Syntheses, Crystal Structure, Characterization and Properties of Two Novel Superamolecular Phosphotungstate-Pyriding Complexes
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Two new inorganic-organic compounds constructed from phosphotungstate and pyridines have been synthesized under hydrothermal conditions. The formula of two compounds are (C<sub>5</sub>H<sub>7</sub>N<sub>2</sub>)<sub>3</sub>(C<sub>5</sub>H<sub>6</sub>N<sub>2</sub>)<sub>3</sub>(PW<sub>12</sub>O<sub>40</sub>)·2H<sub>2</sub>O (<b>1</b>), (C<sub>6</sub>H<sub>8</sub>N)<sub>3</sub>(C<sub>6</sub>H<sub>7</sub>N)(PW<sub>12</sub>O<sub>40</sub>)·9H<sub>2</sub>O (<b>2</b>). They have been characterized by IR, UV-vis, TG-DTA, FL, CV and single-crystal X-ray diffraction. The two compounds are both show three-dimensional network. These compounds exhibit good catalytic activity for catalytic oxidation of methanol over a continuous-flow fixed-bed micro-reactor, when the initial concentration of methanol is 5.37 g×m<sup>−3</sup>, and flow rate is 4.51 mL×min<sup>−1</sup>. 0.2 g compound <b>1 (or</b> compound <b>2)</b> as the catalyst can eliminates methanol completely at 150 °C (175 °C for compound <b>2</b>).
本研究通过水热合成法制备了两种由磷钨酸盐(phosphotungstate)与吡啶类配体构筑的无机-有机杂化化合物。两种化合物的分子式分别为(C₅H₇N₂)₃(C₅H₆N₂)₃(PW₁₂O₄₀)·2H₂O(1)与(C₆H₈N)₃(C₆H₇N)(PW₁₂O₄₀)·9H₂O(2)。采用红外光谱(Infrared Spectroscopy, IR)、紫外-可见吸收光谱(Ultraviolet-Visible Spectroscopy, UV-vis)、热重-差热联用分析(Thermogravimetry-Differential Thermal Analysis, TG-DTA)、荧光光谱(Fluorescence Spectroscopy, FL)、循环伏安法(Cyclic Voltammetry, CV)以及单晶X射线衍射对上述化合物进行了结构表征。两种化合物均呈现三维网状结构。在连续流固定床微反应器中,当甲醇初始浓度为5.37 g·m⁻³、气流流速为4.51 mL·min⁻¹时,该类化合物对甲醇催化氧化反应展现出良好的催化活性:以0.2 g的化合物1(或化合物2)作为催化剂时,可在150 ℃(化合物2则需175 ℃)下完全去除体系中的甲醇。
提供机构:
Cheng, Yang; Zhang, Chuan-Lei; Han, Yu-Zhe; Cai, Qing; Ai, Si-Xia; Deng, Qian
创建时间:
2015-10-17



