Normal University, Hengyang, 421008, PR China<&wdkj&>Key Laboratory of Organometallic New Materials of Hunan Province, Hengyang Normal University, Hengyang, 421008, PR China<&wdkj&>Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, Hengyang Normal University, Hengyang, 421008, PR China<&wdkj&>Hunan Engineering Research Center for Monitoring and Treatment of Heavy Metals Pollution in the Upper Reaches of Xiangjiang River, Hengyang Normal University, Hengyang, 421008, PR China
关键词:
LaPO4;Molten salt corrosion;Y3Al5O12
摘要:
The current study reports the fabrication of (1-x) Y3Al5O12/x LaPO4 (x = 0, 0.1, 0.2, 0.3, 0.4) composites and their evaluation against molten V2O5 corrosion at 900 °C and 1000 °C for 20 h. The phase compositions and microstructures of the samples were analysed using X-ray diffraction (XRD) spectroscopy, as well as scanning electron microscopy (SEM), both before and after the corrosion tests. The yttrium aluminium garnet (Y3Al5O12, YAG) was easily corroded by molten V2O5, with the primary product being YVO4. While LaPO4 exhibited perfect resistance to the molten V2O5 corrosion, it was ineffective at improving the corrosion resistance of the YAG/LaPO4 composite materials. However, the LaPO4/YAG double layers materials prepared with LaPO4 coated on the surface of YAG exhibit excellent resistance to molten V2O5, owing to the formation of the P diffusion layer at the interface between the LaPO4 and YAG, which acts as a sealing layer, preventing the molten V2O5 from penetrating. © 2022 Elsevier Ltd and Techna Group S.r.l.
语种:
英文
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The phonon transport properties in a new ferroelectric carbon–boron framework with host–guest clathrate structure
作者:
Zhang, Zhijian;Shi, Wei
期刊:
EUROPEAN PHYSICAL JOURNAL B ,2022年95(7):107-null ISSN:1434-6028
通讯作者:
Zhang, Zhijian(zhangzhijian_cn@126.com)
作者机构:
[Zhang, Zhijian] Hengyang Normal Univ, Key Lab Funct Met Organ Cpds, Hengyang 421001, Peoples R China.;[Zhang, Zhijian] Hengyang Normal Univ, Key Lab Funct Organometall Mat Hunan Prov, Hengyang 421001, Peoples R China.;[Shi, Wei] Hunan Prov Sci & Technol Affairs Ctr, Changsha 410013, Peoples R China.;[Shi, Wei] Sci & Technol Dept Hunan Prov, Changsha 410013, Peoples R China.
通讯机构:
[Zhijian Zhang] K;Key Laboratory of Functional Metal-Organic Compounds and Key Laboratory of Functional Organometallic Materials of Hunan Province, Hengyang Normal University, Hengyang, China
关键词:
The European Physical Journal B;Condensed Matter;Complex Systems;journal;EPJ
摘要:
In this paper, the phonon properties and thermal conductivity of a new clathrate SrB3C3 are investigated by utilizing first principles calculations combined with phonon Boltzman transport equation. Through analyzing the intrinsic symmetry, four Raman active phonon modes (2T2g and 2Eg) are revealed in the phonon spectrum, and their corresponding vibrational features are presented as well. The lattice thermal conductivity of SrB3C3 at room temperature is calculated to be merely 8.69W/mK, which is evidently smaller than that of traditional Si-based clathrates. Meanwhile, owing to the comparable group velocity with acoustic phonon modes, the optical phonons of SrB3C3 abnormally contribute 40% to the total thermal conductivity. Such low thermal conductivity in SrB3C3 is mainly attributed to the strong phonon anharmonic including both scattering strength and channel. The findings clarify the intrinsic phonon property of SrB3C3, and could help us to pave the way for its future applications in ferroelectric devices. Graphical abstract: [Figure not available: see fulltext.] © 2022, The Author(s), under exclusive licence to EDP Sciences, SIF and Springer-Verlag GmbH Germany, part of Springer Nature.
语种:
英文
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Investigation of Pb (II) and Cd (II) removal from aqueous solution by organic-modified xonotlite
作者:
Zhou, Wei* ;Xin, Junliang;Tang, Wenqing
期刊:
International Journal of Environmental Analytical Chemistry ,2022年102(19):7736-7753 ISSN:0306-7319
通讯作者:
Zhou, Wei
作者机构:
[Xin, Junliang; Zhou, Wei] Hunan Inst Technol, Sch Safety & Environm Engn, Hengyang, Hunan, Peoples R China.;[Tang, Wenqing] Hengyang Normal Univ, Dept Chem & Mat Sci, Hengyang, Hunan, Peoples R China.
