期刊：
Journal of Colloid and Interface Science,2024年678(Pt B):88-94 ISSN：0021-9797
通讯作者：
Yan, Juntao;Sun, Lin-Bing
作者机构：
[Wang, Yang; Peng, Song-Song; Tan, Peng; Liu, Sai; Shao, Xiang-Bin; Liu, Yang; Zhang, Kai] State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, 30 South Puzhu Road, Nanjing 211816, China;[Yan, Juntao] College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China. Electronic address: yanjuntaonihao@163.com;[Sun, Lin-Bing] State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, 30 South Puzhu Road, Nanjing 211816, China. Electronic address: lbsun@njtech.edu.cn
通讯机构：
[Yan, Juntao] C;[Sun, Lin-Bing] S;College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China. Electronic address:;State Key Laboratory of Materials-Oriented Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), College of Chemical Engineering, Nanjing Tech University, 30 South Puzhu Road, Nanjing 211816, China. Electronic address:
关键词：
Basic sites;Ca single atoms;Metal-organic frameworks;Single-atom solid base catalysts
摘要：
Considerable attention has been paid to the preparation of single-atom solid base catalysts (SASBCs) owing to their high activity and maximized utilization of basic sites. At present, the reported fabrication methods of SASBCs, such as two-step reduction strategy and sublimation capture strategy, require high temperature. Such a high activation temperature is easy to cause the sublimation loss of alkali or alkaline earth metal atoms and destructive to the support structure. Herein, a new SASBC, Ca(1)/UiO-67-BPY, is fabricated, in which the alkaline earth metal Ca sites are immobilized onto N-rich metal-organic framework UiO-67-BPY at room temperature. The results show that the atomic configuration of Ca single atoms is coordinated by two N atoms in the framework. The obtained Ca SASBC possesses ordered structure and exhibits high product yield of 87.2% in the Knoevenagel reaction between benzaldehyde and malononitrile. Furthermore, thanks to the Ca single atoms sites anchored on UiO-67-BPY, the Ca(1)/UiO-67-BPY catalyst also shows good stability during cycles. This work might offer new insight in designing SASBCs for different base-catalyzed reactions.
摘要：
本文通过3,3′-((乙基-1,2-二基双((吡啶-2-甲基)杂氮二基))双亚甲基)二(2-羟基-5-甲基苯甲醛)(H2L)和丙二胺在金属离子存在条件下的缩合反应, 得到了一个新型3-甲基吡啶悬臂Cu(II)-Zn(II)异双核配合物, 并通过红外光谱、紫外光谱、电喷雾质谱、X射线单晶衍射等手段对其结构进行了表征。单晶衍射结果表明该配合物属于六方晶系, P63/m空间群, a=1.982 18(17) nm,b=1.982 18(17) nm,c=1.839 4(2) nm, 分子式为C37H41CuN6O4Zn。金属中心Cu(II)和Zn(II)由两个酚氧原子和一个醋酸根桥联, 它们的配位环境都可以近似地看作为四方锥结构, Cu(II)和Zn(II)之间的距离是0.289 7 nm。本文还利用循环伏安实验和黏度实验的方法对该配合物与小牛胸腺DNA(CT-DNA)的相互作用模式进行了研究, 结果表明该配合物与CT-DNA的结合方式为弱的插入模式, 其相应的结合活性为6.92×103 mol/L。 A new 3-methylpyridyl pendant-arms Cu(II)-Zn(II) hetero-binuclear complex was synthesized by condensation reaction of 3,3′-((ethane-1,2-diylbis((pyridin-2-ylmethyl)azanediyl))bis(methylene))bis(2-hydroxy-5-methylbenzaldehyde) (H2L) and propane diamine in the presence of metal ions. The structure was characterized by IR spectroscopy, UV-Vis spectroscopy, ES-MS spectroscopy and X-ray single-crystal diffraction. The crystal structure reveals that the complex crystallizes in hexagonal, space group P63/m, with a=1.982 18(17) nm, b=1.982 18(17) nm and c=1.839 4(2) nm. The coordination environment of Zn(II) and Cu(II) in complex can be described as approximately square pyramid, where the apical positions are occupied by acetate radical. Two metal centers are equivalently bridged by the phenolic oxygens and an acetate radical with the intermetallic separation of 0.289 7 nm. The interaction between the complex and calf thymus DNA (CT-DNA) was measured by cyclic voltammetry and viscosity studies, which shows a weak binding activity of 6.92×103mol/L.
