Lithium–sulfur (Li–S) batteries are recognized as promising candidates for next‐generation electrochemical energy storage systems owing to their high energy density and cost‐effective raw materials. However, the sluggish multielectron sulfur redox reactions are the root cause of most of the issues for Li–S batteries. Herein, a high‐efficiency CoSe electrocatalyst with hierarchical porous nanopolyhedron architecture (CS@HPP) derived from a metal–organic framework is presented as the sulfur host for Li–S batteries. The CS@HPP with high crystal quality and abundant reaction active sites can catalytically accelerate capture/diffusion of polysulfides and precipitation/decomposition of Li2S. Thus, the CS@HPP sulfur cathode exhibits an excellent capacity of 1634.9 mAh g−1, high rate performance, and a long cycle life with a low capacity decay of 0.04% per cycle over 1200 cycles. CoSe nanopolyhedrons are further fabricated on a carbon cloth framework (CC@CS@HPP) to unfold the electrocatalytic activity by its high electrical conductivity and large surface area. A freestanding CC@CS@HPP sulfur cathode with sulfur loading of 8.1 mg cm−2 delivers a high areal capacity of 8.1 mAh cm−2 under a lean electrolyte. This work will enlighten the rational design of structure–catalysis engineering of transition‐metal‐based nanomaterials for diverse applications.
The design of nanostructured electrocatalysts with high activity and long‐term durability for the sluggish lithium polysulfide (LiPS) conversion reaction is essential for the development of high‐performance lithium–sulfur (Li–S) batteries. Here, the self‐assembly of bimetallic selenides on nitrogen‐doped MXene (CoZn‐Se@N‐MX) based on the self‐assembly of metal–organic framework and MXene is reported. A combination of 0D CoZn‐Se nanoparticles and 2D N‐MX nanosheet co‐catalysts forms double lithiophilic‐sulfifilic binding sites that effectively immobilize and catalytically convert LiPS intermediates. This 0D–2D heterostructure catalyst has a hierarchical porous architecture with a large active area and enables rapid Li ion diffusion, reduces the activation energy of Li2S deposition, and lowers the energy barrier of Li2S dissolution. In addition, an assembled CoZn‐Se@N‐MX hybrid synergistically prevents the aggregation of the CoZn‐Se nanoparticles and restacking of the active areas of N‐MX nanosheets during assembly and the LiPS conversion process. The Li–S battery with this 0D–2D catalyst delivers excellent rate capability, ultralong cycling life (over 2000 cycles), and a high areal capacity of 6.6 mAh cm−2 with a low electrolyte/sulfur ratio of 5 µL mg−1.
Metal–organic framework (MOF)-based materials with high porosity, tunable compositions, diverse structures, and versatile functionalities provide great scope for next-generation rechargeable battery applications. Herein, this review summarizes recent advances in pristine MOFs, MOF composites, MOF derivatives, and MOF composite derivatives for high-performance sodium-ion batteries, potassium-ion batteries, Zn-ion batteries, lithium–sulfur batteries, lithium–oxygen batteries, and Zn–air batteries in which the unique roles of MOFs as electrodes, separators, and even electrolyte are highlighted. Furthermore, through the discussion of MOF-based materials in each battery system, the key principles for controllable synthesis of diverse MOF-based materials and electrochemical performance improvement mechanisms are discussed in detail. Finally, the major challenges and perspectives of MOFs are also proposed for next-generation battery applications.
We report the synthesis of a new hierarchical mesoporous TS-1 type zeolite by a simple steam-assisted crystallization method. This novel product exhibits high catalytic activity and a strongly prolonged lifetime in the selective oxidation of 2,3,6-trimethylphenol to trimethyl-p-benzoquinone.
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