Enhancing lithium-sulphur battery performance by strongly binding the discharge products on amino-functionalized reduced graphene oxide

Enhancing lithium-sulphur battery performance by strongly binding the discharge products on amino-functionalized reduced graphene oxide

25 Sep 2014 | Zhiyu Wang¹,²,*, Yanfeng Dong¹,*, Hongjiang Li¹, Zongbin Zhao¹, Hao Bin Wu², Ce Hao¹, Shaohong Liu¹, Jieshan Qiu¹ & Xiong Wen (David) Lou²
This article presents a strategy to enhance the performance of lithium-sulphur (Li-S) batteries by covalently stabilizing sulphur and its discharge products on amino-functionalized reduced graphene oxide (rGO). The approach involves functionalizing rGO with ethylenediamine (EDA), which enables strong chemical bonding between polar lithium sulphides and nonpolar carbon surfaces. This prevents active mass loss and maintains electrical contact, leading to stable capacity retention of 80% for 350 cycles with high capacities and excellent high-rate performance up to 4 C. The study demonstrates a feasible method to overcome long-term cycling issues in Li-S batteries and provides insights into the capacity decay mechanism. Li-S batteries are promising due to their high theoretical energy density (2567 Wh kg⁻¹), but their practical use is hindered by issues such as short lifespan, low efficiency, and safety concerns from the lithium anode. The main challenges include polysulphide dissolution, the insulating nature of sulphur, and significant volume changes during lithiation/delithiation. Using sulphur-carbon composites is a major approach to improve the conductivity and stability of sulphur cathodes, but physical barriers in carbon materials only provide short-term solutions due to weak interactions with highly polar polysulphides. The study shows that strong chemical binding of sulphur and its discharge products to the carbon host is essential to eliminate polysulphide shuttling. The EDA-functionalized rGO (EFG) effectively stabilizes sulphur and its discharge products, leading to a nanocomposite (EFG-S) with exceptional stability and performance. The EFG-S nanocomposite exhibits a high capacity retention of 80% for 350 cycles and a high-rate capability up to 4 C. The strong interaction between EDA moieties and discharge products is confirmed by density-functional theory (DFT) calculations and XPS analysis. The electrochemical performance of the EFG-S nanocomposite is evaluated through cyclic voltammetry (CV), galvanostatic charge/discharge tests, and electrochemical impedance spectroscopy (EIS). The results show excellent cycling stability, high Coulombic efficiency, and superior rate capability. The EFG-S nanocomposite also demonstrates good cycling response to varying current densities and maintains high capacity even after deep cycling. The study highlights the importance of EDA functionalization in enhancing the lifespan and rate capability of EFG-S nanocomposites. The strong interaction between EDA moieties and discharge products, along with the high conductivity and mechanical flexibility of rGO, contributes to the exceptional performance of the EFG-S nanocomposite. The findings suggest that EDA functionalization is a critical factor in improving the electrochemical performance of sulphur-carbon composites for Li-S batteries. The study also emphasizes the need for further research to enhance the safety of Li-S cells and deepen understanding of the Li-SThis article presents a strategy to enhance the performance of lithium-sulphur (Li-S) batteries by covalently stabilizing sulphur and its discharge products on amino-functionalized reduced graphene oxide (rGO). The approach involves functionalizing rGO with ethylenediamine (EDA), which enables strong chemical bonding between polar lithium sulphides and nonpolar carbon surfaces. This prevents active mass loss and maintains electrical contact, leading to stable capacity retention of 80% for 350 cycles with high capacities and excellent high-rate performance up to 4 C. The study demonstrates a feasible method to overcome long-term cycling issues in Li-S batteries and provides insights into the capacity decay mechanism. Li-S batteries are promising due to their high theoretical energy density (2567 Wh kg⁻¹), but their practical use is hindered by issues such as short lifespan, low efficiency, and safety concerns from the lithium anode. The main challenges include polysulphide dissolution, the insulating nature of sulphur, and significant volume changes during lithiation/delithiation. Using sulphur-carbon composites is a major approach to improve the conductivity and stability of sulphur cathodes, but physical barriers in carbon materials only provide short-term solutions due to weak interactions with highly polar polysulphides. The study shows that strong chemical binding of sulphur and its discharge products to the carbon host is essential to eliminate polysulphide shuttling. The EDA-functionalized rGO (EFG) effectively stabilizes sulphur and its discharge products, leading to a nanocomposite (EFG-S) with exceptional stability and performance. The EFG-S nanocomposite exhibits a high capacity retention of 80% for 350 cycles and a high-rate capability up to 4 C. The strong interaction between EDA moieties and discharge products is confirmed by density-functional theory (DFT) calculations and XPS analysis. The electrochemical performance of the EFG-S nanocomposite is evaluated through cyclic voltammetry (CV), galvanostatic charge/discharge tests, and electrochemical impedance spectroscopy (EIS). The results show excellent cycling stability, high Coulombic efficiency, and superior rate capability. The EFG-S nanocomposite also demonstrates good cycling response to varying current densities and maintains high capacity even after deep cycling. The study highlights the importance of EDA functionalization in enhancing the lifespan and rate capability of EFG-S nanocomposites. The strong interaction between EDA moieties and discharge products, along with the high conductivity and mechanical flexibility of rGO, contributes to the exceptional performance of the EFG-S nanocomposite. The findings suggest that EDA functionalization is a critical factor in improving the electrochemical performance of sulphur-carbon composites for Li-S batteries. The study also emphasizes the need for further research to enhance the safety of Li-S cells and deepen understanding of the Li-S
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