Latest ArticlesRhodium (Rh) has received widespread attention in fundamental catalytic research and numerous industrial catalytic applications. Compared to homogeneous catalysts, Rh-based nanomaterials as heterogeneous catalysts are much easier to separate and collect after usage, making them more suitable for commercial use. To this purpose, there has been a constant demand in constructing stable and highly active Rh-based nanomaterials. In contrast to Rh-based solid solutions with a random distribution of metallic atoms in the lattice, Rh-based intermetallic compounds (IMCs) with a fixed stoichiometric ratio and an ordered atomic arrangement can ensure the homogenous distribution of active sites and structural stability in the catalytic process. In this review, we concentrate on the fabrication of Rh-based IMCs for catalytic applications. Various synthetic methods and protocols for the controlled preparation of Rh-based IMC are illustrated. Meanwhile, the catalytic applications and corresponding catalytic mechanisms are discussed. In addition, personal perspectives about the remaining challenges and prospects in this field are provided. We believe this review will be useful in directing the development of Rh-based IMC catalysts for heterogeneous catalysis.
Fluorescent materials that respond to multiple stimuli have broad applications ranging from sensing and bioimaging to information encryption. Herein, we report the design and synthesis of a single-fluorophore-based amphiphile DCSO, which shows temperature-, solvent-, humidity-, and radiation-dependent fluorescence. DCSO consists of a dicyanostilbene (DCS) group as a rigid hydrophobic core with oligo(ethylene glycol) (OEG) chains at both ends as a flexible hydrophilic periphery. The DCS group acts as a highly efficient fluorophore, while the OEG chain endows the molecule with thermo-responsiveness. Fluorescent colors can vary from blue to green to yellow in response to external stimuli. On the basis of light radiation, we demonstrate that this system can be applied to time-dependent information encryption, in which the correct information can only be read at a specific time under irradiation. This work further demonstrates the usefulness and application of single-fluorophore-based luminescent materials with multiple stimuli-responsive functions.
Tumor angiogenesis is closely related to tumor development, immune escape, and drug resistance. Therefore, the development of effective anti-tumor angiogenesis drugs is of great research significance. Although the current clinical angiogenesis inhibitors have achieved certain efficacy, they also pose the problems of limited and short duration of efficacy, drug resistance, and intrinsic toxicity. Anti-tumor angiogenesis strategies targeting endothelial cells (ECs) have attracted widespread attention in the development of highly effective and low toxicity anti-angiogenesis inhibitors. Studies have verified that the trace element selenium (Se) can inhibit tumor growth by inhibiting tumor angiogenesis through different mechanisms. Nevertheless, it is unclear whether Se speciation has different effects on anti-tumor angiogenesis. Herein, we found that Se exhibited effective anti-angiogenic activity, and its mechanisms of activity were determined by its chemical speciation. Organic Se can significantly inhibit tumor angiogenesis by targeting thioredoxin reductase (TrxR) to trigger cell apoptosis and cell cycle arrest and by increasing reactive oxygen species (ROS) production in ECs. Inorganic Se can induce cell cycle arrest and increase ROS production in ECs, showing promising anti-angiogenic effects. Se nanoparticles (SeNPs) slightly inhibit tumor angiogenesis by inducing apoptosis and cell cycle arrest and by increasing the production of ROS. In summary, this study elucidates the anti-angiogenic activity of Se speciation control with a view to providing a scientific reference for the design and development of novel Se-based highly effective and low toxicity angiogenesis inhibitors.
A new cooperative nickel reductive catalysis and N,N-dimethylformamide-mediated strategy for umpolung C–S radical reductive cross coupling of S-(trifluoromethyl)arylsulfonothioates with alkyl halides to produce alkyl aryl thioethers is described. This reaction features excellent selectivity, wide functionality tolerance, broad substrate scope, and facile late-stage modification of biologically relevant molecules. Mechanistic studies recognize initial generation of an amidyl radical anion via thermoinduced reduction of DMF with Sn, followed by umpolung reduction and single electron transfer of the nucleophilic sulfonyl moiety to form a sulphydryl radical and engage the Ni0/NiⅠ/NiⅢ/NiⅠ catalytic cycle.
Condensed-phase synthesis of atomically precise clusters has become a vital branch of cluster science, where solvents are indispensable in the synthesis process. Herein, by employing the density functional theory (DFT) calculations and molecular dynamics (MD) simulations, we demonstrated that polar solvents not only provide an important environment to stabilize clusters, but they can also dramatically alter the electronic property of cluster anions forming novel superhalogen anions. Such a regulation effect was first verified in small model gas-phase pure and doped gold cluster anions, which was further evidenced in a real experimentally synthesized Au18 nanocluster. Different solvation models reveal that the solvent field, which is a noninvasive methodology different from conventional electron-counting rules, can be considered as a novel external field to remarkably increase the electron-binding capability of cluster anions while maintaining their geometrical and electronic structures. Considering the indispensability and convenient availability of the solvents, present findings may boost the potential applications of superatoms in constructing super oxidizers in the condensed phase.
