Supporting information for Hierarchical porous Fe3C@Fe-N-C catalysts from tannin-Fe(III) complexes for efficient oxygen reduction [Dataset]
Figure S1. FTIR spectra of dried mimosa tannin and hydrochars obtained with and without addition of iron (III) chloride, using a Pluronic-127/mimosa tannin mass ratio of 0.5 (FeTHC-R0.5 and THCR0.5, respectively). Figure S2. Fe3C lattice fringes for Fe-N-(FeTC-R0.5). Aberration-corrected HAADF-STEM...
| Autores: | , , , , , , , , |
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| Tipo de recurso: | conjunto de datos |
| Fecha de publicación: | 2024 |
| País: | España |
| Institución: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/381711 |
| Acceso en línea: | http://hdl.handle.net/10261/381711 |
| Access Level: | acceso abierto |
| Palabra clave: | Iron carbide Tannin-metal complex Oxygen reduction reaction http://metadata.un.org/sdg/7 Ensure access to affordable, reliable, sustainable and modern energy for all |
| Sumario: | Figure S1. FTIR spectra of dried mimosa tannin and hydrochars obtained with and without addition of iron (III) chloride, using a Pluronic-127/mimosa tannin mass ratio of 0.5 (FeTHC-R0.5 and THCR0.5, respectively). Figure S2. Fe3C lattice fringes for Fe-N-(FeTC-R0.5). Aberration-corrected HAADF-STEM images and FFT patterns of different Fe3C particles. The images were recorded using an analytical Titan microscope. Figure S3. Aberration-corrected HAADF-STEM images for Fe-N-(FeTC-R0.5). The images were recorded using an analytical Titan microscope. Figure S4. XRD patterns of TC-R0.5, FeTC-R0.5, Fe-N-(TC-R0.5) and N-(FeTC-R0.5). Figure S5. (a) Raw first- and second-order Raman spectra for TC-R0.5 and Fe-N-(FeTC-R0.5). (b) Deconvolution of first-order Raman profiles into 5 bands. Intensity ratios of deconvoluted bands D (⁓1343 cm-1) and 2D (⁓2676 cm-1) to G (⁓1580 cm-1) are included in the figures. Figure S6. (a) Deconvolution of high-resolution N1s XPS spectra and, (b) high-resolution Fe2p XPS spectra of tannin-derived electrocatalysts. Figure S7. Fe3C lattice fringes for FeTC-R0.5. Aberration-corrected HRTEM and HAADFSTEM images of different Fe3C particles obtained using an analytical Titan microscope. Figure S8. Textural properties of Fe-N-(FeTC-R0.5) and reference materials: (a) N2 adsorption (solid curves) and desorption (dotted curves) isotherms at -196 °C; (b) Pore size distribution (PSD) determined by applying the NLDFT method to N2 and H2 isotherms. The insets show zooms. Figure S9. LSV curves of FeTC-R0.5 and Fe-(FeTC-R0.5) in O2-saturated aqueous solutions of 0.1 M KOH (left) and 0.5 M H2SO4 (right) at 5 mV s-1 and 1600 rpm. Figure S10. (a) Electron transfer number, and (b) peroxide yields as a function of applied potential for tannin-derived catalysts obtained using different Pluronic-127/mimosa tannin mass ratios (R) in O2-saturated aqueous solutions of 0.1 M KOH (left) and 0.5 M H2SO4 (right) at 5 mV s-1 and 1600 rpm. Figure S11. Onset potential and E1/2 as a function of the relative contribution of surface N moieties determined by XPS in alkaline (left), and acidic (right) electrolytes, for electrocatalysts obtained from Fe-containing, tannin-derived hydrochars. Figure S12. Nyquist plots for Fe-N-(FeTC-R0.5) in 0.1 M KOH (left) and 0.5 M H2SO4 (right) aqueous solutions saturated with oxygen at 1600 rpm.Figure S13. Tafel plots of tannin-derived electrocatalyst in 0.1 M KOH (a, b) and 0.5 M H2SO4 (c, d) aqueous solutions saturated with oxygen at 1600 rpm.Figure S14. Chronoamperometric responses under continuous oxygen bubbling of Fe-N- (FeTC-R0.5) catalyst and Pt/C at 1600 rpm and at 0.7 V vs. RHE in 0.1 M KOH (left) and at 0.6 V vs. RHE in 0.5 M H2SO4 (right).Figure S15. CV curves of Fe-N-(FeTC-R0.5) before (solid curves) and after (dotted curves) chronoamperometric experiments at 0.7 V vs. RHE in 0.1 M KOH (left) and at 0.6 V vs. RHE in 0.5 M H2SO4 (right) aqueous solutions saturated with oxygen at 20 mV s-1. Figure S16. Methanol tolerance of Fe-N-(FeTC-R0.5) in O2-saturated electrolytes: 0.1 M KOH (left) and 0.5 M H2SO4 (right). Insets show zoomed-in current density vs. potential in the mixed controlled region. Table S1. Nomenclature of as-synthesized materials and experimental details in the hydrochar synthesis and carbonization stages. Table S2. Chemical composition of tannin-derived electrocatalysts determined by elemental analysis and ICP-AES. Table S3. Total Fe and N contents by XPS and distribution of nitrogen species (considering the total N content by XPS) in tannin-derived electrocatalysts, from deconvolution of the N1s XPS spectrum. Table S4. Results of fitting the Mössbauer spectrum of Fe-N-(FeTC-R0.5) with two sextet and two doublet components. The table reports values of isomer shift (IS), quadrupole splitting (QS), linewidth (LW) and hyperfine field (HF). Table S5. Main textural properties of tannin-derived electrocatalysts. Table S6. ORR parameters of tannin-derived electrocatalysts and Pt/C catalysts in alkaline (0.1 M KOH) and acidic (0.5 M H2SO4) media. Table S7. Summary of activity (E1/2) and stability (in terms of current retention after chronoamperometry (CA) tests) in 0.1 M KOH and 0.5 M H2SO4 of the Fe-N-(FeTC-R0.5) material presented here, and compared with biomass-derived M-N-C catalysts from the literature. Table S8. Comparison of Fe-N-(FeTC-R0.5) and other biomass-derived M-N-C catalysts in AEMFCs and PEMFCs. |
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