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负载于γ -AlO、TiO和MCM -41上的锰基催化剂:低O/NO比条件下低温NO氧化的比较

Mn-based catalysts supported on γ-AlO, TiO and MCM-41: a comparison for low-temperature NO oxidation with low ratio of O/NO.

作者信息

Liu Lijun, Shen Boxiong, Si Meng, Yuan Peng, Lu Fengju, Gao Hongpei, Yao Yan, Liang Cai, Xu Hongjie

机构信息

School of Energy and Environmental Engineering, Hebei University of Technology Tianjin China

School of Chemical Engineering, Hebei University of Technology Tianjin China.

出版信息

RSC Adv. 2021 May 25;11(31):18945-18959. doi: 10.1039/d1ra01820e. eCollection 2021 May 24.

Abstract

Mn-Based catalysts supported on γ-AlO, TiO and MCM-41 synthesized by an impregnation method were compared to evaluate their NO catalytic oxidation performance with low ratio O/NO at low temperature (80-200 °C). Activity tests showed that the participation of O remarkably promoted the NO oxidation. The catalytic oxidation performance of the three catalysts decreased in the following order: Mn/γ-AlO > Mn/TiO > Mn/MCM-41, indicating that Mn/γ-AlO exhibited the best catalytic activity. In addition, there was a clear synergistic effect between Mn/γ-AlO and O, followed by Mn/TiO and O. The characterization results of XRD, EDS mapping, BET, H-TPR, XPS and TG showed that Mn/γ-AlO had good manganese dispersion, excellent redox properties, appropriate amounts of coexisting Mn and Mn and abundant chemically adsorbed oxygen, which ensured its good performance. DRIFTS demonstrated the NO adsorption performance on the catalyst surface. As revealed by DRIFTS experiments, the chemically adsorbed oxygen, mainly from the decomposition of O, greatly promoted the NO adsorption and the formation of nitrates. The Mn-based catalysts showed stronger adsorption strength than the corresponding pure supports. Due to the abundant adsorption sites provided by pure γ-AlO, under the interaction of Mn and γ-AlO, the Mn/γ-AlO catalyst exhibited the strongest NO adsorption performance among the three catalysts and produced lots of monodentate nitrates (-O-NO) and bidentate nitrates (-ONO), which were the vital intermediate species for NO formation. Moreover, the NO-TPD studies also demonstrated that Mn/γ-AlO showed the best NO desorption performance among the three catalysts. The good NO adsorption and desorption characteristics of Mn/γ-AlO improved its high catalytic activity. In addition, the activity test results also suggested that Mn/γ-AlO exhibited good SO tolerance.

摘要

通过浸渍法合成的负载在γ -Al₂O₃、TiO₂和MCM -41上的锰基催化剂进行了比较,以评估它们在低温(80 - 200°C)下低O₂/NO比时的NO催化氧化性能。活性测试表明,O₂的参与显著促进了NO的氧化。三种催化剂的催化氧化性能按以下顺序降低:Mn/γ -Al₂O₃>Mn/TiO₂>Mn/MCM -41,表明Mn/γ -Al₂O₃表现出最佳的催化活性。此外,Mn/γ -Al₂O₃与O₂之间存在明显的协同效应,其次是Mn/TiO₂与O₂之间。XRD、EDS图谱、BET、H -TPR、XPS和TG的表征结果表明,Mn/γ -Al₂O₃具有良好的锰分散性、优异的氧化还原性能、适量共存的Mn²⁺和Mn³⁺以及丰富的化学吸附氧,这确保了其良好的性能。漫反射红外傅里叶变换光谱(DRIFTS)证明了催化剂表面的NO吸附性能。如DRIFTS实验所示,主要来自O₂分解的化学吸附氧极大地促进了NO的吸附和硝酸盐的形成。锰基催化剂显示出比相应纯载体更强的吸附强度。由于纯γ -Al₂O₃提供了丰富的吸附位点,在Mn与γ -Al₂O₃的相互作用下,Mn/γ -Al₂O₃催化剂在三种催化剂中表现出最强的NO吸附性能,并产生大量的单齿硝酸盐(-O-NO)和双齿硝酸盐(-ONO),它们是NO形成的重要中间物种。此外,NO -TPD研究还表明,Mn/γ -Al₂O₃在三种催化剂中表现出最佳的NO脱附性能。Mn/γ -Al₂O₃良好的NO吸附和解吸特性提高了其高催化活性。此外,活性测试结果还表明Mn/γ -Al₂O₃表现出良好的SO₂耐受性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/528e/9033454/3d5bb6f7a269/d1ra01820e-f1.jpg

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