首页|Extraordinary Ultrahigh-Capacity and Long Cycle Life Lithium-Ion Batteries Enabled by Graphitic Carbon Nitride-Perylene Polyimide Composites

Extraordinary Ultrahigh-Capacity and Long Cycle Life Lithium-Ion Batteries Enabled by Graphitic Carbon Nitride-Perylene Polyimide Composites

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Graphitic carbon nitride(g-C3N4)is widely used in organic metal-ion batteries owing to its high porosity,facile synthesis,stability,and high-rate performance.However,pristine g-C3N4 nanosheets exhibit poor electrical conductivity,irreversible metal-ion storage capacity,and short-term cycling owing to their high concentration of graphitic-N species.Herein,a series of 3,4:9,10-perylenetetracarboxylic diimide-coupled g-C3N4 composite anode materials,CN-PIx(x=0.2,0.5,0.75,and 1),was investigated,which exhibited an unusually high surface nitrogen content(23.19-39.92 at.％)and the highest pyridinic-N,pyrrolic-N,and graphitic-N contents reported to date.The CN-PI1 anode delivers an unprecedented and continuously increasing ultrahigh discharging capacity of exceeding 8400 mAh g-1(1.96 mWh cm-2)at 100 mA g-1 with high specific energy density(Esp)of～7700 Wh kg-1 and the volumetric energy density(Ev)of～14956 Wh L-1 and an excellent long-term stability(414 mAh g-1 or 0.579 mWh cm-2 at 1 A g-1).Furthermore,the activation of the CN-PIx electrodes contributes to their superior electrochemical performance,resulting from the fact that the Li+is not only stored in the CN-PIx composites but also CN-PIx activated the Li0 adlayer on the CN-PI1-Cu heterojunction as an SEI layer to avoid the direct contact of Lio phase and the electrolyte.The CN-PI1 full cell with LiCoO2 as the cathode delivers a discharge capacity of～587 mAh g-1 at a 1 A g-1 after 250 cycles with a Coulombic efficiency nearly 99％.This study provides a strategy to develop N-doped g-C3N4-based anode materials for realizing long-lasting energy storage devices.

graphitic carbon nitridelithium-ion batteriesorganic electrodeperylene polyimidesemiconductor-metal heterojunction

Michael Ruby Raj、Jungwon Yun、Dong-kyu Son、Gibaek Lee

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Advanced Energy Materials Design Lab,School of Chemical Engineering,Yeungnam University,38541,Gyeongsan-si,Korea

William G.Lowrie Chemical and Biomolecular Engineering,The Ohio State University,Columbus OH 43210,USA

the"Human Resources Program in Energy Technology"of the Korea Institute of Energy Technology Evaluation and PlanningMinistry of Trade,Industry & Energy,Republic of KoreaBasic Science Research Program through the National Research Foundation of KoreaMinistry of Education,Republic of Korea

20204010600100NRF-2019R1I1A3A01046928

2023

10.1002/eem2.12553

能源与环境材料(英文)

能源与环境材料(英文)

CSCD
ISSN：
年,卷(期)：2023.6(6)
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