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Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium-sulfur batteries.

Kim H, Lee J, Ahn H, Kim O, Park MJ - Nat Commun (2015)

Bottom Line: Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases.Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles.Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

View Article: PubMed Central - PubMed

Affiliation: Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 790-784, Korea.

ABSTRACT
Elemental sulfur is one of the most attractive cathode active materials in lithium batteries because of its high theoretical specific capacity. Despite the positive aspect, lithium-sulfur batteries have suffered from severe capacity fading and limited rate capability. Here we report facile large-scale synthesis of a class of organosulfur compounds that could open a new chapter in designing cathode materials to advance lithium-sulfur battery technologies. Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases. Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles. Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

No MeSH data available.


Related in: MedlinePlus

Molecular characteristics of vulcanized TTCAs.(a) Raman spectra of porous TTCA-I (heat treated at 160 °C) and S-TTCA-I (vulcanized at 245 °C), (b) XPS profile of the S-TTCA-I and (c) TGA analysis of the S-TTCA-I, compared with that of elemental sulfur in carbon frameworks (S–C).
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f3: Molecular characteristics of vulcanized TTCAs.(a) Raman spectra of porous TTCA-I (heat treated at 160 °C) and S-TTCA-I (vulcanized at 245 °C), (b) XPS profile of the S-TTCA-I and (c) TGA analysis of the S-TTCA-I, compared with that of elemental sulfur in carbon frameworks (S–C).

Mentions: Molecular characteristics of the vulcanized TTCAs were examined by Raman spectroscopy. Representative spectra of porous TTCA-I and S-TTCA-I are shown in Fig. 3a. The peak centered at 448 cm−l was attributed to N–C–S deformation and was evident in porous TTCA-I. After vulcanization, the characteristic N–C–S deformation peak was shifted to 435 cm−l and was accompanied by the appearance of new peak at 482 cm−l as evidence for the formation of the S–S bonds. This indicates that elemental sulfur (S8) reacts with the thiol groups of TTCA crystals, following the equation in Fig. 1.


Synthesis of three-dimensionally interconnected sulfur-rich polymers for cathode materials of high-rate lithium-sulfur batteries.

Kim H, Lee J, Ahn H, Kim O, Park MJ - Nat Commun (2015)

Molecular characteristics of vulcanized TTCAs.(a) Raman spectra of porous TTCA-I (heat treated at 160 °C) and S-TTCA-I (vulcanized at 245 °C), (b) XPS profile of the S-TTCA-I and (c) TGA analysis of the S-TTCA-I, compared with that of elemental sulfur in carbon frameworks (S–C).
© Copyright Policy - open-access
Related In: Results  -  Collection

License
Show All Figures
getmorefigures.php?uid=PMC4490390&req=5

f3: Molecular characteristics of vulcanized TTCAs.(a) Raman spectra of porous TTCA-I (heat treated at 160 °C) and S-TTCA-I (vulcanized at 245 °C), (b) XPS profile of the S-TTCA-I and (c) TGA analysis of the S-TTCA-I, compared with that of elemental sulfur in carbon frameworks (S–C).
Mentions: Molecular characteristics of the vulcanized TTCAs were examined by Raman spectroscopy. Representative spectra of porous TTCA-I and S-TTCA-I are shown in Fig. 3a. The peak centered at 448 cm−l was attributed to N–C–S deformation and was evident in porous TTCA-I. After vulcanization, the characteristic N–C–S deformation peak was shifted to 435 cm−l and was accompanied by the appearance of new peak at 482 cm−l as evidence for the formation of the S–S bonds. This indicates that elemental sulfur (S8) reacts with the thiol groups of TTCA crystals, following the equation in Fig. 1.

Bottom Line: Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases.Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles.Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

View Article: PubMed Central - PubMed

Affiliation: Department of Chemistry, Pohang University of Science and Technology (POSTECH), Pohang 790-784, Korea.

ABSTRACT
Elemental sulfur is one of the most attractive cathode active materials in lithium batteries because of its high theoretical specific capacity. Despite the positive aspect, lithium-sulfur batteries have suffered from severe capacity fading and limited rate capability. Here we report facile large-scale synthesis of a class of organosulfur compounds that could open a new chapter in designing cathode materials to advance lithium-sulfur battery technologies. Porous trithiocyanuric acid crystals are synthesized for use as a soft template, where the ring-opening polymerization of elemental sulfur takes place along the thiol surfaces to create three-dimensionally interconnected sulfur-rich phases. Our lithium-sulfur cells display discharge capacity of 945 mAh g(-1) after 100 cycles at 0.2 C with high-capacity retention of 92%, as well as lifetimes of 450 cycles. Particularly, the organized amine groups in the crystals increase Li(+)-ion transfer rate, affording a rate performance of 1210, mAh g(-1) at 0.1 C and 730 mAh g(-1) at 5 C.

No MeSH data available.


Related in: MedlinePlus