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On an easy way to prepare highly efficient Fe/N-co-doped carbon nanotube/nanoparticle composite for oxygen reduction reaction in Al–air batteries

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Abstract

Developing an efficient and low-cost oxygen reduction reaction (ORR) catalyst is the key to realize the commercialization of metal–air batteries. Fe/N-co-doped carbon materials (Fe–N–C) are regarded as one of the most promising oxygen reduction reaction (ORR) catalysts to replace expensive and unstable Pt/C in metal–air batteries. In this work, a new kind of Fe/N-co-doped special carbon nanotube/nanoparticle hybrid catalyst was obtained by using cheap precursors, i.e., ketjenblack EC-600JD (KB), melamine and iron nitrate via a facile high-temperature pyrolysis treatment. The catalyst shows a comparative oxygen reduction reaction (ORR) catalytic activity and better stability than commercial 20 wt% Pt/C in the same test conditions. The outstanding performance results from the doping of Fe and N, which could effectively increase the active sites. Furthermore, a special bamboo-like carbon nanotube is generated due to the catalysis of Fe source. The catalyst exhibits good performance in Al–air batteries. The maximum power density can reach to 300 mW cm−2 with the cell voltage of about 1 V and the current density of 300 mA cm−2.

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References

  1. Liu QC, Chang ZW, Li ZJ, Zhang XB (2018) Flexible metal–air batteries: progress, challenges, and perspectives. Small Methods 2:1700231

    Article  Google Scholar 

  2. Yuan S, Zhu YH, Li W, Wang S, Xu D, Li L, Zhang Y, Zhang XB (2017) Surfactant-free aqueous synthesis of pure single crystalline SnSe nanosheet clusters as anode for high energy- and power-density sodium-ion batteries. Adv Mater 29:1602469

    Article  Google Scholar 

  3. Wang S, Sun T, Yuan S, Zhu YH, Zhang XB, Yan JM, Jiang Q (2017) P3-type K0.33Co0.53Mn0.47O20.39H2O: a novel bifunctional electrode for Na-ion batteries. Mater Horiz 4:1122–1127

    Article  Google Scholar 

  4. Xu JJ, Chang ZW, Yin YB, Zhang XB (2017) Nanoengineered ultralight and robust all-metal cathode for high capacity, stable lithium-oxygen batteries. ACS Cent Sci 3:598–604

    Article  Google Scholar 

  5. Ma JL, Bao D, Shi MM, Yan JM, Zhang XB (2017) Reversible nitrogen fixation based on a rechargeable lithium-nitrogen battery for energy storage. Chem 2:525–532

    Article  Google Scholar 

  6. Cheng F, Chen J (2012) Metal–air batteries: from oxygen reduction electrochemistry to cathode catalysts. Chem Soc Rev 41:2172–2192

    Article  Google Scholar 

  7. Liu J, Sun X, Song P, Zhang Y, Xing W, Xu W (2013) High-performance oxygen reduction electrocatalysts based on cheap carbon black, nitrogen, and trace iron. Adv Mater 25:6879–6883

    Article  Google Scholar 

  8. Zhang G, Lou XW (2013) General solution growth of mesoporous NiCo2O4 nanosheets on various conductive substrates as high-performance electrodes for supercapacitors. Adv Mater 25:976–979

    Article  Google Scholar 

  9. Sa YJ, Seo DJ, Woo J, Lim JT, Cheon JY, Yang SY, Lee JM, Kang D, Shin TJ, Shin HS, Jeong HY, Kim CS, Kim MG, Kim TY, Joo SH (2016) A general approach to preferential formation of active Fe–Nx sites in Fe–N/C electrocatalysts for efficient oxygen reduction reaction. J Am Chem Soc 138:15046–15056

    Article  Google Scholar 

  10. Debe MK (2012) Electrocatalyst approaches and challenges for automotive fuel cells. Nature 486:43–51

    Article  Google Scholar 

  11. Wang ZL, Xu D, Xu JJ, Zhang XB (2014) Oxygen electrocatalysts in metal–air batteries: from aqueous to nonaqueous electrolytes. Chem Soc Rev 43:7746–7786

