Low temperature performance and sulfur resistance enhancement of Mn-Ce oxides supported on W-modified MWCNT for NH3-SCR removal of NOx
Low temperature performance and sulfur resistance enhancement of Mn-Ce oxides supported on W-modified MWCNT for NH3-SCR removal of NOx
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W改性MWCNT负载Mn-Ce氧化物的低温性能和抗硫性能增强，用于NH3-SCR脱硝
DOI：
10.1080/10962247.2021.1873205
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发表时间：
2021-01
影响因子：
2.7
通讯作者：
Chenglong Yu
中科院分区：
文献类型：
--
作者：
Xiang Tu;Zugen Liu;Dan He;Baoping Xu;Meijuan Lu;Bichun Huang;Yong Zhang;Chenglong Yu
摘要为了脱除氮氧化物（NOx），采用超声浸渍法制备了复合载体负载型催化剂（Mn-Ce/MWCNT-W）和传统催化剂（Mn-Ce/MWCNT和W-Mn-Ce/MWCNT），并进行了低温氨选择性催化还原（SCR）脱硝反应。系统考察了MWCNT-W复合载体对催化剂低温SCR活性和抗SO2性能的促进作用。与传统催化剂相比，WOx/MWCNT质量比为30%的Mn-Ce/MWCNT-W催化剂在100°C ~ 200°C范围内表现出更高的SCR活性和N2选择性。通过一系列表征发现，与传统催化剂相比，复合载体负载型催化剂具有更多的氧化还原中心和更强的NH3吸附能力。此外，对于这种复合载体负载型催化剂，SCR反应的改善被认为来自于高价态Mn的丰富和良好分散的活性组分。与传统催化剂相比，复合载体负载型催化剂具有更强的抗硫性能。因此，使用MWCNT-W复合载体制备Mn-Ce/MWCNT-W催化剂导致在低温下优异的NOx转化率和抗SO2性能。结论：低温NH3-SCR脱硝技术是一种有效的固定源脱硝技术。载体的物理化学性质不仅影响催化剂的低温SCR活性，而且影响催化剂的抗中毒性能。改性后的载体能促进活性组分的分散，有利于SCR反应的进行。然而，对于LT SCR反应，很少有报道涉及复合载体负载型催化剂的设计和制备。本研究的目的是设计和合成Mn-Ce/MWCNT-W催化剂，并考察复合载体对Mn基催化剂低温SCR活性和抗硫性能的影响。
ABSTRACT To eliminate nitrogen oxides (NOx), composite carrier-supported catalysts (Mn-Ce/MWCNT-W) and traditional catalysts (Mn-Ce/MWCNT and W-Mn-Ce/MWCNT) were prepared using an ultrasonic impregnation method that preformed low-temperature ammonia-selective catalytic reduction (SCR) removal of NOx. The promotion effects of MWCNT-W composite carriers for low temperature SCR activities and SO2 tolerance of the catalysts were systematically investigated. Compared to traditional catalyst, Mn-Ce/MWCNT-W catalyst, with a 30% WOx/MWCNT mass ratio, demonstrated improved SCR activity and high N2-selectivity from 100°C to 200°C. A series of characterizations were carried out and it was found that there were more redox sites and the stronger the NH3 adsorption capacity over the composite carrier-supported catalysts than traditional catalysts. Also, with this composite carrier-supported catalyst, the improvement of SCR reaction was considered to be from the abundance of high valence state Mn and well dispersed active components. Notably, compared to traditional catalyst, the composite carrier-supported catalyst exhibited the stronger sulfur resistance. Thus, using MWCNT-W composite carriers to prepare Mn-Ce/MWCNT-W catalysts resulted in excellent NOx conversion and SO2 resistance at low temperatures. Implications: LT NH3-SCR of NOx is an effective way to remove NOx from stationary sources. The physicochemical properties of the support not only affect a catalyst’s LT SCR activity but also affect the catalyst’s anti-poisoning performance. The modified carriers could promote active component dispersion, which is conducive to SCR reaction. However, for LT SCR reactions, few reports have addressed the design and preparation of composite carrier-supported catalysts. The goal of this study was to design and synthesize Mn-Ce/MWCNT-W catalysts and to observe the influence of composite support in Mn-based catalysts on LT SCR activity and sulfur resistance.
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DOI：
10.1080/10962247.2016.1231144
发表时间：
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影响因子：
2.7
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