Lattice Oxygen Activation Triggered by Ultrasonic Shock Significantly Improves NO Selective Catalytic Reduction

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL
Yan Wang, Baiyun Zhu, Songil Sin, Zhiqiang Zhang, Chong Tan, Zhiwen Gu, Wang Song, Chunkai Huang, Meilin Tao*, Chenghua Zhang, Changjin Tang* and Lin Dong, 
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Abstract

The precise regulation of lattice oxygen is crucial for many redox reactions, but it still remains a formidable challenge. Herein, we reported a facile strategy to induce generation of bulk phase defects in hematite (α-Fe2O3) by ultrasonic treatment, thus achieving exclusive lattice oxygen activation without additional alternation of surface adsorbed oxygen species. This kind of unique lattice oxygen activation afforded negligible disturbance of NH3 adsorption but significant influence on NO2 generation via accelerated oxygen diffusion, resulting in enhanced activity contribution from the Fast-SCR reaction pathway. Particularly, the generation of bulk-phase defects was also found to be conducive to create thermally instable and chemically reactive surface nitrate species, which played a decisive role in activating NO reactant. Accordingly, a triple increment in the deNOx performance of the α-Fe2O3 catalyst for the reaction of selective catalytic reduction of NO with NH3 (NH3–SCR) was achieved.

Abstract Image

Abstract Image

超声波冲击引发的晶格氧活化可显著提高氮氧化物的选择性催化还原能力
晶格氧的精确调节对许多氧化还原反应至关重要,但它仍然是一项艰巨的挑战。在此,我们报告了一种简便的策略,即通过超声波处理诱导赤铁矿(α-Fe2O3)产生体相缺陷,从而实现完全的晶格氧活化,而无需额外的表面吸附氧物种交替。这种独特的晶格氧活化对 NH3 吸附的干扰可以忽略不计,但通过加速氧扩散对 NO2 生成的影响却很大,从而提高了快速 SCR 反应途径的活性贡献。特别是,研究还发现,体相缺陷的产生有利于产生热不稳定和化学反应性强的表面硝酸盐物种,这在激活 NO 反应物方面起着决定性作用。因此,α-Fe2O3 催化剂在选择性催化还原 NO 与 NH3(NH3-SCR)反应中的脱硝性能提高了三倍。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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