Mechanocatalytic Ammonia Synthesis over TiN in Transient Microenvironments
Mechanocatalytic Ammonia Synthesis over TiN in Transient Microenvironments
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DOI：
10.1021/acsenergylett.0c01895
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发表时间：
2020-11-13
影响因子：
22
通讯作者：
Sievers, Carsten
中科院分区：
文献类型：
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作者：
Tricker, Andrew W.;Hebisch, Karoline L.;Sievers, Carsten
环保和节能的氨生产方式对于满足全球粮食需求至关重要。在这里，介绍了一种在标称环境条件下生产氨的新方法。作为概念的证明，通过在连续气流中球磨钛来机械催化合成氨。提出氨合成反应在机械活化条件下遵循瞬态Mars-货车Krevelen机理，其中分子氮掺入钛晶格和氮化钛氢化在化学上不同的环境中发生。X射线粉末衍射和X射线吸收光谱证实了由钛和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。原位形成的氮化钛具有催化活性，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，该方法用于分布式合成氨生产是可行的。
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 N-2. 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.