Atmospherical oxidative coupling of amines by UiO-66-NH2 photocatalysis under milder reaction conditions

Atmospherical oxidative coupling of amines by UiO-66-NH2 photocatalysis under milder reaction conditions
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较温和反应条件下UiO-66-NH2光催化胺的大气氧化偶联

DOI:
10.1016/j.catcom.2019.03.011
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发表时间:
2019-05
影响因子:
3.7
通讯作者:
Lei Ziqiang
Lei Ziqiang
中科院分区:
化学3区
文献类型:
--
作者:
Liu Ruxue;Meng Shuangyan;Ma Yali;Niu Litong;He Shuanghong;Xu Xueqing;Su Bitao;Lu Dedai;Yang Zhiwang;Lei Ziqiang

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为了探讨胺转化为亚胺的反应机理和温和条件,选择UiO-66-NH 2作为光催化剂,研究了光催化下胺转化为亚胺的反应。进行了一系列捕捉活性物种的实验,证明了当在空气中进行反应时,涉及空穴(h+)和超氧自由基(自由基dotO 2 −)。反应也发生,因为存在的氮为中心的自由基阳离子和碳为中心的自由基,这是诱导光生空穴(H+)在厌氧条件下具有相当大的转化率和选择性。实验结果表明,催化剂可循环使用4次。
To assess the mechanism and milder conditions for amines to imines, UiO-66-NH2was chosen as an efficient photocatalyst for the transformation under light irradiation. A series of experiments for the catching of the active species were performed, and it was proved that holes (h+) and superoxide radicals (radical dotO2−) were involved when the reaction was performed under air. The reaction also occurred because of the presence of nitrogen-centered radical cations and carbon-centered radicals, which were induced by photogenerated hole (h+) with considerable conversion and selectivity under anaerobic conditions. Our experiments revealed that the catalyst can be recycled for four times.
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