铜镍双金属催化剂用于乙二醇氨化制乙二胺反应性能研究OA北大核心CSTPCD

Catalytic amination of ethylene glycol(EG)to ethylenediamine(EDA)is a green,efficient and economical route to obtain EDA,but there are still some problems to be solved,such as harsh reaction conditions and poor product selectivity.By adjusting n(Cu):n(Ni),a series of Cua-Ni1-a-Al-O(the value of a is 0.09,0.30,0.50,0.70 and 0.91,respectively)catalysts were prepared by co-precipitation method and used for amination of EG to EDA.The catalysts were characterized by X-ray diffraction(XRD),N2 absorption/desorption and high-resolution transmission electron microscopy(HR-TEM),etc,and the reaction conditions of catalytic amination of EG to EDA were optimized.The results show that the specific surface area of Cu-based monmetallic catalyst can be significantly increased by the introduction of Ni,and Cu0.09-Ni0.91-Al-O has the largest specific surface area(150.20 m2/g)and the smallest average pore size(5.84 nm).The Cu and Ni in Cua-Ni1-a-Al-O exist in the form of CuNi alloy,and the crystallinity and crystal size of the catalyst decrease with the decrease of a.Under the optimal reaction conditions(200 mg Cu0.09-Ni0.91-Al-O,1 mmol EG,15 mL 1,2-dimethoxy-ethane,7 g NH3,3 MPa H2,180℃and reaction for 13 h),the EG conversion rate and EDA yield are 100%and 60%,respectively.Cu0.09-Ni0.91-Al-O is recycled for four times under the optimal reaction conditions,and the catalytic performance of Cu0.09-Ni0.91-Al-O does not change significantly.