| In this thesis,supported non-noble metal catalysts with superior performance were prepared by a co-precipitation method for the N-alkylation of aniline with 2.5-Dihydroxymethylfuran(DHMF).Compared with the previous non-noble metal catalysts,the developed catalysts in this work exhibit good catalytic performance in base-free and gentle conditions.The detailed study includes the following:(1)Synthesis of N-alkylation catalysts and their characterizations.In this study,alumina supported CuNi alloy catalysts with various Cu/Ni ratios were prepared by a co-precipitation method.The obtained catalysts were characterized by various techniques,such as X-ray diffraction,H2 temperature programmable reduction,electron transmission microscopy with EDS phase mapping and X-ray photoelectron spectroscopy.The results reveal the following:Cu and Ni mixed solid solution oxides are formed by calcination of precursors obtained from the co-precipitation,which is further transformed into CuNi alloy phase by the following reduction;the calcination and reduction temperatures play important roles in the formation of CuNi phase and their sizes;when the calcination temperature is too high,NiAlO4 phase will form,which is unfavorable to the formation of CuNi phase in the reduction process,while CuNi formation is not enough at low reduction temperatures.(2)N-alkylation of aniline with DHMF.The catalytic performance for N-alkylation of aniline with DHMF over various alumina supported CuNi catalysts were investigated,and the catalytic reaction conditions were optimized.The catalytic results show the following:the optimized catalyst is Cu3/17Ni6/17Al8/17O:at the optimized reaction conditions(120 ?,24 h,aniline/DHMF of 5/1,mesitylene as solvent),the conversion of DHMF is above 99%,and the selectivity of the desired product and the intermediate are 55%and 11%,respectively.From the combination of characterizations and catalytic results,it is concluded that the CuNi is the catalytically active phase in N-alkylation. |
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