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4. Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Author

Xue, Weijiang, Huang, Mingjun, Li, Yutao, Zhu, Yun Guang, Gao, Rui, Xiao, Xianghui, Zhang, Wenxu, Li, Sipei, Xu, Guiyin, Yu, Yang, Li, Peng, Lopez, Jeffrey, Yu, Daiwei, Dong, Yanhao, Fan, Weiwei, Shi, Zhe, Xiong, Rui, Sun, Cheng-Jun, Hwang, Inhui, Lee, Wah-Keat, Shao-Horn, Yang, Johnson, Jeremiah A, Li, Ju, Xue, Weijiang, Huang, Mingjun, Li, Yutao, Zhu, Yun Guang, Gao, Rui, Xiao, Xianghui, Zhang, Wenxu, Li, Sipei, Xu, Guiyin, Yu, Yang, Li, Peng, Lopez, Jeffrey, Yu, Daiwei, Dong, Yanhao, Fan, Weiwei, Shi, Zhe, Xiong, Rui, Sun, Cheng-Jun, Hwang, Inhui, Lee, Wah-Keat, Shao-Horn, Yang, Johnson, Jeremiah A, and Li, Ju

Published
2022

5. Enhanced Cycling of Ni-Rich Positive Electrodes by Fluorine Modification

Author

Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Yu, Yang, Zhang, Yirui, Giordano, Livia, Zhu, Yun Guang, Maglia, Filippo, Jung, Roland, Gittleson, Forrest S., Shao-Horn, Yang, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Yu, Yang, Zhang, Yirui, Giordano, Livia, Zhu, Yun Guang, Maglia, Filippo, Jung, Roland, Gittleson, Forrest S., and Shao-Horn, Yang

Abstract

BMW

Published
2022

6. Enhanced Cycling of Ni-Rich Positive Electrodes by Fluorine Modification

Author

Yu, Yang, Zhang, Yirui, Giordano, Livia, Zhu, Yun Guang, Maglia, Filippo, Jung, Roland, Gittleson, Forrest S., Shao-horn, Yang, Yu, Yang, Zhang, Yirui, Giordano, Livia, Zhu, Yun Guang, Maglia, Filippo, Jung, Roland, Gittleson, Forrest S., and Shao-horn, Yang

Abstract

BMW

Published
2022

7. Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte

Author

Massachusetts Institute of Technology. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology. Department of Mechanical Engineering, Xue, Weijiang, Huang, Mingjun, Li, Yutao, Zhu, Yun Guang, Gao, Rui, Xiao, Xianghui, Zhang, Wenxu, Li, Sipei, Xu, Guiyin, Yu, Yang, Li, Peng, Lopez, Jeffrey, Yu, Daiwei, Dong, Yanhao, Fan, Weiwei, Shi, Zhe, Xiong, Rui, Sun, Cheng-Jun, Hwang, Inhui, Lee, Wah-Keat, Shao-Horn, Yang, Johnson, Jeremiah A., Li, Ju, Massachusetts Institute of Technology. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Electrical Engineering and Computer Science, Massachusetts Institute of Technology. Department of Mechanical Engineering, Xue, Weijiang, Huang, Mingjun, Li, Yutao, Zhu, Yun Guang, Gao, Rui, Xiao, Xianghui, Zhang, Wenxu, Li, Sipei, Xu, Guiyin, Yu, Yang, Li, Peng, Lopez, Jeffrey, Yu, Daiwei, Dong, Yanhao, Fan, Weiwei, Shi, Zhe, Xiong, Rui, Sun, Cheng-Jun, Hwang, Inhui, Lee, Wah-Keat, Shao-Horn, Yang, Johnson, Jeremiah A., and Li, Ju

Published
2022

8. The Stable 3D Zn Electrode for High-Power Density Zn Metal Batteries

Author

Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Zhu, Yun Guang, Narayanan, Thaneer Malai, Katayama, Yukihisa, Shao-Horn, Yang, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Zhu, Yun Guang, Narayanan, Thaneer Malai, Katayama, Yukihisa, and Shao-Horn, Yang

Abstract

A stable Zn metal electrode can develop rechargeable zinc metal batteries (RZMBs) which have the high theoretical capacity (820 mAh g−1), low redox potential, and intrinsic safety. However, the corrosion of Zn metal in aqueous electrolytes and Zn dendrite formation during the plating process lead to poor cycling and thus hinder the development of RZMBs. Here, we employed ionic liquid-based gel polymer (poly(vinylidene fluoride)-co-hexafluoropropylene, PVDF-HFP) and acetylene black (AB) to achieve a stable and flexible three-dimensional (3D) Zn/AB/PVDF-HFP film electrode with ionic and electronic conductive networks and high surface area, showing 26 times higher plating/stripping current than planar Zn plate. By developing a continuous structure between the ionic liquid-based gel polymer membrane and the flexible 3D Zn/AB/PVDF-HFP electrode, the low resistance, high rate capability and long cycle life (> 800 h) was obtained. Our work shows a flexible Zn film electrode and ionic liquid-based gel polymer electrolyte, could pave the path for rechargeable and high-cycle life thin-film RZMBs., Toyota Motor Corporation

