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Title: Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries

Abstract

Nanostructured carbon host materials are widely used to improve both sulfur utilization rate and reaction kinetics in lithium-sulfur (Li-S) batteries. However, high complexity/cost of materials synthesis and difficulty in processing nano-materials into high-mass-loading electrodes are still significant barriers to the development of low-cost and high-energy Li-S batteries. In this study, we reported a generic and scalable synthesis approach to prepare nitrogen-doped secondary carbon particles. By using nitrogen-containing precursor as an integration reagent, the nanosized Ketjen Black particles were integrated into micron-size secondary ones and nitrogen-doped (NKB) simultaneously through a one-step heat treatment. With NKB as an example material, the effects of particle integration degree on the secondary particles’ structures, pore volume and connectivity, sulfur loading capability, and cell performance were studied and discussed. At an optimal integration condition, the NKB particles had significantly improved particle dimensions with well-maintained high specific surface area and pore volume. Here, contributed by the micron size and high pore volume, the NKB/S were successfully used for high-sulfur-loading cathodes (4–7 mgs/cm-2) and were able to deliver a specific capacity of ~1100 mAh g-1 at a low-porosity (50%) and lean-electrolyte conditions (E/S =4 µL/mg-1). Feasibility of the materials for practical use was validated through scaling up synthesismore » (40 g/batch), large-area electrode coating, and practical pouch cell (1.6 Ah) assembly and test.« less

Authors:
 [1];  [2];  [3];  [4];  [4]; ORCiD logo [3]; ORCiD logo [3];  [4];  [4]; ORCiD logo [4]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Washington State Univ., Pullman, WA (United States)
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States); Univ. of British Columbia, Kelowna, BC (Canada)
  3. Washington State Univ., Pullman, WA (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
OSTI Identifier:
1895298
Report Number(s):
PNNL-SA-175294
Journal ID: ISSN 2211-2855
Grant/Contract Number:  
AC05-76RL01830; AC02-05CH11231; AC02-98CH10886
Resource Type:
Accepted Manuscript
Journal Name:
Nano Energy
Additional Journal Information:
Journal Volume: 103; Journal Issue: Part A; Journal ID: ISSN 2211-2855
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; low porosity sulfur cathode; carbon material; lean electrolyte; high energy Li-S battery

Citation Formats

Feng, Shuo, Liu, Jian, Zhang, Xiahui, Shi, Lili, Anderson, Cassidy S., Lin, Yuehe, Song, Min-Kyu, Liu, Jun, Xiao, Jie, and Lu, Dongping. Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries. United States: N. p., 2022. Web. doi:10.1016/j.nanoen.2022.107794.
Feng, Shuo, Liu, Jian, Zhang, Xiahui, Shi, Lili, Anderson, Cassidy S., Lin, Yuehe, Song, Min-Kyu, Liu, Jun, Xiao, Jie, & Lu, Dongping. Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries. United States. https://doi.org/10.1016/j.nanoen.2022.107794
Feng, Shuo, Liu, Jian, Zhang, Xiahui, Shi, Lili, Anderson, Cassidy S., Lin, Yuehe, Song, Min-Kyu, Liu, Jun, Xiao, Jie, and Lu, Dongping. Fri . "Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries". United States. https://doi.org/10.1016/j.nanoen.2022.107794. https://www.osti.gov/servlets/purl/1895298.
@article{osti_1895298,
title = {Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries},
author = {Feng, Shuo and Liu, Jian and Zhang, Xiahui and Shi, Lili and Anderson, Cassidy S. and Lin, Yuehe and Song, Min-Kyu and Liu, Jun and Xiao, Jie and Lu, Dongping},
abstractNote = {Nanostructured carbon host materials are widely used to improve both sulfur utilization rate and reaction kinetics in lithium-sulfur (Li-S) batteries. However, high complexity/cost of materials synthesis and difficulty in processing nano-materials into high-mass-loading electrodes are still significant barriers to the development of low-cost and high-energy Li-S batteries. In this study, we reported a generic and scalable synthesis approach to prepare nitrogen-doped secondary carbon particles. By using nitrogen-containing precursor as an integration reagent, the nanosized Ketjen Black particles were integrated into micron-size secondary ones and nitrogen-doped (NKB) simultaneously through a one-step heat treatment. With NKB as an example material, the effects of particle integration degree on the secondary particles’ structures, pore volume and connectivity, sulfur loading capability, and cell performance were studied and discussed. At an optimal integration condition, the NKB particles had significantly improved particle dimensions with well-maintained high specific surface area and pore volume. Here, contributed by the micron size and high pore volume, the NKB/S were successfully used for high-sulfur-loading cathodes (4–7 mgs/cm-2) and were able to deliver a specific capacity of ~1100 mAh g-1 at a low-porosity (50%) and lean-electrolyte conditions (E/S =4 µL/mg-1). Feasibility of the materials for practical use was validated through scaling up synthesis (40 g/batch), large-area electrode coating, and practical pouch cell (1.6 Ah) assembly and test.},
doi = {10.1016/j.nanoen.2022.107794},
journal = {Nano Energy},
number = Part A,
volume = 103,
place = {United States},
year = {Fri Sep 09 00:00:00 EDT 2022},
month = {Fri Sep 09 00:00:00 EDT 2022}
}

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