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A bifunctional POM-based Cu-viologen complex with mixed octamolybdate clusters for rapid oxidation desulfurization and effective photogeneration of hydrogen

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Rare Metals 2024年第1期43卷 236-246页

作者： Lin Yang Zhong Zhang Chao-Nan Zhang Xiu-Li Wang College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell Bohai UniversityJinzhou 121013China

The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy ***,a novel bifunctional [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)-based Cu-viologen complex H_(4)[Cu_(2)~ⅠCl_(2)(Hbcbpy)_(4)] [α-Mo_(8)O_(26)] [β-Mo8O_(26)]·H_(2)O(BHU-2,Hbcbpy=1-(4-carboxybenzyl)-4,4'-bipyridinium) was synthesized and characterized by single-crystal X-ray diffraction(XRD),infrared radiation spectra,powder X-ray diffraction(PXRD) and X-ray photoelectron spectroscopy(XPS) *** structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu_(2)ⅠCl_(2)(Hbcbpy)_(4)]^(4+).BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen *** room temperature,BHU-2 can catalyze 96% conversion of methyl phenyl sulfide with 98% selectivity,and the process obeys the pseudo-first-order reaction kinetic with the half-life of9.6 *** notorious 2-chloroethyl ethyl sulfide can achieve 99% conversion with 98% selectivity within only1 min at the presence of BHU-2,and the turnover frequency(TOF) is up to 7400 h^(-1).BHU-2 also exhibits high catalytic activity for the oxidation of other aromatic and aliphatic thioethers within short time at room ***,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H_(2) evolution rate of 1677.85 μmol·g^(-1)·h^(-1) within 10 ***,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.

关键词： Polyoxometalate Metal-organic complex viologen Oxidation desulfurization Photocatalytic hydrogen production

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Steric hindrance shielding viologen against alkali attack in realizing ultrastable aqueous flow batteries

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Journal of Energy Chemistry 2024年第10期97卷 529-534页

作者： Liwen Wang Kai Wan Xianzhi Yuan Zhipeng Xiang Zhiyong Fu Zhenxing Liang Guangdong Provincial Key Laboratory of Fuel Cell Technology School of Chemistry and Chemical Engineering South China University of Technology State Key Laboratory of Pulp and Paper Engineering South China University of Technology Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center

viologens known as a kind of promising negolyte materials for aqueous organic redox flow batteries,face a critical stability challenge due to the SN2 nucleophilic attack by hydroxide ions（OH-） during the battery *** this work,a N-cyclic quaternary ammonium-grafted viologen molecule,viz.1,1'-bis（4,4'-dime thylpiperidiniumyl）-4,4'-bipyridinium tetrachloride(（DBPPy）Cl4),is developed by the molecular engineering *** obtained（DBPPy）Cl4molecule shows a decent solubility of 1.84 M and a redox potential of-0.52 V ***/AgCl,Experimental and theoretical results reveal that the grafted N-cyclic quaternary ammonium groups act as the steric hindrance to prevent nucleophilic attack by OH-,increasing the alkali resistance of the electroactive *** symmetrical battery with 0.50 M（DBPPy）Cl4shows negligible decay during the 13-day cycling *** demonstration,the flow battery utilizing 1.0 M（DBPPy）Cl4as the negolyte and 1-（1-oxyl-2,2',6,6'-tetramethylpiperidin-4-yl）-1'-(3-（trimethylammonio）propyl)-4,4'-bipyridinium trichloride as the posolyte exhibits a high capacity retention rate of 99.99% per cycle at 60 mA cm-2.

