Latest ArticlesIn the physiological environment, nanoparticles (NPs) interact with proteins to form a protein-rich layer on the surface which is called "protein corona". Understanding and analyzing the formation process of protein corona and protein corona-nanoparticles is of great significance for biological related nano research. Many separation techniques have been used to analyze the composition of protein corona, but in situ analysis of protein corona is still absent. With the development of detection technology, sum frequency generation (SFG) is an effective instrument to analyze the surface protein structure and dynamic changes of protein corona in situ. In this work the molecular mechanism and surface structure effect of the interaction between nanoparticles with surface protein corona (S-NPP) and phospholipid membrane were studied. When S-NPP interacts with phospholipid membrane, the bond affinity network formed by the binding water can stabilize S-NPP around the lipid bilayer. In this process, S-NPP can be found wrapped in the hydration shell. This ultimately leads to a more moderate interaction between particles and phospholipid membrane.
Melanoma is one of the most malignant skin tumors, whose high invasion is generally associated with BRAF gene mutation. Although new chemotherapeutic drugs, such as vemurafenib, have been developed to inhibit the growth of melanoma, these drugs are usually administered intravenously or orally, resulting in toxic side effects on major tissues and organs. Tetrahedral framework nucleic acids (tFNAs) are a novel type of DNA nanostructures with excellent biocompatibility and versatility which have been proven to penetrate through skin barrier with ease. In this study, we prepared tFNAs with vemurafenib and connected DNA aptamer AS1411 at the apex of tFNAs (AS1411-tFNAs/vemurafenib). On one hand, AS1411-tFNAs/vemurafenib could kill melanoma cells by blocking the mutated BRAF gene in vitro. Compared with free vemurafenib, AS1411-tFNAs/vemurafenib had no obvious toxicity to normal cells. On the other hand, AS1411-tFNAs could transfer vemurafenib to cross through the skin barrier and permeate into tumor tissues. In vivo, transdermal delivery of AS1411-tFNAs/vemurafenib could inhibit the growth of human A375 melanoma, whose inhibiting effect was stronger than intravenous administration of vemurafenib. These results demonstrated the application prospects of tFNAs combined with chemotherapeutic drugs in skin tumors.
Due to the high electrophilic nature of azo-dienophiles, azo-Diels–Alder proceeds rapidly even without the need of a catalyst and is therefore regarded as the "click reaction". This spontaneity causes strong background reaction and poses a daunting challenge to chemists for developing the catalytic asymmetric version. Reported herein is the first catalytic asymmetric dearomative azo-Diels–Alder reaction between 2-vinylindoles and triazoledione. This protocol makes use of the high energy barrier of dearomatization to avert the strong background reaction of azo-Diels–Alder reaction, allowing the implementation of the projected reaction at ambient temperature. Density functional theory calculations have been performed to gain insights into the reaction mechanism and the origins of the enantioselectivity. By using this method, a variety of tetracyclic indole derivatives have been readily prepared in good to excellent yields and with excellent diastereo- and enantio-selectivities (33 examples, up to 97% yield and > 99% ee, > 20:1 dr).
The electric field-induced irreversible domain wall motion results in a ferroelectric (FE) hysteresis. In antiferroelectrics (AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis, the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr, Sn, Ti)O3 AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.
Photoacoustic agents combining photodynamic therapy (PDT) and photothermal therapy (PTT) functions have emerged as potent theranostic agents for combating cancer. The molecular approaches for enhancing the near-infrared (NIR)-absorption and maximizing non-radiative energy transfer are essential for effective photoacoustic imaging (PAI) and therapy applications. In addition, such molecules with high specificity and affinity to cancer cells are urgently needed, which would further decrease the side effect during treatments. In this study, we applied a heavy-atom engineering strategy and introduced p-aminophenol, -thio, and -seleno moieties into NIR heptamethine cyanine (Cy7) skeleton (Cy7-X-NH2, X = O, S, Se) to significantly increase photothermal conversion efficiency for PTT and promote intersystem crossing for PDT. Additionally, we designed a series of nitroreductase (NTR)-activated photoacoustic probes (Cy7-X-NO2, X = O, S, Se), and target hypoxic tumors with NTR overexpression. Our prostate cancer targeting probe, Cy7-Se-NO2-KUE, exhibited specific tumor photoacoustic signals and effective tumor killing through outstanding synergistic PTT/PDT in vivo. These findings highlighted a versatile strategy for cancer photoacoustic diagnosis and enhanced phototherapy.
