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Formation of N2O greenhouse gas during SCR of NO with NH3 by supported vanadium oxide catalysts
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2017-11-16 , DOI: 10.1016/j.apcatb.2017.11.029
Minghui Zhu , Jun-Kun Lai , Israel E. Wachs

Selective catalytic reduction of NO by NH3 over supported vanadium oxide catalysts has been studied for decades, but the studies mostly concentrated on the dominant N2 product with much less attention paid to the formation of the undesired N2O product. In the present study, fundamental aspects of the N2O formation reaction were elucidated by a series of temperature-programmed surface reaction studies with isotopic labelled reactants. The surface vanadium oxide species on the TiO2 support are active sites for the N2O formation reaction, while tungsten species mainly function as promoters. Oxygen from NO, gaseous O2 and catalyst oxygen all function as oxygen sources for formation of N2O (∼50%, ∼30% and ∼20%, respectively). The rate-determining-step for N2O formation involves breaking of the ammonia NH bond. These new molecular level insights have the potential to guide the rational design of improved SCR catalysts for diesel engines with reduced N2O produced.



中文翻译:

负载型钒氧化物催化剂催化的NO与NH 3 SCR反应中N 2 O温室气体的形成。

数十年来,已经研究了在负载的钒氧化物催化剂上用NH 3选择性催化还原NO的研究,但研究大多集中在占主导地位的N 2产物上,而对形成不希望的N 2 O产物的关注则少得多。在本研究中,通过一系列用同位素标记的反应物进行的程序升温表面反应研究,阐明了N 2 O形成反应的基本方面。TiO 2载体上的表面钒氧化物是N 2 O形成反应的活性位,而钨主要起促进剂的作用。NO,气态O 2中的氧气催化剂氧和催化剂氧都是形成N 2 O的氧源(分别为〜50%,〜30%和〜20%)。N 2 O形成的速率确定步骤涉及到氨N H键的断裂。这些新的分子水平的见识有可能指导合理设计改进的SCR催化剂,以减少N 2 O的产生。

更新日期:2017-11-16
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