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In Situ Formation of Bifunctional Interlayer on 3D Conductive Scaffold for Dendrite Free Li Metal Batteries
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  • Yonghwan Kim,
  • Dohyeong Kim,
  • Minjun Bae,
  • Yujin Chang,
  • Won Young An,
  • Hwichan Hong,
  • Seon Jae Hwang,
  • Dongwan Kim,
  • Jeongyeon Lee,
  • Yuanzhe Piao
Yonghwan Kim
Seoul National University
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Dohyeong Kim
Seoul National University
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Minjun Bae
Seoul National University
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Yujin Chang
Seoul National University
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Won Young An
Seoul National University
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Hwichan Hong
Seoul National University
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Seon Jae Hwang
Seoul National University
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Dongwan Kim
Seoul National University
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Jeongyeon Lee
Seoul National University
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Yuanzhe Piao
Seoul National University

Corresponding Author:[email protected]

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Abstract

Regulating lithium (Li) plating/stripping behavior in three-dimensional (3D) conductive scaffolds is critical to stabilize Li metal batteries (LMBs). Surface protrusions and roughness in these scaffolds can induce uneven distributions of the electric fields and ionic concentrations, forming ’hot spots’. Hot spots may cause uncontrollable Li dendrites growth, presenting significant challenges to the cycle stability and safety of LMBs. To address these issues, we construct a Li ionic conductive-dielectric gradient bifunctional interlayer (ICDL) onto 3D Li-injected graphene/carbon nanotube scaffold (LGCF) via in situ reaction of exfoliated hexagonal boron nitride (fhBN) and molten Li. Microscopic and spectroscopic analyses reveal that ICDL consists of fhBN-rich outer layer and inner layer enriched with Li3N and Li-boron composites (Li-B). The outer layer utilizes dielectric properties to effectively homogenize the electric field, while the inner layer ensures high Li ion conductivity. Moreover, DFT calculations indicate that ICDL can effectively adsorb Li and decrease the Li diffusion barrier, promoting enhanced Li ion transport. The modulation of Li kinetics by ICDL increases the critical length of the Li nucleus, enabling suppression of Li dendrite growth. Attributing to these advantages, the ICDL coated LGCF (ICDL@LGCF) demonstrates impressive long term cycle performances in both symmetric cells and full cells.
06 Aug 2024Submitted to Energy & Environmental Materials
11 Aug 2024Submission Checks Completed
11 Aug 2024Assigned to Editor
11 Aug 2024Review(s) Completed, Editorial Evaluation Pending
16 Aug 2024Reviewer(s) Assigned
02 Sep 2024Editorial Decision: Revise Major
28 Oct 20241st Revision Received
30 Oct 2024Submission Checks Completed
30 Oct 2024Assigned to Editor
30 Oct 2024Review(s) Completed, Editorial Evaluation Pending
31 Oct 2024Reviewer(s) Assigned
07 Nov 2024Editorial Decision: Accept