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Dual additives for stabilizing Li deposition and SEI formation in anode-free Li metal batteries
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  • Baolin Wu,
  • Chunguang Chen,
  • Dmitri Danilov,
  • Zhiqiang Chen,
  • Ming Jiang,
  • Rüdiger-A. Eichel,
  • Peter Notten
Baolin Wu
Forschungszentrum Jülich GmbH
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Chunguang Chen
Chinese Academy of Sciences Institute of Mechanics
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Dmitri Danilov
Eindhoven University of Technology
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Zhiqiang Chen
Eindhoven University of Technology
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Ming Jiang
Hangzhou Dianzi University College of Electronics and Information
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Rüdiger-A. Eichel
Forschungszentrum Jülich GmbH
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Peter Notten
Eindhoven University of Technology

Corresponding Author:p.h.l.notten@tue.nl

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Abstract

Anode-free Li-metal batteries (AFLBs) are of significant interest to energy storage industries due to their intrinsically high energy. However, the accumulative Li dendrites and dead Li continuously consume active Li during cycling. That results in a short lifetime and low Coulombic efficiency (CE) of AFLBs. Introducing effective electrolyte additives can improve the Li deposition homogeneity and solid-state interphase (SEI) stability for AFLBs. Herein, we reveal that introducing dual additives, composed of LiAsF6 and FEC, into a commercial carbonate electrolyte will boost the cycle life and average CE of NCM||Cu AFLBs. The NCM||Cu AFLBs with the dual additives exhibit a capacity retention of about 75% after 50 cycles, much higher than those with bare electrolytes (35%). The average CE of the NCM||Cu AFLBs with additives can maintain 98.3% over 100 cycles. In contrast, the average CE without additives rapidly decline to 97% after only 50 cycles. In situ Raman measurements reveal that the prepared dual additives facilitate denser and smoother Li morphology during Li deposition. The dual additives significantly suppress the Li dendrite growth, enabling stable SEI formation on anode and cathode surfaces. Our results provide a broad view of developing low-cost and high-effective functional electrolytes for high-energy and long-life AFLBs.
15 Feb 2023Submitted to Energy & Environmental Materials
16 Feb 2023Submission Checks Completed
16 Feb 2023Assigned to Editor
19 Feb 2023Review(s) Completed, Editorial Evaluation Pending
19 Feb 2023Reviewer(s) Assigned
13 Mar 2023Editorial Decision: Revise Major
16 Mar 20231st Revision Received
17 Mar 2023Assigned to Editor
17 Mar 2023Submission Checks Completed
17 Mar 2023Review(s) Completed, Editorial Evaluation Pending
23 Mar 2023Reviewer(s) Assigned
26 Apr 2023Editorial Decision: Revise Minor
29 Apr 20232nd Revision Received
30 Apr 2023Assigned to Editor
30 Apr 2023Submission Checks Completed
30 Apr 2023Review(s) Completed, Editorial Evaluation Pending
01 May 2023Editorial Decision: Accept