Latest ArticlesPlatinum (Pt) nanoparticle catalysts remain the most popular cathode materials for oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. Non-metallic alloying of Pt has become an emerging strategy to improve electrocatalytic performance, however, the electrocatalytic ORR mechanisms still need to be understood for further improvement toward practical application. Herein, a rapid microwave reduction method is employed for alloying phosphorous (P) into Pt to form a carbon supported phosphorus-alloyed Pt nanoparticle catalyst (P-Pt/C), which demonstrates the ability to replace commercial Pt/C. By a combination of density functional theory calculations and in-situ electrochemical Raman spectroscopy, the regulation role of P-alloying in the electrocatalytic mechanisms is revealed. It is found that the nearby Pt atoms can convert the ORR pathway from associative one to dissociative one, exhibiting a spontaneous dissociation of *OOH intermediate to *OH and *O species as well as a change of potential determining step to *O protonation. Furthermore, the strategy of large-scale economic synthesis of such alloying Pt-based catalyst is also established, demonstrated by a gram-level synthesis per batch. This study puts insight into the electrocatalytic ORR fundamentals of Pt-alloying with non-metals and provides a basis for the reasonable design and synthesis of efficient nonmetals-alloyed Pt catalysts.
Carbon materials have long been a subject of study, offering diverse properties based on their hybridized structures. Except sp2-hybridized graphene and carbon nanotubes, the focus on sp1-hybridized carbon chains has garnered significant interest due to its unique predicted properties, despite limitations in research and development stemming from its high reactivity. This comprehensive review summaries recent advancements in synthetic methodologies and characterization of the sp1-hybridized carbon chains, encompassing linear carbon chains and cyclo[n]carbons. The review traces significant milestones in synthesis and offers a thorough overview of various properties on linear and cyclic carbon chains, from their initial discovery to recent development. The advancing synthetic methods have led to practical breakthroughs, transitioning theoretical concepts into tangible carbon-chain materials. However, challenges persist in achieving controlled and scalable preparation due to the high reactivity associated with sp1-hybridization. Future research prospects focus on fundamental studies, such as exploring the transition length from polyyne to carbyne and experimentally determining the properties of single carbon chains. This review underscores both the progress made and the compelling avenues for future exploration in the dynamic field of sp1-hybridized carbon chains.
Molecular recognition of fullerene using various host compounds is well-known in literature. But most studies focus on host-guest complexation in solution using host compounds with a single binding cavity. Herein, we report a series of highly preorganized janusarene derivatives with homoditopic binding sites. These novel janusarenes can bind and align various fullerenes such as C60, C70, C84, and Gd@C82 in a highly efficient manner. Robust shape complementary association and assembly are observed in solution, in the bulk solid state, in the liquid crystalline state, or on surface, and the assembled structures are characterized by nuclear magnetic resonance (NMR) titration, X-ray diffraction, polarized optical microscopy, and scanning tunneling microscopy.
Developing high-efficient and low-loading Pt based catalyst is significant for the electrocatalytic pH-universal hydrogen evolution reaction (HER). Herein, the molybdenum carbide nanoparticles supported on the polyhedral N-doped carbon nanotube skeleton (MoC/NCT) composite has been synthesized by a pyrolysis of polyacid organo-metallic phosphate framework precursor. Then, only 2.15 wt% Pt are loaded on the MoC/NCT to form Pt-MoC/NCT catalyst, which performs superior HER activity and stability in entire pH range. Specially, the overpotentials of 22 and 74 mV are respectively attained at 10 mA/cm2 in 1.0 mol/L KOH and 0.5 mol/L H2SO4 electrolytes, approaching or even exceeding commercial Pt/C. More importantly, it can be used as excellent catalyst for efficient hydrogen production at 0–14 pH range. Density functional theory (DFT) calculations demonstrate that the interaction between MoC and Pt leads to the electron redistribution at the corresponding interfaces and the downward shift of the d-band centers, thus optimizing H* adsorption and desorption for promoting the HER activity. Besides, the unique three-dimensional network structure is conductive to the transmission of mass and electrons. In the application of both alkaline and acidic electrolysers, only 1.52 V voltage of solar panel can drive a hydrogen production current density of 10 mA/cm2.
Two dimensional (2D) materials based on boron and carbon have attracted wide attention due to their unique properties. BC compounds have rich active sites and diverse chemical coordination, showing great potential in optoelectronic applications. However, due to the limitation of calculation and experimental conditions, it is still a challenging task to predict new 2D BC monolayer materials. Specifically, we utilized Crystal Diffusion Variational Autoencoder (CDVAE) and pre-trained Materials Graph Neural Network with 3-Body Interactions (M3GNet) model to generate novel and stable BCP materials. Each crystal structure was treated as a high-dimensional vector, where the encoder extracted lattice information and element coordinates, mapping the high-dimensional data into a low-dimensional latent space. The decoder then reconstructed the latent representation back into the original data space. Additionally, our designed attribute predictor network combined the advantages of dilated convolutions and residual connections, effectively increasing the model's receptive field and learning capacity while maintaining relatively low parameter count and computational complexity. By progressively increasing the dilation rate, the model can capture features at different scales. We used the DFT data set of about 1600 BCP monolayer materials to train the diffusion model, and combined with the pre-trained M3GNet model to screen the best candidate structure. Finally, we used DFT calculations to confirm the stability of the candidate structure. The results show that the combination of generative deep learning model and attribute prediction model can help accelerate the discovery and research of new 2D materials, and provide effective methods for exploring the inverse design of new two-dimensional materials.
