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Carbon monoliths with programmable valence bands as de novo anodes for additive-free coupling of alcohols into acetals
FlatChem ( IF 6.2 ) Pub Date : 2021-04-20 , DOI: 10.1016/j.flatc.2021.100248
Xiu Lin , Qi-Yuan Li , Dong Xu , Lu-Sha Gao , Guang-Yao Zhai , Shi-Nan Zhang , Peng Gao , Jie-Sheng Chen , Xin-Hao Li

Designing functional and reusable electrode materials to replace homogeneous versions of scarifying additives or mediators in electrochemical organic synthesis is of great importance for both the fundamental academics and practical production of various useful compounds. Herein, we rediscover the function of nitrogen-doped carbon monoliths (NxC) as de novo anode materials to trigger a new reaction path for the synthesis of acetals from the direct coupling of alcohols without the assistance of any mediator, oxidant, acid, or organic ligand. The lowered valence bands of carbon monoliths induced by doping nitrogen are of key importance for polarizing and activating the pre-adsorbed O–H groups of benzyl alcohol molecules to boost the high Faradaic efficiency (71% at 1.8 V versus Ag/AgCl) and reusability of NxC anodes, meeting the requirements of green chemistry.



中文翻译:

具有可编程价带的碳整体结构,作为从头阳极,用于无添加剂地将醇偶联到乙缩醛中

设计功能性和可重复使用的电极材料,以替代电化学有机合成中均化形式的划痕添加剂或介体,对于基础理论和各种有用化合物的实际生产都至关重要。在此,我们重新发现氮掺杂的碳单块的功能(N X C)作为从头阳极材料可触发一种新的反应路径,无需醇,任何氧化剂,酸或有机配体的帮助,即可直接由醇类直接偶联来合成乙缩醛。掺杂氮引起的碳整体结构的价带降低,对于极化和活化苄醇分子的预先吸附的OH基以提高法拉第效率(与Ag / AgCl相比,在1.8 V时为71%)和重用性至关重要。 N x C阳极,符合绿色化学要求。

更新日期:2021-04-23
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