4.7 Article

Catalytic performance over Mn-Ce catalysts for NH3-SCR of NO at low temperature: Different zeolite supports

出版社

ELSEVIER SCI LTD
DOI: 10.1016/j.jece.2022.107167

关键词

Low-temperature NH3-SCR; Mn-Ce active components; Zeolite supports; Reaction mechanism

资金

  1. National Natural Science Foundation of China [52174298, 51874058]
  2. Graduate Research and Innovation Foundation of Chongqing, China [CYB21002]
  3. Chongqing Human Resources and Social Security Bureau [cx2020028]
  4. Chongqing Talents Plan for Young Talents [CQYC201905017]

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The Mn-Ce/zeolite catalysts were synthesized to study their NH3-SCR performance at low temperatures. The Mn-Ce/X catalyst showed the highest NO conversion and SO2 resistance, while Mn-Ce/ZSM-5 and Mn-Ce/Beta catalysts had high NO conversion at higher temperatures. Furthermore, Mn-Ce/X catalyst had better acid sites and stability, promoting NH3-SCR activity.
To clarify the low-temperature NH3-SCR performance of Mn-Ce/zeolite catalysts and the specific promotion influence between Mn-Ce active components and zeolite supports, Mn-Ce/zeolite catalysts were synthesized using Mn-Ce mix oxides loading on several kinds of zeolites (ZSM-5 zeolite, Beta zeolite, X zeolite and Y zeolite) by impregnation method. The results indicated that Mn-Ce/X catalyst had high NO conversion of nearly 100% at 150 ? and the excellent SO2 resistance at different temperature. The Mn-Ce/ZSM-5 and Mn-Ce/Beta catalysts had NO conversion of about 100% at 275 ? while the Mn-Ce/Y catalyst had the lowest NO conversion. Additionally, Mn-Ce/X catalyst had higher relative ratio of Mn4+ and Ce3+ species, more Bronsted acid sites and better reducibility than that of other three catalysts, which could promote NH3-SCR activity. Moreover, the Bronsted acid sites and the Lewis acid sites on Mn-Ce/X catalyst were more stable at low-temperature. Besides, the SCR reaction of Mn-Ce/ZSM-5, Mn-Ce/Beta and Mn-Ce/X catalysts mainly followed Langmuir-Hinshelwood (L-H) mechanism at lower temperature and Eley-Rideal (E-R) mechanism at higher temperature. Furthermore, Mn-Ce/X catalyst had better adsorption ability of nitrate and nitrite species as well, which could enhance NH3-SCR reaction process

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