Volume 34 Issue 3
Jun.  2021
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Hao Lin, Jin-xun Liu, Hong-jun Fan, Wei-xue Li. Crystallographic and Morphological Sensitivity of N2 Activation over Ruthenium[J]. Chinese Journal of Chemical Physics , 2021, 34(3): 263-272. doi: 10.1063/1674-0068/cjcp2009171
Citation: Hao Lin, Jin-xun Liu, Hong-jun Fan, Wei-xue Li. Crystallographic and Morphological Sensitivity of N2 Activation over Ruthenium[J]. Chinese Journal of Chemical Physics , 2021, 34(3): 263-272. doi: 10.1063/1674-0068/cjcp2009171

Crystallographic and Morphological Sensitivity of N2 Activation over Ruthenium

doi: 10.1063/1674-0068/cjcp2009171
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  • Corresponding author: Hong-jun Fan, E-mail: fanhj@dicp.ac.cn; Wei-xue Li, E-mail: wxli70@ustc.edu.cn
  • Received Date: 2020-09-25
  • Accepted Date: 2020-11-17
  • Publish Date: 2021-06-27
  • Ruthenium (Ru) serves as a promising catalyst for ammonia synthesis via the Haber-Bosch process, identification of the structure sensitivity to improve the activity of Ru is important but not fully explored yet. We present here density functional theory calculations combined with micro-kinetic simulations on nitrogen molecule activation, a crucial step in ammonia synthesis, over a variety of hexagonal close-packed (hcp) and face-center cubic (fcc) Ru facets. Hcp $\left\{ {21\overline 3 0} \right\}$ facet exhibits the highest activity toward N$_2$ dissociation in hcp Ru, followed by the (0001) monatomic step sites. The other hcp Ru facets have N$_2$ dissociation rates at least three orders lower. Fcc $\{211\}$ facet shows the best performance for N$_2$ activation in fcc Ru, followed by $\{311\}$, which indicates stepped surfaces make great contributions to the overall reactivity. Although hcp Ru $\left\{ {21\overline 3 0} \right\}$ facet and (0001) monatomic step sites have lower or comparable activation barriers compared with fcc Ru $\{211\}$ facet, fcc Ru is proposed to be more active than hcp Ru for N$_2$ conversion due to the exposure of the more favorable active sites over step surfaces in fcc Ru. This work provides new insights into the crystal structure sensitivity of N$_2$ activation for mechanistic understanding and rational design of ammonia synthesis over Ru catalysts.

     

  • These authors contributed equally to this work.
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