The assembly of two-dimensional conductive nanomaterials into hierarchical complex architectures precisely controlling internal open porosity and orientation, external morphology, composition, and interaction is expected to provide promising hosts for high-capacity sulfur cathodes. Herein, we have demonstrated a new assembly method for the design of hierarchically structured host and active materials combining Spray Frozen (SF) assembly, melt re-crystallization, and ozonation chemistry. Precisely controlling the internal open porosity and orientation, external morphology, composition, and chemical interaction, hierarchical radially assembled open porous spherical rGO and rod-like nS hybrids were constructed. This rod-like nano-Sulfur (nS) was uniformly distributed on the surface of the microspherical rGO architecture and strongly immobilized via covalent bonding. Consequently, R-rGO/nS showed high specific capacities of 1269.1 and 510.3 mAh g<sup>-1</sup> at 0.1 and 4 C, respectively, and long-term cyclic stability over 500 cycles. Moreover, we demonstrated higher battery performance for the R-rGO/nS compared to that of ice-templated I-rGO/nS, physically mixed P-rGO/nS, and radially assembled R-rGO/bulk S hybrids with the same hybrid composition. Thus, the synergistic effect of chemically hybridizing the rod-like nS with hierarchical spherical architecture was successfully confirmed. This research provides a rational and integrative material design chemistry to control all aspects of internal and external structures and compositions as well as to be applied as a host material accommodating high-capacity active materials

Radially assembled open-porous micro graphene-ball with immobilized sulfur nanorods for lithium-sulfur batteries

2019 Fall National Meeting

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