Atmospheric-pressure nonthermal plasma synthesis of ammonia over ruthenium catalysts

Atmospheric-pressure nonthermal plasma synthesis of ammonia over ruthenium catalysts
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DOI:
10.1002/ppap.201600157
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发表时间:
2017-06-01
影响因子:
3.5
通讯作者:
Nanba, Tetsuya
Nanba, Tetsuya
中科院分区:
物理与天体物理3区
文献类型:
--
作者:
Kim, Hyun-Ha;Teramoto, Yoshiyuki;Nanba, Tetsuya

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采用大气压低温等离子体技术,在钌催化剂上进行了氮氢合成氨的研究。NH_3在N_2-H_2混合物中的形成改变了等离子体的特性,这是由于NH_3的电离势很低(10.15eV)。发现最佳气体比率为N-2:H-2=4:1(按体积计)(即,富N-2条件)。当等离子体在低于250 ℃的温度下操作时,NH3浓度随着比输入能量(SIE)的增加而线性增加。对于Ru(2)-Mg(5)/-Al 2 O3催化剂,在250 ℃下,脉冲振荡的效率是AC振荡情况的四倍。发现RuO 2的存在有利于通过等离子体催化合成NH3。发现加入少量O-2对失活催化剂的原位再生是有效的。金属助剂的作用顺序为Mg>K>Cs>无助剂。
Atmospheric-pressure nonthermal plasma was used to synthesize ammonia from nitrogen and hydrogen over ruthenium catalysts. Formation of NH3 in a N-2-H-2 mixture altered the plasma characteristics due to the low ionization potential of NH3 (10.15eV). The optimum gas ratio was found at N-2:H-2=4:1 by volume (i.e., N-2-rich conditions). When plasma was operated at a temperature below 250 degrees C, the NH3 concentration increased linearly with increasing specific input energy (SIE). For the Ru(2)-Mg(5)/-Al2O3 catalyst at 250 degrees C, pulse energization was four times more efficient than the AC energization case. The presence of RuO2 was found to be beneficial for the NH3 synthesis via plasma-catalysis. The addition of a small amount of O-2 was found to be effective for the in situ regeneration of the deactivated catalyst. The effect of metal promoters was in the order of Mg>K>Cs>no promoter.