催化作用
沸石咪唑盐骨架
化学
氢化物
Atom(片上系统)
试剂
咪唑酯
转移加氢
吸附
光化学
化学工程
无机化学
组合化学
金属
材料科学
金属有机骨架
物理化学
有机化学
钌
嵌入式系统
工程类
计算机科学
作者
Zhidong An,Piaoping Yang,Delong Duan,Jiang Li,Tong Wan,Yue Kong,Stavros Caratzoulas,Shuting Xiang,Jiaxing Liu,Lei Huang,Anatoly I. Frenkel,Yuan‐Ye Jiang,Ran Long,Zhenxing Li,Dionisios G. Vlachos
出处
期刊:Research Square - Research Square
日期:2023-03-08
被引量:1
标识
DOI:10.21203/rs.3.rs-2631124/v1
摘要
Abstract Highly effective and selective noble metal-free catalysts attract significant attention. Here, a single-atom iron catalyst is fabricated by saturated adsorption of trace iron onto zeolitic imidazolate framework-8 (ZIF-8) followed by pyrolysis. Its performance toward catalytic transfer hydrogenation of furfural is comparable to state-of-the-art catalysts and up to four orders higher than other Fe catalysts. Isotopic labeling experiments demonstrate an intermolecular hydride transfer mechanism. First principles simulations, spectroscopic calculations and experiments, and kinetic correlations reveal that the synthesis creates pyrrolic Fe(I)-plN 3 as the active center whose flexibility manifested by being pulled out of the plane, enabled by defects, is crucial for collocating the reagents and allowing the chemistry to proceed. The catalyst catalyzes chemoselectively several substrates and possesses a unique trait whereby the chemistry is hindered for more acidic substrates than the hydrogen donors. This work paves the way toward noble-metal free single-atom catalysts for important chemical reactions.
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