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四氢异喹啉完全选择性双电子温和电化学氧化为二氢异喹啉促进制氢
作者:小柯机器人 发布时间:2023/1/20 3:37:37

同济大学赵国华团队报道了四氢异喹啉完全选择性双电子温和电化学氧化为二氢异喹啉促进制氢。相关研究成果于2023年1月15日发表于国际顶尖学术期刊《德国应用化学》。

不同与之前的生物质衍生物取代水氧化以提高氢气产量,研究发现温和氧化更有利于阴极制氢。

该研究中,通过精确控制四氢异喹啉(THIQs)到二氢异喹啉的两电子温和电化学氧化(DHIQs)来代替四电子深度氧化到异喹啉(IQs),实现了最大的法拉第效率(>99%)和较低的制氢能耗。此外,在1.36V的低电位下,THIQs以高选择性(>99%)制备了高附加值的DHIQ。Operando电化学拉曼和密度泛函理论证明,高选择性归因于Co和Fe相互作用诱导的NiOOH的可调节活性物种,以优先断开THIQs的C-H键,而不是N-H键。

该新方法为生物质辅助制氢提供了重要的见解。

附:英文原文

Title: Boosting Hydrogen Production via Selective Two-electron Mild Electrochemical Oxidation of Tetrahydroisoquinolines Completely to Dihydroisoquinolines

Author: Zhaoyu Zhou, Xun Pan, Lingzhi Sun, Yanan Xie, Jingui Zheng, Lina Li, Guohua Zhao

Issue&Volume: 2023-01-15

Abstract: Different from the previous study that biomass derivatives replace water oxidation for enhancing hydrogen production, we found that mild oxidation was more conductive to cathodic hydrogen production. In this study, maximum Faradaic efficiency (>99%) and lower energy consumption for hydrogen production was achieved by precisely controlling the two-electron mild electrochemical oxidation of tetrahydroisoquinolines (THIQs) to dihydroisoquinolines (DHIQs) in place of the four-electron deep oxidation to isoquinolines (IQs). Moreover, the high value-added DHIQs were prepared from THIQs with high selectivity (>99%) at the low potential of 1.36V. Operando electrochemical Raman and density functional theory proved that the high selectivity was attributed to the regulable active species of NiOOH induced by the interaction of Co and Fe for preferentially breaking C-H bond rather than N-H of THIQs. This novel method provides important insight into efficient biomass-assisted hydrogen production.

DOI: 10.1002/anie.202216347

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202216347

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx

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