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On the possibility of an Eley–Rideal mechanism for ammonia synthesis on Mn6N5+x (x = 1)-(111) surfaces†
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-06-25 00:00:00 , DOI: 10.1039/c8cp02381f Constantinos D. Zeinalipour-Yazdi 1, 2, 3, 4, 5
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-06-25 00:00:00 , DOI: 10.1039/c8cp02381f Constantinos D. Zeinalipour-Yazdi 1, 2, 3, 4, 5
Affiliation
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Recently we reported an Eley–Rideal/Mars–van Krevelen mechanism for ammonia synthesis on cobalt molybdenum nitride (Co3Mo3N). In this mechanism hydrogenation of activated dinitrogen occurs directly from the gas phase in a low barrier step forming a hydrazinylidene intermediate ![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
NNH2. In this paper we study whether such a mechanism of ammonia synthesis could occur on the (111) surface of another metal nitride, Mn6N5+x (x = 1), as this would explain the low-T ammonia synthesis activity of Co3Mo3N. We find that although N2 adsorbs more strongly than H2 on the (111) surface, having also examined the (110) and the (100) surface, N2 is not significantly activated when adsorbed in an end-on configuration. The hydrogenation reactions via an Eley–Rideal mechanism are all high barrier processes (>182 kJ mol−1) and therefore an Eley–Rideal mechanism for ammonia synthesis is predicted to not occur on this material unless there are high temperatures. Our study indicates that the fact that an Eley–Rideal/Mars–van Krevelen mechanism occurs on Co3Mo3N is a result of the stronger activation of dinitrogen at nitrogen vacancies when dinitrogen is adsorbed in an end-on configuration.
中文翻译：
关于在Mn 6 N 5+ x（x = 1）-（111）表面上合成氨的Eley-Rideal机制的可能性†
最近，我们报道了在氮化钴钼（Co 3 Mo 3 N）上合成氨的Eley-Rideal / Mars-van Krevelen机理。在这种机理下，活化的二氮的氢化直接在低势垒步骤中从气相发生，形成了氢化亚苄基中间体NNH 2。在本文中，我们研究了这种氨合成机理是否可能在另一种金属氮化物Mn 6 N 5+ x（x = 1）的（111）表面上发生，因为这可以解释Co的低T氨合成活性。3莫3 N.我们发现，作为n 2吸附比更强烈^ h 2在同样检查了（110）和（100）表面的（111）表面上，当N 2以末端构型吸附时，N 2未被显着活化。通过Eley-Rideal机理进行的氢化反应都是高阻隔过程（> 182 kJ mol -1），因此，除非有高温，否则预计在这种材料上不会发生氨合成的Eley-Rideal机理。我们的研究表明，在Co 3 Mo 3 N上发生Eley-Rideal / Mars-van Krevelen机理的事实是，当以末端形式吸附二氮时，氮空位处的二氮具有更强的活化性。
更新日期：2018-06-25
NNH2. In this paper we study whether such a mechanism of ammonia synthesis could occur on the (111) surface of another metal nitride, Mn6N5+x (x = 1), as this would explain the low-T ammonia synthesis activity of Co3Mo3N. We find that although N2 adsorbs more strongly than H2 on the (111) surface, having also examined the (110) and the (100) surface, N2 is not significantly activated when adsorbed in an end-on configuration. The hydrogenation reactions via an Eley–Rideal mechanism are all high barrier processes (>182 kJ mol−1) and therefore an Eley–Rideal mechanism for ammonia synthesis is predicted to not occur on this material unless there are high temperatures. Our study indicates that the fact that an Eley–Rideal/Mars–van Krevelen mechanism occurs on Co3Mo3N is a result of the stronger activation of dinitrogen at nitrogen vacancies when dinitrogen is adsorbed in an end-on configuration.
中文翻译：
关于在Mn 6 N 5+ x（x = 1）-（111）表面上合成氨的Eley-Rideal机制的可能性†
最近，我们报道了在氮化钴钼（Co 3 Mo 3 N）上合成氨的Eley-Rideal / Mars-van Krevelen机理。在这种机理下，活化的二氮的氢化直接在低势垒步骤中从气相发生，形成了氢化亚苄基中间体
NNH 2。在本文中，我们研究了这种氨合成机理是否可能在另一种金属氮化物Mn 6 N 5+ x（x = 1）的（111）表面上发生，因为这可以解释Co的低T氨合成活性。3莫3 N.我们发现，作为n 2吸附比更强烈^ h 2在同样检查了（110）和（100）表面的（111）表面上，当N 2以末端构型吸附时，N 2未被显着活化。通过Eley-Rideal机理进行的氢化反应都是高阻隔过程（> 182 kJ mol -1），因此，除非有高温，否则预计在这种材料上不会发生氨合成的Eley-Rideal机理。我们的研究表明，在Co 3 Mo 3 N上发生Eley-Rideal / Mars-van Krevelen机理的事实是，当以末端形式吸附二氮时，氮空位处的二氮具有更强的活化性。
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