Limited by single metal active sites and low electrical conductivity, designing nickel‐based metal–organic framework (MOF) materials with high capacity and high energy density remains a challenge. Herein, a series of bi/multimetallic MOF‐74 family materials in situ grown on carbon cloth (CC) by doping Mx+ ions in Ni‐MOF‐74 is fabricated: NiM‐MOF@CC (M = Mn2+, Co2+, Cu2+, Zn2+, Al3+, Fe3+), and NiCoM‐MOF@CC (M = Mn2+, Zn2+, Al3+, Fe3+). The type and ratio of doping metal ions can be adjusted while the original topology is preserved. Different metal ions are confirmed by X‐ray absorption fine structure (XAFS). Furthermore, these Ni‐based MOF electrodes are directly utilized as cathodes for aqueous nickel–zinc batteries (NZBs). Among all the as‐prepared electrodes, NiCo‐MOF@CC‐3 (NCM@CC‐3), with an optimized Co/Ni ratio of 1:1, exhibits the best electrical conductivity, which is according to the density functional theory (DFT) theoretical calculations. The NCM@CC‐3//Zn@CC battery achieves a high specific capacity of 1.77 mAh cm–2, a high areal energy density of 2.97 mWh cm–2, and high cycling stability of 83% capacity retention rate after 6000 cycles. The synthetic strategy based on the coordination effect of metal ions and the concept of binder‐free electrodes provide a new direction for the synthesis of high‐performance materials in the energy‐storage field.

In Situ Synthesis of MOF‐74 Family for High Areal Energy Density of Aqueous Nickel–Zinc Batteries

The employment of weak intermolecular interactions in supramolecular chemistry offers an alternative approach to project artificial chemical environments like the active sites of enzymes. Discrete molecular architectures with defined shapes and geometries have become a revolutionary field of research in recent years because of their intrinsic porosity and ease of synthesis using dynamic non-covalent/covalent interactions. Several porous molecular cages have been constructed from simple building blocks by self-assembly, which undergoes many self-correction processes to form the final architecture. These supramolecular systems have been developed to demonstrate numerous applications, such as guest stabilization, drug delivery, catalysis, smart materials, and many other related fields. In this respect, catalysis in confined nanospaces using such supramolecular cages has seen significant growth over the years. These porous discrete cages contain suitable apertures for easy intake of substrates and smooth release of products to exhibit exceptional catalytic efficacy. This review highlights recent advancements in catalytic activity influenced by the nanocavities of hydrogen-bonded cages, metal-ligand coordination cages, and dynamic or reversible covalently bonded organic cages in different solvent media. Synthetic strategies for these three types of supramolecular systems are discussed briefly and follow similar and simplistic approaches manifested by simple starting materials and benign conditions. These examples demonstrate the progress of various functionalized molecular cages for specific chemical transformations in aqueous and nonaqueous media. Finally, we discuss the enduring challenges related to porous cage compounds that need to be overcome for further developments in this field of work.

Molecular Cavity for Catalysis and Formation of Metal Nanoparticles for Use in Catalysis.

Porous organic cages (POCs) are a relatively new class of low-density crystalline materials that have emerged as a versatile platform for investigating molecular recognition, gas storage and separation, and proton conduction, with potential applications in the fields of porous liquids, highly permeable membranes, heterogeneous catalysis, and microreactors. In common with highly extended porous structures, such as metal–organic frameworks (MOFs), covalent organic frameworks (COFs), and porous organic polymers (POPs), POCs possess all of the advantages of highly specific surface areas, porosities, open pore channels, and tunable structures. In addition, they have discrete molecular structures and exhibit good to excellent solubilities in common solvents, enabling their solution dispersibility and processability—properties that are not readily available in the case of the well-established, insoluble, extended porous frameworks. Here, we present a critical review summarizing in detail recent progress and breakthroughs—especially during the past five years—of all the POCs while taking a close look at their strategic design, precise synthesis, including both irreversible bond-forming chemistry and dynamic covalent chemistry, advanced characterization, and diverse applications. We highlight representative POC examples in an attempt to gain some understanding of their structure–function relationships. We also discuss future challenges and opportunities in the design, synthesis, characterization, and application of POCs. We anticipate that this review will be useful to researchers working in this field when it comes to designing and developing new POCs with desired functions.

https://doi.org/10.1021/acs.chemrev.2c00667

Porous Organic Cages

Metal–organic frameworks and derived materials as photocatalysts for water splitting and carbon dioxide reduction

Post-synthetic modifications of metal–organic cages

Catalysis within coordination cages

Controlling the growth of metal-organic frameworks (MOFs) at the micro-/nanoscopic scale will result in new physical properties and novel functions into the materials without changing the chemical identities and the characteristic features of the MOFs themselves. Herein, we report a facile approach to synthesize a series of MOFs [Co-MOF, CoxNiy-MOFs (x and y represent the molar ratio of Co2+ and Ni2+ and x/y = 1:1, 1:5, 1:10, 1:15, and 1:20), and Ni-MOF] with a one-dimensional micro-/nanoscaled rod-like architecture. From Co-MOF to CoxNiy-MOFs to Ni-MOF, the diameters of the rods turn to be spindly with the increase of Ni2+ content which will facilitate the supercapacitor performances. Interestingly, Co1Ni20-MOF exhibits a highest specific capacity of 597 F g-1 at 0.5 A g-1 and excellent cycle performance (retained 93.59% after 4000 cycles) among these MOF materials owing to its micro-/nanorod structure with a smaller diameter and the synergy effect between the optimum molar ratio of Co2+ and Ni2+.

From Co-MOF to CoNi-MOF to Ni-MOF: A Facile Synthesis of 1D Micro-/Nanomaterials.

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Catalysis within coordination cages

From Co-MOF to CoNi-MOF to Ni-MOF: A Facile Synthesis of 1D Micro-/Nanomaterials.