化学
乙二醇
甲醇
乙烯
催化作用
光化学
产量(工程)
选择性
有机化学
解吸
人工光合作用
光合作用
氢键
无机化学
组合化学
作者
Junyu Gao,Qian Xi,Jinhu Wang,Tianrui Hu,Lei Kang,Li‐Zhu Wu,Yunxuan Zhao,Tierui Zhang
摘要
Photocatalytic C–C coupling of methanol provides an appealing approach to producing ethylene glycol (EG) with theoretically zero-carbon cost loss. However, the high polarity of the O–H group severely inhibited the formation and desorption of key radical intermediates, resulting in a low ethylene glycol yield and selectivity. Herein, we report an ammonia-assisted method to promote the efficient photosynthesis of ethylene glycol by amino/ammonia modification on the catalyst surface. After optimization, a 45-fold enhancement of the ethylene glycol production rate (5085 μmol g –1 h –1 ) and an outstanding rise of carbon selectivity can be obtained (91.1%). As revealed by a series of in situ characterizations, we demonstrate that the hydrogen bond between absorbed methanol and the amino group/ammonia could restrain the preferential oxidation of hydroxyl groups on the catalyst surface, leading to the productive production of key ·CH 2 OH for high-efficiency ethylene glycol photosynthesis. This work demonstrated that nonchemical bonding interactions can effectively modulate radical reaction pathways, thereby enabling high-selectivity photocatalysis.
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