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Boosting the proton conduction in a magnetic dysprosium-organic framework by introducing conjugate NH_(4)^(+)-NH_(3)pairs

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Chinese Chemical Letters 2024年第1期35卷 518-522页

作者： Yi-Ping Qu Qian Zou Song-Song Bao Li-Min Zheng State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

Metal-organic frameworks(MOFs)with inherent porosity and suspended acidic groups are promising proton conducting materials in water or aqua-ammonia *** we report a new lanthanide phosphonate,namely,Dy_(2)(amp_(2)H_(2))_(2)(mal)(H_(2)O)_(2)·5H2O(MDAF-6).It possesses a 3D open-framework structure,and shows a high NH_(3)adsorption capacity of 142.4 cm^(3)/g at P/P0=0.98 at 298 K due to acid-base ***,the proton conductivity of MDAF-6-NH3 is enhanced by five orders of magnitude compared to MDAF-6 after 8.5 h exposure in saturated NH_(3)-H_(2)O vapor,indicating the importance of coexistent conjugate acid-base pairs of H_(3)O+-H_(2)O and NH_(4)^(+)-NH_(3)in promoting proton *** studies of MDAF-6 revealed slow magnetization relaxation under zero dc field,characteristic of singlemolecule magnet *** work provides not only a new multifunctional MOF material,but also a new strategy to improve proton conduction in aqua-ammonia medium.

关键词： Metal-organic framework proton conduction Ammonia adsorption Metal phosphonate Single molecule magnet

Sulfonate-Functionalized Polyoxovanadate-Based Metal-Organic Polyhedra for Enhanced proton conduction via the Synergy of Linker and Metal Cluster Vertex

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Chinese Journal of Structural Chemistry 2022年第8期41卷 12-17页

作者： Yu Zhang Shan-Shan Liu Bo Li Hanqi You Longxi Zhang Zhenyi Zhang Hong-Ying Zang Qi Zheng Weimin Xuan College of Chemistry Chemical Engineering and Biotechnology&State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsDonghua UniversityShanghai 201620China Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education at Universities of Jilin Province Faculty of ChemistryNortheast Normal UniversityChangchun 130024China Bruker(Beijing)Scientific Technology Co. Ltd 9FBuilding No.1Lane 2570Hechuan RdMinhang DistrictShanghai 200233China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China

Metal-organic polyhedra(MOPs)have emerged as novel porous platforms for proton conduction,however,the concerted employment of both linker and metal cluster vertex is rarely applied for the fabrication of MOPs-based high conducting *** we report the synthesis of sulfonate-functionalized polyoxovanadate-based MOPs for enhanced proton conduction via the synergistic effect from linker and metal cluster *** 1 and 2 exhibit octahedral cage configuration constructed from{V_(5)O_(9)Cl}vertex and 5-sulfoisophthalate *** to the ordered packing of octahedral cages along three axes,3D interpenetrated open channels that are lined with high-density sulfonates are thus formed within *** with the proton-conductive{V_(5)O_(9)Cl}vertexs as well as protonated counterions,an extensive H-bonded network is therefore generated for facile proton transfer.2 exhibits high proton conductivity of 3.02×10^(-2)S cm^(-1)at 65℃under 90%RH,recording the highest value for MOPs pellet *** value is enhanced~1order of magnitude compared with that of carboxylate-functionalized analogue 3,clearly illustrating the advantage of combining linker and metal cluster node for enhanced proton *** work will further promote the exploitation of high proton conductive MOPs-based materials by the synergy design strategy.