通讯机构:
[Zhou, Wei] H;Hunan Inst Technol, Sch Safety & Environm Engn, Hengyang, Hunan, Peoples R China.
关键词:
Xonotlite;organic-modified xonotlite;adsorption;Pb(II) and Cd(II);wastewater
摘要:
In this work, a novel xonotlite nanocomposite was synthesised with abandoned eggshell by hydrothermal method, and organic-modied with toluene diisocyanate (TDI) for the removal of Pb(II) and Cd(II) from wastewater. The xonotlite and organic-modified xonotlite were characterised by X-ray diffraction (XRD), scanning electron microscopy (SEM), Brunner-Emmet-Teller (BET) and Fourier transform infrared spectroscopy (FTIR) methods. The effect of solution pH, contact time, adsorbent dose, and initial concentrations were also investigated. The organic-modified xonotlite was found to have a high loading capacity of 467.7 mg g−1 for Pb(II) and 147.6 mg g−1 for Cd(II). The adsorption of Pb (II) and Cd (II) was well fitted by Freundlich model and pseudo-second order model. In the effect of the competing ion, the ions like Na(I) and K(I), had little effect on the Pb(II) and Cd(II) removal efficiency. Furthermore, the organic-modified xonotlite can be reused and shown good recyclability. It was concluded that the organic-modified xonotlite is simple, fast and effective adsorbent for the removal of Pb(II) and Cd(II) in treating wastewater with outstanding adsorption capacity. © 2020 Informa UK Limited, trading as Taylor & Francis Group.
语种:
英文
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一种用于过氧亚硝酰阴离子检测的ESIPT荧光探针及其应用
作者:
龚文平;张春香;阳茜;谷标;申有名
期刊:
分析试验室 ,2022年41(8):874-879 ISSN:1000-0720
通讯作者:
Zhang, Chunxiang(cxzhang81@163.com);Shen, Youming(ymshen79@163.com)
作者机构:
[龚文平; 张春香; 申有名] College of Chemistry and Materials Engineering, Hunan University of Arts and Science, Changde;415000, China;[Yang, Xi; 谷标] Key Laboratory of Functional Metal-Organic Compounds of Human Province, College of Chemistry and Materials Science, Heng-yang Normal University, Hengyang;421008, China;[龚文平; 张春香; 申有名] 415000, China
关键词:
过氧亚硝酰阴离子(ONOO-);荧光探针;分子内质子转移;荧光成像
摘要:
过氧亚硝酰阴离子(ONOO-)是一种体内活性氧化物,在许多生理和病理过程中发挥重要作用。本文通过一步反应,制备了一种简单的分子内质子转移(ESIPT)荧光探针HBT-B。该探针由于分子内的ESIPT过程,自身具有明亮的蓝绿色荧光。当加入ONOO-时,探针HBT-B上的硼酸酯被转化成醌,ESIPT受阻,荧光被淬灭。在最佳条件下,探针HBT-B的荧光强度与ONOO-浓度在0~10 μmol/L内呈良好的线性关系,其定量限为15 nmol/L。利用高分辨质谱和理论计算,研究了探针HBT-B与ONOO-的作用机理。将探针HBT-B用于活细胞内ONOO-检测,得到了满意的结果,表明探针HBT-B在揭示ONOO-生理作用上具有应用前景。
语种:
中文
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3-羟基邻苯二甲酰亚胺全水溶性次氯酸荧光探针及其应用
作者:
张春香;刘旭;靳俊玲;申有名;谷标
期刊:
分析试验室 ,2022年41(2):130-134 ISSN:1000-0720
通讯作者:
Gu, Biao(biaogu@hynu.edu.cn)
作者机构:
[张春香; 刘旭; 靳俊玲] Hunan Province Cooperative Innovation Center for the Construction & Development of Dongting Lake Ecological Economic Zone, College of Chemistry and Materials Engineering, Hunan University of Arts and Science, Changde;415000, China;[申有名; 谷标] Laboratory of Functional Metal-Organic Compounds of Hunan Province, College of Chemistry and Materials Science, Hengyang Normal University, Hengyang;421008, China;[张春香; 刘旭; 靳俊玲] 415000, China
关键词:
荧光探针;次氯酸;激发态分子内质子转移;细胞成像
摘要:
利用二甲基硫代氨基甲酸酯对次氯酸(HOCl)的特异性和吡啶盐的水溶性,以4-羟基异苯并呋喃-1,3-二酮作为原料,设计合成了一种检测HOCl的全水溶性激发态分子内质子转移(ESIPT)荧光探针。由于二甲氨基硫代甲酸酯对羟基的保护,探针分子内的ESIPT作用被阻碍,自身无荧光;当加入HOCl时,HOCl氧化二甲氨基硫代甲酸酯,释放出羟基,分子内出现了ESIPT过程,荧光增强。探针在水溶液中对HOCl的检测线性范围为0~80μmol/L,定量限为94 nmol/L。该探针对HOCl的响应时间为4 min, Stokes位移为113 nm,检测限为94 nmol/L。方法可用于水样和活细胞中HOCl的检测。
语种:
中文
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Iron reduction process and antimony behavior change in paddy soils under stationary flooding conditions
作者:
Long, Jiumei;Zhou, Dongsheng;Huang, Yayuan;Yi, Zhengji;Bin, Dongmei;...
