<p>Direct catalytic decomposition is one of the green methods for N<sub>2</sub>O elimination. However, the activity of catalyst is limited by the slow oxygen desorption rate and the unsatisfactory electronic structure of the active site. In this work, Fe species were introduced into Co/β catalyst to regulate the microstructure of Co active sites and oxygen desorption pathways. A combination of characterization techniques such as XRD, TEM, XPS, DR UV–Vis, etc were employed to elucidate the nature of Co and Fe species in the catalysts. The results demonstrated that the introduction of Fe not only reduced the particle size of CoO<sub>x</sub> species, but also effectively improved the reducibility and deoxygenation capacity of the catalysts. Moreover, in-situ FT-IR and N<sub>2</sub>O-TPD experiments revealed that the oxidization of N<sub>2</sub>O to NO and the decomposition of nitrate species were significantly enhanced over Fe doped Co/β catalyst, thereby facilitated the NO-assisted oxygen desorption process during N<sub>2</sub>O decomposition. As a result, the N<sub>2</sub>O conversion at 420 °C was elevated from 85% of Co/β catalyst to 100% of 1.0Fe-Co/β catalyst, which is much higher than the 22% conversion achieved over Fe/β catalyst. This work could provide the reference for the design of N<sub>2</sub>O decomposition catalysts and understanding of catalytic reaction mechanism.</p><p></p>

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Enhancing NO-assisted oxygen desorption for efficient N2O decomposition by introducing iron into Co/β catalysts

  • Liangliang Zhang,
  • Minxia Yang,
  • Shize Hu,
  • Ruifang Wu,
  • Jiajun Ma,
  • Hui Dang,
  • Ke Zheng,
  • Xiangqian Lin,
  • Yongzhao Wang

摘要

Direct catalytic decomposition is one of the green methods for N2O elimination. However, the activity of catalyst is limited by the slow oxygen desorption rate and the unsatisfactory electronic structure of the active site. In this work, Fe species were introduced into Co/β catalyst to regulate the microstructure of Co active sites and oxygen desorption pathways. A combination of characterization techniques such as XRD, TEM, XPS, DR UV–Vis, etc were employed to elucidate the nature of Co and Fe species in the catalysts. The results demonstrated that the introduction of Fe not only reduced the particle size of CoOx species, but also effectively improved the reducibility and deoxygenation capacity of the catalysts. Moreover, in-situ FT-IR and N2O-TPD experiments revealed that the oxidization of N2O to NO and the decomposition of nitrate species were significantly enhanced over Fe doped Co/β catalyst, thereby facilitated the NO-assisted oxygen desorption process during N2O decomposition. As a result, the N2O conversion at 420 °C was elevated from 85% of Co/β catalyst to 100% of 1.0Fe-Co/β catalyst, which is much higher than the 22% conversion achieved over Fe/β catalyst. This work could provide the reference for the design of N2O decomposition catalysts and understanding of catalytic reaction mechanism.