Modulated noble metal/2D MOF heterostructures for improved hydrogen storage of MgH2

Abstract 2D metal‐organic frameworks‐based (2D MOF‐related) materials benefit from variable topological structures, plentiful open active sites, and high specific surface areas, demonstrating promising applications in gas storage, adsorption and separation, energy conversion, and other domains. In recent years, researchers have innovatively designed multiple strategies to avoid the adverse effects of conventional methods on the synthesis of high‐quality 2D MOFs. This review focuses on the latest advances in creative synthesis techniques for 2D MOF‐related materials from both the top‐down and bottom‐up perspectives. Subsequently, the strategies are categorized and summarized for synthesizing 2D MOF‐related composites and their derivatives. Finally, the current challenges are highlighted faced by 2D MOF‐related materials and some targeted recommendations are put forward to inspire researchers to investigate more effective synthesis methods. 

Recent Progress in 2D Metal-Organic Framework-Related Materials.

The development of methods for the selective binding and separation of pertechnetate anion from aqueous solutions formed during the reprocessing of spent nuclear fuel remains an extremely urgent task. The lack of acceptable solutions of this problem has become one of the main obstacles to the development of nuclear energetics as one of the main sources of energy not related to emissions of carbon dioxide into the atmosphere. This review discusses recent advances in the creation of effective and highly selective receptors on TcO4−, as well as extractants and sorbents allowing the binding of this anion in aqueous solutions, including in highly aggressive environments. Various approaches solving this problem are analyzed critically. They include precipitation and reductive precipitation of TcO4−, its extraction in two-phase water/organic solvent systems, methods of binding TcO4− on inorganic, composite and organic sorbents of different types, as well as the extraction and sorption characteristics used in this case. The collected data and the results of their discussion can contribute to a deeper understanding of ways to solve remaining unsolved problems in this area and planning directions for its further development. 

Recent progress in separation of technetium-99 from spent nuclear fuel and radioactive waste. Challenges and prospects

Ultrathin covalent organic framework (COF) nanosheets are very appealing 2D materials, but the mass production of ultrathin COF nanosheets remains a great challenge. Here, by using cage-like bicyclocalix[2]arene[2]triazines tri-aldehyde (BCTAL) as the building block, 2D COF Cage-COF-1 was estimated to have a very weak interaction between adjacent layers (around 1/50 compared to that of graphite). As a result, 1.2 nm thick trilayer COF nanosheets were facilely exfoliated from the pristine COFs with large lateral size and high thickness homogeneity. The Cage-COF-1 nanosheet is featured by imine linkage, but it is catalytic inactive in oxygen evolution reaction (OER). After post-metalation with Co2+ under ambient conditions, remarkable catalysis activity and stability was observed for Cage-COF-1-Ns/Co, which has lower overpotential (330 mV) and Tafel slope (56 mV/dec) in catalytic OER compared to many other Co catalysts. This work has confirmed that weakening the interlaminar interaction is an effective strategy for the production of ultra-thin COFs nanosheets. Due to the fully exposed and accessible imine linkage, catalysis active metal site can be controllably produced via post-synthesis from nanosheets under very mild conditions. 

Ultra‐thin Cage‐based Covalent Organic Frameworks Nanosheets as Precursor for Pyrolysis‐Free Oxygen Evolution Reaction Electrocatalyst

Selective anion recognition and extraction in aqueous media is a challenging research topic, and the anion-π interaction is an undetermined solution for the development of anion sorbent materials with better affinity and selectivity. Here, noncovalent anion-π interaction was introduced as the driving force for this purpose. A cage-based 2D cationic metal-organic framework, IPM-21, is featured with porous channels formed by complementary V-shape electron-deficient cavities. This 3D rhombic electron-deficient cavity can bind two anions with the clipped π-acidic surfaces, exhibiting much higher affinity toward ReO4- due to the strong complementary effect. This cavity was forced to expand its opening size to seamlessly adopt the ReO4- anion with a large volume. Experimental results found that the binding energy of IPM-21 with ReO4- is around 2.3 kJ/mol higher than that with ClO4-. Parts per million levels of the ReO4- anion in aqueous media can be effectively extracted by IPM-21 with a removal up to 99%, even with mixed competing anions. IPM-21 can be easily recycled and reused by treatment with high concentration aqueous NaClO4. Due to the extremely low interlamellar interaction, the IPM-21 crystal exhibited enhanced ReO4- extraction performance with the recycling times due to self-exfoliation; as a result, ultrathin IPM-21 nanosheets with large lateral sizes were produced in this process.

Anion-π Interaction Powered Perrhenate Recognition and Extraction in Aqueous Media.

The rational design and preparation of monolayer metal-organic framework (MOF) nanosheets remain great challenges. Recently, we found that monolayer MOF nanosheets can be facially exfoliated on a large scale from pristine two-dimensional (2D) MOFs with substantially reduced interlaminar interaction. By employing cage-like bicyclocalix[2]arene[2]triazine tri-imidazole as the building block, a family of cationic two-dimensional metal-organic frameworks (2D MOFs) with steric layer were designed and prepared. The single crystal structures have clearly identified that only very weak and sparse distributed C-H···π interaction exists between adjacent layers.On the basis of density functional theory calculation, the interlayer interaction of these cage-based cationic 2D MOFs was estimated to be 1/46th of that of graphite. Due to the extremely weak interaction, these cationic 2D MOFs tend to degenerate into an "amorphous" state after being soaked in other solvents; they can be readily exfoliated into 1.1 nm thick monolayer nanosheets with a high degree of thickness homogeneity, large lateral size, and significantly enlarged surface area. This work has identified that a cage-like molecule is the ideal building block for 2D cationic MOFs and ultrathin nanosheets; It was futher confirmed that weakening the interlaminar interaction is an effective strategy for facilely producing monolayer nanosheets.

Monolayer Nanosheets Exfoliated from Cage-Based Cationic Metal-Organic Frameworks.

Solid materials possess both long-range order and some degree of disorder are critical for understanding the nature of crystal and glassy state, but how to controllable introduce specific type of disorder into a crystalline material is a big challenge. Our previous work indicated that weakening the inter-layer interaction is an effective strategy to import disorders between the layers.Here, we illustrated that the inter-layer interaction can be weakened to around 1/60 of that of graphite in the self-assembled material, a two-dimensions frameworks formed by B-C-T-A with Cu nodes, which has an obvious layered-structure.

Self-assembled Frameworks Solid with Turbostratic Stacked Crystalline Layers -- A Frustrated 3D Crystal Lattice

With the modern technological developments in the diagnosis and treatment of cancer, the survival rate of cancer patients has increased. On the other hand, the incidence of multiple primary tumors is increasing annually. Lynch syndrome (LS), an autosomal dominant disorder with germline mutations in DNA mismatch repair genes, increases the risk of cancer in patients carrying those mutations. In this report, we present an extremely rare case of an 81-year-old male patient with eight primary malignancies and LS. The patient is still alive having survived for more than 41 years since the initial discovery of the first tumor. The eighth and most recently diagnosed primary cancer was a malignant peripheral nerve sheath tumor. Although there have been numerous reports of malignancies in LS, malignant peripheral nerve sheath tumors have not been reported previously with LS. Here, we report, to the best of our knowledge, the first case of a malignant peripheral nerve sheath tumor with LS.

/pdf/long-term-survival-of-a-lynch-syndrome-patient-with-eight-2e6o8j3r.pdf

Long-Term Survival of a Lynch Syndrome Patient With Eight Primary Tumors: A Case Report

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