期刊:
Applied Geochemistry ,2022年142:105311 ISSN:0883-2927
通讯作者:
Lei, Ming(leiming@hunau.edu.cn)
作者机构:
[Bin, Dongmei; Deng, Jingheng; Long, Jiumei; Zhou, Dongsheng; Wang, Jing; Luo, Yuanlai] Hengyang Normal Univ, Coll Life Sci & Environm, Hunan Key Lab Conservat & Utilizat Biol Resources, Hengyang 421008, Peoples R China.;[Huang, Yayuan; Lei, Ming] Hunan Agr Univ, Coll Resource & Environm, Hunan Engn Res Ctr Safe & High Efficient Utilizat, Changsha 410128, Peoples R China.;[Yi, Zhengji] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
通讯机构:
[Ming Lei] H;Hunan Engineering Research Center for Safe & High-Efficient Utilization of Heavy Metal Pollution Farmland, College of Resource & Environment, Hunan Agricultural University, Changsha, 410128, PR China
关键词:
Antimony species;Citric acid extraction;Iron fraction;Iron reduction;Sequential extraction
摘要:
Although iron reduction coupled with antimony (Sb) behavior change has attracted increasing interest in recent years, this process has not yet been well addressed in paddy soils under natural flooding conditions. This study investigates the iron reduction process in paddy soils using a stationary flooding incubation experiment. The paddy soils used in the study contained 199, 329 and 450 mg/kg of Sb (referred to as LS, MS and HS, respectively). Results showed that iron reduction lasted for 12–14 d under simulated flooding conditions at 25 °C, with the highest total Fe(II) being 778, 791 and 782 mg/kg in LS, MS and HS, respectively. Through the iron reduction process, easily reducible iron (Fe2) and reducible iron (Fe3) decreased by 26.1–38.4% and 4.03–12.8%, respectively, indicating that small fractions of iron oxides underwent reductive dissolution. The abundant phyla of iron-reducing bacteria in these soils were Proteobacteria, Firmicutes and Actinobacteriota. Moreover, up to 14 genera were identified as abundant iron-reducing bacteria in these paddy soils. Among, the most abundant genera were Azospirillum and Magnetospirillum, which are also known to mediate the iron nutrition supply for plants and magnetite formation, respectively. Along with iron reduction, iron oxide-incorporated Sb decreased by 7.87–17.3%, while soil surface-bound Sb increased by 42.4–60.4%. This demonstrates that substantial Sb released from iron reductive dissolution was adsorbed on the soil surface. In addition, the total aqueous Sb increased by 24.9–33.0 μg/L through iron reduction in these flooding soils, indicating that iron reduction promoted Sb mobilization in paddy soils under flooding conditions. Sb was synchronously reduced to Sb(III), with Sb(III) accounting for 51.1–59.4% of the total citric acid extracted Sb at the end of iron reduction. However, the aqueous Sb(III) was lower by orders of magnitude than the corresponding Sb(V) in these soils. This might imply that the strong adsorption affinity of Sb(III) to the soil solid facilitated the increase in soil surface-bound Sb in all flooded paddy soils. © 2022 Elsevier Ltd
语种:
英文
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Hot corrosion behaviour of Gd2O3 doped LaMgAl11O19 thermal barrier coating exposed to molten V2O5 at 900°C
作者:
Cao, Shengjun;Sun, Junbin;Chen, Ting;Wang, Juan;Chen, Mansheng;...
