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Title: Manipulating Adsorption-Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage

Abstract

Hard carbon is one of the most promising anode materials for sodium-ion batteries, but the low coulombic efficiency is still a key barrier. In this paper we synthesized a series of nanostructured hard carbon materials with controlled architectures. Using a combination of in-situ XRD mapping, ex-situ NMR, EPR, electrochemical techniques and simulations, an “adsorption-intercalation” (A-I) mechanism is established for Na ion storage. During the initial stages of Na insertion, Na ions adsorb on the defect sites of hard carbon with a wide adsorption energy distribution, producing a sloping voltage profile. In the second stage, Na ions intercalate into graphitic layers with suitable spacing to form NaCx compounds similar to the Li ion intercalation process in graphite, producing a flat low voltage plateau. The cation intercalation with a flat voltage plateau should be enhanced and the sloping region should be avoided. Guided by this knowledge, non-porous hard carbon material has been developed which has achieved high reversible capacity and coulombic efficiency to fulfill practical application.

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [5];  [4];  [5];  [1];  [1];  [1];  [3]
  1. College of Chemistry and Molecular Sciences, Hubei Key Laboratory of Electrochemical Power Sources, Wuhan University, Wuhan 430072 China
  2. College of Chemistry, Central China Normal University, Wuhan 430079 China; Pacific Northwest National Laboratory, Richland WA 99352 USA
  3. Pacific Northwest National Laboratory, Richland WA 99352 USA
  4. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, School of Materials Science and Engineering, Wuhan University of Technology, Wuhan 430070 China
  5. State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Chinese Academy of Science, Wuhan 430071 China
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1422336
Report Number(s):
PNNL-SA-131546
Journal ID: ISSN 1614-6832; KC0203020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Advanced Energy Materials; Journal Volume: 7; Journal Issue: 17
Country of Publication:
United States
Language:
English

Citation Formats

Qiu, Shen, Xiao, Lifen, Sushko, Maria L., Han, Kee Sung, Shao, Yuyan, Yan, Mengyu, Liang, Xinmiao, Mai, Liqiang, Feng, Jiwen, Cao, Yuliang, Ai, Xinping, Yang, Hanxi, and Liu, Jun. Manipulating Adsorption-Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage. United States: N. p., 2017. Web. doi:10.1002/aenm.201700403.
Qiu, Shen, Xiao, Lifen, Sushko, Maria L., Han, Kee Sung, Shao, Yuyan, Yan, Mengyu, Liang, Xinmiao, Mai, Liqiang, Feng, Jiwen, Cao, Yuliang, Ai, Xinping, Yang, Hanxi, & Liu, Jun. Manipulating Adsorption-Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage. United States. doi:10.1002/aenm.201700403.
Qiu, Shen, Xiao, Lifen, Sushko, Maria L., Han, Kee Sung, Shao, Yuyan, Yan, Mengyu, Liang, Xinmiao, Mai, Liqiang, Feng, Jiwen, Cao, Yuliang, Ai, Xinping, Yang, Hanxi, and Liu, Jun. Fri . "Manipulating Adsorption-Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage". United States. doi:10.1002/aenm.201700403.
@article{osti_1422336,
title = {Manipulating Adsorption-Insertion Mechanisms in Nanostructured Carbon Materials for High-Efficiency Sodium Ion Storage},
author = {Qiu, Shen and Xiao, Lifen and Sushko, Maria L. and Han, Kee Sung and Shao, Yuyan and Yan, Mengyu and Liang, Xinmiao and Mai, Liqiang and Feng, Jiwen and Cao, Yuliang and Ai, Xinping and Yang, Hanxi and Liu, Jun},
abstractNote = {Hard carbon is one of the most promising anode materials for sodium-ion batteries, but the low coulombic efficiency is still a key barrier. In this paper we synthesized a series of nanostructured hard carbon materials with controlled architectures. Using a combination of in-situ XRD mapping, ex-situ NMR, EPR, electrochemical techniques and simulations, an “adsorption-intercalation” (A-I) mechanism is established for Na ion storage. During the initial stages of Na insertion, Na ions adsorb on the defect sites of hard carbon with a wide adsorption energy distribution, producing a sloping voltage profile. In the second stage, Na ions intercalate into graphitic layers with suitable spacing to form NaCx compounds similar to the Li ion intercalation process in graphite, producing a flat low voltage plateau. The cation intercalation with a flat voltage plateau should be enhanced and the sloping region should be avoided. Guided by this knowledge, non-porous hard carbon material has been developed which has achieved high reversible capacity and coulombic efficiency to fulfill practical application.},
doi = {10.1002/aenm.201700403},
journal = {Advanced Energy Materials},
number = 17,
volume = 7,
place = {United States},
year = {Fri May 12 00:00:00 EDT 2017},
month = {Fri May 12 00:00:00 EDT 2017}
}