Zhou - Design, Fabrication and Electrochemical Performance of Nanostructured Carbon Based Materials for High-Energy Lithium–Sulfur Batteries Next-Generation High Performance Lithium–Sulfur Batteries

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Springer Nature Singapore Pte Ltd. 2017

Guangmin Zhou Design, Fabrication and Electrochemical Performance of Nanostructured Carbon Based Materials for High-Energy LithiumSulfur Batteries Springer Theses Recognizing Outstanding Ph.D. Research 10.1007/978-981-10-3406-0_1

1. Introduction

Guangmin Zhou 1

(1)

Shenyang, Peoples Republic of China

Guangmin Zhou

Email:

1.1 Introduction of LithiumSulfur Secondary Battery

Lithium-ion batteries (LIBs) play a dominant role in portable electronic devices for decades due to their high performance compared to the other battery systems [].

Fig. 1.1

Comparison of different energy storage devices in terms of power and energy density

The rhombic stacking of S8 is the stable room-temperature form, which consists of eight sulfur atoms constructing a crown structure. The redox chemistry of sulfur in the cathode relies on a solid (cyclo-S8)liquid (lithium polysulfide)solid (Li2S2/Li2S) reaction with a transformation of S8 + 16 Li+ + 16 e 8 Li2S. This is a two-electron conversion reaction through breaking the SS bonds and forming a series of sulfur species such as Li2S8, Li2S6, Li2S4, Li2S3, Li2S2, and Li2S. During the following charge, Li2S is converted into intermediate lithium polysulfides and finally to S8 resulting in a reversible cycle (Fig. ]. In order to address the above issues and realize the application of high energy density and long cycling life LiS batteries, people investigate all the key components in LiS batteries and great progress has been made in this field. For example, Sion Power adopts LiS batteries as energy storage system and uses solar cell to charge the battery in the daytime and provide electricity through LiS batteries in the night. As a record, the LiS battery can power the unmanned plane for continuous 336 h (14 days). Here we briefly summarize the recent advances in LiS batteries, including the sulfur-based cathode, lithium metal anode, separators and electrolytes, and new designs of LiS batteries with a metallic Li-free anode.

Fig. 1.2

Typical chargedischarge curves in the LiS battery, inset: schematic illustration of the polysulfide shuttle effect in the LiS battery. Reprinted with permission from Ref. []. Copyright 2013, Royal Society of Chemistry

1.1.1 Cathode Materials

Currently the most commonly adopted strategy in designing sulfur cathodes includes sulfurcarbon composites, sulfurconducting polymer composites, sulfur/metal oxide composites, and lithium sulfide materials, which will be briefly introduced below.

1.1.1.1 SulfurCarbon Composites

All kinds of sulfurcarbon composites take the advantages of the conductivity of carbon to overcome the insulating property of sulfur. Abundant sulfur could be loaded on the pores of large surface area carbon-based materials. The pore structure of carbon could provide enough space to accommodate the volume change of sulfur during charge and discharge processes, and mitigate the dissolution of polysulfide intermediates, so the utilization of sulfur and cycle performance can be improved. At the same time, the porous structure could enhance the reaction kinetics by providing the electrolyte ion transport channels. Abundant oxygen-/nitrogen-containing functional groups on the surface of carbon could trap polysulfides by strong surface interactions. Therefore, the sulfurcarbon composites have attracted wide attention.

Nazars group has fabricated CMK-3/S composite with 70 wt% sulfur content by a melt-diffusion strategy []. Elemental sulfur has been loaded to the micropores through a solution infiltration method. When the sulfur loading was lower than 37.1 wt%, sulfur mainly existed in the micropores and small mesopores (<3 nm), which are beneficial for the sulfur confinement. However, when sulfur loading was higher than 37.1 wt%, extra sulfur mainly exists in the large mesopores, which could offer the channels for lithium-ion transportation. When sulfur loading was reduced to only 11.7 wt%, the capacity was maintained at 780 mAh g1 after 50 cycles, indicating the cyclic performance and sulfur loading need to be further enhanced.

Fig. 1.3

a Schematic of sulfur confined in the interconnected pore structure of mesoporous carbon. Reprinted with permission from Macmillan Publishers Ltd.: Ref. [] by permission of John Wiley & Sons Ltd.

The above results suggest that mesoporous carbon could store sulfur and offer the facile transport paths for Li ions while the microporous structure exhibits more powerful capability in trapping sulfur. However, the polysulfide dissolution still exists in the above systems. When the diameter of the micropore is lower than that of S8 (~0.7 nm), the chain-like sulfur molecules in the carbon micropores could not transform to the large S8 rings, but maintain as S24 molecules, which leads to the reduction process starting from S24 to S2 instead of the transition from S8 to S24 and eliminating the shuttle effect of lithium polysulfides []. The irreversible chemical reactions between the polysulfides and carbonates and the dissolution of the polysulfides into the ethers can be effectively avoided due to the steric hindrance. The sulfur cathode based on this strategy exhibits excellent rate capability and cycling stability. However, microporous carbon faces the challenge of small pore volume and low sulfur loading, which impedes the realization of high energy density. Further optimization of mesoporemicropore ratio is also required for achieving high-performance LiS batteries.

The excellent electrical conductivity, large specific surface area, and flexible two-dimensional structure of graphene makes it a promising encapsulation material for sulfur cathodes by forming conductive network, buffering the volume change, and improving the electrochemical activity of sulfur. Besides, the easy functionalization of graphene could also establish strong chemical interaction between graphene and polysulfides to stabilize sulfur cathodes. Dais group has reported a graphene/sulfur composite by wrapping PEG-coated sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles, as shown in Fig. ].

Fig. 1.4

a Schematics of the synthesis steps for a PEG-S/graphene composite. Reprinted with permission from Ref. [] by permission of John Wiley & Sons Ltd.

However, due to the easy aggregation and stacking of graphene, it compromises their advantages in the applications of LiS batteries. Zhao et al. proposed a novel graphene/single-walled carbon nanotube (G/SWCNT) hybrid by placing SWCNTs among graphene planes through covalent CC bonding under the catalysis growth on layered double hydroxide [].

Surface chemistry is another important factor which could affect the performance of LiS batteries. Zhang et al. coated sulfur on the surface of graphene oxide (GO) sheets by a simple chemical reactiondeposition strategy and a subsequent low-temperature thermal treatment method [].

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