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Selective formation of pyridinic-type nitrogen-doped graphene and its application in lithium-ion battery anodes

Bagley, Jacob D. and Kishore Kumar, Deepan and See, Kimberly A. and Yeh, Nai-Chang (2020) Selective formation of pyridinic-type nitrogen-doped graphene and its application in lithium-ion battery anodes. RSC Advances, 10 (65). pp. 39562-39571. ISSN 2046-2069. https://resolver.caltech.edu/CaltechAUTHORS:20201030-102416804

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Abstract

We report a high-yield single-step method for synthesizing nitrogen-doped graphene nanostripes (N-GNSPs) with an unprecedentedly high percentage of pyridinic-type doping (>86% of the nitrogen sites), and investigate the performance of the resulting N-GNSPs as a lithium-ion battery (LIB) anode material. The as-grown N-GNSPs are compared with undoped GNSPs using scanning electron microscopy (SEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), helium ion-beam microscopy (HIM), and electrochemical methods. As an anode material we find that pyridinic-type N-GNSPs perform similarly to undoped GNSPs, suggesting that pyridinic sites alone are not responsible for the enhanced performance of nitrogen-doped graphene observed in previous studies, which contradicts common conjectures. In addition, post-mortem XPS measurements of nitrogen-doped graphene cycled as a lithium-ion battery anode are conducted for the first time, which reveal direct evidence for irreversible chemical changes at the nitrogen sites during cycling. These findings therefore provide new insights into the mechanistic models of doped graphene as LIB anodes, which are important in improving the anode designs for better LIB performance.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1039/d0ra06199aDOIArticle
http://www.rsc.org/suppdata/d0/ra/d0ra06199a/d0ra06199a1.pdfPublisherSupplementary Information
ORCID:
AuthorORCID
Bagley, Jacob D.0000-0001-9490-1341
Kishore Kumar, Deepan0000-0003-0236-8805
See, Kimberly A.0000-0002-0133-9693
Yeh, Nai-Chang0000-0002-1826-419X
Additional Information:© The Royal Society of Chemistry 2020. Open Access Article. This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. Received 16th July 2020; Accepted 19th October 2020; First published 29 Oct 2020. This research was jointly supported by the United Advanced Materials and the National Science Foundation under the Institute for Quantum Information and Matter (IQIM) at Caltech (Award #1733907). We thank Professor George R. Rossman for allowing our access to his Raman spectroscopic facilities, and also acknowledge the use of XPS/UPS at the Beckman Institute and HIM at the Kavli Nanoscience Institute at Caltech. Author contributions: J. D. Bagley developed the 8-chamber PECVD growth system, synthesized N-GNSPs, carried out Raman spectroscopic characterization, SEM surface characterization, XPS studies, and fabrications of LIB anodes and coin cells. D. Kishore Kumar carried out the HIM measurement and synthesized GNSPs. K. See contributed to the LIB studies and provided the facilities for the coin cell fabrications. N.-C. Yeh coordinated the research project and data analysis, and wrote the manuscript together with J. D. Bagley. There are no conflicts to declare.
Group:Institute for Quantum Information and Matter, Kavli Nanoscience Institute
Funders:
Funding AgencyGrant Number
United Advanced MaterialsUNSPECIFIED
NSFPHY-1733907
Institute for Quantum Information and Matter (IQIM)UNSPECIFIED
Caltech Beckman InstituteUNSPECIFIED
Kavli Nanoscience InstituteUNSPECIFIED
Issue or Number:65
Record Number:CaltechAUTHORS:20201030-102416804
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20201030-102416804
Official Citation:Selective formation of pyridinic-type nitrogen-doped graphene and its application in lithium-ion battery anodes. RSC Adv., 2020, 10, 39562-39571; doi: 10.1039/d0ra06199a
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106354
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:30 Oct 2020 17:40
Last Modified:30 Oct 2020 17:40

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