    Article  Google Scholar 

  12. Cao R, Lee J, Liu M, Cho J (2012) Non-precious catalysts: recent progress in non-precious catalysts for metal–air batteries. Adv Energy Mater 2:816–829

    Article  Google Scholar 

  13. Ding W, Li L, Xiong K, Wang Y, Li W, Nie Y, Chen S, Qi X, Wei Z (2015) Shape fixing via salt recrystallization: a morphology-controlled approach to convert nanostructured polymer to carbon nanomaterial as a highly active catalyst for oxygen reduction reaction. J Am Chem Soc 137:5414–5420

    Article  Google Scholar 

  14. Jiang WJ, Gu L, Li L, Zhang Y, Zhang X, Zhang LJ, Wang JQ, Hu JS, Wei Z, Wan LJ (2016) Understanding the high activity of Fe–N–C electrocatalysts in oxygen reduction: Fe/Fe3C nanoparticles boost the activity of Fe–Nx. J Am Chem Soc 138:3570–3578

    Article  Google Scholar 

  15. Steele BCH, Heinzel A (2001) Materials for fuel-cell technologies. Nature 414:345–352

    Article  Google Scholar 

  16. Wang Z, Cao X, Ping J, Wang Y, Lin T, Huang X, Ma Q, Wang F, He C, Zhang H (2015) Electrochemical doping of three-dimensional graphene networks used as efficient electrocatalysts for oxygen reduction reaction. Nanoscale 7:9394–9398

    Article  Google Scholar 

  17. Wu G, Zelenay P (2013) Nanostructured nonprecious metal catalysts for oxygen reduction reaction. Acc Chem Res 46:1878–1889

    Article  Google Scholar 

  18. Wang MQ, Yang WH, Wang HH, Chen C, Zhou ZY, Sun SG (2014) Pyrolyzed Fe–N–C composite as an efficient non-precious metal catalyst for oxygen reduction reaction in acidic medium. ACS Catal 4:3928–3936

    Article  Google Scholar 

  19. Jiang Y, Lu Y, Lv X, Han D, Zhang Q, Niu L, Chen W (2013) Enhanced catalytic performance of Pt-free iron phthalocyanine by graphene support for efficient oxygen reduction reaction. ACS Catal 3:1263–1271

    Article  Google Scholar 

  20. Niu W, Li L, Liu X, Wang N, Liu J, Zhou W, Tang Z, Chen S (2015) Mesoporous N-doped carbons prepared with thermally removable nanoparticle templates: an efficient electrocatalyst for oxygen reduction reaction. J Am Chem Soc 137:5555–5562

    Article  Google Scholar 

  21. Wang Q, Zhou ZY, Lai YJ, You Y, Liu JG, Wu XL, Terefe E, Chen C, Song L, Rauf M, Tian N, Sun SG (2014) Phenylenediamine-based FeNx/C catalyst with high activity for oxygen reduction in acid medium and its active-site probing. J Am Chem Soc 136:10882–10885

    Article  Google Scholar 

  22. Lin L, Zhu Q, Xu AW (2014) Noble-metal-free Fe–N/C catalyst for highly efficient oxygen reduction reaction under both alkaline and acidic conditions. J Am Chem Soc 136:11027–11033

    Article  Google Scholar 

  23. Maldonado S, Stevenson KJ (2005) Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes. J Phys Chem B 109:4707–4716

    Article  Google Scholar 

  24. Li W, Wu J, Higgins DC, Choi JY, Chen Z (2015) Determination of iron active sites in pyrolyzed iron-based catalysts for the oxygen reduction reaction. ACS Catal 2:2761–2768

    Article  Google Scholar 

  25. Chung HT, Won JH, Zelenay P (2013) Active and stable carbon nanotube/nanoparticle composite electrocatalyst for oxygen reduction. Nat Commun 4:1922–1926

