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构建用于高效低温甲烷燃烧的Pd(PdO)/CoO@SiO核壳结构。

Construction of a Pd(PdO)/CoO@SiO core-shell structure for efficient low-temperature methane combustion.

作者信息

Ma Yongde, Li Shusheng, Zhang Tianhua, Zhang Yangyu, Wang Xiuyun, Xiao Yihong, Zhan Yingying, Jiang Lilong

机构信息

National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou, Fujian 350002, China.

出版信息

Nanoscale. 2021 Mar 12;13(9):5026-5032. doi: 10.1039/d0nr08723h.

Abstract

Catalytic combustion is a promising way to remove trace amounts of CH4 to alleviate serious environmental concerns. However, the reactivity of a catalyst at low temperature is usually limited because of the difficulty to activate the C-H bond of methane. Herein, we design a Pd(PdO)/Co3O4@SiO2 bimetallic oxide core-shell catalyst which shows much higher activity in the methane combustion reaction compared with Pd(PdO)/SiO2 and Co3O4@SiO2 catalysts without a core-shell structure. The T50% and T90% of Pd(PdO)/Co3O4@SiO2 are 357 °C and 445 °C, respectively, which decrease by 67 °C and 55 °C in comparison with those of Pd(PdO)/SiO2. Extensive characterization demonstrates that the bimetallic oxide core-shell structure can effectively enhance the metal interaction between Pd and Co, which can weaken the strength of the Co-O bond in Pd(PdO)/Co3O4@SiO2. The weakening of the Co-O bond could promote the release of more lattice oxygen species to participate in the C-H breaking, resulting in superior catalytic performance in methane combustion at low temperature.

摘要

催化燃烧是去除痕量CH4以缓解严重环境问题的一种有前景的方法。然而,由于难以活化甲烷的C-H键,催化剂在低温下的反应活性通常受到限制。在此,我们设计了一种Pd(PdO)/Co3O4@SiO2双金属氧化物核壳催化剂,与没有核壳结构的Pd(PdO)/SiO2和Co3O4@SiO2催化剂相比,它在甲烷燃烧反应中表现出更高的活性。Pd(PdO)/Co3O4@SiO2的T50%和T90%分别为357℃和445℃,与Pd(PdO)/SiO2相比分别降低了67℃和55℃。广泛的表征表明,双金属氧化物核壳结构可以有效地增强Pd和Co之间的金属相互作用,这可以削弱Pd(PdO)/Co3O4@SiO2中Co-O键的强度。Co-O键的削弱可以促进更多晶格氧物种的释放以参与C-H键的断裂,从而在低温甲烷燃烧中表现出优异的催化性能。

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