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Title: Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities

Abstract

Affordable sodium ion batteries hold great promise for revolutionizing stationary energy storage technologies. Sodium layered cathode materials are usually multicomponent transition metal (TM) oxides and each TM plays a unique role in the operating cathode chemistry, e.g., redox activity, structural stabilization. Engineering the three-dimensional (3D) distribution of TM cations in individual cathode particles can take advantage of a depth-dependent charging mechanism and enable a path towards tuning local TM–O chemical environments and building resilience against cathode–electrolyte interfacial reactions that are responsible for capacity fading, voltage decay and safety hazards. In this study, we create 3D compositional heterogeneity in a ternary and biphasic (O3–P3) sodium layered cathode material (Na 0.9Cu 0.2Fe 0.28Mn 0.52O 2). The cells containing this material deliver stable voltage profiles, and discharge capacities of 125 mA h g –1 at C/10 with almost no capacity fading after 100 cycles and 75 mA h g –1 at 1C with negligible capacity fading after 200 cycles. The direct performance comparison shows that this material outperforms other materials with similar global compositions but different mesoscale chemical distributions. Synchrotron X-ray spectroscopy/imaging and density functional theory studies reveal depth-dependent chemical environments due to changes to factors such as charge compensation and strength ofmore » orbital hybridization. Finally, 3D spectroscopic tomography illuminates the path towards optimizing multicomponent sodium layered cathode materials, to prevent the migration of TMs upon prolonged cycling. Furthermore, the study reports an inaugural effort of multifaceted and counterintuitive investigation of sodium layered cathode materials and strongly implies that there is plenty of room at the bottom by tuning nano/meso scale chemical distributions for stable cathode chemistry.« less

Authors:
ORCiD logo [1];  [2];  [3];  [1];  [4];  [1];  [5];  [2];  [4];  [4];  [2];  [2]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Xiamen Univ., Xiamen (China); Xiamen Univ. Malaysia, Sepang (Malaysia)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. City Univ. of Hong Kong, Kowloon (Hong Kong)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); Virginia Tech University; National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1484286
Alternate Identifier(s):
OSTI ID: 1457067
Grant/Contract Number:  
AC02-06CH11357; AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Energy & Environmental Science
Additional Journal Information:
Journal Volume: 11; Journal Issue: 9; Journal ID: ISSN 1754-5692
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Rahman, Muhammad Mominur, Xu, Yahong, Cheng, Hao, Shi, Qianli, Kou, Ronghui, Mu, Linqin, Liu, Qi, Xia, Sihao, Xiao, Xianghui, Sun, Cheng -Jun, Sokaras, Dimosthenis, Nordlund, Dennis, Zheng, Jin -Cheng, Liu, Yijin, and Lin, Feng. Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities. United States: N. p., 2018. Web. doi:10.1039/c8ee00309b.
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Rahman, Muhammad Mominur, Xu, Yahong, Cheng, Hao, Shi, Qianli, Kou, Ronghui, Mu, Linqin, Liu, Qi, Xia, Sihao, Xiao, Xianghui, Sun, Cheng -Jun, Sokaras, Dimosthenis, Nordlund, Dennis, Zheng, Jin -Cheng, Liu, Yijin, & Lin, Feng. Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities. United States. doi:10.1039/c8ee00309b.
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Rahman, Muhammad Mominur, Xu, Yahong, Cheng, Hao, Shi, Qianli, Kou, Ronghui, Mu, Linqin, Liu, Qi, Xia, Sihao, Xiao, Xianghui, Sun, Cheng -Jun, Sokaras, Dimosthenis, Nordlund, Dennis, Zheng, Jin -Cheng, Liu, Yijin, and Lin, Feng. Mon . "Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities". United States. doi:10.1039/c8ee00309b. https://www.osti.gov/servlets/purl/1484286.
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@article{osti_1484286,
title = {Empowering multicomponent cathode materials for sodium ion batteries by exploring three-dimensional compositional heterogeneities},
author = {Rahman, Muhammad Mominur and Xu, Yahong and Cheng, Hao and Shi, Qianli and Kou, Ronghui and Mu, Linqin and Liu, Qi and Xia, Sihao and Xiao, Xianghui and Sun, Cheng -Jun and Sokaras, Dimosthenis and Nordlund, Dennis and Zheng, Jin -Cheng and Liu, Yijin and Lin, Feng},
abstractNote = {Affordable sodium ion batteries hold great promise for revolutionizing stationary energy storage technologies. Sodium layered cathode materials are usually multicomponent transition metal (TM) oxides and each TM plays a unique role in the operating cathode chemistry, e.g., redox activity, structural stabilization. Engineering the three-dimensional (3D) distribution of TM cations in individual cathode particles can take advantage of a depth-dependent charging mechanism and enable a path towards tuning local TM–O chemical environments and building resilience against cathode–electrolyte interfacial reactions that are responsible for capacity fading, voltage decay and safety hazards. In this study, we create 3D compositional heterogeneity in a ternary and biphasic (O3–P3) sodium layered cathode material (Na0.9Cu0.2Fe0.28Mn0.52O2). The cells containing this material deliver stable voltage profiles, and discharge capacities of 125 mA h g–1 at C/10 with almost no capacity fading after 100 cycles and 75 mA h g–1 at 1C with negligible capacity fading after 200 cycles. The direct performance comparison shows that this material outperforms other materials with similar global compositions but different mesoscale chemical distributions. Synchrotron X-ray spectroscopy/imaging and density functional theory studies reveal depth-dependent chemical environments due to changes to factors such as charge compensation and strength of orbital hybridization. Finally, 3D spectroscopic tomography illuminates the path towards optimizing multicomponent sodium layered cathode materials, to prevent the migration of TMs upon prolonged cycling. Furthermore, the study reports an inaugural effort of multifaceted and counterintuitive investigation of sodium layered cathode materials and strongly implies that there is plenty of room at the bottom by tuning nano/meso scale chemical distributions for stable cathode chemistry.},
doi = {10.1039/c8ee00309b},
journal = {Energy & Environmental Science},
number = 9,
volume = 11,
place = {United States},
year = {2018},
month = {6}
}
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DOI:  10.1039/c8ee00309b
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Figures / Tables:

Figure 1 Figure 1: Physicochemical characterization of the pristine CFM-Cu powder. (a) XRD pattern of the pristine CFM-Cu powder. (b) SEM micrographs of the pristine CFM-Cu powder. (c) Soft XAS spectra (TEY mode) of the pristine CFM-Cu powder, where the peak labeled with “*” originated from the surface carbonate species.
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