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A novel thermomechanically stable LaF_3–CsH_5(PO_4)_2 composite electrolyte with high proton conductivity at elevated temperatures over 150 °C

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Journal of Energy chemistry 2019年第3期28卷 114-120页

作者： Jie Xiong Yunjie Huang Jing Li Liying Ma Guoxiao Xu Zhao Liu Weiwei Cai Hansong Cheng Sustainable Energy Laboratory Faculty of Materials Science and Chemistry China University of Geosciences (Wuhan) College of chemistry Chemical Engineering and Material Science Zaozhuang University

A facile strategy is introduced to upgrade thermomechanical stability of the cesium pentahydrogen diphosphate(CPD), which is the most efficient inorganic electrolyte among all solid proton conductors,by constructing P–OH···F hydrogen bonds with lanthanum fluoride(LaF_3). The optimal combination of the LaF_3–CPD composite electrolyte is found to be 1:2 in a molar ratio(LaF_3–CPD-2). LaF_3–CPD-2 composite maintains robust solid state, even at a temperature up to 200 °C, which is 50 °C higher than the melting temperature of CPD. Meanwhile, the considerable proton conductivity of CPD is achieved in the LaF_3–CPD-2 composite electrolyte due to the synergistic effect of the P–OH···F hydrogen bonds and the intrinsic proton conductive property of CPD. Last but not least, the LaF_3–CPD-2 composite manifests excellent conductivity durability at 150 °C and low humidity condition with sizeable proton conductivity of0.0262 S cm^(-1) after 60 h operation, implying that the LaF_3–CPD composite could be a promising candidate for intermediate temperature proton conductors.

关键词： Intermediate temperature fuel cell Hydrogen bond Cesium pentahydrogen diphosphate Lanthanum fluoride Thermomechanical stability

Continuous polypyrrole nanotubes encapsulated Co_(3)O_(4)nanoparticles with oxygen vacancies and electron transport channels boosting peroxymonosulfate activation

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Nano Research 2023年第8期16卷 11018-11029页

作者： Dingyang Chen Wanning Wu Xinyue Zhao Danyang Feng Rui Zhao Guangshan Zhu Key Laboratory of Polyoxometalate and Reticular material chemistry of Ministry of Education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

Co_(3)O_(4)particles are promising heterogeneous catalysts for peroxymonosulfate(PMS)activation;whereas they still surfer from the extensive agglomeration,serious Co leaching,poor electronic conductivity,and difficult recovery.Herein,a novel hybrid nanoarchitectonic constructed by encapsulating Co_(3)O_(4)nanoparticles into continuous polypyrrole(PPy)nanotubes(Co_(3)O_(4)@PPy hybrids)was developed using electrospun fibers as the templates,which boosted the catalytic degradation toward tetracycline(TC).The continuous polypyrrole nanotubes could provide the confined spaces,offer effective electron transfer pathway,suppress cobalt ion loss,facilitate the oxygen vacancy(Ovac)formation,and accelerate the Co^(2+)/Co^(3+)cycles.Co_(3)O_(4)@PPy hybrids thereby exhibited a remarkably enhanced catalytic activity with the TC degradation efficiency of 97.2%(kobs=0.244 min^(−1))within 20 min and total organic carbon(TOC)removal rate of 66.8%.Furthermore,the recycle test,real natural water treatment,and fluidized-column catalytic experiments indicated the potential of Co_(3)O_(4)@PPy hybrids in the practical large-scale applications.

关键词： polypyrrole(PPy)nanotube Co_(3)O_(4) peroxymonosulfate(PMS) tetracycline(TC)degradation

多电子反应的共轭梯型聚合物作为高容量锂离子电池有机负极材料

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science China materials 2022年第9期65卷 2354-2362页

作者：于杰陈新宇王恒国高波韩东来司振君 Key Laboratory of Polyoxometalate and Reticular material chemistry of Ministry of Education and faculty of chemistry Northeast Normal UniversityChangchun 130024China School of materials science and Engineering Changchun University of Science and TechnologyChangchun 130022China

梯形共轭聚合物(LCPs)由于其固有的稳定性、较低的溶解性、可调的结构和强的π-π分子间相互作用,在可充电锂离子电池(LIBs)中引起了广泛关注.在此,我们通过四氨基苯醌和芳香族二酐之间的缩聚反应合成了两种富含杂原子氮/氧的LCPs(TNL和... 详细信息

梯形共轭聚合物(LCPs)由于其固有的稳定性、较低的溶解性、可调的结构和强的π-π分子间相互作用,在可充电锂离子电池(LIBs)中引起了广泛关注.在此,我们通过四氨基苯醌和芳香族二酐之间的缩聚反应合成了两种富含杂原子氮/氧的LCPs(TNL和TPL).得益于多环芳烃体系中的刚性骨架,大共轭结构和杂原子驱动的超锂化过程,富氮/氧杂原子的LCPs作为LIBs的有机负极材料显示出高比容量和优异的长期循环稳定性.特别地,在0.05 A g^(-1)电流密度下,TNL展现了1063.5 mA h g^(-1)的高可逆比容量,良好的循环性能(在1 A g^(-1)电流密度下循环1000次后容量保持率为75.2%),以及优异的倍率性能(即使在2 A g^(-1)的电流密度下仍具有260.6 mA h g^(-1)比容量).此外,通过理论计算进一步证实了超锂化存储机制,表明C=O、C=N和芳香环的多个活性位点的锂离子存储机制.此外,还通过将TNL负极与LiCoO_(2)正极匹配来组装全电池,证明了其实际应用的可行性.

