<p>In this paper, the effects of silica-alumina ratio and copper loading on the performance of Cu-SSZ-13 molecular sieve catalysts in selective catalytic reduction (SCR) reaction were investigated. The differences in NO<sub>x</sub> conversion, N<sub>2</sub> selectivity, NH<sub>3</sub> adsorption performance, and reaction mechanism were systematically analyzed by preparing Cu-SSZ-13 catalysts with different silica-to-aluminum ratios (9, 20, and 30) and copper loadings (0.1&#xa0;mol/L and 0.075&#xa0;mol/L). It was found that catalysts with lower silica-to-aluminum ratio (e.g., SAR9-Cu0.1) had more Brønsted acid sites (B-acid sites), which could provide more active sites for Cu ion exchange and NH<sub>3</sub> adsorption, and thus exhibited higher SCR catalytic activity and N<sub>2</sub> selectivity. The increase in Cu loading also helps to increase the number of active sites of the catalyst, which further enhances the NO<sub>x</sub> conversion efficiency of the catalyst. The adsorption characteristics of NH<sub>3</sub> on the catalyst surface, the formation and conversion process of nitrate species, and the mechanism of the effect of different Si/Al ratios and copper loadings on the catalyst performance were revealed by means of the characterization of NH<sub>3</sub>-TPD, NH<sub>3</sub>-TPO,XPS,XRD,BET,Pyridine infrared and in situ DRIFTS. The results show that the bridged nitrate has good thermal stability at high temperature and exhibits high activity in the reaction with NH<sub>3</sub>. This study provides a theoretical basis for optimizing the design of Cu-SSZ-13 catalyst and its practical application in diesel exhaust treatment.</p> Graphic abstract <p></p>

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Effect of silicon-aluminum ratio and copper load on the catalyst performance of Cu-SSZ-13 molecular sieve

  • Bin Guan,
  • Kaiyou Shu,
  • Lei Zhu,
  • Tiankui Zhu,
  • Zhongqi Zhuang,
  • Xuehan Hu,
  • Chenyu Zhu,
  • Sikai Zhao,
  • Junyan Chen,
  • Junjie Gao,
  • Hongtao Dang,
  • Luyang Zhang,
  • Yuan Li,
  • Luoxin Xu,
  • Wenbo Zeng,
  • Shuai Chen,
  • Linhui Wang,
  • Can Zhu,
  • Jiaming He,
  • Qinghan Xian,
  • Zhen Huang

摘要

In this paper, the effects of silica-alumina ratio and copper loading on the performance of Cu-SSZ-13 molecular sieve catalysts in selective catalytic reduction (SCR) reaction were investigated. The differences in NOx conversion, N2 selectivity, NH3 adsorption performance, and reaction mechanism were systematically analyzed by preparing Cu-SSZ-13 catalysts with different silica-to-aluminum ratios (9, 20, and 30) and copper loadings (0.1 mol/L and 0.075 mol/L). It was found that catalysts with lower silica-to-aluminum ratio (e.g., SAR9-Cu0.1) had more Brønsted acid sites (B-acid sites), which could provide more active sites for Cu ion exchange and NH3 adsorption, and thus exhibited higher SCR catalytic activity and N2 selectivity. The increase in Cu loading also helps to increase the number of active sites of the catalyst, which further enhances the NOx conversion efficiency of the catalyst. The adsorption characteristics of NH3 on the catalyst surface, the formation and conversion process of nitrate species, and the mechanism of the effect of different Si/Al ratios and copper loadings on the catalyst performance were revealed by means of the characterization of NH3-TPD, NH3-TPO,XPS,XRD,BET,Pyridine infrared and in situ DRIFTS. The results show that the bridged nitrate has good thermal stability at high temperature and exhibits high activity in the reaction with NH3. This study provides a theoretical basis for optimizing the design of Cu-SSZ-13 catalyst and its practical application in diesel exhaust treatment.

Graphic abstract