A universal principle for a rational design of single-atom electrocatalysts

Haoxiang Xu, Daojian Cheng, Dapeng Cao, Xiao C Zeng

Research output: Contribution to journalArticle

78 Citations (Scopus)

Abstract

Developing highly active single-atom catalysts for electrochemical reactions is a key to future renewable energy technology. Here we present a universal design principle to evaluate the activity of graphene-based single-atom catalysts towards the oxygen reduction, oxygen evolution and hydrogen evolution reactions. Our results indicate that the catalytic activity of single-atom catalysts is highly correlated with the local environment of the metal centre, namely its coordination number and electronegativity and the electronegativity of the nearest neighbour atoms, validated by available experimental data. More importantly, we reveal that this design principle can be extended to metal-macrocycle complexes. The principle not only offers a strategy to design highly active nonprecious metal single-atom catalysts with specific active centres, for example, Fe-pyridine/pyrrole-N4 for the oxygen reduction reaction; Co-pyrrole-N4 for the oxygen evolution reaction; and Mn-pyrrole-N4 for the hydrogen evolution reaction to replace precious Pt/Ir/Ru-based catalysts, but also suggests that macrocyclic metal complexes could be used as an alternative to graphene-based single-atom catalysts.

Original languageEnglish (US)
Pages (from-to)339-348
Number of pages10
JournalNature Catalysis
Volume1
Issue number5
DOIs
StatePublished - May 1 2018

Fingerprint

Electrocatalysts
Pyrroles
Oxygen
Atoms
Catalysts
Graphite
Coordination Complexes
Hydrogen
Electronegativity
Metals
Renewable Energy
Metal complexes
Graphene
Technology
Pyridine
Catalyst activity

ASJC Scopus subject areas

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

Cite this

A universal principle for a rational design of single-atom electrocatalysts. / Xu, Haoxiang; Cheng, Daojian; Cao, Dapeng; Zeng, Xiao C.

In: Nature Catalysis, Vol. 1, No. 5, 01.05.2018, p. 339-348.

Research output: Contribution to journalArticle

Xu, Haoxiang ; Cheng, Daojian ; Cao, Dapeng ; Zeng, Xiao C. / A universal principle for a rational design of single-atom electrocatalysts. In: Nature Catalysis. 2018 ; Vol. 1, No. 5. pp. 339-348.
@article{e6fe5baeb6164423a542094b328376ce,
title = "A universal principle for a rational design of single-atom electrocatalysts",
abstract = "Developing highly active single-atom catalysts for electrochemical reactions is a key to future renewable energy technology. Here we present a universal design principle to evaluate the activity of graphene-based single-atom catalysts towards the oxygen reduction, oxygen evolution and hydrogen evolution reactions. Our results indicate that the catalytic activity of single-atom catalysts is highly correlated with the local environment of the metal centre, namely its coordination number and electronegativity and the electronegativity of the nearest neighbour atoms, validated by available experimental data. More importantly, we reveal that this design principle can be extended to metal-macrocycle complexes. The principle not only offers a strategy to design highly active nonprecious metal single-atom catalysts with specific active centres, for example, Fe-pyridine/pyrrole-N4 for the oxygen reduction reaction; Co-pyrrole-N4 for the oxygen evolution reaction; and Mn-pyrrole-N4 for the hydrogen evolution reaction to replace precious Pt/Ir/Ru-based catalysts, but also suggests that macrocyclic metal complexes could be used as an alternative to graphene-based single-atom catalysts.",
author = "Haoxiang Xu and Daojian Cheng and Dapeng Cao and Zeng, {Xiao C}",
year = "2018",
month = "5",
day = "1",
doi = "10.1038/s41929-018-0063-z",
language = "English (US)",
volume = "1",
pages = "339--348",
journal = "Nature Catalysis",
issn = "2520-1158",
publisher = "Nature Publishing Group",
number = "5",

}

TY - JOUR

T1 - A universal principle for a rational design of single-atom electrocatalysts

AU - Xu, Haoxiang

AU - Cheng, Daojian

AU - Cao, Dapeng

AU - Zeng, Xiao C

PY - 2018/5/1

Y1 - 2018/5/1

N2 - Developing highly active single-atom catalysts for electrochemical reactions is a key to future renewable energy technology. Here we present a universal design principle to evaluate the activity of graphene-based single-atom catalysts towards the oxygen reduction, oxygen evolution and hydrogen evolution reactions. Our results indicate that the catalytic activity of single-atom catalysts is highly correlated with the local environment of the metal centre, namely its coordination number and electronegativity and the electronegativity of the nearest neighbour atoms, validated by available experimental data. More importantly, we reveal that this design principle can be extended to metal-macrocycle complexes. The principle not only offers a strategy to design highly active nonprecious metal single-atom catalysts with specific active centres, for example, Fe-pyridine/pyrrole-N4 for the oxygen reduction reaction; Co-pyrrole-N4 for the oxygen evolution reaction; and Mn-pyrrole-N4 for the hydrogen evolution reaction to replace precious Pt/Ir/Ru-based catalysts, but also suggests that macrocyclic metal complexes could be used as an alternative to graphene-based single-atom catalysts.

AB - Developing highly active single-atom catalysts for electrochemical reactions is a key to future renewable energy technology. Here we present a universal design principle to evaluate the activity of graphene-based single-atom catalysts towards the oxygen reduction, oxygen evolution and hydrogen evolution reactions. Our results indicate that the catalytic activity of single-atom catalysts is highly correlated with the local environment of the metal centre, namely its coordination number and electronegativity and the electronegativity of the nearest neighbour atoms, validated by available experimental data. More importantly, we reveal that this design principle can be extended to metal-macrocycle complexes. The principle not only offers a strategy to design highly active nonprecious metal single-atom catalysts with specific active centres, for example, Fe-pyridine/pyrrole-N4 for the oxygen reduction reaction; Co-pyrrole-N4 for the oxygen evolution reaction; and Mn-pyrrole-N4 for the hydrogen evolution reaction to replace precious Pt/Ir/Ru-based catalysts, but also suggests that macrocyclic metal complexes could be used as an alternative to graphene-based single-atom catalysts.

UR - http://www.scopus.com/inward/record.url?scp=85048382098&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85048382098&partnerID=8YFLogxK

U2 - 10.1038/s41929-018-0063-z

DO - 10.1038/s41929-018-0063-z

M3 - Article

VL - 1

SP - 339

EP - 348

JO - Nature Catalysis

JF - Nature Catalysis

SN - 2520-1158

IS - 5

ER -