关键词： ladder-type conjugated polymers polycyclic aromatic systems multielectron reactions superlithiation mechanism lithium-ion batteries

Pompon-like NiCo_(2)O_(4) nanospheres:a potential candidate for the counter electrode in quantum dot-sensitized solar cells

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钨科技(英文) 2023年第2期5卷 235-246页

作者： Qiu Zhang Ting-Ting Zhang Feng-Yan Li Lin Xu Key Laboratory of Polyoxometalate and Reticular material chemistry of Ministry of Education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

To find a novel counter electrode(CE)material for quantum dot-sensitized solar cells(QDSSCs),pompon-like NiCo_(2)O_(4) nanospheres are synthesized by a facile solvothermal and post-calcination method and we attempt to apply it as a CE material for QDS SC.The catalytic performance of NiCo_(2)O_(4) counter electrode is investigated in detail through electrochemical impedance spectroscopy,Tafel test and cyclic voltammetry.The catalytic activity of NiCo_(2)O_(4) CE is superior to that of nanoflower-like Cu2S CE and traditional Cu2S/brass CE,which is mainly attributed to the large specific surface area,outstanding electrical conductivity of bimetallic oxides and the synergistic promotion effect of metals with different valence states.Under standard sunlight(air mass AM 1.5G 100 mW·cm^(-2)),the CdS/CdSe/ZnS-sensitized solar cell assembled with NiCo_(2)O_(4) CE achieved a photoelectric conversion efficiency of 5.55%,with a short current density of 22.49 mA·cm^(-2),an open circuit voltage of 0.574 V,and a fill factor of 0.43,which is slightly higher than the QDSSCs with nanoflower-like Cu_(2)S CE(4.75%)and traditional Cu_(2)S/brass CE(4.69%).This research provides ideas for discovering innovative and efficient CE materials for QDSSCs.

关键词： QDSSCs Counter electrodes NiCo_(2)O_(4) Cu_(2)S

The roles of active species in photo-decomposition of organic compounds by microwave powered electrodeless discharge lamps

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Journal of Environmental sciences 2015年第7期27卷 60-68页

作者： Jun Hong Bo Han Nannan Yuan Jingli Gu School of Environmental Studies China University of Geosciences Faculty of Material Science and Chemistry China University of Geosciences

Knowledge of the effective radiation spectrum irradiating substrates from microwave powered electrodeless discharge lamps（MEDLs）, and the active species that directly oxidize substrates in the photolytic process, is fragmentary and unclear. In this work, we conducted a comparative study using MEDLs made with quartz envelopes（MEDL-quartz） and with borosilicate Pyrex envelopes（MEDL-Pyrex） targeting the degradation of Rhodamine B（Rh B）via radical-extinguishing tests. We found that UVC/UVB radiation is essential to generate·OH and H2O2 in the MEDL-quartz system. The degradation of Rh B mostly originates from·OH species, which account for a contribution of 53.8%, while the remaining contribution is attributed to oxidation by H2O2 and direct photolysis. This degradation is influenced by several parameters. Acidic and neutral p Hs, but not extreme alkaline p H, benefit the degradation. To ensure a high intensity of UVC/UVB, the optimum ratio of the MEDL volume to the aqueous solution volume（VL/VS） is 0.4. Concentrations of 0.15-0.20 mmol/L of Rh B are suitable to obtain an effective quantum absorbance in the MEDL-quartz system,showing a high decomposition rate of 5.6 × 10^-3（mmol/L）min-1. Moreover, two other substrates, Reactive Brilliant Red X-3B and Safranine T, were tested and found to be efficiently degraded in the MEDL-quartz system.