关键词： Alkali resistance Aqueous organic flow batteries Stability Steric hindrance viologen

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Polymeric viologen-based electron transfer mediator for improving the photoelectrochemical water splitting on Sb_(2)Se_(3) photocathode

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Fundamental Research 2024年第2期4卷 291-299页

作者： Chang Liu Fusheng Li Linqin Wang Zeju Li Yilong Zhao Yingzheng Li Wenlong Li Ziqi Zhao Ke Fan Fei Li Licheng Sun State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT-KTH Joint Education and Research Centre on Molecular DevicesInstitute for Energy Science and TechnologyDalian University of TechnologyDalian 116024China Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024China Department of Chemistry School of Engineering Sciences in ChemistryBiotechnology and HealthKTH Royal Institute of TechnologyStockholm 10044Sweden

The photogenerated charge carrier separation and transportation of inside photocathodes can greatly influence the performance of photoelectrochemical(PEC)H2 production *** TiO_(2) with p-type semiconductors to construct heterojunction structures is one of the most widely used strategies to facilitate charge separation and ***,the band position of TiO_(2) could not perfectly match with all p-type ***,taking antimony selenide(Sb_(2)Se_(3))as an example,a rational strategy was developed by introducing a viologen electron transfer mediator(ETM)containing polymeric film(poly-1,1′-dially-[4,4′-bipyridine]-1,1′-diium,denoted as PV^(2+))at the interface between Sb_(2)Se_(3) and TiO_(2) to regulate the energy band alignment,which could inhibit the recombination of photogenerated charge carriers of *** Pt as a catalyst,the constructed Sb_(2)Se_(3)/PV^(2+)/TiO_(2)/Pt photocathode showed a superior PEC hydrogen generation activity with a photocurrent density of−18.6 mA cm^(-2) vs.a reversible hydrogen electrode(RHE)and a half-cell solar-to-hydrogen efficiency(HC-STH)of 1.54%at 0.17 V ***,which was much better than that of the related Sb_(2)Se_(3)/TiO_(2)/Pt photocathode without PV^(2+)(−9.8 mA cm^(-2),0.51%at 0.10 V ***).

关键词： viologen Electron transfer mediator Sb2Se3 photocathode Solar water splitting Hydrogen evolution reaction

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Ultrastable viologen Ionic Liquids-Based Ionogels for Visible Strain Sensor Integrated with Electrochromism,Electrofluorochromism,and Strain Sensing

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CCS Chemistry 2023年第8期5卷 1917-1930页

作者： Yueyan Zhang Mengying Guo Guoping Li Xiaoliang Chen Zishun Liu Jinyou Shao YongAn Huang Gang He Frontier Institute of Science and Technology Xi’an Jiaotong UniversityXi’an 710054 Micro-/Nano-technology Research Center State Key Laboratory for Manufacturing Systems EngineeringXi’an Jiaotong UniversityXi’an 710054 International Center for Applied Mechanics State Key Laboratory for Strength and Vibration of Mechanical StructuresXi’an Jiaotong UniversityXi’an 710049 State Key Laboratory of Digital Manufacturing Equipment and Technology Huazhong University of Science and TechnologyWuhan 430074

Flexible electronics play a key role in the development of human society and our daily *** they are expected to revolutionize personal health ***,it remains challenging to fabricate smart sensors with high robustness,reliability,and visible ***,high-performance electrochromic(EC),electro-fluorochromic(EFC),and double-network ionogels with excellent transmissivity,high mechanical robustness,and ultrastable reversibility are prepared by combination of thienoviologen-containing ionic liquids with poly(ethyl acrylate)*** ionogels exhibit good mechanical properties(1000%stretchability and 3.2 kJ m^(−2) fracture energy).The ionogel-based EC devices have a significantly simplified device fabrication process as well as superior cycling stability in which 88%of the contract ratio is maintained at 88%at 500 cycles,even after being stored for 2 years under ambient atmosphere(relative humidity:30%∼40%,25°C).The conductivity of ionogels showed a fast and reproducible response to strain,and the conductivity decreased with increased *** virtue of the EC and EFC properties of the thienoviologen component,the EC and EFC efficiency decreased with the increased strain loaded on the ionogels,and almost no EC or EFC phenomena were observed when the strain was above 300%.This feasible strategy provides an opportunity for the development of visible strain sensors to monitor the body’s movements through color and fluorescence emission.

