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Title: Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density

Abstract

Even though tremendous achievement has been made experimentally in the performance of lithium–sulfur (Li–S) battery, theoretical studies in this area are lagging behind due to the complexity of the Li–S systems and the effects of solvent. Because of this, a new methodology is developed for investigating the 2D hexaaminobenzene-based coordination polymers (2D-HAB-CPs) as cathode candidate materials for Li–S batteries via density functional theory calculations in combination with an in-house developed charge polarized solvent model and a genetic algorithm structure global search code. With high ratios of transition metal atoms and two-coordinated nitrogen atoms, excellent electric conductivity, and structural porosity, the 2D-HAB-CP is able to address all of the three main challenges facing Li–S batteries: confining the lithium polysulfides from dissolution, facilitating the electron conductivity and buffering the volumetric expansion during the lithiation process. In addition, the theoretical energy density of this system is as high as 1395 Wh kg-1. These results demonstrate that the 2D-HAB-CP is a promising cathode material for Li–S batteries. The proposed computational framework not only opens a new avenue for understanding the key role played by solution and liquid electrolytes in Li–S batteries, but also can be generally applied to other processes with liquids involved.

Authors:
ORCiD logo [1];  [1];  [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Peking Univ., Shenzhen (China). Shenzhen Graduate School, School of Advanced Materials
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1543468
Alternate Identifier(s):
OSTI ID: 1461706
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 25; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; chemistry; energy & fuels; materials science; physics; 2D hexaaminobenzene-based coordination polymers; cathode materials; Li-S batteries

Citation Formats

Gao, Guoping, Zheng, Fan, Pan, Feng, and Wang, Lin-Wang. Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density. United States: N. p., 2018. Web. doi:10.1002/aenm.201801823.
Gao, Guoping, Zheng, Fan, Pan, Feng, & Wang, Lin-Wang. Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density. United States. doi:10.1002/aenm.201801823.
Gao, Guoping, Zheng, Fan, Pan, Feng, and Wang, Lin-Wang. Wed . "Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density". United States. doi:10.1002/aenm.201801823. https://www.osti.gov/servlets/purl/1543468.
@article{osti_1543468,
title = {Theoretical Investigation of 2D Conductive Microporous Coordination Polymers as Li-S Battery Cathode with Ultrahigh Energy Density},
author = {Gao, Guoping and Zheng, Fan and Pan, Feng and Wang, Lin-Wang},
abstractNote = {Even though tremendous achievement has been made experimentally in the performance of lithium–sulfur (Li–S) battery, theoretical studies in this area are lagging behind due to the complexity of the Li–S systems and the effects of solvent. Because of this, a new methodology is developed for investigating the 2D hexaaminobenzene-based coordination polymers (2D-HAB-CPs) as cathode candidate materials for Li–S batteries via density functional theory calculations in combination with an in-house developed charge polarized solvent model and a genetic algorithm structure global search code. With high ratios of transition metal atoms and two-coordinated nitrogen atoms, excellent electric conductivity, and structural porosity, the 2D-HAB-CP is able to address all of the three main challenges facing Li–S batteries: confining the lithium polysulfides from dissolution, facilitating the electron conductivity and buffering the volumetric expansion during the lithiation process. In addition, the theoretical energy density of this system is as high as 1395 Wh kg-1. These results demonstrate that the 2D-HAB-CP is a promising cathode material for Li–S batteries. The proposed computational framework not only opens a new avenue for understanding the key role played by solution and liquid electrolytes in Li–S batteries, but also can be generally applied to other processes with liquids involved.},
doi = {10.1002/aenm.201801823},
journal = {Advanced Energy Materials},
number = 25,
volume = 8,
place = {United States},
year = {2018},
month = {7}
}

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Figures / Tables:

Figure 1 Figure 1: (a) The geometric structure of Mn-HAB-CP monolayer. (b)The band structure of Mn-HAB-CP monolayer along the high symmetry Γ-K-M-Γ directions and the associated Brillouin zone. The Fermi energy in the band structure is at 0.

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    Works referencing / citing this record:

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      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.