Latest ArticlesThe extraction of radioactive minor actinides (An(Ⅲ)) from lanthanides (Ln(Ⅲ)) is an extremely important step in nuclear waste reprocessing. Designing ligands with high-performance actinide-selectivity remains an essential task. Recent works have reported that some polyazole based ligands exhibit good An(Ⅲ)/Ln(Ⅲ) separation performance. Herein, we first evaluated the effects of different polyazole side chains on the Am(Ⅲ)/Eu(Ⅲ) selectivity by exploring three pyridine-derived polyazole ligands L1, L2 and L3 with 1,2,4-triazole, 1,2,3-triazole, and pyrazole side chains, respectively, using scalar relativistic theoretical methods. The coordination structures, bonding properties and thermodynamic behaviors of AmL(NO3)3 and EuL(NO3)3 complexes were investigated, which clarifies that the side chains do affect the electronic structure of ligand and its selectivity for Am(Ⅲ)/Eu(Ⅲ) ions. Moreover, L1 with 1,2,4-triazole side chains exhibited the highest selectivity for Am(Ⅲ) over Eu(Ⅲ) while the lowest complexation ability for metal ions among the three pyridine-derived polyazole ligands. Subsequently, we designed a new ligand L4 containing 1,2,4-triazole side chains and a preorganized phenanthroline backbone. Theoretically, such a new ligand was verified to show stronger complexation ability and higher selectivity for Am(Ⅲ)/Eu(Ⅲ) ions than L1. This work clarifies the complexation nature of polyazole based ligands with Am(Ⅲ)/Eu(Ⅲ) ions and provides design strategies for highly efficient polyazole based ligands for An(Ⅲ)/Ln(Ⅲ) separation.
As a powerful noninvasive imaging technology, positron emission tomography (PET) has been playing an important role in disease theranostics and drug discovery. The successful application of PET relies on not only the biological properties of PET tracers but also the availability of facile and efficient radiochemical reactions to enable practical production and widespread use of PET tracers. Most recently, photochemistry is emerging as a novel, mild and efficient approach to generating PET agents. In this review, we focus on the recent advances in newly developed photocatalytic radiochemical reactions, innovation on automated photochemical radiosynthesis modules, as well as implementation in late-stage radiolabeling and radiopharmaceutical synthesis for PET imaging. We believe that this review will inspire the development of more promising radiolabeling protocols for the preparation of clinically useful PET agents.
The self-assembled structures of H3BDA molecule with multiple meta-dicarboxylic groups and their stimulus responses to the guest molecules (COR and T4PT) are thoroughly investigated by scanning tunneling microscopy (STM). STM observations display that two kinds of nanostructures are fabricated by H3BDA molecules through intermolecular hydrogen bonds, in which a linear structure is formed at a higher concentration and a flower-like structure is obtained at a lower concentration. After the addition of COR and T4PT, H3BDA appears different responsiveness resulting in different co-assembled structures, respectively. The linear structure is regulated into a flower-like structure by COR and COR molecules are trapped in the cavities. When the pyridine derivative (T4PT) is introduced, a new bicomponent porous structure emerges via the hydrogen bond formed between the carboxyl group and the pyridine. Furthermore, the deposition of additional COR to the H3BDA/T4PT system results in the breakdown of the porous structure and the generation of H3BDA/COR host–guest system. Combined with density functional theory (DFT) calculations and molecular dynamics (MD) simulations, the transformation phenomenon of bi-component nanostructure induced by guest molecules is formulated. The results are expected to understand the modification effect of guest molecules on the host network, which is of great significance for the design and construction of multi-component nanostructures and crystal engineering.
An eco-friendly and practical method for the clean preparation of 5-amino-1,2,4-thiadiazoles was developed. With WS2 as the semiconductor photocatalyst, both TEMPO and O2 (in air) as the redox catalysts, a variety of thiadiazoles were semi-heterogeneously formed in high to quantitative yields and could be easily collected by CPME extraction and rinsing. Furthermore, the catalytic system can be reusable for at least 5 reaction runs.
Heterogeneous porous carbon (PC) materials have gained unique importance in the catalysis community due to their captivating properties, including high specific surface area, tunable porosity, and functionality. PC can play a prominent role in the sustainable synthesis of functional heterocycles, as they are a low-cost alternative while being an efficient and user-friendly material. This review examines the preparation and applicability of these carbonaceous materials used as catalysts or support for biologically active heterocycles synthesis, including hydrogenation, oxidation, oxidative dehydrogenation, cross-coupling, and other organic reactions. Moreover, the challenges, potential future development directions, and opportunities in the synthesis of potent bioactive heterocycles over PC materials have been addressed. This review will inspire further research to explore novel PC materials and their implications in heterocyclization.
