The electrochemistry of stable sulfur isotopes versus lithium

Author:

Li Xue-Ting12,Zhao Yao3ORCID,Zhu Yu-Hui12,Wang Wen-Peng1ORCID,Zhang Ying1,Wang Fuyi3ORCID,Guo Yu-Guo12ORCID,Xin Sen12ORCID,Bai Chunli12ORCID

Affiliation:

1. Beijing National Laboratory for Molecular Sciences, Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China

2. University of Chinese Academy of Sciences, Beijing 100049, China

3. Beijing National Laboratory for Molecular Sciences, Key Laboratory of Analytical Chemistry for Living Biosystems, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Abstract

Sulfur in nature consists of two abundant stable isotopes, with two more neutrons in the heavy one ( 34 S) than in the light one ( 32 S). The two isotopes show similar physicochemical properties and are usually considered an integral system for chemical research in various fields. In this work, a model study based on a Li–S battery was performed to reveal the variation between the electrochemical properties of the two S isotopes. Provided with the same octatomic ring structure, the cyclo - 34 S 8 molecules form stronger S–S bonds than cyclo - 32 S 8 and are more prone to react with Li. The soluble Li polysulfides generated by the Li– 34 S conversion reaction show a stronger cation–solvent interaction yet a weaker cation–anion interaction than the 32 S-based counterparts, which facilitates quick solvation of polysulfides yet hinders their migration from the cathode to the anode. Consequently, the Li– 34 S cell shows improved cathode reaction kinetics at the solid–liquid interface and inhibited shuttle of polysulfides through the electrolyte so that it demonstrates better cycling performance than the Li– 32 S cell. Based on the varied shuttle kinetics of the isotopic-S-based polysulfides, an electrochemical separation method for 34 S/ 32 S isotope is proposed, which enables a notably higher separation factor than the conventional separation methods via chemical exchange or distillation and brings opportunities to low-cost manufacture, utilization, and research of heavy chalcogen isotopes.

Funder

北京市科学技术委员会 | Natural Science Foundation of Beijing Municipality

Basic Science Center Project of National Natural Science Foundation of China

CAS Project for Young Scientists in Basic Research

MOST | National Natural Science Foundation of China

Young Elite Scientist Sponsorship Program by CAST

MOST | National Key Research and Development Program of China

Publisher

Proceedings of the National Academy of Sciences

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