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Title: Dendrite–Free Potassium Metal Anodes in a Carbonate Electrolyte

Abstract

Potassium (K) metal anodes suffer from a challenging problem of dendrite growth. In this study, it is demonstrated that a tailored current collector will stabilize the metal plating–stripping behavior even with a conventional KPF6–carbonate electrolyte. A 3D copper current collector is functionalized with partially reduced graphene oxide to create a potassiophilic surface, the electrode being denoted as rGO@3D–Cu. Potassiophilic versus potassiophobic experiments demonstrate that molten K fully wets rGO@3D–Cu after 6 s, but does not wet unfunctionalized 3D–Cu. Electrochemically, a unique synergy is achieved that is driven by interfacial tension and geometry: the adherent rGO underlayer promotes 2D layer–by–layer (Frank–van der Merwe) metal film growth at early stages of plating, while the tortuous 3D–Cu electrode reduces the current density and geometrically frustrates dendrites. The rGO@3D–Cu symmetric cells and half–cells achieve state–of–the–art plating and stripping performance. Here, the symmetric rGO@3D–Cu cells exhibit stable cycling at 0.1–2 mA cm–2, while baseline Cu prematurely fails when the current reaches 0.5 mA cm–2. The half–cells cells of rGO@3D–Cu (no K reservoir) are stable at 0.5 mA cm–2 for 10 000 min (100 cycles), and at 1 mA cm–2 for 5000 min. The baseline 3D–Cu, planar rGO@Cu, and planar Cu foil fails after 5110, 3012,more » and 1410 min, respectively.« less

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States)
  2. National Univ. of Singapore (Singapore)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Electricity (OE)
OSTI Identifier:
1606027
Alternate Identifier(s):
OSTI ID: 1580157; OSTI ID: 1634976
Report Number(s):
LA-UR-19-32524
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
AC05-00OR22725; SC0018074; 89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 7; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; lithium‐metal anodes; potassium ion batteries (PIBs/KIBs); potassium sulfur batteries; sodium‐metal anodes; solid electrolyte interphase (SEI); 36 MATERIALS SCIENCE; Material Science

Citation Formats

Liu, Pengcheng, Wang, Yixian, Gu, Qilin, Nanda, Jagjit, Watt, John Daniel, and Mitlin, David. Dendrite–Free Potassium Metal Anodes in a Carbonate Electrolyte. United States: N. p., 2019. Web. https://doi.org/10.1002/adma.201906735.
Liu, Pengcheng, Wang, Yixian, Gu, Qilin, Nanda, Jagjit, Watt, John Daniel, & Mitlin, David. Dendrite–Free Potassium Metal Anodes in a Carbonate Electrolyte. United States. https://doi.org/10.1002/adma.201906735
Liu, Pengcheng, Wang, Yixian, Gu, Qilin, Nanda, Jagjit, Watt, John Daniel, and Mitlin, David. Fri . "Dendrite–Free Potassium Metal Anodes in a Carbonate Electrolyte". United States. https://doi.org/10.1002/adma.201906735. https://www.osti.gov/servlets/purl/1606027.
@article{osti_1606027,
title = {Dendrite–Free Potassium Metal Anodes in a Carbonate Electrolyte},
author = {Liu, Pengcheng and Wang, Yixian and Gu, Qilin and Nanda, Jagjit and Watt, John Daniel and Mitlin, David},
abstractNote = {Potassium (K) metal anodes suffer from a challenging problem of dendrite growth. In this study, it is demonstrated that a tailored current collector will stabilize the metal plating–stripping behavior even with a conventional KPF6–carbonate electrolyte. A 3D copper current collector is functionalized with partially reduced graphene oxide to create a potassiophilic surface, the electrode being denoted as rGO@3D–Cu. Potassiophilic versus potassiophobic experiments demonstrate that molten K fully wets rGO@3D–Cu after 6 s, but does not wet unfunctionalized 3D–Cu. Electrochemically, a unique synergy is achieved that is driven by interfacial tension and geometry: the adherent rGO underlayer promotes 2D layer–by–layer (Frank–van der Merwe) metal film growth at early stages of plating, while the tortuous 3D–Cu electrode reduces the current density and geometrically frustrates dendrites. The rGO@3D–Cu symmetric cells and half–cells achieve state–of–the–art plating and stripping performance. Here, the symmetric rGO@3D–Cu cells exhibit stable cycling at 0.1–2 mA cm–2, while baseline Cu prematurely fails when the current reaches 0.5 mA cm–2. The half–cells cells of rGO@3D–Cu (no K reservoir) are stable at 0.5 mA cm–2 for 10 000 min (100 cycles), and at 1 mA cm–2 for 5000 min. The baseline 3D–Cu, planar rGO@Cu, and planar Cu foil fails after 5110, 3012, and 1410 min, respectively.},
doi = {10.1002/adma.201906735},
journal = {Advanced Materials},
number = 7,
volume = 32,
place = {United States},
year = {2019},
month = {12}
}

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