Latest ArticlesActivity-based Ubiquitin probes (Ub-ABPs) carrying a reporter group have emerged as effective tools for the investigation of deubiquitinating enzymes (DUBs), such as studying the molecular mechanism of DUBs, profiling new DUBs. But so far, the synthesis of commonly used biotin-bearing Ub-ABPs is a technical challenge. Here, we report a one-pot semi-synthetic strategy for the acquiring of Ub-ABPs carrying a biotin tag through sequential enzymatic ligation, N-S acyl transfer and aminolysis reaction without any purification steps. These probes enable to capture the different family of DUBs for enrichment and immunoblotting using the attached biotin tag.
Sodium-ion batteries (SIBs) have received significant attention in large-scale energy storage due to their low cost and abundant resources. To obtain high-performance SIBs, many intensive studies about electrode materials have been carried out, especially the cathode material. As various types of cathode material for SIBs, a 3D open framework structural Na3V2(PO4)2F3 (NVPF) with Na superionic conductor (NASICON) structure is a promising cathode material owing to its high operating potential and high energy density. However, its electrochemical properties are severely limited by the poor electronic conductivity due to the insulated [PO4] tetrahedral unit. In this review, the challenges and strategies for NVPF are presented, and the synthetic strategy for NVPF is also analyzed in detail. Furthermore, recent developments of modification research to enhance their electrochemical performance are discussed, including designing the crystal structure, adjusting the electrode structure, and optimizing the electrolyte components. Finally, further research and application for future development of NVPF are prospected.
Artificial photosynthesis of valuable chemicals from CO2 is a potential way to achieve sustainable carbon cycle. The CO2 conversion activity is still inhibited by the sluggish charge kinetics and poor CO2 activation. Herein, Ag nanoparticles coupled BiOBr have been constructed by in-situ photoreduction strategy. The crafting of interface between Ag nanoparticles and BiOBr nanosheets, achieving an ultra-fast charge transfer. The BiOBr semiconductor excited electrons and plasmonic Ag nanoparticles generated high-energy hot electrons synchronous accelerates the C=O double bond activation. Thus, the optimized Ag/BiOBr-2 heterostructure shows excellent CO2 photoreduction activity with CO production of 133.75 and 6.83 µmol/g under 5 h of 300 W Xe lamp and visible light (λ > 400 nm) irradiation, which is 1.51 and 2.81 folds versus the pristine BiOBr, respectively. The mechanism of CO2 photoreduction was in-depth understood through in-situ FT-IR spectrum and density functional theory calculations. This study provides some new perspectives into efficient photocatalytic CO2 reduction.
Herein, an intense electrochemiluminescence (ECL) was achieved based on Pt hollow nanospheres/rubrene nanoleaves (Pt HNSs/Rub NLs) without the addition of any coreactant, which was employed for ultrasensitive detection of carcinoembryonic antigen (CEA) coupled with an M-shaped DNA walker (M-DNA walker) as signal switch. Specifically, in comparison with platinum nanoparticles (Pt NPs), Pt HNSs revealed excellent catalytic performance and pore confinement-enhanced ECL, which could significantly amplify ECL intensity of Rub NLs/dissolved O2 (DO) binary system. Then, the tracks and M-DNA walker were confined on the Pt HNSs simultaneously to promote the reaction efficiency, whose M-structure boosted the interaction sites between walking strands and tracks and reduced the rigidity of their recognition. Once the CEA approached the sensing interface, the M-DNA walker was activated based on highly specific aptamer recognition to recover ECL intensity with the assistance of exonuclease Ⅲ (Exo Ⅲ). As proof of concept, the "on-off-on" switch aptasensor was constructed for CEA detection with a low detection limit of 0.20 fg/mL. The principle of the constructed ECL aptasensor also enables a universal platform for sensitive detection of other tumor markers.
The construction of highly active catalysts for methanol oxidation reaction (MOR) is central to direct methanol fuel cells. Tremendous progress has been made in transition metal phosphides (TMPs) based catalysts. However, TMPs would be partially damaged and transformed into new substances (e.g., Pt-M-P composite, where M represents a second transition metal) during Pt deposition process. This would pose a large obstacle to the cognition of the real promoting effects of TMPs in MOR. Herein, Co2P co-catalysts (Pt-P/Co2P@NPC, where NPC stands for N and P co-doped carbon) and Pt-Co-P composite catalysts (Pt-Co-P/NPC) were controllably synthesized. Electrocatalysis tests show that the Pt-Co-P/NPC exhibits superior MOR activity as high as 1016 mA/mgPt, significantly exceeding that of Pt-P/Co2P@NPC (345 mA/mgPt). This result indicates that the promoting effect is ascribed primarily to the resultant Pt-Co-P composite, in sharply contrast to previous viewpoint that Co2P itself improves the activity. Further mechanistic studies reveal that Pt-Co-P/NPC exhibits much stronger electron interaction and thus manifesting a remarkably weaker CO absorption than Pt-P/Co2P@NPC and Pt/C. Moreover, Pt-Co-P is also more capable of producing oxygen-containing adsorbate and thus accelerating the removal of surface-bonded CO*, ultimately boosting the MOR performance.
