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Synergistic Effect of (110) Facets and Oxygen Vacancies in Ru/CeO2 Nanorods for Low-Temperature Ammonia Decomposition
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DOI:10.1002/cctc.70881.png)
Abstract
En 中文
Developing highly active catalysts for low-temperature ammonia decomposition is crucial for generating COx-free hydrogen, yet the reaction is fundamentally limited by sluggish N2 desorption kinetics. This study systematically uncovers the facet-dependent electronic interplay between Ru and CeO2 supported by tuning their nanoscale morphologies into five distinct shapes: rod, hollow sphere, broom, irregular particle, and cube. Among these, the rod-shaped Ru/CeO2 catalyst (Ru/CeO2-r) demonstrates exceptional low-temperature activity, achieving 100% NH3 conversion at 450°C and a remarkable hydrogen production rate of 840 mmol·gcat−1·h−1. Combined experimental characterizations and Density Functional Theory (DFT) calculations identify N2 desorption as the rate-determining step and reveal the underlying catalytic mechanism. The preferential exposure of the (110) facet on the rod morphology features a lower oxygen vacancy formation energy, which facilitates the transfer of abundant electrons from the CeO2 support to the Ru active sites, thereby lowering the valence state. This localized enhancement of the electron cloud density upon Ru effectively accelerates the recombinative desorption of N2, thereby unlocking superior catalytic performance. These findings provide a compelling structural and electronic design rationale for developing highly efficient Ru-based catalysts for hydrogen energy applications.
Keywords:
ammonia decomposition
crystal facet
electron density
hydrogen production
Ru/CeO2 catalyst
ruthenium
supported catalysts
Journal
IF:
3.9
Papers:
9.4K
Citations:
2.5W
