Research ArticleMATERIALS SCIENCE

Transition metal–assisted carbonization of small organic molecules toward functional carbon materials

See allHide authors and affiliations

Science Advances  27 Jul 2018:
Vol. 4, no. 7, eaat0788
DOI: 10.1126/sciadv.aat0788
  • Fig. 1 Preparation of CMs.

    (A) Schematic illustration of the preparation process of CMs. (B) Structures of the investigated SOMs for the CM preparation.

  • Fig. 2 TGA analyses.

    (A) TGA curves of different SOMs (TMS-free) in N2 atmosphere. (B) TGA curves of different SOMs with Co(NO3)2 in N2 atmosphere. (C) TGA curves of oPD with different TMSs in N2 atmosphere. (D) TGA curves of oPD with different Co(NO3)2 contents in N2 atmosphere.

  • Fig. 3 Microscopic characterization of CMs.

    (A to F) SEM and TEM images of CM-DCD/Co (A and B), CM-oPD/Co (C and D), and CM-BPy/Co (E and F). (G and H) HRTEM images of CM-DCD/Co (G) and CM-oPD/Co (H).

  • Fig. 4 Textural properties and chemical compositions of CMs.

    (A) Nitrogen adsorption/desorption isotherms of selected CMs. STP, standard temperature and pressure. (B) PSD of CM-DBrBPy/Co and CM-DBrBPy/Co/SiO2. (C) XRD patterns of CMs. a.u., arbitrary units. (D) Raman spectra of CMs. (E) XPS survey spectra of CM-DCD/Co and CM-BTH/Co. (F) High-resolution XPS spectra of the deconvoluted N 1s peak and Co 2p peak for CM-DCD/Co.

  • Fig. 5 Catalytic performance of CMs for selective oxidization of ethylbenzene and hydrogenation of nitrobenzene.

    (A) Reaction equation of selective oxidization of ethylbenzene. TBHP, tert-butyl hydroperoxide. (B and C) Activity (B) and stability (C) tests of CM catalysts for ethylbenzene oxidization. (D) Reaction equation of hydrogenation of nitrobenzene. (E and F) Activity (E) and stability (F) tests of CM catalysts for nitrobenzene hydrogenation.

  • Fig. 6 Electrocatalytic performance of CMs for HER.

    (A and B) Polarization curves of CM-DBrPhen/Co/SiO2 and commercial Pt/C catalyst in 0.5 M H2SO4 (A) and 1 M KOH (B). (C) Chronopotentiometry tests of CM-DBrPhen/Co/SiO2 at 10 mA cm−2 in 0.5 M H2SO4 and 1 M KOH, respectively.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/7/eaat0788/DC1

    Fig. S1. TGA analyses.

    Fig. S2. SEM and TEM images of CM-x/Co samples.

    Fig. S3. TEM images of oPD-derived CMs prepared with different TMSs.

    Fig. S4. SEM and TEM images of SiO2-templating CMs.

    Fig. S5. Characterizations of CM-oPD/Co/SBA-15, and CM-Phen/Co/SBA-15.

    Fig. S6. STEM-EDS elemental mapping images of CM-DCD/Co and CM-DCD/Co/SiO2.

    Fig. S7. STEM-EDS elemental mapping images of CM-oPD/Co and CM-oPD/Co/SiO2.

    Fig. S8. STEM-EDS elemental mapping images of CM-BTH/Co and CM-BTH/Co/SiO2.

    Fig. S9. XPS survey spectra of the DBrPhen/Co(NO3)2 precursor and its carbonization products obtained at 200° to 500°C.

    Fig. S10. GPC result of the sample that prepared by heating DBrPhen with Co(NO3)2 at 250°C for 0.5 hours under N2.

    Fig. S11. Images of dispersing carbonization product obtained by heating DBrPhen with Co(NO3)2 at 400°C for 2 hours under N2.

    Fig. S12. UV-vis absorption spectra for DBrBTh and the carbonization product obtained by heating BTh/Co(NO3)2 at 200°C for 0.5 hours under N2.

    Fig. S13. The structures of four SOMs that could not be converted into CMs.

    Fig. S14. XRD patterns of CM-Phen/Co, CM-Phen/Co/SiO2, CM-DBrPhen/Co, and CM-DBrPhen/Co/SiO2.

    Fig. S15. Detailed characterizations of CM-Phen/Co and CM-Phen/Co/SiO2 catalysts.

    Fig. S16. Detailed characterizations of CM-DBrPhen/Co and CM-DBrPhen/Co/SiO2 catalysts.

    Fig. S17. The poisoning experiments for ethylbenzene oxidization and nitrobenzene hydrogenation.

    Fig. S18. Catalytic performance for selective oxidization of ethylbenzene using O2 as the oxidant and hydrogenation of nitrobenzene using H2 as the reductant.

    Fig. S19. The poisoning experiments for HER.

    Fig. S20. Tafel curves of CM-DBrPhen/Co/SiO2 and commercial Pt/C catalyst.

