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Carboxylate-induced Various Structures of Ni(II) Complexes with Fluorescence Sensing and Bifunctional Electrochemical Properties

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Chemical Research in Chinese Universities 2019年第4期35卷 549-555页

作者： LU Xue LIU Guocheng WANG Xiang lin hongyan WANG Xiuli Liaoning Province Silicon Materials Engineering Technology Research Centre Department of Chemistry Bohai University Jinzhou 121013P. R. China

We synthesized three new Ni(II) coordination polymers [Ni(LXHLPXH2O)2]- H2O(CP1),[Ni(LXNIP)]-2H2O(CP2) and [Ni(LXNDCXH20)2](CP3)[L=N,N′-bis(pyridme-3-yl)thiophene-2,5-dicarboxamide, H2HIP=5-hydroxyisophthalic acid, H2NIP=5-nitroisophthalic acid, H2NDC=2,6-naphthalenedicarboxylie acid] by hydrothermal method, which were characterized by means of infrared spectra(IR), TG analyses, PXRD and single-crystal X-ray diffraction. The CPI is a ID tubular structure based on [Ni-HIP]2 loops and pairs of L ligands. CP2 is a 2D 3,5-connected architecture, which consists of Ni-L linear chains and (Ni-NIP)2 double chains. CP3 is a 2D network, which features 4-connected topology. Solid-state luminescent behaviours of CP-P3 were investigated. The CPI can detect Fe^3+ ions through luminescence quenching. The electrochemical properties of CPI buk-modified carbon paste electrode(CP1-CPE) has also been investigated, which has bifunctional electrocatalytic activity for oxidation of ascorbic acid and reduction of NO2^-.

关键词： Carboxylate-induced Coordination polymer Fluorescent recognition Bifunctional electrocatalysis

Three Ni（II） Coordination Polymers with Various Architectures Based on Asymmetric Bis-pyridyl-amide and Polycarboxylates： Syntheses, Structures and Properties

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Chemical Research in Chinese Universities 2016年第5期32卷 719-724页

作者： WU Xiaomei LIU Guocheng WANG Xiuli SHAO Jiyan lin hongyan WANG Xiang Department of Chemistry Liaoning Province Silicon Materials Engineering Technology Research Centre Bohai University Jinzhou 121000 P. R. China

Three different dimensionalNi（II） coordination polymers, [Ni（3-pna）（HIP）（H2O）3]-H20（1）, [Ni（3-pna）- （1,3,5-HBTC）]（2） and [Ni2（H2O）（3-pna）2（1,4-CHDC）2]4（3）（3-pna=3-pyridylnicotinamide, H2HIP=5-hydroxyisoph- thalic acid, 1,3,5-H3BTC=l,3,5-benzenetricarboxylic acid, 1,4-H2CHDC=l,4-cyclohexanedicarboxylic acid）, were synthesized under hydrothermal conditions and characterized by means of infrared spectra（IR）, thermal gravimetric （TG） analyses, powder X-ray diffraction（PXRD） and single-crystal X-ray diffraction. Complex 1 has a structure of 1D single-stranded chain, which is further stretched by hydrogen-bond interactions to form a 2D supramolecular sheet. Complex 2 shows a 2D network, which is stretched to 3D supramolecular frameworks through hydrogen-bond interactions. Complex 3 reveals a 3D skeleton with a （3,3,6,6）-connected {3·72} {32·4 } {33·42·5·73·85·9 } {33·45·52·72·82·9} topology. The effects of different polycarboxylates on the ultimate architectures of the complexes 1--3 were dis- cussed. Furthermore, the fluorescent and photocatalytic properties of the title complexes were also investigated.

关键词： Crystal structure Dipyridylamide Polycarboxylate Photoluminescence property Photocatalytic property

Two New Inorganic-organic Hybrid Compounds Constructed from Different Polymolybdates and Transition Metal-amine Subunits

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Chemical Research in Chinese Universities 2015年第3期31卷 337-341页

作者： WANG Xiuli LIU Danna HAN Na lin hongyan LUAN Jian TIAN Aixiang Liaoning Province Silicon Materials Engineering Technology Research Centre Department of ChemistryBohai University Jinzhou 121000 P.R.China

