Strategies towards enabling lithium metal in batteries: interphases and electrodes

Horstmann, Birger; Shi, Jiayan; Amine, Rachid; Werres, Martin; He, Xin; Jia, Hao; Hausen, Florian; Cekic‐Laskovic, Isidora; Wiemers‐Meyer, Simon; Lopez, Jeffrey; Galvez-Aranda, Diego E.; Baakes, Florian; Bresser, Dominic; Su, Chi‐Cheung; Xu, Yaobin; Xu, Wu; Jakes, Peter; Eichel, Rüdiger‐A.; Figgemeier, Egbert; Krewer, Ulrike; Seminario, Jorge M.; Balbuena, Perla B.; Wang, Chongmin; Passerini, Stefano; Shao‐Horn, Yang; Winter, Martin; Amine, Khalil; Kostecki, Robert; Latz, Arnulf

doi:10.1039/d1ee00767j

Cited by 175 publications

(190 citation statements)

References 235 publications

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“…As a result, larger overpotential would be needed to maintain a constant applied deposition current based on the Butler–Volmer equation, thereby leading to a progressively increasing overvoltage as presented in Fig. 2 e [ 51 ]. It is also remarkable that cells with the Na/In/C electrode can also deliver a long life span over 300 h at 1 and 2 mA cm −2 with a higher capacity of 3 mAh cm −2 as shown in Fig.…”

Section: Resultsmentioning

confidence: 99%

“…5 c) and Cl 2p spectra (Fig. 5 b), suggesting apparent enrichments of NaF and NaCl products in the SEI component [ 51 ]. The absence of F signal of the pure Na metal anode after 50 cycles can be largely attributed to the continuous breaking of SEI on the Na dendrite structures (Figs.…”

Section: Resultsmentioning

confidence: 99%

“…The absence of F signal of the pure Na metal anode after 50 cycles can be largely attributed to the continuous breaking of SEI on the Na dendrite structures (Figs. 4 a-c and S11a-f, S13), leading to the unnecessary consumption of electrolyte and thus causing ultralow contents of preferable NaF and –CF 3 [ 51 ]. Furthermore, it is apparent that peaks located at 441.3/441.6 and 449.2/449.8 eV (Fig.…”

Section: Resultsmentioning

confidence: 99%

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Fabricating Na/In/C Composite Anode with Natrophilic Na–In Alloy Enables Superior Na Ion Deposition in the EC/PC Electrolyte

Wang

et al. 2021

Nano-Micro Lett.

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In conventional ethylene carbonate (EC)/propylene carbonate (PC) electrolyte, sodium metal reacts spontaneously and deleteriously with solvent molecules. This significantly limits the practical feasibility of high-voltage sodium metal batteries based on Na metal chemistry. Herein, we present a sodium metal alloy strategy via introducing NaIn and Na2In phases in a Na/In/C composite, aiming at boosting Na ion deposition stability in the common EC/PC electrolyte. Symmetric cells with Na/In/C electrodes achieve an impressive long-term cycling capability at 1 mA cm−2 (> 870 h) and 5 mA cm−2 (> 560 h), respectively, with a capacity of 1 mAh cm−2. In situ optical microscopy clearly unravels a stable Na ion dynamic deposition process on the Na/In/C composite electrode surface, attributing to a dendrite-free and smooth morphology. Furthermore, theoretical simulations reveal intrinsic mechanism for the reversible Na ion deposition behavior with the composite Na/In/C electrode. Upon pairing with a high-voltage NaVPOF cathode, Na/In/C anode illustrates a better suitability in SMBs. This work promises an alternative alloying strategy for enhancing Na metal interfacial stability in the common EC/PC electrolyte for their future applications.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Fabricating Na/In/C Composite Anode with Natrophilic Na–In Alloy Enables Superior Na Ion Deposition in the EC/PC Electrolyte

Wang

et al. 2021

Nano-Micro Lett.

