Latest ArticlesThe cell surface membrane proteome is a class of proteins encoded by ~25% of all protein-coding genes in living organisms and plays a key role in mediating communication between the cells and their surrounding environment. However, most cell surface membrane proteins (CSMPs) are naturally expressed at very low levels compared with intracellular proteins. The difficulties in their purification with high specificity further hinder the understanding of their structure and function. In this study, we developed a new photolabeling probe to achieve efficient tagging and facile enrichment of the CSMPs. The probe is composed of a lipid tail for cell surface localization, a polyethylene glycol (PEG) spacer for increased water solubility, two 4-(N-maleimido)benzophenone (MBP) groups for UV-active tagging of the CSMPs, and a biotin tag for subsequent isolation. Application of this photolabeling probe resulted in the successful enrichment and identification of 3098 annotated CSMPs in HT22 cells with close to 70% selectivity. The proposed photolabeling probe and enrichment strategy were demonstrated to be a powerful method for deep cell surface proteome profiling, representing one of the largest groups of current drug targets.
Black phosphorus (BP) as an uprising two-dimensional material exhibits attractive potential in the field of electrocatalysis due to the inherent advantages of high carrier mobility and abundant lone pair electrons. However, the exposed active electrons compel BP to be deactivated by oxidative degradation. Herein, the electronic signature of acceptor-donor heterointerfacial interactions between BP and Co3O4 is realized via wet ball milling. The preferential migration of active electrons from BP to Co3O4 is achieved at the heterointerface since the Fermi level of BP is higher than that of Co3O4. Such relative energetic consideration promotes reasonable oxygen electrocatalytic active sites. Moreover, it significantly suppresses the oxidative degradation of BP. Consequently, the resulting Co3O4/BP heterojunction possesses superior oxygen bifunctional electrocatalytic activity than its parent catalysts. Most importantly, this work promotes an efficient route towards BP-based multifunctional catalysts.
Finding transition metal catalysts for effective catalytic conversion of CO to CO2 has attracted much attention. MXene as a new 2D layered material of early transition metal carbides, nitrides, and carbo-nitrides is a robust support for achoring metal atoms. In this study, the electronic structure, geometries, thermodynamic stability, and catalytic activity of MXene (Mo2CS2) supported single noble metal atoms (NM = Ru, Rh, Pd, Ir, Pt and Au) have been systematically examined using first-principles calculations and ab initio molecular dynamic (AIMD) simulations. First, AIMD simulations and phonon spectra demonstrate the dynamic and thermal stabilities of Mo2CS2 monolayer. Three likely reaction pathways, Langmuir-Hinshelwood (LH), Eley-Rideal (ER), and Termolecular Eley–Rideal (TER) for CO oxidation on the Ru1- and Ir1@Mo2CS2 SACs, have been studied in detail. It is found that CO oxidation mainly proceeds via the TER mechanism under mild reaction conditions. The corresponding rate-determining steps are the dissociation of the intermediate (OCO-Ru1-OCO) and formation of OCO-Ir1-OCO intermediate. The downshift d-band center of Ru1- and Ir1@Mo2CS2 help to enhance activity and improve catalytst stability. Moreover, a microkinetic study predicts a maximum CO oxidation rate of 4.01 × 102 s-1 and 4.15 × 103 s-1 (298.15 K) following the TER pathway for the Ru1- and Ir1@Mo2CS2 catalysts, respectively. This work provides guideline for fabricating and designing highly efficient SACs with superb catalyts using MXene materials.
In this paper, Fe36Co44 nanocluster structure is used to catalyze the hydrolysis reaction of ammonia borane to produce H2. Firstly, we complete the construction of Fe36Co44 cluster structure and calculate the electronic properties of the cluster. By comparing the adsorption process of Ammonia Borane (AB) in active sites of the cluster, which have different Effective Coordination Number (ECN), the qualitative relationship between ECN and the catalytic activation of AB is clarified, and the optimal catalytic active site is obtained. Then, from the perspective of different reaction paths, we study the hydrolysis reaction of AB in multiple paths, and obtain 5 different reaction paths and energy profiles. The calculation results show that in the case of NH bond priority break (path 5), the reaction has the minimum rate-determining step (RDS) barrier (about 1.02 eV) and the entire reaction is exothermic (about 0.40 eV). So, path 5 is an optimal catalytic reaction path. This study will have an important guiding significance for the study of the AB hydrolysis reaction mechanism.
The development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction (HER) and oxygen evolution reactions (OER) in alkaline media is essential for the electrochemical overall water splitting technologies. Herein, we demonstrate that the HER/OER performance of CoSe2 can be significantly enhanced by tuning the 3d-orbital electron filling degree through Mo doping. Both density functional theory (DFT) calculations and experimental results imply that the doping of Mo with higher proportion of the unoccupied d-orbital (Pun) could not only serve as the active center for water adsorption to enhance the water molecule activation, but also modulate the electronic structures of Co metal center leading to the optimized adsorption strength of *H. As expected, the obtained Mo-CoSe2 exhibits a remarkable bifunctional performance with overpotential of only 85 mV for HER and 245 mV for OER to achieve the current density of 10 mA/cm2 in alkaline media. This work will provide a valuable insight to design highly efficient bifunctional electrocatalyst towards HER and OER.
