Issue

Vol. 9 No. 3 (2017)

Nitrogen-Doped Carbon Nanotube-Supported Pd Catalyst for Improved Electrocatalytic Performance toward Ethanol Electrooxidation

https://doi.org/10.1007/s40820-017-0129-5
Ying Wei
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China
Xinyuan Zhang
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China
Zhiyong Luo
College of Chemistry, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China
Dian Tang
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China
Changxin Chen
Department of Micro/Nano Electronics, School of Electronic Information and Electrical Engineering, Shanghai Jiao Tong University, Shanghai 200240, People’s Republic of China
Teng Zhang
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China
Zailai Xie
College of Chemistry, Fuzhou University, Fuzhou 350108, Fujian, People’s Republic of China

Corresponding Author: Zailai Xie

zlxie@fzu.edu.cn

Nano-Micro Letters, Vol. 9 No. 3 (2017), Article Number: 28

Abstract

In this study, hydrothermal carbonization (HTC) was applied for surface functionalization of carbon nanotubes (CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carbon layers on the surface of the CNTs. By controlling the ratio of glucose to urea, nitrogen contents of up to 1.7 wt% were achieved. The nitrogen-doped carbon nanotube-supported Pd catalysts exhibited superior electrochemical activity for ethanol oxidation relative to the pristine CNTs. Importantly, a 1.5-fold increase in the specific activity was observed for the Pd/HTC-N1.67%CNTs relative to the catalyst without nitrogen doping (Pd/HTC-CNTs). Further experiments indicated that the introduction of nitrogen species on the surface of the CNTs improved the Pd(0) loading and increased the binding energy.


Highlights:


1 Hydrothermal carbonization (HTC) enabled the deposition of an N-doped carbon layer on the surface of carbon nanotubes (CNTs).
2 Nitrogen-doped CNTs facilitated the uniform distribution of Pd nanoparticles.
3 The interaction between nitrogen in the CNTs and Pd favored the existence of metallic Pd in the catalysts.
4 Pd/HTC-N1.67%CNTs showed the highest specific activity toward ethanol oxidation.

