化学
氮氧化物
催化作用
镍
除氧
卤化物
双功能
烷基
亲核细胞
催化循环
组合化学
无机化学
有机化学
燃烧
作者
Sudakar Padmanaban,Jonghoon Choi,Hugo Vázquez‐Lima,Donghwi Ko,Dagyum Yoo,Jinseong Gwak,Kyung‐Bin Cho,Yunho Lee
摘要
Nitrogen oxide (NOx) conversion is an important process for balancing the global nitrogen cycle. Distinct from the biological NOx transformation, we have devised a synthetic approach to this issue by utilizing a bifunctional metal catalyst for producing value-added products from NOx. Here, we present a novel catalysis based on a Ni pincer system, effectively converting Ni-NOx to Ni-NO via deoxygenation with CO(g). This is followed by transfer of the in situ generated nitroso group to organic substrates, which favorably occurs at the flattened Ni(I)-NO site via its nucleophilic reaction. Successful catalytic production of oximes from benzyl halides using NaNO2 is presented with a turnover number of >200 under mild conditions. In a key step of the catalysis, a nickel(I)-•NO species effectively activates alkyl halides, which is carefully evaluated by both experimental and theoretical methods. Our nickel catalyst effectively fulfills a dual purpose, namely, deoxygenating NOx anions and catalyzing C-N coupling.
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