Journal ArticleDOI
A universal principle for a rational design of single-atom electrocatalysts
Haoxiang Xu,Daojian Cheng,Dapeng Cao,Xiao Cheng Zeng,Xiao Cheng Zeng +4 more
- Vol. 1, Iss: 5, pp 339-348
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TLDR
In this article, a universal design principle was proposed to evaluate the catalytic activity of single-atom catalysts for electrochemical reactions, which is a key to future renewable energy technology.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.read more
Citations
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Journal ArticleDOI
B-Doped MnN4-G Nanosheets as Bifunctional Electrocatalysts for Both Oxygen Reduction and Oxygen Evolution Reactions
Abstract: Non-platinum-group (NPG) single-metal-atom electrocatalysts with bifunctional catalytic capabilities for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are highly sought f...
Journal ArticleDOI
Non-precious metal cathodes for anion exchange membrane fuel cells from ball-milled iron and nitrogen doped carbide-derived carbons
Sander Ratso,Andrea Zitolo,Maike Käärik,Maido Merisalu,Arvo Kikas,Vambola Kisand,Mihkel Rähn,Päärn Paiste,Jaan Leis,Väino Sammelselg,Steven Holdcroft,Frédéric Jaouen,Kaido Tammeveski +12 more
TL;DR: In this paper, the authors show a synthesis method to produce highly active non-precious metal catalysts and study the effect of synthesis parameters on the oxygen reduction reaction (ORR) activity in high pH conditions.
Journal ArticleDOI
Catalyst: Single-Atom Catalysis: Directing the Way toward the Nature of Catalysis
TL;DR: Xuning Li et al. as discussed by the authors used in situ/operando characterization techniques in single-atom catalysis, focusing on in situ and operando characterization of single atom catalytic decomposition.
Journal ArticleDOI
Effect of Zn atom in Fe-N-C catalysts for electro-catalytic reactions: theoretical considerations
TL;DR: In this article, the effect of Zn atoms on the electrocatalytic performance of Fe-N-C catalysts was investigated by using density functional theory method, which showed that all the calculated Fe-Zn-Nx structures are thermodynamically stable due to the negative formation energies and relative stabilities.
Journal ArticleDOI
Catalytic Activity Origin and Design Principles of Graphitic Carbon Nitride Electrocatalysts for Hydrogen Evolution
TL;DR: In this article, a descriptor and design principle to accurately predict the HER electrocatalytic activities of heteroatom-doped graphitic carbon nitrogen (g-C3N4) was developed.
References
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Journal ArticleDOI
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Journal ArticleDOI
From ultrasoft pseudopotentials to the projector augmented-wave method
Georg Kresse,Daniel P. Joubert +1 more
TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Journal ArticleDOI
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
Georg Kresse,Jürgen Furthmüller +1 more
TL;DR: A detailed description and comparison of algorithms for performing ab-initio quantum-mechanical calculations using pseudopotentials and a plane-wave basis set is presented in this article. But this is not a comparison of our algorithm with the one presented in this paper.
Journal ArticleDOI
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
Sergei L. Dudarev,Gianluigi A. Botton,Sergey Y. Savrasov,Colin J. Humphreys,Adrian P. Sutton +4 more
TL;DR: In this article, the authors improved the description of both electron energy loss spectra and parameters characterizing the structural stability of the material compared with local spin density functional theory by taking better account of electron correlations in the $3d$ shell of metal ions in nickel oxide.