scholarly journals Interfacial Barrier Free Organic-Inorganic Hybrid Electrolytes for All Solid-State Batteries

2020 ◽  
Author(s):  
Myeong Ju Lee ◽  
Dong Ok Shin ◽  
Ju Young Kim ◽  
Jimin Oh ◽  
Jumi Kim ◽  
...  

Abstract Organic-inorganic hybrid solid electrolytes (HSEs) are expected to overcome the inherent limitations of rigid fragile inorganic electrolytes for solid state batteries. Li-ion conductive filler such as garnet Li7La3Zr2O12 (LLZO) is proposed for the high performance of HSEs, unfortunately, which suffers from native surface layer resistance to Li-ion transport. Here we present highly conductive polyvinylidene fluoride (PVDF)-based HSEs incorporating LLZO fillers, whose resistive barriers are eliminated by dry etching. Our optimal composition of etched LLZO fillers (30 wt%) leads to ionic conductivity of 4.05 x 10-4 S cm-1, about two-fold improvement from non-etched counterpart. Li symmetric cells with etched fillers exhibit low interfacial resistance of 110 Ω cm2 and minimal overpotential of 46 mV. Moreover, high capacity of 79 mA h g-1 is highlighted at 4C, comparable or superior to liquid electrolyte or sulfide-based electrolyte devices. Interfacial environment in HSEs ideally modified for Li-ion transport is identified by 7Li NMR measurements.

Nanomaterials ◽  
2021 ◽  
Vol 11 (4) ◽  
pp. 946
Author(s):  
Qianyi Yang ◽  
Fuqiang Lu ◽  
Yulin Liu ◽  
Yijie Zhang ◽  
Xiujuan Wang ◽  
...  

Solid electrolytes with high Li-ion conductivity and electrochemical stability are very important for developing high-performance all-solid-state batteries. In this work, Li2(BH4)(NH2) is nanoconfined in the mesoporous silica molecule sieve (SBA-15) using a melting–infiltration approach. This electrolyte exhibits excellent Li-ion conduction properties, achieving a Li-ion conductivity of 5.0 × 10−3 S cm−1 at 55 °C, an electrochemical stability window of 0 to 3.2 V and a Li-ion transference number of 0.97. In addition, this electrolyte can enable the stable cycling of Li|Li2(BH4)(NH2)@SBA-15|TiS2 cells, which exhibit a reversible specific capacity of 150 mAh g−1 with a Coulombic efficiency of 96% after 55 cycles.


Author(s):  
Shi Wang ◽  
Xiang-Chun Li ◽  
Tao Cheng ◽  
Yuan-Yuan Liu ◽  
Qiange Li ◽  
...  

Covalent organic frameworks (COFs) with well-tailored channels have the potential to efficiently transport ions yet remain to be explored. The ion transport capability is generally limited due to the lack...


2020 ◽  
Vol 8 (37) ◽  
pp. 19603-19611
Author(s):  
Adam R. Symington ◽  
John Purton ◽  
Joel Statham ◽  
Marco Molinari ◽  
M. Saiful Islam ◽  
...  

Solid electrolytes for all-solid-state batteries are generating considerable research interest as a means to improving their safety, stability and performance.


2020 ◽  
Author(s):  
Liangbing Hu ◽  
Chunpeng Yang ◽  
Qisheng Wu ◽  
Weiqi Xie ◽  
Xin Zhang ◽  
...  

Abstract While solid-state batteries are tantalizing for achieving improved safety and higher energy density, solid ion conductors currently available fail to satisfy the rigorous requirements for battery electrolytes and electrodes. Inorganic ion conductors allow fast ion transport, but their rigid and brittle nature prevents good interfacial contact and impedes device integration and stability. Conversely, flexible polymeric ion conductors provide better interfacial compatibility and mechanical tolerance, but suffer from inferior ionic conductivity (< 10−5 S cm−1 at room temperature) due to the coupling of ion transport with the polymer chain motion1-3. In this work, we report a general design strategy for achieving one-dimensional (1D), high-performance polymer solid-state ion conductors through molecular channel engineering, which we demonstrate via Cu2+-coordination of cellulose nanofibrils. The cellulose nanofibrils by themselves are not ionic conductive; however, by opening the molecular channels between the cellulose chains through Cu2+ coordination we are able to achieve a Li-ion conductivity as high as 1.5×10−3 S cm−1 at room temperature—a record among all known polymer ion conductors. This improved conductivity is enabled by a unique Li+ hopping mechanism that is decoupled from the polymer segmental motion. Also benefitted from such decoupling, the cellulose-based ion conductor demonstrates multiple advantages, including a high transference number (0.78 vs. 0.2–0.5 in other polymers2), low activation energy (0.19 eV), and a wide electrochemical stability window (4.5 V) that accommodate both Li metal anode and high-voltage cathodes. Furthermore, we demonstrate this 1D ion conductor not only as a thin, high-conductivity solid-state electrolyte but also as an effective ion-conducting additive for the solid cathode, providing continuous ion transport pathways with a low percolation threshold, which allowed us to utilize the thickest LiFePO4 solid-state cathode ever reported for high energy density. This approach has been validated with other polymers and cations (e.g., Na+ and Zn2+) with record-high conductivities, offering a universal strategy for fast single-ion transport in polymer matrices, with significance that could go far beyond safe, high-performance solid-state batteries.


