Aqueous Zn metal batteries have attracted extensive attention due to their intrinsic advantages. However, zinc ions tend to deposit irregularly, seriously depleting the capacity and stability of the battery. The construction of zincophilic sites can effectively regulate the nucleation and growth of Zn, but there is a defect that these sites will be covered with gradual failure after long-term cycling. Here, in combination with the sustained-compensated strategy, interfacial zincophilic sites are continuously constructed, thus effectively avoiding the threat of dendrites and improving the electrochemical performance. Impressively, at 10 mA cm −2 and 5 mAh cm −2 , the protected Zn metal exhibits excellent cycling stability over 2000 cycles in the Zn//Zn battery. Moreover, even the cathode mass loading is considerably high (35 mg cm −2 ), and the Zn//NVO full cell significantly outperforms with high areal capacity (up to 4 mAh cm −2 ). This novel strategy provides a direction for the development of high-capacity aqueous batteries.

Small organic chalcogenides molecules are receiving more attention in conjunction with the development of rechargeable lithium metal batteries (LMBs) especially lithium-sulfur (Li−S) batteries due to their abundant resources, reversible redox, high capacities, tunable structures, unique functional adjustability, and strong interaction with congener polysulfides. In this review, the working principles are generalized of small organo-chalcogenide molecules in three important parts of batteries: electrolyte, interface, and cathode. First, in terms of regulating kinetics in electrolyte, small organochalcogenide molecules can not only act as redox mediator to accelerate the redox kinetics of sulfur, but also change the inherently slow solid-solid process to form a faster redox pathway, which will bring light to the development of cryogenic Li−S batteries. Second, for interface chemistry, the introduction of small organo-chalcogenide molecules can construct more elastic and stable anodic single-SEI or cathodic/anodic dual-SEI, thus effectively improving the cycling stability of batteries. Third, small organo-chalcogenide molecules can be used as cathode materials in the form of liquid phase, solid phase, or precursor of polymers. Finally, advised optimizations are proposed about further mechanism deciphering, battery configuration design, machine learning, thereby providing direction to bridge the gap between rational modulation and practical battery implementation for small organochalcogenide molecules.

To optimize anode and cathode degradation issues in high-voltage (5 V-class) lithium metal batteries (LMBs), robust solid-electrolyte interfaces (SEI) on the surface of both anode and cathode are highly desired. Here, a nonafluorobutane-1-sulfonic acid (NFSA) additive is introduced to assist in the formation of the more stable and robust SEI to protect both anode and cathode. Typically, local high concentrations of lithium nonafluorobutane-1-sulfonate (NFSALi) and nonafluorobutane-1-sulfonate anion (NFSA − ) could be achieved at the surface of anode and cathode respectively, through spontaneous chemical processes. The lowest unoccupied molecular orbital energy of NFSALi is lower and the highest occupied molecular orbital (energy of NFSA − is higher than electrolyte solvents. Thus, conformal and dense SEI passivation films are generated on the surface of both anode and cathode derived from electrochemical decomposition of NFSALi and NFSA − , respectively. Consequently, stable operation of Li metal anode and high-voltage cathode are realized. The LiNi 0.5 Mn 1.5 O 4 (LNMO)//Li LMBs with NFSA-containing electrolyte show great cycling stability with 93% capacity retention after 400 cycles and more stable Coulombic efficiency. This work specifies the double functions of NFSA as an interfacial layer forming additive to solve the degradation problems of high-voltage (5 V-class) LMBs, enabling high-energy LMBs with significantly improved battery performance.