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Ammonia is a carbon-free hydrogen carrier, and development of non-noble metal catalyst to decompose ammonia into hydrogen is desirable for practical applications. However, the metal catalyst is challenged by the sintering of metal particles under high-temperature reaction conditions. In this study, a series of Li-, Al-, and Co-containing hydrotalcite-like compounds (HTlc) were synthesized by co-precipitation and used as precursors to prepare well-dispersed and thermally stable Co nanoparticle catalysts for ammonia decomposition. The obtained precursors and catalysts were characterized by means of X-ray powder diffraction (XRD), temperature-programmed reduction (H-2-TPR), X-ray photoelectron spectroscopy (XPS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and so on. All of the precursors formed hydrotalcite-like phase, which consisted of Li-Al-(Co) HTlc and/or Co-Al HTlc dependent on the Co content. Upon calcination at 500 degrees C, HTlc decomposed into an Al-substituted Co3O4 spinel oxide, as confirmed by two distinctly separated reduction steps in H-2-TPR. Following reduction at 700 degrees C, well-dispersed Co metal nanoparticles with an average particle size of similar to 9.2-12.4 nm were obtained. It was suggested that the incorporation of Al3+ into Co3O4 led to a strong interaction between cobalt and aluminum, which suppressed the crystal growth of Co3O4 and the sintering of Co metal during the thermal treatments, resulting in good Co dispersion. The optimal LiAlCo(1.5) catalyst showed superior activity than that prepared by impregnation method, giving almost complete conversion of ammonia at 575 degrees C under a space velocity of 5,000 mL g(cat)(-1) h(-1). More importantly, this catalyst maintained stable activity at 625 degrees C for 100 h, exhibiting high stability and sintering resistance. The good catalytic performance was attributed to the high Co metal dispersion and strong metal-support interaction benefiting from the uniform distribution of cobalt in the HTlc precursor. These results demonstrate the applicability of HTlc to the preparation of metal catalysts with improved dispersion and thermal stability.
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MOLECULAR CATALYSIS
ISSN: 2468-8231
Year: 2025
Volume: 572
3 . 9 0 0
JCR@2023
Cited Count:
WoS CC Cited Count: 1
SCOPUS Cited Count: 1
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
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