The promoting effect of S-doping on the NH3-SCR performance of MnOx/TiO2 catalyst

The promoting effect of S-doping on the NH3-SCR performance of MnOx/TiO2 catalyst
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S掺杂对MnOx/TiO2催化剂NH3-SCR性能的促进作用

DOI:
10.1016/j.apsusc.2019.144694
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发表时间:
2020-04-01
影响因子:
6.7
通讯作者:
Shen, Zhongyun
Shen, Zhongyun
中科院分区:
材料科学1区
文献类型:
--
作者:
Liu, Xuesong;Yu, Qifan;Shen, Zhongyun

文献摘要

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采用溶胶-凝胶法制备了一系列S掺杂的MnOx/TiO 2催化剂,以提高SCR性能。当S:Ti摩尔比为0.05:1时,催化剂的低温SCR性能最好,活性温度窗口最宽。根据各种分析结果,通过S4+取代Ti 4+,在TiO 2晶格中掺入适量的S,形成Ti-O-S键,随着表面积的增加,表面Mn 4+物种和活性氧物种(O-2(-))沿着增加。这些增强的性能改善了适当的S掺杂的MnOx/TiO 2催化剂的布朗斯台德酸中心和氧化还原性能。S掺杂的这些优点可以从根本上提高MnOx/TiO 2催化剂的dc-NOx能力。同时,原位DRIFT实验表明,适当的S掺杂后,吸附的NH 4+和气相NO2物种大大增加,沿着增加的是吸附的NH3和NOx物种的反应活性。在SCR反应中,S掺杂催化剂同时发生了E-R和L-H机理,而S掺杂的促进作用是通过促进L-H途径实现的。
A series of S-doped MnOx/TiO2 catalysts were prepared by sol-gel method for the purpose of enhancing SCR performance. The obtained catalyst with mole ratio of S:Ti = 0.05:1 exhibited the best low temperature SCR performance and the widest active temperature window. According to the results of various analyses, the proper S was doped into TiO2 lattice via the replacement of Ti4+ by S4+ to generate Ti-O-S bond, along with increasing surface area, more surface Mn4+ species and more active oxygen species (O-2(-)). These enhanced properties improved the Bronsted acid sites and redox property of the properly S-doped MnOx/TiO2 catalyst. These advantages of S doping can essentially benefit the dc-NOx ability of MnOx/TiO2 catalysts. Meanwhile, the in situ DRIFT experiments revealed that the adsorbed NH4+ and gas-phase NO2 species were greatly increased after proper S-doping, along with the enhanced reactivity of the adsorbed NH3 and NOx species. Both E-R and L-H mechanisms occurred on the S-doped catalysts, while the promoting effect of S-doping was performed by facilitating the L-H route during SCR reaction.