Latest ArticlesFluorescence lateral flow immunoassay (LFA) has emerged as a powerful tool for rapid screening of various biomarkers owing to its simplicity, sensitivity and flexibility. It is noteworthy that fluorescent probe mainly determines the analytical performance of LFA. Due to the emission and excitation wavelengths are located in the visible region, most fluorophores are inevitably subject to light scattering and background autofluorescence. Herein, we reported a novel LFA sensor based on the second near-infrared (NIR-Ⅱ) fluorescent probe with excellent anti-interference capability. The designed NIR-Ⅱ probe was the Nd3+ and Yb3+ doped rare earth nanoparticles (RENPs) by employing Nd3+ as energy donor and Yb3+ as energy acceptor, which of the donor-acceptor energy transfer (ET) efficiency reached up to 80.7%. Meanwhile, relying on the convenient and effective encapsulation strategy of poly(lactic-co-glycolic acid) (PLGA) microspheres to RENPs, the surface functionalized NIR-Ⅱ probe (RE@PLGA) was obtained for subsequent bioconjugation. Benefiting from the optical advantages of NIR-Ⅱ probe, this proposed NIR-Ⅱ LFA displayed a good linear relationship ranging from 7 ng/mL to 200 ng/mL for the detection of α-fetoprotein (AFP), an important biomarker of hepatocellular carcinoma (HCC). The limit of detection (LOD) was determined as low as 3.0 ng/mL, which was of 8.3 times lower than clinical cutoff value. It is promising that LFA sensor based on this efficient RENPs probe provides new opportunities for high sensitive detection of various biomarkers in biological samples.
As more and more studies have shown that lipid molecules play an important role in the whole biology, in-depth analysis of lipid structure has become particularly important in lipidomics. Mass spectrometry (MS), as the preferred tool for lipid analysis, has greatly promoted the development of this field. However, the existing MS methods still face many difficulties in the in-depth or even comprehensive analysis of lipid structure. In this review, we discuss recent advances in MS methods based on double bond-specific chemistries for the resolving of C=C location and geometry isomers of lipids. This progress has greatly advanced the lipidomics analysis to a deeper structural level and facilitated the development of structural lipid biology.
Customized design of well-defined cathode structures with abundant adsorption sites and rapid diffusion dynamics, holds great promise in filling capacity gap of carbonaceous cathodes towards high-performance Zn-ion hybrid supercapacitors (ZHC). Herein, we fabricate a series of dynamics-oriented hierarchical porous carbons derived from the unique organic-inorganic interpenetrating polymer networks. The interpenetrating polymer networks are obtained through physically knitting polyferric chloride (PFC) network into the highly crosslinked resorcinol-formaldehyde (RF) network. Instead of covalent bonding, physical interpenetrating force in such RF-PFC networks efficiently relieves the RF skeleton shrinkage upon pyrolysis. Meanwhile, the in-situ PFC network sacrifices as a structure-directing agent to suppress the macrophase separation, and correspondingly 3D hierarchical porous structure with plentiful ion-diffusion channels (pore volume of 1.35 cm3/g) is generated in the representative HPC4 via nanospace occupation and swelling effect. Further removal of Fe fillers leaves behind a large accessible specific surface area of 1550 m2/g for enhanced Zn-ion adsorption. When used as the cathode for ZHC, HPC4 demonstrates a remarkable electrochemical performance with a specific capacity of 215.1 mAh/g at 0.5 A/g and a high Zn2+ ion diffusion coefficient of 11.1 × 10−18 cm2/s. The ZHC device yields 117.0 Wh/kg energy output at a power density of 272.1 W/kg, coupled with good cycle lifespan (100,000 cycles@10 A/g). This work inspires innovative insights to accelerate Zn diffusion dynamics by structure elaboration towards high-capacity cathode materials.
Phosphorus-based anode is a promising anode for sodium-ion batteries (SIBs) due to its high specific capacity, however, suffers from poor electronic conductivity and unfavorable electrochemical reversibility. Incorporating metals such as copper (Cu) into phosphorus has been demonstrated to not only improve the electronic conductivity but also accommodate the volume change during cycling, yet the underline sodiation mechanism is not clear. Herein, take a copper phosphide and reduced graphene oxide (CuP2/C) composite as an example, which delivers a high reversible capacity of > 900 mAh/g. Interestingly, it is revealed that the native oxidation PO components of the CuP2/C composite show higher electrochemical reversibility than the bulk CuP2, based on a quantitative analysis of high-resolution solid-state 31P NMR, ex-situ XPS and synchrotron X-ray diffraction characterization techniques. The sodiation products Na3PO4 and Na4P2O7 derived from PO could react with Na-P alloys and regenerate to PO during charge process, which probably accounts for the high reversible capacity of the CuP2/C anode. The findings also illustrate that the phosphorus transforms into nanocrystalline Na3P and NaP alloys, which laterally shows crystallization-amorphization evolution process during cycling.
Selective separation of amino acids and proteins is crucial in various areas of research, including proteomics, protein structure and function studies, protein purification and drug development, and biosensing and biodetection. A nanocomposite film is formed by combining layer-by-layer self-assembled gold nanospheres (AuNPs) driven by cucurbit[7]uril (CB[7]) and polymethyl methacrylate (PMMA) film. Due to the host-guest interactions, the selective transmission of L-tryptophan in the nanocomposite film is confirmed by the current-voltage measurements using a picoammeter. Furthermore, by adjusting the particle size of AuNPs to increase channel size, lysozyme containing multiple tryptophan residues can selectively pass through the nanocomposite film, indicating the high versatility and adaptability of the nanocomposite film. This study will provide a new direction for the selective separation of amino acids and proteins.
