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核壳结构Cu@CoCr的合成和对硼氨配合物水解的催化性能
引用本文:沈晓晨,戴敏,高鸣,王志斌,赵斌,丁维平.核壳结构Cu@CoCr的合成和对硼氨配合物水解的催化性能[J].无机化学学报,2013,29(5):999-1006.
作者姓名:沈晓晨  戴敏  高鸣  王志斌  赵斌  丁维平
作者单位:1. 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
2. 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
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。
摘    要:通过一步法原位合成了核壳结构的Cu@CoCr三元合金催化剂,该合成方法条件温和、步骤简便。25℃下,Cu0.4@Co0.5Cr0.1三元合金催化剂对于硼氨配合物水解反应的TOF值达到0.242 0 molH2.moLcat-1.s-1,接近Pt、Pd等贵金属的催化活性,反应的活化能仅为35 kJ.mol-1,5次重复使用后仍能保持初始活性的35%。与非核壳结构的CuCoCr合金相比,核壳结构的Cu@CoCr三元合金催化剂的催化性能及稳定性均有明显提高。此外材料自身具有磁性,可进行磁分离,适合于实际应用。

关 键 词:原位合成  核壳结构  合金  硼氨配合物  多相催化  产氢
收稿时间:2012/11/12 0:00:00
修稿时间:2013/1/17 0:00:00

Core-Shell Structured Cu@CoCr Catalyst: Synthesis and Catalytic Performance for Hydrolysis of Ammonia Borane Aqueous Solution
SHEN Xiao-Chen,DAI Min,GAO Ming,WANG Zhi-Bin,ZHAO Bin and DING Wei-Ping.Core-Shell Structured Cu@CoCr Catalyst: Synthesis and Catalytic Performance for Hydrolysis of Ammonia Borane Aqueous Solution[J].Chinese Journal of Inorganic Chemistry,2013,29(5):999-1006.
Authors:SHEN Xiao-Chen  DAI Min  GAO Ming  WANG Zhi-Bin  ZHAO Bin and DING Wei-Ping
Institution:Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;State Key Laboratory of Coordination Chemistry, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China;Key Laboratory of Mesoscopic Chemistry of Ministry of Education, School of Chemistry & Chemical Engineering, Nanjing University, Nanjing 210093, China
Abstract:The core/shell structured ternary alloy of Cu@CoCr was synthesized by a one-step in-situ synthesis method under mild conditions. The catalytic performance of Cu@CoCr was studied for the hydrolysis of NH3BH3 (AB) aqueous solution. The TOF (turn over frequency) of 0.242 0 molH2·moLcat-1·s-1 for Cu0.4@Co0.5Cr0.1 catalyst on AB hydrolysis reaction is close to the noble-metal based catalysts, such as Pt, Pd, etc. The activation energy of this catalyst is only 35 kJ·mol-1. After 5 cycles, this catalyst still keeps 35% of its initial activity. Compared to the non-core/shell structured CuCoCr alloy, the Cu@CoCr catalyst shows great improvements in activity, stability and reusability. Furthermore, the Cu@CoCr catalysts could be recovered by a magnet based on its magnetic properties.
Keywords:in-situ synthesis  core/shell structure  alloy  ammonia borane  heterogeneous catalysis  hydrogen generation
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