<sup>7</sup>Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries

Marbella, Lauren E.; Zekoll, Stefanie; Kasemchainan, Jitti; Emge, Steffen P.; Bruce, Peter G.; Grey, Clare P.

doi:10.1021/acs.chemmater.8b04875

Cited by 112 publications

(100 citation statements)

References 25 publications

Supporting

Mentioning

100

Contrasting

Order By: Relevance

“…Figure S7 (Supporting Information) depicts that after the cycling tests, the cell impedance still consists of two distinct arcs, similar to that before the tests, which confirms that no shorting takes place after the cycling test. Moreover, after cycling tests, the cell impedance decreases, which is related to the locally formed lithium on the Li/LLZT interface or within the LLZT pellets during the stripping–plating process and agrees with previous literature 1g,11a,20f,25. In Figure d and Figure S8 (Supporting Information), the long‐term stability of the Li/LLZT interface is tested by cycling the symmetric Li r /LLZT/Li r cell at ±2.2 mA cm −2 with a capacity of 0.88 mAh cm −2 and at ±0.1 mA cm −2 with a capacity of 0.06 mAh cm −2 for 80 and 950 h, respectively.…”

Section: Resultsmentioning

confidence: 99%

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Zheng

Tian

et al. 2019

Adv Funct Materials

128

View full text Add to dashboard Cite

Solid-state lithium batteries are widely considered as next-generation lithiumion battery technology due to the potential advantages in safety and performance. Among the various solid electrolyte materials, Li-garnet electrolytes are promising due to their high ionic conductivity and good chemical and electrochemical stabilities. However, the high electrode/electrolyte interfacial impedance is one of the major challenges. Moreover, short circuiting caused by lithium dendrite formation is reported when using Li-garnet electrolytes. Here, it is demonstrated that Li-garnet electrolytes wet well with lithium metal by removing the intrinsic impurity layer on the surface of the lithium metal. The Li/garnet interfacial impedance is determined to be 6.95 Ω cm 2 at room temperature. Lithium symmetric cells based on the Li-garnet electrolytes are cycled at room temperature for 950 h and current density as high as 13.3 mA cm −2 without showing signs of short circuiting. Experimental and computational results reveal that it is the surface oxide layer on the lithium metal together with the garnet surface that majorly determines the Li/garnet interfacial property. These findings suggest that removing the superficial impurity layer on the lithium metal can enhance the wettability, which may impact the manufacturing process of future high energy density garnet-based solid-state lithium batteries. are gratefully acknowledged for assisting with relevant experimental analysis. Center for High Performance Computing of SJTU is gratefully acknowledged for providing computational facilities for all the simulations. Conflict of InterestThe authors declare no conflict of interest.

show abstract

Section: Resultsmentioning

confidence: 99%

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Zheng

Tian

et al. 2019

Adv Funct Materials

128

View full text Add to dashboard Cite

show abstract

“…[88] Morphologically, lithium dendrites were always observed at specific spots on garnet surface ( Figure 6A), and preferentially existed along the cracks, open pores, and grain boundaries in bulk garnet ( Figure 6B-D). [89][90][91][92] In addition, Figure 6. Lithium dendrite in solid electrolyte.…”

