Li Yifan, Hou Yaqin, Zhang Yongzhao, Yang Yatao, Huang Zhanggen
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China; University of Chinese Academy of Sciences, Beijing 100049, PR China.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, PR China.
J Colloid Interface Sci. 2022 Feb 15;608(Pt 3):2224-2234. doi: 10.1016/j.jcis.2021.10.078. Epub 2021 Oct 19.
Surface interface regulation is an important research content in the field of heterogeneous catalysis. To improve the interface interaction between the active component and matrix, tremendous efforts have been dedicated to tailoring the morphology, size, and structure of composite catalysts. In this work, we report a confinement strategy to synthesize a series of core-shell catalysts loaded with metal oxides on titania nanotubes (TNTs), which were applied to the selective catalytic reduction of NO with ammonia. Interestingly, the core-shell catalyst with confinement of TNTs exhibited the remarkable activity at low temperature region, N selectivity and sulfur tolerance. Benefiting from the superior interfacial confinement characteristic of TNTs and FeO, strong component interactions, the surface acid sites and strong oxidizability of MnO were properly regulated, thus obtained the outstanding activity, N selectivity and provide chemical protection to effectively prevent SO poisoning. As far as the reaction mechanism, we found that the adsorption and reactivity of Lewis acid sites were the dominant factors affecting the activity in the NH-SCR process by in situ DRIFT spectra. In general, our work provides an innovative strategy for constructing an TNTs-enwrapped nanocomposite with nano-confinement and core-shell structure to improve the low temperature SCR process.
表面界面调控是多相催化领域的重要研究内容。为了改善活性组分与载体之间的界面相互作用,人们在调控复合催化剂的形貌、尺寸和结构方面付出了巨大努力。在本工作中,我们报道了一种限域策略,用于合成一系列在二氧化钛纳米管(TNTs)上负载金属氧化物的核壳催化剂,并将其应用于氨选择性催化还原NO。有趣的是,具有TNTs限域结构的核壳催化剂在低温区域表现出显著的活性、N选择性和抗硫性。得益于TNTs和FeO优异的界面限域特性、强烈的组分相互作用,MnO的表面酸性位点和强氧化性得到了适当调控,从而获得了出色的活性、N选择性,并提供化学保护以有效防止SO中毒。就反应机理而言,通过原位漫反射红外傅里叶变换光谱(DRIFT),我们发现路易斯酸位点的吸附和反应性是影响NH-SCR过程活性的主要因素。总的来说,我们的工作为构建具有纳米限域和核壳结构的TNTs包裹纳米复合材料以改善低温SCR过程提供了一种创新策略。