Mechanism of Low Pressure Plasma-Assisted CO2 Hydrogenation Over Ni-USY by Microsecond Time-resolved FTIR Spectroscopy
Mechanism of Low Pressure Plasma-Assisted CO2 Hydrogenation Over Ni-USY by Microsecond Time-resolved FTIR Spectroscopy
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DOI：
10.1007/s11244-017-0849-2
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发表时间：
2017-12-01
影响因子：
3.6
通讯作者：
Thibault-Starzyk, Frederic
中科院分区：
文献类型：
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作者：
Azzolina-Jury, Federico;Thibault-Starzyk, Frederic
掺杂镍（14% wt.）的 H-USY 沸石在部分真空下等离子体辅助 CO2 加氢中用作催化剂。研究发现 CO 是该反应的主要产物，它是由等离子体辅助 CO2 在气相中解离产生的。被等离子体振动激发的CO2分子也以甲酸盐的形式吸附在金属镍上，并进一步转化为直链羰基化合物。然后这些物质被氢化形成甲烷。由于催化剂表现出低碱性行为，甲烷是由镍表面上的直链羰基氢化产生的，而不是由碳酸盐物质产生的。使用 Operando 时间分辨 FTIR 光谱数据提出了等离子体（辉光放电）辅助的该反应的详细机制。
Zeolite H-USY doped with nickel (14% wt.) was used as a catalyst in the plasma-assisted CO2 hydrogenation under partial vacuum. CO was found to be the main product of the reaction and it is generated by plasma-assisted CO2 dissociation in the gas phase. The CO2 molecules vibrationally excited by plasma are also adsorbed on metallic nickel as formates which are further transformed into linear carbonyls. These species are then hydrogenated to form methane. Since the catalyst presents a low basic behavior, methane is produced from hydrogenation of linear carbonyls on nickel surface rather than from carbonates species. A detailed mechanism for this reaction assisted by plasma (glow discharge) is proposed using Operando time-resolved FTIR spectroscopic data.