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Title: Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries

Abstract

Despite the outstanding gravimetric performance of lithium-sulfur (Li-S) batteries, their practical volumetric energy density is normally lower than that of lithium-ion batteries, mainly due to the low density of nanostructured sulfur as well as the porous carbon hosts. Here, a novel approach is developed to fabricate high-density graphene bulk materials with ink-bottle-like mesopores by phosphoric acid (H 3PO 4) activation. These pores can effectively confine the polysulfides due to their unique structure with a wide body and narrow neck, which shows only a 0.05% capacity fade per cycle for 500 cycles (75% capacity retention) for accommodating polysulfides. With a density of 1.16 g cm -3, a hybrid cathode containing 54 wt% sulfur delivers a high volumetric capacity of 653 mA h cm -3. As a result, a device-level volumetric energy density as high as 408 W h L -1 is achieved with a cathode thickness of 100 mu m. This is a periodic yet practical advance to improve the volumetric performance of Li-S batteries from a device perspective. Furthermore, this work suggests a design principle for the real use Li-S batteries although there is a long way ahead to bridge the gap between Li-S batteries and Li-ion batteries in volumetricmore » performance.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [1];  [1];  [1];  [3];  [2]; ORCiD logo [4];  [5]
  1. Tianjin Univ., Tianjin (China)
  2. Tsinghua Univ., Shenzhen (China)
  3. UNSW Australia (The Univ. of New South Wales), Sydney, NSW (Australia)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Tianjin Univ., Tianjin (China); Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1466311
Alternate Identifier(s):
OSTI ID: 1425506
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 8; Journal Issue: 18; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; graphene monolith; ink-bottle-like pores; lithium-polysulfide batteries; polysulfides; volumetric performance

Citation Formats

Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, and Yang, Quan -Hong. Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries. United States: N. p., 2018. Web. doi:10.1002/aenm.201703438.
Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, & Yang, Quan -Hong. Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries. United States. doi:10.1002/aenm.201703438.
Li, Huan, Tao, Ying, Zhang, Chen, Liu, Donghai, Luo, Jiayan, Fan, Weichao, Xu, Yue, Li, Youzhi, You, Conghui, Pan, Zheng -Ze, Ye, Mingchun, Chen, Zhengyu, Dong, Zhang, Wang, Da -Wei, Kang, Feiyu, Lu, Jun, and Yang, Quan -Hong. Mon . "Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries". United States. doi:10.1002/aenm.201703438. https://www.osti.gov/servlets/purl/1466311.
@article{osti_1466311,
title = {Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries},
author = {Li, Huan and Tao, Ying and Zhang, Chen and Liu, Donghai and Luo, Jiayan and Fan, Weichao and Xu, Yue and Li, Youzhi and You, Conghui and Pan, Zheng -Ze and Ye, Mingchun and Chen, Zhengyu and Dong, Zhang and Wang, Da -Wei and Kang, Feiyu and Lu, Jun and Yang, Quan -Hong},
abstractNote = {Despite the outstanding gravimetric performance of lithium-sulfur (Li-S) batteries, their practical volumetric energy density is normally lower than that of lithium-ion batteries, mainly due to the low density of nanostructured sulfur as well as the porous carbon hosts. Here, a novel approach is developed to fabricate high-density graphene bulk materials with ink-bottle-like mesopores by phosphoric acid (H3PO4) activation. These pores can effectively confine the polysulfides due to their unique structure with a wide body and narrow neck, which shows only a 0.05% capacity fade per cycle for 500 cycles (75% capacity retention) for accommodating polysulfides. With a density of 1.16 g cm-3, a hybrid cathode containing 54 wt% sulfur delivers a high volumetric capacity of 653 mA h cm-3. As a result, a device-level volumetric energy density as high as 408 W h L-1 is achieved with a cathode thickness of 100 mu m. This is a periodic yet practical advance to improve the volumetric performance of Li-S batteries from a device perspective. Furthermore, this work suggests a design principle for the real use Li-S batteries although there is a long way ahead to bridge the gap between Li-S batteries and Li-ion batteries in volumetric performance.},
doi = {10.1002/aenm.201703438},
journal = {Advanced Energy Materials},
number = 18,
volume = 8,
place = {United States},
year = {2018},
month = {3}
}

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Cited by: 20 works
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Figures / Tables:

Fig. 1 Fig. 1 : Starting from a 3D graphene hydrogel, a commonly freeze-drying method results in a graphene monolith (GM) with hierarchical pores with low density (a); However, by H3PO4 activation and CEID method, a high density graphene monolith with large amounts of inkbottle-like pores (69%) was prepared (b); N2 adsorption-desorptionmore » isotherm (77K) of a typical (c) GM and (d) IBGM, where IBGM is prepared by controlling the H3PO4/GM mass ratio at 3 and is heat treated at 600 oC after washing; High-resolution TEM images of GM (e) and IBGM (f); (g) Pore size distributions determined by accumulative pore volume of IBGM; (h) FTIR spectra of GM and IBGM; (i) The cycling performance of IBGM and GM as the carbon host for confining the polysulfides at 0.5 C.« less

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