Investigating the structural evolution of thiolate protected gold clusters from first-principles

We present a theoretical framework for the computation of anharmonic vibrational frequencies for large systems, with a particular focus on determining adsorbate frequencies from first principles. We give a detailed account of our local implementation of the vibrational self-consistent field approach and its correlation corrections. We show that our approach is both robust, accurate and can be easily deployed on computational grids in order to provide an efficient computational tool. We also present results on the vibrational spectrum of hydrogen fluoride on pyrene, on the thiophene molecule in the gas phase, and on small neutral gold clusters.

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Structural evolution of (Au2S)n (n = 1–8) clusters from first principles global optimization

RSC Advances ◽

10.1039/c5ra06137g ◽

2015 ◽

Vol 5 (77) ◽

pp. 62543-62550 ◽

Cited By ~ 13

Author(s):

Yiqun Feng ◽

Longjiu Cheng

Keyword(s):

Global Optimization ◽

First Principles ◽

Structural Evolution

First principles global optimization reveals the structural evolution and novel geometries of (Au2S)n nanoclusters at n = 1–8.

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Structural evolution of (Ti0.5V0.5)+1GeC (n= 1–4) under pressure from first principles

Computational Materials Science ◽

10.1016/j.commatsci.2016.10.036 ◽

2017 ◽

Vol 127 ◽

pp. 251-260 ◽

Cited By ~ 11

Author(s):

Ze-Jin Yang ◽

Rong-Feng Linghu ◽

Qing-He Gao ◽

Heng-Na Xiong ◽

Zhi-Jun Xu ◽

...

Keyword(s):

First Principles ◽

Structural Evolution

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Structural Evolution, Redox Mechanism, and Ionic Diffusion in Rhombohedral Na2FeFe(CN)6 for Sodium-Ion Batteries: First-Principles Calculations

Journal of The Electrochemical Society ◽

10.1149/1945-7111/ac49cf ◽

2022 ◽

Author(s):

Ya-Ping Wang ◽

B. P. Hou ◽

Xin-Rui Cao ◽

Shunqing Wu ◽

Zi-Zhong Zhu

Keyword(s):

First Principles ◽

Rational Design ◽

Low Cost ◽

Magnetic Moments ◽

Three Dimensional ◽

Structural Evolution ◽

Sodium Ion ◽

High Rate ◽

Sodium Ion Batteries ◽

First Principles Calculations

Abstract Prussian blue analogs (Na2FeFe(CN)6) have been regarded as potential cathode materials for sodium-ion batteries (SIBs) due to their low-cost iron resources and open framework. Herein, the detailed first-principles calculations have been performed to investigate the electrochemical properties of NaxFeFe(CN)6 during Na ion extraction. The material undergoes a phase transition from a dense rhombohedral to open cubic structure upon half-desodiation, which is resulted from competition of the Na−N Coulomb attraction and d−π covalent bonding of Fe−N. The analyses on the density of states, magnetic moments and Bader charges of NaxFeFe(CN)6 reveal that there involve in the successive redox reactions of high-spin Fe2+/Fe3+ and low-spin Fe2+/Fe3+ couples during desodiation. Moreover, the facile three-dimensional diffusion channels for Na+ ions exhibit low diffusion barriers of 0.4 eV ~ 0.44 eV, which ensures a rapid Na+ transport in the NaxFeFe(CN)6 framework, contributing to high rate performance of the battery. This study gives a deeper understanding of the electrochemical mechanisms of NaxFeFe(CN)6 during Na+ extraction, which is beneficial for the rational design of superior PBA cathodes for SIBs.

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