On the distinct reactivity of two isomers of [IrC4H2]+ toward methane and water

IF 10.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Science China Chemistry Pub Date : 2022-07-20 DOI:10.1007/s11426-022-1342-4

Bowei Yuan, Zizhuang Liu, Xiao-Nan Wu, Shaodong Zhou

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引用次数: 1

Abstract

The gas-phase reactions of [IrC₄H₂]⁺ with methane and water have been explored by using mass spectrometry combined with quantum chemical calculations. Interestingly, under the employed conditions, two isomers of [IrC₄H₂]⁺ co-exist with different reactivity. One of them only activates methane while the other is solely reactive with water to produce CO. Apparently, upon varying the coordination patterns, the Ir center gains rather distinct capabilities of mediating the bond breaking and making processes. The reactivity toward methane mainly depends on the orbital orientation, while the π-aromaticity of the reaction complex matters for the conversion of water. The experimental and theoretical findings in this work do not only imply the promising role the Ir atom can play in the bulk-system methane conversion, but may also be instructive on how to construct a high-performance center for steam reforming of methane.

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[IrC4H2]+的两种异构体对甲烷和水的不同反应性

采用质谱法结合量子化学计算，研究了[IrC4H2]+与甲烷和水的气相反应。有趣的是，在实验条件下，[IrC4H2]+的两种异构体共存，反应活性不同。其中一种只激活甲烷，而另一种只与水反应生成一氧化碳。显然，通过改变配位模式，Ir中心获得了相当独特的调节断键和成键过程的能力。对甲烷的反应性主要取决于轨道取向，而反应配合物的π芳构度对水的转化有影响。本工作的实验和理论结果不仅揭示了Ir原子在本体体系甲烷转化中的重要作用，而且对如何建立高效的甲烷蒸汽重整中心具有指导意义。

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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来源期刊

Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

7.30%

发文量

3787

审稿时长

2.2 months

期刊介绍： Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.