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Palladium-ytterbium bimetallic electrocatalysts supported on carbon black, titanium suboxide, or poly(diallyldimethylammonium chloride)-functionalized titanium suboxide towards methanol oxidation in alkaline media

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Abstract

Palladium-ytterbium (Pd-Yb) bimetallic catalysts with different Pd/Yb ratios supported on carbon black (20%Pd-x%Yb/C, x = 0, 1, 5, 10, and 15) were prepared by a sodium borohydride reduction method. The 20%Pd-5%Yb/C catalyst exhibited the best electrocatalytic activity towards methanol oxidation in alkaline media. The improved electrocatalytic activity and stability of 20%Pd-5%Yb/C can be explained by a bi-functional mechanism. In addition, the higher content of metallic palladium caused by the addition of ytterbium also contributes to the better catalytic activity of the 20%Pd+5%Yb/C catalyst. In view of the good electrocatalytic performance of 20%Pd+5%Yb/C, the 20%Pd+5%Yb catalyst supported on titanium suboxide (20%Pd+5%Yb/Ti4O7) was prepared. However, the Pd-Yb particles supported on Ti4O7 were seriously agglomerated. To improve the dispersion status of alloy particles, the Ti4O7 was functionalized with poly(diallyldimethylammonium chloride) (Ti4O7-PDDA). Electrochemical characterizations showed that no matter Ti4O7 or Ti4O7-PDDA as supports, Pd-Yb catalysts exhibited better catalytic activity than 20%Pd-5%Yb/C. The improvement mainly results from the further increase of metallic Pd due to the presence of Ti4O7.

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References

  1. Li J, Zhu Q-L, Xu Q (2015) Pd nanoparticles supported on hierarchically porous carbons derived from assembled nanoparticles of a zeolitic imidazolate framework (ZIF-8) for methanol electrooxidation. Chem Commun 51:10827–10830

    Article  CAS  Google Scholar 

  2. Lee Y-W, Ko AR, Han S-B, Kim H-S, Kim D-Y, Kim S-J, Park K-W (2010) Cuboctahedral Pd nanoparticles on WC for enhanced methanol electrooxidation in alkaline solution. Chem Commun 46:9241–9243

    Article  CAS  Google Scholar 

  3. Moon J-S, Lee Y-W, Han S-B, Park K-W (2014) Pd nanoparticles on mesoporous tungsten carbide as a non-Pt electrocatalyst for methanol electrooxidation reaction in alkaline solution. Int J Hydrog Energy 39:7798–7804

    Article  CAS  Google Scholar 

  4. Wang H, Xu C, Cheng F, Zhang M, Wang S, Jiang SP (2008) Pd/Pt core–shell nanowire arrays as highly effective electrocatalysts for methanol electrooxidation in direct methanol fuel cells. Electrochem Commun 10:1575–1578

    Article  CAS  Google Scholar 

  5. Alcaide F, Alvarez G, Cabot PL, Grande H-J, Miguel O, Querejeta A (2011) Testing of carbon supported Pd–Pt electrocatalysts for methanol electrooxidation in direct methanol fuel cells. Int J Hydrog Energy 36:4432–4439

    Article  CAS  Google Scholar 

  6. Lee Y-W, Han S-B, Park K-W (2009) Electrochemical properties of Pd nanostructures in alkaline solution. Electrochem Commun 11:1968–1971

    Article  CAS  Google Scholar 

  7. Tang W, Gan L, Wu B, Mao L, Yin D (2015) Carboxymethyl chitosan-assisted uniformly anchored Pd nanoparticles on carbon nanotubes for methanol electrooxidation in alkaline media. Micro Nano Lett 10:119–121

    Article  CAS  Google Scholar 

  8. Wang M, Liu W, Huang C (2009) Investigation of PdNiO/C catalyst for methanol electrooxidation. Int J Hydrog Energy 34:2758–2764

    Article  CAS  Google Scholar 

  9. Zhou L-N, Zhang X-T, Wang Z-H, Guo S, Li Y-J (2016) Cubic superstructures composed of PtPd alloy nanocubes and their enhanced electrocatalysis for methanol oxidation. Chem Commun 52:12737–12740

    Article  CAS  Google Scholar 

  10. Chu Y-Y, Wang Z-B, Jiang Z-Z, Gu D-M, Yin G-P (2012) Facile synthesis of hollow spherical sandwich PtPd/C catalyst by electrostatic self-assembly in polyol solution for methanol electrooxidation. J Power Sources 203:17–25