Rhein (Rhe), an anthraquinone derivative, exhibits excellent anti-inflammatory effects and other pharmacological activities, but its clinical application remains limited due to poor solubility. The present work aims at the improvement of solubility and oral bioavailability of Rhe through cocrystal formation. For this purpose, Rhe and matrine (Mat) were selected as pharmaceutical ingredient (API) and cocrystal former (CCF), respectively, and the Rhe-Mat cocrystal was synthesized and characterized by single crystal X-ray diffraction (SXRD), powder X-ray diffraction (PXRD), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC). The formation mechanism of Rhe-Mat cocrystal was elucidated by molecular surface electrostatic potential (MSEP). It is worth mentioning that the 50-fold increment of dissolution in vitro was observed in pure water in the form of Rhe-Mat cocrystal. Furthermore, the in vivo studies revealed that Rhe-Mat cocrystal indicated the faster absorption rate and the higher peak blood concentration than the pure Rhe. Hence, it can be concluded that current study successfully improved the solubility and oral bioavailability of Rhe.
MicroRNAs (miRNAs) have attracted significant attention in biomedical research and clinical diagnosis. However, due to their inherent characteristics of low abundance and the high complexity of corresponding biological matrices, simultaneous detection of multiple miRNAs at low abundance is still a challenge. In this work, a method coupling exponential amplification reaction (EXPAR) with matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) is developed for label-free and simultaneous detection of multiple miRNAs. The assay can be performed under isothermal conditions in a single reaction tube, and finished in less than 30 min. It exhibits good quantification ability and with attomolar-level sensitivity for miRNAs detection. It also shows high specificity to distinguish miRNAs at single-nucleotide resolution. We used the method to detect the miRNA-21, let-7a, miRNA-100, and miRNA-125b in samples of spiked human serum and breast cancer cells (i.e., MCF-7, MDA-MB-231 and SK-BR-3). The quantification results were well consistent with the standard real-time fluorescence EXPAR. Consequently, the label-free mass-spectrometric platform could be a potential tool for miRNAs analysis in complex biological samples, and may be used for clinical diagnosis.
Metal oxides derived from metal-organic framework (MOF) have attracted considerable attention due to its excellent performance and unique structure. Doping is considered as an effective method to improve gas-sensing performance. However, nonmetal doped metal oxides derived from MOF as gas-sensing materials have not been reported. Within this work, N atoms were successfully doped into the lattice of ZnO nanoparticles using ZIF-8 as a self-sacrificial template through a thermal treatment process with the assistant of urea. The obtained N-ZnO exhibited competitive ethanol-sensing performance, in which the response value of N-ZnO-5 to 100 ppm ethanol reached 115 at 190 ℃ with a satisfactory selectivity. It was found that the N-doping in ZnO facilitated the formation of oxygen vacancy that promoted the generation of adsorbed oxygen species to achieve the enhanced gas-sensing performance. Besides, the larger specific surface area resulting from the size reduction during the urea-assisted pyrolysis process can also be responsible for the improving of the ethanol-sensing performance.
The conversion of carbon dioxide into useful fuels or chemical feedstocks is of great importance for achieving carbon emission peak and carbon neutrality. The harvesting and conversion of solar energy will provide a sustainable and environmentally friendly energy source for human production and living. Very recently, photothermal catalysis has been proved to exhibit great advantages in reducing the reaction temperature, promoting the catalytic activity, and manipulating the reaction pathway in comparison with traditional thermal catalysis. In this review, we firstly introduced the fundamental mechanisms and categories of photothermal catalysis to understand the synergy or the difference between photochemical and thermochemical reaction pathways. Subsequently, the criteria and strategies for photothermal catalyst design are discussed in order to inspire the development of high-efficiency photothermal catalytic route by achieving intense absorption of broadband solar energy spectrum and high conversion capability of solar-to-heat. Recent progress in CO2 reduction achieved by photothermal catalysis was summarized in terms of production types. In the end, the future challenges and perspectives of photothermal catalytic CO2 reduction are presented. We hope that this review will not only deepen the understanding of photothermal catalysis, but also inspire the design, preparation and application of high-performance photothermal catalysts, aiming at alleviating non-renewable fossil energy consumption and carbon emissions for early carbon emission peak and carbon neutrality.
Photocatalytic hydrogen evolution from water splitting is a promising strategy for realizing the vision of carbon neutrality. Herein, a novel SrTiO3-SrCO3 n-n heterojunction was used for the first time for water splitting to generate H2. The heterojunction was synthesized by a soft chemical one-pot hydrothermal method. The SrTiO3-SrCO3 loading with 3 wt% Pt shows the maximum photocatalytic H2 evolution rate of 3.62 mmol h−1g−1 under simulated sunlight irradiation, which is 20.1 times higher than that of pristine SrTiO3. The apparent quantum efficiency of SrTiO3-SrCO3 reaches 21.73% at 313 nm, and it shows good stability during cyclic experiment. The formation of compact SrTiO3-SrCO3 heterojunction with strong interfacial electronic interaction promotes the transmission and separation of photo-generated carriers. The results of XPS, PL, PC, EIS and DFT support the mechanism of improving photocatalytic activity based on carrier dynamics. This work provides a facile and effective method to enhance the activity of SrTiO3-based heterojunction photocatalysts.
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