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| CaO catalyzes NH3 oxidation, while sulfated CaO catalyzes NO reduction by NH3 in the presence of O2, and the adsorption and transformation of ammonia over CaO and sulfated CaO has been investigated by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to understand their catalytic mechanism. It has been found that ammonia is first adsorbed over Lewis or Brönsted acid sites, and later undergoes hydrogen abstraction giving rise to either NH2 amide or NH imide intermediates. The intermediates react with NO or lattice O to produce N2 or NO. Comparing the DRIFTS of NH3 adsorption over CaO and sulfated CaO, it is obvious that ammonia adsorbed over CaO is activated mainly in NH form apt to react with surface oxygen to produce NO, while ammonia adsorbed over sulfated CaO is activated mainly in NH2 form apt to reduce NO. The DRIFTS results agree with experimental data and explain the catalytic mechanisms of CaO and sulfated CaO. |
金蟲 (正式寫手)
| 氧化鈣可催化氨的氧化,而硫化后的氧化鈣能催化氨在氧氣中還原一氧化氮,為了解其催化機(jī)理,通過原位的漫反射紅外傅里葉光譜,研究了氨在氧化鈣和硫化后的氧化鈣上的吸附和轉(zhuǎn)化。結(jié)果表明氨首先作為路易斯酸被吸附,然后經(jīng)過脫氫生成NH2或NH中間體,該中間體與NO或O反應(yīng)生成N2或NO。比較兩種吸附NH3的DRIFT,結(jié)果顯示氧化鈣吸附的氨主要以NH的形式被活化后與氧化硫反應(yīng)生成NO,而硫化后氧化鈣的吸附氨主要NH2的形式被活化后產(chǎn)生NO。DRIFTS研究結(jié)果與實(shí)驗(yàn)的數(shù)據(jù)一致,并解釋了氧化鈣和硫化后氧化鈣的催化機(jī)理。 外行 盡請(qǐng)指正 |
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