    Article  CAS  Google Scholar 

  11. Li S-S, Lv J-J, Hu Y-Y, Zheng J-N, Chen J-R, Wang A-J, Feng J-J (2014) Facile synthesis of porous Pt–Pd nanospheres supported on reduced graphene oxide nanosheets for enhanced methanol electrooxidation. J Power Sources 247:213–218

    Article  CAS  Google Scholar 

  12. Zhu C, Wen D, Oschatz M, Holzschuh M, Liu W, Herrmann A-K, Simon F, Kaskel S, Eychmueller A (2015) Kinetically controlled synthesis of PdNi bimetallic porous nanostructures with enhanced electrocatalytic activity. Small 11:1430–1434

    Article  CAS  Google Scholar 

  13. Miao F, Tao B, Chu PK (2012) Preparation and electrochemistry of Pd–Ni/Si nanowire nanocomposite catalytic anode for direct ethanol fuel cell. Dalton Trans 41:5055–5059

    Article  CAS  Google Scholar 

  14. Liu Z, Zhang X, Hong L (2009) Physical and electrochemical characterizations of nanostructured Pd/C and PdNi/C catalysts for methanol oxidation. Electrochem Commun 11:925–928

    Article  CAS  Google Scholar 

  15. Li R, Mao H, Zhang J, Huang T, Yu A (2013) Rapid synthesis of porous Pd and PdNi catalysts using hydrogen bubble dynamic template and their enhanced catalytic performance for methanol electrooxidation. J Power Sources 241:660–667

    Article  CAS  Google Scholar 

  16. Xu H, Yan B, Zhang K, Wang J, Li S, Wang C, Shiraishi Y, Du Y, Yang P (2017) Facile fabrication of novel PdRu nanoflowers as highly active catalysts for the electrooxidation of methanol. J Colloid Interface Sci 505:1–8

    Article  CAS  Google Scholar 

  17. Awasthi R, Singh RN (2013) Graphene-supported Pd–Ru nanoparticles with superior methanol electrooxidation activity. Carbon 51:282–289

    Article  CAS  Google Scholar 

  18. Awasthi R, Singh RN (2012) Optimization of the Pd–Sn–GNS nanocomposite for enhanced electrooxidation of methanol. Int J Hydrog Energy 37:2103–2110

    Article  CAS  Google Scholar 

  19. Li H-H, Zhao S, Gong M, Cui C-H, He D, Liang H-W, Wu L, Yu S-H (2013) Ultrathin PtPdTe nanowires as superior catalysts for methanol electrooxidation. Angew Chem Int Ed 52:7472–7476

    Article  CAS  Google Scholar 

  20. Yang Y, Wang L, Li A, Jia Z, Wang Y, Qi T (2015) Novel palladium–yttrium (Pd–Y/C) catalysts for methanol electrooxidation in alkaline media. J Solid State Electrochem 19:923–927

    Article  CAS  Google Scholar 

  21. Wang L, Wang Y, Li A, Yang Y, Tang Q, Cao H, Qi T, Li C (2014) Electrocatalysis of carbon black- or poly(diallyldimethylammonium chloride)-functionalized activated carbon nanotubes-supported Pd–Tb towards methanol oxidation in alkaline media. J Power Sources 257:138–146

    Article  CAS  Google Scholar 

  22. Nassr ABAA, Quetschke A, Koslowski E, Bron M (2013) Electrocatalytic oxidation of formic acid on Pd/MWCNTs nanocatalysts prepared by the polyol method. Electrochim Acta 102:202–211

    Article  CAS  Google Scholar 

  23. Zhao H, Tang Q, Wang Y, Qi T, Wang X (2014) Pd nanoparticles supported on PDDA-functionalized Ti4O7 as an effective catalyst for formic acid electrooxidation. ECS Solid State Lett 3:M37–M40

    Article  CAS  Google Scholar 

  24. Zhao H, Wang Y, Tang Q, Wang L, Zhang H, Quan C, Qi T (2014) Pt catalyst supported on titanium suboxide for formic acid electrooxidation reaction. Int J Hydrog Energy 39:9621–9627

    Article  CAS  Google Scholar 

  25. Senevirathne K, Hui R, Campbell S, Ye S, Zhang J (2012) Electrocatalytic activity and durability of Pt/NbO2 and Pt/Ti4O7 nanofibers for PEM fuel cell oxygen reduction reaction. Electrochim Acta 59:538–547

