TY - JOUR
T1 - Tuning the local chemistry of SPAN to realize the development of room-temperature sodium-sulfur pouch cells
AU - Sanjaykumar, C.
AU - Sungjemmenla, None
AU - Chandra, Mahesh
AU - Soni, Chhail Bihari
AU - Vineeth, S. K.
AU - Das, Sweta
AU - Cohen, Nevo
AU - Kumar, Hemant
AU - Mandler, Daniel
AU - Kumar, Vipin
N1 - Publisher Copyright: © 2025 The Royal Society of Chemistry.
PY - 2024
Y1 - 2024
N2 - Sulfurized polyacrylonitrile (SPAN), a nitrogen-rich carbon-sulfur framework, is a promising alternative to the elemental sulfur cathode. However, repetitive formation and breaking of carbon-sulfur bonds causes irreversible capacity loss. The capacity loss of SPAN can be fixed by altering the local environment of the SPAN. This work demonstrates a metal monosulfide, i.e., zinc sulfide (ZnS), as a SPAN cathode additive to fix the capacity loss and boost the overall performance of the cathode. Besides improving the sulfur loading, it alters the local carbon-sulfur environment. The presence of ZnS is expected to shorten the sulfur-sulfur bond of the SPAN matrix, leading to a change in the local nitrogen environment. The ratio of pyridinic-nitrogen to pyrrolic-nitrogen increases sharply upon including ZnS. A coin-cell with ZnS doped SPAN cathode exhibits excellent cycling stability for over 450 cycles, with minimal decay of about 0.07% per cycle. DFT calculations reveal that the addition of ZnS enhances SPAN's sodium migration and electronic conductivity by lowering sodium migration barriers and reducing the HOMO/LUMO gap, improving charge transfer kinetics. Furthermore, a multi-layered pouch cell featuring a ZnS doped SPAN cathode demonstrates the efficiency of the proposed cathode. The pouch cell exhibits excellent cycling stability and coulombic efficiency for over 250 cycles. This study provides a pathway to engineer the local chemistry of the cathode to design innovative cathode materials for a stable and reversible RT-Na/S battery.
AB - Sulfurized polyacrylonitrile (SPAN), a nitrogen-rich carbon-sulfur framework, is a promising alternative to the elemental sulfur cathode. However, repetitive formation and breaking of carbon-sulfur bonds causes irreversible capacity loss. The capacity loss of SPAN can be fixed by altering the local environment of the SPAN. This work demonstrates a metal monosulfide, i.e., zinc sulfide (ZnS), as a SPAN cathode additive to fix the capacity loss and boost the overall performance of the cathode. Besides improving the sulfur loading, it alters the local carbon-sulfur environment. The presence of ZnS is expected to shorten the sulfur-sulfur bond of the SPAN matrix, leading to a change in the local nitrogen environment. The ratio of pyridinic-nitrogen to pyrrolic-nitrogen increases sharply upon including ZnS. A coin-cell with ZnS doped SPAN cathode exhibits excellent cycling stability for over 450 cycles, with minimal decay of about 0.07% per cycle. DFT calculations reveal that the addition of ZnS enhances SPAN's sodium migration and electronic conductivity by lowering sodium migration barriers and reducing the HOMO/LUMO gap, improving charge transfer kinetics. Furthermore, a multi-layered pouch cell featuring a ZnS doped SPAN cathode demonstrates the efficiency of the proposed cathode. The pouch cell exhibits excellent cycling stability and coulombic efficiency for over 250 cycles. This study provides a pathway to engineer the local chemistry of the cathode to design innovative cathode materials for a stable and reversible RT-Na/S battery.
UR - http://www.scopus.com/inward/record.url?scp=85211613623&partnerID=8YFLogxK
U2 - https://doi.org/10.1039/d4ta05581k
DO - https://doi.org/10.1039/d4ta05581k
M3 - مقالة
SN - 2050-7488
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
ER -