Developing efficient and stable electrocatalyst to hydrogen evolution reaction adaptable for electrolytes with different pH is a big challenge. In this work, a hierarchically structured ternary nanohybrid composed of flower-like Ru nanoparticles, rigid macrocyclic cucurbit[6]uril (CB[6]) and carboxylated multi-walled carbon nanotubes (MWCNTs) was successfully prepared by chemical wet method. Benefited by the structural merits of flower-like Ru nanoparticles exposed abundant active sites supported by the MWCNTs holding superior mass transport and electrons transfer ability as well as the existence of CB[6], the obtained catalyst exhibited outstanding HER activities with overpotentials of 27, 37 and 70 mV at −10 mA/cm2 in alkaline, acidic, and neutral electrolytes, respectively. Under the same electrocatalytic operation conditions, the HER performance is comparable or superior to commercial Pt/C catalyst (47, 27 and 49 mV). Besides, chronopotentiometric and accelerated stability test also revealed its extraordinary stability, which could be further employed for electrocatalytic procedure in a broad pH range.
A series of heterotrinuclear Ti2Ni(CO)n– (n = 6–9) carbonyls have been generated via a laser vaporization supersonic cluster source and characterized by mass-selected photoelectron velocity-map imaging spectroscopy. Quantum chemical calculations have been carried out to identify the structures and understand the experimental spectral features. The results indicate that a building block of Ti-Ti-Ni-C four-membered ring with the C atom bonded to Ti, Ti, and Ni is dominated in the n = 6–8 complexes, whereas a structural motif of Ti-Ti-Ni triangle core is preferred in n = 9. These complexes are found to be capable of simultaneously accommodating all the main modes of metal-CO coordination (i.e., terminal, bridging, and side-on modes), where the corresponding mode points to the weak, moderate, high CO bond activation, respectively. The number of CO ligands for a specific bonding mode varies with the cluster size. These findings have important implications for molecular-level understanding of the interaction of CO with alloy surfaces/interfaces and tuning the appropriate CO activation via the selection of different metals.
A regiodivergent hydrophosphorylation of enynes with phosphites has been developed using earth-abundant nickel catalyst. The manipulation of regioselectivity can be achieved by regulating the insertion order of alkyne bonds with (RO)2P(O)–Ni–H or R2P(O)O–Ni–H species, respectively. Under the Ni/Xantphos catalysis, 4,1-hydrophosphorylation is selectively obtained while the adding of acid can promote reactions towards 1,2-addition. By employing an additional Pd–H catalysis, 2,1-hydrophosphorylation is also an accessible task in one-pot reaction. Mechanistic studies and analysis have also been performed to interpret the origin of the regioselective regulation. This work highlights the arts in accessing different regioisomers by diverting common elementary reaction steps.
The biocompatibility and biodegradability of peptide self-assembled materials makes them suitable for many biological applications, such as targeted drug delivery, bioimaging, and tracking of therapeutic agents. According to our previous research, self-assembled fluorescent peptide nanoparticles can overcome the intrinsic optical properties of peptides. However, monochromatic fluorescent nanomaterials have many limitations as luminescent agents in biomedical applications. Therefore, combining different fluorescent species into one nanostructure to prepare fluorescent nanoparticles with multiple emission wavelengths has become a very attractive research area in the bioimaging field. In this study, the tetrapeptide Trp-Trp-Trp-Trp (WWWW) was self-assembled into multicolor fluorescent nanoparticles (TPNPs). The results have demonstrated that TPNPs have the blue, green, red and near infrared (NIR) fluorescence emission wavelength. Moreover, TPNPs have shown excellent performance in multicolor bioimaging, biocompatibility, and photostability. The facile preparation and multicolor fluorescence features make TPNPs potentially useful in multiplex bioanalysis and diagnostics.
Rational regulation of stable graphitic carbon nitride (CN) for superior peroxymonosulfate (PMS) activation is important in the catalytic degradation of water contaminants. In this work, the copper oxide and oxygen co-doped graphitic carbon nitride (CuO/O-CN) was prepared via one-step synthesis and applied in activating PMS for oxytetracycline (OTC) degradation, displaying superior catalytic performance. Systematic characterization and theoretical calculations indicated that the synergistic effect between the oxygen site of CN and CuO can modulate the electronic structure of the whole composite further facilitating the formation of non-radical 1O2 and various reactive radicals. Results of the influencing factor experiments revealed that CuO/O-CN has a strong resistance to the environmental impact. The degradation efficiency of OTC in the real water environment even exceeded that in the deionized water. After four successive runs of the optimal catalyst, the OTC removal rate was still as high as 91.3%. This work developed a high-efficiency PMS activator to remove refractory pollutants via both radical pathway and non-radical pathway, which showed a promising potential in the treatment of wastewaters.
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