Liposomes are one of the significant classes of antitumor nanomaterials and the most successful nanomedicine drugs in clinical translation. However, it is difficult to accurately reveal liposome delivery modes and drug release rates at different pH values to assess the biodistribution and drug delivery pathways in vivo. Here, we established a strategy to integrate Bi-doped carbon quantum dots (CQDs) with liposomes to produce fluorescence visualization and therapeutic effects, namely lipo/Bi-doped CQDs. Lipo/Bi-doped CQDs show good water solubility and physicochemical properties, which can be used for in vitro labeling of colon cancer (CT26) cells and in vivo imaging localization tracking tumors for monitoring. Simultaneously, thanks to the excellent pH sensitivity and ion doping characteristic of Bi-doped CQDs, lipo/Bi-doped CQDs can be used to reveal the drug release rate of liposomes at different pH values and exhibit potential effects in vivo antitumor therapy.
Humans have relied on biomass for survival and development since the Stone Age. All aspects of human needs for materials are covered by tools, fuel, and buildings. Nowadays, metals and petroleum-based materials are widely used in highly developed industries. Unfortunately, environmental contamination and the loss of natural resources have led to the reemergence of biomass resources as efficient and sustainable energy sources. Notably, simple and direct applications can no longer meet the demand for functionalization, high performance of materials and construction materials. Therefore, it is imperative to modify biomass and combine its utilisation to produce functionalization and high performance materials. For example, construction materials with superior mechanical properties and water resistance can be produced by reinforcing fibres to facilitate crosslinking. Water-oil separation or adsorption effects of hydrogels and aerogels are determined by the porosity and lightness of biomass, biocomposite conductor is prepared by chimaeric conductive material. Here, we review the approaches that have been taken to devise an environmentally friendly yet fully recyclable and sustainable functionalised biocomposites from biomass and its potential directions for future research.
One of the largest subfamilies within the famous Daphniphyllum alkaloid family is made up of the yuzurimine-type (or macrodaphniphyllamine-type) alkaloids. Their complex aza-polycyclic caged structures, several contiguous stereogenic centers, and vicinal all-carbon quaternary centers make these alkaloids formidable challenge for synthetic chemists. Recently, synthesis of these alkaloids has received extensive attention from our community. Herein, we wish to report the total synthesis of C14–epi-deoxycalyciphylline H, a putative member of yuzurimine-type alkaloid subfamily. Key transformations employed in our approach include an intramolecular Prins reaction and a Pd-catalyzed enyne cycloisomerization. In addition, synthesis of a daphnezomine L-type alkaloid, paxdaphnidine A, was also studied.
Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed PdPt nanoalloy onto ferrite perovskite (PdPt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy (O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd4+ is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd2+/Pd shell and metallic solid-solution core structure. The density function theory (DFT) calculations further buttress that the dissociation of CH was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.
Electrochemical nitrogen reduction reaction (ENRR) provides a promising strategy to achieve sustainable synthesis of ammonia. However, despite great efforts devoted to this research field, the problems such as low energy efficiency and weak selectivity still impede its practical implementation. Most of the research to date has been concentrated on creating sophisticated electrocatalysts, and adequate knowledge of electrolytes is still lacking. Herein, the recent progress in electrolytes for ENRR, including alkaline, neutral, acidic, water-in-salt, organic, ionic liquid, and mixed water-organic electrolytes, is thoroughly reviewed to obtain an in-depth understanding of their effects on electrocatalytic performance. Recently developed representative electrocatalysts in various types of electrolytes are also introduced, and future research priorities of different electrolytes are proposed to develop new and efficient ENRR systems.
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