Keywords

Direct alcohol fuel cells Hydrothermal carbonization Nitrogen-doped carbon nanotubes Pd-based catalyst Ethanol electrocatalyst
Wei, Ying, Xinyuan Zhang, Zhiyong Luo, Dian Tang, Changxin Chen, Teng Zhang, and Zailai Xie. 2017. “Nitrogen-Doped Carbon Nanotube-Supported Pd Catalyst for Improved Electrocatalytic Performance Toward Ethanol Electrooxidation”. Nano-Micro Letters 9 (3):28. https://doi.org/10.1007/s40820-017-0129-5.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. C. Lamy, A. Lima, V. LeRhun, F. Delime, C. Coutanceau, J.-M. Léger, Recent advances in the development of direct alcohol fuel cells (DAFC). J. Power Sources 105(2), 283–296 (2002). doi:10.1016/S0378-7753(01)00954-5
  2. Z. Zhang, C. Zhang, J. Sun, T. Kou, Q. Bai, Y. Wang, Y. Ding, Ultrafine nanoporous PdFe/Fe3O4 catalysts with doubly enhanced activities towards electro-oxidation of methanol and ethanol in alkaline media. J. Mater. Chem. 1(11), 3620–3628 (2013). doi:10.1039/c3ta01464a
  3. M.K. Debe, Electrocatalyst approaches and challenges for automotive fuel cells. Nature 486(7401), 43–51 (2012). doi:10.1038/nature11115
  4. L. Yu, J. Xi, CeO2 nanoparticles improved Pt-based catalysts for direct alcohol fuel cells. Int. J. Hydrogen Energy 37(21), 15938–15947 (2012). doi:10.1016/j.ijhydene.2012.08.063
  5. Y.H. Chu, Y.G. Shul, Combinatorial investigation of Pt–Ru–Sn alloys as an anode electrocatalysts for direct alcohol fuel cells. Int. J. Hydrogen Energy 35(20), 11261–11270 (2010). doi:10.1016/j.ijhydene.2010.07.062
  6. Y. Zhou, C. Liu, J. Liu, X. Cai, Y. Lu, H. Zhang, X. Sun, S. Wang, Self-decoration of PtNi alloy nanoparticles on multi-walled carbon nanotubes for highly efficient methanol electro-oxidation. Nano-Micro Lett. 8(4), 371–380 (2016). doi:10.1007/s40820-016-0096-2
  7. C.W. Xu, H. Wang, P.K. Shen, S.P. Jiang, Highly ordered pd nanowire arrays as effective electrocatalysts for ethanol oxidation in direct alcohol fuel cells. Adv. Mater. 19(23), 4256–4259 (2007). doi:10.1002/adma.200602911
  8. T. Maiyalagan, K. Scott, Performance of carbon nanofiber supported Pd–Ni catalysts for electro-oxidation of ethanol in alkaline medium. J. Power Sources 195(16), 5246–5251 (2010). doi:10.1016/j.jpowsour.2010.03.022
  9. F. Zhu, M. Wang, Y. He, G. Ma, Z. Zhang, X. Wang, A comparative study of elemental additives (Ni, Co and Ag) on electrocatalytic activity improvement of PdSn-based catalysts for ethanol and formic acid electro-oxidation. Electrochim. Acta 148, 291–301 (2014). doi:10.1016/j.electacta.2014.10.062
  10. X. Wang, F. Zhu, Y. He, M. Wang, Z. Zhang, Z. Ma, R. Li, Highly active carbon supported ternary PdSnPtx (x = 0.1–0.7) catalysts for ethanol electro-oxidation in alkaline and acid media. J. Colloid Interface Sci. 468, 200–210 (2016). doi:10.1016/j.jcis.2016.01.068
  11. X. Wang, G. Ma, F. Zhu, N. Lin, B. Tang, Z. Zhang, Preparation and characterization of micro-arc-induced Pd/TM(TM = Ni, Co and Ti) catalysts and comparison of their electrocatalytic activities toward ethanol oxidation. Electrochim. Acta 114, 500–508 (2013). doi:10.1016/j.electacta.2013.10.049
  12. B. Yoon, C.M. Wai, Microemulsion-templated synthesis of carbon nanotube-supported pd and rh nanoparticles for catalytic applications. J. Am. Chem. Soc. 127(49), 17174–17175 (2005). doi:10.1021/ja055530f
  13. O. Winjobi, Z. Zhang, C. Liang, W. Li, Carbon nanotube supported platinum–palladium nanoparticles for formic acid oxidation. Electrochim. Acta 55(13), 4217–4221 (2010). doi:10.1016/j.electacta.2010.02.062
  14. F. Hu, G. Cui, Z. Wei, P.K. Shen, Improved kinetics of ethanol oxidation on Pd catalysts supported on tungsten carbides/carbon nanotubes. Electrochem. Commun. 10(9), 1303–1306 (2008). doi:10.1016/j.elecom.2008.06.019
  15. M.M.O. Thotiyl, T.R. Kumar, S. Sampath, Pd supported on titanium nitride for efficient ethanol oxidation. J. Phys. Chem. C 114(41), 17934–17941 (2010). doi:10.1021/jp1038514
  16. R. Li, Z. Ma, F. Zhang, H. Meng, M. Wang, X.-Q. Bao, B. Tang, X. Wang, Facile Cu3P-C hybrid supported strategy to improve Pt nanoparticle electrocatalytic performance toward methanol, ethanol, glycol and formic acid electro-oxidation. Electrochim. Acta 220, 193–204 (2016). doi:10.1016/j.electacta.2016.10.105
  17. Y. Yan, J. Miao, Z. Yang, F.-X. Xiao, H.B. Yang, B. Liu, Y. Yang, Carbon nanotube catalysts: recent advances in synthesis, characterization and applications. Chem. Soc. Rev. 44(10), 3295–3346 (2015). doi:10.1039/c4cs00492b
  18. D.-W. Wang, D. Su, Heterogeneous nanocarbon materials for oxygen reduction reaction. Energy Environ. Sci. 7(2), 576–591 (2014). doi:10.1039/c3ee43463j
  19. W.Y. Wong, W.R.W. Daud, A.B. Mohamad, A.A.H. Kadhum, K.S. Loh, E.H. Majlan, Recent progress in nitrogen-doped carbon and its composites as electrocatalysts for fuel cell applications. Int. J. Hydrogen Energy 38(22), 9370–9386 (2013). doi:10.1016/j.ijhydene.2012.12.095