To address the insulating nature and the shuttle effect of iodide species that would deteriorate the battery performance, herein iron nitride is well-dispersed into porous carbon fibers with good flexibility via the facile electrospinning method and subsequent pyrolysis. The polyacrylonitrile precursor introduces the nitrogen doping under thermal treatment while the addition of iron acetylacetonate leads to the in-situ formation of iron nitride among the carbon matrix. The crucial pyrolysis procedure is adjustable to determine the hierarchical porous structure and final composition of the novel carbon fiber composites. As the self-supporting electrode for loading iodine, the zinc-iodine battery exhibits a large specific capacity of 214 mAh/g and good cycling stability over 1600 h. In the combination of in-situ/ex-situ experimental measurements with the theoretical analysis, the in-depth understanding of intrinsic interaction between composited support and iodine species elucidates the essential mechanism to promote the redox kinetics of iodine via the anchoring effect and electrocatalytic conversion, thus improving cycling life and rate performance. Such fundamental principles on the basic redox conversion of iodine species would evoke the rational design of advanced iodine-based electrodes for improving battery performance.
Silver selenide thin film is one of the best candidates for thermoelectric devices. In the previous report, we demonstrated that high-performanced [201] oriented β-Ag2Se thin films can be prepared by direct metal surface element reaction (DMSER) solution selenization in a really short time at room temperature. However, the underlying mechanism of the fast reaction process were not discussed in depth. Herein, based on hard soft acid base (HASB) theory and strong oxidation, we further explored the possible reaction mechanism of the in-situ growth of β-Ag2Se thin films as the function of the reaction time. The time-dependent experimental results showed that the formation of the β-Ag2Se on elemental Ag precursor (~690 nm thick) in Se/Na2S precursor solution is in a growth driven mode with no obvious orientation or growth rate selections to the elemental Ag precursors. Our investigations provide a prerequisite for the further preparation of thermoelectric materials with excellent properties.
Finding more effective and safe non-viral vectors to transfer genes into cancer cells has become the key of immune gene therapy for cancer. Herein a triblock compound MPEG2000–PDLLA4000–MPEG2000 modified by cationic liposome DOTAP was used as a non-viral vector DOTAP/MPEG2000–PDLLA4000–MPEG2000 (DMPM) to effectively transfer interleukin (IL)-12 plasmid (pIL-12) into tumor tissue. IL-12 produced by transfected tumor cells successfully inducing lymphocyte proliferation and promoting interferon-γ (IFN-γ) secretion, which resulted in tumor cells death. The ability of DMPM to transfer pIL-12 and the immune effect induced by IL-12 in cells had been explored. The anti-tumor effect, mechanism and safety of pIL-12/DMPM in mice cancer model were investigated in this study. Our results showed that the pIL-12 transferred by DMPM was highly expressed both in CT26 cells and B16-F10 cells. IL-12 expressed in the culture supernatant of transfected tumor cells stimulated lymphocyte proliferation and promoted IFN-γ secretion. The experimental result confirmed that pIL-12/DMPM therapy significantly reduced tumor growth in mice model. We designed the nanocomposite DMPM to deliver pIL-12 for cancer treatment and explored its therapeutic efficacy and the underlying anti-tumor mechanism. Our study suggested pIL-12 loaded by DMPM complex would be an effective strategy for cancer treatment.
Benzene is a volatile organic compound that can seriously harm human health, while it can serve as a precursor to produce chemicals of more complex structures in chemical industry. Capturing benzene using adsorbents is of great importance for human health, when the separation of hydrocarbons including benzene from crude oil was referred to as one of the “seven chemical separations to change the world”. In this work, we reported the efficient and selective separation of benzene from BTX and cyclohexane by hydrogen bonding self-assembly nonporous adaptive crystals AdaOH for the first time under mild and user-friendly conditions. Separation of benzene and cyclohexane (v/v = 1:1) can be achieved by AdaOH with a purity of benzene up to 96.8%. Separation of BTX (v/v; benzene:toluene:o-xylene:m-xylene:p-xylene= 1:1:1:1:1) can be achieved by AdaOH with a purity of benzene increased from 20% to 82.9%. Our results suggest that separation of benzene using the activated AdaOH as a non-porous adaptive crystal for selectively and efficiently capturing benzene can solve the challenge in separation of benzene from other chemicals such as cyclohexane in chemical industry, and can be helpful for removal of benzene that is released from the vehicles to air. The advantages of commercially availability, easy preparation, high separation efficiency and selectivity for benzene might endow this material with enormous potential for practical uses in areas like petrochemical industry.
The abuse of antibiotics has brought great harm to the human living environment and health, so it is extremely significant to develop an efficient and simple method to detect trace antibiotic residues in various wastewaters. Herein, a new two-dimensional (2D) Cd-based metal−organic framework (Cd-MOF, namely LCU-111) and its mixed matrix membranes (MMMs) is sifted as luminescence sensors for efficient monitoring antibiotic nitrofurazone (NFZ) in various aqueous systems and applied as visible fingerprint identifying. The LCU-111 has good selectivity, sensibility, reproducibility and anti-interference for luminescent quenching NFZ with low detection limits (LODs) of 0.4567, 0.3649 and 0.8071 ppm in aqueous solution, HEPES biological buffer, and real urban Tuhai River water, respectively. Interestingly, the luminescent test papers and MMMs allow the NFZ sensing easier and more rapid by naked eyes, only with a low LOD of 0.8117 ppm for MMMs sensor. Notably, by combining multiple experiments with density functional theory (DFT) calculations, the photo-induced electron transfer (PET) quenching mechanism is further elucidated. More importantly, potential practical applications of LCU-111 for latent fingerprint visualization provide lifelike evidences for effective identification of individuals, which can be applied in criminal investigation.
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