期刊:
Ceramics International ,2021年47(13):18792-18799 ISSN:0272-8842
通讯作者:
Sun, Junbin(jbsun2018@hynu.edu.cn);Lu, Weihong(123377836@qq.com)
作者机构:
[Sun, Junbin; Lu, Weihong; Chen, Mansheng; Chen, Ting; Li, Wenyi; Cao, Shengjun; Wang, Juan] Hengyang Normal Univ, Hunan Engn Res Ctr Monitoring & Treatment Heavy M, Hunan Prov Univ Key Lab Funct Organomet Mat, Key Lab Funct Met Organ Cpds Hunan Prov,Coll Chem, Hengyang 421008, Peoples R China.;[Wang, Jinshuang] Xinyang Normal Univ, Henan Prov Key Lab Utilisat Nonmetall Mineral Sou, Xinyang 464000, Peoples R China.;[Hui, Yu] Shenyang Acad Environm Sci, Atmospher Environm Res Ctr, Shenyang 110016, Peoples R China.
通讯机构:
[Junbin Sun; Weihong Lu] C;College of Chemistry and Material Science, Hengyang Normal University, Hunan Province Universities Key Laboratory of Functional Organometallic Materials, Key Laboratory of Functional Metal-Organic Compounds of Hunan Province, Hunan Engineering Research Center for Monitoring and Treatment of Heavy Metals Pollution in the Upper Reaches of Xiangjiang River, Hengyang, 421008, PR China
关键词:
LaMgAl11O19;Hot corrosion;Molten V2O5
摘要:
This study investigates the hot corrosion behaviours of La1-xGdxMgAl11O19 (x = 0, 0.2, 0.4, 0.6, 0.8) bulk ceramics and ceramic coatings. The hot corrosion resistance of the ceramic coating was inferior to that of the bulk ceramic, owing to the formation of an amorphous phase during the plasma spraying process. The smaller size of Gd3+ in comparison with La3+ facilitated the ready combination of Gd3+ with VO43−. LaVO4 was obtained as the corrosion product in the LaMgAl11O19 (LMA) sample. Upon doping the LMA with Gd2O3, the LaVO4 was almost entirely replaced by GdVO4. Therefore, the sacrificial action of GdMgAl11O19 protected the LMA from hot corrosion, while also providing a new method for modifying the corrosion resistance of molten slag. © 2021 Elsevier Ltd and Techna Group S.r.l.
语种:
英文
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Phase and microstructure evolution of Sc2O3–CeO2 –ZrO2ceramics in Na2SO4 + V2O5 molten salts
作者:
Wang, Jinshuang;Chen, Luyao;Chen, Mengdi;Wu, Yuyang;Wang, Yinghui;...
期刊:
Ceramics International ,2021年47(16):22965-22975 ISSN:0272-8842
通讯作者:
Wang, Jinshuang(wangjinshuang88@126.com);Jing, Qiangshan(9jqshan@163.com)
作者机构:
[Wu, Yuyang; Liu, Bing; Chen, Mengdi; Jing, Qiangshan; Yu, Yongsheng; Chen, Luyao; Wang, Yinghui; Wang, Jinshuang] Xinyang Normal Univ, Henan Prov Key Lab Utilizat Nonmetall Mineral Sou, Xinyang 464000, Peoples R China.;[Sun, Junbin] Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organometall Mat, Key Lab Funct Met Organ Cpds Hunan Prov, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
通讯机构:
[Jinshuang Wang; Qiangshan Jing] H;Henan Province Key Laboratory of Utilization of Non-metallic Mineral in the South of Henan, Xinyang Normal University, Xinyang, 464000, China
关键词:
ZrO2;Hot corrosion;Mineralization effect;Phase transformation
摘要:
In this study, the destabilization resistance of Sc2O3 and CeO2 co-stabilized ZrO2 (SCZ) ceramics was tested in Na2SO4 + V2O5 molten salts at 750°C–1100 °C. The phase structure and microstructure evolution of the samples during the hot corrosion testing were analyzed with X-ray diffraction (XRD), Raman spectra, scanning electron microscopy (SEM), energy dispersive X-ray spectrum (EDS), and X-ray photoelectron spectroscopy (XPS). Results showed that the destabilization of SCZ ceramics at 750 °C was the result of the chemical reaction with V2O5 to produce m-ZrO2 and CeVO4, and little ScVO4 was detected in the Sc2O3-rich SCZ ceramics. The primary corrosion products at 900 °C and 1100 °C were CeO2 and m-ZrO2 due to the mineralization effect. The Sc2O3-rich SCZ ceramics exhibited excellent degradation resistance and phase stability owing to the enhanced bond strength and the decreased size misfit between Zr4+ and Sc3+. The destabilization mechanism of SCZ ceramic under hot corrosion was also discussed. © 2021 Elsevier Ltd and Techna Group S.r.l.
