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Parallelogram 3d-4f-5d heterometallic clusters based on trilacunary tungstoantimonates with excellent proton conductivity

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Chinese Chemical Letters 2024年第3期35卷 528-531页

作者： Haiying Wang Han Xu Chaolong Chen Yingjie Zhu Yikang Zhang Dongdi Zhang Jingyang Niu Henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Molecular SciencesHenan UniversityKaifeng 475004China School of Pharmaceutical Science&Yunnan Key Laboratory of Pharmacology for Natural Products Kunming Medical UniversityKunming 650500China Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Two 3d-4f-5d heterometallic cluster-containing polyoxometalates,formulated as Na_(22){(SbW_(9)O_(33))_(4)[La_(3)W_(6)MO_(18)(H_(2)O)_(8)(CH_(3)COO)_(4)]_(2)}·nH_(2)O(abbreviated as La_(6)M_(2),M=Co/Mn)were synthesized and structurally ***-crystal X-ray diffraction analyses reveal that the polyanions of La_(6)Co_(2)and La_(6)Mn_(2)consist of the uncommon 3d-4f-5d clusters{La_(6)W_(12)Co_(2)}and{La_(6)W_(12)Mn_(2)},which are encapsulated by four trilacunary Keggin tungstoantimonates to form the parallelogram-shaped title ***,the polyanions can be extended into a two-dimensional(2D)frame by the linkage of peripheral Na+*** inner space of the 2D layer was filled with water molecules and thus an H-bonded network was formed,which is expected to exhibit a fascinating proton *** study of water-assisted proton conduction demonstrated that La_(6)Co_(2)and La_(6)Mn_(2)were temperature-and humiditydependent proton conductors,respectively,and the proton conductivities could reach 1.3×10^(-2)and 2.3×10^(-2)S/cm at 65℃and 90%RH conditions.

关键词： Polyoxometalate Parallelogram Heterometallic 3d-4f-5d cluster proton conductivity

Carbazole Based Anionic MOF for proton conductivity

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Chinese Journal of Structural Chemistry 2021年第1期40卷 55-60,2页

作者： GUO Shan-Shan HUANG Lv-Lan YE Ying-Xiang LIU Li-Zhen YAO Zi-Zhu XIANG Sheng-Chang ZHANG Jin-Dan ZHANG Zhang-Jing College of Chemistry and Materials Science Fujian Provincial Key Laboratory of Polymer MaterialsFujian Normal UniversityFuzhou 350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

A non-interpenetrated anionic In-MOF(FJU-302)based on a linear H2 bpdc and an angled H2 cdc as dual-ligands was characterized by FT-IR,TGA and X-ray single-crystal/powder ***-302 crystallizes in the monoclinic system and I4_(1)/amd space group with a=27.1274(8),b=27.1274(8),c=29.788(3)Å,V=21921(2)Å^(3),Z=16,M_(r)=608.32,D_(c)=0.737 g/cm^(3),F(000)=4848,μ(Cu Kα)=3.659 mm^(–1),R=0.0800 and wR=0.1911 for 5703 observed reflections(I>2s(I)),and R=0.1470 and w R=0.2342 for all *** this work,a carbazole based anionic In-MOF(FJU-302)was designed and synthesized,and the proton conductivity from subzero temperature(–30℃)to 70℃ was measured without additional ***-302 presents a max proton conductivity of 6.47×10^(–4) S·cm^(–1) at 70℃,and it can maintain 5.88×10^(–7) S·cm^(–1) at–30℃.This work reports a first carbazole based MOF for proton conductivity at subzero temperature conditions.

关键词： metal-organic frameworks carbazole proton conductivity

Experimental measurement of proton conductivity and electronic conductivity of membrane electrode assembly for proton exchange membrane fuel cells

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Progress in Natural Science:Materials International 2020年第6期30卷 912-917页

作者： Ruili Sun Zhangxun Xia Congrong Yang Fenning Jing Suli Wang Gongquan Sun Division of Fuel Cells and Battery Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Key Laboratory of Fuel Cells & Hybrid Power Sources Chinese Academy of Sciences University of Chinese Academy of Sciences

Charge transport processes involving the proton migration and electron transfer for different parts of membrane electrode assemble(MEA) play an essential role for developing the novel electrode and enhancing the electrochemical performance towards proton exchange membrane fuel cells(PEMFCs). However, the coupled charge transport processes make it difficult for evaluating proton conductivity and electronic conductivity of different parts in MEAs under operation conditions of fuel cells. Here in this work, we propose an experiment approach for separating the electronic conductivity and proton conductivity of different components of MEA at the operating conditions of PEMFCs. This approach involves two different measuring devices, which both consist of electron or proton conducting layers, sealing layers and sample layer, followed by tailoring the thickness of sample layers and via electrochemical impedance spectroscopy(EIS) to quantity the electronic conductivity and proton conductivity of different layers. These experiment results show the great potential in the development of different components of MEA.

