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Defective Auδ−-Ov interfacial sites boost C-H bond activation for enhanced selective oxidation of amino alcohols to amino acids
Journal of Catalysis ( IF 6.5 ) Pub Date : 2023-12-29 , DOI: 10.1016/j.jcat.2023.115284
Ying Liao , Yue Pan , Xiang Feng , Xiaobo Chen , Yibin Liu , Chaohe Yang , Hao Yan
Journal of Catalysis ( IF 6.5 ) Pub Date : 2023-12-29 , DOI: 10.1016/j.jcat.2023.115284
Ying Liao , Yue Pan , Xiang Feng , Xiaobo Chen , Yibin Liu , Chaohe Yang , Hao Yan
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Designing efficient active sites to facilitate the oxidation of hydroxyl group to carboxylic acid under the influence of nitrogen-containing functional groups is worth exploring, but it is rarely investigated. Herein, we construct defective Au-ZrO interfacial structures by tuning the calcination temperature of ZrO support to boost the oxidation of amino alcohols to amino acids. Interestingly, the modification of calcination temperature induces the escape of saturated coordination oxygen atoms in ZrO support, leaving behind abundant surface oxygen vacancy (O). The as-formed Au-O interfacial site displays the unique synergistic adsorption effect and electron transfer ability. Specifically, the O site voluntarily adsorbs the –NH group of amino alcohol, thus ensuring that the electron-rich Au nearby O site adsorbs the hydroxyl groups and activates the C-H bond activation of NHCHCHO* intermediates. Consequently, Au/ZrO-600 catalyst with more defective Au-O interfacial sites exhibits 98.8 % product yield for the oxidation of diethanolamine to iminodiacetic acid at only 30 °C. The catalyst system is further extended to the oxidation of other amino alcohols, involving monoethanolamine and triethanolamine, to their corresponding amino acids with excellent catalytic performance.
中文翻译:
有缺陷的 Auδ−Ov 界面位点促进 CH 键活化,从而增强氨基醇选择性氧化为氨基酸
设计有效的活性位点以促进羟基在含氮官能团的影响下氧化成羧酸值得探索,但很少研究。在此,我们通过调节 ZrO 载体的煅烧温度来促进氨基醇氧化为氨基酸,从而构建有缺陷的 Au-ZrO 界面结构。有趣的是,煅烧温度的改变会导致ZrO载体中饱和配位氧原子的逃逸,留下大量的表面氧空位(O)。形成的Au-O界面位点表现出独特的协同吸附效应和电子传输能力。具体来说,O位自愿吸附氨基醇的-NH基团,从而确保O位附近的富电子Au吸附羟基并激活NHCHCHO*中间体的CH键活化。因此,具有更多缺陷Au-O界面位点的Au/ZrO-600催化剂在仅30℃下将二乙醇胺氧化成亚氨基二乙酸时表现出98.8%的产物产率。该催化剂体系进一步扩展到其他氨基醇(包括单乙醇胺和三乙醇胺)氧化为其相应氨基酸,具有优异的催化性能。
更新日期:2023-12-29
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
有缺陷的 Auδ−Ov 界面位点促进 CH 键活化,从而增强氨基醇选择性氧化为氨基酸
设计有效的活性位点以促进羟基在含氮官能团的影响下氧化成羧酸值得探索,但很少研究。在此,我们通过调节 ZrO 载体的煅烧温度来促进氨基醇氧化为氨基酸,从而构建有缺陷的 Au-ZrO 界面结构。有趣的是,煅烧温度的改变会导致ZrO载体中饱和配位氧原子的逃逸,留下大量的表面氧空位(O)。形成的Au-O界面位点表现出独特的协同吸附效应和电子传输能力。具体来说,O位自愿吸附氨基醇的-NH基团,从而确保O位附近的富电子Au吸附羟基并激活NHCHCHO*中间体的CH键活化。因此,具有更多缺陷Au-O界面位点的Au/ZrO-600催化剂在仅30℃下将二乙醇胺氧化成亚氨基二乙酸时表现出98.8%的产物产率。该催化剂体系进一步扩展到其他氨基醇(包括单乙醇胺和三乙醇胺)氧化为其相应氨基酸,具有优异的催化性能。