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探究非热等离子体(NTP)在甲烷混合 NTP 催化氧化中作用。

Probing the Role of a Non-Thermal Plasma (NTP) in the Hybrid NTP Catalytic Oxidation of Methane.

机构信息

UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell Oxon, Didcot, OX11 0FA, UK.

Department of Chemistry, University College London, 20 Gordon Street, London, WC1 0AJ, UK.

出版信息

Angew Chem Int Ed Engl. 2017 Aug 1;56(32):9351-9355. doi: 10.1002/anie.201703550. Epub 2017 Jul 6.

Abstract

Three recurring hypotheses are often used to explain the effect of non-thermal plasmas (NTPs) on NTP catalytic hybrid reactions; namely, modification or heating of the catalyst or creation of new reaction pathways by plasma-produced species. NTP-assisted methane (CH ) oxidation over Pd/Al O was investigated by direct monitoring of the X-ray absorption fine structure of the catalyst, coupled with end-of-pipe mass spectrometry. This in situ study revealed that the catalyst did not undergo any significant structural changes under NTP conditions. However, the NTP did lead to an increase in the temperature of the Pd nanoparticles; although this temperature rise was insufficient to activate the thermal CH oxidation reaction. The contribution of a lower activation barrier alternative reaction pathway involving the formation of CH (g) from electron impact reactions is proposed.

摘要

三种常见的假设常用于解释非热等离子体(NTP)对 NTP 催化混合反应的影响;即,通过等离子体产生的物质来改变或加热催化剂或创造新的反应途径。通过直接监测催化剂的 X 射线吸收精细结构,并结合尾气质谱,研究了 NTP 辅助下 Pd/Al2O3 上的甲烷(CH4)氧化反应。这项原位研究表明,在 NTP 条件下,催化剂没有发生任何显著的结构变化。然而,NTP 确实导致了 Pd 纳米颗粒温度的升高;尽管这种温度升高不足以激活热 CH 氧化反应。提出了一种涉及电子碰撞反应形成 CH(g)的较低活化能替代反应途径的贡献。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/05e5/5577514/e6cc4de4c8b6/ANIE-56-9351-g001.jpg

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