    Article  Google Scholar 

  26. Li Q, Pan H, Higgins D, Cao R, Zhang G, Lv H, Wu K, Cho J, Wu G (2015) Metal-organic framework-derived bamboo-like nitrogen-doped graphene tubes as an active matrix for hybrid oxygen-reduction electrocatalysts. Small 11:1443–1452

    Article  Google Scholar 

  27. Wen Z, Ci S, Zhang F, Feng X, Cui S, Mao S, Luo S, He Z, Chen J (2012) Nitrogen-enriched core-shell structured Fe/Fe(3)C-C nanorods as advanced electrocatalysts for oxygen reduction reaction. Adv Mater 24:1399–1404

    Article  Google Scholar 

  28. Qu D (2007) Investigation of oxygen reduction on activated carbon electrodes in alkaline solution. Carbon 45:1296–1301

    Article  Google Scholar 

  29. Wong WY, Daud WRW, Mohamad AB, Kadhum AAH, Loh KS, Majlan EH (2013) Influence of nitrogen doping on carbon nanotubes towards the structure, composition and oxygen reduction reaction. Int J Hydrogen Energy 38:9421–9430

    Article  Google Scholar 

  30. Yang Z, Nie H, Chen X, Chen X, Huang S (2013) Recent progress in doped carbon nanomaterials as effective cathode catalysts for fuel cell oxygen reduction reaction. J Power Sources 236:238–249

    Article  Google Scholar 

  31. Liang J, Zhou RF, Chen XM, Tang YH, Qiao SZ (2014) Fe–N decorated hybrids of CNTs grown on hierarchically porous carbon for high-performance oxygen reduction. Adv Mater 26:6074–6079

    Article  Google Scholar 

  32. Liu S, Zhang H, Zhao Q, Zhang X, Liu R, Ge X, Wang G, Zhao H, Cai W (2016) Metal-organic framework derived nitrogen-doped porous carbon@graphene sandwich-like structured composites as bifunctional electrocatalysts for oxygen reduction and evolution reactions. Carbon 106:74–83

    Article  Google Scholar 

  33. Liu C, Wang J, Li J, Luo R, Sun X, Shen J, Han W, Wang L (2017) Fe/N decorated mulberry-like hollow mesoporous carbon fibers as efficient electrocatalysts for oxygen reduction reaction. Carbon 114:706–716

    Article  Google Scholar 

  34. Qian Y, Du P, Wu P, Cai C, Gervasio DF (2016) Chemical nature of catalytic active sites for the oxygen reduction reaction on nitrogen-doped carbon-supported non-noble metal catalysts. J Phys Chem C 120:9884–9896

    Article  Google Scholar 

  35. Li F, Fu L, Li J, Feng Q, Wang HY, Tang YG (2017) Fe7C3–Fe3N/FeNxCy decorated carbon materials as highly efficient catalyst for oxygen reduction reaction in Al–air batteries. Nanosci Nanotechnol Lett 9:1909–1918

    Article  Google Scholar 

  36. Li J, Zhou N, Song J, Fu L, Yan J, Tang YG, Wang HY (2018) Cu-MOF-derived Cu/Cu2O nanoparticles and CuNxCy species to boost oxygen reduction activity of ketjenblack carbon in Al–air battery. ACS Sustain Chem Eng 6:413–421

    Article  Google Scholar 

  37. Li F, Fu L, Li J, Yan J, Tang YG, Pan Y, Wang HY (2017) Ag/Fe3O4-N-doped ketjenblack carbon composite as highly efficient oxygen reduction catalyst in Al–air batteries. J Electrochem Soc 164:3595–3601

    Article  Google Scholar 

  38. Liu K, Zhou Z, Wang HY, Huang X, Xu J, Tang YG, Li J, Chu H, Chen J (2016) N-doped carbon supported Co3O4 nanoparticles as an advanced electrocatalyst for oxygen reduction reaction in Al–air battery. RSC Adv 6:55552–55559