通讯机构：
Sichuan Institute of Product Quality Supervision and Inspection, Chengdu, China
关键词：
双核锰配合物;大环金属配合物;晶体结构;DNA结合能力
摘要：
通过3，3′-((乙烷-1，2-二基双(2-甲基吡啶杂氮二基)双(亚甲基))双(2-羟基-5-甲基苯甲醛)与2-羟基-1，3-丙二胺的缩合反应得到一种具有双吡啶悬臂的双核锰配合物。通过X射线单晶衍射确定了该配合物结构，结果显示其分子式为［Mn2(C37H43N6O6)］·(ClO4)2。该配合物属于单斜晶系，P21/c空间群，晶胞参数为：a=1.096 50(19) nm, b=1.419 5(3) nm, c=3.109 4(5) nm, β=108.153(5)°。进一步分析表明两个二价锰离子分别与(Namine)2(Nimine)2O3和(Nimine)2O4体系配位，它们与配位原子形成的几何构型分别是十面体和扭曲的八面体。两个中心锰离子距离为0.331 6 nm，由酚氧原子和醋酸根共同桥联。另外，本文也利用伏安法和黏度法对该配合物与小牛胸腺DNA的结合能力进行研究，实验结果表明它们之间的结合方式为弱的插入作用。 A new dinuclear manganese(Ⅱ) complex with bis-pyridine pendant-arms was synthesized by condensation between 3,3′-((ethane-1,2-diylbis((pyridin-2-ylmethyl)azanediyl)) bis(methylene))bis(2-hydroxy-5-methylbenzaldehyde) and 2-hydroxy-1,3-diaminopropane in the presence of manganese(Ⅱ). The complex was determined by X-ray diffraction single crystal structure analysis, and the corresponding formula is ［Mn2(C37H43N6O6)］·(ClO4)2. The results indicate that the complex crystallizes in monoclinic, space group P21/c, with a=1.096 50(19) nm, b=1.419 5(3) nm, c=3.109 4(5) nm, β=108.153(5)°. The crystal structure shows that the two manganese(Ⅱ) ions in the phenolbased macrocyclic dinuclear complex are coordinated with (Namine)2(Nimine)2O3 and (Nimine)2O4 sites, the corresponding geometry around each manganese(Ⅱ) center are decahedron and distorted octahedron. Two manganese(Ⅱ) centers are equivalently bridged by the phenolic oxygens and an acetate radical with the intermetallic separation of 0.331 6 nm. Moreover, the binding ability of the complex toward calf thymus DNA were analyzed by voltammetric and viscosity method, which indicate the bonding mode between them is weak intercalation.
作者机构：
[闫俊涛; 寇慧芝; 王洋] School of Chemical and Environmental Engineering, Wuhan Polytechnic University, Wuhan, 430023, China;[杨术明] College of Chemistry and Chemical Engineering, Xinyang Normal University, Xinyang, Henan 464000, China
通讯机构：
[Yan, J.] S;School of Chemical and Environmental Engineering, China
关键词：
disulfide;lithium;molybdenum complex;molybdenum disulfide;nanorod;nanotube;unclassified drug;Article;cyclic potentiometry;high resolution transmission electron microscopy;lithiation;nanofabrication;precursor;priority journal;scanning electron microscopy;surface property;synthesis;X ray diffraction
摘要：
MoS2 with a 2D layered structure and high theoretical capacity has been regarded as a promising candidate for anode materials in lithium ion batteries. But its poor cyclic stability and low rate capability hinder its practical applications. Herein, hierarchical MoS2 nanotori consisting of MoS2 nanosheets with an increased interlayer distance were synthesized by a facile hydrothermal reaction for the first time. A possible formation mechanism of the hierarchical MoS2 nanotori is proposed based on the scanning electronic microscopy (SEM) results and the influence of the MoO3 precursor on the morphology of the MoS2 obtained. The hierarchical MoS2 nanotori display superior reversible capacity, good rate capability and improved cyclic performance, which can be attributed to their hierarchical surface, hollow structure feature and increased layer distance. The formation mechanism of hierarchical MoS2 nanotori proposed here should offer a new technique for the design and synthesis of MoS2 with different morphologies using MoO3 as the growth template.
关键词：
5-Hydroxymethyl furfural;Cellulose;Glucose;Phosphotungstic acid;Two-step process
摘要：
The synthesis of 5-hydroxymethyl furfural (HMF) from cellulose via a two-step process was investigated. To optimize reaction conditions, the separate conversion of cellulose and glucose was first performed in tetrahydrofuran (THF) and N, N-dimethylformamide (DMF) via a one-step process using hosphotungstic acid (PHA) as catalyst. The direct conversion of cellulose to HMF was then performed via the two-step process. The first step and the second step were carried out in THF and the mixture solvent composed of THF/DMF, respectively. Cellulose was converted to HMF and glucose in the first step in THF. Both of cellulose and the as-formed glucose were then converted to HMF in the second step. The conversion of cellulose to HMF and glucose were significantly improved by the two-step process, and the total yield of HMF and glucose was elevated from 52.1 to 97.0%. A possible mechanism for the formation of HMF from cellulose via the two-step process was also proposed.
摘要：
The hollow Co9S8 nanospheres with ca. 50 nm were elaborately fabricated by a facile solvothermal method and characterized by powder X-ray diffraction (XRD), Scanning electron microscopy (SEM) and BET measurement to result in a specific surface area of 226 m(2) g(-1). The prepared hollow Co9S8 nanosphere electrode delivers a initial specific capacitance of 234.7 F g(-1) at a current density of 0.5 A g(-1), which can be retained up to the 60th cycle, indicating the good cycleability and excellent rate capability. As a consequence, the energy density of the prepared Co9S8 pseudocapacitor could reach up to 17.96 Wh kg(-1) at a power density of 32.82 W kg(-1), which is much more than those of common electric double capacitors, exhibiting the pseudocapacitive characteristic. This might be due to the unique hollow Co9S8 nanosphere structure to shorten the path of the electron transportation and the ionic diffusion.