Two new polyoxometalate（POM）-based hybrid compounds, [Cu（en）][H4Mo4O16]0.5（1）（en=ethylenediamine） and [Ag（3-CsH6N2）2][H2PMo12O40]（2）（3-C5H6N2=3-aminopyridine）, containing different transition metal- amine subunits were hydrothermally synthesized and characterized by elemental analyses, infrared spectroscopy and single-crystal X-ray diffraction. For compound 1, each [H4Mo4O16]4-（M04O16） cluster was linked to four neighboring Mo4O16 clusters through four [Cu（en）]2＋ subunits to yield a （2,4）-connected 2D layer, which was further extended to a 3D supramolecular network via hydrogen bonding interactions. For compound 2, the adjacent [H2PMo12O40]- clusters were bridged by [Ag（3-C5H6N2）2]＋ subunits to generate a 1D chain. The electrochemical behaviors and the photoca- talytic activities of compounds 1 and 2 were studied in detail.

关键词： Polyoxometalate Metal-amine unit Crystal structure Electrochemical property Photocatalysis

Homogeneity-Breaking Instability of Periodic Solutions of Gierer-Meindardt Model

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Journal of Harbin Institute of Technology(New Series) 2024年第2期31卷 62-67页

作者： Aying Wan Zhiqiang Song hongyan lin Nan Xiang Department of Science and Technology Hulunbuir UniversityHulun Buir 021008Inner MongoliaChina School of Engineering Hulunbuir UniversityHulun Buir 021008Inner MongoliaChina School of Mathematics and Physics Hulunbuir UniversityHulun Buir 021008Inner MongoliaChina

The homogeneity-breaking instability of the periodic solutions triggered by Hopf bifurcations of a diffusive Gierer-Meinhart system is studied in this *** conditions on the diffusion coefficients and the cross diffusi... 详细信息

关键词： Gierer-Meindardt model cross-diffusion homogeneity-breaking instability Hopf bifurcations

Polyoxometalate-based metal-organic complexes constructed from a new bis-pyrimidine-amide ligand with high capacitance performance and selectivity for the detection of Cr(Ⅵ)

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Chinese Chemical Letters 2022年第9期33卷 4389-4394页

作者： Qianqian Liu Junjun Lu hongyan lin Xiuli Wang Zhihan Chang Yongzhen Chen Yuchen Zhang College of Chemistry and Materials Engineering Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar CellBohai UniversityJinzhou 121013China

In this paper,three new polyoxometalates(POM)-based metal–organic complexes constructed from a new semi-rigid organic ligand N,N'-bis(4-pyrimidinecarboxamido)-1,2-cyclohexane(4-bpmah)H_(2)[Cu(4-bpmah)_(2)(SiMo_(12)O_(40))(H_(2)O)_(2)]·2H_(2)O(1),H[Cu(4-bpmah)_(2)(PMo_(12)O_(4)0)(H_(2)O)_(2)]·2H_(2)O(2)and[Cu(4-bpmah)(H_(2)O)_(2)]·[Cu_(2)(TeMo_(6)O_(24))(H_(2)O)_(10)]·4H_(2)O(3)were synthesized by hydrothermal *** crystal X-ray analyses showed that complexes 1 and 2 were isostructural,in which the isolated Keggin-type[SiMo1_(2)O_(40)]^(4–)/[PMo_(12)O_(40)]^(3–)anions and[Cu(4-bpmah)_(2)(H_(2)O)2]^(2n+)units were expanded into 3D supramolecular structures through hydrogen bond *** complex 3,the 1D[Cu(4-bpmah)(H_(2)O)_(2)]^(2n+)metal–organic chains and isolated[Cu_(2)(TeMo_(6)O_(24))(H_(2)O)_(10)]^(2n–)units were expanded into a 3D supramolecular framework by the hydrogen bond *** this paper,carbon cloth working electrodes composited by the title complexes(1/CC,2/CC and 3/CC)were prepared and used as electrodes for *** performance of supercapacitors as well as the influence of electrolyte solution and title complexes quality load on the performance of supercapacitors were ***,the electrochemistry and electrocatalytic behaviors of complexes 1–3 bulk-modified carbon paste electrodes(1-CPE,2-CPE and 3-CPE)toward the reduction of KBrO_(3),KNO_(2),Cr(Ⅵ),as well as their sensing behaviors on Cr(Ⅵ)were investigated.

