Unfolding the Hidden Message of Anode-Free Lithium Metal Battery

2020 ◽  
Author(s):  
Chen-Jui Huang ◽  
Balamurugan Thirumalraj ◽  
Hsien-Chu Tao ◽  
Kassie Nigus Shitaw ◽  
Tesfaye Teka Hagos ◽  
...  

Abstract Lithium metal batteries (LMBs) have been revisited and gained great attention due to significantly mitigated formation of Li dendrite in the past decade. Recently, anode-free lithium metal batteries (AFLMBs) are proposed and have been studied intensively to potentially outperform LMBs due to higher energy density and reduced safety hazards since the absence of Li metal during the fabrication process of the cell. In general, researchers compare capacity retention, reversible capacity, or rate capability of the cells to study the electrochemical performance of batteries. However, evaluating the behavior of batteries from limited aspects would easily overlook other information hidden deep inside the meretricious results or even lead to misguided data interpretation. In this work, an integrated protocol combining different types of cell configuration is proposed and validated for the first time to unravel the concealed messages in LMBs and AFLMBs. Irreversible coulombic efficiency (irr-CE) from various contributions including reductive electrolyte decomposition, dead Li formation, 1st intrinsic irreversible capacity of a cathode, and the subsequent irreversible reactions at cathode containing oxidative electrolyte decomposition and cathode degradation upon cycling are successfully determined separately by the integrated protocol for the first time. The decrypted information obtained from the proposed protocol provides an insightful understanding of behaviors of LMBs and AFLMBs, which promotes their development for practical applications.

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Chen-Jui Huang ◽  
Balamurugan Thirumalraj ◽  
Hsien-Chu Tao ◽  
Kassie Nigus Shitaw ◽  
Hogiartha Sutiono ◽  
...  

AbstractAnode-free lithium metal batteries are the most promising candidate to outperform lithium metal batteries due to higher energy density and reduced safety hazards with the absence of metallic lithium anode during initial cell fabrication. In general, researchers report capacity retention, reversible capacity, or rate capability of the cells to study the electrochemical performance of anode-free lithium metal batteries. However, evaluating the behavior of batteries from limited aspects may easily overlook other information hidden deep inside the meretricious results or even lead to misguided data interpretation. In this work, we present an integrated protocol combining different types of cell configuration to determine various sources of irreversible coulombic efficiency in anode-free lithium metal cells. The decrypted information from the protocol provides an insightful understanding of the behaviors of LMBs and AFLMBs, which promotes their development for practical applications.


2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Tianyi Wang ◽  
Yanbin Li ◽  
Jinqiang Zhang ◽  
Kang Yan ◽  
Pauline Jaumaux ◽  
...  

Abstract The practical applications of lithium metal anodes in high-energy-density lithium metal batteries have been hindered by their formation and growth of lithium dendrites. Herein, we discover that certain protein could efficiently prevent and eliminate the growth of wispy lithium dendrites, leading to long cycle life and high Coulombic efficiency of lithium metal anodes. We contend that the protein molecules function as a “self-defense” agent, mitigating the formation of lithium embryos, thus mimicking natural, pathological immunization mechanisms. When added into the electrolyte, protein molecules are automatically adsorbed on the surface of lithium metal anodes, particularly on the tips of lithium buds, through spatial conformation and secondary structure transformation from α-helix to β-sheets. This effectively changes the electric field distribution around the tips of lithium buds and results in homogeneous plating and stripping of lithium metal anodes. Furthermore, we develop a slow sustained-release strategy to overcome the limited dispersibility of protein in the ether-based electrolyte and achieve a remarkably enhanced cycling performance of more than 2000 cycles for lithium metal batteries.


2019 ◽  
Vol 7 (40) ◽  
pp. 23173-23181 ◽  
Author(s):  
Zhaoshuai Zhang ◽  
Long Zhang ◽  
Yanyan Liu ◽  
Tingting Yang ◽  
Zhiwen Wang ◽  
...  

PO43−–ester interactions realize dendrite-free Li deposition in PCL–LAGP, evidenced by galvanostatic cycling and in situ TEM observations. The corresponding battery achieves high coulombic efficiency ∼100% and a rate capability ≥10C.


2021 ◽  
Vol 13 (1) ◽  
Author(s):  
Lei Zheng ◽  
Feng Guo ◽  
Tuo Kang ◽  
Yingzhu Fan ◽  
Wei Gu ◽  
...  

AbstractLithium metal is regarded as the ultimate negative electrode material for secondary batteries due to its high energy density. However, it suffers from poor cycling stability because of its high reactivity with liquid electrolytes. Therefore, continuous efforts have been put into improving the cycling Coulombic efficiency (CE) to extend the lifespan of the lithium metal negative electrode. Herein, we report that using dual-salt additives of LiPF6 and LiNO3 in an ether solvent-based electrolyte can significantly improve the cycling stability and rate capability of a Li-carbon (Li-CNT) composite. As a result, an average cycling CE as high as 99.30% was obtained for the Li-CNT at a current density of 2.5 mA cm–2 and an negative electrode to positive electrode capacity (N/P) ratio of 2. The cycling stability and rate capability enhancement of the Li-CNT negative electrode could be attributed to the formation of a better solid electrolyte interphase layer that contains both inorganic components and organic polyether. The former component mainly originates from the decomposition of the LiNO3 additive, while the latter comes from the LiPF6-induced ring-opening polymerization of the ether solvent. This novel surface chemistry significantly improves the CE of Li negative electrode, revealing its importance for the practical application of lithium metal batteries.


