Boosting electrocatalytic CO2 reduction to formate via carbon nanofiber encapsulated bismuth nanoparticles with ultrahigh mass activity

doi:10.1016/S1872-2067(22)64177-9

Abstract

Abstract:

Electrochemical CO₂ conversion is one of the most promising technologies to achieve carbon neutrality. However, it still suffers from some nonnegligible challenges on low production rate and unsatisfied current densities for potential large-scale applications. Herein, we prepare ultrasmall Bi nanoparticles uniformly encapsulated in the carbon nanofibers through electrospinning techniques, which is denoted as Bi/CNFs-900. Gratifyingly, this Bi/CNFs-900 catalyst demonstrates excellent performance and stability on CO₂ electro-reduction in a broad potential window. Specifically, it can produce formate with a Faradaic efficiency over 90% and a high partial current density of -235.3 mA cm^-2 at −1.23 V vs. RHE in a flow-cell. Furthermore, the confinement effect of carbon nanofibers largely restricts the severe aggregation of bismuth nanoparticles during synthesis as well as electrolysis procedure, which greatly increases the accessible active sites and decreases the actual mass fraction of bismuth composition. Consequently, Bi/CNFs-900 not only achieves ultrahigh mass activity of -1.6 A mg_Bi^-1, but also possesses an unprecedented formate production rate of 4403.3 μmol h^-1 cm^-2. DFT calculations and in situ Raman spectroscopy further uncover the possible reaction mechanism for CO₂ reduction toward formate. These results could provide an economical and industrial-viable strategy for the preparation of electrocatalysts in CO₂ reduction.

Key words: CO₂ electro-reduction, Bismuth nanoparticle, Carbon nanofiber, Formate, Mass activity

Yan Kong, Xingxing Jiang, Xuan Li, Jianju Sun, Qi Hu, Xiaoyan Chai, Hengpan Yang, Chuanxin He. Boosting electrocatalytic CO₂ reduction to formate via carbon nanofiber encapsulated bismuth nanoparticles with ultrahigh mass activity[J]. Chinese Journal of Catalysis, 2023, 45: 95-106.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64177-9

https://www.cjcatal.com/EN/Y2023/V45/I2/95

Figures/Tables 7

Fig. 1. Schematic illustration of the preparation for Bi/CNFs samples.

Fig. 2. Low-magnification (a), high-resolution (inset images show the lattice fringes) (b) and high-magnification (c) TEM images of Bi/CNFs-900. (d) Particle size distributions image of Bi/CNFs-900. HAADF-STEM image (e) and the corresponding elemental mapping (Bi, C, N) (f,g,h) of Bi/CNFs-900.

Fig. 3. (a) XRD patterns of CNFs, Bi/CNFs-900, and Bi BP. (b) Raman spectra. (c) Nitrogen adsorption-desorption isotherms. (d) Pore size distributions of Bi/CNFs-900, Bi/CNFs-1000, CNFs, and Bi BPs.

Fig. 4. Electrochemical performances of Bi-based catalysts. (a) The LSV curves of Bi/CNFs-900 in N2 and CO2 atmosphere. (b) LSV curves of four samples. Faradaic efficiencies (c), mass activity (d), and yield rate (f) of formate for Bi/CNFs-900 or Bi BPs. (e) Production rate of Bi/CNFs-900 at different potentials. The error bars indicate the standard deviations of three independent experiments.

Fig. 5. Mass activity (a) and FEformate (b) as a function of jformate for Bi-based catalysts compared to other previous studies in the H-cell or Flow-cell. (c) Durability test and FE toward formate during extended measurement of Bi/CNFs-900 at -1.09 V vs. RHE, inset images show TEM and FESEM of Bi/CNFs-900 after durability tests.

Fig. 6. EIS plots (a) and Cdl (b) of Bi/CNFs-900, CNFs, and Bi BPs. (c) Survey XPS spectra of Bi/CNFs-900, Bi/CNFs-1000, Bi BPs, and CNFs. (d) XPS spectra of Bi 4f for Bi/CNFs-900 and Bi BPs.

Fig. 7. (a) Potential-dependent in situ Raman spectra of Bi/CNFs-900 catalyst in CO2-saturated 0.5 mol L-1 KHCO3. (b) Single oxidative LSV scans in N2-saturated 0.1 mol L-1 KOH electrolyte for Bi/CNFs-900, Bi/CNFs-1000, Bi BPs, and CNFs. Gibbs free energy diagrams for CO2RR toward formate (c), and CO2RR toward CO (d).

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Boosting electrocatalytic CO₂ reduction to formate via carbon nanofiber encapsulated bismuth nanoparticles with ultrahigh mass activity

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