Mechanistic aspects of plasma-enhanced catalytic methane decomposition by time-resolved operando diffuse reflectance infrared Fourier transform spectroscopy
Mechanistic aspects of plasma-enhanced catalytic methane decomposition by time-resolved operando diffuse reflectance infrared Fourier transform spectroscopy
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时间分辨操作漫反射红外傅里叶变换光谱等离子体增强催化甲烷分解的机理
DOI：
10.1088/1361-6463/ab795b
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Oehrlein, G. S.
中科院分区：
文献类型：
--
作者：
Zhang, S.;Li, Y.;Knoll, A.;Oehrlein, G. S.
为了研究等离子体增强催化反应的机理，采用Ar/O2常压等离子体射流（APPJ）辅助负载型Ni催化剂对甲烷进行催化分解。时间分辨的Ni催化剂的表面响应的研究，通过操作漫反射红外傅里叶变换光谱（DRIFTS）使用各种实验设置。考察了室温和500 ℃的催化剂温度以及3、5和8 mm的筛-催化剂表面距离，流过APPJ的Ar/O2气体混合物的O2量为0或0.5%。在暴露的镍催化剂的APPJ低氧操作条件（纯Ar射流）的过程中观察到的表面键合的C-O的协同效应。只有当存在等离子体时才形成表面键合的C-O，并且C-O信号随着催化剂温度的升高而增强。当负载型Ni催化剂经受使用高度氧化条件的等离子体产生的颗粒通量时，抑制了表面键合的C-O的存在。当等离子体源操作条件在高催化剂温度（500 C）下从低氧部分改变为高氧部分时，下游测量的气相中的等离子体催化CO和CO2产生反映了C-O键的表面行为。用DRIFTS研究了催化剂表面的CH n（n= 1，2，3）物种，发现CH n的破坏与C-O的形成有关.特别是，时间分辨的CH n响应表明，当Ni催化剂暴露于等离子体源时，CH n到C-O的可能的转化过程。这一发现可能表明等离子体介导的再生催化剂的等离子体-催化剂表面相互作用。
To study mechanistic aspects of plasma-enhanced catalysis, methane is decomposed by a supported Ni catalyst assisted by an Ar/O 2 atmospheric pressure plasma jet (APPJ). The time-resolved surface response of the Ni catalyst is investigated by operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) using various experimental settings. Catalyst temperatures of room temperature and 500 C and nozzle-catalyst surface distances of 3, 5 and 8 mm were examined, and the amount of O 2 of the Ar/O 2 gas mixture flowing through the APPJ was either 0 or 0.5%. A synergistic effect of surface bonded C–O was observed during the exposure of the Ni catalyst to the APPJ for low oxygen operating conditions (pure Ar jet). Surface bonded C–O formed only when there was plasma present and the C–O signal was enhanced for higher catalyst temperature. When the supported Ni catalyst was subjected to the plasma-generated particle fluxes using highly oxidizing conditions, the presence of surface bonded C–O was suppressed. The plasma-catalytic CO and CO 2 production in the gas phase measured downstream mirrored the surface behavior of C–O bonds when the plasma source operating condition was changed from a low oxygen portion to a high oxygen portion at high catalyst temperature (500 C). CH n (n= 1, 2, 3) species on the catalyst surface were also studied by DRIFTS, and CH n destruction was found to correlate with C–O formation. In particular, the time-resolved CH n response showed a possible conversion process of CH n to C–O when the Ni catalyst was exposed to the plasma source. This finding may indicate a plasma-mediated regeneration of the catalyst by plasma-catalyst surface interactions.
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影响因子：
3.4
作者：
Knoll, A. J.;Zhang, S.;Oehrlein, G. S.
通讯作者：
Oehrlein, G. S.
酰胺、蛋白质和多肽
DOI：
10.1007/978-94-011-6017-9_12
发表时间：
1975
期刊：
Journal of Physics D: Applied Physics
影响因子：
--
作者：
L. J. Bellamy
通讯作者：
L. J. Bellamy
影响因子：
3.6
作者：
Azzolina-Jury, Federico;Thibault-Starzyk, Frederic
通讯作者：
Thibault-Starzyk, Frederic
硫化Ni-W/Al2O3加氢处理催化剂的一氧化碳和氧化学吸附及其功能
影响因子：
5.3
作者：
J. Duchet;J. Lavalley;Saïd Housni;D. Ouafi;J. Bachelier;M. Lakhdar;A. Mennour;D. Cornet
通讯作者：
D. Cornet