The selective 2e− ORR reaction on polymeric carbon nitride framework is one of the most promising approaches for solar-driven hydrogen peroxide production. Poly(heptazine imide) (PHI) as a class of K+-incorporated crystalline carbon nitride framework, is highly active for photocatalytic H2O2 production. An upgrade on the H2O2 photoproduction performance of PHI is realized and the mechanistic insights are revealed in this work. By photochemical reaction, the electron withdrawing groups of hydroxyl group and cyano group are grafted on the surface of PHI frameworks. The dual polarization sites on the surface contribute significantly to the enhancement of the exciton dissociation. The optimized PHI with dual polarization sites exhibits a remarkable photocatalytic H2O2 production performance, which is 2 times of the active pristine PHI. Most importantly, the photochemical reaction method is generally applicable to improve the exciton dissociation of a wide range of polymeric carbon nitride frameworks with various structure and compositions; and the thiourea-derived polymeric carbon nitride framework with dual surface polarization sites exhibits a remarkable photocatalytic performance with a high H2O2 production rate of 40.5 mmol h−1 g−1.
The concentration of metallic elements is closely associated with overall health. However, the discharge of untreated industrial wastewater can lead to metal-containing pollutants entering the human body through the food chain, disrupting the organism's homeostasis and posing a risk to human health. Covalent organic framework materials (COFs) have emerged as a novel porous material for detecting or adsorbing metal ions due to their unique pore structure, topological structure and flexible design. This paper summarizes the role, toxicity, and sources of metal ions related to human health, as well as the design, synthesis and performance of COFs fluorescent materials for detecting these elements. The interaction mechanism of different fluorescent COFs and metal ions are discussed. Additionally, the remaining challenges and prospects of COFs fluorescence sensors are provided. We believe this review will be useful in directing the development of fluorescent COFs towards metal ions.
Recently, organic-inorganic hybrid metal halides (HMHs) have attracted extensive attention as promising multifunctional materials by virtue of their structural diversity and tunable photophysical properties. However, it remains a challenge to design HMHs with specific functions on demand. Herein, by introducing R/S-methylbenzylamine (R/S-MBA) and doping Sb3+, we have achieved both second harmonic generation (SHG) and circularly polarized luminescence (CPL) properties in lead-free indium halides. The introduction of chiral organic cations can break the symmetry and induce the indium halides to crystallize in the chiral space group. The Sb3+ with ns2 electronic configuration can serve as the dopants to promote the formation of self-trapped excitons, so as to activate highly efficient luminescence. As a result, the as-prepared Sb3+ doped (R/S-MBA)3InCl6 show not only SHG responses but also CPL signals with luminescence dissymmetry factor of −5.3 × 10−3 and 4.7 × 10−3. This work provides a new inspiration for the exploitation of chiral multifunctional materials.
Electrocatalysis is a surface-sensitive process, in which the catalytic activity of electrocatalyst highly relates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the catalytically active sites. Surface chemical microenvironment engineering via organic molecules functionalization is a promising strategy to tune the electrocatalytic activity since it can well modify the electrode/electrolyte interface and alter the reaction pathways. In this review, we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules functionalization, with the special focus on the organic molecule-assisted growth mechanism and unique electronic effect. More importantly, the applications of organic molecule functionalized catalysts in various electrocatalytic reactions are also systematically summarized, along with a deep discussion on the conclusion and perspective. This work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.
Satisfactory ionic conductivity, excellent mechanical stability, and high-temperature resistance are the prerequisites for the safe application of solid polymer electrolytes (SPEs) in all-solid-state lithium metal batteries (ASSLMBs). In this study, a novel poly(m-phenylene isophthalamide) (PMIA)-core/poly(ethylene oxide) (PEO)-shell nanofiber membrane and the functional Li6.4La3Zr1.4Ta0.6O12 (LLZTO) ceramic nanoparticle are simultaneously introduced into the PEO-based SPEs to prepare composite polymer electrolytes (CPEs). The core PMIA layer of composite nanofibers can greatly improve the mechanical strength and thermal stability of the CPEs, while the shell PEO layer can provide the 3D continuous transport channels for lithium ions. In addition, the introduction of functional LLZTO nanoparticle not only reduces the crystallinity of PEO, but also promotes the dissociation of lithium salts and releases more Li+ ions through its interaction with the Lewis acid-base of anions, thereby overall improving the transport of lithium ions. Consequently, the optimized CPEs present high ionic conductivity of 1.38×10−4 S/cm at 30 ℃, significantly improved mechanical strength (8.5 MPa), remarkable thermal stability (without obvious shrinkage at 150 ℃), and conspicuous Li dendrites blocking ability (> 1800 h). The CPEs also both have good compatibility and cyclic stability with LiFePO4 (> 2000 cycles) and high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) (> 500 cycles) cathodes. In addition, even at low temperature (40 ℃), the assembled LiFePO4/CPEs/Li battery still can cycle stably. The novel design can provide an effective way to exploit high-performance solid-state electrolytes.
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