Shedding light on rechargeable Na/Cl 2 battery

Author:

Zhu Guanzhou1,Liang Peng1,Huang Cheng-Liang23,Wu Shu-Chi1,Huang Cheng-Chia2,Li Yuan-Yao2,Jiang Shi-Kai4,Huang Wei-Hsiang5,Li Jiachen1,Wang Feifei6,Hwang Bing-Joe4ORCID,Dai Hongjie1

Affiliation:

1. Department of Chemistry and Bio-X, Stanford University, Stanford, CA 94305

2. Department of Chemical Engineering, National Chung Cheng University, Chia-Yi 62102, Taiwan

3. Department of Electrical Engineering, National Chung Cheng University, Chia-Yi 62102, Taiwan

4. Department of Chemical Engineering, National Taiwan University of Science and Technology, Taipei 10607, Taiwan

5. National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan

6. Department of Electrical and Electronic Engineering, The University of Hong Kong, Hong Kong 999077, China

Abstract

Advancing new ideas of rechargeable batteries represents an important path to meeting the ever-increasing energy storage needs. Recently, we showed rechargeable sodium/chlorine (Na/Cl 2 ) (or lithium/chlorine Li/Cl 2 ) batteries that used a Na (or Li) metal negative electrode, a microporous amorphous carbon nanosphere (aCNS) positive electrode, and an electrolyte containing dissolved aluminum chloride and fluoride additives in thionyl chloride [G. Zhu et al. , Nature 596 , 525–530 (2021) and G. Zhu et al. , J. Am. Chem. Soc. 144 , 22505–22513 (2022)]. The main battery redox reaction involved conversion between NaCl and Cl 2 trapped in the carbon positive electrode, delivering a cyclable capacity of up to 1,200 mAh g −1 (based on positive electrode mass) at a ~3.5 V discharge voltage [G. Zhu et al. , Nature 596 , 525–530 (2021) and G. Zhu et al. , J. Am. Chem. Soc. 144 , 22505–22513 (2022)]. Here, we identified by X-ray photoelectron spectroscopy (XPS) that upon charging a Na/Cl 2 battery, chlorination of carbon in the positive electrode occurred to form carbon-chlorine (C-Cl) accompanied by molecular Cl 2 infiltrating the porous aCNS, consistent with Cl 2 probed by mass spectrometry. Synchrotron X-ray diffraction observed the development of graphitic ordering in the initially amorphous aCNS under battery charging when the carbon matrix was oxidized/chlorinated and infiltrated with Cl 2 . The C-Cl, Cl 2 species and graphitic ordering were reversible upon discharge, accompanied by NaCl formation. The results revealed redox conversion between NaCl and Cl 2 , reversible graphitic ordering/amorphourization of carbon through battery charge/discharge, and probed trapped Cl 2 in porous carbon by XPS.

Publisher

Proceedings of the National Academy of Sciences

Subject

Multidisciplinary

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