Ammonia synthesis and by-product formation from H2O, H2 and N2 by dielectric barrier discharge combined with an Ru/Al2O3 catalyst

Ammonia synthesis and by-product formation from H2O, H2 and N2 by dielectric barrier discharge combined with an Ru/Al2O3 catalyst
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通过介质阻挡放电与 Ru/Al2O3 催化剂相结合,由 H2O、H2 和 N2 合成氨并形成副产物

DOI:
10.1039/c6ra21351k
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发表时间:
2016-11
期刊:
RSC Advance
影响因子:
--
通讯作者:
Wenhao Yang
Wenhao Yang
中科院分区:
其他
文献类型:
--
作者:
Deyuan Xie;Ye Sun;Tianle Zhu;Xing Fan;Xiaowei Hong;Wenhao Yang

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在常压和室温条件下,研究了Ru/Al2O3催化剂结合介质阻挡放电由H2O + N2、H2 + N2或H2O + H2 + N2合成NH3的方法。研究了反应气体组成、能量密度和放电频率对NH3产率和副产物生成的影响。结果表明,由H2O和N2组成的反应气体可生成NH3。含H2的反应气的NH3产率远高于H2O和N2组成的反应气。H2O的存在对H2和N2合成NH3有促进作用,特别是对于H2含量小于10%的反应气体。NH3产率随能量密度的增加先升高后降低。当能量密度为1400 J L−1,反应气体为0.14% H2O、40% H2和N2时,产率可达680 mg kW−1 h−1。放电频率对NH3产率影响较大,在13 kHz时NH3产率最大。除NH3外,含有H2O的反应气体还会生成N2O和NO2等副产物。然而,在H2的存在下,它们的形成可以被抑制,这是由于H2对副产物的还原作用。
NH3 synthesis from H2O + N2, H2 + N2 or H2O + H2 + N2 by dielectric barrier discharge combined with an Ru/Al2O3 catalyst is studied at atmospheric pressure and room temperature. Additionally, the effects of reaction gas composition, energy density, and discharge frequency on NH3 yield and by-product formation are investigated. The results show that NH3 can be formed from reaction gases consisting of H2O and N2. The NH3 yield of the reaction gas containing H2 is much higher than that of the reaction gas consisting of H2O and N2. The presence of H2O has a promotion effect on NH3 synthesis from H2 and N2, especially for reaction gases with an H2 content less than 10%. The NH3 yield first increases and then decreases with an increase in the energy density. The maximum yield of 680 mg kW−1 h−1 occurs at the energy density of 1400 J L−1 and in the reaction gas of 0.14% H2O, 40% H2 and N2. The discharge frequency has a great effect on the NH3 yield, and maximum NH3 yield is obtained at the frequency of 13 kHz. Besides NH3, some by-products, such as N2O and NO2, are also formed with reaction gases containing H2O. However, their formation can be suppressed in the presence of H2, which is attributed to the reduction effect of H2 on the by-products.
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