关键词： proton exchange membrane fuel cells Membrane electrode assembly proton conductivity Electronic conductivity

Influences of Structure Disorder and Temperature on Properties of proton conductivity in Hydrogen-Bond Molecular Systems

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Communications in Theoretical Physics 2007年第2期47卷 235-243页

作者： PANG Xiao-Feng YU Jia-Feng Institute of Life Science and Technology University of Electronic Science and Technology Chengdu 610054 China International Centre for Materials Physics the Chinese Academy of Sciences Shenyang 110015 China

The dynamic properties of proton conductivity along hydrogen-bonded molecular systems, for example, ice crystal, with structure disorder or damping and finite temperatures exposed in an externally applied electric-field have been numerically studied by Runge-Kutta way in our soliton model. The results obtained show that the proton-soliton is very robust against the structure disorder including the fluctuation of the force constant and disorder in the sequence of masses and thermal perturbation and damping of medium, the velocity of its conductivity increases with increasing of the externally applied electric-field and decreasing of the damping coefficient of medium, but the proton-soliton disperses for quite great fluctuation of the ＂force constant and damping coefficient. In the numerical simulation we find that the proton-soliton in our model is thermally stable in a large region of temperature of T ≤ 273 K under influences of damping and externally applied electric-field in ice crvstal. This shows that our model is available and appropriate to ice.

关键词： proton conductivity structure disorder temperature hydrogen bonded system

Synthesis,proton conductivity and Humidity Sensing Property ofγ-Type Zirconium Hydrogen Phosphate,Zr(HPO_4)_2·2H_2O

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Chemical Research in Chinese Universities 1999年第1期15卷 7-11页

作者： FENG Shou-hua ZHAO Hui LI Lian-sheng Martha Greenblatt Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun 130023 Department of Chemistry Rutgersthe State University of New JerseyPiscatawayNJ 08855USA

A γ - type of layered zirconium hydrogen phosphate, Zr(HPO 4) 2·2H 2O( γ ZrP), was synthesized under hydrothermal conditions and characterized by powder X ray diffraction and thermogravimetric analysis. The temperature dependence of the proton conductivity in γ ZrP was investigated in a temperature range of 23￣413 ℃ by ac impedance spectroscopy. The variation of the conductivity with water loss and phase transitions was observed. The best proton conductivity in γ ZrP is 6×10 -4 S·cm -1 at 60 ℃. The proton conductivities in the dehydrated sample are ￣10 -5 at 150 ℃ and ￣10 -4 S·cm -1 at 350 ℃, respectively. The conductivities as a function of humidity in the temperature range of 120￣200 ℃ were measured.

关键词： Synthesis γ-Type zirconium hydrogen phosphate proton conductivity Humidity sensing property

Flexible side arms of ditopic linker as effective tools to boost proton conductivity of Ni_(8)-pyrazolate metal-organic framework

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Chinese Chemical Letters 2022年第6期33卷 3227-3230页

作者： Jieying Hu Hu Zhang Zihao Feng Qian-Ru Luo Can-Min Wu Yuan-Hui Zhong Jian-Rong Li Lai-Hon Chung Wei-Ming Liao Jun He School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China

Two primitive metal-organic frameworks(MOFs),Ni L1 and Ni L2,based on Ni_(8)O_(6)-cluster and ditopic pyrazolate linkers,L1(with rigid alkyne arms)and L2(with flexible alkyne chains),were *** proton conductivities of these MOFs in pristine form and imidazole-encapsulated forms,Im@Ni L1 and Im@Ni L2,were measured and *** introduction of imidazole molecules,the proton conductivity could be increased by 3 to 5 orders of magnitude and reached as high as 1.72×10^(-2)S/cm(at 98%RH and 80℃).Also,whether imidazole molecules were introduced or not,Ni_(8)O_(6)-based MOFs with L2 in general gave better proton conductivity than those with L1 signifying that flexible side arms indeed assist proton conduction probably via establishment of efficient proton-conducting channels along with formation of highly ordered domains of water/imidazole molecules within the network *** the active Ni_(8)O_(6)-cluster,tuning flexibility of linker pendants serves as an alternative approach to regulate/modulate the proton conductivity of MOFs.

