Two series of lanthanide metal–organic frameworks (Ln-MOFs) from two structurally related flexible carboxylate-based ligands were solvothermally synthesized. H3L2 with additional −CH2− group provides more flexibility and different coordination modes and conformations compared with H3L1. As a result, 2-Ln MOFs are modulated from two-dimensional kgd of 1-Ln to three-dimensional rtl topological frameworks and further achieve enhanced chemical stability. The Eu- and Tb-MOFs exhibit strong fluorescent emission at the solid state because of the antenna effect of the ligands. Interestingly, the emissions can be tuned by simply doping Eu3+ and Tb3+ of different concentrations within the Eu x Tb 1–x MOFs. Notably, 2-Ln MOFs realize nearly white light emission by means of a trichromatic approach (red of Eu(III), green of Tb(III), and blue of the H3L2 ligand). Furthermore, 2-Ln MOFs also exhibit water stability and demonstrate high selective and sensitive sensing activities toward Fe(III) and Cr(VI) in aqueous solutions. The results further highlight the importance of the ligand flexibility on tuning MOF structures with improved structural stability and ion-sensing properties.
The Gag protein of human immunodeficiency virus type 1 directs the virion assembly process. Gag proteins must extensively multimerize during the formation of the spherical immature virion shell. In vitro, virus-like particles can be generated from Gag proteins that lack the N-terminal myristic acid modification or the nucleocapsid (NC) protein. The precise requirements for Gag-Gag multimerization under conditions present in mammalian cells, however, have not been fully elucidated. In this study, a Gag-Gag multimerization assay measuring fluorescence resonance energy transfer was employed to define the Gag domains that are essential for homomultimerization. Three essential components were identified: protein-protein interactions contributed by residues within both the N-and C-terminal domains of capsid (CA), basic residues in NC, and the presence of myristic acid. The requirement of myristic acid for multimerization was reproduced using the heterologous myristoylation sequence from v-src. Only when a leucine zipper dimerization motif was placed in the position of NC was a nonmyristoylated Gag protein able to multimerize. These results support a threecomponent model for Gag-Gag multimerization that includes membrane interactions mediated by the myristoylated N terminus of Gag, protein-protein interactions between CA domains, and NC-RNA interactions.
The construction of an efficient oxygen reduction reaction and oxygen evolution reaction (ORR/OER) bifunctional electrocatalyst is of great significance but still remains a giant challenge for high-performance metal−air batteries. In this study, uniform FeS/Fe 3 C nanoparticles embedded in a porous N,S-dual doped carbon honeycomb-like composite (abbr. FeS/Fe 3 C@NS-C-900) have been conveniently fabricated by pyrolysis of a single-crystal Fe-MOF, which has a low potential gap ΔE of ca. 0.72 V, a competitive power density of 90.9 mW/cm 2 , a specific capacity as high as 750 mAh/g Zn , and excellent cycling stabilities over 865 h (1730 cycles) at 2 mA/cm 2 when applied as a cathode material for rechargeable zinc−air batteries. In addition, the two series-linked Zn−air batteries successfully powered a 2.4 V LED light as a real power source. The efficient ORR/OER bifunctional electrocatalytic activity and longterm durability of the obtained composite might be attributed to the characteristic honeycomb-like porous structure with sufficient accessible active sites, the synergistic effect of FeS and Fe 3 C, and the N,S codoped porous carbon, which provides a promising application potential for portable electronic Zn−air battery related devices.
Rationale: Ferroptosis is a regulated process of cell death caused by iron-dependent accumulation of lipid hydroperoxides (LPO). It is sensitive to epithelial-to-mesenchymal transition (EMT) cells, a well-known therapy-resistant state of cancer. Previous studies on nanomaterials did not investigate the immense value of ferroptosis therapy (FT) in epithelial cell carcinoma during EMT. Herein, we describe an EMT-specific nanodevice for a comprehensive FT strategy involving LPO burst.Methods: Mitochondrial membrane anchored oxidation/reduction response and Fenton-Reaction-Accelerable magnetic nanophotosensitizer complex self-assemblies loading sorafenib (CSO-SS-Cy7-Hex/SPION/Srfn) were constructed in this study for LPO produced to overcome the therapy-resistant state of cancer. Both in vitro and in vivo experiments were performed using breast cancer cells to investigate the anti-tumor efficacy of the complex self-assemblies.Results: The nano-device enriched the tumor sites by magnetic targeting of enhanced permeability and retention effects (EPR), which were disassembled by the redox response under high levels of ROS and GSH in FT cells. Superparamagnetic iron oxide nanoparticles (SPION) released Fe2+ and Fe3+ in the acidic environment of lysosomes, and the NIR photosensitizer Cy7-Hex anchored to the mitochondrial membrane, combined sorafenib (Srfn) leading to LPO burst, which was accumulated ~18-fold of treatment group in breast cancer cells. In vivo pharmacodynamic test results showed that this nanodevice with small particle size and high cytotoxicity increased Srfn circulation and shortened the period of epithelial cancer treatment.Conclusion: Ferroptosis therapy had a successful effect on EMT cells. These findings have great potential in the treatment of therapy-resistant epithelial cell carcinomas.
