Latest ArticlesThe properties of layered double hydroxides (LDHs), including the adjustability of cations in host layers, exchangeability of anions between layers, and tunability of the crystal structure, render them unique characteristics in preparation and applications. Relating to the structural characteristics of LDHs, this work analyzes the research status, advantages and disadvantages of the synthetic methods for LDHs, including hydrothermal, electrodeposition, co-precipitation and anion exchange methods. In addition, the application status and prospects are reviewed, such as photo/electrocatalysis, electrochemical energy storage, magnetic materials, pollutant adsorption, and other fields. Lastly, the critical issues and solutions in the developing process of LDHs are analyzed and proposed.
Four unprecedented sulfur-containing cytochalasans, thiocytochalasins A−D (1−4), were isolated from an endophytic fungus Phoma multirostrata XJ-2-1. Thiocytochalasins A (1) and B (2) feature a novel 5/6/14/5 tetracyclic scaffold, which are the first examples of cytochalasan containing a thiophene moiety. Thiocytochalasins C (3) and D (4) are epimeric cytochalasan homodimers formed via a thioether bridge. Their structures with absolute configurations were established by detailed analysis of the HRESIMS, NMR, and X-ray crystallography. The plausible biogenetic pathway of 1−4 was postulated. Compounds 3 and 4 exhibited significant cytotoxicity against CT26 cells with IC50 values of 0.85 and 0.76 µmol/L, respectively.
The development of organic materials with white-light emission and thermally activated delayed fluorescence (TADF) properties in the solid state remain a challenge. Herein, a series of white-light-emitting organic luminogens have been developed and are found to show aggregation-induced delayed fluorescence (AIDF) characteristics. The AIDF emitters present dual-emission consisted of prompt fluorescence and TADF in the crystalline state. Their white-light emissions can be easily tuned by altering the chemical structure and connecting position of the heterocyclic aromatic substituent. Under the stimuli of mechanical force and solvent vapor, the compounds exhibit remarkable and reversible mechanochromism, in which their emission colors are switchable between white and yellow. Upon grinding, they also display linearly tunable luminescence colors, as well as force-induced TADF enhancement, which may be associated with the more compact molecular packing and the restriction of intramolecular motions. The results from time-resolved emission scanning and theoretical calculation suggest that the dual-emission of the AIDF luminogens likely results from the twisted intramolecular charge transfer transitions of the molecules, and the reversible mechanochromism properties probably stem from the interconversion of the quasi-axial and the quasi-equatorial conformations.
Rechargeable aqueous zinc-ion batteries have attracted extensive interest because of low cost and high safety. However, the relationship between structure change of cathode and the zinc ion storage mechanism is still complex and challenging. Herein, open-structured ferric vanadate (Fe2V4O13) has been developed as cathode material for aqueous zinc-ion batteries. Intriguingly, two zinc ion storage mechanism can be observed simultaneously for the Fe2V4O13 electrode, i.e., classical intercalation/deintercalation storage mechanism in the tunnel structure of Fe2V4O13, and reversible phase transformation from ferric vanadate to zinc vanadate, which is verified by combined studies using various in-situ and ex-situ techniques. As a result, the Fe2V4O13 cathode delivers a high discharge capacity of 380 mAh/g at 0.2 A/g, and stable cyclic performance up to 1000 cycles at 10 A/g in the operating window of 0.2–1.6 V with 2 mol/L Zn(CF3SO3)2 aqueous solution. Moreover, the assembled Fe2V4O13//Zn flexible quasi-solid-state battery also exhibits a relatively high mechanical strength and good cycling stability. The findings reveal a new perspective of zinc ion storage mechanism for Fe2V4O13, which may also be applicable to other vanadate cathodes, providing a new direction for the investigation and design of zinc-ion batteries.
Clear cell renal cell carcinoma (ccRCC) is a heterogeneous malignancy with poor prognosis. Methylation of the N6 position of adenosine (m6A), the most common epigenetic modification in both messenger RNAs and noncoding RNAs, has been reported to regulate the initiation and progression of ccRCC. However, whether and how m6A-related long noncoding RNAs (m6ArlncRNAs) signify the progression of ccRCC remain unclear. We found m6ArlncRNAs are effective signatures illustrating immune landscape and risk stratification in ccRCC. We identified two differently expressed m6ArlncRNAs (DEm6ArlncRNAs), AC008870.2 and EMX2OS, as independent risk factors for overall survival of ccRCC patients, by applying stringent variable selection procedure to data from the Cancer Genome Atlas Kidney Renal Clear Cell Carcinoma project. The risk score generated from the DEm6ArlncRNA expression categorizes patients into either high or low-risk groups, between which, enrichment analysis indicated an enrichment in immunerelated pathways. Under different DEm6ArlncRNA transcription pattern, the two risk groups differ in immune cell population composition and expression levels of therapy targeting genes. Nanoparticle is satisfactory strategy to delivering therapeutic drugs. For further clinical translation, we designed a novel nanoparticle delivery system packaged STM2457 (STM@8P4 NPs), which selectively inhibits AC008870.2- correlated m6A writer. STM@8P4 NPs loaded drug successfully with uniform particle size, long-term stability and high release efficiency. STM@8P4 NPs can easily enter ccRCC cells and showed a highly efficient ccRCC killing activity in vitro. Our results therefore indicate that m6ArlncRNAs expression can depict tumor microenvironment, predict prognosis for ccRCC patient and give hint to therapeutic strategies in ccRCC.
