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Generation of abundant defects in Mn-Co mixed oxides by a facile agar-gel method for highly efficient catalysis of total toluene oxidation
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2020-09-20 , DOI: 10.1016/j.apcatb.2020.119560
Peifen Wang , Jing Wang , Xiaowei An , Jin Shi , Wenfeng Shangguan , Xiaogang Hao , Guangwen Xu , Bing Tang , Abuliti Abudula , Guoqing Guan

A facile agar-gel method was successfully applied to prepare a series of homogenous Mn-Co mixed oxides with different Mn/Co molar ratios for highly efficient catalysis of total toluene oxidation. The obtained Mn2Co1 mixed oxide exhibited a high catalytic activity with excellent durability as well as high tolerability even under 20 vol.% water vapor environment. Characterizations by XRF, XRD, N2 adsorption-desorption, SEM, TEM, H2-TPR, O2-TPD, XPS measurements with density functional theory (DFT) calculations indicated that the obtained optimum Mn-Co mixed oxide had high specific surface area, large amounts of Co3+, Mn3+, and Mn4+ species, abundant adsorbed oxygen species, rich lattice defects, high reducibility at low temperature, and excellent O2 adsorption ability. Meanwhile, in situ DRIFTS spectra measurements confirmed the generated intermediates at different environments during the toluene oxidation and revealed that both adsorbed oxygen and lattice oxygen species could simultaneously participate in the toluene adsorption-oxidation process, especially the rate-controlling step should be the C=C breakage of aromatic ring. It is expected that the present agar-gel method with low cost and convenient operation could be widely applied for the designing of novel mixed metal oxides catalysts for VOCs oxidation.



中文翻译:

通过快速琼脂-凝胶法在Mn-Co混合氧化物中生成大量缺陷,以高效催化总甲苯氧化

一种简便的琼脂凝胶法已成功地用于制备一系列具有不同Mn / Co摩尔比的均相Mn-Co混合氧化物,以高效催化总甲苯氧化。所得的Mn 2 Co 1混合氧化物即使在20体积%的水蒸气环境下也显示出高催化活性,优异的耐久性以及高耐受性。通过XRF,XRD,N 2吸附-解吸,SEM,TEM,H 2 -TPR,O 2 -TPD,XPS的表征以及密度泛函理论(DFT)计算表明,所获得的最佳Mn-Co混合氧化物具有较高的比表面积。面积,大量的Co 3+,Mn 3+和Mn 4+种类,丰富的吸附氧种类,丰富的晶格缺陷,低温下的高还原性和优异的O 2吸附能力。同时,原位DRIFTS光谱测量证实了甲苯氧化过程中在不同环境下生成的中间体,并揭示了吸附的氧和晶格氧物种都可以同时参与甲苯的吸附-氧化过程,特别是速率控制步骤应为C = C芳香环断裂。期望本发明的成本低廉且操作方便的琼脂凝胶方法可广泛用于设计用于VOCs氧化的新型混合金属氧化物催化剂。

更新日期:2020-10-02
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