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The selective removal of the β‐emitting pertechnetate ion (99TcO4−) from nuclear waste streams is technically challenging. Herein, a practical approach is proposed for the selective removal of 99TcO4− (or its surrogate ReO4−) under extreme conditions of high acidity, alkalinity, ionic strength, and radiation field. Hollow porous N‐doped carbon capsules loaded with ruthenium clusters (Ru@HNCC) are first prepared, then modified with a cationic polymeric network (R) containing imidazolium‐N+ units (Ru@HNCC‐R) for selective 99TcO4− and ReO4− binding. The Ru@HNCC‐R capsules offer high binding affinities for 99TcO4−/ReO4− under wide‐ranging conditions. An electrochemical redox process then transforms adsorbed ReO4− to bulk ReO3, delivering record‐high removal capacities, fast kinetics, and excellent long‐term durability for removing ReO4− (as a proxy for 99TcO4−) in a 3 m HNO3, simulated nuclear waste‐Hanford melter recycle stream and an alkaline high‐level waste stream (HLW) at the U.S. Savannah River Site (SRS). In situ Raman and X‐ray absorption spectroscopy (XAS) analyses showed that adsorbed Re(VII) is electrocatalytically reduced on Ru sites to a Re(IV)O2 intermediate, which can then be re‐oxidized to insoluble Re(VI)O3 for facile collection. This approach overcomes many of the challenges associated with the selective separation and removal of 99TcO4−/ReO4− under extreme conditions, offering new vistas for nuclear waste management and environmental remediation. [ABSTRACT FROM AUTHOR]

Seawater contains uranium at a concentration of ≈3.3 ppb, thus representing a rich and sustainable nuclear fuel source. Herein, an adsorption–electrocatalytic platform is developed for uranium extraction from seawater, comprising atomically dispersed indium anchored on hollow nitrogen‐doped carbon capsules functionalized with flexible amidoxime moieties (In–Nx–C–R, where R denotes amidoxime groups). In–Nx–C–R exhibits excellent uranyl capture properties, enabling a uranium removal rate of 6.35 mg g−1 in 24 h, representing one of the best uranium extractants reported to date. Importantly, In–Nx–C–R demonstrates exceptional selectivity for uranium extraction relative to vanadium in seawater (8.75 times more selective for the former). X‐ray absorption spectroscopy (XAS) reveals that the amidoxime groups serve as uranyl chelating sites, thus allowing selective adsorption over other ions. XAS and in situ Raman results directly indicate that the absorbed uranyl can be electrocatalytically reduced to an unstable U(V) intermediate, then re‐oxidizes to U(VI) in the form of insoluble Na2O(UO3·H2O)x for collection, through reversible single electron transfer processes involving InNx sites. These results provide detailed mechanistic understanding of the uranium extraction process at a molecular level. This work provides a roadmap for the adsorption–electrocatalytic extraction of uranium from seawater, adding to the growing suite of technologies for harvesting valuable metals from the earth's oceans. [ABSTRACT FROM AUTHOR]

Preorganization is a basic design principle used by nature that allows for synergistic pathways to be expressed. Herein, a full account of the conceptual and experimental development from randomly distributed functionalities to a convergent arrangement that facilitates cooperative binding is given, thus conferring exceptional affinity toward the analyte of interest. The resulting material with chelating groups populated adjacently in a spatially locked manner displays up to two orders of magnitude improvement compared to a random and isolated manner using uranium sequestration as a model application. This adsorbent shows exceptional extraction efficiencies, capable of reducing the uranium concentration from 5 ppm to less than 1 ppb within 10 min, even though the system is permeated with high concentrations of competing ions. The efficiency is further supported by its ability to extract uranium from seawater with an uptake capability of 5.01 mg g−1, placing it among the highest‐capacity seawater uranium extraction materials described to date. The concept presented here uncovers a new paradigm in the design of efficient sorbent materials by manipulating the spatial distribution to amplify the cooperation of functions. [ABSTRACT FROM AUTHOR]

We demonstrated that the oxygen reduction reaction (ORR) activity over catalysts derived from pyrolyzed cobalt zeolitic imidazolate frameworks (ZIFs) depends strongly on the imidazole ligand structure and cobalt content. The activity and durability of these catalysts were tested in the proton exchange membrane fuel cell for the first time. The membrane electrode assembly containing a catalyst derived from Co/Zn bimetallic ZIF at the cathode achieved an open-circuit voltage of 0.93 V, a current density of 28 mA cm−2 at 0.8 V iR-free, and a peak power density of 374 mW cm−2. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs) are an emerging class of functional nanostructures with intriguing properties, due to their unprecedented combination of high crystallinity, tunable pore size, large surface area, and unique molecular architecture. The range of properties characterized in COFs has rapidly expanded to include those of interest for numerous applications ranging from energy to environment. Here, a background overview is provided, consisting of a brief introduction of porous materials and the design feature of COFs. Then, recent advancements of COFs as a designer platform for a plethora of applications are emphasized together with discussions about the strategies and principles involved. Finally, challenges remaining for this type material for real applications are outlined. Covalent organic frameworks (COFs) are porous crystalline polymers with tunable composition and structural architecture, enabling precise control over functionality, density, and spatial arrangement. This universal control makes them a particularly promising platform for task‐led design. Recent advancements of COFs for numerous applications are reviewed and the challenges and opportunities associated with processing and large‐scale synthesis are discussed. [ABSTRACT FROM AUTHOR]

Covalent organic frameworks (COFs) are an emerging class of functional nanostructures with intriguing properties, due to their unprecedented combination of high crystallinity, tunable pore size, large surface area, and unique molecular architecture. The enormous possible design space available within COFs provides virtually unlimited room for imagination, allowing designed incorporation of different functionalities. In article number 1801410, Qi Sun, Shengqian Ma, and co‐workers review the recent advancements of COFs for numerous applications. [ABSTRACT FROM AUTHOR]