Vacancy engineering of carbon support strengthens the interaction with in-situ synthesized Pt nanodendrites for boosted oxygen reduction electrocatalysis

doi:10.1016/S1872-2067(23)64620-0

Abstract

Abstract:

Controlling the morphology of Pt nanostructures can provide a great opportunity to improve their catalytic properties by increasing their active sites and atomic utilization. Here, Pt nanodentrites (NDs) dispersed on intrinsic vacancy-rich hollow nitrogen-doped carbon (Pt@HNC-V) have been successfully prepared through an integrated strategy of in situ Cl^- mediated growth and carbon intrinsic vacancy engineering. Raman and electron paramagnetic resonance measurements have demonstrated that our method enables selective transformation of precursors into vacancy-rich samples or vacancy-free ones through a variable etching route. Moreover, X-ray absorption and X-ray photoelectron spectroscopy further verified that the vacancy-rich sample (Pt@HNC-V-800) demonstrates a lower Pt-Pt bond coordination number (8.64) and a stronger electron-donating effect of Pt compared with the vacancy-free Pt@HNC sample. In addition, density functional theory calculations indicate that the vacancy-rich Pt@HNC-V lowers the oxygen overpotential, resulting in optimized adsorption energies of oxygen reduction reaction (ORR) intermediates on Pt NDs and thus yielding improved oxygen reduction reaction activity. Benefiting from Pt NDs with abundant active sites and the strong electronic effect between them and the intrinsic carbon vacancy substrate, the half-wave potential of ORR for Pt@HNC-V-800 is as high as 0.947 V, and the mass activity is 1.55 A mg^-1Pt, which is significantly higher than that of commercial Pt/C. The synergy between Pt NDs and carbon intrinsic vacancy engineering can enhance the overall ORR performance, which is beneficial for material preparations in the field of energy and catalysis.

Key words: Oxygen reduction reaction, Pt nanodendrites, Carbon intrinsic vacancy, Electrocatalyst, Metal-support interaction

Wei Liao, Qian Zhou, Jin Long, Chenzhong Wu, Bin Wang, Qiong Peng, Jianxin Cao, Qingmei Wang. Vacancy engineering of carbon support strengthens the interaction with in-situ synthesized Pt nanodendrites for boosted oxygen reduction electrocatalysis[J]. Chinese Journal of Catalysis, 2024, 59: 260-271.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64620-0

https://www.cjcatal.com/EN/Y2024/V59/I4/260

Figures/Tables 5

Scheme 1. Schematic illustration of the preparations for Pt@HNC-V-T and Pt@HNC catalysts.

Fig. 1. (a) Schematic of synthesis for Pt@HNC-V-800-T and Pt@HNC samples. TEM images and corresponding HRTEM images of Pt@HNC-V-800 (b,d) and Pt@HNC (c,e) catalysts. (f-j) HAADF-STEM images of Pt@HNC-V-800 and elemental mapping images. Raman spectra (k) and EPR spectra (l) of Pt@HNC-V-800-T catalysts.

Fig. 2. XRD patterns (a), XPS spectra of Pt 4f (b), and CO stripping curves (c) of Pt@HNC-V-800, Pt@HNC, and Pt/C. (d) Pt L3-edge XANES spectra of Pt@HNC-V-800, Pt@HNC, Pt foil, and PtO2. (e) The k2-weighted Fourier transform EXAFS spectra. Corresponding EXAFS fits for Pt@HNC-V-800 (f) and Pt@HNC (g) in the k and R spaces. (h) WT for k2-weighted Pt L3-edge EXAFS signals in the Pt@HNC-V-800, Pt@HNC, and reference samples (Pt foil and PtO2).

Fig. 3. ORR polarization plots (a) and Tafel slopes (b) of Pt@HNC-V-T, Pt@HNC, and Pt/C catalysts. (c) ORR polarization curves of Pt@HNC-V-800 with various rotation rates at a scan rate of 10 mV/s and corresponding Koutecky-Levich curves (inset). (d) The corresponding mass activities and specific activities at 0.9 V vs. RHE for Pt@HNC-V-T, Pt@HNC, and Pt/C catalysts. ORR polarization curves of Pt@HNC-V-800 (e), Pt@HNC (f), and Pt/C (g) catalysts before and after the durability test. The insets in (e)-(g) show the CV curves of Pt@HNC-V-800, Pt@HNC, and Pt/C catalysts before and after the durability test. MA (h) and SA (i) at 0.9 V vs. RHE for Pt@HNC-V-800, Pt@HNC, and Pt/C catalysts.

Fig. 4. (a) DFT calculates models. (b) Proposed ORR mechanisms of the Pt@HNC-V model. Free-energy illustration of three catalyst models at U = 0 V (c) and U = 1.23 V (d). (e) Binding energy for Pt NDs on carbon substrates for the catalyst models. The DOS on Pt@HNC-V (f) and Pt@HNC (g) models. (h) Comparison of DOS on Pt of different models.

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