Towards anti-perovskite nitrides as potential nitrogen storage materials for chemical looping ammonia production: Reduction of Co3ZnN, Ni3ZnN, Co3InN and Ni3InN under hydrogen
Towards anti-perovskite nitrides as potential nitrogen storage materials for chemical looping ammonia production: Reduction of Co3ZnN, Ni3ZnN, Co3InN and Ni3InN under hydrogen
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DOI：
10.1016/j.cattod.2020.03.022
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发表时间：
2021-03-12
期刊：
影响因子：
5.3
通讯作者：
Hargreaves, J. S. J.
中科院分区：
文献类型：
--
作者：
Goto, Y.;Daisley, A.;Hargreaves, J. S. J.
研究了反钙钛矿氮化物 Co3ZnN、Ni3ZnN、Co3InN 和 Ni3InN 在氢还原时的氨生成特性。通过相应前体氧化物的氨解反应，所有氮化物均制备出具有理想反钙钛矿结构（空间群：Pm-3m）的单相，并且观察到所有氮化物与H-2/Ar反应时均能高产率产生氨。 Co3ZnN、Ni3ZnN、Co3InN和Ni3InN在400℃下的累积氨产值分别为3069、2925、289和1029 μ mol-NH3 g(-1)，释放速率的顺序为Ni3ZnN > Co3ZnN > Ni3InN > Co3InN。 X射线衍射研究表明，Co3ZnN和Co3InN在晶格N损失后分解，而Ni3ZnN和Ni3InN通过中间相Ni3ZnNx和Ni3InNy转化为Ni3Zn和Ni3In。这些中间相的晶体结构与其初始结构相关，表明Ni3ZnN和Ni3InN中晶格N的损失是拓扑定向的。
The ammonia production properties upon reduction in hydrogen of the anti-perovskite nitrides Co3ZnN, Ni3ZnN, Co3InN, and Ni3InN have been investigated. Single phases with ideal anti-perovskite structures (Space group: Pm-3m) were prepared for all the nitrides by the ammonolysis of the corresponding precursor oxides and all the nitrides were observed to produce ammonia in high yields when reacted with H-2/Ar. The cumulative ammonia production values at 400 degrees C were 3069, 2925, 289, and 1029 mu mol-NH3 g(-1) for Co3ZnN, Ni3ZnN, Co3InN, and Ni3InN, respectively and the order of the release rates was Ni3ZnN > Co3ZnN > Ni3InN > Co3InN. X-ray diffraction studies revealed that Co3ZnN and Co3InN decomposed upon the loss of lattice N, whereas Ni3ZnN and Ni3InN were transformed into Ni3Zn and Ni3In via the intermediate phases Ni3ZnNx and Ni3InNy. The crystal structures of these intermediate phases are related to their initial structures, indicating that the loss of lattice N in Ni3ZnN and Ni3InN was topotactic.