Lithium–sulfur batteries are recognized as one of the most promising next‐generation energy‐storage technologies owing to their high energy density and low cost. Nevertheless, the shuttle effect of polysulfide intermediates and the formation of lithium dendrites are the principal reasons that restrict the practical adoption of current Li–S batteries. Adjustable frameworks, structural variety, and functional adaptability of covalent organic frameworks (COFs) have the potential to overcome the issues associated with Li–S battery technology. Herein, a summary is presented of emerging COF materials in addressing the challenging problems in terms of sulfur hosts, modified separators, artificial solid electrolyte interphase layers, and solid‐state electrolytes. This comprehensive overview focuses on the design and chemistry of COFs used to upgrade Li–S batteries. Furthermore, existing difficulties, prospective remedies, and prospective research directions for COFs for Li–S batteries are discussed, laying the groundwork for future advancements in this class of fascinating materials.

Covalent Organic Framework Based Lithium–Sulfur Batteries: Materials, Interfaces, and Solid‐State Electrolytes

Ionic conduction plays a critical role in the process of electrode reactions and the charge transfer kinetics in a rechargeable battery. Covalent organic frameworks (COFs) have emerged as an exciting new class of ionic conductors, and have made great progress in terms of their application in rechargeable batteries. The unique features of COFs, such as well‐defined directional channels, functional diversity, and structural robustness, endow COF‐based conductors with a low ionic diffusion energy barrier and excellent temperature tolerance, which are much superior to the classic inorganic or polymer conductors. Here, a comprehensive analysis and summary of the unique ion‐conducting behavior of COF‐based conductors are presented, and the design principles for ion‐conducting COFs are emphasized. Moreover, a systematic overview of the recent progress in the development of ion‐conducting COFs serving as electrodes, separators, solid electrolytes, and artificial interphase materials for diverse battery applications, such as metal‐ion batteries, lithium metal batteries, lithium–sulfur batteries, lithium–CO2 batteries, zinc–air batteries, etc., is proposed. This review is expected to provide theoretical guidance for design of novel kinds of ionic conductor bearing intrinsic framework structures and to boost further research enthusiasm for ion‐conducting COFs in rechargeable batteries.

Covalent Organic Framework for Rechargeable Batteries: Mechanisms and Properties of Ionic Conduction

Redox-active covalent organic frameworks (COFs) have recently emerged as advanced electrodes in polymer batteries. COFs provide ideal molecular precision for understanding redox mechanisms and increasing the theoretical charge-storage capacities. Furthermore, the functional groups on the pore surface of COFs provide highly ordered and easily accessible interaction sites, which can be modeled to establish a synergy between ex situ/in situ mechanism studies and computational methods, permitting the creation of predesigned structure–property relationships. This perspective integrates and categorizes the redox functionalities of COFs, providing a deeper understanding of the mechanistic investigation of guest ion interactions in batteries. Additionally, it highlights the tunable electronic and structural properties that influence the activation of redox reactions in this promising organic electrode material.

https://pubs.acs.org/doi/pdf/10.1021/jacs.3c01131

Covalent Organic Frameworks as Model Materials for Fundamental and Mechanistic Understanding of Organic Battery Design Principles

Porous Organic Polymers with Defined Morphologies: Synthesis, Assembly, and Emerging Applications

Lithium metal batteries are highly desired for durable and high‐power energy storage devices due to high theoretical capacity and lowest redox potential. Nevertheless, high activity of Li, large volume change, and Li dendrite formation during cycling severely hinder their further application. Herein, an inventive Cu collector decorated with holey MoO2‐Mo3N2 heterojunction nanobelts‐coated reductive graphene oxide (G‐MoO2‐Mo3N2, GMM) for high‐performance Li metal batteries is reported. The collector features synergistic functions of remarkable lithiophilicity, a built‐in electric field formed by splendid interfacial contact, and dense lithiophilic‐enriched solid electrolyte interphase layer. They facilitate robust charge transfer and ionic diffusion, and meliorate inhomogenous Li‐ion flux for inhibiting the growth of dendrites. In addition, the incorporation of flexible graphene layer enhances the structural integrity and electron transport kinetics. Remarkably, it is demonstrated that GMM significantly enhances Coulombic efficiency of ≈99.5% over 1566 cycles (0.5 mA cm−2/0.5 mAh cm−2). Furthermore, excellent cycling and rate capability of full cells with the GMM@Cu anode and high areal loading of LiFePO4 cathode (22.2 mg cm−2) are also realized. This work illustrates the superiority of synergetic design of lithiophilic sites plus electron transport kinetics for the current collector of Li‐metal anode to seek the high energy density.

Lithiophilic Interphase Porous Buffer Layer toward Uniform Nucleation in Lithium Metal Anodes

Highly Stable Lithium Metal Anode Enabled by Lithiophilic and Spatial-Confined Spherical-Covalent Organic Framework

Self-Exfoliated Covalent Organic Framework Nano-mesh Enabled Regular Charge Distribution for Highly Stable Lithium Metal Battery

Copper-involved highly efficient oxygen reduction reaction in both alkaline and acidic media

Palladium‐catalyzed long‐range isomerization of aryl olefins

Herein, a smartphone-based portable reader with integrated optics for standard microtiter plates (96 wells) has been designed and demonstrated for high-throughput quantitation of validated biomarkers in serum. The customized optical attachment was simply constructed with a convex lens and a light source, by which the transmitted light through a 96-well microtiter plate was converged for imaging with a smartphone, so that accurate and wide-range reading of the plate can be achieved. More importantly, relying on the digitized colorimetric analysis of the obtained images, concentrations of various biomarkers can be determined directly using the customized mobile app. A set of validated biomarkers for inflammation and infection, C-reactive protein (CRP), serum amyloid A (SAA), and procalcitonin (PCT) have been quantitated with this new system; both the response ranges and limits of detection meet the requirement of clinical tests. The consistency with the results obtained using a commercial microplate reader proves its reliability and precision, augments its potential as a point-of-care diagnostic device for on-site testing or resource-limited settings.

Smartphone-based microplate reader for high-throughput quantitation of disease markers in serum.

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