Constructing Li‐Rich Artificial SEI Layer in Alloy–Polymer Composite Electrolyte to Achieve High Ionic Conductivity for All‐Solid‐State Lithium Metal Batteries

Liu, Yuxuan; Hu, Renzong; Zhang, De-Chao; Liu, Jiangwen; Liu, Fang; Cui, Jie; Lin, Zuopeng; Wu, Jinsong; Zhu, Min

doi:10.1002/adma.202004711

Cited by 99 publications

(74 citation statements)

References 72 publications

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“…h) Comparison of ASSLBs using PEO‐based electrolytes reported recently in the open literature. [ 47–51 ] Note that the batteries for comparison are assembled in coin cells otherwise specified.…”

Section: Resultsmentioning

confidence: 99%

“…Moreover, due to the reinforcement of the robust fiber network, an ultrathin solid electrolyte with a thickness of 17 µm is obtained with improved mechanical strength for dendrite suppression. [47][48][49][50][51] Note that the batteries for comparison are assembled in coin cells otherwise specified.…”

Section: Discussionmentioning

confidence: 99%

“…Demonstration of the I-FPG pouch cell: d) Voltage profiles and e) cycling performance of the pouch cell at 0.3 C under 60 °C; photographs of the pouch cell powering an electronic device f) when bending and g) after cutting. h) Comparison of ASSLBs using PEO-based electrolytes reported recently in the open literature [47][48][49][50][51]. Note that the batteries for comparison are assembled in coin cells otherwise specified.…”

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confidence: 99%

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A High‐Capacity, Long‐Cycling All‐Solid‐State Lithium Battery Enabled by Integrated Cathode/Ultrathin Solid Electrolyte

Lin

Sun

et al. 2021

Advanced Energy Materials

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flammable organic liquid electrolytes to solid-state electrolytes not only endows all-solid-state lithium batteries (ASSLBs) with considerable improvements in battery safety, but also potentially allows the use of Li metal anode, which is regarded as the ultimate anode due to its high theoretical specific capacity (3860 mAh g -1 ) and low electrochemical potential (−3.04 V versus standard hydrogen electrode). [3][4][5][6][7] Thus, ASSLBs have been widely exploited as next-generation energy storage technologies with enhanced energy density and safety. [8] However, current ASSLBs are far from competitive with commercial LIBs in terms of battery performance and ease of manufacturing. [9,10] This is because conventional ASSLB assembly requires laborious fabrication of solid electrolyte and electrodes separately, followed by stacking each component together, which inevitably results in poor interfacial contact. [11,12] Radically different from LIBs, solid electrolyte in ASSLBs cannot spontaneously wet the electrodes as liquid electrolyte does, leading to discontinuous ion transport at the cathode/solid electrolyte interfaces and inside the porous cathode, which results in a large interfacial resistance and low active material utilization. [13] As a consequence, the mass loading of most reported ASSLBs is too low (usually <4 mg cm -2 ) to meet the requirement for practical energy-dense batteries. [14] In addition, due to unfavorable mechanical properties, typical solid electrolytes need to be fabricated to be overly thick as a way of ensuring their integrity under unavoidable stress during conventional cell assembly processes. [9,15] For instance, pure ceramic solid electrolytes are generally too brittle to be produced with a thickness less than 100 µm. [16,17] Although blending the ceramics with polymers can endow the composite solid electrolyte with good flexibility, it is still challenging to reduce the thickness to be comparable with that of separators (usually <30 µm) in current LIBs, which, as a result, considerably sacrifices the battery energy density. [15,18] Even worse, the inferior mechanical strength of solid electrolytes renders a poor Li dendrite suppression capability, resulting in poor cyclability of the battery. [19] These limitations of conventional ASSLB manufacturing impose a great penalty on the attainable energy density and cyclability of the battery.To address these issues, several strategies have been developed for ASSLBs. For instance, Hu et al. reported on a dense/ porous bilayer garnet electrolyte, where the porous layer served Current all-solid-state lithium battery (ASSLB) manufacturing typically involves laborious fabrication and assembly of individual electrodes and solid electrolyte, which inevitably result in large interfacial resistances. Moreover, due to the unfavorable mechanical strength, most solid electrolytes are fabricated to be overly thick and are incapable of retarding lithium dendrite formation. These factors limit the attainable energy density and cyclability of ASSLBs. Her...

