Skip to main content
SpringerLink
Log in

Enhanced sulfur dioxide electrooxidation performance on a modified XC-72 carbon catalyst

  • Original Paper
  • Published:
Journal of Solid State Electrochemistry Aims and scope Submit manuscript

Abstract

Vulcan XC-72 is a carbon catalyst that is widely used in electrochemistry. The electrooxidation of SO2 plays a significant role in the domain of environmental protection. In this work, successive thermal and pyrolytic processes were applied to Vulcan XC-72 in order to obtain a modified catalyst that promotes SO2 electrooxidation to a much greater degree than Vulcan XC-72 does. The preparation of this modified XC-72 involved three steps: doping, pore creation, and carbonization. These modification processes were shown to greatly increase the catalytic activity of the modified XC-72 during SO2 electrooxidation. The catalytic performance of the modified XC-72 towards SO2 electrooxidation was characterized via linear sweep voltammograms and cyclic voltammograms; the results showed that the onset potential and the E imax/2 obtained with the modified XC-72 were 60 mV and 128 mV lower, respectively, than attained with Vulcan XC-72. The structural and physical properties of the modified XC-72 were characterized using TEM, XPS, and BET. The increased surface area and optimized pore structure of the modified XC-72, as well as the presence of pyridinic N constituents in this material, are believed to contribute to its enhanced capacity to catalyze the electrooxidation of SO2.

ᅟ

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1a–d
Fig. 2a–b
Fig. 3a–b
Fig. 4a–c

Similar content being viewed by others

References

  1. Spotnitz RM, Loeffler CE, Langer SH (1981) Electrogenerative oxidation of sulphur dioxide. J Appl Electrochem 11(4):403–405

  2. Allen JA, Rowe G, Hinkley JT, Donne SW (2014) Electrochemical aspects of the hybrid sulfur cycle for large scale hydrogen production. Int J Hydrog Energy 39(22):11376–11389

    Article  CAS  Google Scholar 

  3. Baturina OA, Gould BD, Garsany Y, Swider-Lyons KE (2010) Insights on the SO2 poisoning of Pt3Co/VC and Pt/VC fuel cell catalysts. Electrochim Acta 55(22):6676–6686

  4. Kriek RJ, Rossmeisl J, Siahrostami S, Bjorketun ME (2014) H2 production through electro-oxidation of SO2: identifying the fundamental limitations. Phys Chem Chem Phys 16(20):9572–9579

  5. Quijada C, Rodes A, Vazquez JL, Perez JM, Aldaz A (1995) Electrochemical behavior of aqueous SO2 at Pt electrodes in acidic medium—a voltammetric and in-situ Fourier-transform Ir study. 1. Oxidation of SO2 on PT electrodes with sulfur-oxygen adsorbed species. J Electroanal Chem 394(1–2):217–227

  6. Fu J, Hou M, Du C, Shao Z, Yi B (2009) Potential dependence of sulfur dioxide poisoning and oxidation at the cathode of proton exchange membrane fuel cells. J Power Sources 187(1):32–38

    Article  CAS  Google Scholar 

  7. Baturina OA, Gould BD, Northrup PA, Swider-Lyons KE (2013) SO2 adsorption products on Pt nanoparticles as a function of electrode potential and oxidative properties of carrier gas: in situ sulfur K-edge XANES approach. Catal Today 205:106–110

  8. O’Brien JA, Hinkley JT, Donne SW, Lindquist SE (2010) The electrochemical oxidation of aqueous sulfur dioxide: a critical review of work with respect to the hybrid sulfur cycle. Electrochim Acta 55(3):573–591

    Article  Google Scholar 

  9. Hu Y, Yang C, Cao L, Yang J (2013) An electrochemical membrane reactor for a recycled FGD process. Chem Eng J 223:563–571

    Article  CAS  Google Scholar 

  10. Ohashi N, Yoshizawa K, Endou A, Takami S, Kubo M, Miyamoto A (2001) Adsorption properties of SO2 on ultrafine precious metal particles studied using density functional calculation. Appl Surf Sci 177(3):180–188

