Optimization of Magnesium‐Doped Lithium Metal Anode for High Performance Lithium Metal Batteries through Modeling and Experiment

Gao, Peiyuan; Wu, Haiping; Zhang, Xianhui; Jia, Hao; Kim, Ju‐Myung; Engelhard, Mark H.; Niu, Chaojiang; Xu, Zhijie; Zhang, Ji‐Guang; Xu, Wu

doi:10.1002/anie.202103344

Cited by 41 publications

(19 citation statements)

References 31 publications

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“…One effective solution towards the accumulation of inactive Li is to essentially regulate SEI to avoid the growth of dendritic Li. [9] In retrospect, numerous researches have anticipatively been focused on stabilizing SEI and suppressing Li dendrite growth, [10] which indirectly decrease the accumulation of inactive Li. [11] These strategies to some extent have successfully enabled the primary operation of LMBs for extended lifespans.…”

Section: Introductionmentioning

confidence: 99%

Reclaiming Inactive Lithium with a Triiodide/Iodide Redox Couple for Practical Lithium Metal Batteries

et al. 2021

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High-energy-density lithium (Li)m etal batteries suffer from as hort lifespan owing to apparently ceaseless inactive Li accumulation, which is accompanied by the consumption of electrolyte and active Li reservoir,s eriously deteriorating the cyclability of batteries.H erein, at riiodide/ iodide (I 3 À /I À )redox couple initiated by stannic iodide (SnI 4 )is demonstrated to reclaim inactive Li. The reduction of I 3 À converts inactive Li into soluble LiI, which then diffuses to the cathode side.T he oxidation of LiI by the delithiated cathode transforms cathode into the lithiation state and regenerates I 3 À ,r eclaiming Li ion from inactive Li. The regenerated I 3 À engages the further redox reactions.F urthermore,t he formation of Sn mitigates the corrosion of I 3 À on active Li reservoir sacrificially.I nw orking Li j Li-Ni 0.5 Co 0.2 Mn 0.3 O 2 batteries,t he accumulated inactive Li is significantly reclaimed by the reversible I 3 À /I À redox couple, improving the lifespan of batteries by twice.This work initiates ac reative solution to reclaim inactive Li for prolonging the lifespan of practical Li metal batteries.

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Section: Introductionmentioning

confidence: 99%

Reclaiming Inactive Lithium with a Triiodide/Iodide Redox Couple for Practical Lithium Metal Batteries

et al. 2021

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“…The lattice constant of the bcc phase calculated in this research is in perfect agreement with the experimental value ( a 0 = 3.49 Å). Also, the (100) plane proved to be the most stable lithium surface face by various groups employing DFT. − Thus, in the following, all the models in this research were based on the Li(100) surface. The slab model of the most stable Li(100) surface contains four atomic layers in thickness with two bottom layers fixed (Figure S1); a 4 × 4 supercell in the lateral plane is adopted in A2-Li and A5-Li models, and a 5 × 5 supercell is adopted in A8-Li and A10-Li models.…”

Section: Resultsmentioning

confidence: 99%

Lithiophilic Property of Artificial Alkoxides and Mercaptide Layers to Guide Uniform Li Nucleation for Stable Lithium Metal Anodes

et al. 2021

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The practical application of Li metal anodes is hindered by the uncontrollable growth of Li dendrites and low utilization of active Li. Construction of an organic artificial layer on the Li surface is demonstrated as one of the most effective ways to solve the above problems. However, the lithiophilic property of the organic artificial layer with electronegative functional groups and the influence on Li nucleation are poorly understood. Herein, we demonstrated that the organic artificial layer with electronegative O and S atoms could improve the lithiophilicity of the Li surface via both first principles calculations and experimental verifications, contributing to homogeneous Li deposition. Metallic Li surfaces with n-terminal alkoxides and mercaptides were established. The alkoxide-treated and mercaptide-treated Li surface exhibits lithiophilic properties with improved adsorption energies toward a Li atom. With the increase of carbon chain length, the lithiophilicity of alkoxide-treated Li increased. Specifically, the mercaptide-treated Li with a stable lattice structure exhibited a better electrochemical performance than alkoxide-treated Li. This work probes the lithiophilic property of the Li surface with O-containing and S-containing organic artificial layers and affords guidance to organic artificial layers for Li metal anodes.

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“…Moreover, the quantitative understanding of the deposition process is still challenging. Further theoretical simulations, for example, finite element modeling, are expected to provide a deeper understanding of the evolution of Li plating/stripping in host materials [ 109 – 113 ]. Porosity contributions and electrode thickness design.…”

Section: Conclusion and Perspectivementioning

confidence: 99%

Advances in the Emerging Gradient Designs of Li Metal Hosts

Guan

Liu

et al. 2022

Research

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Developing host has been recognized a potential countermeasure to circumvent the intrinsic drawbacks of Li metal anode (LMA), such as uncontrolled dendrite growth, unstable solid electrolyte interface, and infinite volume fluctuations. To realize proper Li accommodation, particularly bottom-up deposition of Li metal, gradient designs of host materials including lithiophilicity and/or conductivity have attracted a great deal of attention in recent years. However, a critical and specialized review on this quickly evolving topic is still absent. In this review, we attempt to comprehensively summarize and update the related advances in guiding Li nucleation and deposition. First, the fundamentals regarding Li deposition are discussed, with particular attention to the gradient design principles of host materials. Correspondingly, the progress of creating different gradients in terms of lithiophilicity, conductivity, and their hybrid is systematically reviewed. Finally, future challenges and perspective on the gradient design of advanced hosts towards practical LMAs are provided, which would provide a useful guidance for future studies.

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Optimization of Magnesium‐Doped Lithium Metal Anode for High Performance Lithium Metal Batteries through Modeling and Experiment

Cited by 41 publications

References 31 publications

Reclaiming Inactive Lithium with a Triiodide/Iodide Redox Couple for Practical Lithium Metal Batteries

Reclaiming Inactive Lithium with a Triiodide/Iodide Redox Couple for Practical Lithium Metal Batteries

Lithiophilic Property of Artificial Alkoxides and Mercaptide Layers to Guide Uniform Li Nucleation for Stable Lithium Metal Anodes

Advances in the Emerging Gradient Designs of Li Metal Hosts

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