Selective catalytic reduction of NO with NH3 over copper-manganese spinel oxides at low temperature: effects of calcination temperature and dispersant
摘要
By controlling preparation conditions, a series of catalysts were synthesized. Among them, ST-400 presented primary CuMn2O4 spinel phase and expectant denitration efficiency at low temperature. Then, various concentrations Hexadecyl trimethyl ammonium Bromide (hereinafter referred to as CTAB) were added into ST-400. Among them, 0.3C-ST-400 showed higher NO removal rate, more acid sites and greater redox performance. What’s more, due to the strong interaction and electron transfer of metal ions, there was equilibrium: 2Mn3+ ⇄ Mn2+ + Mn4+ and Cu2+ + Mn3+ ⇄ Cu+ + Mn4+, and the addition of CTAB could promote the equilibrium to the right. More concentration of Mn4+ and chemisorbed oxygen would be the facilitation for catalytic activity at low temperatures. In situ DRIFT experiments indicated that Langmuir–Hinshelwood mechanism plays a major role over both ST-400 and 0.3C-ST-400. However, compared with ST-400, the addition of CTAB results in the present of Eley–Rideal mechanism over 0.3C-ST-400. Besides, the CTAB promotes the adsorption intensity of NH3 and nitrate species as well as the conversion to active nitrate species, which will markedly stimulate the effect of Langmuir–Hinshelwood mechanism. In consequence, the propre addition of CTAB is a novel strategy in favor of NH3-SCR activity-enhancement research.
Graphical Abstract