The potential of manganese nitride based materials as nitrogen transfer reagents for nitrogen chemical looping

The potential of manganese nitride based materials as nitrogen transfer reagents for nitrogen chemical looping
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DOI:
10.1016/j.apcatb.2017.04.073
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发表时间:
2018-04-01
影响因子:
22.1
通讯作者:
Hargreaves, Justin S. J.
Hargreaves, Justin S. J.
中科院分区:
化学1区
文献类型:
--
作者:
Laassiri, Said;Zeinalipour-Yazdi, Constantinos D.;Hargreaves, Justin S. J.

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对氮化锰相关材料在合成氨中的应用潜力进行了系统的研究。以NaNH_2为活性氮源,通过低温氮化制备A-Mn-N(A= Fe,Co,K,Li)材料。晶格氮的反应性进行了评估,使用氨合成作为模型反应。在Mn 3 N2的情况下,观察到有限的反应性,并且发现仅3.1%的可用晶格氮对氢具有反应性以产生氨,而大部分晶格氮作为N-2损失。然而,共金属的存在在形成氮化锰的氮转移性质中起着关键作用,并且强烈影响其反应性。特别是,掺杂氮化锰与低水平的锂导致在低温下的反应性增强。在Li-Mn-N系统的情况下,在400 ℃下形成的氨的分数对应于总可用晶格氮的15%朝向氢的反应。Li-Mn-N在用氢气还原后呈现出高的热化学稳定性,这限制了使用来自气相的N-2的再生步骤。然而,本文中呈现的结果表明Li-Mn-N系统值得进一步关注。(C)2017作者由爱思唯尔公司出版
A systematic study was carried out to investigate the potential of manganese nitride related materials for ammonia production. A-Mn-N (A= Fe, Co, K, Li) materials were synthesised by nitriding their oxide counterparts at low temperature using NaNH2 as a source of reactive nitrogen. The reactivity of lattice nitrogen was assessed using ammonia synthesis as a model reaction. In the case of Mn3N2, limited reactivity was observed and only 3.1% of the available lattice nitrogen was found to be reactive towards hydrogen to yield ammonia while most of the lattice nitrogen was lost as N-2. However, the presence of a co-metal played a key role in shaping the nitrogen transfer properties of manganese nitride and impacted strongly upon its reactivity. In particular, doping manganese nitride with low levels of lithium resulted in enhanced reactivity at low temperature. In the case of the Li-Mn-N system, the fraction of ammonia formed at 400 degrees C corresponded to the reaction of 15% of the total available lattice nitrogen towards hydrogen. Li-Mn-N presented high thermochemical stability after reduction with hydrogen which limited the regeneration step using N-2 from the gas phase. However, the results presented herein demonstrate the Li-Mn-N system to be worthy of further attention. (C) 2017 The Authors. Published by Elsevier B.V.