Abstract
Silicon (Si) is a promising anode material to realize many-fold higher anode capacity in next-generation lithium-ion batteries (LIBs). Si electrochemistry has strong dependence on the property of the Si interface, and therefore, Si surface engineering has attracted considerable research interest to address the challenges of Si electrodes such as dramatic volume changes and the high reactivity of Si surface. Molecular nanostructures, including metal–organic frameworks (MOFs), covalent–organic frameworks (COFs) and monolayers, have been employed in recent years to decorate or functionalize Si anode surfaces to improve their electrochemical performance. These materials have the advantages of facile preparation, nanoscale controllability and structural diversity, and thus could be utilized as versatile platforms for Si surface modification. This review aims to summarize the recent applications of MOFs, COFs and monolayers for Si anode development. The functionalities and common design strategies of these molecular structures are demonstrated.
Highlights
Applications of Molecular StructuresMobile power systems have become fundamental components in the operation of modern society
1027.8 mAh g−1 at the rate of 1 A g−1 over 500 cycles (79% retention). Another metal–organic frameworks (MOFs) used for Si anodes is Prussian blue analogues (PBAs) [65], where the PBA-derived carbon coating helped the Si nanocomposite to present a reversible capacity of 725 mAh g–1 after 200 cycles
1864 mAh g−1 capacity at a high rate of 2 A g−1 after 1000 cycles with a retention ratio of about 60% (Figure 3c). These results demonstrate that covalent–organic frameworks (COFs) coating is an effective strategy to protect Si materials to reduce electrolyte decomposition and solid electrolyte interphase (SEI) formation, and to realize good electrochemical performance of Si anodes
Summary
Mobile power systems have become fundamental components in the operation of modern society. Molecular structures fabricated in a bottom-up manner are attractive alternatives for engineering Si electrodes. Such materials include metal–organic frameworks (MOFs), covalent–organic frameworks (COFs) and monolayers, which could be readily prepared in a self-organized manner, often under relatively mild conditions or via spontaneous reactions [34,35,36]. These types of materials have well-defined molecular structures and two-dimensional (2D) or three-dimensional (3D) nano-ordered configurations. Detailed descriptions of each material are provided in the corresponding sections, along with their properties and applications
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