关键词： ionogels flexible electronics viologen electrochromism strain sensor

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Soluble triarylamine functionalized symmetric viologen for all-solid-state electrochromic supercapacitors

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Science China Chemistry 2020年第11期63卷 1632-1644页

作者： Yanling Zhuang Weiwei Zhao Longlu Wang Feiyang Li Weikang Wang Shujuan Liu Wei Huang Qiang Zhao Key Laboratory for Organic Electronics and Information Displays&Jiangsu Key Laboratory for Biosensors Institute of Advanced MaterialsNanjing University of Posts and TelecommunicationsNanjing 210023China Frontiers Science Center for Flexible Electronics&Shaanxi Institute of Flexible Electronics Northwestern Polytechnical UniversityXi’an 710072China

Electrochromic supercapacitors have drawn enormous attention due to their ability to monitor the charge and discharge processes through color changes of electroactive ***,there are few work on small organic molecules as active materials for all-solid-state electrochromic ***,we reported two novel multifunctional symmetric viologens(TPA-bpy and CZ-bpy),which showed different solvatochromic,electrochromic,electroluminochromic and energy storage behaviors despite their similar chemical *** different performances between these two viologens were attributed to the difference in the intramolecular charge transfer capability and the solubility in organic *** containing TPA-bpy displayed faster response time and higher coloration efficiency due to the introduction of packing-disruptive and three-dimensional triarylamine ***,devices containing TPA-bpy also showed energy storage characteristics with an obvious color change from purple to *** showed a wide voltage window(2.0 V),long discharge time(230.3 s at 0.01 mA cm−2),and excellent cycling stability with 90%capacitance retention after 6,000 *** work provides a new and convenient strategy towards the development of novel electrochromic capacitive materials.

关键词： viologen solvatochromism electrochromism electroluminochromism supercapacitors

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HIGH IMMOBILIZATION OF ANTIBACTERIAL MOIETIES ONTO MONODISPERSE MICROSPHERES BY DISPERSION POLYMERIZATION USING BICATIONIC viologen SURFMER

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Chinese Journal of Polymer Science 2012年第6期30卷 865-872页

作者：刘莲英杨万泰 Key Laboratory of Carbon Fiber and Functional Polymers Ministry of EducationCollege of Materials Science and EngineeringBeijing University of Chemical Technology

In order to achieve monodisperse particles with high content of antibacterial groups covalently bonded on surface, a bicationie viologen, N-hexyl-N-（4-vinylbenzyl）-4,4＇-bipyridinium bromide chloride （HVV） was devised as a surfrner in dispersion polymerization of styrene （St） using a mixture of methanol （or ethylene glycol） and water as media. Effects of content of HVV, its addition profile and composition of reaction media on particles size and incorporation of HVV moieties were mainly investigated. The attachment of silver and gold nanoparticles on particle surface under UV irradiation ascertained the surface-bonded HVV segments. SEM, TEM observations and XPS, zata potential measurements indicated that increase of initial HVV contents and addition of HVV （when polymerization had been performed for 3 h） led to grown particles and enhanced immobilization of HVV moieties. Using a mixture of ethylene glycol and water as reaction media, small particles （520-142 nm） with highly attached HVV moieties were prepared. Furthermore, antibacterial efficacy of the resultant particles against S. aureus was assayed, and particles with more HVV moieties anchored on surface demonstrated greater efficiency of antibacterial activity.

关键词： Antibacterial microsphere Monodispersity Dispersion polymerization viologen Surfmer.

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Two electron utilization of methyl viologen anolyte in nonaqueous organic redox flow battery

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Journal of Energy Chemistry 2018年第5期27卷 1326-1332页

作者： Bo Hu T.Leo Liu The Department of Chemistry and Biochemistry Utah State University

Methyl viologen （MV） as a bench-mark anolyte material has been frequently applied in aqueous organic redox flow batteries （AORFBs） towards large-scale renewable energy storage. However, only the first re- duction of MV was utilized in aqueous electrolytes because of the insoluble MV0generated from the second reduction of MV. Herein, we report that methyl viologen with bis（trifluoromethane）sulfonamide counter anion, MVTFSI, can achieve two reversible reductions in a nonaqueous supporting elec- trolyte. Paired with （Ferrocenylmethyl）trimethylammonium bis（trifluoromethanesulfonyl）imide, FcNFFSI, as catholyte, the MVTFS/FcNTFSI nonaqueous organic redox flow battery （NOARFB） can take advantage of either one electron or two electron storage of the methyl viologen moiety and provide theoretical energy density of 24.9Wh/L and a cell voltage of up to 1.5V. Using a highly conductive LiTFSI/CH_3CN supporting electrolyte and a porous Daramic separator, the NOARFB displayed excellent cycling performance, includ- ing up to a 68.3g energy efficiency at 40 mA/cm2, and more than 88g total capacity retention after 100 cycles.

