Study on catalytic performance of supported transition metal oxide catalyst for ozone decomposition
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摘要: 通过浸渍法制备了γ-Al2O3负载镍、锰、钴等不同金属氧化物催化剂，在25 ℃、200000 mL/（gcat·h）的空速条件下，研究了其臭氧催化分解性能。结果表明，10%NiO/γ-Al2O3催化剂催化活性最佳，20 h内臭氧转化率高于96%。借助XRD、XPS、TEM、SEM-EDS、H2-TPR等表征手段，揭示出在NiO/γ-Al2O3催化剂表面形成的镍铝尖晶石结构可能是其优良臭氧分解性能的内在原因。此外，揭示出在不同过渡金属氧化物负载型催化剂上臭氧分解机理不同，相关研究为镍、锰等过渡金属氧化物催化剂催化分解臭氧的反应机理提供了新思路，并为开发高效的臭氧分解催化剂提供了指导。Abstract: In this paper, γ-Al2O3 supported nickel, manganese, cobalt, and other metal oxide catalysts were prepared by the impregnation method respectively, and its ozone catalytic decomposition performance was studied at 25 ℃ under a WHSV of 200000 mL/(gcat·h). The results showed that 10% NiO/γ-Al2O3 catalyst demonstrates superior catalytic activity, and the ozone conversion rate is higher than 96% within 20 h. According to the characterizations of XRD, XPS, TEM, SEM-EDS and H2-TPR, its excellent ozone may be attributed to the formation of NiAl2O4 spinel on the surface of NiO/γ-Al2O3 catalyst. Furthermore, the mechanism of ozone decomposition on different transition metal oxide catalysts is divergent. The related study sheds new light on the reaction mechanism of ozone catalytic decomposition over transition metal oxides such as nickel and manganese, it also provides the guidelines for the development of efficient ozone decomposition catalysts.
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Key words:
- ozone /
- catalytic decomposition /
- catalyst /
- metal oxide
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图 4 三种催化剂的扫描电镜照片
Figure 4 SEM and EDS images of three catalysts
(a), (b): Ni-Al; (c), (d): Mn-Al; (e), (f): Co-Al
图 5 催化剂10% MOx/γ-Al2O3的透射电镜照片
Figure 5 TEM image of 10% MOx/γ-Al2O3
(a), (e): Ni-Al; (b): Mn-Al; (c), (d): Co-Al
图 6 不同催化剂的H2-TPR和O2-TPD谱图
Figure 6 Redox properties of different catalysts
(a): H2-TPR; (b): O2-TPD
图 7 反应前后三种催化剂的XPS谱图
Figure 7 XPS spectra of fresh and used catalysts
(a): Ni 2p3/2 of Ni-Al; (b): Mn 2p3/2 of Mn-Al; (c): Co 2p3/2 of Co-Al
表 1 不同催化剂的理化结构参数
Table 1 Texture properties of different catalysts
Sample SBET/（m2·g−1） Pore volume/（cm3·g−1） Pore diameter/nm γ-Al2O3 202 0.334 4.34 Ni-Al 175 0.293 4.34 Mn-Al 177 0.292 4.34 Co-Al 168 0.268 4.33 Fe-Al 180 0.27 4.33 Cu-Al 175 0.27 4.33 
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表 2 钴氧化物负载型催化剂的元素分析
Table 2 Elemental distributions over the Co-Al catalyst
Element Weight/% Atomic/% S1 S2 S1 S2 O 40.46 33.02 53.89 50.07 Al 57.40 45.88 45.34 41.25 Co 2.14 21.10 0.77 8.68
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表 3 镍氧化物负载型催化剂的元素分析
Table 3 Elemental distributions over the Ni-Al catalyst
Element Weight/% Atomic/% S1 S2 S1 S2 O 46.61 41.89 61.37 56.48 Al 46.15 51.31 36.03 41.02 Ni 7.25 6.79 2.6 2.5
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