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
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Journal ArticleDOI
Nanocasting SiO 2 into metal–organic frameworks imparts dual protection to high-loading Fe single-atom electrocatalysts
Long Jiao,Rui Zhang,Gang Wan,Weijie Yang,Xin Wan,Hua Zhou,Jianglan Shui,Shu-Hong Yu,Hai-Long Jiang +8 more
TL;DR: A dual protection strategy has been developed by nanocasting SiO2 into metal–organic frameworks to prepare high-loading SACs with excellent catalytic performance toward oxygen reduction and a general synthetic methodology toward high-content Sacs (such as FeSA, CoSA, NiSA).
Journal ArticleDOI
Single-atom cobalt electrocatalysts for foldable solid-state Zn-air battery
TL;DR: In this article, a single-atom cobalt electrocatalyst with CoN4 moieties dispersed on nitrogen-doped graphitic nanosheet (CoN4/NG) by a surfactant-assisted approach is presented.
Journal ArticleDOI
Theory-guided design of catalytic materials using scaling relationships and reactivity descriptors
Zhi-Jian Zhao,Sihang Liu,Shenjun Zha,Dongfang Cheng,Felix Studt,Graeme Henkelman,Jinlong Gong +6 more
TL;DR: This Review describes scaling relationships and reactivity descriptors for heterogeneous catalysis, including electronic descriptors represented by d-band theory, structural descriptors, which can be directly applied to catalyst design, and, ultimately, universal descriptors.
Journal ArticleDOI
Carbon-Supported Divacancy-Anchored Platinum Single-Atom Electrocatalysts with Superhigh Pt Utilization for the Oxygen Reduction Reaction.
Jing Liu,Menggai Jiao,Bingbao Mei,Yuxin Tong,Yuping Li,Mingbo Ruan,Ping Song,Gongquan Sun,Luhua Jiang,Luhua Jiang,Ying Wang,Zheng Jiang,Lin Gu,Zhen Zhou,Weilin Xu +14 more
TL;DR: Physical characterization and density functional theory computations reveal that single Pt atoms anchored stably by four carbon atoms in carbon divacancies (Pt-C4 ) are the main active centers for the observed high ORR performance.
Journal ArticleDOI
Strategies to Break the Scaling Relation toward Enhanced Oxygen Electrocatalysis
TL;DR: In this paper, the authors provide guidelines for the rational design of efficient catalysts for oxygen electrocatalysis beyond the limitation posed by scaling relations, including reaction of the mechanism and origin of the adsorption-energy scaling relationship.
References
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Georg Kresse,Daniel P. Joubert +1 more
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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
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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.