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通过构建桥联锰位工程提高 MnO 催化剂对 NO 还原的 N 选择性。

Improved N Selectivity of MnO Catalysts for NO Reduction by Engineering Bridged Mn Sites.

机构信息

International Joint Laboratory of Catalytic Chemistry, State Key Laboratory of Advanced Special Steel, Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, China.

出版信息

Langmuir. 2023 May 30;39(21):7434-7443. doi: 10.1021/acs.langmuir.3c00663. Epub 2023 May 18.

Abstract

Mn-based catalysts are promising for selective catalytic reduction (SCR) of NO with NH at low temperatures due to their excellent redox capacity. However, the N selectivity of Mn-based catalysts is an urgent problem for practical application owing to excessive oxidizability. To solve this issue, we report a Mn-based catalyst using amorphous ZrTiO as the support (Mn/ZrTi-A) with both excellent low-temperature NO conversion and N selectivity. It is found that the amorphous structure of ZrTiO modulates the metal-support interaction for anchoring the highly dispersed active MnO species and constructs a uniquely bridged Mn bonded with the support through oxygen linked to Ti and Zr, respectively, which regulates the optimal oxidizability of the MnO species. As a result, Mn/ZrTi-A is not conducive to the formation of ammonium nitrate that readily decomposes to NO, thus further increasing N selectivity. This work investigates the role of an amorphous support in promoting the N selectivity of a manganese-based catalyst and sheds light on the design of efficient low-temperature deNO catalysts.

摘要

基于锰的催化剂由于其优异的氧化还原能力,在低温下用 NH 选择性催化还原(SCR)NO 方面很有前景。然而,由于过度的氧化性,基于锰的催化剂的 N 选择性是实际应用中亟待解决的问题。为了解决这个问题,我们报告了一种使用非晶 ZrTiO 作为载体的基于锰的催化剂(Mn/ZrTi-A),该催化剂具有优异的低温 NO 转化和 N 选择性。研究发现,ZrTiO 的非晶结构调节了金属-载体相互作用,从而固定了高度分散的活性 MnO 物种,并通过氧分别与 Ti 和 Zr 相连,构建了独特的桥接 Mn 与载体相连,这调节了 MnO 物种的最佳氧化能力。因此,Mn/ZrTi-A 不利于易于分解为 NO 的硝酸铵的形成,从而进一步提高 N 选择性。这项工作研究了非晶载体在提高锰基催化剂的 N 选择性方面的作用,为设计高效的低温脱硝催化剂提供了思路。

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