文献类型：期刊文献

英文题名：Engineering Ni/NiAlmO heterojunction catalysts for efficient multisite cooperation in the N-alkylation of aniline

作者：Chen, Zhou[1];Lv, Shengyao[1];Zhang, Zhongyao[1];Chen, Wenyao[1];Qian, Gang[1];Zhang, Jing[1];Zhou, Xinggui[1];Chen, De[1,2];Yuan, Weikang[1];Duan, Xuezhi[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn & Low Carbon Technol, Shanghai, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, Trondheim, Norway

年份：2026

外文期刊名：AICHE JOURNAL

收录：;EI(收录号：20262320828567);WOS:【SCI-EXPANDED(收录号:WOS:001775642100001)】；

基金：This work was financially supported by the National Key R&D Program of China (2024YFA1510303), the Natural Science Foundation of China (22478107, 22038003, 22178100, 22178101, and U22B20141), the Shanghai Rising Star Program (24QA2701900), the Shanghai Pilot Program for Basic Research (22TQ1400100-15), the Innovation Program of Shanghai Municipal Education Commission, and the Shanghai Science and Technology Innovation Action Plan (22JC1403800). The authors thank the staff members from the BL11B beamline of Shanghai Synchrotron Radiation Facility (SSRF) for assistance during data collection.

语种：英文

外文关键词：multisite cooperative catalysis; N-alkylation; Ni/Ni(Al)O heterojunctions; O-H bond cleavage; oxide structure regulation

摘要：Alkylation of amines with alcohols offers a sustainable route featuring high atom economy and minimal waste, yet remains kinetically challenging due to the inertness of alcohols and the need for coordinated activation of multiple sites. In this work, we report a strategy of engineering Ni/NiAlmO heterojunction structure that synergizes Ni-0 and Ni(Al)O sites toward efficient N-alkylation. A series of Ni/NiAlmO catalysts with varied Ni/Al ratios were prepared by coprecipitation and characterized. The results show a gradual evolution of the oxide phase from Ni(Al)O toward NiO with decreasing Al content, with Ni/NiAl0.5O exhibiting the most apparent Ni/Ni(Al)O heterojunction and the highest catalytic activity. Density functional theory calculations demonstrate that Ni(Al)O lowers the barrier for O-H cleavage in ethanol relative to NiO, thereby cooperating with Ni-0 sites for subsequent C-H activation. This multisite synergistic strategy provides a new avenue for the rational design and preparation of efficient N-alkylation catalysts.