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作 者:Yan Li Haiyang Cheng Chao Zhang Bin Zhang Tong Liu Qifan Wu Xinluona Su Weiwei Lin Fengyu Zhao
机构地区:[1]State Key Laboratory of Electroanalytical Chemistry,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China [2]Laboratory of Green Chemistry and Process,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences Changchun 130022,China [3]Department of Environmental Science and Engineering,Heilongfiang University,Harbin 150080,China
出 处:《Science China Chemistry》2017年第7期920-926,共7页中国科学(化学英文版)
基 金:supported by the National Basic Research Program of China(2016YFA0602900);Youth Innovation Promotion Association CAS(2016206);Jilin Provincial Science and Technology Program of China(20150301012GX)
摘 要:Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al_2O_3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al_2O_3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H_2 and NH_3 pressure were examined, and the reaction processes were discussed in detail.Hexamethylenediamine(HMDA) is an important reagent for the synthesis of Nylon-6,6, and it is usually produced by the hydrogenation of adiponitrile using a toxic reagent of hydrocyanic acid. Herein, we developed an environmental friendly route to produce HMDA via catalytic reductive amination of 1,6-hexanediol(HDO) in the presence of hydrogen. The activities of several heterogeneous metal catalysts such as supported Ni, Co, Ru, Pt, Pd catalysts were screened for the present reaction in supercritical ammonia without any additives. Among the catalysts examined, Ru/Al2O3 presented a high catalytic activity and highest selectivity for the desired product of HMDA. The high performance of Ru/Al2O3 was discussed based on the Ru dispersion and the surface properties like the acid-basicity. In addition, the reaction parameters such as reaction temperature,time, H2 and NH3 pressure were examined, and the reaction processes were discussed in detail.
关 键 词:1 6-hexanediol hexamethylenediamine supercritical ammonia reductive amination Ru/Al2O3
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