Lewis and Brønsted Acid Synergistic Catalysis for Efficient Synthesis of Hydroxylamine over Heteroatom Zeolites

被引:0
作者
Fang, Nan [1 ]
Huo, Kai [3 ]
Jin, Yucheng [1 ]
Liu, Dongxu [1 ]
Lin, Huanhao [1 ]
Wu, Huiying [1 ]
Liu, Xuguang [1 ,3 ]
Liu, Yueming [1 ,2 ]
He, Mingyuan [2 ]
机构
[1] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, State Key Lab Petr Mol & Proc Engn, Shanghai 200062, Peoples R China
[2] Inst Eco Chongming, Shanghai 202162, Peoples R China
[3] Qingdao Univ Sci & Technol, Coll Mat Sci & Engn, Qingdao 266042, Peoples R China
基金
中国国家自然科学基金;
关键词
synergistic catalysis; hydroxylamine; heteroatomzeolite; Lewis acid sites; Bronsted acid sites; HIGHLY SELECTIVE SYNTHESIS; LIQUID-PHASE AMMOXIMATION; REACTION-MECHANISMS; HYDROGEN-PEROXIDE; OXIME; TITANOSILICATE; DECOMPOSITION; CONVERSION; OXIDATION; CHEMISTRY;
D O I
10.1021/acscatal.4c00179
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Environmental and efficient synthesis of NH2OH is challenging. Herein, we have provided a route for efficient NH2OH formation by NH3 oxidation via the synergistic catalysis of Lewis acid sites of the framework Ti (Ti LAS) and Br & oslash;nsted acid sites of the framework Al (Al BAS) in Ti-Al-MOR zeolites. Ti LAS was the active center for formation of transition-state NH2OH, while Al BAS could provide the proton H to convert transition-state NH2OH absorbed on Ti LAS to a [NH3OH](+) species. Protonation effect would not only promote the catalytic cycle process resulting from accelerating the desorption of transition-state NH2OH, but also improve the stability of NH2OH, being less prone to oxidative decomposition. In this work, we presented the synergistic catalysis between LAS and BAS over Ti-containing heteroatom zeolites to accelerate the catalytic cycle, which provided an environmental and efficient method for NH2OH formation.
引用
收藏
页码:4786 / 4790
页数:5
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