关键词： metal-organic polyhedra proton conduction polyoxovanadate synergistic effect

Nanostructured Polymer Composite Electrolytes with Self-Assembled Polyoxometalate Networks for proton conduction

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CCS Chemistry 2022年第1期4卷 151-161页

作者： Gang Wang Jialin Li Lichao Shang Haibo He Tingting Cui Shengchao Chai Chengji Zhao Lixin Wu Haolong Li State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012 Key Laboratory of High Performance Plastics Ministry of EducationCollege of ChemistryJilin UniversityChangchun 130012

The key challenge for the use of polymer electrolytes is to realize a high ionic conductivity without scarifying their mechanical ***,we report a facile strategy to prepare a nanostructured polymer electrolyte with both high proton conductivity and high modulus,based on the electrostatic self-assembly of polyoxometalate cluster H_(3)PW_(12)O_(40)(PW)and comb copolymer poly(ether-etherketone)-grafted-poly(vinyl pyrrolidone)(PEEK-gPVP).The incorporation of protonic acid PW can enable the PEEK-g-PVP to be highly proton conductive and create flexible composite electrolyte ***,nanoscale phase separation between PEEK domains and PVP/PW domains spontaneously occurs in these membranes,forming a bicontinuous structure with three-dimensional(3D)-connected PW *** to the dual role of PW networks as both proton transport pathways and mechanical enhancers,these membranes exhibit proton conductivities higher than 30 mS cm^(−1) and modulus over 4 ***,the direct methanol fuel cells equipped with these membranes show good cell *** the wide tunability of comb copolymers and polyoxometalates,this system can be extended to develop a variety of functional electrolyte materials,for example,the lithium-ion conductive electrolytes by using polyoxometalatebased lithium salts,which provides a promising platform to explore versatile electrolyte materials for energy and electronic applications.

关键词： self-assembly polyoxometalates polymer electrolytes nanocomposites proton conduction

Ultrathin nanoporous metal electrodes facilitate high proton conduction for low-Pt PEMFCs

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Nano Research 2021年第8期14卷 2681-2688页

作者： Shuai Shi Xianglong Wen Qinqin Sang Shuai Yin Kaili Wang Jian Zhang Min Hu Huiming Yin Jia He Yi Ding Tianjin Key Laboratory of Advanced Functional Porous Materials Institute for New Energy Materials&Low-Carbon TechnologiesSchool oj Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Design of catalyst layers(CLs)with high proton conductivity in membrane electrode assemblies(MEAs)is an important issue for proton exchange membrane fuel cells(PEMFCs).Herein,an ultrathin catalyst layer was constructed based on Pt-decorated nanoporous gold(NPG-Pt)with sub-Debye-length thickness for proton *** the absence of ionomer incorporation in the CLs,these integrated carbon-free electrodes can deliver maximum mass-specific power density of 198.21 and 25.91 kW·gPt^(-1) when serving individually as the anode and cathode,at a Pt loading of 5.6 and 22.0 pg·cm^(-2),respectively,comparable to the best reported nano-catalysts for ***-depth quantitative experimental measurements and finite-element analyses indicate that improved proton conduction plays a critical role in activation,ohmic and mass transfer polarizations.

关键词： nanoporous metal electrode proton exchange membrane fuel cell(PEMFC) ultrathin catalyst layer proton conduction dealloying

Pillared-layer MOF Based on Template-directed Method: Synthesis, Structure and proton conduction Properties

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Chinese Journal of Structural Chemistry 2020年第7期39卷 1337-1342页

作者： WANG Fu-Xiang REN Guo-Jian TIAN Rui-Jing FENG Li-Juan YANG Yong-Hang DENG Yong-Yan PAN Qin-He Key Laboratory of Advanced Materials of Tropical Island Resources Ministry of EducationSchool of ScienceHainan UniversityHaikou 570228China School of Information Engineering Changchun Sci-Tech UniversityChangchun 130600China

By using Co(NH3)63+as the template,a new complex HNU-38 was synthesized under hydrothermal reaction through the adoption of H3BTC and Cl-as the ligands(H3BTC=1,3,5-benzenetricarboxylic acid).HNU-38 crystallized in the monoclinic system,P21/c space group with a=9.9696(3),b=17.0580(6),c=16.5263(6)?,β=100.400(2)o,Z=4,V=2764.31(16)?3,Mr=883.63,Dc=2.123 g/cm3,F(000)=1736,S=0.920,R=0.0358 and wR=0.0838(Ⅰ>2σ(Ⅰ)).In HNU-38,the Cd2+and BTC3-were linked together to form layers with Cl-serving as the *** should be noted that(H2O)n chains were found in the channels and play a co-templating role along with the Co(NH3)63+cations in HNU-38,and the proton conduction properties were investigated.

