Enhanced transfer hydrogenation of 2-heptanone to 2-heptanol over synergistic Co/ZnO catalysts

Dongpei Zhang , Jiefeng Liu , Sicheng Shao , Quanxing Zhang , Mengyuan Liu , Yuangao Wang , Mingyu Ma , Ning Cao , Guangyu Zhang , Jinyao Wang , Junwei Yang , Wenjuan Yan , Xin Jin , Chaohe Yang
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Abstract

2-Heptanol is an important secondary alcohol, applied in food, pharmaceutical and plastic industries. However, current industrial synthetic methods require energy intensive hydrogenation of 2-heptanone using homogeneous noble catalysts in alkaline medium. In this work, we presented a systematic study on enhanced transfer hydrogenation of 2-heptanone to 2-heptanol using non-noble Co/ZnO catalysts without alkaline promoters. The strong synergism of Co and ZnO contributes to formation of amorphous metallic Co species and electronically reconfigured CoO species, leading to a 20-fold activity enhancement at 180 °C and a TOF of 89.4 h−1 over Co0.09/ZnO-500 catalysts. Structure-dependency studies further revealed that, the lattice strain between Co and ZnO induced the generation of multi-phased Co/CoO/Co:ZnO interfaces, facilitating tandem H2 generation, spillover and activation of C=O bond (of 2-heptanone molecule), respectively. The insights of molecular catalysis on interface of amorphous Co/ZnO for enhanced C=O bond activation, provide fundamental understanding for transfer hydrogenation of various other ketones into valuable alcohols.

在协同 Co/ZnO 催化剂上增强 2-庚酮向 2-庚醇的转移加氢反应
2- 庚醇是一种重要的仲醇,可用于食品、制药和塑料工业。然而,目前的工业合成方法需要在碱性介质中使用均相惰性催化剂对 2-庚酮进行高能耗氢化。在这项工作中,我们系统地研究了在不使用碱性促进剂的情况下,使用非贵族 Co/ZnO 催化剂将 2-庚酮增强转移加氢为 2-庚醇的过程。Co 和 ZnO 的强协同作用促成了无定形金属 Co 物种和电子重构 CoO 物种的形成,使 Co0.09/ZnO-500 催化剂在 180 °C 时的活性提高了 20 倍,TOF 达到 89.4 h-1。结构依赖性研究进一步表明,Co 和 ZnO 之间的晶格应变诱导生成了多相 Co/CoO/Co:ZnO 界面,分别促进了串联 H2 生成、溢出和(2-庚酮分子)C=O 键的活化。无定形 Co/ZnO 界面的分子催化作用增强了 C=O 键的活化,这为将其他各种酮转移氢化为有价值的醇提供了基本的认识。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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