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Interrogation of the Plasma-Catalyst Interface via In Situ/Operando Transmission Infrared Spectroscopy
ACS Engineering Au Pub Date : 2022-08-05 , DOI: 10.1021/acsengineeringau.2c00026
Russell J Clarke 1 , Jason C Hicks 1
Affiliation  

Plasma-surface coupling has emerged as a promising approach to perform chemical transformations under mild conditions that are otherwise difficult or impossible thermally. However, a few examples of inexpensive and accessible in situ/operando techniques exist for observing plasma-solid interactions, which has prevented a thorough understanding of underlying surface mechanisms. Here, we provide a simple and adaptable design for a dielectric barrier discharge (DBD) plasma cell capable of interfacing with Fourier transform infrared spectroscopy (FTIR), optical emission spectroscopy (OES), and mass spectrometry (MS) to simultaneously characterize the surface, the plasma phase, and the gas phase, respectively. The system was demonstrated using two example applications: (1) plasma oxidation of primary amine functionalized SBA-15 and (2) catalytic low temperature nitrogen oxidation. The results from application (1) provided direct evidence of a 1% O2/He plasma interacting with the aminosilica surface by selective oxidation of the amino groups to nitro groups without altering the alkyl tether. Application (2) was used to detect the evolution of NOX species bound to both platinum and silica surfaces under plasma stimulation. Together, the experimental results showcase the breadth of possible applications for this device and confirm its potential as an essential tool for conducting research on plasma-surface coupling.

中文翻译:

通过原位/操作透射红外光谱对等离子体-催化剂界面的询问

等离子表面耦合已成为一种有前途的方法,可以在温和条件下进行化学转化,否则很难或不可能进行热反应。然而,一些廉价且易于获得的原位/操作的例子存在用于观察等离子体-固体相互作用的技术,这阻碍了对潜在表面机制的透彻理解。在这里,我们为能够与傅立叶变换红外光谱 (FTIR)、光学发射光谱 (OES) 和质谱 (MS) 接口以同时表征表面的介质阻挡放电 (DBD) 等离子体电池提供了一种简单且适应性强的设计,分别为等离子相和气相。该系统使用两个示例应用进行了演示:(1) 伯胺官能化 SBA-15 的等离子体氧化和 (2) 催化低温氮氧化。应用 (1) 的结果提供了 1% O 2的直接证据/He 等离子体通过将氨基选择性氧化为硝基而不改变烷基链而与氨基二氧化硅表面相互作用。应用程序 (2) 用于检测在等离子体刺激下结合到铂和二氧化硅表面的 NO X物种的演变。总之,实验结果展示了该设备可能应用的广度,并证实了其作为进行等离子体表面耦合研究的重要工具的潜力。
更新日期:2022-08-05
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