TY - JOUR
T1 - Design Principles for Optimum Performance of Porous Carbons in Lithium-Sulfur Batteries
AU - Sahore, Ritu
AU - Levin, Barnaby D. A.
AU - Pan, Mian
AU - Muller, David A.
AU - DiSalvo, Francis J.
AU - Giannelis, Emmanuel P.
N1 - KAUST Repository Item: Exported on 2022-06-02
Acknowledged KAUST grant number(s): KUS-C1-018-02
Acknowledgements: This work is supported by the Energy Materials Center at Cornell (EMC2) – an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under award number DE-SC0001086 and in part by award no. KUS-C1-018-02 made by King Abdullah University of Science and Technology (KAUST), KAUST baseline fund. This work made use of the Cornell Center for Materials Research Shared Facilities supported through the NSF MRSEC program (DMR-1120296). In addition to support from the Energy Material Center at Cornell (EMC2) (see above), B. D. A. Levin and D. A. Muller acknowledge support for cryo-TEM studies of lithium–sulfur battery cathodes from the New York State Center for Future Energy Systems (CFES), a joint Center for Advanced Technology between Cornell University and Rensselaer Polytechnic Institute, supported by the New York State, Empire State Development Division of Science, Technology and Innovation (NYSTAR), under contract number C100126. The authors thank Michael J. Zachman and Prof. Lena Kourkoutis of Cornell University for useful discussions regarding cryo-TEM. The authors thank John Grazul for assistance in the TEM facilities. The authors would also like to thank Dr. Ira D. Bloom and Dr. Zhengcheng (John) Zhang at Argonne National Laboratory for their support in completion of the revision experiments.
This publication acknowledges KAUST support, but has no KAUST affiliated authors.
PY - 2016/5/2
Y1 - 2016/5/2
N2 - A series of experiments is presented that establishes for the first time the role of some of the key design parameters of porous carbons including surface area, pore volume, and pore size on battery performance. A series of hierarchical porous carbons is used as a model system with an open, 3D, interconnected porous framework and highly controlled porosity. Specifically, carbons with surface areas ranging from ≈500–2800 m2 g−1, pore volume from ≈0.6–5 cm3 g−1, and pore size from micropores (≈1 nm) to large mesopores (≈30 nm) are synthesized and tested. At high sulfur loadings (≈80 wt% S), pore volume is more important than surface area with respect to sulfur utilization. Mesopore size, in the range tested, does not affect the sulfur utilization. No relationship between porosity and long-term cycle life is observed. All systems fail after 200–300 cycles, which is likely due to the consumption of the LiNO3 additive over cycling. Moreover, cryo-scanning transmission electron microscopy imaging of these carbon–sulfur composites combined with X-ray diffraction (XRD) provides further insights into the effect of initial sulfur distribution on sulfur utilization while also revealing the inadequacy of the indirect characterization techniques alone in reliably predicting distribution of sulfur within porous carbon matrices.
AB - A series of experiments is presented that establishes for the first time the role of some of the key design parameters of porous carbons including surface area, pore volume, and pore size on battery performance. A series of hierarchical porous carbons is used as a model system with an open, 3D, interconnected porous framework and highly controlled porosity. Specifically, carbons with surface areas ranging from ≈500–2800 m2 g−1, pore volume from ≈0.6–5 cm3 g−1, and pore size from micropores (≈1 nm) to large mesopores (≈30 nm) are synthesized and tested. At high sulfur loadings (≈80 wt% S), pore volume is more important than surface area with respect to sulfur utilization. Mesopore size, in the range tested, does not affect the sulfur utilization. No relationship between porosity and long-term cycle life is observed. All systems fail after 200–300 cycles, which is likely due to the consumption of the LiNO3 additive over cycling. Moreover, cryo-scanning transmission electron microscopy imaging of these carbon–sulfur composites combined with X-ray diffraction (XRD) provides further insights into the effect of initial sulfur distribution on sulfur utilization while also revealing the inadequacy of the indirect characterization techniques alone in reliably predicting distribution of sulfur within porous carbon matrices.
UR - http://hdl.handle.net/10754/678412
UR - https://onlinelibrary.wiley.com/doi/10.1002/aenm.201600134
UR - http://www.scopus.com/inward/record.url?scp=84964714792&partnerID=8YFLogxK
U2 - 10.1002/aenm.201600134
DO - 10.1002/aenm.201600134
M3 - Article
SN - 1614-6840
VL - 6
SP - 1600134
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 14
ER -