Citation: Jingjun Liu, Xuemin Jin, Weiwei Song, Feng Wang, Nan Wang, Ye Song. Facile preparation of modified carbon black-LaMnO₃ hybrids and the effect of covalent coupling on the catalytic activity for oxygen reduction reaction[J]. Chinese Journal of Catalysis, ;2014, 35(7): 1173-1188. doi: 10.1016/S1872-2067(14)60066-8 shu

Facile preparation of modified carbon black-LaMnO₃ hybrids and the effect of covalent coupling on the catalytic activity for oxygen reduction reaction

1.
State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Electrochemical Process and Technology for Materials, Beijing University of Chemical Technology, Beijing 100029, China

Corresponding author: Feng Wang,
Received Date: 5 December 2013
Available Online: 28 February 2014
Fund Project: This work was supported by the National Natural Science Foundation of China (51272018, 51125007) (51272018, 51125007)D Program (2009BAE87B00). (2009BAE87B00)

Covalent coupling between LaMnO₃nanoparticles and carbon black to produce a composite catalyst for oxygen reduction reaction (ORR) was achieved by physical mixing of modified carbon and perovskite-type LaMnO₃ nanoparticles, followed by sintering at different temperatures. Perovskite-type LaMnO₃ nanoparticles were first synthesized via chemical precipitation, and the carbon support (Vulcan XC-72) was modified using graphitization, followed by HNO₃ and ammonia treatments. The morphology and electronic states of the carbon black-LaMnO₃ hybrid catalyst were characterized by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The loaded LaMnO₃ particles featured rod-like, three bars-like, and bamboo rod-like structures and were homogeneously dispersed in the carbon matrix that featured a hollow spherical structure. At a sintering temperature of about 300℃, C-O-M (M=La, Mn) bonds formed at the interface between the carbon and LaMnO₃ nanoparticles. Electrochemical measurements in 1 mol/L NaOH showed that the carbon-LaMnO₃ hybrid prepared at a LaMnO₃/GCB mass ratio of 2:3 displayed the highest electrocatalytic activity towards ORR among all the synthesized hybrid catalysts. The electrocatalytic activity was comparable with that obtained by commercial Pt/C catalyst (E-TEK). The average electron transfer number of ORR was ~3.81, and the corresponding yield of the hydrogen peroxide intermediatewas ~9.5%. The remarkably improved electrocatalytic activity towards ORR was likely because of the formation of covalent bonds (C-O-M) between the LaMnO₃ nanoparticles and carbon that can effectively enhance the ORR kinetics. This information is important to understand the physical origin of the electrocatalytic activity of carbon-supported rare earth oxides as catalysts for ORR.
- LaMnO₃particle,
- Carbon black,
- Electrocatalytic,
- Covalent coupling,
- Oxygen reduction reaction
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沈阳化工大学材料科学与工程学院沈阳 110142

Facile preparation of modified carbon black-LaMnO3 hybrids and the effect of covalent coupling on the catalytic activity for oxygen reduction reaction

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通讯作者: 陈斌, bchen63@163.com

Facile preparation of modified carbon black-LaMnO₃ hybrids and the effect of covalent coupling on the catalytic activity for oxygen reduction reaction