语种:
英文
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Rationally constructing CoO and CoSe2 hybrid with CNTs-graphene for impressively enhanced oxygen evolution and DFT calculations
作者:
Xu, Deyao;Long, Xuanda;Xiao, Juanxiu;Zhang, Zhiliang;Liu, Guiyu;...
期刊:
Chemical Engineering Journal ,2021年422:129982 ISSN:1385-8947
通讯作者:
Qian, Dong;Liu, Jinlong;Li, Junhua
作者机构:
[Liu, Jinlong; Qian, Dong; Liu, JL; Long, Xuanda; Zhang, Zhiliang; Xu, Deyao] Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Resources, Changsha 410083, Peoples R China.;[Li, Junhua; Xu, Deyao] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.;[Xiao, Juanxiu] Hainan Univ, State Lab Marine Resource Utilizat South China Se, Haikou 570228, Hainan, Peoples R China.;[Liu, Guiyu] South Univ Sci & Technol China, Dept Mat Sci & Engn, Shenzhen 518005, Peoples R China.;[Tong, Haixia] Changsha Univ Sci & Technol, Inst Chem & Biol Engn, Changsha 410114, Peoples R China.
通讯机构:
[Qian, D; Liu, JL] C;[Li, Junhua] H;Cent South Univ, Coll Chem & Chem Engn, Hunan Prov Key Lab Chem Power Resources, Changsha 410083, Peoples R China.;Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.
关键词:
Carbon nanotubes;Cobalt oxide;Cobalt selenide;Graphene;Oxygen evolution
摘要:
Constructing CoO–CoSe2 heterostructures through partial selenization of CoO is proposed to ameliorate the electrocatalytic performance of Co-based compounds toward oxygen evolution reaction (OER). Moreover, with reduced graphene oxide as a platform to in-situ grow N-doped bamboo-like carbon nanotubes encapsulating part of CoO and CoSe2 nanoparticles, we fabricated a novel hybrid (denoted as CoO–CoSe2@N-CNTs/rGO) via a combination of two-stage calcination and subsequent selenization treatment. As an OER electrocatalyst in 1.0 M KOH, CoO–CoSe2@N-CNTs/rGO affords low overpotentials (250 mV@10 mA cm−2 and 322 mV@100 mA cm−2), favorable kinetics (a Tafel slope of 68 mV dec−1), and excellent durability, outperforming commercial RuO2 and most Co-based electrocatalysts reported till date. Comprehensive experiment results uncover that the exceptional electrocatalytic performance mainly emanates from the synergistic effect between CoSe2 and CoO in heterostructure, N doping effect in CNT and rGO, and the confining effect of N-CNTs and rGO for CoO–CoSe2, resulting in more active sites and enhance conductivity. More importantly, density functional theory calculations disclose that the concurrent N doping and desirable encapsulation of the CoO–CoSe2 nanoparticle in N-CNT can optimize the adsorption energies of OER intermediates and increase the electric conductivity, thereby expediting the OER. This work is helpful to foster understanding on the structure–performance correlations of electrocatalysts with multi-active sites and multi-components for diverse applications. © 2021 Elsevier B.V.
语种:
英文
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Sandwich-Structured Sn4P3@MXene Hybrid Anodes with High Initial Coulombic Efficiency for High-Rate Lithium-Ion Batteries
作者:
Fan, Wufeng;Xue, Junpeng;Wang, Deping;Chen, Yuxi;Liu, Hongbo;...