Published
2022

9. A high-rate and high-efficiency molten-salt sodium–oxygen battery

Author

Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Electrochemical Energy Laboratory, Zhu, Yun Guang, Leverick, Graham, Accogli, Alessandra, Gordiz, Kiarash, Zhang, Yirui, Shao-Horn, Yang, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Electrochemical Energy Laboratory, Zhu, Yun Guang, Leverick, Graham, Accogli, Alessandra, Gordiz, Kiarash, Zhang, Yirui, and Shao-Horn, Yang

Abstract

Alkali metal–oxygen batteries can provide greater specific energy than Li-ion batteries but often suffer from low power density, cycleability, and energy efficiency due to the sluggish kinetics of the oxygen electrode and parasitic reactions at both the oxygen and alkali metal electrodes. In this study, we demonstrated a molten-salt Na–O2 battery operating at 443 K with high areal energy (33 mW h cm2 geo) and power densities (19 mW cm2 geo), with high energy efficiency (B90% at 5 mA cm2 geo), and stable cycling (400 cycles with no capacity loss). Raman, pressure tracking and titration measurements were used to show that the dominant discharge product is Na2O2. Moreover, the redox activity of nitrate anions in the molten salt was found to be critical to enable the formation of Na2O2. Through 18O-labeling experiments as well as discharging Na–Ar cells, we demonstrated that the discharge reaction occurs via the electrochemical reduction of NaNO3 to Na2O and NaNO2, where chemical reactions with O2 lead to the formation of Na2O2 from Na2O, and the regeneration of NaNO3 from NaNO2.

Published
2022

11. Stabilizing electrode–electrolyte interfaces to realize high-voltage Li||LiCoO2 batteries by a sulfonamide-based electrolyte

Author

Massachusetts Institute of Technology. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Xue, Weijiang, Gao, Rui, Shi, Zhe, Xiao, Xianghui, Zhang, Wenxu, Zhang, Yirui, Zhu, Yun Guang, Waluyo, Iradwikanari, Li, Yao, Hill, Megan R., Zhu, Zhi, Li, Sa, Kuznetsov, Oleg, Zhang, Yiman, Lee, Wah-Keat, Hunt, Adrian, Harutyunyan, Avetik, Shao-Horn, Yang, Johnson, Jeremiah A., Li, Ju, Massachusetts Institute of Technology. Department of Nuclear Science and Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Research Laboratory of Electronics, Xue, Weijiang, Gao, Rui, Shi, Zhe, Xiao, Xianghui, Zhang, Wenxu, Zhang, Yirui, Zhu, Yun Guang, Waluyo, Iradwikanari, Li, Yao, Hill, Megan R., Zhu, Zhi, Li, Sa, Kuznetsov, Oleg, Zhang, Yiman, Lee, Wah-Keat, Hunt, Adrian, Harutyunyan, Avetik, Shao-Horn, Yang, Johnson, Jeremiah A., and Li, Ju

Abstract

High-voltage lithium-metal batteries (LMBs) with LiCoO2 (LCO) as the cathode have high volumetric and gravimetric energy densities. However, it remains a challenge for stable cycling of LCO >4.5 VLi. Here we demonstrate that a rationally designed sulfonamide-based electrolyte can greatly improve the cycling stability at high voltages up to 4.7 VLi by stabilizing the electrode–electrolyte interfaces (EEIs) on both the Li-metal anode (LMA) and high-voltage LCO cathode. With the sulfonamide-based electrolyte, commercial LCO cathodes retain 89% and 85% of their capacities after 200 and 100 cycles under high charging voltages of 4.55 VLi and 4.6 VLi, respectively, significantly outperforming traditional carbonate-based electrolytes. The surface degradation, impedance growth, and detrimental side reactions in terms of gas evolution and Co dissolution are well suppressed. Our work demonstrates a promising strategy for designing new electrolytes to realize high-energy Li||LCO batteries.

Published
2021

12. High-energy and high-power Zn–Ni flow batteries with semi-solid electrodes

Author

Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Zhu, Yun Guang, Narayanan, Thaneer Malai, Tulodziecki, Michal, Sanchez-Casalongue, Hernan, Horn, Quinn C., Meda, Laura, Yang, Yu, Sun, Jame, Regier, Tom, McKinley, Gareth H, Shao-Horn, Yang, Massachusetts Institute of Technology. Research Laboratory of Electronics, Massachusetts Institute of Technology. Department of Mechanical Engineering, Massachusetts Institute of Technology. Department of Materials Science and Engineering, Zhu, Yun Guang, Narayanan, Thaneer Malai, Tulodziecki, Michal, Sanchez-Casalongue, Hernan, Horn, Quinn C., Meda, Laura, Yang, Yu, Sun, Jame, Regier, Tom, McKinley, Gareth H, and Shao-Horn, Yang