Joule ◽  
2020 ◽  
Vol 4 (6) ◽  
pp. 1311-1323 ◽  
Author(s):  
Zhu Cheng ◽  
Ming Liu ◽  
Swapna Ganapathy ◽  
Chao Li ◽  
Zhaolong Li ◽  
...  

Author(s):  
Yang Yang ◽  
Jie Cui ◽  
Hui-Juan Guo ◽  
Xi Shen ◽  
Yuan Yao ◽  
...  

Intensive understanding of the Li-ion transport mechanism in solid-state-electrolytes (SSEs) is crucial for the buildup of industrially scalable solid-state batteries. Here, we report the charge distribution near the electrode/SSEs interface...


2018 ◽  
Vol 6 (13) ◽  
pp. 5296-5303 ◽  
Author(s):  
Hany El-Shinawi ◽  
Anna Regoutz ◽  
David J. Payne ◽  
Edmund J. Cussen ◽  
Serena A. Corr

All solid-state batteries based on NASICON-type LiM2(PO4)3 electrolyte phases are highly promising owing to their high ionic conductivities and chemical stabilities.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Ming Liu ◽  
Chao Wang ◽  
Chenglong Zhao ◽  
Eveline van der Maas ◽  
Kui Lin ◽  
...  

AbstractA key challenge for solid-state-batteries development is to design electrode-electrolyte interfaces that combine (electro)chemical and mechanical stability with facile Li-ion transport. However, while the solid-electrolyte/electrode interfacial area should be maximized to facilitate the transport of high electrical currents on the one hand, on the other hand, this area should be minimized to reduce the parasitic interfacial reactions and promote the overall cell stability. To improve these aspects simultaneously, we report the use of an interfacial inorganic coating and the study of its impact on the local Li-ion transport over the grain boundaries. Via exchange-NMR measurements, we quantify the equilibrium between the various phases present at the interface between an S-based positive electrode and an inorganic solid-electrolyte. We also demonstrate the beneficial effect of the LiI coating on the all-solid-state cell performances, which leads to efficient sulfur activation and prevention of solid-electrolyte decomposition. Finally, we report 200 cycles with a stable capacity of around 600 mAh g−1 at 0.264 mA cm−2 for a full lab-scale cell comprising of LiI-coated Li2S-based cathode, Li-In alloy anode and Li6PS5Cl solid electrolyte.


Materials ◽  
2020 ◽  
Vol 13 (7) ◽  
pp. 1719 ◽  
Author(s):  
Qinghui Li ◽  
Chang Xu ◽  
Bing Huang ◽  
Xin Yin

NASICON-type solid electrolytes with excellent stability in moisture are promising in all-solid-state batteries and redox flow batteries. However, NASIOCN LiZr2(PO4)3 (LZP), which is more stable with lithium metal than the commercial Li1.3Al0.3Ti1.7(PO4)3, exhibits a low Li-ion conductivity of 10−6 S cm−1 because the fast conducting rhombohedral phase only exists above 50 °C. In this paper, the high-ionic conductive rhombohedral phase is stabilized by Y3+ doping at room temperature, and the hot-pressing technique is employed to further improve the density of the pellet. The dense Li1.1Y0.1Zr1.9(PO4)3 pellet prepared by hot-pressing shows a high Li-ion conductivity of 9 × 10−5 S cm−1, which is two orders of magnitude higher than that of LiZr2(PO4)3. The in-situ formed Li3P layer on the surface of Li1.1Y0.1Zr1.9(PO4)3 after contact with the lithium metal increases the wettability of the pellet by the metallic lithium anode. Moreover, the Li1.1Y0.1Zr1.9(PO4)3 pellet shows a relatively small interfacial resistance in symmetric Li/Li and all-solid-state Li-metal cells, providing these cells a small overpotential and a long cycling life.


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