Electrocatalytic nitrogen reduction reaction (NRR) is an environmentally friendly method for sustainable ammonia synthesis under ambient conditions. Searching for efficient NRR electrocatalysts with high activity and selectivity is currently urgent but remains great challenge. Herein, we systematically investigate the NRR catalytic activities of single and double transition metal atoms (TM = Fe, Co, Ni and Mo) anchored on g-C6N6 monolayers by performing first-principles calculation. Based on the stability, activity, and selectivity analysis, Mo2@g-C6N6 monolayer is screened out as the most promising candidate for NRR. Further exploration of the reaction mechanism demonstrates that the Mo dimer anchored on g-C6N6 can sufficiently activate and efficiently reduce the inert nitrogen molecule to ammonia through a preferred distal pathway with a particularly low limiting potential of -0.06 V. In addition, we find that Mo2@g-C6N6 has excellent NRR selectivity over the competing hydrogen evolution reaction, with the Faradaic efficiency being 100%. Our work not only predicts a kind of ideal NRR electrocatalyst but also encouraging more experimental and theoretical efforts to develop novel double-atom catalysts (DACs) for NRR.
In recent years, with the emergence of new pollutants, the effective treatment of wastewater has become very important. Persulfate-based advanced oxidation processes have been successfully applied to the treatment of wastewater, such as wastewater containing antibiotics, pharmaceuticals and personal care products, dyes, endocrine-disrupting chemicals, chlorinated organic pollutants, and phenolics, for the degradation of refractory organic contaminants. This paper summarizes the production of sulfate radicals, which can be generated by the activation of persulfate via conventional and emerging approaches. The existing problems of persulfate-based advanced oxidation processes were analyzed in detail, including residual sulfates, coexisting factors (coexisting inorganic anions and natural organic matter), and energy consumption. This paper proposes corresponding possible solutions to the problems mentioned above, and this paper could provide a reference for the application of persulfate-based advanced oxidation processes in actual wastewater treatment.
By integrating one strain-many compounds (OSMAC) and LC–MS-based molecular networking strategies, distachydrimanes A–F (1–6), six novel phenylspirodrimane dimers and hybrids representing two types of unprecedented terpenoid-polyketide hybrid skeletons, were isolated from the modified fermented rice substrate of a coral-derived fungus Stachybotrys chartarum. All the structures incorporating their absolute configurations were elucidated based on comprehensive spectroscopic analyses, mainly including HRESIMS and NMR data, single-crystal X-ray diffraction (Cu Kα), and comparison of the experimental electronic circular dichroism (ECD) data. Architecturally, compounds 1–6 represent an unprecedented class of dimeric phenylspirodrimanes with an unexpected C-18–C-23′ linkage, of which compounds 1–3 also feature an unexpected 5-methyl-1, 3-benzenediol moiety via a carbon-carbon linkage. The bioactivity assay demonstrated that compounds 1, 5 and 6 induced cell proliferation inhibition, G0/G1 cell cycle arrest, senescence and mitochondrial-mediated apoptosis in L1210 cells, highlighting their potentials as a new category of anticancer agents.
Amino acids are basic units to construct a protein with the assistance of various interactions. During this building process, steric hindrance derived from amino acid side groups or side chains is a factor that could not be ignored. In this contribution, adsorption behaviors of C-terminal amino acid derivatives with amino acid residues fused in 3, 4, 9, 10-perylenetetracarboxylic dianhydride were investigated by scanning tunneling microscopy (STM) and density functional theory (DFT) calculations at various liquid/solid interfaces. STM results at 1-phenyloctane/HOPG interface show that N, N'-3, 4, 9, 10-perylenedicarboximide (GP) and N, N'-methyl-3, 4, 9, 10-perylenedicarboximide (AP) formed linear and herringbone structures, respectively. The driving force could be attributed to different H-bonding sites induced by steric hindrance at side groups. N, N'-Benzyl-3, 4, 9, 10-perylenedicarboximide (PP) generates both linear and herringbone structures because steric hindrance changes the H-bonding sites between PP molecules, whereas N, N'-isopropyl-3, 4, 9, 10-perylenedicarboximide (LP) failed to be imaged because of strong steric hindrance coming from larger side group. To further investigate the impact of steric hindrance, we utilized octanoic acid (OA) as solvent to capture the adsorption details of LP and PP. We found that OA molecules drag PP and LP molecules in a different direction to generate linear structure, impeding the molecular rotation. The structure–solvent relationship shows that the steric hindrance is brought by the large side group, which makes it easier to recognize OA molecules at the interface. These results demonstrate that steric effect plays a significant role in altering interaction sites of the compounds during the adsorption process at the liquid/solid interface.
Improving the utilization of excitons has always been an important topic for the development of electroluminescence devices. In this work, we designed and synthesized three red TADF emitters TPA-DBT12, TPA-DBT3 and DTPA-DBT by employing dibenzothioxanthone (DBT) acceptor framework to stabilize the locally excited triplet state to participate in the reverse intersystem crossing (RISC) process. The fast RISC process and singlet radiation decay process gave rise to evidently enhanced exciton utilization. All of the red OLEDs based on these materials showed maximum EQE over 11% and high exciton utilization close to 100%. This work not only extend the acceptor framework for red materials but also provide a new perspective for the design of highly efficient red TADF materials with 100% exciton utilization by managing locally excited triplet state.
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