(Grand Challenges of Energy Science) Disordered Cathode Materials for Li-Ion Batteries
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1 (Grand Challenges of Energy Science) Disordered Cathode Materials for Li-Ion Batteries Alexander Urban, Dong-Hwa Seo, Jinhyuk Lee, Aziz Abdellahi, and Gerbrand Ceder Department of Materials Science and Engineering, University of California, Berkeley. Berkeley, CA, April 13, 2017
2 Li-ion batteries have enabled a technological revolution Li-ion batteries made possible Modern portable electronics Electric vehicles Huge demand for better LIBs Make smartphones last longer/more powerful Increase range of EVs 2
3 Li-ion batteries function by shuttling Li ions charge e e discharge charge e LiLi+ Li Li Li Li LiLi+ Li Li Li Li Negative Electrode Electrolyte Positive Electrode Anode and cathode are conventionally named following the discharge direction. 3
4 Figures of merit criteria for improved LIBs Capacity Voltage = Energy Density Capacity Voltage Amount of electrons (= Li) per mass or volume that can utilized Potential difference between electrodes. Cathode material (positive electrode) is current bottleneck for capacity & voltage. 4
5 Cathode research has focused on ordered TM oxides O Limitations TM Limited chemistry (Co, Ni, Mn, Al) Li Not entire Li content usable Limited capacity: mah/g O3-type layered LiCoO2-structure Close-packed O framework Alternating Li and TM layers High density LCO (Co) NCA (Ni, Co, Al) NCM (Ni, Co, Mn) 5
6 Energy densities of layered cathodes Energy Density (Wh/kg) Greater specific capacities needed Data from: Nitta et al., Materials Today 18 (2015)
7 Cation-Disordered Cathode Materials for Li-Ion Batteries 7
8 Cation-disordered Li1.211Mo0.467Cr0.3O2 (LMCO) Jinhyuk Lee well-separated Li and TM layers Xin Li layered O3 disordered rocksalt intense cation mixing (34-52%) J. Lee, A. Urban, X. Li, D. Su, G. Hautier, G. Ceder, Science 343 (2014)
9 Cation-disordered LMCO has a remarkable capacity 1 Li per LiMO2 LiCoO2 ~1 Li atom per LiMO2 formula unit can be reversibly cycled J. Lee, A. Urban, X. Li, D. Su, G. Hautier, G. Ceder, Science 343 (2014)
10 Cation-disorder creates fast 0-TM diffusion channels 3+/4+ 3+/4+ 2-TM 3+/4+ Layered? 3+/4+ 1-TM? TM Cation disordered 1+ 10
11 Only 0-TM channels are active when disordered only 0-TM active both channels active 1-TM 1-TM 0-TM 0-TM disordered structures Distribution of diffusion barriers calculated with DFT (PBE) and NEB J. Lee, A. Urban, X. Li, D. Su, G. Hautier, G. Ceder, Science 343 (2014)
12 Around 10% Li excess enables 0-TM percolation One Li 0-TM cyclable at ~25 % Li excess Li1.211Mo0.467Cr0.3O2 Disordered Percolation threshold Layered A. Urban, J. Lee, and G. Ceder, Adv. Energy Mater. 4 (2014)
13 Impact on Li-ion battery cathode research 1991: Li 3 V 2 O 5 = Li 1.2 V 0.8 O 2 C. Delmas, S. Brèthes and M. Ménétrier ω-li x V 2 O 5, J. Power Sources 34 (1991) : LiMO 2 (M=Ti, Mn, Fe, Co, Ni) by mechanochemical synthesis (ball-milling) M. Obrovac, O. Mao, and J. Dahn, Solid State Ionics 112 (1998) : Li Mo Cr 0.3 O 2 J. Lee, A. Urban, X. Li, D. Su, G. Hautier, and G. Ceder, Science 343 (2014) : Li 2 VO 2 F = Li V O F R. Chen, S. Ren, M. Knapp, D. Wang, R. Witter, M. Fichtner, and H. Hahn, Adv. Energy Mater. 5 (2015) : Li 1.3 Nb x M 0.7-x O 2 (M = Mn, Fe, Co, Ni) N. Yabuuchi, M. Takeuchi, M. Nakayama, H. Shiiba, M. Ogawa, K. Nakayama, T. Ohta, D. Endo, T. Ozaki, T. Inamasu, K. Sato, and S. Komaba, Proc. Natl. Acad. Sci. USA 112 (2015) : Li 1.25 Nb 0.25 Mn 0.5 O 2 R. Wang, X. Li, L. Liu, J. Lee, D.-H. Seo, S.-H. Bo, A. Urban, G. Ceder, Electrochem. Commun. 60 (2015) : Li 1.2 Ni Ti Mo O 2 J. Lee, D.-H. Seo, M. Balasubramanian, N. Twu, X. Li and G. Ceder, Energy Environ. Sci. 8 (2015) : Li 1+x Ti 2x Fe 1-3x O 2 S. L. Glazier, J. Li, J. Zhou, T. Bond and J. R. Dahn, Chem. Mater. 27 (2015) : Li Ni Mo O 2 N. Yabuuchi, Y. Tahara, S. Komaba, S. Kitada and Y. Kajiya, Chem. Mater. 28 (2016) : Li 1.3 Nb 0.3 V 0.4 O 2 N. Yabuuchi, M. Takeuchi, S. Komaba, S. Ichikawa, T. Ozaki, and T. Inamasu, Chem. Commun. 52 (2016)
14 The new materials have high energy densities Energy Density (Wh/kg) LCO, NMC, NCA data from: Nitta et al., Materials Today 18 (2015)
15 Can disordered materials achieve high voltages? Energy Density (Wh/kg) Higher voltage desirable LCO, NMC, NCA data from: Nitta et al., Materials Today 18 (2015)
16 Figures of merit criteria for improved LIBs Capacity Voltage Amount of electrons (= Li) per mass or volume that can utilized Potential difference between electrodes. 16
17 Effect of disorder on redox & voltage Aziz Abdellahi Dong-Hwa Seo Jinhyuk Lee Energy (ev) Voltage (V) A. Abdellahi, A. Urban, S. Dacek, and G. Ceder, Chem. Mater. 28 (2016) Transition Metal D.-H. Seo, J. Lee, A. Urban, R. Malik, S. Kang, and G. Ceder, Nat. Chem. 8 (2016) A. Abdellahi, A. Urban, S. Dacek, and G. Ceder, Chem. Mater. 28 (2016)
18 Current understanding of cation disorder 1. Cation order does (almost) not matter for capacity Cation mixing does not affect practical capacity for compositions with more than 15% Li excess 2. Cation disorder may increase structural stability Increased structural stability (lattice parameters) 3. Disorder affects the voltage Average voltage & voltage profile (slope) Redox mechanism, oxygen redox Dong-Hwa Seo A. Urban, J. Lee, and G. Ceder, Adv. Energy Mater. 4 (2014) J. Lee, A. Urban, X. Li, D. Su, G. Hautier, G. Ceder, Science 343 (2014)
19 Acknowledgments Dong-Hwa Seo Jinhyuk Lee Xin Li Aziz Abdellahi (now Harvard U) (now at A123) Gerd Ceder 19
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