    Fig. S21. Electrocatalytic performance of CMs for ORR in acidic medium.

    Fig. S22. HER polarization curves of CM-oPD/Co/SiO2 and CM-oPD/CoCu/SiO2 in 0.5 M H2SO4.

    Table S1. Summary of carbon yield, texture properties, elemental composition of CMs prepared with Co(NO3)2 as the catalyst.

    Table S2. Carbon yields of oPD with different TMSs as catalysts.

    Table S3. Carbon yields of oPD with different amounts of Co(NO3)2 as catalysts.

    Table S4. Summary of carbon yield, texture properties, and elemental composition of CMs prepared with Co(NO3)2 as the catalyst and SiO2 nanoparticles as hard templates.

    Table S5. HER performance comparison.

    Note S1. The proposed mechanism for different microstructures of CM-x/Co samples.

    Note S2. Synthesis of high–surface area CMs from SOMs with SBA-15 as templates.

    Note S3. Detailed characterization analysis of CM-Phen/Co, CM-Phen/Co/SiO2, CM-DBrPhen/Co, and CM-DBrPhen/Co/SiO2.

    Note S4. Electrocatalytic performance of CMs for ORR.

    References (5565)

  • Supplementary Materials

    This PDF file includes:

    • Fig. S1. TGA analyses.
    • Fig. S2. SEM and TEM images of CM-x/Co samples.
    • Fig. S3. TEM images of oPD-derived CMs prepared with different TMSs.
    • Fig. S4. SEM and TEM images of SiO2-templating CMs.
    • Fig. S5. Characterizations of CM-oPD/Co/SBA-15, and CM-Phen/Co/SBA-15.
    • Fig. S6. STEM-EDS elemental mapping images of CM-DCD/Co and CM-DCD/Co/SiO2.
    • Fig. S7. STEM-EDS elemental mapping images of CM-oPD/Co and CM-oPD/Co/SiO2.
    • Fig. S8. STEM-EDS elemental mapping images of CM-BTH/Co and CM-BTH/Co/SiO2.
    • Fig. S9. XPS survey spectra of the DBrPhen/Co(NO3)2 precursor and its carbonization products obtained at 200° to 500°C.
    • Fig. S10. GPC result of the sample that prepared by heating DBrPhen with Co(NO3)2 at 250°C for 0.5 hours under N2.
    • Fig. S11. Images of dispersing carbonization product obtained by heating DBrPhen with Co(NO3)2 at 400°C for 2 hours under N2.
    • Fig. S12. UV-vis absorption spectra for DBrBTh and the carbonization product obtained by heating BTh/Co(NO3)2 at 200°C for 0.5 hours under N2.
    • Fig. S13. The structures of four SOMs that could not be converted into CMs.
    • Fig. S14. XRD patterns of CM-Phen/Co, CM-Phen/Co/SiO2, CM-DBrPhen/Co, and CM-DBrPhen/Co/SiO2.
    • Fig. S15. Detailed characterizations of CM-Phen/Co and CM-Phen/Co/SiO2 catalysts.
    • Fig. S16. Detailed characterizations of CM-DBrPhen/Co and CM-DBrPhen/Co/SiO2 catalysts.
    • Fig. S17. The poisoning experiments for ethylbenzene oxidization and nitrobenzene hydrogenation.
    • Fig. S18. Catalytic performance for selective oxidization of ethylbenzene using O2 as the oxidant and hydrogenation of nitrobenzene using H2 as the reductant.
    • Fig. S19. The poisoning experiments for HER.
    • Fig. S20. Tafel curves of CM-DBrPhen/Co/SiO2 and commercial Pt/C catalyst.
    • Fig. S21. Electrocatalytic performance of CMs for ORR in acidic medium.
    • Fig. S22. HER polarization curves of CM-oPD/Co/SiO2 and CM-oPD/CoCu/SiO2 in 0.5 M H2SO4.
    • Table S1. Summary of carbon yield, texture properties, elemental composition of CMs prepared with Co(NO3)2 as the catalyst.
    • Table S2. Carbon yields of oPD with different TMSs as catalysts.
    • Table S3. Carbon yields of oPD with different amounts of Co(NO3)2 as catalysts.
    • Table S4. Summary of carbon yield, texture properties, and elemental composition of CMs prepared with Co(NO3)2 as the catalyst and SiO2 nanoparticles as hard templates.
    • Table S5. HER performance comparison.
    • Note S1. The proposed mechanism for different microstructures of CM-x/Co samples.
    • Note S2. Synthesis of high–surface area CMs from SOMs with SBA-15 as templates.
    • Note S3. Detailed characterization analysis of CM-Phen/Co, CM-Phen/Co/SiO2, CM-DBrPhen/Co, and CM-DBrPhen/Co/SiO2.
    • Note S4. Electrocatalytic performance of CMs for ORR.
    • References (5565)

    Download PDF

    Files in this Data Supplement:

Stay Connected to Science Advances

Navigate This Article