  20. R. Chetty, S. Kundu, W. Xia, M. Bron, W. Schuhmann, V. Chirila, W. Brandl, T. Reinecke, M. Muhler, PtRu nanoparticles supported on nitrogen-doped multiwalled carbon nanotubes as catalyst for methanol electrooxidation. Electrochim. Acta 54(17), 4208–4215 (2009). doi:10.1016/j.electacta.2009.02.073
  21. H. Jin, T. Xiong, Y. Li, X. Xu, M. Li, Y. Wang, Improved electrocatalytic activity for ethanol oxidation by Pd@N-doped carbon from biomass. Chem. Commun. 50(84), 12637–12640 (2014). doi:10.1039/c4cc06206j
  22. C.E. Chan-Thaw, A. Villa, G.M. Veith, L. Prati, Identifying the role of N-heteroatom location in the activity of metal catalysts for alcohol oxidation. ChemCatChem 7(8), 1338–1346 (2015). doi:10.1002/cctc.201402951
  23. J. Chang, X. Sun, L. Feng, W. Xing, X. Qin, G. Shao, Effect of nitrogen-doped acetylene carbon black supported Pd nanocatalyst on formic acid electrooxidation. J. Power Sources 239, 94–102 (2013). doi:10.1016/j.jpowsour.2013.03.066
  24. Y. Shao, J. Sui, G. Yin, Y. Gao, Nitrogen-doped carbon nanostructures and their composites as catalytic materials for proton exchange membrane fuel cell. Appl. Catal. B 79(1), 89–99 (2008). doi:10.1016/j.apcatb.2007.09.047
  25. E. Antolini, Nitrogen-doped carbons by sustainable N- and C-containing natural resources as nonprecious catalysts and catalyst supports for low temperature fuel cells. Renew. Sust. Energy Rev. 58, 34–51 (2016). doi:10.1016/j.rser.2015.12.330
  26. M. Sevilla, L. Yu, L. Zhao, C.O. Ania, M.-M. Titiricic, Surface modification of CNTs with N-Doped carbon: an effective way of enhancing their performance in supercapacitors. ACS Sustain. Chem. Eng. 2(4), 1049–1055 (2014). doi:10.1021/sc500069h
  27. Q.-L. Zhang, J.-N. Zheng, T.-Q. Xu, A.-J. Wang, J. Wei, J.-R. Chen, J.-J. Feng, Simple one-pot preparation of Pd-on-Cu nanocrystals supported on reduced graphene oxide for enhanced ethanol electrooxidation. Electrochim. Acta 132, 551–560 (2014). doi:10.1016/j.electacta.2014.03.159
  28. Z.X. Liang, T.S. Zhao, J.B. Xu, L.D. Zhu, Mechanism study of the ethanol oxidation reaction on palladium in alkaline media. Electrochim. Acta 54(8), 2203–2208 (2009). doi:10.1016/j.electacta.2008.10.034
  29. J.-N. Zheng, L.-L. He, F.-Y. Chen, A.-J. Wang, M.-W. Xue, J.-J. Feng, A facile general strategy for synthesis of palladium-based bimetallic alloyed nanodendrites with enhanced electrocatalytic performance for methanol and ethylene glycol oxidation. J. Mater. Chem. A 2(32), 12899–12906 (2014). doi:10.1039/C4TA01647E
  30. F. Zhu, G. Ma, Z. Bai, R. Hang, B. Tang, Z. Zhang, X. Wang, High activity of carbon nanotubes supported binary and ternary Pd-based catalysts for methanol, ethanol and formic acid electro-oxidation. J. Power Sources 242, 610–620 (2013). doi:10.1016/j.jpowsour.2013.05.145
  31. W. Li, Y. Huang, D. Tang, T. Zhang, Y. Wang, A new composite support for Pd catalysts for ethylene glycol electrooxidation in alkaline solution: effect of (Ru, Sn)O2 solid solution. Electrochim. Acta 174, 178–184 (2015). doi:10.1016/j.electacta.2015.05.166
  32. H. Chen, Y. Huang, D. Tang, T. Zhang, Y. Wang, Ethanol oxidation on Pd/C promoted with CaSiO3 in alkaline medium. Electrochim. Acta 158, 18–23 (2015). doi:10.1016/j.electacta.2015.01.103
  33. J. Zhao, M. Shao, D. Yan, S. Zhang, Z. Lu et al., A hierarchical heterostructure based on Pd nanoparticles/layered double hydroxide nanowalls for enhanced ethanol electrooxidation. J. Mater. Chem. A 1(19), 5840–5846 (2013). doi:10.1039/c3ta10588a
  34. P. Wu, Y. Huang, L. Kang, M. Wu, Y. Wang, Multisource synergistic electrocatalytic oxidation effect of strongly coupled PdM (M = Sn, Pb)/N-doped graphene nanocomposite on small organic molecules. Sci. Rep. 5, 14173 (2015). doi:10.1038/srep14173
  35. G. Yang, Y. Chen, Y. Zhou, Y. Tang, T. Lu, Preparation of carbon supported Pd–P catalyst with high content of element phosphorus and its electrocatalytic performance for formic acid oxidation. Electrochem. Commun. 12(3), 492–495 (2010). doi:10.1016/j.elecom.2010.01.029
  36. K.S. Kim, A.F. Gossmann, N. Winograd, X-ray photoelectron spectroscopic studies of palladium oxides and the palladium-oxygen electrode. Anal. Chem. 46(2), 197–200 (1974). doi:10.1021/ac60338a037
  37. R. Arrigo, M.E. Schuster, Z. Xie, Y. Yi, G. Wowsnick et al., Nature of the N-Pd interaction in nitrogen-doped carbon nanotube catalysts. ACS Catal. 5(5), 2740–2753 (2015). doi:10.1021/acscatal.5b00094
  38. L. Chen, X. Cui, Y. Wang, M. Wang, F. Cui et al., One-step hydrothermal synthesis of nitrogen-doped carbon nanotubes as an efficient electrocatalyst for oxygen reduction reactions. Chem. Asian J. 9(10), 2915–2920 (2014). doi:10.1002/asia.201402334
  39. X. Chen, G. Wu, J. Chen, X. Chen, Z. Xie, X. Wang, Synthesis of “clean” and well-dispersive pd nanoparticles with excellent electrocatalytic property on graphene oxide. J. Am. Chem. Soc. 133(11), 3693–3695 (2011). doi:10.1021/ja110313d
Read More
Author biographies are not available.
Download this PDF file
PDF
Statistic
Read Counter : 3343 Download : 2542