Interface charge density modulation of a lamellar-like spatially separated Ni9S8 nanosheet/Nb2O5 nanobelt heterostructure catalyst coupled with nitrogen and metal (M = Co, Fe, or Cu) atoms to accelerate acidic and alkaline hydrogen evolution reactions

Sundaram Chandrasekaran, Na Li, Yang Zhuang, Lijun Sui, Zhizhong Xiao, Dayong Fan, Vanchiappan Aravindan, Chris Bowen, Huidan Lu, Yongping Liu

Research output: Contribution to journalArticlepeer-review

7 Citations (SciVal)

Abstract

The creation of heterostructures based on non-precious metals with platinum-like hydrogen evolution reaction (HER) performance remains a challenge for hydrogen fuel technologies. Motivated by the fascinating properties of heterostructures, we establish here an effective approach to fabricate the heterostructured M−N−Ni9S8/Nb2O5 (M = Co, Fe, or Cu) catalysts using spatially separated Ni9S8 nanosheet/Nb2O5 nanobelts that are coupled with nitrogen (N) and metal atoms. Due to its improved intrinsic activity, interface-rich structure, abundant active sites, and large surface area the Co−N−Ni9S8/Nb2O5 heterostructure achieved a low acidic HER overpotential of −171 mV at −10 mA cm−2, thereby performing better than existing heterostructures. Moreover, for the alkaline HER, the Cu−N−Ni9S8/Nb2O5 heterostructure required a low overpotential of −109 mV at −10 mA cm−2, which is close to the performance of Pt/C catalyst. Density functional theory (DFT) predictions indicate that the local charge distribution and electronic properties at the heterointerface of Ni9S8/Nb2O5 can be significantly modulated by co-doping of metals with N atoms, resulting in optimal adsorption energy and reduced water dissociation barrier; thereby accelerating the acidic and alkaline HER activity. This work, therefore, provides a new design principle to create advanced heterostructured catalysts.

Original languageEnglish
Article number134073
JournalChemical Engineering Journal
Volume431
Early online date11 Dec 2021
DOIs
Publication statusPublished - 1 Mar 2022

Keywords

  • Density functional theory
  • Electrocatalyst
  • Hydrogen evolution reaction
  • Interface engineering
  • NbO nanobelts
  • NiS/NbO heterostructure

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Industrial and Manufacturing Engineering

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