Critical Role of Aromatic C(sp2)-H in Boosting Lithium-Ion Storage

Jiabiao Lian; Gokila Subburam; Sherif A El-Khodary; Kai Zhang; Bobo Zou; Juan Wang; Chuan Wang; Jianmin Ma; Xiaojun Wu

doi:10.1021/jacs.3c12051

Critical Role of Aromatic C(sp²)-H in Boosting Lithium-Ion Storage

J Am Chem Soc. 2024 Mar 27;146(12):8110-8119. doi: 10.1021/jacs.3c12051. Epub 2024 Mar 15.

Authors

Jiabiao Lian¹, Gokila Subburam¹, Sherif A El-Khodary¹, Kai Zhang², Bobo Zou¹, Juan Wang¹, Chuan Wang³, Jianmin Ma⁴, Xiaojun Wu²

Affiliations

¹ Institute for Energy Research, School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, P. R. China.
² Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Material Sciences, CAS Key Laboratory of Materials for Energy Conversion, and Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
³ Institute of Advanced Synthesis, School of Chemistry and Molecular Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University, Nanjing 211800, P. R. China.
⁴ School of Chemistry, Tiangong University, Tianjin 300387, P. R. China.

PMID: 38489846
DOI: 10.1021/jacs.3c12051

Abstract

Exploring high-sloping-capacity carbons is of great significance in the development of high-power lithium-ion batteries/capacitors (LIBs/LICs). Herein, an ion-catalyzed self-template method is utilized to synthesize the hydrogen-rich carbon nanoribbon (HCNR), achieving high specific and rate capacity (1144.2/471.8 mAh g^-1 at 0.1/2.5 A g^-1). The Li⁺ storage mechanism of the HCNR is elucidated by in situ spectroscopic techniques. Intriguingly, the protonated aromatic sp²-hybridized carbon (C(sp²)-H) can provide additional active sites for Li⁺ uptake via reversible rehybridization to sp³-C, which is the origin of the high sloping capacity. The presence of this sloping feature suggests a highly capacitance-dominated storage process, characterized by rapid kinetics that facilitates superior rate performance. For practical usage, the HCNR-based LIC device can deliver high energy/power densities of 198.3 Wh kg^-1/17.9 kW kg^-1. This work offers mechanistic insights on the crucial role of aromatic C(sp²)-H in boosting Li⁺ storage and opens up new avenues to develop such sloping-type carbons for high-performance rechargeable batteries/capacitors.