Hierarchical Porous, N-Containing Carbon Supports for High Loading Sulfur Cathodes.

Jae-Woo Park,Sung Yong Cho,Byeong-Hyeon An,Hui-Ju Kang,Gazi A K M Rafiqul Bari,Young-Si Jun,Hyun Jin Hwang,Tae-Gyu Lee

doi:10.3390/nano11020408

Jae-Woo Park, Sung Yong Cho + Show 6 more

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https://doi.org/10.3390/nano11020408

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Abstract

The lithium-polysulfide (LiPS) dissolution from the cathode to the organic electrolyte is the main challenge for high-energy-density lithium-sulfur batteries (LSBs). Herein, we present a multi-functional porous carbon, melamine cyanurate (MCA)-glucose-derived carbon (MGC), with superior porosity, electrical conductivity, and polysulfide affinity as an efficient sulfur support to mitigate the shuttle effect. MGC is prepared via a reactive templating approach, wherein the organic MCA crystals are utilized as the pore-/micro-structure-directing agent and nitrogen source. The homogeneous coating of spherical MCA crystal particles with glucose followed by carbonization at 600 °C leads to the formation of hierarchical porous hollow carbon spheres with abundant pyridinic N-functional groups without losing their microstructural ordering. Moreover, MGC enables facile penetration and intensive anchoring of LiPS, especially under high loading sulfur conditions. Consequently, the MGC cathode exhibited a high areal capacity of 5.79 mAh cm−2 at 1 mA cm−2 and high loading sulfur of 6.0 mg cm−2 with a minor capacity decay rate of 0.18% per cycle for 100 cycles.

Highlights

Grid-scale energy systems and electric vehicles require high-energy-density batteries.The current-state-of-the-art energy storage technology, i.e., lithium-ion batteries (LIBs), has already reached its theoretical limit [1,2]
A molecular cooperative assembly-mediated synthesis method was used to generate porous N-containing carbon supports without sacrificing the structural order
To achieve these, (1) hierarchically porous structure, (2) pyridinic N-functional groups, and (3) more aromatically condensed structure possessing carbon is prepared. This was obtained through the simple mixing of glucose as a carbon source and melamine and cyanuric acid (MCA) as a reactive template and by carbonization of the mixture

Summary

Introduction

Grid-scale energy systems and electric vehicles require high-energy-density batteries. The current-state-of-the-art energy storage technology, i.e., lithium-ion batteries (LIBs), has already reached its theoretical limit [1,2]. To become more competitive with LIBs, the next-generation battery technologies must consider energy density, power density, cycle performance, and cost. Among the various energy storage systems, rechargeable lithium–sulfur batteries (LSBs) are widely considered as one of the most promising candidates [3,4]. LSBs have a high theoretical energy density ~2800 Wh L−1 ) and are cost-effective because they use inexpensive, abundant, and eco-friendly elemental sulfur (S8 ) as their cathode active material [5]. The same manufacturing process existing for LIBs can be employed for the LSBs [6]. Given the operating voltage of ~2.1 V vs. Li/Li+ , the practical LSBs to replace the commercial

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