Preparation and Formation Mechanism of a n-Butylammonium/MnO2 Layered Hybrid via a One-Pot Synthesis under Moderate Condition
Preparation and Formation Mechanism of a n-Butylammonium/MnO2 Layered Hybrid via a One-Pot Synthesis under Moderate Condition
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温和条件下一锅合成正丁基铵/MnO2层状杂化物的制备及形成机理
DOI：
10.1039/c1dt11145k
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发表时间：
2012
期刊：
影响因子：
--
通讯作者：
Gunzi Saito
中科院分区：
文献类型：
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作者：
Kazuya Kai;Yukihiro Yoshida;Yoji Kobayashi;Hiroshi Kageyama;Gunzi Saito
有机/无机层状杂化物的制备依赖于多步骤加工。因此，缩短合成程序对于未来可能的应用非常重要，但只有少数研究报告了一锅合成。在这项工作中，我们建立了一种简单的一锅溶液法来合成层状烷基铵/MnO2杂化物，通过在40℃下搅拌MnCl2和烷基胺/H2O2水溶液；该反应概念是在烷基胺存在的水溶液中发生 Mn(II) 离子的化学氧化。此外，通过跟踪反应过程中的结构和光学变化，研究了层状正丁基铵/MnO2杂化物的形成机理，发现一锅反应包括3个步骤； β-MnOOH的形成，β-Mn(III)OOH的局部立构氧化形成质子化的层状氧化锰HxMn(III,IV)O2·yH2O，层间H+(或H3O+)与正丁基铵进行离子交换，形成层状正丁基铵/MnO2。
The preparation of organic/inorganic layered hybrids has relied on multistep processing. Thus, shortening the synthetic procedure is important for possible future applications, but only a few studies report one-pot syntheses. In this work, we established a simple one-pot solution process to synthesize layered alkyl ammonium/MnO2 hybrids, by stirring MnCl2 and alkyl amine/H2O2 aqueous solutions at 40 °C; the reaction concept is a chemical oxidation of Mn(II) ions in the presence of alkyl amine in aqueous solution. Furthermore, the formation mechanism of the layered n-butylammonium/MnO2 hybrid was examined by following the structural and optical changes during the reaction, revealing that the one-pot reaction includes 3 steps; formation of β-MnOOH, topotactic oxidation of β-Mn(III)OOH to form the protonated layered manganese oxide HxMn(III, IV)O2·yH2O, and ion-exchange of interlayer H+ (or H3O+) with n-butylammonium to form layered n-butylammonium/MnO2.