催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
3期
294-301
,共8页
氮氧化物%氨%锰铁基催化剂%低温选择性催化还原%原位漫反射傅里叶变换红外光谱
氮氧化物%氨%錳鐵基催化劑%低溫選擇性催化還原%原位漫反射傅裏葉變換紅外光譜
담양화물%안%맹철기최화제%저온선택성최화환원%원위만반사부리협변환홍외광보
Nitrogen Oxide%Ammonia%Manganese-iron catalysts%Low temperature selective catalytic reduction%In situ diffuse reflectance infrared%Fourier transform spectroscopy
采用自蔓延燃烧法制备了Ti0.9Mn0.05Fe0.05O2-δ催化剂,运用原位漫反射傅里叶变换红外光谱对该催化剂的NO和NH3稳态吸附以及NO和NH3瞬态反应进行了详细地分析与讨论.结果表明,相比于Lewis酸性位,150oC时Br?nsted酸性位吸附的NH3更具有SCR活性;与双齿硝酸盐和桥式硝酸盐相比, NO吸附产生的单齿硝酸盐是主要的中间物种;该SCR反应遵循Eley-Rideal和Langmuir-Hinshelwood机理,但以后者为主.另外, O2的存在有利于NO的氧化和配位态NH3的活化.
採用自蔓延燃燒法製備瞭Ti0.9Mn0.05Fe0.05O2-δ催化劑,運用原位漫反射傅裏葉變換紅外光譜對該催化劑的NO和NH3穩態吸附以及NO和NH3瞬態反應進行瞭詳細地分析與討論.結果錶明,相比于Lewis痠性位,150oC時Br?nsted痠性位吸附的NH3更具有SCR活性;與雙齒硝痠鹽和橋式硝痠鹽相比, NO吸附產生的單齒硝痠鹽是主要的中間物種;該SCR反應遵循Eley-Rideal和Langmuir-Hinshelwood機理,但以後者為主.另外, O2的存在有利于NO的氧化和配位態NH3的活化.
채용자만연연소법제비료Ti0.9Mn0.05Fe0.05O2-δ최화제,운용원위만반사부리협변환홍외광보대해최화제적NO화NH3은태흡부이급NO화NH3순태반응진행료상세지분석여토론.결과표명,상비우Lewis산성위,150oC시Br?nsted산성위흡부적NH3경구유SCR활성;여쌍치초산염화교식초산염상비, NO흡부산생적단치초산염시주요적중간물충;해SCR반응준순Eley-Rideal화Langmuir-Hinshelwood궤리,단이후자위주.령외, O2적존재유리우NO적양화화배위태NH3적활화.
To investigate the mechanism of selective catalytic reduction (SCR) of NOx with NH3, Ti0.9Mn0.05Fe0.05O2-δ catalyst was prepared by self-propagating high-temperature synthesis (SHS) method and evaluated at 25-450 °C. The catalyst was characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). The possible SCR mechanism over Ti0.9Mn0.05Fe0.05O2-δ was studied by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). Ti0.9Mn0.05Fe0.05O2-δ showed both high SCR activity and N2 selectivity over a broad temperature win-dow of 100-350 °C. The XRD and TEM results indicated that the active components of Mn and Fe were in a highly dispersed state and in an amorphous form on TiO2. The DRIFTS results revealed that Br?nsted acid sites were the active centers for NO removal and monodentate nitrates were the key intermediate in the SCR reaction. At 150 °C, both Langmuir-Hinshelwood and Eley-Rideal mechanisms are involved in the SCR reaction, while the former one mechanism dominates the cata-lytic activity of Ti0.9Mn0.05Fe0.05O2-δ. Additionally, the presence of O2 significantly affects NO oxidation and coordinated NH3 activation.