Mechanocatalytic Ammonia Synthesis over TiN in Transient Microenvironments,ACS Energy Letters

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Mechanocatalytic Ammonia Synthesis over TiN in Transient Microenvironments
ACS Energy Letters ( IF 19.3 ) Pub Date : 2020-10-08 , DOI: 10.1021/acsenergylett.0c01895
Andrew W. Tricker _{1,

2} , Karoline L. Hebisch ₁ , Marco Buchmann ₃ , Yu-Hsuan Liu ₄ , Marcus Rose ₃ , Eli Stavitski ₅ , Andrew J. Medford ₁ , Marta C. Hatzell ₆ , Carsten Sievers _{1,

2}

Affiliation

Environmentally friendly and energy-efficient ways to produce ammonia are essential to meet global food demands. Here, a new approach for ammonia production at nominally ambient conditions is introduced. As proof of concept, ammonia is synthesized mechanocatalytically by ball milling titanium in a continuous gas flow. The ammonia synthesis reaction is proposed to follow a transient Mars–van Krevelen mechanism under mechanically activated conditions, where molecular nitrogen incorporation into the titanium lattice and titanium nitride hydrogenation occur in thermodynamically distinct environments. X-ray powder diffraction and X-ray absorption spectroscopy confirm the formation of titanium nitride from titanium and N₂. The reactivity of nitrided titanium supports that lattice nitrogen plays a role in ammonia formation. The in situ formed titanium nitride is catalytically active, and the nitride regeneration reaction is determined to be the rate-limiting step. A preliminary technoeconomic analysis shows that this approach could be feasible for distributed ammonia production.

中文翻译：

瞬态微环境中TiN上的机械催化氨合成

生产氨的环保和节能方式对于满足全球食品需求至关重要。在此，介绍了一种在名义环境条件下生产氨的新方法。作为概念上的证明，氨是通过在连续气流中球磨钛而机械催化合成的。提出了氨合成反应应遵循在机械活化条件下的瞬时Mars-van Krevelen机理，其中分子氮掺入钛晶格和氮化钛氢化发生在热力学上不同的环境中。X射线粉末衍射和X射线吸收光谱证实由钛和N ₂形成氮化钛。氮化钛的反应性支持晶格氮在氨形成中起作用。在原位形成的氮化钛是催化活性的，并且氮化物再生反应被确定为限速步骤。初步的技术经济分析表明，这种方法对于分布式氨生产是可行的。

更新日期：2020-11-13

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