Abstract

Flow battery technology offers a promising low-cost option for stationary energy storage applications. Aqueous zinc–nickel battery chemistry is intrinsically safer than non-aqueous battery chemistry (e.g. lithium-based batteries) and offers comparable energy density. In this work, we show how combining high power density and low-yield stress electrodes can minimize energy loss due to pumping, and have demonstrate methods to achieve high energy and power density for ZnO/Ni(OH)2 electrodes by changing composition and optimizing testing protocols. Firstly, mechanically stable and homogeneous Ni(OH)2/carbon and ZnO/Zn flowable electrodes in 7 M KOH electrolyte were designed using a microgel dispersion as the suspending matrix. By determining the critical volume fractions for conductivity percolation, colloidal suspensions with 6.2 vol% of carbon and 23.1 vol% of Zn were selected for preparing catholytes and anolytes to ensure that these semi-solid electrodes possess high voltage and high coulombic efficiencies. The resulting flowable electrodes exhibited non-Newtonian rheology with a yield stress of approximately ∼200 Pa, which assists in maintaining mechanical stability of the suspensions. An energy density of up to 134 W h Lcatholyte−1 and power density up to ∼159 mW cmgeo.−2 was demonstrated for semi-solid ZnO/Ni(OH)2 electrodes, and coulombic efficiency of 94% was achieved during cycling by optimizing the charging protocol to 60% SOC of Ni(OH)2. Lastly, semi-solid ZnO and Ni(OH)2 flow cells were built and tested using an intermittent mode of operation. The high energy and power densities, high coulombic efficiency, and negligible pumping loss of the Zn–Ni semi-solid electrodes developed in the present work present a promising system for further development.

Published
2020

15. Catalyst engineering for lithium ion batteries: The catalytic role of Ge in enhancing the electrochemical performance of SnO2(GeO2)0.13/G anodes

Author

Zhu, Yun Guang, Wang, Ye, Han, Zhao, Shi, Yumeng, Wong, Jen It, Huang, Zhi Xiang, Ostrikov, Ken, Yang, Hui, Zhu, Yun Guang, Wang, Ye, Han, Zhao, Shi, Yumeng, Wong, Jen It, Huang, Zhi Xiang, Ostrikov, Ken, and Yang, Hui

Abstract

The catalytic role of germanium (Ge) was investigated to improve the electrochemical performance of tin dioxide grown on graphene (SnO(2)/G) nanocomposites as an anode material of lithium ion batteries (LIBs). Germanium dioxide (GeO(20) and SnO(2) nanoparticles (<10 nm) were uniformly anchored on the graphene sheets via a simple single-step hydrothermal method. The synthesized SnO(2)(GeO(2))0.13/G nanocomposites can deliver a capacity of 1200 mA h g(-1) at a current density of 100 mA g(-1), which is much higher than the traditional theoretical specific capacity of such nanocomposites (∼ 702 mA h g(-1)). More importantly, the SnO(2)(GeO(2))0.13/G nanocomposites exhibited an improved rate, large current capability (885 mA h g(-1) at a discharge current of 2000 mA g(-1)) and excellent long cycling stability (almost 100% retention after 600 cycles). The enhanced electrochemical performance was attributed to the catalytic effect of Ge, which enabled the reversible reaction of metals (Sn and Ge) to metals oxide (SnO(2) and GeO(2)) during the charge/discharge processes. Our demonstrated approach towards nanocomposite catalyst engineering opens new avenues for next-generation high-performance rechargeable Li-ion batteries anode materials.

Published
2014

16. Molecular Design of Stable Sulfamide- and Sulfonamide-based Electrolytes for Aprotic Li-O 2 Batteries.

Author

Feng S, Huang M, Lamb JR, Zhang W, Tatara R, Zhang Y, Zhu YG, Perkinson CF, Johnson JA, and Shao-Horn Y

Abstract

Electrolyte instability is one of the most challenging impediments to enabling Lithium-Oxygen (Li-O 2 ) batteries for practical use. The use of physical organic chemistry principles to rationally design new molecular components may enable the discovery of electrolytes with stability profiles that cannot be achieved with existing formulations. Here, we report on the development of sulfamide- and sulfonamide-based small molecules that are liquids at room temperature, capable of dissolving reasonably high concentration of Li salts (e.g., LiTFSI), and are exceptionally stable under the harsh chemical and electrochemical conditions of aprotic Li-O 2 batteries. In particular, N , N -dimethyl-trifluoromethanesulfonamide was found to be highly resistant to chemical degradation by peroxide and superoxide, stable against electrochemical oxidation up to 4.5 V Li , and stable for > 90 cycles in a Li-O 2 cell when cycled at < 4.2 V Li . This study provides guiding principles for the development of next-generation electrolyte components based on sulfamides and sulfonamides.

Published
2019
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