关键词： template synthesis metal-organic framework pillared-layer proton conduction

Incorporation of polyoxometalate-based acid–base pair into a sulfonated MIL-101 for achieving proton-conduction materials with high proton conductivity and high stability

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Tungsten 2022年第2期4卷 130-137页

作者： Wan-Yu Zhang Ying Lu Zhuo Li Yang Wang Xiu-Wei Sun Qian Wang Zhong Zhang Shu-Xia Liu Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education College of ChemistryNortheast Normal UniversityChangchun130024China

Currently,it is of great significance to develop new proton-conduction materials with high proton conductivity,high stability,and good conducting durability to meet the demands of fuel cell and ***,we prepared two composites DETA-HPW@MIL-101-SO_(3)H 1 and TETA-HPW@MIL-101-SO3H 2(DETA=diethylenetriamine,HPW=H_(3)PW_(12))_(4)0·xH_(2)O,MIL=Material Institut Lavoisier,TETA=triethylenetetramine)by encapsulating polyoxometalate(POM)and organic amine into a sulfonated MIL-101 through a step-by-step dipping ***,1 and 2 have high proton conductivities of 6.4×10^(−2) and 2.9×10^(−2) S·cm^(−1) at 65℃ and 95%relative humidity(RH),respectively,which can be attributed to the fast proton transfer among acid–base pairs formed between HPW and organic amine as well between sulfonic acid and organic ***,the time-dependent test in proton conductivity displays that their proton-conduction properties have good stability and durability,which benefit from that the electrostatic interactions among acid–base pairs and the limitation of opening size of MIL-101-SO3H make HPW and organic amine stably exist in the cages of MIL-101-SO_(3)*** remarkable proton-conduction properties(high proton conductivity and high stability)of the two composites make them become promising proton-conduction materials.

关键词： Polyoxometalate Acid-base pair MIL-101-SO3H proton conduction

proton conduction of Tb-benzophenone-3,3'-disulfonyl-4,4'-dicarboxylate framework

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Proton conduction of Tb-benzophenone-3,3'-disulfonyl-4,4'-di...

What are the effects of the serine triad on proton conduction of an influenza B M2 channel? An investigation by molecular dynamics simulations

2018年中西部地区无机化学化工学术研讨会

作者：李振涛张文文王玉玲刘庆燕江西师范大学化学化工学院

A novel Tb-benzophenone-3,3’-disulfonyl-4,4’-dicarboxylate compound(1) was synthesized and structurally characterized. The Tb(Ⅲ) ions are bridged by the carboxylate groups of BODSDC4–(benzophenone-3,3’-disulfonyl-4,4’-dicarboxylate) ligands to give a one-dimensional(1 D) chain, which is further linked by the BODSDC4– ligands to yield a three-dimensional(3 D) framework featuring 1 D channels. The 1 D open channels surrounded by high-density hydrophilic sulfonate groups facilitates enrichment of the solvate water molecules in the channels, resulting in a high proton conductivity of 6.57 × 10 S cm-1 at 95% RH and 85 ℃. The proton conductivity at 25 ℃ are 1.17 × 10 S cm at 50% RH and 2.16 × 10 S cm at 95% RH, which indicates that the conductivity is highly humidity dependent and increases by raising RH. As the temperature increases, the Nyquist plots display a noticeable increase in the conductivity(σ) with temperature from 25(2.16 × 10-5 S cm-1) to 85 ℃(6.57 × 10-4 S cm-1) under 95% RH. Additionally, 1 shows a steady increase in conductivity when the RH was increased from 50% to 85%. Finally, the curves of the humidity-dependent proton conductivity can be measured by repeatedly decreasing and increasing the humidity at 85℃ in the range of 50-95% without distinct change. It indicates 1 is stable under impedance measurements and different RH. This work is provides an excellent example for design of the proton conductive MOF materials based on the sulfonate-carboxylate organic ligands.