Visual assessment of tumor metastatic capacity is crucial for predicting hepatocellular carcinoma (HCC) prognosis and guiding clinical therapeutic approaches. In this study, we developed an enzyme-responsive probe based on the peptide GK10, which is selectively cleaved by matrix metalloproteinase-9 (MMP-9), a critical marker for metastasis in HCC. The GK10 peptide was conjugated with near-infrared fluorescent molecule IR783, fluorescent quencher black hole quencher 3 (BHQ3), and magnetic resonance (MR) contrast agent DOTA-Gd, forming the IR783-GK10-BHQ3-Gd probe. Upon MMP-9 cleavage of GK10, BHQ3 is released from the probe, thereby amplifying the previously quenched IR783 fluorescence signal. In vitro experiments demonstrate the probe’s impressive detection limit for MMP-9, as low as 1.84 ng/mL. Moreover, in vivo imaging results reveal that the probe can differentiate liver cancers with varying metastatic capacities. The fluorescence and MR imaging signal intensity of high metastatic HCC are approximately 1.2 times greater than that of low metastatic HCC. Thus, this engineered probe holds promise as a valuable tool for evaluating HCC metastatic capacity through fluorescence-MR dual-mode imaging.
Diabetes mellitus (DM) is a serious health problem in the world, and infections are common complications in diabetic patients, particularly methicillin-resistant Staphylococcus aureus (MRSA) infections, which substantially increases mortality in patients. In clinical practice, the treatment of diabetic complication-related infections involves multiple issues such as drug resistance when combining antidiabetic drugs with antibiotics. In this study, a series of derivatives were synthesized with alkyl radicals with different chain lengths substituted at the C8 and C12 positions of berberine, with compounds CY1 and CY3 with good antidiabetic and antibacterial activities screened out after identification. Then, oral liposomes (CY1-Lip and CY3-Lip) were prepared, and their particle sizes, stability, and pharmacokinetics were investigated. In acquired mouse models of diabetes, induced with an acute MRSA lung infection, we demonstrate that CY1-Lip and CY3-Lip can effectively reduce levels of fasting blood glucose (FBG), fasting insulin (FINS), and insulin resistance index among diabetic mice with pneumonia, thus exerting their multi-targets effects. Furthermore, both preparations significantly reduced lung MRSA loads and improved lung tissue lesions, reduced high infiltration of M1 macrophages in lung, and suppressed the expression levels of pro-inflammatory factors such as necrosis factor-α (TNF-α) and interleukin-6 (IL-6). This provides new insights into the clinical treatment of diabetes complicated with pulmonary infections.
Lung cancer-derived exosomes are a kind of valuable and clinically-predictable biomarkers for lung cancer, but they have the limitations in individual differences when being applied in liquid biopsy. To improve their application value and accuracy in clinical diagnosis, a dual-labelled electrochemical method is herein reported for precise assessment of lung cancer-derived exosomes. To do so, two probes are prepared for the dual labeling of exosome membrane to run DNA assembly reactions: One is modified with cholesterol and can insert into exosome membrane through hydrophobic interaction; another one is linked with programmed death ligand-1 (PD-L1) antibody and can bind to exosome surface-expressing PD-L1 via specific immunoreaction. Quantum dots-tagged signal strands are used to collect respective DNA products, and produce stripping signals corresponding to the amounts of total exosome and surface-expressing PD-L1, respectively. A wide linear relationship is established for the quantitative determination of lung cancer-derived exosomes in the range from 103 to 1010 particles/mL, whereas the ratiometric value of the two stripping signals is proven to have a better diagnostic use in screening and staging of lung cancer when being applied to clinical samples. Therefore, our method might provide a new insight into precise diagnosis of lung cancer, and offer sufficient information to reflect the biomarker level and guide the personalized treatment level even at an early stage in clinic.
Recently, MP-10, a previous drug candidate with potent inhibition of phosphodiesterase 10A (PDE10A) in clinical phase II trials for schizophrenia or Alzheimer's disease, has shown significant potential in preventing and treating cardiovascular diseases. However, its poor metabolic stability and high permeability across the blood-brain barrier (BBB) make it unsuitable for preventing and treating peripheral cardiovascular diseases. Herein, the hit-to-lead optimization was performed to discover novel 3-trifluoromethyl-substituted pyrazole derivatives as potent and selective PDE10A inhibitors. The structure-activity relationships, biological characterization, molecular mechanism, and drug-like evaluation were discussed to identify compound C7 which showed potent inhibition against PDE10A (half maximal inhibitory concentration, IC50 = 11.9 nmol/L), more than 840-fold selectivity over other PDE subtypes, enhanced liver microsomes stability (T1/2 = 239 min) compared to MP-10 and low BBB permeability. Importantly, oral pretreatment with C7·3HCl at a dose of 5.0 mg/kg significantly attenuated the pathological and functional changes induced by isoprenaline (ISO)-induced pathological cardiac hypertrophy in mice, particularly suppressing increase of cardiac weight, atrial natriuretic peptide (ANP) and β-myosin heavy chain (β-MHC) hypertrophic markers along with cardiac fibrosis. These findings further support that targeting PDE10A provides an innovative therapeutic approach for preventing and treating cardiac diseases.
Herein, we report an iron-promoted carbonylation-rearrangement of α-aminoaryl-tethered alkylidene cyclopropanes with CO2 to generate quinolinofuran derivatives. A variety of quinolinofuran derivatives are obtained in moderate to excellent yields, and two promising luminescent material molecules have been synthesized using the developed method. The Lewis acid FeCl3 was introduced into this reaction, which effectively promoted the ring opening and rearrangement of cyclopropanes. This reaction features a broad substrate scope, satisfactory functional group tolerance, facile scalability, and easy derivatization of the products.
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