Latest ArticlesThe first total synthesis of dracaenins A and B is achieved in four steps. The synthesis features the convergent coupling of three readily available fragments with minimized use of protecting groups. The chemical synthesis enables the discovery of their activity in stimulating platelet aggregation, and thus, sheds light on the possible origin of the hemostatic effect of dragon's blood.
Salinity tolerance of ambient electric arc ionization (AEAI) was evaluated by comparing electrospray ionization for various samples at NaCl concentrations from 0 to 1000 mmol/L. AEAI-mass spectrometry (AEAI-MS) exhibited an excellent signal intensity even at NaCl concentrations of 1000 mmol/L, while the ESI-MS had no signal because high salinity has a strong inhibitory effect on analytes. The sodium adduct was verified using LiCl instead of NaCl. AEAI-MS successfully quantified saline samples with an excellent quantitative ability (R2 ≥ 0.998). We also achieved some analytical samples in the buffer solution at a very high concentration and even in a saturated salt solution. Overall, AEAI-MS has protonated ions for most target analytes. In addition, the relationship between auxiliary temperature and the distance from the sample to the arc was investigated, and the results indicated that thermal desorption plays an important role in AEAI source.
Complex coordinated functional groups [MAxBy] (M = Central coordination element; A, B = P, O, S, Se, F, Cl, Br or I) are composed of different types of anions A, B jointly linked to the same central cation M, which are in high potential to tune the physical properties of materials, e.g., second-order susceptibility, energy gaps and birefringence. Recently, Compound containing complex coordinated functional groups have attracted great attention in the nonlinear optical (NLO) field and a large number of this type crystals exhibit promising NLO performance. However, the inherent relationship between ionic group structure and optical properties of complex coordinated NLO materials have not been systematically studied. This article systematically summarizes complex coordinated NLO materials in recent five years from the perspective of the internal relationship between crystal structure and optical properties. In addition, we propose the ideal combination and arrangement modes for structural building units, and also reveal the influence of complex coordinated functional groups [MAxBy] toward the NLO response, optical band gap and phase matching ability of complex coordinated NLO materials.
Supraparticles (SPs), such as assembly of inorganic components with organic, have made tremendous attention in biochemical analysis, which represents a novel but challenging research orientation. Herein, a single-SPs multifunctional fluorescent sensor array has been developed for high-throughput detection of heavy metal ions in biofluids, which is based on an inorganic/organic hybrid SPs consisting of carbon dots (CDs) and an easily available porphyrin [5, 10, 15, 20-tetra(4-carboxyphenyl)porphyrin (TCPP)]. TCPP can aggregate with the CDs to form the assembly (CDs/TCPP SPs) through the electrostatic and π-π stacking interaction. There are two independent and clearly separated fluorescence emission peaks at 470 and 668 nm in the resultant CDs/TCPP SPs under 380 nm excitation. As a proof-of concept design, F470, F668, F668/F470 of SPs are chosen as three sensor components to constitute our sensor array. With the addition of metal ions, three sensor components can generate different fluorescence response patterns for discriminating 11 heavy metal ions via principal component analysis (PCA). Additionally, thiols can readily capture Cu2+ to switch the fluorescence of CDs/TCPP initially altered by Cu2+. Hence, CDs/TCPP-Cu2+ ensemble is further demonstrated to be a powerful sensor array for pattern recognition of 7 thiols and even chiral recognition of cysteine enantiomers. This novel strategy avoids the tanglesome synthesis of multiple sensing probes and dedicates an innovative method for the facile establishment of tongue-mimic sensors, which would prospectively sprout more homologous assumptions to broaden its application toward more biosensing fields.