  11. Taieb D, Ben Brahim A (2013) Electrochemical method for sulphur dioxide removal from flue gases: application on sulphuric acid plant in Tunisia. C R Chim 16(1):39–50

  12. Ramaker DE, Gatewood D, Korovina A, Garsany Y, Swider-Lyons KE (2010) Resolving sulfur oxidation and removal from Pt and Pt3Co electrocatalysts using in situ X-ray absorption spectroscopy. J Phys Chem C 114(27):11886–11897

  13. O’Brien JA, Hinkley JT, Donne SW (2012) Electrochemical oxidation of aqueous sulfur dioxide. II. Comparative studies on platinum and gold electrodes. J Electrochem Soc 159(9):F585–F593

  14. Zhai J, Hou M, Zhang H, Zhou Z, Fu J, Shao Z, Yi B (2011) Study of sulfur dioxide crossover in proton exchange membrane fuel cells. J Power Sources 196(6):3172–3177

    Article  CAS  Google Scholar 

  15. Zhai J, Hou M, Liang D, Shao Z, Yi B (2012) Investigation on the electrochemical removal of SO2 in ambient air for proton exchange membrane fuel cells. Electrochem Commun 18:131–134

  16. Xie F, Shao Z-G, Zhang G, Zhai J, Lu W, Qin X, Lin W, Yi B (2012) A quantitative research on S- and SO2-poisoning Pt/Vulcan carbon fuel cell catalyst. Electrochim Acta 67:50–54

  17. Quijada C, Rodes A, Huerta F, Vazquez JL (1998) In situ FT-IRRAS study of SO2 adlayers formed on Pt(111) electrodes from open-circuit adsorption in acidic media. Electrochim Acta 44(6–7):1091–1096

  18. Lee S-K, Kim C-H, Cho W-C, Kang K-S, Park C-S, Bae K-K (2009) The effect of Pt loading amount on SO2 oxidation reaction in an SO2-depolarized electrolyzer used in the hybrid sulfur (HyS) process. Int J Hydrog Energy 34(11):4701–4707

  19. Quijada C, Rodes A, Vazquez JL, Perez JM, Aldaz A (1995) Electrochemical behavior of aqueous sulfur dioxide at polycrystalline Pt electrodes in acidic medium—a voltammetric and in-situ FT-IR study. 2. Promoted oxidation of sulfur dioxide. Reduction of sulfur dioxide. J Electroanal Chem 398(1–2):105–115

  20. Garsany Y, Baturina OA, Swider-Lyons KE (2009) Oxygen reduction reaction kinetics of SO2-contaminated Pt3Co and Pt/Vulcan carbon electrocatalysts. J Electrochem Soc 156(7):B848–B855

  21. Quijada C, Morallon E, Vazquez JL, Berlouis LEA (2000) Electrochemical behaviour of aqueous SO2 at polycrystalline gold electrodes in acidic media. A voltammetric and in-situ vibrational study. Part II. Oxidation of SO2 on bare and sulphur-modified electrodes. Electrochim Acta 46(5):651–659

  22. Quijada C, Vazquez JL (2005) Electrochemical reactivity of aqueous SO2 on glassy carbon electrodes in acidic media. Electrochim Acta 50(27):5449–5457

  23. Mu C, Hou M, Xiao Y, Zhang H, Hong S, Shao Z (2015) Electrochemical oxidation of sulfur dioxide on nitrogen-doped graphite in acidic media. Electrochim Acta 171:29–34

    Article  CAS  Google Scholar 

  24. Besenhard JO, Fritz HP (1983) The electrochemistry of black carbons. Angew Chem Int Ed Engl 22(12):950–975

    Article  Google Scholar 

  25. Zhou W, Zhou J, Zhou Y, Lu J, Zhou K, Yang L, Tang Z, Li L, Chen S (2015) N-doped carbon-wrapped cobalt nanoparticles on N-doped graphene nanosheets for high-efficiency hydrogen production. Chem Mater 27(6):2026–2032

