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<p>The development of molecular sieve designs capable of achieving high catalytic efficiency in the oxidation of NO to NO₂ while exhibiting notable SO₂ resistance remains a significant scientific and technological challenge. Barium slag (Bs) is abundant in silicates, aluminosilicate minerals, and various active elements (e.g., Fe and Ba), which serve as indispensable precursor for the synthesis of molecular sieves. In this study, a Mn-based bifunctional catalyst supported on Bs–ZSM–5 (designated as MF@BsZ<sub><i>x</i></sub>) was successfully synthesized. This catalyst not only facilitates the oxidation of NO but also exhibits resistance to SO₂ poisoning, consequently enhancing its operational durability and applicability. The primary characterization techniques, including the combination of NO temperature-programmed reduction (NO-TPR) and density functional theory (DFT), were employed to achieve a more in-depth comprehension of the mechanisms underlying NO oxidation and SO₂ resistance. The in situ encapsulation of Mn and Fe species within the Bs–ZSM–5 zeolite promoted the close interaction between acidic and redox-active sites, thereby accelerating the oxidation kinetics of the generated intermediate species. The ample Brønsted acid sites (Mn<sup>4</sup>⁺–O<i>ᵥ</i>–Fe<sup>3</sup>⁺ interfacial sites) promoted the cleavage of O=O bonds and the formation of O–N=O bonds. The preferential adsorption of SO₂ onto barium ions, coupled with the formation of a protective barium sulfate layer, functions to preclude the internal catalytic components from corrosion. This research offers a valuable reference for the high-value utilization of hazardous waste and for resolving the scientific challenges related to molecular sieves sulfur poisoning.</p>

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A facile BaSO₄ surface coated Mn/Barium slag-ZSM–5 bifunctional catalyst with enhanced SO2 resistance for NO oxidation: a dual-protection mechanism

  • 期刊论文

  • 发表日期：

    2026年4月7日

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  • Yadong Wu,
  • JinJuan Li

摘要

The development of molecular sieve designs capable of achieving high catalytic efficiency in the oxidation of NO to NO₂ while exhibiting notable SO₂ resistance remains a significant scientific and technological challenge. Barium slag (Bs) is abundant in silicates, aluminosilicate minerals, and various active elements (e.g., Fe and Ba), which serve as indispensable precursor for the synthesis of molecular sieves. In this study, a Mn-based bifunctional catalyst supported on Bs–ZSM–5 (designated as MF@BsZx) was successfully synthesized. This catalyst not only facilitates the oxidation of NO but also exhibits resistance to SO₂ poisoning, consequently enhancing its operational durability and applicability. The primary characterization techniques, including the combination of NO temperature-programmed reduction (NO-TPR) and density functional theory (DFT), were employed to achieve a more in-depth comprehension of the mechanisms underlying NO oxidation and SO₂ resistance. The in situ encapsulation of Mn and Fe species within the Bs–ZSM–5 zeolite promoted the close interaction between acidic and redox-active sites, thereby accelerating the oxidation kinetics of the generated intermediate species. The ample Brønsted acid sites (Mn4⁺–Oᵥ–Fe3⁺ interfacial sites) promoted the cleavage of O=O bonds and the formation of O–N=O bonds. The preferential adsorption of SO₂ onto barium ions, coupled with the formation of a protective barium sulfate layer, functions to preclude the internal catalytic components from corrosion. This research offers a valuable reference for the high-value utilization of hazardous waste and for resolving the scientific challenges related to molecular sieves sulfur poisoning.