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Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

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confidence: 99%

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A High‐Capacity, Long‐Cycling All‐Solid‐State Lithium Battery Enabled by Integrated Cathode/Ultrathin Solid Electrolyte

Lin

Sun

et al. 2021

Advanced Energy Materials

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“…The Li + transference number ( t Li+ ) has been used as a significant parameter to analyze the influence on Li + transport by interfacial engineering and electrolyte design to deal with troublesome dendritic Li deposition. [ 35 ] It can be obtained by the potentiostatic polarization method pioneered by Bruce and co‐workers [ 36 ] and calculated according to Equation (S1) (Supporting Information). The t Li+ increased from 0.22 for bare Li to 0.37 for LSIF (calculated from Figure 3b,c, and Table S1, Supporting Information), which was mainly ascribed to the increased ion pair (Li + and TFSI – ) dissociation and the fraction of free Li + induced by interaction of the Li salt with the prelithiated LSIF.…”

Section: Resultsmentioning

confidence: 99%

Porous Lithiophilic Li–Si Alloy‐Type Interfacial Framework via Self‐Discharge Mechanism for Stable Lithium Metal Anode with Superior Rate

Park

Choi

et al. 2021

Advanced Energy Materials

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Lithium is regarded as an ideal anode for next‐generation Li metal batteries (LMB) as it exhibits extraordinarily high theoretical capacity and the lowest electrochemical potential among all anode candidates. However, safety concerns and poor cycling stability of Li induced by uncontrollable dendrite growth and severe side reactions impede its practical application for LMB. Although various strategies for fabricating Li anodes have been suggested, developing high‐rate LMB remains a significant challenge. To address this challenge, the use of a 3D porous Li–Si alloy‐type interfacial framework (LSIF) created via a “self‐discharge” mechanism with the aid of an electrolyte is proposed here. Exploiting the in situ spontaneous prelithiation, lithiophilic Li15Si4 particles are homogenously arranged to build porous 3D LSIF. The balanced ionic/electronic conducting LSIF serves as a stable Li host, helping to suppress dendrite growth and volume expansion during cycling. The LSIF@Li anode possesses a strong affinity toward Li, rapid Li diffusion kinetics, and low nucleation/diffusion barriers. Moreover, the LSIF@Li symmetric cells are capable of stable cycling (over 1000 cycles) even at an ultrahigh current density (15 mA cm–2). When paired with LiNi0.5Co0.2Mn0.3O2 or LiFePO4, LSIF@Li full cells show improved rate capability and long‐term cycling stability (≈2000 cycles) at 10 C.

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“…We compared the rate performance of this work with the reported advanced SPEs in Fig. 5g 35,[44][45][46][47][48][49][50][51] . The strategy we proposed strongly enhances capacity retention at high current density with simple PEO-LiTFSI without any modi cations, better than other SPEs of complex design (details in Table S5).…”

Section: Performance With Insu Cient Ionic Conductivitymentioning

confidence: 99%

Expand the effective carriers in solid polymer electrolytes via anion-hosting cathode

Sun

Chen

et al. 2021

Preprint

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The non-reactive anion migration deteriorates the limited ionic conductivity of the solid polymer electrolytes (SPEs) and accelerates solid-state batteries failure. Here, we introduce an integrated approach in which polyvinyl ferrocene (PVF) cathode encourage anions and Li+ to act as effective carriers simultaneously. The concentration polarization and poor rate performance, caused by insufficient effective carriers, were addressed by the participation of anions in electrode reaction. Specifically, the PVF|Li battery matched with unmodified SPE (PEO-LiTFSI) showed 107 mAh g− 1 initial capacity at 100 µA cm− 2 and maintained 70% retention for more than 2800 cycles at 300 µA cm− 2 and 60°C. Moreover, the slight capacity decrease at 1000 µA cm− 2 and the successful batteries operation at minimal ionic conductivity (8.13×10− 6 S cm− 1) show that the current carrying capacity of SPEs was greatly improved without complex design. This strategy weakens the strict requirements for ion conductance and interface engineering of SPEs, and provides an efficient scenario for constructing advanced polymer-based all-solid-state batteries.

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Constructing Li‐Rich Artificial SEI Layer in Alloy–Polymer Composite Electrolyte to Achieve High Ionic Conductivity for All‐Solid‐State Lithium Metal Batteries

Cited by 99 publications

References 72 publications

A High‐Capacity, Long‐Cycling All‐Solid‐State Lithium Battery Enabled by Integrated Cathode/Ultrathin Solid Electrolyte

A High‐Capacity, Long‐Cycling All‐Solid‐State Lithium Battery Enabled by Integrated Cathode/Ultrathin Solid Electrolyte

Porous Lithiophilic Li–Si Alloy‐Type Interfacial Framework via Self‐Discharge Mechanism for Stable Lithium Metal Anode with Superior Rate

Expand the effective carriers in solid polymer electrolytes via anion-hosting cathode

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