Developing a conductive catalyst with high catalytic activity is considered to be an effective strategy for improving cathode kinetics of lithium–sulfur batteries, especially at large current density and with lean electrolytes. Lattice‐strain engineering has been a strategy to tune the local structure of catalysts and to help understand the structure–activity relationship between strain and catalyst performance. Here, Co0.9Zn0.1Te2@NC is constructed after zinc atoms are uniformly doped into the CoTe2 lattice. The experimental/theoretical results indicate that a change of the coordination environment for the cobalt atom by the lattice strain modulates the d‐band center with more electrons occupied in antibonding orbitals, thus balancing the adsorption of polysulfides and the intrinsic catalytic effect, thereby activating the intrinsic activity of the catalyst. Benefiting from the merits, with only 4 wt% dosages of catalyst in the cathode, an initial discharge capacity of 1030 mAh g−1 can be achieved at 1 C and stable cycling performances are achieved for 1500/2500 cycles at 1 C/2 C. Upon sulfur loading of 7.7 mg cm−2, the areal capacity can reach 12.8 mAh cm−2. This work provides a guiding methodology for the design of catalytic materials and refinement of adsorption‐catalysis strategies for the rational design of cathode in lithium–sulfur batteries.
Improving the intrinsic catalytic activity of electrocatalysts is considered to be the "gold standard" to inhibit the shuttle effect in Li-S batteries. The question of how to expose active sites for anchoring and catalytic conversion of the polysulfides represents the direction of this research. The assembly of 0D nanoparticles or 2D nanosheets into 3D spherical superstructure is one of the problems of materials synthesis. Here, a spherical superstructure hafnium diboride derived from metal-organic framework (MOF) nanoparticles is synthesized by one-step borification. Benefiting from its unique superstructure, the obtained HfB 2 exhibits excellent catalytic activity for the conversion of polysulfide. Theoretical calculations indicate that the strong spin-orbital coupling property of electron configuration of 5d Hf induces p orbitals of nonmetallic atoms closer to the Fermi level, thus endowing the anions with redox activity and unconventional superconductivity. These merits enable the HfB 2 -based sulfur cathode to deliver a high initial discharge capacity of 1433 mAh g −1 at 0.2 C and 580 mAh g −1 at 5 C. With sulfur loading of 12.8 mg cm −2 and electrolyte dosage of 4 μL mg −1 , the areal capacity can reach 15.5 mAh cm −2 . This work provides a new understanding for designing superstructure borides involving 5d metals in Li-S batteries.
Benefiting from the admirable energy density (1086 Wh kg−1), overwhelming security, and low environmental impact, rechargeable zinc–air batteries (ZABs) are deemed to be attractive candidates for lithium‐ion batteries. The exploration of novel oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) bifunctional catalysts is the key to promoting the development of zinc–air batteries. Transitional metal phosphides (TMPs) especially Fe‐based TMPs are deemed to be a rational type of catalyst, however, their catalytic performance still needs to be further improved. Considering Fe (heme) and Cu (copper terminal oxidases) are nature's options for ORR catalysis in many forms of life from bacteria to humans. Herein, a general “in situ etch‐adsorption‐phosphatization” strategy is designed for the fabrication of hollow FeP/Fe2P/Cu3P‐N, P codoped carbon (FeP/Cu3P‐NPC) catalyst as the cathode of liquid and flexible ZABs. The liquid ZABs manifest a high peak power density of 158.5 mW cm−2 and outstanding long‐term cycling performance (≈1100 cycles at 2 mA cm−2). Similarly, the flexible ZABs deliver superior cycling stability of 81 h at 2 mA cm−2 without bending and 26 h with different bending angles.
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