2020 ◽  
Author(s):  
Kehua Dai ◽  
Jing Mao ◽  
Zengqing Zhuo ◽  
Guo Ai ◽  
Wenfeng Mao ◽  
...  

<div>Lattice oxygen redox reactions (ORR) offers opportunities for developing highcapacity batteries, however, suffers the notoriously high voltage hysteresis and low initial coulombic efficiency, which hinder its practical applications. Particularly, ORR was widely considered inherent to these kinetic issues. In this paper, unambiguous evidence of strong and reversible ORR is found in Na<sub>2/3</sub>Ni<sub>1/3</sub>Mn<sub>2/3</sub>O<sub>2</sub>, which displays negligible voltage hysteresis (0.1 V) and high initial coulombic efficiency with a highly stable electrochemical profile. Our independent and quantitative analysis of all the Ni, Mn and O states consistently interpret the redox mechanism of Na<sub>2/3</sub>Ni<sub>1/3</sub>Mn<sub>2/3</sub>O<sub>2</sub>, which reveals, for the first time, a conventional 3d transition-metal ORR system with facile kinetics and highly stable electrochemical profile that previously found only in cationic redox systems.</div>


2013 ◽  
Vol 1540 ◽  
Author(s):  
Chia-Yi Lin ◽  
Chien-Te Hsieh ◽  
Ruey-Shin Juang

ABSTRACTAn efficient microwave-assisted polyol (MP) approach is report to prepare SnO2/graphene hybrid as an anode material for lithium ion batteries. The key factor to this MP method is to start with uniform graphene oxide (GO) suspension, in which a large amount of surface oxygenate groups ensures homogeneous distribution of the SnO2 nanoparticles onto the GO sheets under the microwave irradiation. The period for the microwave heating only takes 10 min. The obtained SnO2/graphene hybrid anode possesses a reversible capacity of 967 mAh g-1 at 0.1 C and a high Coulombic efficiency of 80.5% at the first cycle. The cycling performance and the rate capability of the hybrid anode are enhanced in comparison with that of the bare graphene anode. This improvement of electrochemical performance can be attributed to the formation of a 3-dimensional framework. Accordingly, this study provides an economical MP route for the fabrication of SnO2/graphene hybrid as an anode material for high-performance Li-ion batteries.


2019 ◽  
Vol 55 (9) ◽  
pp. 1256-1258 ◽  
Author(s):  
Hieu Quang Pham ◽  
Eui-Hyung Hwang ◽  
Young-Gil Kwon ◽  
Seung-Wan Song

We report for the first time a promising approach to achieve the maximum capacity of LiNi0.8Co0.1Mn0.1O2 cathodes in a non-flammable electrolyte for safe and high-energy density lithium-ion and lithium metal batteries.


2019 ◽  
Vol 48 (28) ◽  
pp. 10422-10426 ◽  
Author(s):  
Xing Meng ◽  
Hai-Ning Wang ◽  
Yan-Hong Zou ◽  
Lu-Song Wang ◽  
Zi-Yan Zhou

POM-based metallogels are employed as anode materials for the first time, which exhibit high reversible capacity, high rate capability, and good cycling stability.


2020 ◽  
Vol 24 ◽  
pp. 336-342 ◽  
Author(s):  
Zhiyang Lyu ◽  
Gwendolyn J.H. Lim ◽  
Rui Guo ◽  
Zhenghui Pan ◽  
Xin Zhang ◽  
...  

Author(s):  
Dominik Steinle ◽  
Zhen Chen ◽  
Huu-Dat Nguyen ◽  
Matthias Kuenzel ◽  
Cristina Iojoiu ◽  
...  

AbstractPolymer-based electrolytes potentially enable enhanced safety and increased energy density of lithium-metal batteries employing high capacity, transition metal oxide–positive electrodes. Herein, we report the investigation of lithium-metal battery cells comprising Li[Ni0.6Mn0.2Co0.2]O2 as active material for the positive electrode and a poly(arylene ether sulfone)-based single-ion conductor as the electrolyte incorporating ethylene carbonate (EC) as selectively coordinating molecular transporter. The resulting lithium-metal battery cells provide very stable cycling for more than 300 cycles accompanied by excellent average Coulombic efficiency (99.95%) at an anodic cutoff potential of 4.2 V. To further increase the achievable energy density, the stepwise increase to 4.3 V and 4.4 V is herein investigated, highlighting that the polymer electrolyte offers comparable cycling stability, at least, as common liquid organic electrolytes. Moreover, the impact of temperature and the EC content on the rate capability is evaluated, showing that the cells with a higher EC content offer a capacity retention at 2C rate equal to 61% of the capacity recorded at 0.05 C at 60 °C.


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