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The interactions between uranium and non‐innocent organic species are an essential component of fundamental uranium redox chemistry. However, they have seldom been explored in the context of multidimensional, porous materials. Uranium‐based metal–organic frameworks (MOFs) offer a new angle to study these interactions, as these self‐assembled species stabilize uranium species through immobilization by organic linkers within a crystalline framework, while potentially providing a method for adjusting metal oxidation state through coordination of non‐innocent linkers. We report the synthesis of the MOF NU‐1700, assembled from U4+‐paddlewheel nodes and catecholate‐based linkers. We propose this highly unusual structure, which contains two U4+ ions in a paddlewheel built from four linkers—a first among uranium materials—as a result of extensive characterization via powder X‐ray diffraction (PXRD), sorption, transmission electron microscopy (TEM), and thermogravimetric analysis (TGA), in addition to density functional theory (DFT) calculations. [ABSTRACT FROM AUTHOR]

Defect engineering has emerged as an effective approach for modulating the electronic structure and physicochemical properties of carbon materials. Porous carbon materials with abundant defects are regarded as prospective electrode materials for capacitive deionization. Nevertheless, constructing defect-rich carbon materials and revealing the relationship between desalination capacity and intrinsic defects remains a daunting challenge. Herein, the defect-rich interconnected hierarchical porous carbon (IHPC) was fabricated via sol-gel method to form a supramolecular hydrogel containing highly dispersed K+ using coal, polyvinylpyrrolidone, and KOH as raw materials, followed by homogeneous activation. The spectroscopic studies coupled with density functional theory calculations demonstrate that the introduction of intrinsic defects can optimize the distribution of electron density to promote charge transfer, thereby enhancing saline ions adsorption. The plentiful adsorption sites, robust charge transfer kinetics and rapid ion diffusion derived from the multiple advantageous characteristics of IHPC facilitate a high desalination capacity of 31.25 mg g−1 in 800 mg L−1 NaCl solution. Meanwhile, it also presented excellent desalination performances in KCl (31.42 mg g−1), CaCl 2 (29.55 mg g−1), and MgCl 2 (26.65 mg g−1) solutions. The higher desalination capacity, rapid salt adsorption rate as well as outstanding cycling stability rank the IHPC as a potential candidate for capacitive deionization applications. • Defect-rich interconnected hierarchical porous carbons (IHPC) were prepared by homogeneous activation strategy. • Interconnecting hierarchical porous structures and abundant defects provide an abundance of adsorption sites. • The IHPC electrode reveals superior desalination capacity of 31.25 mg g−1 and high stability. [ABSTRACT FROM AUTHOR]

[Display omitted] The structural defects and oxygen-containing functional groups of carbon materials as electrode materials for supercapacitors or capacitive deionization devices are critical to their electrochemical performance. The tuning of surface oxygen-containing functional groups and carbon defects during pyrolysis is key to achieve a high performance in ion storage. Herein, quinonyl-dominant defective porous carbon is prepared by a pyrolysis and cross-linking route using lavender stem and potassium acetate as precursor. Benefiting from the presence of abundant defect and surface quinonyl groups, porous carbon shows an ultra-high specific capacitance of 401 F g−1 (1 A g−1) and a high capacitance retention of 63% at a high current density of 100 A g−1 in a KOH solution. Meanwhile, as a capacitive deionization electrode material, it also exhibited a high adsorption capacity of 25.5 mg g−1 in 500 mg L-1 NaCl solution at 1.2 V. Theoretical density functional theory (DFT) calculation demonstrates that surface quinonyl groups and carbon defects can synergistically facilitate the adsorption of K+ and Na+ during the charge/discharge process. This work provides a new perspective for understanding the role of surface oxygen-containing groups and intrinsic defects of porous carbon materials in electrochemical energy storage and desalination applications. [ABSTRACT FROM AUTHOR]