Because of the high theoretical capacity of 1675 mAh g and high energy density of 2600 Wh kg, respectively, lithium-sulfur batteries are attracting intense interest. However, it remains an enormous challenge to realize high utilizations and loadings of sulfur in cathodes for the practical applications of Li-S batteries. Herein, we design a quasi-2D Co@N-C composite with honeycomb architecture as a multifunctional sulfur host via a simple sacrificial templates method. The cellular flake with large surface area and honeycomb architecture can encapsulate much more sulfur, leading to high sulfur content (HSC) composites, and by stacking these HSC flakes, a high sulfur loading (HSL) electrode can be realized due to their high layer bulk density. Compared to our previous work in multifunctional Co-N-C composites, the cellular Co@N-C composite displays a distinct enhancement in the sulfur content, sulfur loading, cycle stability, and rate performance. Benefiting from the cellular morphology, a composite with an HSC of 93.6 wt % and an electrode with an HSL of 7.5 mg cm can be obtained simultaneously, which exhibited excellent rate performance up to 10 C (3.6 mg cm) and great cycling stability.

Investigations of the Ag (I)-substituted Keggin K[HAgPWO] as a bifunctional Lewis acidic and basic catalyst are reported that explore the stabilization of LiS moieties so that reversible redox reactions in S-based electrodes would be possible. Spectroscopic investigations showed that the LiS-moieties can be strongly adsorbed on the {AgPWO} cluster, where the Ag(I) ion can act as a Lewis acid site to further enhance the adsorption of the S-moieties, and these interactions were investigated and rationalized using DFT. These results were used to construct an electrode for use in a Li-S battery with a very high S utilization of 94%, and a coulometric capacity of 1580 mAh g. This means, as a result of using the AgPOM, both a high active S content, as well as a high areal S mass loading, is achieved in the composite electrode giving a highly stable battery with cycling performance at high rates (1050 and 810 mAh g at 1C and 2C over 100 to 300 cycles, respectively).

An electron conductive matrix, or collector, facilitates electron transport in an electrochemical device. It is stationary and does not change during the entire operation once it is built. The interface of this matrix and an electrode is constructed at a 2D level at the micro‐scale, and naturally limits the breadth and depth of electrochemical reactions. Herein, the idea of an enhanced electrode coupled with a conducting molecule that can extend interfacial reactions is first introduced. With a spatialized interspace, this electrode can change the present understanding of the electrode process and opens up a new realm of electrode‐based reaction chemistry. A lithium–sulfur (Li–S) battery is used as the target for implementing the enhanced electrode owing to the complex multi‐electron reaction. Through the interaction of π–π stacking between graphite‐based carbon and iron (II) phthalocyanine (FePc), soluble FePc can be decorated on the surface of an electrode that has the capability of transporting electrons. The scanning tunneling microscope break junction characterization and density functional theory indicate that FePc has a strong molecular electronic conductivity. The reactants obtain electrons more easily from the conducting molecule than from the collector directly. As a result, the performance of the corresponding Li–S battery considerably improves.