TY - JOUR
T1 - Nitrogen and sulfur co-doped graphene nanoribbons with well-ordered stepped edges for high-performance potassium-ion battery anodes
AU - Choi, Juhyung
AU - Jin, Aihua
AU - Jung, Hyun Dong
AU - Ko, Dongjin
AU - Um, Ji Hyun
AU - Choi, Yoon Jeong
AU - Kim, So Hee
AU - Back, Seoin
AU - Yu, Seung Ho
AU - Piao, Yuanzhe
N1 - Funding Information:
J. Choi, A. Jin, and H. D. Jung contributed equally to this work. Y. P. acknowledges the support of the Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education ( NRF-2021R1A2C1008380 ) and the Nano Material Technology Development Program (NRF-2015M3A7B6027970) of MSIP/NRF. S.-H. Y. acknowledges the support of the National Research Foundation of Korea (NRF) through a grant funded by the Korean government (MSIT) ( NRF-2020R1C1C1012308 ). S. B. acknowledges the support from the National Research Foundation of Korea (NRF) through a grant that was funded by the Ministry of Science and ICT ( 2015M3D3A1A01064929 ) and the generous supercomputing time from KISTI (KSC-2021-CRE-0060). A. J. acknowledges the support of the National Research Foundation of Korea (NRF) through a grant funded by the Korean government (MSIT) ( NRF-2020R1A2C1012342 ). J. H. U. acknowledges the support provided by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education ( NRF-2021R1I1A1A01044891 ).
Publisher Copyright:
© 2022
PY - 2022/6
Y1 - 2022/6
N2 - Graphitic carbon materials, particularly few-layered graphene, exhibit great potentials as potassium-ion battery (PIBs) anodes. However, bulk graphene-based materials have the disordered structure owing to randomly stacked graphene layers, which causes the high migration barrier during K+ intercalation/deintercalation reactions and thus the surface-dominated capacitive response. Here, we present a novel nanoarchitecture of nitrogen and sulfur co-doped graphene nanoribbons with well-ordered stepped edges (NS–sGNR) via the electrochemical unzipping of multiwalled carbon nanotubes (MWCNTs) and the subsequent N/S co-doping process for high-performance PIB anodes. As an anode material for PIBs, the prepared sample exhibits high initial capacity (329.1 mAh g−1 at 50 mA g−1), superior rate capability (211.7 mAh g−1 at high current density, 2000 mA g−1), outstanding reversibility of K-staging, and stable long-term cyclability. Theoretical calculations were conducted to demonstrate that sGNRs with NS co-doping (NS–sGNR) exhibit much improved K+ intercalation properties, such as the K+ adsorption energy, charge transfer, and migration barriers, compared with the parallel-edged GNRs. Particularly, the migration barrier (the rate-determining step) can be substantially reduced at the stepped edges during K+ intercalation.
AB - Graphitic carbon materials, particularly few-layered graphene, exhibit great potentials as potassium-ion battery (PIBs) anodes. However, bulk graphene-based materials have the disordered structure owing to randomly stacked graphene layers, which causes the high migration barrier during K+ intercalation/deintercalation reactions and thus the surface-dominated capacitive response. Here, we present a novel nanoarchitecture of nitrogen and sulfur co-doped graphene nanoribbons with well-ordered stepped edges (NS–sGNR) via the electrochemical unzipping of multiwalled carbon nanotubes (MWCNTs) and the subsequent N/S co-doping process for high-performance PIB anodes. As an anode material for PIBs, the prepared sample exhibits high initial capacity (329.1 mAh g−1 at 50 mA g−1), superior rate capability (211.7 mAh g−1 at high current density, 2000 mA g−1), outstanding reversibility of K-staging, and stable long-term cyclability. Theoretical calculations were conducted to demonstrate that sGNRs with NS co-doping (NS–sGNR) exhibit much improved K+ intercalation properties, such as the K+ adsorption energy, charge transfer, and migration barriers, compared with the parallel-edged GNRs. Particularly, the migration barrier (the rate-determining step) can be substantially reduced at the stepped edges during K+ intercalation.
UR - http://www.scopus.com/inward/record.url?scp=85127115280&partnerID=8YFLogxK
U2 - 10.1016/j.ensm.2022.03.041
DO - 10.1016/j.ensm.2022.03.041
M3 - Article
AN - SCOPUS:85127115280
SN - 2405-8297
VL - 48
SP - 325
EP - 334
JO - Energy Storage Materials
JF - Energy Storage Materials
ER -