| 核壳结构Cu@CoW的合成和对硼氨配合物水解的催化性能 |
| Synthesis of Core/Shell Structured Cu@CoW Catalyst and Its Catalytic Properties for Hydrolysis of Ammonia Borane Aqueous Solution |
| 作者 | 单位 | E-mail | | 戴敏 | 南京大学介观化学教育部重点实验室, 南京大学化学化工学院, 南京 210093 | | | 沈晓晨 | 南京大学介观化学教育部重点实验室, 南京大学化学化工学院, 南京 210093 | | | 王青 | 南京大学介观化学教育部重点实验室, 南京大学化学化工学院, 南京 210093 | | | 王志斌 | 南京大学配位化学国家重点实验室, 南京大学化学化工学院, 南京 210093 | | | 赵斌 | 南京大学介观化学教育部重点实验室, 南京大学化学化工学院, 南京 210093 | binzhao@nju.edu.cn | | 丁维平 | 南京大学介观化学教育部重点实验室, 南京大学化学化工学院, 南京 210093 | |
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| 摘要: 分别以硼氨配合物和硼氢化钠为还原剂合成了核壳结构的Cu@CoW三元合金催化剂和非核壳结构的CuCoW三元合金催化剂，25 ℃下，Cu0.4@Co0.5W0.1三元合金催化剂对于硼氨配合物水解反应的TOF（转换频率）值达到0.369 0 molH2·molcat-1·s-1，明显高于非核壳结构的Cu0.4Co0.5W0.1催化剂，接近Pt、Pd等贵金属的催化活性，反应的活化能为49 kJ·mol-1。与非核壳结构的CuCoW合金相比，核壳结构的Cu@CoW三元合金催化剂的催化性能及稳定性均有明显提高。 |
| 关键词: 核壳结构 合金 硼氨配合物 多相催化 产氢 |
| 基金项目: 江苏省自然科学基金（No.BK2010387）、国家自然科学基金（No.41172239）、中央高校基础科研业务费专项基金（No.1118020513;1106020513）资助项目。 |
| Abstract: The core/shell structured Cu@CoW and non-crystalline CuCoW alloy were synthesized under mild conditions with NH3BH3 (AB) and NaBH4 as reductant respectively. The catalytic properties were studied on the hydrolysis of AB aqueous solution. The TOF (turn over frequency) of Cu0.4@Co0.5W0.1 catalyst for AB hydrolysis reaction at 25 ℃ reached 0.369 0 molH2·molcat-1·s-1, which was much higher than Cu0.4Co0.5W0.1 and close to the noble-metal based catalysts, such as Pt, Pd, etc. The activation energy of this catalyst was 49 kJ·mol-1. Compared with the non-core/shell structured CuCoW alloy, the Cu@CoW catalyst showed apparent improvements in activity, stability and reusability. The Cu@CoW catalysts with low cost, easy preparation and simply being recovered are suitable for practical application. |
| Keywords: core/shell structure alloy ammonia borane heterogeneous catalysis hydrogen generation |
| 投稿时间：2014-05-04 修订日期：2014-07-01 |
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| 戴敏,沈晓晨,王青,王志斌,赵斌,丁维平.核壳结构Cu@CoW的合成和对硼氨配合物水解的催化性能[J].无机化学学报,2014,30(10):2375-2381. |
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