Combination of theoretical and in situ experimental investigations of the role of lithium dopant in manganese nitride: a two-stage reagent for ammonia synthesis
Combination of theoretical and in situ experimental investigations of the role of lithium dopant in manganese nitride: a two-stage reagent for ammonia synthesis
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锂掺杂剂在氮化锰中的作用的理论与原位实验相结合：氨合成的两阶段试剂
DOI：
10.1039/c9fd00131j
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发表时间：
2021
影响因子：
3.4
通讯作者：
Laassiri S
中科院分区：
文献类型：
--
作者：
Laassiri S
氮化锰相关材料作为用于通过氮化学循环合成氨的两阶段试剂是令人感兴趣的。然而，除非它们掺杂有共阳离子，否则氮化锰是热化学稳定的，并且需要高温以在还原条件下产生氨，从而阻碍它们用作氮转移材料。然而，当使用锂作为掺杂剂时，可以在低至300 °C的反应温度下观察到氨生成。为了开发用于改进氮化物材料在两阶段试剂的上下文中的反应性的策略，有必要了解掺杂剂在氨合成机理中的内在作用。为此，我们研究了锂在增加氮化锰反应性的作用，通过原位中子衍射研究和N2和H2同位素交换反应补充DFT计算。
Manganese nitride related materials are of interest as two-stage reagents for ammonia synthesis via nitrogen chemical looping. However, unless they are doped with a co-cation, manganese nitrides are thermochemically stable and a high temperature is required to produce ammonia under reducing conditions, thereby hindering their use as nitrogen transfer materials. Nevertheless, when lithium is used as dopant, ammonia generation can be observed at a reaction temperature as low as 300 °C. In order to develop strategies for the improvement of the reactivity of nitride materials in the context of two-stage reagents, it is necessary to understand the intrinsic role of the dopant in the mechanism of ammonia synthesis. To this end, we have investigated the role of lithium in increasing the manganese nitride reactivity by in situ neutron diffraction studies and N2 and H2 isotopic exchange reactions supplemented by DFT calculations.