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Effects of different Zr/Ti ratios on NH3–SCR over MnOx/ZryTi1-yO2: Characterization and reaction mechanism
Molecular Catalysis ( IF 3.9 ) Pub Date : 2017-10-06 , DOI: 10.1016/j.mcat.2017.09.019
Bohan Jia , Jiaxiu Guo , Song Shu , Ningjie Fang , Jianjun Li , Yinghao Chu

A series of ZryTi1-yO2 (y = 0.1, 0.4, 0.5, 0.6 and 0.9) are prepared by co-precipitation method and Mn(NO3)2 is impregnated on them to achieve a 5 wt% Mn loading. The catalytic activity of MnOx/ZryTi1-yO2 for the selective reduction of NO with ammonia (NH3–SCR) in the range of 80–360 °C is evaluated by a fixed-bed reactor. The prepared catalysts are characterized by N2 adsorption-desorption, XRD, XPS, H2–TPR, NH3–TPD and in situ DIRFTS. The results showed that different Zr/Ti ratios influence the NH3–SCR activity of MnOx/ZryTi1-yO2, but they have high N2 selectivity at low temperature and similar changes in the range of 80–360 °C. MnOx/Zr0.6Ti0.4O2 achieves 80% of NO removal efficiency at 140 °C and can keep 100% from 200 to 360 °C, and it exhibits an excellent resistance of H2O at 200 °C and a certain tolerance to SO2. The pores of all prepared catalysts are composed of many mesopores with pore width centered at 4 nm and some micropores with pore width centered at 1.75 nm. MnOx/Zr0.4Ti0.6O2 has 344 m2/g of BET surface area, 0.42 cm3/g of total pore volume with 0.075 cm3/g of micropore volume, but MnOx/Zr0.6Ti0.4O2 has the highest contents of Mn4+ (52.0%) and Oβ (32.8%) and more Lewis acid sites. Zr/Ti ratios change Mn valence and O species in MnOx/ZryTi1-yO2, and Mn4+ can promote the adsorption of NH3 and accelerates the formation of NH4NO3 to improve NO removal with NH3 by L–H mechanism.



中文翻译:

不同Zr / Ti比对MnO x / Zr y Ti 1- y O 2上NH 3 -SCR的影响:表征和反应机理

 通过共沉淀法制备一系列Zr y Ti 1- y O 2y = 0.1、0.4、0.5、0.6和0.9),并在其上浸渍Mn(NO 32以实现5%的Mn负载量。 。通过固定床反应器评估了MnO x / Zr y Ti 1- y O 2在80–360°C范围内用氨气(NH 3 -SCR)选择性还原NO的催化活性。制备的催化剂的特征在于N 2吸附-解吸,XRD,XPS,H 2 -TPR,NH 3 -TPD以及原位差异。结果表明,不同的Zr / Ti比会影响MnO x / Zr y Ti 1- y O 2的NH 3 -SCR活性,但它们在低温下具有较高的N 2选择性,并且在80-360°范围内具有相似的变化C。MnO x / Zr 0.6 Ti 0.4 O 2在140°C时达到80%的NO去除效率,并且在200至360°C时可以保持100%,并且在200°C时具有出色的H 2 O耐受性和一定的耐受性到SO 2。所有制得的催化剂的孔均由许多中孔,其孔宽度以4 nm为中心,以及一些微孔中的孔宽度以1.75 nm为中心。的MnO X / Zr的0.40.6 ø 2具有344米2 / g的BET表面积的,0.42厘米3与0.075厘米总孔体积的/克3 / g的微孔体积的,但MnO的X / Zr的0.60.4 Ò 2具有Mn 4+(52.0%)和(32.8%)的含量最高,路易斯酸位点更多。Zr / Ti比改变MnO x / Zr y Ti中的Mn价和O物种1- ÿ Ò 2和Mn 4+可以促进NH的吸附3和加速NH的形成4 NO 3,以提高NO脱除用NH 3通过L-H机制。

更新日期:2017-10-06
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