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Construction of Polarized Carbon-Nickel Catalytic Surfaces for Potent, Durable, and Economic Hydrogen Evolution Reactions

Journal Article


Abstract


  • Electrocatalytic hydrogen evolution reaction (HER) in alkaline solution is hindered by its sluggish kinetics toward water dissociation. Nickel-based catalysts, as low-cost and effective candidates, show great potentials to replace platinum (Pt)-based materials in the alkaline media. The main challenge regarding this type of catalysts is their relatively poor durability. In this work, we conceive and construct a charge-polarized carbon layer derived from carbon quantum dots (CQDs) on Ni 3 N nanostructure (Ni 3 N@CQDs) surfaces, which simultaneously exhibit durable and enhanced catalytic activity. The Ni 3 N@CQDs shows an overpotential of 69 mV at a current density of 10 mA cm -2 in a 1 M KOH aqueous solution, lower than that of Pt electrode (116 mV) at the same conditions. Density functional theory (DFT) simulations reveal that Ni 3 N and interfacial oxygen polarize charge distributions between originally equal C-C bonds in CQDs. The partially negatively charged C sites become effective catalytic centers for the key water dissociation step via the formation of new C-H bond (Volmer step) and thus boost the HER activity. Furthermore, the coated carbon is also found to protect interior Ni 3 N from oxidization/hydroxylation and therefore guarantees its durability. This work provides a practical design of robust and durable HER electrocatalysts based on nonprecious metals.

UOW Authors


  •   Zhou, Min (external author)
  •   Weng, Qunhong (external author)
  •   Popov, Zakhar (external author)
  •   Yang, Yijun (external author)
  •   Antipina, Liubov (external author)
  •   Sorokin, Pavel (external author)
  •   Wang, Xi (external author)
  •   Bando, Yoshio
  •   Golberg, Dmitri (external author)

Publication Date


  • 2018

Citation


  • Zhou, M., Weng, Q., Popov, Z., Yang, Y., Antipina, L., Sorokin, P., Wang, X., Bando, Y. & Golberg, D. (2018). Construction of Polarized Carbon-Nickel Catalytic Surfaces for Potent, Durable, and Economic Hydrogen Evolution Reactions. ACS Nano, 12 (5), 4148-4155.

Scopus Eid


  • 2-s2.0-85047393686

Number Of Pages


  • 7

Start Page


  • 4148

End Page


  • 4155

Volume


  • 12

Issue


  • 5

Place Of Publication


  • United States

Abstract


  • Electrocatalytic hydrogen evolution reaction (HER) in alkaline solution is hindered by its sluggish kinetics toward water dissociation. Nickel-based catalysts, as low-cost and effective candidates, show great potentials to replace platinum (Pt)-based materials in the alkaline media. The main challenge regarding this type of catalysts is their relatively poor durability. In this work, we conceive and construct a charge-polarized carbon layer derived from carbon quantum dots (CQDs) on Ni 3 N nanostructure (Ni 3 N@CQDs) surfaces, which simultaneously exhibit durable and enhanced catalytic activity. The Ni 3 N@CQDs shows an overpotential of 69 mV at a current density of 10 mA cm -2 in a 1 M KOH aqueous solution, lower than that of Pt electrode (116 mV) at the same conditions. Density functional theory (DFT) simulations reveal that Ni 3 N and interfacial oxygen polarize charge distributions between originally equal C-C bonds in CQDs. The partially negatively charged C sites become effective catalytic centers for the key water dissociation step via the formation of new C-H bond (Volmer step) and thus boost the HER activity. Furthermore, the coated carbon is also found to protect interior Ni 3 N from oxidization/hydroxylation and therefore guarantees its durability. This work provides a practical design of robust and durable HER electrocatalysts based on nonprecious metals.

UOW Authors


  •   Zhou, Min (external author)
  •   Weng, Qunhong (external author)
  •   Popov, Zakhar (external author)
  •   Yang, Yijun (external author)
  •   Antipina, Liubov (external author)
  •   Sorokin, Pavel (external author)
  •   Wang, Xi (external author)
  •   Bando, Yoshio
  •   Golberg, Dmitri (external author)

Publication Date


  • 2018

Citation


  • Zhou, M., Weng, Q., Popov, Z., Yang, Y., Antipina, L., Sorokin, P., Wang, X., Bando, Y. & Golberg, D. (2018). Construction of Polarized Carbon-Nickel Catalytic Surfaces for Potent, Durable, and Economic Hydrogen Evolution Reactions. ACS Nano, 12 (5), 4148-4155.

Scopus Eid


  • 2-s2.0-85047393686

Number Of Pages


  • 7

Start Page


  • 4148

End Page


  • 4155

Volume


  • 12

Issue


  • 5

Place Of Publication


  • United States