Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (6): 963-970.DOI: 10.1016/S1872-2067(20)63716-0
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Jing Lia, Xiang Sunb, Yongzheng Duana, Dongmei Jiaa, Yuejin Lia,b, Jianguo Wangb,*()
Received:
2020-07-28
Accepted:
2020-09-14
Online:
2021-06-18
Published:
2021-01-30
Contact:
Jianguo Wang
About author:
*Tel/Fax: +86-571-88871037; E-mail: jgw@zjut.edu.cnSupported by:
Jing Li, Xiang Sun, Yongzheng Duan, Dongmei Jia, Yuejin Li, Jianguo Wang. Enhanced oxygen reduction reaction performance over Pd catalysts by oxygen-surface-modified SiC[J]. Chinese Journal of Catalysis, 2021, 42(6): 963-970.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63716-0
Fig. 1. TEM characterization of the Pd/O-SiC catalyst. (a) TEM image (inset: Pd particle size in the Pd/O-SiC catalyst); (b) HRTEM image; (c) EDX pattern; (d-h) EDS elemental mapping images of Si, C, O, and Pd in Pd/O-SiC.
Fig. 2. XRD and XPS characterizations of catalysts. (a) XRD patterns; (b) Pd 3d; (c) Si 2p; (d) C 1s XPS high-resolution spectra of O-SiC and Pd/O-SiC with various Pd loadings.
Fig. 3. Electronic structures of Pd/O-SiC and Pd/C. Charge density difference, binding energies, and Bader charge of Pd4 supported on O-SiC (a,c) and graphene (b,d). The blue and yellow areas in Fig. 3(a)-(b) represent negative and positive charges, respectively.
Fig. 4. Electrochemical analysis of catalysts. (a) CV results for Pd/O-SiC, O-SiC, Pd/C, and Pt/C catalysts in O2-saturated 0.1 M KOH solution obtained with a scan rate of 100 mV s-1. (b) ORR polarization curves of different catalysts acquired at 1600 rpm. The potential scan rate was 20 mV s-1. (c) Rotation-rate-dependent voltammograms of Pd/O-SiC in 0.1 M KOH solution at 400-2500 rpm. The inset shows the K-L plots of the Pd/O-SiC catalyst. (d) RRDE measurements (1600 rpm) of Pd/O-SiC (inset: Electron-transfer numbers and peroxide percentage of the Pd/O-SiC electrode). (e) Tafel plots of Pd/O-SiC, O-SiC, Pd/C, and Pt/C catalysts. (f) Chronoamperometric responses for ORR at Pd/O-SiC and Pt/C electrodes. The inset shows the comparison of the methanol oxidation tolerance of Pd/O-SiC and Pt/C at 0.50 VRHE.
Fig. 5. Optimized structures and binding energies of OOH adsorbed on Pd4/O-SiC (a) and Pd4/C (b); (c) Gibbs free energy diagrams of ORR over Pd4/O-SiC and Pd4/C.
Fig. 6. DFT calculations of Pd4/SiC. (a) Bader charge and binding energies of Pd4 supported on SiC; (b) Charge density difference of Pd4/SiC. Blue and yellow areas represent negative and positive charges, respectively; (c) Optimized structures and binding energies of OOH adsorbed on Pd4/SiC; (d) Gibbs free energy diagrams of ORR over Pd4/SiC and Pd4/O-SiC.
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