Advanced 3D Hollow-Out ZnZrO@C Combined with Hierarchical Zeolite for Highly Active and Selective CO Hydrogenation to Aromatics

02 engineering and technology 0210 nano-technology 01 natural sciences 0104 chemical sciences
DOI: 10.1021/acscatal.0c01418 Publication Date: 2020-06-05T14:41:00Z
ABSTRACT
Herein, we explore a facile "defect-mediated outward contraction" strategy to fabricate three-dimensional (3D) hollow-out ZnZrO@C (HO-ZnZrO@C) materials by carbonizing local defect-engineered multivariate UiO-66(ZnZr) (MTV-UiO-66(ZnZr)). The defects mainly result from geometrical substitution of distinct Zn secondary building units for Zr counterparts on MTV-UiO-66 crystals. as-synthesized HO-ZnZrO@C catalyst possesses rich surface oxygen vacancies ultrafine ZnZrO nanoparticles, which are confined in robust 3D hierarchical carbon frameworks with open and successive channels. H-ZSM-5 tandem prepared powder mixing not only affords selectivity aromatics up 73.1% but also suppresses the CH4 down 3.4% at CO conversion 35.2%. Particularly, achieve record-high space–time yield 0.302 g goxide–1 h–1 methanol-mediated COx hydrogenation high catalytic stability. 2,6-di-tert-butyl-pyridine adsorption FT-IR results indicate that mode between decreases number external Brønsted acid sites H-ZSM-5, is beneficial selective intermediates aromatics. Our might an avenue rational design highly nanostructures targeted functionalities various advanced applications.
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