用零价金属粉末与醇或水合成钼催化氨

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Taichi Mitsumoto, Yoshiaki Nishibayashi
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引用次数: 0

摘要

我们最近在环境反应条件下使用二碘化钐和水实现了从二氮高效氨生成。然而,建立一条无碳、无二氧化碳排放的绿色合成氨生产路线还需要进一步的研究。在这项研究中,我们开发了一种新的钼催化固氮方法,在环境反应条件下,使用零价金属粉末作为还原剂和醇或水作为质子源的组合。在该反应体系中,钐化合物是钼配合物的重要电子介质。值得注意的是,在三碘化钐存在的情况下,锌粉和水的结合有利于在环境反应条件下高度选择性地产生氨,而不是二氢,在催化剂中每个Mo原子产生高达900当量的氨。有趣的是,使用以其强大的还原能力而闻名的镁粉,可以将所需的钐化合物数量减少到催化水平。我们相信,从这个反应系统中获得的新见解代表了实现绿色氨生产的重要一步。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Molybdenum-Catalyzed Ammonia Synthesis by Using Zero-Valent Metal Powder with Alcohols or Water

Molybdenum-Catalyzed Ammonia Synthesis by Using Zero-Valent Metal Powder with Alcohols or Water

We have recently achieved a highly effective ammonia formation from dinitrogen using samarium diiodide and water under ambient reaction conditions. However, further research is needed to establish a carbon-free green ammonia production route without carbon dioxide emissions. In this study, we have developed a novel molybdenum-catalyzed nitrogen fixation method using a combination of zero-valent metal powders as reductants and alcohols or H2O as a proton source under ambient reaction conditions. In this reaction system, samarium compounds serve as crucial electron mediators for the molybdenum complexes. Remarkably, the combination of zinc powder and water in the presence of samarium triiodide facilitates highly selective ammonia production over dihydrogen under ambient reaction conditions, yielding up to 900 equiv of ammonia per Mo atom in the catalyst. Intriguingly, using magnesium powder, known for its potent reducing capability, reduces the requisite amount of samarium compounds to catalytic levels. We believe that the novel insights gained from this reaction system represent a substantial step toward achieving green ammonia production.

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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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