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Chinese Journal of Catalysis 2019年第2期40卷 168-176页

作者： Yanan Liu Liubo Ma Congcong Shen Xin Wang Xiao Zhou Zhiwei Zhao Anwu Xu Division of Nanomaterials and Chemistry Hefei National Laboratory for Physical Sciences at MicroscaleDepartment of Chemistry PhysicsUniversity of Science and Technology of ChinaHefei 230026AnhuiChina College of Biological Chemical Science and Engineering Jiaxing UniversityJiaxing 314001ZhejiangChina

Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low *** this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption *** VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good *** optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure *** role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs *** is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.

关键词： VOPc/g-C3N4 π-πinteraction Visible light photocatalysis Hydrogen evolution Charge separation efficiency

Boosting CO_(2) electroreduction performance over fullerene-modified MOF-545-Co promoted by π –π interaction

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Chinese Chemical Letters 2023年第4期34卷 559-563页

作者： Xue Dong Zhifeng Xin Dong He Jia-Ling Zhang Ya-Qian Lan Qian-Feng Zhang Yifa Chen Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa’anshan 243002China National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Key Lab.of ETESPG(GHEI)School of ChemistrySouth China Normal UniversityGuangzhou 510006China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread applications. Herein, fullerene molecules(i.e., C60and C70) have been successfully introduced into the pore-channels of a Co-porphyrin based MOF through a facile strategy. Thus-obtained hybrid materials present higher electron-transfer ability, enhanced CO_(2)adsorption-enthalpy and CO_(2)electroreduction activity. Notably, the charge transfer resistance(Rct) of C60@MOF-545-Co is almost 5 times lower of than that of MOF-545-Co, as well as 1.5 times increased for the CO_(2)adsorption enthalpy. As expect, the FECO of C60@MOF-545-Co(97.0%) is largely higher than MOF-545-Co(70.2%), C60@MOF-545(19.4%), C60(11.5%)and physical mixture(70.3%) and presented as one of the best CO_(2)electroreduction catalysts reported in H-cell system. The facile strategy would give rise to new insight into the exploration of powerful MOFbased hybrid materials in high-efficiency CO_(2)electroreduction.

关键词： Fullerene Metal organic framework Electrocatalytic performance π-πinteraction CO_(2)RR

Conjugated polymerized bimetallic phthalocyanine based electrocatalyst with Fe-N_(4)/Co-N_(4) dual-sites synergistic effect for zinc-air battery

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Journal of Energy Chemistry 2023年第11期86卷 41-53,I0002页

作者： Shuaifeng Wang Zhongfang Li Wenjie Duan Peng Sun Jigang Wang Qiang Liu Lei Zhang Yanqiong Zhuang School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255049ShandongChina

The bifunctional oxygen catalyst is essential for zinc-air batteries(ZABs).Here,an efficient bifunctional oxygen catalyst,PPcFeCo/3D-G,is obtained throughπ-πinteraction between the conjugated polymerized iron-cobalt phthalocyanine(PPcFeCo)with excellent thermal stability and three-dimensional graphene(3D-G).The bimetallic synergistic effect of PPcFeCo,verified by DFT(Density functional theory)calculation,andπ-πinteractions enhances the catalytic activity and durability of the PPcFeCo/*** electrochemical performance,the PPcFeCo/3D-G with a high electron transfer number(3.98,@0.768 V ***)has excellent half-wave potential(E_(1/2)=0.890 V ***)and exhibits outstanding reversibility(ΔE=0.700 V,ΔE=Ej=10-E_(1/2)).The liquid ZAB(LZAB)employed PPcFeCo/3D-G displays a high power density(222 m W cm^(-2)),a specific capacity(792 m A h g-1),and excellent durability(120 h).This work has guiding significance for the preparation of high-efficiency bifunctional catalysts.

关键词： Zn-airbattery Bifunctional oxygen catalysts Polymerized iron-cobalt phthalocyanine Bimetallic synergy π-πinteraction

Functional Amphiphilic Poly(2-oxazoline)Block Copolymers as Drug Carriers:the Relationship between Structure and Drug Loading Capacity

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Chinese Journal of Polymer Science 2021年第7期39卷 865-873页

作者： Si Dong Sheng Ma Zhi-Lin Liu Li-Li Ma Yu Zhang Zhao-Hui Tang Ming-Xiao Deng Wan-Tong Song College of Chemistry Northeast Normal UniversityChangchun 130024China Key Laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Poly(2-oxazoline)(POx)is a kind of polymeric amides that can be viewed as conformational isomers of polypeptides with excellent cyto-and hemo-compatibility,and is promising to be used as drug ***,the drug loading capacity(DLC)of POx for many drugs is still low except several hydrophobic ones including paclitaxel(PTX).Herein,we prepared a series of amphiphilic POx block copolymers with various functional groups,and investigated the relationship between functional structures and the *** POxs with benzyl,carboxyl,and amino groups in the side-chain were synthesized based on a poly(2-methyl-2-oxazoline)-block-poly(2-buty1-2-oxazoline-co-2-buteny1-2-oxazoline)(PMeOx-P(nBuOx-co-ButenOx),PMBEOx)precursor,followed by click reaction between vinyl and the 2-phenylethanethiol,thioglycolic acid and *** thin-film hydration method,eight commonly used drugs with various characteristics were encapsulated within these functional POx *** found that amine-containing drugs were more easily encapsulated by POx with carboxyl groups,while amine functionalities in POx enhanced the loading capacity of drugs with carboxyl *** addition,n-n interactions resulted in enhanced DLC of most drugs,except several hydrophobic drugs with aromatic to total carbon ratios less than *** general,we could successfully encapsulate all the selected drugs with a DLC%over 10%using properly selected functional *** above results confirm that the DLC of polymeric carriers can be adjusted by modifying the functional groups,and the prepared series of functional POxs provide an option for various drug loadings.

关键词： Poly(2-oxaozoline) Polymeric micelles Drug loading π-πinteraction Electrostatic interaction

Strong and tough graphene papers constructed with pyrene-containing small molecules via π-π/Hbonding synergistic interactions

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Science China Materials 2021年第5期64卷 1206-1218页

作者： Hong Yuan Liangbing Ge Kun Ni Xiukai Kan Si-Ming Chen Mengting Gao Fei Pan Jianglin Ye Fang Xu Na Shu Jieyun Li Tao Suo Shu-Hong Yu Yanwu Zhu Hefei National Laboratory for Physical Sciences at the Microscale&CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and EngineeringiChEMUniversity of Science and Technology of ChinaHefei 230026China Division of Nanomaterials and Chemistry Hefei National Laboratory for Physical Sciences at the MicroscaleCAS Center for Excellence in NanoscienceHefei Science Center of CASCollaborative Innovation Center of Suzhou Nano Science and TechnologyDepartment of ChemistryUniversity of Science and Technology of ChinaHefei 230026China School of Aeronautics Northwestern Polytechnical UniversityXi’an 710072China

Lightweight yet strong paper with high toughness is desirable especially for impact protection. Herein we demonstrated electrically conductive and mechanically robust paper(AP/PB-GP) made of reduced graphene oxide via interfacial crosslinking with 1-aminopyrene(AP) and 1-pyrenebutyrat(PB) small molecules. The AP/PB-GP with thickness of over ten micrometer delivers a record-high toughness(~69.67 ± 15.3 MJ m^(-3) in average), simultaneously with superior strength(close to 1 GPa), allowing an impressive specific penetration energy absorption(~0.17 MJ kg^(-1)) at high impact velocities when used for ballistic impact protection. Detailed interfacial and structural analysis reveals that the reinforcement is synergistically determined by π-π interaction and H-bonding linkage between adjacent graphene lamellae. Especially, the defective pores within the graphene platelets benefit the favorable adsorption of the pyrene-containing molecules, which imperatively maximizes the interfacial binding, facilitating deflecting crack and plastic deformation under loading. Density functional theory simulation suggests that the coupling between the polar functional groups, e.g., –COOH, at the edges of graphene platelets and –NH_(2) and –COOH of AP/PB are critical to the formation of hydrogen bonding network.

关键词： graphene paper π-πinteraction H-bonding synergistic reinforcement mechanical properties

Synthesis and Crystal Structure of a New Chain Coordination Polymer [Cu(inio)_2(H_2O)]_∞(Inio = Isonicotinic Acid N-Oxide)

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Chinese Journal of Structural Chemistry 2003年第4期22卷 415-418页

作者：李秀玲陈久桐牛德仲盛居廷张大鹏 Department of Chemistry Xuzhou Normal University Xuzhou 221116 China Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences Fuzhou 350002 China

