Latest ArticlesHerein, the nanoscaled ATP-responsive upconversion metal-organic frameworks (UCMOFs) are aqueous-phase synthesized for co-delivery of therapeutic protein cytochrome c (Cyt c) and chemodrugs doxorubicin (DOX), achieving targeted combinational therapy of human cervical cancer. The UCMOFs are rationally fabricated by growing ZIF-90 on mesoporous silica-coated upconversion nanoparticles (UCNPs), in which the ZIF-90 layer attenuates the upconversion luminescence (UCL) and the rigid frameworks increase the stability of encapsulated proteins. Once the UCMOF@DOX/Cyt c are internalized into HeLa cells via specific recognition of sgc8 aptamers, the intracellular ATP triggers the dissolution of ZIF-90 into Zn2+, which facilitates not only the release of Cyt c and DOX but also the restoration of UCL for real-time monitoring of drug release. It has been demonstrated that the therapeutic efficacy is greatly improved by the combination of caspase-mediated apoptosis activated by Cyt c (protein therapeutics), DNA fragmentation induced by DOX (chemotherapy), and Zn2+-promoted generation of reactive oxygen species (ROS) (oxidative stress). Overall, our proposed multifunctional UCMOFs provide an effective platform for targeted combinational cancer therapy and in situ imaging, which hold great promise in biomedical and clinical applications.
The rational design of nanozymes with superior activities is essential for improving bioassay performances. Herein, nitrogen and boron co-doped graphene nanoribbons (NB-GNRs) are prepared by a hydrothermal method using urea as the nitrogen source and boric acid as the boron source, respectively. The introduction of co-doped and edge structures provides high defects and active sites. The resultant NB-GNRs nanozymes show superior peroxidase-like activities to nitrogen-doped and boron-doped counterparts due to the synergistic effects. By taking advantage of their peroxidase-like activities, NB-GNRs are used for the first time to develop enzyme-linked immunosorbent assay for the detection of interleukin-6. The biosensors exhibit a high performance with a linear range from 0.001 ng/mL to 1000 ng/mL and a detection limit of 0.3 pg/mL. Due to their low cost and high stability, the proposed nanomaterials show great promise in biocatalysis, immunoassay development and environmental monitoring.
Early and precise diagnosis are propitious to timely treatment and simultaneously increase the chance of successful treatments. It is of critical importance to develop rapid, sensitive, and reliable sensing techniques of physiological biomarkers for disease diagnosis. Due to the advantages of structural designability and property tunability, nanoscale metal-organic frameworks (nMOFs) have been widely applied in the field of biomedicine in recent years. Particularly, enhanced stability, more modification sites and improved distribution make nMOFs more suitable as biosensors for detection of biomarkers. This review article will summarize the recent advancements of nMOFs-based biosensors for detection of biomarkers, classified into four sections via different sensing modes: fluorescent sensing, colorimetric sensing, electrochemical sensing and surface-enhanced Raman scattering (SERS) sensing within the latest years. Except introducing and comparing the role of nMOFs in different sensing modes, designing strategies of nMOFs-based biosensors are involved as well. At last, a brief conclusion and outlook for further applications are provided, which is helpful for exploring multi-functional biologic nano-platforms with nMOFs. We expect that this review can inspire the interest on this promising research area of nMOFs-based biosensors for detection of biomarker and early diagnosis.
A new electrochemical strategy for trifluoromethylation/cyclization using TfNHNHBoc as a CF3 source was established. This approach was realized by the direct electrolysis of TfNHNHBoc under external oxidant-free and catalyst-free conditions, and afforded various trifluoromethylated oxindoles with good functional group compatibility and broad substrate scope. Preliminary mechanistic studies show that the reaction proceeds by a radical process.
Octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) is one of the most widely used powerful explosives. The direct and selective detection of HMX, without the requirement of specialized equipment, remains a great challenge due to its extremely low volatility, unfavorable reduction potential and lack of aromatic rings. Here, we report the first chemical probe of direct identification of HMX at ppb sensitivity based on a designed metal-organic cage (MOC). The cage features two unsaturated dicopper units and four electron donating amino groups inside the cavity, providing multiple binding sites to selectively enhance host-guest events. It was found that compared to other explosive molecules the capture of HMX inside the cavity would strongly modulate the emissive behavior of the host cage, resulting in highly induced fluorescence "turn-on" (160 folds). Based on the density functional theory (DFT) simulation, the mutual fit of both size and binding sites between host and guest leads to the synergistic effects that perturb the ligand-to-metal charge-transfer (LMCT) process, which is probably the origin of such selective HMX-induced turn-on behavior.
Herein, a facile synthesis of valuable pyrido[1,2-a]pyrimidine-4-thiones is reported via novel thiocarbonylation of C(sp3)-H bonds with carbon disulfide (CS2). This reaction features easy availability of substrates, good functional group tolerance, high yields, facile scalability and atom economy. Mechanistic investigations indicate that sulfate anion and sulfuric anhydride anion might be involved in this reaction.
Nickel/(S)-t-Bu-PHOX complex catalyzed asymmetric arylative cyclization of N-alkynones has been achieved, delivering 1, 2, 3, 6-tetrahydropyridines containing a chiral tertiary alcohol in high yields and excellent enantioselectivities, which provides efficient access to chiral tetrahydropyridine and piperidine analogues.
All-hydrocarbon stapling strategy has been widely applied for enhancing the proteolytic stability of peptides. However, two major technical hurdles to some extent limit the development of stapled peptides for therapeutic usage: rational selection of the stapling sites and the corresponding deletion of the native side chains. Previously we described the development of the olefin-terminated amino acids with the retention of native side chains and successfully applied them in the synthesis of hydrocarbon stapled peptides with single side-chain retention. Here, we explored the feasibility and effectiveness of hydrocarbon stapling strategy characterized as double side-chains retention. Modeled after a lengthy human immunodeficiency virus-1 (HIV-1) fusion inhibitor SC34EK, Leui, Seri+4 and Lysi, Leui+4 stapled peptides with the retention of double side-chains were effectively obtained. Our complementary study provided a convenient alternative to address where to install the staple in sequence for conventional all-hydrocarbon peptide stapling. Furthermore, this method not only conferred conformational reinforcement for SC34EK with high α-helicity and protease resistance, but also preserved the structural characteristic (key peripheral residues, charge and solubility) of the linear peptide to the maximum, which are crucial for anti-HIV-1 activity.
Constitutionally adaptive chemistry of selenium-containing crown ethers (CEs) offers a new platform for controlling/switching the hydration of bolaamphiphile skeletons in water in an effective and simple manner by the virtue of covalent bonding. The adaptive behaviour of the macrocyclic bolaamphiphiles (transformations between C7SeBola and C7SeOBola) in response to redox environment was found to be a decisive factor.
Remote ether groups could be used as directing groups to prepare fully substituted 5-ether-1,2,3-triazoles with exclusive 1,5-regioselectivities and excellent chemoselectivities. Ether group could coordinate with iridium catalyst by lone-pair electron at a distance (up to four σ bonds) away from alkyne to control the regioselectivity by weak coordination effect. The cycloaddition reaction chemoselectively occurred at the propargyl ether moiety of diyne to give unique fully substituted 4-alkynyl-triazole.
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