A superior Mn5CeTi5Ox catalysts for synergistic catalytic removal of chlorobenzene and NOx: Performance enhancement and mechanism studies

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-10-24 DOI:10.1016/j.mcat.2024.114634
Bo Yang, Liuying Wang, Qiuxiang Gu, Yujie Lei, Qiong Huang, Mindong Chen
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Abstract

The transition metal titanium-doped Mn-Ce-Ox catalysts catalyst were employed to achieve synergetic removal of NO and CB at 180–220 °C. The Mn5CeTi5Ox catalyst with a molar ratio of Mn/Ce/Ti = 5:1:5 exhibits excellent activity, and the NOx and CB removal efficiencies reach 96 % and 89 % at 160–220 °C, respectively. The selectivity for N2 and CO2 are 93 % and 78 %, respectively. The N2-physisorption, NH3-TPD, H2-TPR and XPS results show that Ti doping makes the catalyst possess a mesoporous structure, suitable particle sizes, and excellent redox and Lewis site properties. All of these features contribute to the observed high NO and CB removal efficiency. The synergetic removal of CB and NO over Mn5CeTi5Ox results from the synergistic catalysis between the redox and the solid acid. On the one hand, in the synergistic removal process, CB and NH3 are competitively adsorbed on the catalyst surface, resulting in a decrease in the NH3-SCR activity. On the other hand, the removal of NO and CB has a synergetic effect. The byproduct NO2 produced by the NH3-SCR reaction promotes the oxidation of CB, which is beneficial for CB removal. Moreover, the consumption of NO2 indirectly promotes the NH3-SCR reaction, which partially compensates for the decrease in the NO removal efficiency caused by competitive adsorption between NH3 and CB. Ti doping promotes the participation of the SCR byproduct NO2 in the CBCO reaction and promotes the formation of maleic acid, an intermediate product of CB oxidation. In summary, the Mn5CeTi5Ox catalyst exhibits good activity for the synergistic removal of NOx and CB and is a promising candidate for the effective and economical removal of NO and CB during waste incineration.

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一种用于协同催化去除氯苯和氮氧化物的优异 Mn5CeTi5Ox 催化剂:性能提升和机理研究
采用掺杂过渡金属钛的锰-铈-氧化物催化剂,在 180-220 ℃条件下实现了协同脱除 NO 和 CB。摩尔比为 Mn/Ce/Ti = 5:1:5 的 Mn5CeTi5Ox 催化剂表现出优异的活性,在 160-220 ℃ 下,NOx 和 CB 的去除率分别达到 96 % 和 89 %。对 N2 和 CO2 的选择性分别为 93 % 和 78 %。N2-吸附、NH3-TPD、H2-TPR 和 XPS 结果表明,钛掺杂使催化剂具有介孔结构、合适的粒度以及优异的氧化还原和路易斯位点特性。所有这些特征都有助于观察到较高的 NO 和 CB 去除效率。Mn5CeTi5Ox 对 CB 和 NO 的协同去除作用源于氧化还原和固体酸之间的协同催化作用。一方面,在协同去除过程中,CB 和 NH3 竞争性地吸附在催化剂表面,导致 NH3-SCR 活性降低。另一方面,NO 和 CB 的去除具有协同效应。NH3-SCR 反应产生的副产物 NO2 促进了 CB 的氧化,有利于 CB 的去除。此外,NO2 的消耗也间接促进了 NH3-SCR 反应,从而部分弥补了 NH3 和 CB 之间竞争性吸附导致的 NO 去除效率的降低。钛的掺杂促进了 SCR 副产物 NO2 参与 CBCO 反应,并促进了 CB 氧化的中间产物马来酸的形成。总之,Mn5CeTi5Ox 催化剂在协同去除 NOx 和 CB 方面表现出良好的活性,是垃圾焚烧过程中有效、经济地去除 NO 和 CB 的理想催化剂。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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