    Article  CAS  Google Scholar 

  26. Wu Z, Iqbal Z, Wang X (2015) Metal-free, carbon-based catalysts for oxygen reduction reactions. Front Chem Sci Eng 9(3):280–294

    Article  CAS  Google Scholar 

  27. Bagreev A, Bashkova S, Bandosz TJ (2002) Adsorption of SO2 on activated carbons: the effect of nitrogen functionality and pore sizes. Langmuir 18(4):1257–1264

  28. Qu DY, Shi H (1998) Studies of activated carbons used in double-layer capacitors. J Power Sources 74(1):99–107

    Article  CAS  Google Scholar 

  29. Biddinger EJ, Ozkan US (2010) Role of graphitic edge plane exposure in carbon nanostructures for oxygen reduction reaction. J Phys Chem C 114(36):15306–15314

    Article  CAS  Google Scholar 

  30. Furmaniak S, Terzyk AP, Szymanski GS, Gauden PA, Motak M, Kowalczyk P, Rychlicki G (2006) Thermodynamics of the CMMS approach and carbon surface chemistry in SO2 adsorption. Langmuir 22(16):6887–6892

  31. Trogadas P, Fuller TF, Strasser P (2014) Carbon as catalyst and support for electrochemical energy conversion. Carbon 75:5–42

    Article  CAS  Google Scholar 

  32. Chiou CY, Chou TC (1998) Characteristics of the gas-diffusion electrode for SO2 sensors. Electroanalysis 10(13):897–903

  33. Punyawudho K, Ma S, Van Zee JW, Monnier JR (2011) Effect of O2 on the adsorption of SO2 on carbon-supported Pt electrocatalysts. Langmuir 27(12):7524–7530

  34. Mortari DA, Crnkovic PM, Avila I, Milioli FE (2010) Interpretation of the mechanism diffusion in the gas-solid process of the dessulfurization reaction. Quim Nov. 33(9):1887–1891

  35. Nikolov I, Vitanova I, Najdenov V, Milusheva T, Vitanov T (1997) Effect of pyrolysis temperature of the catalytic activity of active carbon plus cobalt phthalocyanine in sulfur dioxide oxidation by oxygen. J Appl Electrochem 27(1):77–82

    Article  CAS  Google Scholar 

  36. Ozdemir S, Gole JL (2010) Selectivity improvement and response time scale of porous silicon conductometric gas sensors. ECS Trans 33(8):111–115

  37. Lua AC, Yang T (2009) Theoretical analysis and experimental study on SO2 adsorption onto pistachio-nut-shell activated carbon. AICHE J 55(2):423–433

  38. Monteiro MJ, Ando RA, Siqueira LJA, Camilo FF, Santos PS, Ribeiro MCC, Torresi RM (2011) Effect of SO2 on the transport properties of an imidazolium ionic liquid and its lithium solution. J Phys Chem B 115(31):9662–9670

  39. Potgieter M, Parrondo J, Ramani VK, Kriek RJ (2016) Evaluation of polycrystalline platinum and rhodium surfaces for the electro-oxidation of aqueous sulfur dioxide. Electrocatalysis 7(1):50–59

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was financially supported by the National Key Technology Support Program (no. 2015BAG06B00) and the Major Program of the National Natural Science Foundation of China (no. 61433013).

Author information

Authors and Affiliations

  1. Fuel Cell System and Engineering Laboratory, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, People’s Republic of China

    Qing Zhao, Ming Hou, Shangfeng Jiang, Jun Ai, Limin Zheng & Zhigang Shao

  2. University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing, 100049, People’s Republic of China

    Qing Zhao & Shangfeng Jiang

Authors
  1. Qing Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ming Hou
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Shangfeng Jiang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Jun Ai
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Limin Zheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Zhigang Shao
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Qing Zhao or Ming Hou.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhao, Q., Hou, M., Jiang, S. et al. Enhanced sulfur dioxide electrooxidation performance on a modified XC-72 carbon catalyst. J Solid State Electrochem 21, 3113–3120 (2017). https://doi.org/10.1007/s10008-017-3633-0

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10008-017-3633-0

Keywords

Search

Navigation