The shuttle effect of polysulfides and Li2S sluggish nucleation are the major problems hampering the further development of lithium–sulfur batteries. The reasonable design for sulfur host materials with catalytic function has been an effective strategy for promoting polysulfide conversion. Compared with other types of transition metal compounds, transition metal borides with high conductivity and catalytic capability are more suitable as sulfur host materials. Herein, a niobium diboride (NbB2) nanoparticle with abundant and high-efficiency catalytic sites has been synthesized by facile solid-phase reaction. The NbB2 with both high conductivity and catalytic nature could regulate 3D-nucleation and growth of Li2S, decrease the reaction energy barrier, and accelerate the transformation of polysulfides. Thus, the NbB2 cathode could retain a high capacity of 1014 mAh g–1 after 100 cycles. In addition, the high initial specific capacities of 703/609 mAh g–1 are also achieved at 5 C/10 C and could run for 1000/1300 cycles within a low decay rate of 0.057%/0.051%. Even with a high sulfur loading up to 16.5 mg cm–2, an initial areal capacity of 17 mAh cm–2 could be achieved at 0.1 C. This work demonstrates a successful method for enhancing the kinetics of polysulfide conversion and directing Li2S nucleation.
The removal of C2H2 and C2H6 from C2H4 streams is of great significance for feedstock purification to produce polyethylene and other commodity chemicals but the simultaneous adsorption of C2H6 and C2H2 over C2H4 from a ternary mixture has never been realized. Herein, a robust metal–organic framework, TJT‐100, was designed and synthesized, which demonstrates remarkably selective adsorption of C2H2 and C2H6 over C2H4. Breakthrough experiments show that TJT‐100 can be used as an adsorbent for high‐performance purification of C2H4 from a ternary mixture of C2H2/C2H4/C2H6 (0.5:99:0.5) to afford a C2H4 purity greater than 99.997 %, beyond that required for ethylene polymerization. Computational studies reveal that the uncoordinated carboxylate oxygen atoms and coordinated water molecules pointing towards the pore can trap C2H2 and C2H6 through the formation of multiple C−H⋅⋅⋅O electrostatic interactions, while the corresponding C2H4–framework interaction is unfavorable.
By using the reduced Schiff base tricarboxylate ligand H 3 cip, one novel 3D Cd-based coordination polymer (Cd-CP) with the formula [Cd(Hcip)(bpea) 0.5 (H 2 O)] n (H 3 cip = 5-(3-carboxybenzylamino)isophthalic acid, bpea = 1,2-bis(4-pyridyl)ethane) has been solvothermally synthesized. The prepared Cd-CP possesses a 4-connected CdSO 4 net based on dinuclear {Cd 2 } units. Luminescence measurements revealed that the complex exhibited ratiometric turn-on luminescence responses toward Al 3+ and Cr 3+ with a significant color change, which could be easily distinguished by the naked eye under ultraviolet light. Cd-CP can also respond to Fe 3+ through a turn-off mechanism. Interestingly, the luminescence quenched by Fe 3+ @Cd-CP can be recovered and increased significantly by adding some competitive Al 3+ , while Cr 3+ can only marginally increase the luminescence intensity of Fe 3+ @Cd-CP. Moreover, the detection of the three aforementioned metal ions can be realized by using Cd-CP-coated test papers, extending the potential application regions of the reported material to point-of-care tests and environmental field studies.
B-cell abnormality including excessive activation and lymphopenia is a central feature of systemic lupus erythematosus (SLE). Although activation threshold, auto-reaction and death of B cells can be affected by intrinsical and/or external signaling, the underlying mechanisms are unclear. Herein, we demonstrate that co-activation of Toll-like receptor 7 (TLR7) and B-cell receptor (BCR) pathways is a core event for the survival/dead states of B cells in SLE. We found that the mortalities of CD19+CD27- and CD19+IgM+ B-cell subsets were increased in the peripheral blood mononuclear cells (PBMCs) of SLE patients. The gene microarray analysis of CD19+ B cells from active SLE patients showed that the differentially expressed genes were closely correlated to TLR7, BCR, apoptosis, necroptosis and immune pathways. We also found that co-activation of TLR7 and BCR could trigger normal B cells to take on SLE-like B-cell characters including the elevated viability, activation and proliferation in the first 3 days and necroptosis in the later days. Moreover, the necroptotic B cells exhibited mitochondrial dysfunction and hypoxia, along with the elevated expression of necroptosis-related genes, consistent with that in both SLE B-cell microarray and real-time PCR verification. Expectedly, pretreatment with the receptor-interacting protein kinase 1 (RIPK1) inhibitor Necrostatin-1, and not the apoptosis inhibitor zVAD, suppressed B-cell death. Importantly, B cells from additional SLE patients also significantly displayed high expression levels of necroptosis-related genes compared with those from healthy donors. These data indicate that co-activation of TLR7 and BCR pathways can promote B cells to hyperactivation and ultimately necroptosis. Our finding provides a new explanation on B-cell lymphopenia in active SLE patients. These data suggest that extrinsic factors may increase the intrinsical abnormality of B cells in SLE patients.
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