关键词： Polyoxometalates Metal–organic complexes Supercapacitor Electrocatalysis Electrochemical sensors

Substituent groups from aromatic dicarboxylates modulated structural diversification in the assembly of Co(Ⅱ)complexes based on the bis-pyridyl-bis-amide ligands

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Science China Chemistry 2013年第5期56卷 557-566页

作者： WANG XiuLi MU Bao lin hongyan YANG Song LIU GuoCheng TIAN AiXiang ZHANG JuWen Department of Chemistry Bohai University

Four coordination polymers based on two bis-pyridyl-bis-amide ligands and three aromatic dicarboxylates with different substituent groups, namely, [Co（3-bpcb）x.5（NPH）（H20）]＂ 4H20 （1）, [Co（3-bpcb）（NIPH）] （2）, [Co（3-bpcb）0.5（5-H2AIP）]＂ 2H20 （3）, [Co（3-bpcd）0.5（5-H2AIP）（H20）]＂ 2H20 （4） [3-bpcb = N,N＇-bis（3-pyridinecarboxamide）-l,4-benzene, 3-bpcd = N,N＇-bis（3- pyridine）cyclohexane-l,4-dicarboxamide, H2NPH = 3-nitrophthalic acid, H2NIPH = 5-nitroisophthalic acid, 5-HaAIP = 5-aminoisophthalic acid] have been synthetized under hydrothermal conditions. Complex 1 displays a one dimensional （1D） chain based on the binuclear [Co2（NPH）2] units and 3-bpeb ligands, which is extended into a three dimensional （3D） supra- molecular framework through hydrogen bonding and n-n stacking interactions. In complex 2, the （3,5）-connected two dimen- sional （2D） layers are constructed from 1D Co-NIPH chains and bidentate-bridging 3-bpeb ligands. Complex 3 is a 2D double layer based on Co-5-H2AIP 2D layers and 3-bpeb pillars. Complex 4 also displays a 2D network, which is constructed from the Co-5-H2AIP 1D double chains and 3-bpcd ligands. Finally, complexes 2--4 are extended into 3D supramolecular frame- works by hydrogen bonding or n-re stacking interactions. The substituent groups of dicarboxylates play an important role in the assembly and structures of the title complexes. In addition, the fluorescent properties of complexes 1-4 and the electrochemi- cal behaviors of 3 and 4 at room temperature have been investigated.

关键词： coordination polymer bis-pyridyl-bis-amide ligand hydrothermal reaction fluorescent property

Effect of Reaction Conditions on the Assembly, Structures and Fluorescent Sensing Behaviors of Cd（II） Metal-organic Complexes

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Chemical Research in Chinese Universities 2016年第1期32卷 8-15页

作者： LE Mao LUAN Jian ZHAO Xunzhang TANG Tang CHEN Panwen LIU Guocheng lin hongyan Department of Chemistry Bohai University Jinzhou 121013 P. R. China

Three Cd（II） metal-organic complexes, namely [Cd（phen）2Cl2]（1）, [Cd（phen）Cl2]（2） and [Cd（phen）（cam）]. H2O（3）（phen=1,10-phenanthroline, H2cam=camphoric acid）, were hydrothermally synthesized using Cd2＋, phen and Hacam as raw materials under different conditions of pH values, reaction temperatures or reactant ratios. The prepared complexes were structurally characterized by means of single-crystal X-ray diffraction, and the results show that complex 1 is a 2D supramolecular complex, which consists of [Cd（phen）2Cl2] mononuclear subunits, while complex 2 shows a 1D chain structure, in which Cd（II） ions are connected by chloride（Cl ） bridges, with phen hanging on both sides of the chain. No cam anions have been observed in the structures of complexes 1 and 2. In complex 3, cam connects Cd（lI） ions to construct a 2D network, in which phen acts as terminal ligands. The adjacent 1D chains for complex 2 and the adjacent 2D layers for complex 3 are further linked by hydrogen bonding interac- tions or π-π intermolecular interactions to form 3D supramolecular networks, respectively. The effects of reaction conditions on the assembly and structures of the complexes have been discussed. The fluorescent and photocatalytic properties of complexes 1-3 and the fluorescent sensing behaviors of complexes 2 and 3 have also been investigated.

