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Spinel structured CoaMnbOx mixed oxide catalyst for the selective catalytic reduction of NOx with NH3
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2017-09-17 , DOI: 10.1016/j.apcatb.2017.09.034
Dongmei Meng , Qian Xu , Yunlei Jiao , Yun Guo , Yanglong Guo , Li Wang , Guanzhong Lu , Wangcheng Zhan

A highly efficient catalyst of a CoaMnbOx mixed oxide prepared by the co-precipitation method was developed for the selective catalytic reduction (SCR) of NOx with ammonia. With an increase in the Mn content, the catalytic activity of the CoaMnbOx mixed oxide exhibited a volcano-type tendency, and when Co/Mn molar ratio reached 7:3 (Co7Mn3Ox), the operation temperature for achieving >80% NOx conversion was 170 °C (116–285 °C window). The formation of spinel structured MnCo2O4 is highly important, and the presence of the spinel structure in Co7Mn3Ox contributes to the increase in active sites and thermal stability and promotes SO2 and/or H2O resistance. In comparison with MnOx or CoOx alone, the CoaMnbOx catalysts possess improved redox properties and more surface acid sites due to synergistic effects between the Co and Mn species. Among the CoaMnbOx catalysts with different Co/Mn molar ratios, a higher NH3 and NO + O2 adsorption ability was found for the Co7Mn3Ox catalyst, originating from its MnCo2O4.5 phase and higher surface area, which leads to the higher activity of the Co7Mn3Ox catalyst. In situ DRIFTs indicated that bridging nitrate and bidentate nitrate are the intermediate species in the NH3-SCR reaction, and the high NO adsorption ability and improved redox properties of the Co7Mn3Ox catalyst are beneficial for the formation of nitrate species on the catalyst surface. Furthermore, NH3 species adsorbed at Lewis acid sites taken part in SCR reaction, while the reactivity of NH3 species adsorbed at Brönsted acid was not definitized.



中文翻译:

尖晶石结构的Co a Mn b O x混合氧化物催化剂,用于用NH 3选择性催化还原NO x

开发了一种通过共沉淀法制备的高效Co a Mn b O x混合氧化物催化剂,用于将NO x与氨选择性催化还原(SCR)。随着Mn含量的增加,Co a Mn b O x复合氧化物的催化活性呈现出火山型趋势,当Co / Mn摩尔比达到7:3(Co 7 Mn 3 O x)时,操作温度实现> 80%的NO X转化率是170℃(116-285℃的窗口)。尖晶石结构的MnCo 2 O 4的形成Co 2 Mn 3 O x中尖晶石结构的存在有助于活性位点的增加和热稳定性,并提高了对SO 2和/或H 2 O的抵抗力。与单独的MnO x或CoO x相比,由于Co和Mn物种之间的协同作用,Co a Mn b O x催化剂具有改善的氧化还原性能和更多的表面酸位。在具有不同Co / Mn摩尔比的Co a Mn b O x催化剂中,较高的NH 3和NO + O 2发现Co 7 Mn 3 O x催化剂的吸附能力源自其MnCo 2 O 4.5相和较高的表面积,这导致Co 7 Mn 3 O x催化剂的活性更高。原位DRIFTs表明硝酸盐和硝酸齿状硝酸盐的桥接是NH 3 -SCR反应的中间物种,Co 7 Mn 3 O x催化剂的高NO吸附能力和改善的氧化还原性能有利于在NH 3 -SCR反应中形成硝酸盐物种。催化剂表面。此外,NH 3路易斯酸位点上吸附的NH 3物种参与SCR反应,而布朗斯台德酸上吸附的NH 3物种的反应性尚未确定。

更新日期:2017-09-17
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