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多孔单晶中的扭曲表面可提供增强的催化活性和稳定性。

Twisted Surfaces in Porous Single Crystals to Deliver Enhanced Catalytic Activity and Stability.

作者信息

Lin Guoming, Li Hao, Xie Kui

机构信息

Key Laboratory of Optoelectronic Materials Chemistry and Physics, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.

Key Laboratory of Design & Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, China.

出版信息

Angew Chem Int Ed Engl. 2020 Sep 14;59(38):16440-16444. doi: 10.1002/anie.202006299. Epub 2020 Jul 10.

Abstract

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 Nb N 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-N , Nb-N , Mo-N , and Mo-N 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.

摘要

将有序晶格结构与无序相互连接的孔隙相结合的多孔单晶,将为在多孔微结构中创建扭曲表面提供一种替代方案。现在,过渡金属氮化物NbN和MoN单晶在2厘米尺度上生长,以在扭曲表面创建明确的活性结构。观察到对乙烷非氧化脱氢制乙烯具有高催化活性和稳定性。扭曲表面上包括Nb-N、Nb-N、Mo-N和Mo-N的不饱和金属-氮配位结构主要负责在扭曲表面上通过分子乙烷中H的化学吸附进行C-H活化,这不仅提高了脱氢性能,还避免了乙烷的深度裂解以增强抗结焦性。即使在运行50小时后也未观察到降解,证明乙烷转化率为11-25%,乙烯选择性为98-99%。

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