  26. Li L-L, Liu K-P, Yang G-H, Wang C-M, Zhang J-R, Zhu J-J (2011) Fabrication of graphene-quantum dots composites for sensitive electrogenerated chemiluminescence immunosensing. Adv Funct Mater 21:869–878

    Article  CAS  Google Scholar 

  27. Wang Y, Liu H, Wang L, Wang H, Du X, Wang F, Qi T, Lee J-M, Wang X (2013) Pd catalyst supported on a chitosan-functionalized large-area 3D reduced graphene oxide for formic acid electrooxidation reaction. J Mater Chem 1:6839–6848

    Article  CAS  Google Scholar 

  28. Wang Y, Wang X, Li CM (2010) Electrocatalysis of Pd–Co supported on carbon black or ball-milled carbon nanotubes towards methanol oxidation in alkaline media. Appl Catal, B 99:229–234

    Article  CAS  Google Scholar 

  29. Huang J, Liu Z, He C, Gan LM (2005) Synthesis of PtRu nanoparticles from the hydrosilylation reaction and application as catalyst for direct methanol fuel cell. J Phys Chem B 109:16644–16649

    Article  CAS  Google Scholar 

  30. Xu M-W, Gao G-Y, Zhou W-J, Zhang K-F, Li H-L (2008) Novel Pd/β-MnO2 nanotubes composites as catalysts for methanol oxidation in alkaline solution. J Power Sources 175:217–220

    Article  CAS  Google Scholar 

  31. Liu J, Ye J, Xu C, Jiang SP, Tong Y (2008) Electro-oxidation of methanol, 1-propanol and 2-propanol on Pt and Pd in alkaline medium. J Power Sources 177:67–70

    Article  CAS  Google Scholar 

  32. Mancharan R, Goodenough JB (1992) Methanol oxidation in acid on ordered NiTi. J Mater Chem 2:875–887

    Article  Google Scholar 

  33. Cohen JL, Volpe DJ, Abruna HD (2007) Electrochemical determination of activation energies for methanol oxidation on polycrystalline platinum in acidic and alkaline electrolytes. Phys Chem Chem Phys 9:49–77

    Article  CAS  Google Scholar 

  34. Vigier F, Coutanceau C, Hahn F, Belgsir EM, Lamy C (2004) On the mechanism of ethanol electro-oxidation on Pt and PtSn catalysts: electrochemical and in situ IR reflectance spectroscopy studies. J Electroanal Chem 563:81–89

    Article  CAS  Google Scholar 

  35. Cui Z, Li CM, Jiang SP (2011) PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells. Phys Chem Chem Phys 13:16349–16357

    Article  CAS  Google Scholar 

  36. Qu W-L, Wang Z-B, Jiang Z-Z, Gu D-M, Yin G-P (2012) Investigation on performance of Pd/Al2O3–C catalyst synthesized by microwave assisted polyol process for electrooxidation of formic acid. RSC Adv 2:344–350

    Article  CAS  Google Scholar 

  37. He N, Qin C, Wang R, Ma S, Wang Y, Qi T (2016) Electro-catalysis of carbon black or titanium sub-oxide supported Pd–Gd towards formic acid electro-oxidation. RSC Adv 6:68989–68996

    Article  CAS  Google Scholar 

  38. Leonov I, Yaresko AN, Antonov VN, Schwingenschlögl U, Eyert V, Anisimov VI (2006) Charge order and spin-singlet pair formation in Ti4O7. J Phys Condens Matter 18:10955–10964

    CAS  Google Scholar 

Download references

Funding

The authors are grateful for the financial support by the Key Research Program of Frontier Sciences of Chinese Academy of Sciences (Grant No. QYZDJ-SSW-JSC021), the Chinese National Programs for High Technology Research and Development (2014AA06A513), as well as by the 973 Program (Grant No. 2015CB251303).

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Correspondence to Yi Wang or Jiehua Liu.

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Gong, Y., He, Y., Li, A. et al. Palladium-ytterbium bimetallic electrocatalysts supported on carbon black, titanium suboxide, or poly(diallyldimethylammonium chloride)-functionalized titanium suboxide towards methanol oxidation in alkaline media. Ionics 24, 3085–3094 (2018). https://doi.org/10.1007/s11581-018-2506-6

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  • DOI: https://doi.org/10.1007/s11581-018-2506-6

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