Regulating carbon work function to boost electrocatalytic activity for the oxygen reduction reaction

doi:10.1016/S1872-2067(20)63701-9

Abstract

Abstract:

Electronic regulation of carbon is essential for developing non-platinum electrocatalysts for oxygen reduction reactions (ORRs). In this work, we used Cs to further regulate the electronic structure of nitrogen-doped (N-doped) carbon. The Cs atoms coordinated with the nitrogen atom in the N-doped carbon for injecting electrons into the carbon conjugate structure and reducing the work function of the carbon network. The low-work-function surface improved electron donation, facilitated O₂ dissociation, and enhanced the adsorption of an OOH* intermediate. Thus, electrocatalytic performance for the ORR was improved. The material shows potential as an ORR electrocatalyst comparable with Pt/C.

Key words: Cesium doping, Nitrogen-doped carbon, Electronic regulation, Work function, Oxygen reduction reaction

Yazhi Cai, Li Tao, Gen Huang, Nana Zhang, Yuqin Zou, Shuangyin Wang. Regulating carbon work function to boost electrocatalytic activity for the oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2021, 42(6): 938-944.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63701-9

https://www.cjcatal.com/EN/Y2021/V42/I6/938

Figures/Tables 4

Scheme 1. Schematic illustrations of the preparation of the Cs-N/C and N/C.

Fig. 1. SEM images of Cs-N/C (a) and N/C (b); (c) TEM image of Cs-N/C; (d) HRTEM image of Cs-N/C (inset in (d) shows SAED pattern of Cs-N/C); (e) EDS elemental mapping images of Cs-N/C.

Fig. 2. (a) XRD patterns for Cs-N/C and N/C; (b) XPS survey for Cs-N/C and N/C; (c) Cs 3d spectra for Cs-N/C and Cs2CO3; (d) Raman spectra for Cs-N/C and N/C; (e) C 1s spectra for N/C and Cs-N/C; (f) N 1s spectra for N/C and Cs-N/C.

Fig. 3. (a) The UPS spectra of Cs-N/C and N/C; (b) ORR polarization curves of Cs-N/C, N/C and Pt/C; (c) Tafel plots of Cs-N/C, N/C and Pt/C; (d) Correlation of jk of Cs-N/C and N/C at various potentials with their work function values; (e) Koutecky-Levich plots at 0.7 V of Cs-N/C and N/C; (f) Nyquist plots of Cs-N/C at 0.79, 0.76, 0.74 V and N/C at the potential of 0.93, 0.91, 0.89 V vs RHE.

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