期刊:
ACS Applied Materials & Interfaces ,2021年13(51):61055-61066 ISSN:1944-8244
通讯作者:
Xia, Xiaohong
作者机构:
[Chen, Yuxi; Xia, Xiaohong; Fan, Wufeng; Xue, Junpeng; Liu, Hongbo] Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China.;[Wang, Deping] Hengyang Normal Univ, Coll Chem & Mat Sci, Key Lab Funct Organometall Mat, Hengyang 421008, Hunan, Peoples R China.;[Xia, Xiaohong] Hunan Univ, Hunan Joint Int Lab Adv Mat & Technol Clean Energ, Changsha 410082, Hunan, Peoples R China.
通讯机构:
[Xia, Xiaohong] H;Hunan Univ, Coll Mat Sci & Engn, Changsha 410082, Hunan, Peoples R China.;Hunan Univ, Hunan Joint Int Lab Adv Mat & Technol Clean Energ, Changsha 410082, Hunan, Peoples R China.
关键词:
MXenes;enhanced initial Coulombic efficiency;lithium-ion batteries;outstanding rate capability;tin phosphide
摘要:
The high theoretical capacity makes metal phosphides appropriate anode candidates for Li-ion batteries, but their applications are restricted due to the limited structural instability caused by the huge volume change, as in other high-capacity materials. Here, we design an integrated electrode consisting of Sn4P3 nanoparticles sandwiched between transition-metal carbide (MXene) nanosheets. Tetramethylammonium hydroxide (TMAOH) plays an essential role in the formation of such sandwich structures by producing negatively charged MXene sheets with expanded layer spacings. The strong C-O-P oxygen bridge bond enables tight anchoring of Sn4P3 nanoparticles on the surface of MXene layers. The obtained Sn4P3-based nanocomposites exhibit high reversible capacity with an initial Coulombic efficiency of 82% and outstanding rate performance (1519 mAh cm-3 at a current density of 5 A g-1). The conductive and flexible MXene layers on both sides of Sn4P3 nanoparticles provide the desired electric conductivity and elastomeric space to accommodate the large volume change of Sn4P3 during lithiation. Therefore, the Sn4P3@MXene hybrid exhibits an enhanced cyclic performance of 820 mAh g-1 after 300 cycles at a current density of 1 A g-1. © 2021 American Chemical Society.
语种:
英文
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Influence of amorphous phase in LaMgAl11O19 on properties of LaMgAl11O19/YSZ thermal barrier coatings
作者:
Wang, Yajun;Ma, Xinxin* ;Ma, Rui;Tang, Guangze;Sun, Junbin;...
期刊:
Ceramics International ,2021年47(7):9188-9193 ISSN:0272-8842
通讯作者:
Ma, Xinxin
作者机构:
[Wang, Yajun; Tang, Guangze] Harbin Inst Technol, Sch Mat Sci & Engn, Harbin 150001, Peoples R China.;[Wang, Yajun; Ma, Rui] Beijing Power Machinery Inst, Beijing 100074, Peoples R China.;[Ma, Xinxin] Harbin Inst Technol, State Key Lab Adv Welding & Joining, Harbin 150001, Peoples R China.;[Sun, Junbin] Hengyang Normal Univ, Coll Chem & Mat Sci, Hengyang 421008, Peoples R China.;[Cao, Xueqiang] Wuhan Univ Technol, State Key Lab Silicate Mat Architecture, Wuhan 430070, Peoples R China.
通讯机构:
[Ma, Xinxin] H;Harbin Inst Technol, State Key Lab Adv Welding & Joining, Harbin 150001, Peoples R China.
关键词:
Amorphous;Rare earths hexaaluminates;Thermal barrier coatings
摘要:
Double ceramic layer thermal barrier coatings (DCL-TBCs) of LaMgAl11O19/YSZ (LMA/YSZ) were prepared by atmospheric plasma spraying (APS). Composition, microstructure and phase stability of coatings were analyzed by X-ray diffraction (XRD), scanning electron microscope (SEM) and differential scanning calorimetry (DSC). The amorphous phase content of LMA coating increased with increasing the plasma gun current from 350 A to 650 A. The DCL-TBCs of LMA/YSZ whose LMA coating was prepared with a plasma gun current of 600 A (600LMA/YSZ) had the lower amorphous phase content, an excellent thermal insulation performance and the longest thermal cycling lifetime, indicating that properties of LMA coating could be largely improved by adjusting the APS conditions.