关键词： Cd(II) complex 1,10-Phenanthroline Camphanic acid Fluorescent sensing behavior Photocatalytic property

The structure of 4-hydroxylphenylpyruvate dioxygenase complexed with 4-hydroxylphenylpyruvic acid reveals an unexpected inhibition mechanism

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Chinese Chemical Letters 2021年第6期32卷 1920-1924页

作者： Xiaoning Wang hongyan lin Junjun Liu Xinyun Zhao Xi Chen Wenchao Yang Guangfu Yang Chang-guo Zhan College of Chemistry and Material Science South-Central University for NationalitiesWuhan 430074China Key Laboratory of Pesticide&Chemical Biology of Ministry of Education College of ChemistryCentral China Normal UniversityWuhan 430079China School of Pharmacy Tongji Medical College of Huazhong University of Science&TechnologyWuhan 430030China Department of Pharmaceutical Sciences College of PharmacyUniversity of KentuckyLexingtonKY 40536United States

4-Hydroxyphenylpyruvate dioxygenase(HPPD)is an important target for both drug and pesticide *** a typical Fe(II)-dependent dioxygenase,HPPD catalyzes the complicated transformation of 4-hydroxyphenylpyruvic acid(HPPA)to homogentisic acid(HGA).The binding mode of HPPA in the catalytic pocket of HPPD is a focus of research ***,we reported the crystal structure of Arabidopsis thaliana HPPD(At HPPD)complexed with HPPA and a cobalt ion,which was supposed to mimic the pre-reactive structure of At HPPD-HPPA-Fe(II).Unexpectedly,the present study shows that the restored At HPPD-HPPA-Fe(II)complex is still nonreactive toward the bound ***/MM and QM calculations reveal that the HPPA resists the electrophilic attacking of the bound dioxygen by the trim of its phenyl ring,and the residue Phe381 plays a key role in orienting the phenyl *** study on the F381 A mutant reveals that the HPPD-HPPA complex observed in the crystal structure should be an intermediate of the substrate transportation instead of the pre-reactive *** importantly,the binding mode of the HPPA in this complex is shared with several well-known HPPD inhibitors,suggesting that these inhibitors resist the association of dioxygen(and exert their inhibitory roles)in the same way as the *** present study provides insights into the inhibition mechanism of HPPD inhibitors.

关键词： 4-Hydroxyphenylpyruvate dioxygenase QM/MM calculation Potential surface scan Substrate self-inhibition

QM/MM study on the O_(2)activation reaction of 4-hydroxylphenyl pyruvate dioxygenase reveals a common mechanism forα-ketoglutarate dependent dioxygenase

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Chinese Chemical Letters 2023年第5期34卷 461-465页

作者： linhui Li Suitian Lai hongyan lin Xinyun Zhao Xin Li Xi Chen Junjun Liu Guangfu Yang Changguo Zhan College of Chemistry and Material Science South-Central Minzu UniversityWuhan 430074China Key Laboratory of Pesticide&Chemical Biology of Ministry of Education College of ChemistryCentral China Normal UniversityWuhan 430079China School of Pharmacy Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430030China Department of Pharmaceutical Sciences College of PharmacyUniversity of KentuckyLexingtonKY 40536United States

The dioxygen activation catalyzed by 4-hydorxylphenyl pyruvate dioxygenase(HPPD)were reinvestigated by using hybrid quantum mechanics/molecular mechanics(QM/MM)approaches at the B3LYP/6-311++G(d,p):AMBER *** studies showed that this reaction consisted of two steps including the dioxygen addition/decarboxylation and hetero O-O bond cleavage,where the first step was found to be *** former step initially runs on a septet potential energy surface(PES),then switches to a quintet PES after crossing a septet/quintet minimum energy crossing point(MECP)5-7M2,whereas the rest step runs on the quintet *** reliability of our theoretical predictions is supported by the excellent agreement of the calculated free-energy barrier value of 16.9 kcal/mol with available experimental value of 16-17 kcal/*** present study challenges the widely accepted view which holds that the O2activation catalyzed byα-keto glutamate(α-KG)dioxygenase mainly runs on the quintet PES and provides new insight into the catalytic mechanism ofα-KG dioxygenase and/or other related Fe(Ⅱ)-dependent oxygenase.

关键词： 4-Hydroxylphenyl pyruvate dioxygenase O_(2)activation QM/MM Mechanism Minimum energy crossing point