    Article  Google Scholar 

  39. Li J, Chen J, Wang HY, Ren Y, Liu K, Tang YG, Shao M (2017) Fe/N co-doped carbon materials with controllable structure as highly efficient electrocatalysts for oxygen reduction reaction in Al–air batteries. Energy Storage Mater 8:49–58

    Article  Google Scholar 

  40. Liu R, Wu D, Feng X, Mllen K (2010) Nitrogen-doped ordered mesoporous graphitic arrays with high electrocatalytic activity for oxygen reduction. Angew Chem 122:2619–2623

    Article  Google Scholar 

  41. Song P, Zhang Y, Pan J, Zhuang L, Xu W (2015) Cheap carbon black-based high-performance electrocatalysts for pxygen reduction reaction. Chem Commun 51:1972–1975

    Article  Google Scholar 

  42. Yang W, Fellinger TP, Antonietti M (2011) Efficient metal-free oxygen reduction in alkaline medium on high-surface-area mesoporous nitrogen-doped carbons made from ionic liquids and nucleobases. J Am Chem Soc 133:206–209

    Article  Google Scholar 

  43. Liu S, Dong Y, Wang Z, Huang H, Zhao Z, Qiu J (2015) Towards efficient electrocatalysts for oxygen reduction by doping cobalt into graphene-supported graphitic carbon nitride. J Mater Chem A 3:19657–19661

    Article  Google Scholar 

  44. Huang X, Yang Z, Dong B, Wang Y, Tang T, Hou Y (2017) In situ Fe2N@N-doped porous carbon hybrids as superior catalysts for oxygen reduction reaction. Nanoscale 9:8102–8106

    Article  Google Scholar 

  45. Osmieri L, Ricardo EC, Videlaa AHAM, Ocónb P, Specchiaa S (2017) Performance of a Fe–N–C catalyst for the oxygen reduction reaction in direct methanol fuel cell: cathode formulation optimization and short-term durability. Appl Catal B 201:253–265

    Article  Google Scholar 

  46. Yang M, Chen H, Yang D, Gao Y, Li H (2016) Using nitrogen-rich polymeric network and iron(II) acetate as precursors to synthesize highly efficient electrocatalyst for oxygen reduction reaction in alkaline media. J Power Sources 307:152–159

    Article  Google Scholar 

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Acknowledgements

This research was financially supported by the National Nature Science Foundation of China (Nos. 21571189, 21671200 and 21771062), the Hunan Provincial Science and Technology Plan Project (Nos. 2016TP1007 and 2017TP1001), the Opening Project of Material Corrosion and Protection Key Laboratory of Sichuan Province of China (Nos. 2016CL04 and 2017CL17), the Innovation-Driven Project of Central South University (No. 2016CXS009) and the Talents Project of Si Chuan University of Science and Engineering (No. 2014RC30).

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Authors and Affiliations

  1. Hunan Provincial Key Laboratory of Chemical Power Sources, Hunan Provincial Key Laboratory of Efficient and Clean Utilization of Manganese Resources, College of Chemistry and Chemical Engineering, Central South University, Lushan South Road 932, Changsha, 410083, Hunan Province, People’s Republic of China

    Liping Wang, Liang Fu, Jingsha Li, Haiyan Wang & Yougen Tang

  2. College of Chemistry and Chemical Engineering, Yangtze Normal University, Fuling, 408100, People’s Republic of China

    Liang Fu & Hualin Xie

  3. Material Corrosion and Protection Key Laboratory of Sichuan Province, Zigong, 643000, People’s Republic of China

    Xianguang Zeng

  4. College of Science, Hunan Agricultural University, Changsha, 410128, People’s Republic of China

    Xiaobing Huang

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  1. Liping Wang
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Correspondence to Haiyan Wang or Yougen Tang.

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Wang, L., Fu, L., Li, J. et al. On an easy way to prepare highly efficient Fe/N-co-doped carbon nanotube/nanoparticle composite for oxygen reduction reaction in Al–air batteries. J Mater Sci 53, 10280–10291 (2018). https://doi.org/10.1007/s10853-018-2245-0

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