研究人员揭示尿素的电氧化是通过分子内N
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研究人员揭示尿素的电氧化是通过分子内N

作者:澳门巴黎人 时间:2020-12-30 17:59

本期文章:《德国应用化学》:Online/在线发表

近日,湖南大学化学与化工学院教授Qinghua Liu及其小组揭示电氧化尿素的机理是通过分子内N-N键的耦合。 2020年12月24日,国际知名学术期刊《德国应用化学》发表了这一成果。

专注于β‐Ni(OH) 2电极上的NOR,研究人员揭示了含氮亲核体的转化机理。对于两步NOR,质子耦合电子转移(PCET)是电生成电极催化剂从β‐Ni(OH) 2 脱氢生成β‐Ni(OH)O和自发亲核体脱氢氧化反应的桥梁。该理论可以很好地解释肼和伯胺的氧化反应,但不足以用于尿素氧化反应(UOR)。

通过在UOR过程中原位反应追踪化学键断裂和生成,研究人员提出可能的UOR机理是分子内N-N键耦合,伴随着PECT、水化和重排过程,造成了高的表现以及100% N2 选择性。这些发现不仅阐明了NOR过程中含氮分子的进化,而且为氮循环电催化奠定了基础。

据悉,氮是各个生物体的一个重要的营养,氮循环对于人类社会非常重要。含氮亲核体电氧化反应(NOR)在可用氮的降解和转化中起着至关重要的作用。

附:英文原文

Title: Unveiling the electrooxidation of urea: the intramolecular coupling of N‐N bond

Author: Shuangyin Wang, Wei Chen, Leitao Xu, Xiaorong Zhu, Yu-Cheng Huang, Wang Zhou, Dongdong Wang, Yangyang Zhou, Shiqian Du, Qiling Li, Chao Xie, Li Tao, Chung-Li Dong, Jilei Liu, Yanyong Wang, Ru Chen, Hui Su, Chen Chen, Yuqin Zou, Yafei Li, Qinghua Liu

Issue&Volume: 24 December 2020

Abstract: Nitrogen is an essential nutrient for every organism and the nitrogen cycle is significant for human society. Nitrogenous nucleophile electrooxidation reaction (NOR) plays a vital role in the degradation and transformation of available nitrogen. Here, focusing on NOR based on β‐Ni(OH) 2  electrode, we decipher the transformation mechanism of nitrogenous nucleophile. For two‐step NOR, proton‐coupled electron transfer (PCET) is the bridge between electrogenerated electrocatalyst dehydrogenation from β‐Ni(OH) 2  to β‐Ni(OH)O and spontaneous nucleophile dehydrogenation oxidation reaction. This theory can give a good explanation for hydrazine and primary amine oxidation reactions, but is insufficient for urea oxidation reaction (UOR). Through operando tracing bond rupture and formation processes during UOR and theoretical calculation, we propose the possible UOR mechanism that intramolecular coupling of N‐N bond, accompanying with PCET, hydration and rearrangement processes, results in high‐performance and ~100% N  2  ‐selectivity. These discoveries not only clarify the evolution of nitrogenous molecules during NOR, but also lay fundamental for nitrogen cycle electrocatalysis.

DOI: 10.1002/anie.202015773

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202015773

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:12.959
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx