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[Research background]

Rechargeable aluminum batteries (RABs), as a new generation of energy storage systems, have received extensive attention from researchers due to their advantages such as high safety, high energy density, and wide range of raw materials at low cost. However, due to the high intrinsic charge density of aluminum ions (Al3+, 364Cmm-3) (six times higher than lithium ions), their reactions on traditional electrode materials have to overcome the use of strong Coulombic forces, which often leads to large lattice strain, electrode material pulverization, and poor cycle stability, which are also the core challenges of RABs cathode materials.

[Job Description]

In response to this challenge, Professor Hu Yuxiang and Professor Li Hongyi from Beijing University of Technology recently proposed a new superlattice type cathode material system. Taking the superlattice type tungsten selenide cathode material (S-WSe2) as an example, based on the stable crystal structure and expanded interlayer spacing brought by the superlattice material, they effectively release the stress and strain caused by irreversible damage to the electrode material caused by high charge density Al3+. Long cycle stability has been achieved (the capacity can still reach 110mAhg-1 after cycling more than 1500 cycles at 2Ag-1). The mechanism of the insertion and removal of aluminum ions during the charge and discharge process was investigated by non in-situ XPS and TEM, as well as in situ XRD and Raman characterization. The work was published in "Small Methods" under the title of "Superlattice Stabilized WSe2 Catalyst for Rechargeable Aluminum Batteries", with Cui Fangyan as the first author of this article.

[Core content]

Layered transition metal dihalogenated compounds (TMDCs) have received widespread attention in recent years due to their appropriate aluminum selenium/sulfur bonds, adjustable interlayer spacing, and theoretically rich ion accommodation capabilities. Among them, tungsten selenide (WSe2) has good application prospects in metal ion batteries due to its theoretical high capacity, high conductivity, wide interlayer space, and suitable metal selenium bonding paths, but it has not been reported in RABs. However, the interaction of strong electrostatic forces and inherently high charge density Al3+can still lead to irreversible destruction and the crushing/dissolution of active materials (Figure 1a). Therefore, it is extremely necessary to develop a new strategy for stabilizing the WSe2 structure and study the new generation energy storage system RABs. Superlattice type compounds are materials composed of two (or more) alternating periodic components, particularly suitable for accommodating active ions with high charge density. Therefore, this article uses a simple chemical synthesis method to introduce organic molecules into TMDCs (taking WSe2 as an example) to construct a superlattice type positive electrode to achieve reversible insertion/removal of Al3+, achieving long-term cyclic stability of the electrode.

Figure 1. Characterization of the superlattice type S-WSe2. a) XRD spectra of S-WSe2 and original WSe2. b) XPS spectra of W4f, c) Se3d, d) Na2p in S-WSe2. e) SEM diagram, f) TEM diagram. g) HR-TEM diagram of S-WSe2, h) interlayer distance profile. i) HAADF-STEM diagram and mapping of S-WSe2.

Figure 2. Electrochemical performance testing of S-WSe2 and WSe2. a) The CV curve of S-WSe2 at 0.25V-1.95V at a scanning rate of 0.50mVs-1, b) the discharge-charge curve at a current density of 100mAg-1, c) the constant current intermittent titration (GITT) curve, d) the ratio performance comparison with other typical RABs cathode materials, e) the electrochemical impedance spectroscopy (EIS) curve and its fitting results, f) the long-term cycle stability of S-WSe2 at 500mAg-1, g) Cyclic stability test of S-WSe2 at a high current density of 2Ag-1.

Figure 3. Study on the reaction mechanism of S-WSe2 cathode in RABs.

In this study, a superlattice type S-WSe2 was proposed as a typical positive electrode and its performance as an aluminum battery positive electrode was studied. It was found that its long-term stability was greatly improved. Through DFT simulation verification, introducing anionic organic layer (SDBS) into S-WSe2 can not only inhibit crystal strain, improve crystal stability, reduce active material dissolution, but also expand interlayer space, reduce diffusion energy barrier, and improve diffusion kinetic behavior. Accordingly, S-WSe2 exhibits the best cycle stability and significantly enhanced magnification performance in TMDCs. At the same time, the reaction mechanism of the superlattice type S-WSe2 electrode was revealed in detail through various in-situ/non in-situ characterization. In summary, this superlattice structure and organic intercalation strategy have opened up a new direction for overcoming the inherent weaknesses of RABs and developing highly stable electrodes.

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