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

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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

Bibliographical note

Funding Information:
This work was financially supported by the National Natural Science Foundation of China (Nos. 22062005 , 22165005 and U20A20128 ), Guangxi Science Fund for Distinguished Young Scholars (No. 2019GXNSFFA245016 ), and Scientific Research Start-Up Project Program of Guilin University of Technology (No. RD2000002183 ), Guilin, PR China.

Funding

This work was financially supported by the National Natural Science Foundation of China (Nos. 22062005 , 22165005 and U20A20128 ), Guangxi Science Fund for Distinguished Young Scholars (No. 2019GXNSFFA245016 ), and Scientific Research Start-Up Project Program of Guilin University of Technology (No. RD2000002183 ), Guilin, PR China.

Keywords

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

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry
  • General Chemical Engineering
  • Industrial and Manufacturing Engineering

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