A General Method for Transition Metal Single Atoms Anchored on Honeycomb-Like Nitrogen-Doped Carbon Nanosheets

Xiaoyan Zhang, Shan Zhang, Yong Yang, Liguang Wang, Zijie Mu, Haishuang Zhu, Xiaoqing Zhu, Huanhuan Xing, Hongyin Xia, Bolong Huang (Corresponding Author), Jing Li, Shaojun Guo, Erkang Wang

Research output: Journal article publicationJournal articleAcademic researchpeer-review

43 Citations (Scopus)

Abstract

Excavating and developing highly efficient and cost-effective nonnoble metal single-atom catalysts for electrocatalytic reactions is of paramount significance but still in its infancy. Herein, reported is a general NaCl template-assisted strategy for rationally designing and preparing a series of isolated transition metal single atoms (Fe/Co/Ni) anchored on honeycomb-like nitrogen-doped carbon matrix (M1-HNC-T1-T2, M = Fe/Co/Ni, T1 = 500 °C, T2 = 850 °C). The resulting M1-HNC-500-850 with M-N4 active sites exhibits superior capability for oxygen reduction reaction (ORR) with the half-wave potential order of Fe1-HNC-500-850 > Co1-HNC-500-850 > Ni1-HNC-500-850, in which Fe1-HNC-500-850 shows better performance than commercial Pt/C. Density functional theory calculations reveal a choice strategy that the strong p–d-coupled spatial charge separation results the Fe-N4 effectively merges active electrons for elevating d-band activity in a van-Hove singularity like character. This essentially generalizes an optimal electronic exchange-and-transfer (ExT) capability for boosting sluggish alkaline ORR activity. This work not only presents a universal strategy for preparing single-atom electrocatalyst to accelerate the kinetics of cathodic ORR but also provides an insight into the relationship between the electronic structure and the electrocatalytical activity.

Original languageEnglish
Article number1906905
JournalAdvanced Materials
Volume32
Issue number10
DOIs
Publication statusPublished - 1 Mar 2020

Keywords

  • NaCl template-assisted strategy
  • oxygen reduction reaction
  • p–d-coupled spatial charge separation
  • single-atom electrocatalysts

ASJC Scopus subject areas

  • Materials Science(all)
  • Mechanics of Materials
  • Mechanical Engineering

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