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“…[61] Therefore, the capacity fade for the control group cell is mainly attributed to the side reaction between Li-metal and the liquid electrolyte. [62][63][64][65] After cycling, we clearly observed the accumulation of residual SEI on the current collector surface (Figure S18, Supporting Information). In addition, LSnS/SBS-Li anode also experienced fast fading after 15 cycles as the protective layer was degraded over cycling (Figure S19, Supporting Information).…”

Section: Electrochemical Performancementioning

confidence: 99%

A Self‐Healable Sulfide/Polymer Composite Electrolyte for Long‐Life, Low‐Lithium‐Excess Lithium‐Metal Batteries

Ren

Cui

Bhargav

et al. 2021

Adv Funct Materials

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Solid electrolyte-protected lithium-metal anodes promise energy-dense, safe cells. While sulfide solid electrolytes enable facile processability and fast ion transport, they suffer from complex chemo-mechanical issues, including Li plating-induced fracture and Li stripping-induced contact loss. To address these issues, a grafting approach is implemented to functionalize the sulfide solid electrolyte (Li 3,85 Sn 0.85 Sb 0.15 S 4 ) with a self-healing unit. This leads to a dynamic bonding between the solid electrolyte network and a mechanically robust polymer scaffold, which reversibly accommodates the volume changes of the lithium-metal anode. Moreover, the approach improves the interfacial contact between the lithium-metal anode and the composite electrolyte, enabling stable cycling at a mild stack pressure (160 kPa). With a negative to positive capacity ratio equals to 1, pouch full cells with a high-nickel cathode (nickel content > 90%) and lithium-metal anode display 92% capacity retention for 140 cycles. Engineering the interface between solid electrolyte and the polymeric binder offers a promising pathway to address the chemomechanical issues.

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“…On the other hand, the design of three-dimensional (3D) porous structures as hosts for Li is particularly attractive because 3D structures can not only effectively regulate Li deposition but also accommodate the volume changes of the Li anode. [31][32][33][34][35] Crucially, the large surface area of 3D structures provides more electrochemical reaction sites, enables faster electron transfer, and lowers the areal current density. [35] This can reduce the overpotentials during Li plating/stripping process and is beneficial for stable Li deposition and the suppression of Li dendrite growth.…”

Section: Introductionmentioning

confidence: 99%

A 3D Porous Inverse Opal Ni Structure on a Cu Current Collector for Stable Lithium‐Metal Batteries

Jeong

Kim

et al. 2021

Batteries & Supercaps

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Lithium (Li) metal is considered the best anode material for next‐generation high‐energy density Li‐metal batteries. However, Li dendrite formation and growth hinder the practical applications of Li metal anodes. Herein, we report a three‐dimensional (3D) porous inverse opal nickel structure on a copper foil current collector (Ni IO@Cu) that has a controllable pore size and thickness and is fabricated via colloidal self‐assembly and electrodeposition. The uniform interconnected pores with a large surface area of the Ni IO@Cu structure can effectively dissipate high areal current densities, resulting in the stable formation of a solid electrolyte interface and dense, dendrite‐free, flat lithium deposits. In comparison to the use of bare Cu, the use of the Ni IO@Cu current collector resulted in greatly improved stability and lowered the voltage hysteresis in various Li plating/stripping tests. Moreover, Li‐ion battery and Li‐sulfur battery full cells prepared using the Ni IO@Cu also displayed excellent cycling performance. This work further demonstrates the significance of the 3D porous structure for preparing dendrite‐free Li metal anodes.

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Strategies towards enabling lithium metal in batteries: interphases and electrodes

Abstract: Perspective on recent improvements in experiment and theory towards realizing lithium metal electrodes with liquid electrolytes.

Cited by 175 publications

References 235 publications

Fabricating Na/In/C Composite Anode with Natrophilic Na–In Alloy Enables Superior Na Ion Deposition in the EC/PC Electrolyte

Fabricating Na/In/C Composite Anode with Natrophilic Na–In Alloy Enables Superior Na Ion Deposition in the EC/PC Electrolyte

A Self‐Healable Sulfide/Polymer Composite Electrolyte for Long‐Life, Low‐Lithium‐Excess Lithium‐Metal Batteries

A 3D Porous Inverse Opal Ni Structure on a Cu Current Collector for Stable Lithium‐Metal Batteries

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