关键词： Redox flow battery viologen Ferrocene Energy storage

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Ac voltammetric and square wave voltammetric study of the self-assembled monolayers of thiol-functionalized viologen derivative

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Chinese Journal of Chemistry 1997年第2期15卷 130-137页

作者： Li, JH Yang, CH Yan, JC Chen, WQ Dong, SJ CHINESE ACAD SCI CHANGCHUN INST APPL CHEMELECTROANALYT CHEM LABCHANGCHUN 130022JILINPEOPLES R CHINA

Electroactive self-assembled monolayers (SAMs) containing viologen group are formed through the adsorption of thiol-functionalized viologen compound CH3(CH2)(9)V2+(CH2)(8)SH, where V2+ is N,N'-dialkylbipyridinium (i.e. a viologen group), onto gold electrodes from methanol/water solution and its electrochemical behavior is investigated ty Ac voltammetry and square wave voltammetry, which have the high sensitivity against background charging. The viologen SAM formed is a sub-monolayer and the normal potentials corresponding to the two successive one-electron transfer processes of the active centers (viologen) are -360 mV and -750 mV (vs. Ag/AgCl) in 0.1 mol/L phosphate buffer solutions (pH 6.96) respectively, and the standard electron transfer rate constant is 9.0 s(-1). The electrochemical behavior of this SAM in various solutions has been preliminarily discussed.

关键词： self-assembled monolayers viologen Ac voltammetry square wave voltammetry

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A New Iodocuprate/methyl viologen-based Hybird：Structure,Properties and Photocatalytic Activity for the Degradation of Organic Dye

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Chinese Journal of Structural Chemistry 2017年第6期36卷 1020-1026页

作者：李小康蒋阳琴 College of Chemistry and Chemical Engineering Gannan Normal University

A new copper iodide/organic hybrid incorporated with methyl viologen, [（MV）（Cu2I4）·H2O]n（1, MV = methyl viologen）, has been solvothermally synthesized and structurally determined by X-ray diffraction method. 1 crystallizes in tetragonal system, space group P42212 with Mr = 838.95, a = 12.4721（18）, c = 6.5892（13A, V = 1025.0（3） A3, Z = 2, Dc = 2.7125 g/cm3, F（000） = 756, μ（Mo Kα） = 8.097 mm–1, the final R = 0.0273 and wR = 0.0665 for 1062 observed reflections with I 〉 2σ（I）. In 1, the（Cu2I4）n2n- chain was constructed from edge-sharing of distorted Cu I4 tetrahedra. Its absorption spectrum and photoluminescence were investigated, and energy band gap of 1.76 e V indicates its semiconductor nature. Interestingly, 1 exhibits photocatalytic activity for the degradation of rhodamine B.

关键词： organic-inorganic hybrid iodocuprates viologen photocatalytic degradation

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SELECTIVE　REDUCTION　OF　NITROARENE　MEDIATED　BY　AN　INSOLUBLE　RESIN　WITH　viologen　STRUCTURE　AS　ELECTRON-TRANSFER　CATALYST

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Chinese Chemical Letters 1995年第9期6卷 745-746页

作者： Fu Tian LIU Hong LI Bing Lin HE(Institute of Polymer Chemistry, Nankai University, Tianjin 300071) Nankai Univ Inst Polymer Chem Tianjin 300071 Peoples R China

Abstract: : The substituted nitroarenes were reduced effectively to the corresponding aniline deriva tives by an insoluble resin with viologen structure as an electron-transfer catalyst(ETC) in dichloromethane-resin... 详细信息

关键词： AS ELECTRON-TRANSFER STRUCTURE viologen CATALYST WITH BY AN

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