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
Single atom electrocatalysts supported on graphene or graphene-like carbons
Huilong Fei,Juncai Dong,Dongliang Chen,Tiandou Hu,Xidong Duan,Imran Shakir,Imran Shakir,Yu Huang,Xiangfeng Duan +8 more
TL;DR: G-SACs that integrate the merits of heterogeneous catalysts and homogeneity, such as high activity, selectivity, stability, maximized atom utilization efficiency and easy separation from reactants/products are highlighted.
Journal ArticleDOI
Atomic-Level Modulation of Electronic Density at Cobalt Single-Atom Sites Derived from Metal-Organic Frameworks: Enhanced Oxygen Reduction Performance.
Yuanjun Chen,Rui Gao,Shufang Ji,Haijing Li,Kun Tang,Peng Jiang,Haibo Hu,Zedong Zhang,Haigang Hao,Qingyun Qu,Xiao Liang,Wenxing Chen,Juncai Dong,Dingsheng Wang,Yadong Li +14 more
TL;DR: In this paper, the correlation between atomic configuration induced electronic density of single-atom Co active sites and oxygen reduction reaction (ORR) performance was demonstrated by combining density-functional theory (DFT) calculations and electrochemical analysis.
Journal ArticleDOI
Enabling Direct H2O2 Production in Acidic Media through Rational Design of Transition Metal Single Atom Catalyst
Jiajian Gao,Hongbin Yang,Xiang Huang,Sung Fu Hung,Weizheng Cai,Chunmiao Jia,Shu Miao,Hao Ming Chen,Xiaofeng Yang,Yanqiang Huang,Tao Zhang,Bin Liu +11 more
TL;DR: In this article, a cobalt single-atom catalyst (Co SAC) anchored in nitrogen-doped graphene, with optimized adsorption energy of the *OOH intermediate, exhibited a high H2O2 production rate, which even slightly outperformed the state-of-the-art noble metal-based electrocatalysts.
Journal ArticleDOI
Non-precious-metal catalysts for alkaline water electrolysis: operando characterizations, theoretical calculations, and recent advances
Jian Wang,Yang Gao,Hui Kong,Juwon Kim,Subin Choi,Francesco Ciucci,Yong Hao,Shihe Yang,Zongping Shao,Jongwoo Lim +9 more
TL;DR: The most recent advances in NPCs for AWE were systematically reviewed, emphasizing the application of in situ/operando experimental methods and density functional theory (DFT) calculations in their understanding and development.
References
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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.