羧酸盐和配位对活性ruvoxo物种形成的影响。

IF 3.9 2区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Scientific Reports Pub Date : 2025-02-18 DOI:10.1038/s41598-025-89062-5

Jamal El-Abid, Kevin M Dorst, Andrew K Inge, Oscar Verho, Varun Kundi, Priyank V Kumar, Anders Thapper, Biswanath Das

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引用次数: 0

摘要

了解Ru(V)-氧的结构对于设计用于可持续能源应用的新型催化剂至关重要，例如用于绿色制氢的水裂解。本研究报道了一种由三联吡啶和邻菲罗啉羧酸配体稳定的Ru(V)-氧中间体的EPR检测。羧酸基团和钌中心之间的相互作用，以及氧化条件下pcet依赖的半半性，在实现高价态中起着关键作用。中心金属周围协调环境的细微变化也被证明是必不可少的。低温核磁共振、高分辨率质谱、紫外可见光谱和密度泛函理论计算支持这些发现。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Carboxylate and coordination influence on the formation of an active RuV Oxo species.

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Carboxylate and coordination influence on the formation of an active Ru^V Oxo species.

Understanding the structure of Ru(V)-oxo species is crucial for designing novel catalysts for sustainable energy applications, such as water splitting for green hydrogen production. This study reports the EPR detection of a Ru(V)-oxo intermediate stabilized by terpyridine and phenanthroline carboxylate ligands. The interaction between the carboxylate group and the ruthenium center, along with PCET-dependent hemilability under oxidative conditions, plays a critical role in achieving the high-valent state. Subtle changes in the coordination environment around the central metal also proved to be essential. Low-temperature NMR, high-resolution mass spectrometry, UV-Vis spectroscopy, and density functional theory calculations support these findings.

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来源期刊

Scientific Reports Natural Science Disciplines-

CiteScore

7.50

自引率

4.30%

发文量

19567

审稿时长

3.9 months

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