关键词： Microwave Electrodeless discharge lamps UVC/UVB Species Degradation

Density Functional Theory Study on the First Hyperpolarizabilities of Mono-and Bimetal Ir(Ⅰ)/Rh(Ⅰ)2,2'-Bidipyrrins Complexes

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Chinese Journal of Structural chemistry 2017年第6期36卷 877-885页

作者：荆丽雪王丽陈珍珍陈赫仇永清 Institute of Functional material chemistry Faculty of ChemistryNortheast Normal University

Metal complexes with excellent nonlinear optical（NLO） properties have attracted considerable attention. The geometry structure, electronic spectra and NLO properties of 2,2？-bidipyrrins（L） and mono-and bimetal Ir（I）/Rh（I）–L complexes have been investigated by density functional theory method. Our calculations revealed that L with planar configuration shows the largest first hyperpolarizability value, which is 2.2 to 5.5 times larger than that of others. It is attributed to the single direction of intramolecular charge transfer. When metal ions were embedded in ligands, the first hyperpolarizability values of mono-and bimetal Ir/Rh（I）–L complexes were smaller than that of L, and that of bimetal Ir/Rh（I）–L complexes were smaller than the corresponding monometallic Ir/Rh（I）–L. This is caused by the intramolecular charge transfer from multiple directions as well as the amount of charge transfer. On the other hand, on increasing the number of metal ions, the charge transfer in the opposite direction cancels each other more obviously. Our work would provide some theoretical reference for the second-order NLO responses of mono-and bimetal complexes.

关键词： Ir（I）/Rh（I） complexes DFT second-order NLO response ,charge-transfer

Frustrated Lewis pairs in situ formation in B-based porous aromatic frameworks for efficient o-phenylenediamine cyclization

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Chinese Chemical Letters 2023年第5期34卷 567-570页

作者： Anqi Dai Shulin Li Tienan Wang Yuting Yang Yuyang Tian Xiaofei Jing Guangshan Zhu Key Laboratory of Polyoxometalate and Reticular material chemistry of Ministry of Education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

Benzimidazoles are very important chemical materials in the pharmaceutical industry,and the most common synthetic route is cyclization of o-phenylenediamine with carbon sources,in which utilization of inexpensive and abundant CO_(2)as C1 source is very impressive.Porous aromatic frameworks(PAFs)with highly desired skeletons have attracted great attentions in gas capture and catalysis.Herein,B-based PAF-165 and PAF-166 are designed and synthesized via Friedel-Crafts alkylation reaction,which present high surface areas as well as high stability.Benefiting from the abundant electron-deficient B centers,both PAFs exhibit excellent selective CO_(2)adsorption abilities.The presence of sterically hindered B units in PAFs can act as Lewis acid active sites for the frustrated Lewis pairs(FLPs)in situ formation with ophenylenediamine,thus promoting the synthesis of benzimidazole.The optimal reaction conditions for o-phenylenediamine cyclization with PAF catalysts are explored,and the reaction mechanism is also proposed.This work provides feasible ideas for incorporating FLPs within porous materials as reusable heterogeneous catalysts for CO_(2)capture and conversion.

关键词： Porous aromatic frameworks(PAFs) CO_(2)capture and conversion Gas sorption Frustrated lewis pairs(FLPs) Heterogeneous catalysis

Simple Preparation, Structure and Conductivity of Nickel(Ⅱ) Benzenetricarboxylate Ni_3(BTC)_2·12H_2O

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Chinese Journal of Structural chemistry 2014年第3期33卷 401-406页

作者：谭海燕刘城王朝晖吴金平 Sustainable Energy Laboratory Faculty of Material Science and Chemistry China University of Geosciences Wuhan

Proton-conductive crystalline metal-organic framework nickel（Ⅱ） benzenetricar- boxylate Ni3（BTC）2A12H2O（MOF-Ni） was prepared by the reaction of nickel（Ⅱ） nitrate and 1,3,5- benzenetricarboxylic（BTC） acid in a mixed solvent of N,N-dimethylformamide（DMF）/C2H5OH/ H2O （1：1：1, ν/ν） at low temperature and short reaction time. It was characterized by thermo- gravimetric analyses （TG）, FT-IR and N2 adsorption-desorption. Single-crystal X-ray diffraction analysis indicated that the complex belongs to monoclinic system, space group C2 with α = 17.407（6）, b = 12.878（5）, c = 6.542（2） A, β = 112.07°, V = 1359.0（8） A^3, Dc = 1.971 g/cm3, μ = 2.166 mm^-1 and Z = 2. Linear polarization resistance （LPR） analysis showed that the complex possesses semiconducting properties.

关键词： metal-organic framework solvothermal synthesis, mixed solution semiconducting properties

A smart photodynamic therapy strategy: depletion of glutathione in cancer cells

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science Bulletin 2017年第5期62卷 312-313页

作者： Fujian Huang Fan Xia Faculty of Material Science and Chemistry China University of Geosciences Hubei Key Laboratory of Bioinorganic chemistry & Materia Medica School of Chemistry and Chemical EngineeringHuazhong University of Science and Technology

Photodynamic therapy(PDT)is a promising cancer treatment method with fewer side effects,minimal invasion and low toxicity compared with other traditional cancer therapy methods,such as radiotherapy,chemotherapy and su... 详细信息

关键词： PDT depletion of glutathione in cancer cells A smart photodynamic therapy strategy