Detection of nucleoside derivatives has paramount importance because they are the essential biomolecular units for all life. Herein, we report a host-guest approach by using a fluorescent tetraphenylethene-based octacationic cage as host and 8-hydroxypyrene-1, 3, 6-trisulfonic acid trisodium salt (HPTS) as guest and fluorescent indicator to form non-fluorescent 1:1:1 host-(endo-exo)guest complex in water. This new host-(endo-exo)guest complex can be successfully used for detecting nucleosides (e.g., ATP and GTP), DNA (e.g., sm-DNA), and antibiotics (e.g., Penicillin G) with off-on fluorescence response via a competitive host-guest exchange with HPTS as exo-guest in water. Furthermore, this on-off-on fluorescent host-guest complex is also used for cell imaging based on ATP concentration in HeLa cells. Therefore, this study not only provides insight into the construction of a supramolecular probe with on-off-on fluorescence via host-guest complexation and exchange in solution, but also realizes a universal method for detecting and monitoring biomolecules.
Conformational regulation among two or more distant sites is not only one of the main pathways to accomplish multiple tasks in complex biological systems but also represents a powerful strategy to obtain stimuli-responsive supramolecular nanoconstructs with tailored physicochemical performance. We herein report the fabrication of a photochromic supramolecular assembly, which can be synergistically activated by the conformational regulation with bis(4, 8-disulfonato-1, 5-naphtho)-32-crown-8 and then reversibly switched by the through-space communication between restricted stilbazolium salt and photochromic dithienylethene. This work demonstrates that the synergistic conformational modulation via intra- and intermolecular interactions can be developed as a generalizable approach to construct more advanced biomimetic nanomaterials.
Reported here is the comprehensive investigation on the formation of biphen[n]arenes by tailoring reaction modules. Five new macrocyclic arenes and four oligomers were synthesized by the condensation of monomers possessing different multimethoxyphenyl reaction modules and paraformaldehyde. We proved that the number and sites of methoxy on reaction modules greatly affected the reaction activity, shape, and connection mode of macrocycles. Moreover, the triangular and saddle-shaped configuration of macrocycles were revealed by single crystal structures. The results provided a typical and fundamental guidance in designing new macrocyclic arenes.
The increase of atmospheric CO2 concentration has caused many environmental issues. Electrochemical CO2 reduction reaction (CO2RR) has been considered as a promising strategy to mitigate these challenges. The electrocatalysts with a low overpotential, high Faradaic efficiency, and excellent selectivity are of great significance for the CO2RR. Carbon-based materials including metal-free carbon catalysts and metal-based carbon catalysts have shown great potential in the CO2RR, owing to the tailorable porous structures, abundant natural resources, resistance to acids and bases, high-temperature stability, and environmental friendliness. In this review, various carbon materials including graphene, carbon nanotubes, quantum dots, porous carbon, and MOF-derived catalysts, etc., for the CO2RR have been summarized. Particularly, recent progress in terms of the mechanism and pathway of CO2 conversion has been comprehensively reviewed. Finally, the opportunities and challenges of carbon-based electrocatalysts for the CO2RR are proposed.
The development of efficient method to prepare poly(silyl ether)s (PSEs) is highly desirable. Herein, an environmentally sustainable copper-catalyzed dehydrocoupling polymerization was developed with good yields and high molecular weight (up to 48, 400 of Mn and up to 97% yield). Monomers of different types (AB type or AA and BB type) are suitable to afford PSEs. The PSEs show good thermal stability and low glass-transition temperature.
Biomedicine is one of the fastest growing areas of additive manufacturing. Especially, in the field of in vitro diagnostics (IVD), contributions of 3D printing include ⅰ) rapid prototyping and iterative IVD proof-of-concept designing ranging from materials, devices to system integration; ⅱ) conceptual design simplification and improved practicality of IVD products; ⅲ) shifting the IVD applications from centralized labs to point-of-care testing (POCT). In this review, the latest developments of 3D printing and its advantages in IVD applications are summarized. A series of 3D-printed objects for IVD applications, including single-function modules, multi-function devices which integrate several single-function modules for specific analytical applications such as sample pre-treatment and chemo-/bio-sensing, and all-in-one systems which integrate multi-function devices and the instrument operating them, are analyzed from the perspective of functional integration. The current and potential commercial applications of 3D-printed objects in the IVD field are highlighted. The features of 3D printing, especially rapid prototyping and low start-up, enable the easy fabrication of bespoke modules, devices and systems for a range of analytical applications, and broadens the commercial IVD prospects.
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