关键词： proton conduction Tb-MOF benzophenone-3,3’-disulfonyl-4,4’-dicarboxylate

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What are the effects of the serine triad on proton conductio...

Dimensional regulation in gigantic molybdenum blue wheels featuring{(W)Mo5}motifs for enhanced proton conductivity

2019中国化学会第十五届全国计算（机）化学学术会议

作者：张玥 Qing-chuan Zheng 吉林大学 Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryInternational Joint Research Laboratory of Nano-Micro Architecture Chemistry Jilin University Key Laboratory for Molecular Enzymology and Engineering of the Ministry of Education Jilin University

The tetrameric influenza B M2 channel（BM2）, an acid activated proton channel, is important in the influenza virus B lifecycle. A conserved HxxxW motif is responsible for proton conduction and channel gating. In this study, to explore the effects of the serine triad（S9, S12 and S16） on proton conduction, we performed classical molecular dynamics（CMD） simulations and adaptive steered molecular dynamics（ASMD） simulations at different protonation states of the H19 tetrad. The results of the pore radius and the C-terminal tilt angle show that the electrostatic repulsion induced by protonated H19 is the key driving force for opening the BM2 channel. The open states could be stabilized by the hydrogen bonds between S16 and protonated H19. The solvent accessible surface area and water density indicate that the polar hydrophilic environment provided by the serine triad facilitates the formation of a water wire, and then exhibits favourable effects on proton conduction. The mutant research verifies and supports these views. Our work clarifies the effects of the serine triad on proton conduction in the BM2 channel, which would help us deeply understand the proton conduction mechanism in BM2 and provides a new perspective for antiviral drug design against BM2.

关键词： influenza virus B M2 channel membrane protein proton conduction molecular dynamics simulations

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Nano Research 2024年第9期17卷 8261-8268页

作者： Yu-Lun Wu Jing Du Hai-Ying Zhang Ming-Jun Hou Qiao-Yue Li Wei-Chao Chen Kui-Zhan Shao Bo Zhu Chao Qin Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Department of ChemistryNortheast Normal UniversityChangchun 130024China Hebei Key Laboratory of Organic Functional Molecules National Demonstration Center for Experimental Chemistry EducationTesting and Analysis CenterCollege of Chemistry and Materials ScienceHebei Normal UniversityShijiazhuang 050024China State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchun 130021China

Dimensional regulation in polyoxometalates is an effective strategy during the design and synthesis of polyoxometalates-based high proton conductors,but it is not available to ***,the precise regulation of dimensionality has been realized in an unprecedented gigantic molybdenum blue wheel family featuring pentagonal{(W)Mo5}motifs through optimizing the molar ratio of Mo/W,including[Gd_(2)Mo_(124)W_(14)O_(422)(H_(2)O)62]38-(0D-{Mo_(124)W_(14)},1),[Mo_(126)W_(14)O441(H_(2)O)51]^(70-)(1D-{Mo_(126)W_(14)}n,2),and[Mo_(124)W_(14)O_(430)(H_(2)O)50]60-(2D-{Mo_(124)W_(14)}n,3).Such important{(W)Mo5}structural motif brings new reactivity into gigantic Mo blue *** are different numbers and sites of{Mo2}defects in each wheel-shaped monomer in 1-3,which leads to the monomers of 2 and 3 to form 1D and 2D architectures via Mo-O-Mo covalent bonds driven by{Mo2}-mediated H_(2)O ligands substitution process,respectively,thus achieving the controllable dimensional *** expected,the proton conductivity of 3 is 10 times higher than that of 1 and 1.7 times higher than that of *** continuous proton hopping sites in 2D network are responsible for the enhanced proton conductivity with lower activation *** study highlights that this dimensional regulation approach remains great potential in preparing polyoxometalates-based high proton conductive materials.

关键词： polyoxometalate molybdenum blue wheels Mo/W mixed-addenda polyoxometalates dimensional regulation proton conduction