语种:
英文
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Preparation and properties of LaMgAl11O19 thermal barrier coatings doped with Gd2O3
作者:
Sun, Junbin* ;Wang, Jinshuang;Hui, Yu;Chen, Xiaolong*
期刊:
Ceramics International ,2020年46(4):4174-4179 ISSN:0272-8842
通讯作者:
Sun, Junbin;Chen, Xiaolong
作者机构:
[Sun, Junbin] Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organometall Mat, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;[Chen, Xiaolong] Jinan Univ, Inst Adv Wear & Corros Resistant & Funct Mat, Guangzhou 510632, Peoples R China.;[Wang, Jinshuang] Xinyang Normal Univ, Henan Prov Key Lab Utilisat Nonmetall Mineral Sou, Xinyang 464000, Peoples R China.;[Hui, Yu] Shenyang Acad Environm Sci, Atmospher Environm Res Ctr, Shenyang 110016, Peoples R China.
通讯机构:
[Sun, Junbin] H;[Chen, Xiaolong] J;Hengyang Normal Univ, Hunan Prov Univ Key Lab Funct Organometall Mat, Coll Chem & Mat Sci, Key Lab Funct Met Organ Cpds Hunan Prov, Hengyang 421008, Peoples R China.;Jinan Univ, Inst Adv Wear & Corros Resistant & Funct Mat, Guangzhou 510632, Peoples R China.
关键词:
Amorphous;Doping;Gd2O3;LaMgAl11O19;Thermal barrier coatings
摘要:
As a rare earth hexaaluminate, LaMgAl11O19 (LMA) has been one of the most promising materials used as thermal barrier coatings (TBCs). A large amount of amorphous phase, however, often exists in the plasma-sprayed LMA coating and significantly reduces the service lifetime of TBCs. In this study, La1-xGdxMgAl11O19 (x = 0, 0.2, 0.4, 0.6, and 0.8) ceramic powders are synthesised by solid-state reaction, and all of these powders are employed to prepare the corresponding coatings. The phase compositions and microstructures of samples are examined by X-ray diffraction and scanning electron microscopy, respectively. The linear thermal expansion behaviour and thermal cycling behaviour of the coatings are also analysed. The results show that the amorphous phase content is decreased and the thermal expansion behaviour is improved by doping the coatings with Gd2O3. The thermal cycling lifetime of the coating, however, basically remains unchanged. © 2019 Elsevier Ltd and Techna Group S.r.l.
语种:
英文
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Oxidized divinyl oligoacene-bridged diruthenium complexes: Bridged localized radical characters and reduced aromaticity in bridge cores
作者:
Ou, Ya-Ping;Zhang, Jing;Hu, Yuxuan;Yin, Jun;Chi, Chunyan;...
期刊:
DALTON TRANSACTIONS ,2020年49(46):16877-16886 ISSN:1477-9226
通讯作者:
Liu, Sheng Hua
作者机构:
[Ou, Ya-Ping] Hengyang Normal Univ, Key Lab Funct Met Organ Cpds Hunan Prov, Key Lab Funct Organometall Mat, Hunan Prov Coll,Coll Chem & Mat Sci, Hengyang 421008, Hunan, Peoples R China.;[Ou, Ya-Ping; Zhang, Jing; Liu, Sheng Hua; Hu, Yuxuan; Yin, Jun] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.;[Ou, Ya-Ping; Chi, Chunyan] Natl Univ Singapore, Dept Chem, 3 Sci Dr 3, Singapore 117543, Singapore.
通讯机构:
[Liu, Sheng Hua] C;Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ, Wuhan 430079, Peoples R China.
摘要:
A series of bimetallic ruthenium vinyl complexes 1-5 bridged by oligoacenes were synthesized and characterized in this study. Comparative cyclic voltammetry results from 1-5 indicated that the first oxidation potential decreased gradually with the extension of conjugate ligands. Upon oxidation to singly oxidized species 1+-5+, rather small ν(CO) changes in the infrared (IR) spectra and the characteristic bands of metal-to-ligand charge transfer absorptions in the near IR (NIR) region predicted via time-dependent DFT calculations suggested that strong bridged ligands participate in redox processes. NIR absorptions were not observed in complexes 4+ and 5+ possibly because of instability in their twisted and noncoplanar geometry. Electron paramagnetic resonance results and spin density distribution demonstrated that the bridged localized degrees of 1+-5+ successively increased with the extension of oligoacene from benzene to tetracene. Further comparative analysis of neutral molecules and monocations to the aromaticity and π-electron density of bridge cores indicated a step-by-step transformation process from an aromatic to quinoidal radical upon oxidation © The Royal Society of Chemistry.
语种:
英文
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