Influence of Solvent on Selective Catalytic Reduction of Nitrogen Oxides with Ammonia over Cu-CHA Zeolite

化学 催化作用 溶剂 选择性催化还原 反应性(心理学) 沸石 催化循环 分子 无机化学 光化学 反应机理 漫反射红外傅里叶变换 质子溶剂 红外光谱学 有机化学 替代医学 病理 医学 光催化
作者
Jamal Abdul Nasir,Jingcheng Guan,Thomas W. Keal,Alec W. Desmoutier,You Lü,Andrew M. Beale,C. Richard A. Catlow,Alexey A. Sokol
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:145 (1): 247-259 被引量:26
标识
DOI:10.1021/jacs.2c09823
摘要

The copper-exchanged zeolite Cu-CHA has received considerable attention in recent years, owing to its application in the selective catalytic reduction (SCR) of NOx species. Here, we study the NH3-SCR reaction mechanism on Cu-CHA using the hybrid quantum mechanical/molecular mechanical (QM/MM) technique and investigate the effects of solvent on the reactivity of active Cu species. To this end, a comparison is made between water- and ammonia-solvated and bare Cu species. The results show the promoting effect of solvent on the oxidation component of the NH3-SCR cycle since the formation of important nitrate species is found to be energetically more favorable on the solvated Cu sites than in the absence of solvent molecules. Conversely, both solvent molecules are predicted to inhibit the reduction component of the NH3-SCR cycle. Diffuse reflectance infrared fourier-transform spectroscopy (DRIFTS) experiments exploiting (concentration) modulation excitation spectroscopy (MES) and phase-sensitive detection (PSD) identified spectroscopic signatures of Cu-nitrate and Cu-nitrosamine (H2NNO), important species which had not been previously observed experimentally. This is further supported by the QM/MM-calculated harmonic vibrational analysis. Additional insights are provided into the reactivity of solvated active sites and the formation of key intermediates including their formation energies and vibrational spectroscopic signatures, allowing the development of a detailed understanding of the reaction mechanism. We demonstrate the role of solvated active sites and their influence on the energetics of important species that must be explicitly considered for an accurate understanding of NH3-SCR kinetics.
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