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1. Lithium-ion intercalation by coupled ion-electron transfer

Author

Zhang, Yirui, primary, Fraggedakis, Dimitrios, additional, Gao, Tao, additional, Pathak, Shakul, additional, Zhuang, Debbie, additional, Grosu, Cristina, additional, Samantaray, Yash, additional, Neto, Armando R.C., additional, Duggirala, Sravani R., additional, Huang, Botao, additional, Zhu, Yun Guang, additional, Giordano, Livia, additional, Tatara, Ryoichi, additional, Agarwal, Harsh, additional, Stephens, Ryan M., additional, Bazant, Martin Z., additional, and Shao-Horn, Yang, additional

Published
2024
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11. 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

12. 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

13. 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

14. 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

15. 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

16. 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

24. 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

26. 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

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

Author

Xue, Weijiang, primary, Gao, Rui, additional, Shi, Zhe, additional, Xiao, Xianghui, additional, Zhang, Wenxu, additional, Zhang, Yirui, additional, Zhu, Yun Guang, additional, Waluyo, Iradwikanari, additional, Li, Yao, additional, Hill, Megan R., additional, Zhu, Zhi, additional, Li, Sa, additional, Kuznetsov, Oleg, additional, Zhang, Yiman, additional, Lee, Wah-Keat, additional, Hunt, Adrian, additional, Harutyunyan, Avetik, additional, Shao-Horn, Yang, additional, Johnson, Jeremiah A., additional, and Li, Ju, additional

Published
2021
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32. Six-Electron Reduction of LiIO3to LiOH in Aprotic Solvents and Implications for Li–O2Batteries

Author

Leverick, Graham, Zhu, Yun Guang, Lohmar, Sarah, Bardé, Fanny, Cotte, Stéphane, and Shao-Horn, Yang

Abstract

Batteries that leverage conversion reactions such as Li–O2batteries can offer increased gravimetric energy density over Li-ion batteries. Li–O2batteries with added LiI and H2O in the electrolyte that can form LiOH during discharge have been identified as potentially having high gravimetric energy density. Unfortunately, charging such Li–O2batteries can lead to the formation of parasitic LiIO3instead of O2, where the impact of LiIO3on the cycle life of Li–O2batteries is not known. In this work, we study the six-electron reduction of LiIO3to LiOH to elucidate whether parasitic LiIO3in Li–O2batteries can be electrochemically active during discharge, as well as to assess the viability of a battery chemistry based on the conversion of LiIO3to LiOH. Drop-cast LiIO3electrodes were shown to form LiOH on discharge with carbon electrodes at voltages of 2.1–2.6 VLiusing Raman spectroscopy and X-ray diffraction measurements. In addition, quantification using iodometric and acid–base titrations confirmed that the consumption of LiIO3and formation of LiOH during discharge was consistent with a six-electron reduction of LiIO3to LiOH. By studying the influence of solvent and water content on the discharge process, the overpotential during discharge was shown to linearly correlate with the logarithm of electrolyte viscosity divided by the solubility of LiIO3, which suggests that the discharge process was limited by the mass transport of soluble LiIO3. While LiIO3electrodes have shown high gravimetric energy densities up to ∼1550 W h/kgLiIO3/H2O_react, significant challenges remain to be overcome to increase the rate capability and cyclability of this chemistry.

Published
2022
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37. Interrogation of the Reaction Mechanism in a Na–O2Battery Using In SituTransmission Electron Microscopy

Author

Han, Shaobo, Cai, Chao, Yang, Fei, Zhu, Yuanmin, Sun, Qian, Zhu, Yun Guang, Li, Hui, Wang, Haijiang, Shao-Horn, Yang, Sun, Xueliang, and Gu, Meng

Abstract

Critical factors that govern the composition and morphology of discharge products are largely unknown for Na–O2batteries. Here we report a reversible oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) process in a sodium–oxygen battery observed using in situenvironmental-transmission electron microscopy (TEM) experiment. The reaction mechanism and phase evolution are probed using in situelectron diffraction and TEM imaging. The reversible ORR and OER cycling lies upon the nanosized copper clusters that were formed in situby sodiation of CuS. In situelectron diffraction revealed the formation of NaO2initially, which then disproportionated into orthorhombic and hexagonal Na2O2and O2. Na2O2was the major final ORR product that uniformly covered the whole wire-shape cathode. This uniform product morphology largely increased the application feasibility of Na–O2batteries in industry. In the following OER process, the Na2O2transformed to NaO2, which resulted in volume expansion at first, and then the NaO2decomposed to sodium ions and O2gas. Galvanostatic charge/discharge profiles of CuS in real Na–O2cells revealed a maximum capacity over 3 mAh cm–2with a discharge cutoff voltage of 1.8 V and high cycling stability. The nanosized copper catalyst plays a dominating role in controlling the morphology, chemical composition of discharge products, and reversibility of this Na–O2battery. Our finding shines light on the exploration of effective catalysts for the Na–O2battery.

Published
2020
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42. 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

48. High Specific-Capacity Al-Graphite Dual-Ion Batteries

Author

Zhu, Yun Guang, Fang, Jen-Hung, and Shao-Horn, Yang

Abstract

Rechargeable Al-graphite dual ion batteries are believed as a promising stationary energy storage system due to its low cost and long cycling life. Through engineering both Al and graphite electrodes using poly(vinylidene fluoride) and poly(vinylidene fluoride)-co-hexafluoropropylene (PVDF-HFP) copolymer as both binder and ionic network, Al-graphite batteries with high specific capacities and rate capabilities were demonstrated. We employed high-surface-area acetylene black (AB) as the substrate for Al plating to enhance the rate capability (up to 20 mA cm−2geo) and stability (>500 h) of Al plating/stripping. The utilization of graphite was increased by anchoring graphite particles in the PVDF-HFP ionic network. With these Al and graphite electrodes, Al-graphite dual ion batteries were shown to have a specific capacity of ∼140 mAh g−1Cat a current density of 186 mA g−1Cand high cycling stability (∼0.07% decay per cycle based on the fully activated capacity at 2.98 A g−1C). The 3D electrode design (Al negative and carbon positive electrode) with stable structure and high surface area can facilitate the development of the new Al-based battery chemistries (Al-Cl2, Al-Br2, and Al-O2, etc.).

Published
2023
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49. Dual redox catalysts for oxygen reduction and evolution reactions: towards a redox flow Li–O2 battery.

Author

Zhu, Yun Guang, Jia, Chuankun, Yang, Jing, Pan, Feng, Huang, Qizhao, and Wang, Qing

Subjects
*OXYGEN reduction, *OXYGEN evolution reactions, *LITHIUM cells, *OXIDATION-reduction reaction, *LITHIUM compounds, *CATHODES
Abstract

A redox flow lithium–oxygen battery (RFLOB) by using soluble redox catalysts with good performance was demonstrated for large-scale energy storage. The new device enables the reversible formation and decomposition of Li2O2via redox targeting reactions in a gas diffusion tank, spatially separated from the electrode, which obviates the passivation and pore clogging of the cathode. [ABSTRACT FROM AUTHOR]

Published
2015
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