c60支持的单Pt原子选择性活化CH4。

IF 4.6 2区 化学 Q2 CHEMISTRY, PHYSICAL
Jiao-Jiao Chen*, Xi-Guan Zhao, Bo-Han Zang, Hui-Ru Jia, Qing-Yu Liu, Xun-Lei Ding and Sheng-Gui He*, 
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引用次数: 0

摘要

负载型单原子催化剂(SACs)在选择性活化C-H键方面表现出巨大的潜力,使甲烷(CH4)能够直接转化为高附加值的化工产品。在此,得益于最先进的质谱技术和新设计的变温双离子阱反应器,我们成功地将单个Pt-原子固定在独特的零维碳载体(C60)上,并观察到与惰性裸Pt-相比,C60Pt-在室温下对CH4活化的反应性显着增强。C60载体在改变单金属位(Pt-→Pt0)电子态方面的关键作用被强调为增强与CH4轨道相互作用的关键因素。此外,C60的电子缓冲能力也有利于选择性地激活CH4,只切割一个碳氢键。这一发现不仅提供了对CH4活化的支持SACs的原子尺度见解,而且强调了在设计直接转化CH4的相关催化剂时考虑C60的积极支持作用的重要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

C60-Supported Single Pt Atom for Selective CH4 Activation

C60-Supported Single Pt Atom for Selective CH4 Activation

Supported single-atom catalysts (SACs) exhibit great potential for the selective activation of C–H bonds, enabling the direct conversion of methane (CH4) into high value-added chemical products. Herein, benefiting from state-of-the-art mass spectrometry coupled with newly designed variable-temperature double ion trap reactors, we successfully immobilized a single Pt atom on a unique zero-dimensional carbon support (C60) and observed a significantly enhanced reactivity of C60Pt toward CH4 activation at room temperature compared to inert bare Pt. The crucial role of the C60 support in modifying the electronic state of the single metal site (Pt → Pt0) was highlighted as a key factor in enhancing orbital interactions with CH4. Furthermore, the electron-buffering capability of C60 also facilitates selective CH4 activation by cleaving only one C–H bond. This finding not only provides atomic-scale insights into supported SACs for CH4 activation but also underscores the importance of considering the positive support effects of C60 in designing related catalysts for direct CH4 conversion.

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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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