Hydrogen, as a cheap, clean, and cost-effective secondary energy source, performs an essential role in optimizing today’s energy structure. Magnesium hydride (MgH2) represents an attractive hydrogen carrier for storage and transportation, however, the kinetic behavior and operating temperature remain undesirable. In this work, a dual-phase multi-site alloy (MsA) anchored on carbon substrates was designed, and its superior catalytic effects on the hydrogen storage properties of MgH2 were reported. Mechanism analysis identified that multi-site FeNi3/NiCu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH2−MsA systems. Concretely, the unique multi-metallic site structure attached to the surface of MgH2 provided substantial reversible channels and accessible active sites conducive to the adsorption, activation, and nucleation of H atoms. In addition, the coupling system formed by FeNi3 and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH2 and H atoms. Hence, the onset dehydrogenation temperature of MgH2 + 5 wt% MsA was reduced to 195 ℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 kJ/mol. 5.08 wt% H2 could be released at 250 ℃ in 20 min, reaching a high dehydrogenation rate of 0.254 wt% H2/min, yet that for MgH2 at a higher temperature of 335 ℃ was only 0.145 wt% H2/min. Then, the dehydrogenated MgH2−MsA sample could absorb hydrogen from room temperature (30 ℃) and charge 3.93 wt% H2 at 100 ℃ within 20 min under 3.0 MPa H2 pressure. Benefiting from carbon substrates, the 5 wt% MsA doped-MgH2 could still maintain 6.36 wt% hydrogen capacity after 20 cycles. In conclusion, this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.
Nanomaterials provide an ideal platform for biomolecular display due to their dimensions approach the molecular scale, facilitating binding behavior akin to that observed in solution-based processes. DNA nanoprobes hold great promise as miniature detectives capable of detecting miRNAs within cells. However, current nanoprobes face a challenge in achieving the required precision for accurate miRNA detection, particularly within the intricate confines of the cellular microenvironment, due to interference with biological autofluorescence, off-target effects, and a lack of spatiotemporal control. Here, we have designed a dual-stimuli responsive DNA tracker, synergistically utilizing specific intracellular cues and external triggers, which enables spatiotemporal-controlled and precise detection and imaging of miRNAs "on demand". The tracker, which combines zeolitic imidazolate framework-67 (ZIF-67) and unique hairpin DNA structures, effectively anchored onto the ZIF-67 through electrostatic interactions, remains in a dormant state until activated by abundant cellular ATP, resulting in the release of the hairpin structures that include a PC linker incorporated into the loop region. Subsequent irradiation triggers specific recognition of the target miRNA. The newly developed HP-PC-BT@ZIF-67 tracker demonstrates precise spatiotemporal miRNA detection and exhibits excellent biocompatibility, enabling specific miRNA recognition "on demand" within cancer cells. This research presents a reliable miRNA imaging platform in the intricate cellular environment, opening up the possibilities for precise biomedical analysis and disease diagnosis.
An N-heterocyclic carbene (NHC) catalyzed enantioselective cyclisation and trifluoromethylation of olefins with cinnamaldehydes via radical relay cross-coupling in the presence of Togni reagent is reported and δ-lactones tolerated with stereogenic centers at β- and γ-positions are obtained in moderate to high yields and with high enantioselectivities. Further computational studies explain that the radical cross-coupling step is the key to determining the enantioselectivity. Energy analysis of key transition states and intermediates also provides a reasonable explanation for the difficulty of diastereoselective control. DFT calculations also reveal that the hydrogen-bonding interaction plays a vital role in the promotion of this chemistry.
Immunotherapy offers significant potential but is often hampered by the immunosuppressive environment in oral squamous cell carcinoma (OSCC). To address this, we propose an enhanced immunotherapeutic strategy that revitalizes the tumor immune microenvironment (TIME) in OSCC by integrating upconversion-based photodynamic therapy (PDT) with chemotherapy. Using a red blood cell membrane-inspired biomimetic nanoplatform, our approach concurrently delivers chlorin e6@upconversion nanoparticles (Ce6@UCNP) and doxorubicin (DOX). By leveraging fluorescence resonance energy transfer (FRET) for 980 nm to 660 nm upconversion excitation, we address challenges such as limited tissue penetration and tissue damage, as well as nanoplatform issues including immunogenicity and targeting inaccuracy Our integrated approach enhances PDT and chemotherapy with the goal of transforming immunologically "cold" tumors into "hot" ones through a cascaded therapy, thereby revitalizing the tumor immune microenvironment in OSCC.
The demand for enhanced optical properties in advanced fluorescence technologies has driven research into the structure-property relationship of fluorophores. In this paper, we use naphthalene fluorophores NaDC-Aze and PhDO-Aze as a case study to emphasize the pivotal role of cross conjugation in tuning the optical structure-property relationship. NaDC-Aze and PhDO-Aze, formed by hybridizing two distinct conjugated systems in a single naphthalene molecule, exhibit spectral characteristics from both conjugated systems. Experimental data and theoretical calculations demonstrate the coexistence of two electron-delocalization systems in a cross-conjugation manner in both NaDC-Aze and PhDO-Aze. The cross-conjugation fluorophores exhibit high brightness, large Stokes shift, and a broad absorption wavelength range by combining distinct spectral properties from its parent fluorophores. These spectral properties will be advantageous for certain applications (i.e., panchromatic absorption in organic solar cells, and fluorophores compatible with a wide range of excitation wavelengths).
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