Section: Lithium Dendritementioning

confidence: 99%

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Wang

Zhu

et al. 2020

Advanced Energy Materials

View full text Add to dashboard Cite

liquid electrolytes. ASSLBs exhibit overwhelming advantages as follows: 1) No electrolyte leakage. The most obvious advantage of ASSLBs is the avoidance of electrolyte leakage, and related issues such as fire hazard, electrical short circuit and corruption. In addition, ASSLBs do not need advance sealants, pressurizing electrolyte, and flame retardant failsafe. [1,2] 2) No thermal runaway. Thermal runaway will cause the rise of internal temperature, pressure, and vent of flammable gases in conventional LIBs, at a risk of explosion and shrapnel. [3,4] ASSLBs avoid the use of organic electrolytes and prevent the thermal runaway for a large extent. [5] 3) High resistance to lithium dendrite. The lithium dendrite may form during deposition process and penetrate through the separator, potentially cause a short circuit in conventional LIBs. [6] ASSLBs using solid electrolytes (SEs) with high shear modulus are expected to prevent/alleviate the dendrite penetration and extend the cell life. 4) Higher energy density. [7] The conventional LIBs are not suitable for the application of high voltage cathode and lithium metal anode because of narrow electrochemical window of liquid electrolytes, as well as failure in preventing lithium dendrite. ASSLBs facilitate the application of high voltage cathode materials and high energy density lithium metal anode, therefore increasing the energy density of the whole cell. Figure 1 shows the scheme of a typical ASSLB. Similar with conventional LIBs, the main components of ASSLB are cathode, SE, and anode. The distinctive component is SE, and its properties support the great advantages of ASSLBs. These properties include stability at ultrahigh and ultralow temperature, high mechanical strength, [8] wider electrochemical window (with passivation), and so on. [9-11] According to the category of SE, ASSLBs are divided into polymer-based, oxide-based, and sulfide-based systems, corresponding to the polymer, oxide, and sulfide electrolytes, respectively. Therein, oxide electrolytes exhibit moderate ionic conductivity, high shear modulus, and better stability with atmosphere and electrodes, are promising candidates for ASSLB. Specifically, oxide electrolytes are classified into LISICON (Li 14 ZnGe 4 O 16), NASICION (LiTi 2 (PO 4) 3), perovskite (Li 3x La 0.67-x □ 0.33-2x TiO 3), garnet (Li 3-7 LnMO 12 , Ln = Y, Pr, Nd, La, Sm-Lu, M = Zr, Sb, W, etc.), and so on based on their structure. Without reductive Ge, Ti elements in the composition, garnets are normally considered most promising among oxide electrolytes. [12,13] Garnet-type electrolytes in the formula of Li 3-7 Ln 3 M 2 O 12 , show a space group 3 Ia d. Lithium content ranges from 3 to 7 based on the substitution elements at Ln and M sites. [14,15] All-solid-state lithium batteries (ASSLBs) are considered to be the nextgeneration energy storage system, because of their overwhelming advantages in energy density and safety compared to conventional lithium ion batteries. Among various systems, garnet-based ASSLBs are one of the most promis...

show abstract

“…[ 81 ] MRI is sensitive to ion concentration and element distribution, [ 82 ] which is also utilized to characterize the state of charge (SOC) of battery. [ 83 ] Marbella et al [ 84 ] tracked Li microstructural growth in the garnet‐type solid electrolyte Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 in the early stage ( Figure ), and attributed inhomogeneous Li stripping/plating in Li–LLZTO–Li cells to the microstructural Li, which ultimately leads to dendrite growth with increasing cycle time.…”

Section: Characterization Techniques For Interface In All‐solid‐statementioning

confidence: 99%

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Gao

et al. 2020

Small Methods

View full text Add to dashboard Cite

The interface is a critical factor of electrochemical performance for all‐solid‐state batteries (ASSBs). Comprehending the composition, structure, morphology, and their evolution in the interface during charge/discharge cycling is greatly important for the development and practical application of ASSBs. The characterization techniques are very crucial and powerful for investigating the interface properties of ASSBs. This review briefly describes how the interface is generated in ASSBs, and then emphatically summarizes some important advanced techniques used to characterize the interface in ASSBs. The principle, advantage, and application of the techniques in the interface investigation are systematically discussed. This review provides fundamental insights and perspectives for developing the characterization techniques to deeply understand the interfacial behaviors of ASSBs, which is valuable for accelerating the commercialization of ASSBs used in electronic devices, electric vehicles, and large‐scale energy storage.

show abstract

⁷Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries

Cited by 112 publications

References 25 publications

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Contact Info

Product

Resources

About

7Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries

Cited by 112 publications

References 25 publications

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Intrinsic Lithiophilicity of Li–Garnet Electrolytes Enabling High‐Rate Lithium Cycling

Interfaces in Garnet‐Based All‐Solid‐State Lithium Batteries

Advanced Characterization Techniques for Interface in All‐Solid‐State Batteries

Contact Info

Product

Resources

About

⁷Li NMR Chemical Shift Imaging To Detect Microstructural Growth of Lithium in All-Solid-State Batteries