A new Cu(Ⅱ) coordination polymer [Cu(inio)2(H2O)] (inio = isonicotinic acid N-oxide) with chemical formula C12H10CuN2O7 was prepared and its crystal structure has been determined by X-ray analysis. The complex crystallizes in the monoclinic system, space group C2/c with a = 12.455(3), b = 6.202(1), c = 16.555(3) ? b = 106.776(3), V = 1224.3(4) 3, Z = 4, Mr = 357.76, Dc =1.941 g/cm3, m(MoKa) = 1.827 mm-1, F(000) = 724, R = 0.0601 and wR = 0.1417 for 908 observed reflections (I > 2s(I)). The Cu(Ⅱ) atom is coordinated by an elongated square pyramid geometry. The deprotonated isonicotinic acid N-oxides form a double-bridge between each pair of Cu(Ⅱ) ions in trans form through two oxygen atoms from the carboxyl groups and two other oxygen atoms from the -NO groups, respectively, which leads to an infinite one dimensional chain. The two adjacent elongated Cu(Ⅱ) square pyramidal geometries are arranged in trans form in the same chain. The OH…O hydrogen bonds extend the chain structure into two-dimensional layers.

关键词： crystal structure copper isonicotinic acid N-oxide elongated square pyramid hydrogen bond π-πinteraction

Iron-doping Accelerating NADH Oxidation over Carbon Nitride

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Chemical Research in Chinese Universities 2020年第6期36卷 1076-1082页

作者： ZHANG Yuanyuan HUANG Xiaohua LI Jiashu LIN Gang LIU Wengang CHEN Zupeng LIU Jian College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042P.R.China College of Chemical Engineering Nanjing Forestry UniversityNanjing 210037P.R.China

As a state-of-the-art conjugated polymer photocatalyst,graphitic carbon nitride(abbreviated as g-C3Na)has shown sreat potential in photocatalvtic cofactor(reduced form of nicotinamide adenine ***)***,Fe-doped g-CaNa was engineered for photocatalvtic NADH *** n-r interaction between the NADH molecule and the conjugated heptazine buildine block facilitates the adsorption of NADH onto the framework as revealed by density functional theory(DFT)calculations,Furthermore,iron doping promoted the oxidation kinetics of NADH under blue LED *** conversion ratio of NADH to its oxidized form could be up to 85.7%in 20 min,comparing with 59.4%for metal-free *** assay employing formate dehydrogenase(FDH)further verified the selectivity of the products,with 67.5%+2.6%of enzymatically active 1,4-NADH being regenerated following the oxidation *** experiments suggest the dominant role of photo-induced electrons in theoxidation of *** work could shed light on developing a novel cofactor regeneration route through the syner-gistic effect between the metal doping and noncovalent interaction based on the coniugated polymer.

关键词： Cofactor regeneration NADH oxidation Photocatalysis Carbon nitride π-πinteraction

Precisely Controlled Two-Dimensional Rhombic Copolymer Micelles for Sensitive Flexible Tunneling Devices

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CCS Chemistry 2021年第5期3卷 1399-1409页

作者： Liang Han Hua Fan Yulin Zhu Meijing Wang Feng Pan Dapeng Yu Yue Zhao Feng He Department of Chemistry Shenzhen Grubbs InstituteSouthern University of Science and TechnologyShenzhen 518055 Department of Physics Institute for Quantum Science and EngineeringSouthern University of Science and TechnologyShenzhen 518055 School of Advanced Materials Shenzhen Graduate SchoolPeking UniversityShenzhen 518055 Guangdong Provincial Key Laboratory of Catalysis Southern University of Science and TechnologyShenzhen 518055

Nanoscale two-dimensional(2D)organic materials have attracted significant interest on account of their unique properties,which result from their ultrathin and flat *** 2D nanomaterials prepared by bottom-up approaches have great potential in the creation of nanoscale devices with various applications,each controlled by the properties of its single-molecular ***,we report a uniform and controllable 2D rhombic micelles formed by block copolymers(BCPs)with poly(p-phenylenevinylene)(PPV)as core *** supramolecular 2D nanostructures created in this way and driven byπ-πinteractions realize the precise separation of the semiconducting and insulating constituents of the constructed *** a vertical tunneling device design,the 2D rhombic micelles exhibited an on-off current ratio of>10^(4)and a high on-state current density of 6000 A cm^(−2)as the insulating layer was compressed by a conductive atomic force microscopy(C-AFM)*** tunneling device also shows a reproducible sensitivity on a flexible substrate,opening up potential flexible pressure sensor applications for such novel supramolecular 2D nanostructures.

关键词： block copolymer 2D self-assembly π-πinteraction controllable self-assembly tunneling device pressure sensor