Latest ArticlesDNA-functionalized gold nanoparticles are one of the most versatile bionanomaterials for biomedical and clinical diagnosis. Herein, we discovered that the performance of DNAzyme cleaving the substrate is highly related to its length. This intriguing phenomenon only appears at the interfaces of DNA-functionalized gold nanoparticles. We systematically investigated the causes of this phenomenon. We conjectured that the DNAzyme with extended nucleotides that do not match its substrate strand is vulnerable to non-specific adsorption, electrostatic repulsion, and steric hindrance. Based on our improved understanding of this phenomenon, we have successfully developed a highly sensitive and specific amplifiable biosensor to detect human apurinic/apyrimidinic endonuclease 1.
Selective hydrogenation of substituted nitroarenes is an important reaction to obtain amines. Supported metal catalysts are wildly used in this reaction because the surface structure of supports can tune the properties of the supported metal nanoparticles (NPs) and promote the selectivity to amines. Herein, Pt NPs were immobilized on FeOOH, Fe3O4 and α-Fe2O3 nanorods to synthesize a series of iron compounds supported Pt catalysts by liquid phase reduction method. Chemoselective hydrogenation of 3-nitrostyrene to 3-aminostyrene was used as probe reaction to evaluate the performance of the catalysts. The results show that Pt/FeOOH exhibits the highest selectivity and activity. FeOOH support with pores and -OH groups can tune the electronic structure of Pt NPs. The positive charge of Pt NPs supported on FeOOH is key factor for improving the catalytic performance.
A [3 + 2]/[2 + 1] cycloaddition reaction of gem-difluorocyclopropenes is presented, offering a mild and efficient approach to accessing tri- and tetra-substituted 4-fluoropyridines in moderate to good yields with excellent regioselectivity. Multiple synthetic applications, including process-scale reactions, modification of bioactive molecules, derivatization reactions and synthesis of the analogue of the PKM2 modulator, are subsequently described.
Oxygen evolution reaction (OER) is pivotal to drive green hydrogen generation from water electrolysis, but yet is strictly overshadowed by the sluggish reaction kinetics. Earth-abundant and cut-price transition-metal compounds, particularly CoFe layered-double-hydroxides (LDHs), show the distinct superiorities in contrast to noble metals and their derivatives. In this review, we firstly underline their fundamental issues in electrocatalytic water oxidation, including CoFe LDHs crystal structure, the surface of (hydr)oxides confined to OER and the controversial roles of Fe species, aiming at understanding the structure-related activity and catalytic mechanism. Advanced approaches for optimizing OER activity of CoFe LDHs are then comprehensively overviewed, which will shed light on the different working mechanisms and provide a concise analysis of their unique advantages. Finally, a perspective on the future development of CoFe LDHs electrocatalysts is offered. We hope this review can give a concise and explicit guidance for the development of transition-metal-based electrocatalysts in the energy field.
A rhodium-catalyzed [4 + 3] cycloaddition reaction between N-methoxybenzamides and gem-difluorocyclopropenes is described. The reaction offers a mild and efficient approach towards the synthesis of fluorinated 2H-azepin-2-ones with broad substrate scope. A consecutive HOAc-assisted CN bond formation and fluorine elimination are involved as key steps for success as illustrated by detailed DFT studies.
Microfluidic devices have become a powerful tool for chemical and biologic applications. To control different functional parts on the microchip, valve plays a key role in the device. In conventional methods, physio-mechanical valves are usually used on microfluidic chip. Herein, we reported a chemo-mechanical switchable valve on microfluidic chip by using a thermally responsive block copolymer. The wettability changes of capillary with copolymer modification on inner surface were investigated to verify the function as a valve. Capillaries with modification of poly-(N-isopropylacrylamide-co-hexafluoroisopropyl acrylate) (P(NIPAAm-co-HFIPA)) with a 20% HFIPA was demonstrated capable of control aqueous solution stop or go through. Then short capillaries with copolymer modification were integrated in microchannels as valves. With the temperature changing around lower critical solution temperature (LCST), the integrated chemo-mechanical switchable valve exhibited excellent "OPEN–CLOSE'' behavior for microflow control. After optimization of the block copolymer sequences and molar ratio, a switching time as low as 20 s was achieved. The developed micro valve was demonstrated effective for flow control on microchip.
An efficient photo-Fenton catalyst (FeS2@HTCN) was designed by maximizing the synergistic effect of FeS2 nanoparticles and hollow tubular g-C3N4 (HTCN). Molecule self-assembly and molten salts-assisted calcination were used to engineering the hollow structured g-C3N4 before anchoring FeS2 nanoparticles on the walls of HTCN via reflux method. Compared to bulk g-C3N4, the unique structure of HTCN and heterojunction in the composite endowed FeS2@HTCN with more active sites and abundant channels for electron transfer and charge separation. The enriched electrons can improve the Fe3+ recycling and boost Fe2+ catalyzed •OH production via H2O2. As-prepared photo-Fenton catalyst was successfully applied to the treatment of industrial paint wastewater. The paint wastewater with its COD as high as 8200 mg/L can be effectively degraded with 0.2 mol/L H2O2 in 90 min under visible light irradiation. The photo-Fenton system was further evaluated according to the process stability and economic benefit, proving that the strategy presented in this work would be applicable to the treatment of real wastewater.
Pure organic room-temperature phosphorescence (RTP) materials have attracted wide attention owing to their excellent luminescent properties and great potential in various applications. In this work, iminostilbene and its analogues are applied to realize RTP emission by copolymerizing with acrylamide. It can be concluded that the growth of alkane chain in monomers can enhance the lifetime and photoluminescence quantum yield of RTP emission, and polymers with the larger conjugated structure of the monomer show a longer RTP emission wavelength. This work provides a series of new pure organic RTP materials and might provide new thoughts for designing more advanced and superior RTP materials.
Naphthyridine-fused bisimidazolium salts were designed and synthesized for the first time. The study of the Cu(Ⅱ) and Pd(Ⅱ) complexes demonstrated that the deprotonated dicarbene ligands are rigid chelating C, C-ligands with strong electron-donating ability in analogy with the classic phenanthroline N, N-ligands.
Enzyme assisted DNA probes are powerful tools in molecular diagnostics for their simplicity, rapidity, and low detection limit. However, cost of probes, difficulty in optimization and disturbance of secondary structure hindered the wider application of enzyme assisted DNA probes. To solve the problems, we designed a new system named shared-probe system. By introducing two unlabeled single stranded DNA named Sh1 and Sh2 as the bridge between probe and the substrate, the same sequence of dually labeled probe with stable performance was shared for different mutations, thus sparing the expense and time cost on designing, synthesizing and optimizing corresponding probes. Besides, the hybridization between Sh1 and the substrate could overcome secondary structures, which guaranteed the detection of different substrates. The performance and generality of the design were tested by low abundance detection in synthetic single DNA samples and the limit of detection was 0.05% for PTENR130Q, EGFR-L858R and 0.02% for BRCA1-NM007294.3. In genomic DNA samples, the limit of detection of 0.1% can be achieved for EGFR-L858R, demonstrating the potential of clinical application in our design.
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