| 双核铁肟硼酸基多孔金属有机聚合物的合成、结构及其电催化析氧性能 |
| Binuclear Iron Oxime Boric Acid Based Metal-Containing Porous Organic Polymer: Synthesis, Structure and Electrocatalytic Oxygen Evolution Properties |
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| 摘要: 采用氯化亚铁、2，6-二甲酰基-4-甲基苯酚二肟（H3DFMP）和四（4-硼酸基苯基）甲烷（TBPM），通过一步配位作用和硼酸酯化脱水聚合反应，合成了一例含金属的三维多孔有机聚合物（Fe2-POP）。Fe2-POP是以双核亚铁配位H3DFMP的直线单元与TBPM的四面体单元连接而成的具有三维金刚石结构的多孔有机聚合物。对模型化合物的X射线单晶衍射分析验证了双核亚铁配合物单元的结构特征。红外光谱和固体核磁表征证明了Fe2-POP中C=N和B-O键的形成。Fe2-POP具有较高的比表面积（510 m2·g-1）和均一的孔径（0.6~0.8 nm）。X射线光电子能谱表明了Fe2-POP中二价铁的存在。扫描电子显微镜和透射电子显微镜显示该聚合物是由50~100 nm的球形颗粒组成。电化学测试表明，Fe2-POP展现出了优异的电催化析氧性能，在10 mA·cm-2电流密度下所需析氧反应过电位仅为258 mV，Tafel斜率为71.0 mV·dec-1。 |
| 关键词: 双核铁 多孔有机聚合物 硼酸酯化脱水聚合 电催化 析氧反应 |
| 基金项目: 国家自然科学基金（No.22075108，21771089，21905116）和江苏省自然科学基金资助项目（No.BK20190614）资助。 |
| Abstract: A three-dimensional metal-containing porous organic polymer (Fe2-POP) was synthesized using ferrous chloride, 2, 6-diformyl-4-methylphenol dioxime (H3DFMP) and tetra(4-(dihydroxy)borylphenyl)methane (TBPM) through one-step coordination and boric acid esterification dehydration polymerization reaction. Binuclear iron as the linear unit was formed by coordination between iron ion and H3DFMP, while TBPM was used as the tetrahedral linking unit, so that the three-dimensional porous organic polymer Fe2-POP with dia topology was produced. X-ray single crystal diffraction analysis of the model compound (MC-1) verified the structural characteristics of the dinuclear ferrous unit. Infrared spectroscopy and solid-state nuclear magnetism characterizations proved the formation of C=N and B-O in Fe2-POP. Fe2-POP had a high specific surface area of 510 m2·g-1 and uniform pore size (0.6-0.8 nm). X-ray photoelectron spectroscopy indicated the presence of divalent iron in Fe2-POP. Scanning electron microscopy and transmission electron microscopy showed that Fe2-POP was composed of 50-100 nm sphere-shaped particles. Electrochemical tests showed that Fe2-POP exhibited excellent electrochemical properties towards oxygen evolution reaction, and it only needed a small overpotential of 258 mV to deliver a current density of 10 mA·cm-2, and the Tafel slope was 71.0 mV·dec-1. |
| Keywords: binuclear iron porous organic polymers boric acid esterification dehydration polymerization electrocatalysis oxygen evolution reaction |
| 投稿时间：2021-06-18 修订日期：2021-09-27 |
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| 石亚翔,张文达,方欣,晏晓东,顾志国.双核铁肟硼酸基多孔金属有机聚合物的合成、结构及其电催化析氧性能[J].无机化学学报,2021,37(12):2193-2202. |
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