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作 者:Zhinuo Wang Ming Yin Jifeng Pang Xianquan Li Yanan Xing Yang Su Shimin Liu Xiaoyan Liu Pengfei Wu Mingyuan Zheng Tao Zhang
机构地区:[1]CAS Key Laboratory of Science and Technology on Applied Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China [2]University of Chinese Academy of Sciences,Beijing 100049,China [3]School of Materials Science and Engineering,Dalian Jiaotong University,Dalian 116028,Liaoning,China [4]Dalian National Laboratory for Clean Energy,Chinese Academy of Sciences,Dalian 116023,Liaoning,China
出 处:《Journal of Energy Chemistry》2022年第9期306-317,I0009,共13页能源化学(英文版)
基 金:supported by the National Science Foundation of China(21690081,21721004 and 21776268);the“Transformational Technologies for Clean Energy and Demonstration,”Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 21060200)。
摘 要:Upgrading ethanol to n-butanol is an attractive way for renewable n-butanol production. Herein, Cu was selected to modify NiMgAlO catalysts for improving ethanol conversion and n-butanol selectivity. Over the optimized 2%Cu-NiMgAlO catalyst, ethanol conversion and n-butanol selectivity were enhanced to 30.0% and 64.2%, respectively, in 200 h time on stream at 523 K. According to physicochemical characterizations and theoretical calculations, the key role of multiple active sites in this reaction was extensively investigated. The plate-like structure of hydrotalcite was maintained over 2%Cu-NiMgAlO catalysts, with an average Ni particle size of ca. 5.4 nm. The presence of Cu species created CuNi alloy sites and Lewis acid-base pairs, and increased hydrogen transfer and condensation reactions, resulting in elevated ethanol conversion and n-butanol selectivity. Additionally, CuNi alloy had a strong interaction with CuNiMgAl oxides, forming homogeneous boundary due to their close ionic radius and lattice matching, and afforded the long time stability in the ethanol to n-butanol reaction.
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