关键词： proton conductivity Metal-organic framework Pyrazolate linkers Nickel-oxide cluster Imidazole encapsulation

Synthesis，proton　conductivity　and　High－Temperature　Humidity　Sensing　Property　of　Zr（HPO_4）_2·H_2O　and　Its　Aluminium－substituted　Compositions

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Chemical Research in Chinese Universities 1996年第4期12卷 313-321页

作者： WANG Ge and FENG Shou-hua(Key Laboratory of Inorganic Hydrothermal Synthesis,)Department of Chemistry,Jilin University,Changchun,130023)WANG Bo and Martha Greenblatt(Deparrment of Chemistry,Rutgers,The State University of New Jersey,New Brenswick,NJ 08903 JILIN UNIV DEPT CHEMKEY LAB INORGAN HYDROTHERMAL SYNTHCHANGCHUN 130023PEOPLES R CHINA RUTGERS STATE UNIV DEPT CHEMNEW BRUNSWICKNJ 08903

A series of aluminium-containing α-type hydrated zirconium hydrogen phosphates,Zr_(1-x)Alx (H_(1+x/2)PO_4 )_2 with x=0-0.06,were hydrothermally synthesized and characterizedby means of X-ray diffraction,differential thermal analysis and thermogravimetric *** proton conductivity,1.2×10￣(-4) S·cm￣(-1)at 180℃ was found in Zr_(0.98)Al_(0.02)(H_(1.01)PO_4)_2·H_***-sensing measurements were carried out at 120℃ and 140℃ *** a limited substitution of Al for Zr can enhance both proton conductivity and humidity sensitivity.

关键词： s:Aluminium-containing α-type hydrated zirconium hydrogen phosphates proton conductivity Humidity sensing property

Enhanced proton conductivity of viscose-based membranes via ionic modification and dyeing processes for fuel cell applications

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Journal of Materiomics 2023年第3期9卷 587-600页

作者： Haoyu Wu Tianchi Zhou Bin Wang Jinli Qiao Flexible Functional Materials Institute Yancheng Institute of Technology1 Hope Avenue RoadYancheng224051China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua University2999 Ren'min North RoadShanghai201620China Shanghai Engineering Research Center of Marine Renewable Energy Shanghai201306China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

proton exchange membranes(PEMs),which are crucial fuel cell parts,play an important role in the field of energy ***,the further development of conventional PEMs based on synthetic polymers is greatly limited by high energy consumption and difficult *** this work,we reported the fabrication of a novel viscose-based PEM via cationic modification and dyeing treatment with the reactive dyes ***-efficiency proton transmission channels can be constructed due to the for-mation of the complex internal three-dimensional network of the as-prepared viscose-based PEM.Hþconductivity(sHþ)and water uptake are intensively investigated by changing the cationic agents and KE-7B1,and the maximum sHþreaches 44.19 mS/cm at 80℃and 98%relative humidity(RH).Furthermore,the prepared membrane shows the lowest calculated activation energy value(12.25 kJ/mol),indicating that both Grotthuss and Vehicle mechanisms play an important role in ionic *** membrane chemical structure and micromorphology are analyzed and the proton transmission modes are explored in detail,supplemented with research on the hydrophilic/hydrophobic characteristics and crystallinity of the *** application stability of the membranes is also evaluated analyzing the thermal,mechanical,and oxygen resistance properties,and the results show that all the prepared membranes can maintain good thermal stability within 200℃.The maximum tensile strength reaches 42.12 MPa,and the mass losses of the membranes soaked in 30%(in mass,same below)H_(2)O_(2)solution for 120 h can be restricted to 10%.Therefore,as a novel PEM,the obtained dye viscose-based membranes show great potential for application in fuel cells.

关键词： Membrane Viscose Reactive dyes proton conductivity Fuel cell

Single molecule magnetic behavior and photo-enhanced proton conductivity in a series of photochromic complexes

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Chinese Chemical Letters 2022年第3期33卷 1417-1421页

作者： Qian Zhang Jixiang Hu Qi Li Dongxue Feng Zhenni Gao Guoming Wang College of Chemistry and Chemical Engineering Qingdao UniversityQingdao 266071China

Molecules with multifunctional properties are of immense interest in hybrid materials, while challenges still existed because of the limited compatibility of multiple functionalities in a single system. In this work, a series of metal-organic complexes were synthesized and characterized under the assembly of electron donor phosphonate, electron acceptor polypyridine ligand and spin carrier rare earth ions. All the compounds exhibited remarkable and reversible responses with photochromism and photomodulated fluorescence, originated from photogenerated radicals via electron transfer from phosphonates to polypyridine ligands. For the Dy analog, slow magnetic relaxation was observed at cryogenic temperature, indicating the single-molecule magnetic behavior. Furthermore, photogenerated radicals could enhance the proton conductive behavior, with about 2 times larger in magnitude after light irradiation for Dy and Y compounds. The introduction of photoluminescence, magnetism and proton conduction into metallic phosphonates can provide potential applications for photochromic materials.

关键词： Multifunctional Electron transfer Photochromism Single molecule magnetic behavior proton conductivity