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Impact of Pressure and Hydrogen Dilution on the Kinetics of Methane Decomposition in AC-Excited, High Pressure Plasmas
Plasma Chemistry and Plasma Processing ( IF 3.6 ) Pub Date : 2023-10-31 , DOI: 10.1007/s11090-023-10416-w
Norleakvisoth Lim , Yu Wu , Michael J. Gordon

The kinetics of methane decomposition in low frequency (60 Hz) AC arc plasmas was investigated using on-line mass spectrometry and optical emission spectroscopy (OES) in a batch reactor configuration at pressures up to 3 bar absolute. Plasma conversion of CH4 results largely from thermal dissociation and was seen to follow first-order kinetics up to high conversions (> 90%) without observing any rate impedance from reverse hydrocracking. H– and C-atom selectivities for H2, C2H2, and C2H4 were 78% (1.56 mol H2/mol CH4 reacted), 36% (0.18 mol C2H2/mol CH4), and 30% (0.15 mol C2H4/mol CH4), respectively, at 3 bar. In other experiments, H2 diluent concentration played an important role in CH4 dissociation and final product distributions; H abstraction reactions increased the rate of CH4 decomposition at low H2 (yH2 < 0.6) while high H2 (yH2 > 0.6) impeded CH4 decomposition due to hydrocracking of C2 products. The rate of CH4 dissociation was seen to increase with pressure, up to 0.11 mol/m3/s, and the specific energy requirement (SER) decreased with pressure to 365 kJ/mol CH4 at 3 bar. The latter suggests that even higher operating pressures may improve the efficiency of plasma conversion of CH4, and ultimately that plasma pyrolysis may be a viable and energy efficient route to clean (turquoise) H2 and further implementation of chemical process electrification.



中文翻译:

压力和氢气稀释对交流激励高压等离子体中甲烷分解动力学的影响

在间歇式反应器配置中,在绝对压力高达 3 bar 的情况下,使用在线质谱和光学发射光谱 (OES) 研究了低频 (60 Hz) 交流电弧等离子体中甲烷分解的动力学。CH 4的等离子体转化主要源自热解离,并且被认为遵循一级动力学直至高转化率(> 90%),而没有观察到来自反向加氢裂化的任何速率阻抗。H 2、C 2 H 2和C 2 H 4的H-和C-原子选择性为78%(1.56 mol H 2 /mol CH 4反应)、36%(0.18 mol C 2 H 2 /mol CH 4) 、和30%(0.15 mol C 2 H 4 /mol CH 4),分别在3巴下。在其他实验中,H 2稀释剂浓度对CH 4解离和最终产物分布起着重要作用。H提取反应在低H 2 (y H2 < 0.6)下增加CH 4分解速率 ,而高H 2 (y H2 > 0.6)由于C 2产物的加氢裂化而 阻碍CH 4分解。观察到CH 4解离速率随压力增加,高达0.11 mol/m 3 /s,并且比能量需求(SER)随压力降低至3巴下的365 kJ/mol CH 4 。后者表明,甚至更高的操作压力可以提高CH 4的等离子体转化效率,并且最终等离子体热解可能是获得清洁(绿松石色)H 2并进一步实现化学过程电气化的可行且节能的途径。

更新日期:2023-11-01
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