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Twisted Surfaces in Porous Single Crystals to Deliver Enhanced Catalytic Activity and Stability.
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-06-02 , DOI: 10.1002/anie.202006299
Guoming Lin 1 , Hao Li 1 , Kui Xie 1, 2, 3
Affiliation  

Porous single crystals which combine ordered lattice structures and disordered inter‐connected pores would provide an alternative to create twisted surface in porous microstructures. Now, transition‐metal nitride Nb4N5 and MoN single crystals are grown on a 2 cm scale to create well‐defined active structures at twisted surfaces. High catalytic activity and stability toward non‐oxidative dehydrogenation of ethane to ethylene is observed. Unsaturated metal–nitrogen coordination structures including Nb‐N1/5, Nb‐N2/5, Mo‐N1/3, and Mo‐N1/6 at the twisted surface mainly account for the C−H activation with chemisorption of H in molecular ethane at the twisted surface, which not only improves dehydrogenation performance but also avoids the deep cracking of ethane to enhance coking resistance. 11–25 % ethane conversion and 98–99 % ethylene selectivity is demonstrated without degradation being observed even after the operation of 50 hours.

中文翻译:

多孔单晶中的扭曲表面可提供增强的催化活性和稳定性。

结合有序晶格结构和无序互连孔的多孔单晶将为在多孔微结构中产生扭曲的表面提供另一种选择。现在,过渡金属氮化物Nb 4 N 5和MoN单晶以2 cm的规模生长,以在扭曲的表面上创建清晰的有源结构。观察到较高的催化活性和乙烷对乙烷非氧化脱氢的稳定性。不饱和金属-氮配位结构,包括Nb-N 1/ 5,Nb-N 2/ 5,Mo-N 1/3和Mo-N 1/6在扭曲的表面上,主要是由于扭曲表面上的分子乙烷中H的化学吸附导致了CH活化,这不仅提高了脱氢性能,而且避免了乙烷的深度裂化,从而提高了耐焦化性。在运行50小时后,乙烷转化率为11–25%,乙烯选择性为98–99%,未观察到降解。
更新日期:2020-06-02
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