Latest ArticlesDiagnostic C9orf72 hexanucleotide repeat expansions (C9-HRE) is essential for the early and accurate diagnosis of amyotrophic lateral sclerosis (ALS) and will provide support for the prognosis and gene therapy of ALS. In the present study, by combining catalytic hairpin assembly (CHA) with Mycobacterium smegmatis porin A (MspA) nanopore, a new nanopore-based strategy for the detection of C9-HRE was reported. Less than 30 repeats of C9-HRE could be detected via this method, and the results have the potential to help distinguish between patients and healthy individuals. Moreover, the method demonstrated its great specificity for C9-HRE by identifying other repeat expansions. Given the high selectivity, this approach had been successfully used to detect C9-HRE in cell and blood samples with high accuracy. This detection strategy is user-friendly and has a strong anti-interference ability, thus providing a powerful tool for clinical diagnosis.
Due to the various pH liquid environment in nature, the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute. However, the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive capability. In this work, a carbon dots-enhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dynamic PVA-borax network into a PAAm covalent polymer network. The formed hydrogel presents a partial gel-sol transition under controlled pH environments. At low pH environments (< 6.0), the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel, and brings the lubricating properties on the hydrogel surface. Moreover, the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel, the blue sol layer can be observed more visually under the fluorescence microscope. The pH-response also exhibits well reversibility. The prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.
Imine bonds are among the most explored building motifs in dynamic chemistry, polymers, and materials, and yet, their acid-resistance remains a longstanding issue. Herein we demonstrate a concept of internal protecting groups for improving the kinetic stability of dynamic imine bonds and polymers. Systematic examination of structure-reactivity relationship of a series of aldehydes/imines bearing a neighboring carboxyl allowed uncovering of required structural features for dynamically masking imine bonds with cyclic structures. Mechanistic studies indicated that noncovalent interactions along with sterics control the ring-chain equilibrium and the stability of imine bonds. The incorporation of internal protecting groups into imine polymers further enabled their controlled stability in acidic media. Moreover, a combination of dynamic covalent network and coordination supramolecular network provided a facile means for the modulation of luminescent and mechanical properties of polymers. The strategies and results reported should be beneficial to molecular assemblies, dynamic polymers, biological delivery, and intelligent materials.
Microbial fuel cells (MFCs) have a simple structure and excellent pollutant treatment and power generation performance. However, the slow kinetics of the oxygen reduction reaction (ORR) at the MFC cathode limit power generation. The electrochemical performance of MFCs can be improved through electrocatalysis. Thus far, metal-based catalysts have shown astonishing results in the field of electrocatalysis, enabling MFC devices to demonstrate power generation capabilities comparable to those of Pt, thus showing enormous potential. This article reviews the research progress of meta-based MFC cathode ORR catalysts, including the ORR reaction mechanism of MFC, different types of catalysts, and preparation strategies. The catalytic effects of different catalysts in MFC are compared and summarized. Before discussing the practical application and expanded manufacturing of catalysts, we summarize the key challenges that must be addressed when using metal-based catalysts in MFC, with the aim of providing a scientific direction for the future development of advanced materials.
Covalent organic polymer (COP) thin film-based memristors have generated intensive research interest, but the studies are still in their infancy. Herein, by controlling the content of hydroxyl groups in the aldehyde monomer, Py-COP thin films with different electronic push-pull effects were fabricated bearing distinct memory performances, where the films were prepared by the solid-liquid interface method on the ITO substrates and further fabricated as memory devices with ITO/Py-COPs/Ag architectures. The Py-COP-1-based memory device only exhibited binary memory behavior with an ON/OFF ratio of 1:101.87. In contrast, the device based on Py-COP-2 demonstrated ternary memory behavior with an ON/OFF ratio of 1:100.6: 103.1 and a ternary yield of 55%. The ternary memory mechanism of the ITO/Py-COP-2/Ag memory device is most likely due to the combination of the trapping of charge carriers and conductive filaments. Interestingly, the Py-COPs-based devices can successfully emulate the synaptic potentiation/depression behavior, clarifying the programmability of these devices in neuromorphic systems. These results suggest that the electronic properties of COPs can be precisely tuned at the molecular level, which provides a promising route for designing multi-level memory devices.
It is of great interest to make a degradable material widely tailorable to replace petroleum-derived products among diverse applications. Here, we report the construction of a new multi-purpose degradable material for the first time via a simple ternary copolymerization system comprising ε-caprolactone (ε-CL), cyclohexane oxide (CHO) and CO2. Under low pressure of 1 bar ~5 bar, the ring-opening polymerization (ROP) of ε-CL and ring-opening copolymerization (ROCOP) of CO2 and CHO can simultaneously proceed. The carbonate units are randomly distributed on the polymer chain. These random terpolymers have controllable molar mass (10–106 kDa) and compositions (4–33 mol% CO2). And the obtained materials show large-span tunability from tough plastic to elastomer and even adhesive.
As key biomarkers, amyloid-β (Aβ) plaques are frequently used to diagnose Alzheimer's disease (AD). Although fluorescence imaging has proven to be effective in detecting these plaques, the gold standard probe thioflavin T (ThT), used for Aβ aggregates, cannot be applied in vivo owing to its invasive nature. Therefore, the development of novel fluorescent probes capable of identifying Aβ plaques in situ is necessary. Based on the ThT structure, two π-conjugated heterocyclic D-π-A probes were designed bearing the hydroxytricyanopyrrole acceptor and N,N-dimethylaminophenyl donor. These probes exhibited red to near-infrared fluorescence emission (λmax = 732 nm), large Stokes shifts (>100 nm), exceptional signal-to-noise ratio, rapid response (<30 s), and high binding affinity (NT-HTCP = 33.32 nmol/L; NF-HTCP = 53.35 nmol/L) for Aβ aggregates. As the best candidate, NT-HTCP was used for in situ imaging of Aβ plaques in AD mouse models. Furthermore, in vivo research demonstrated that NT-HTCP could cross the blood–brain barrier and continue imaging the Aβ plaques with a good signal-to-noise ratio. Additionally, the outcomes of the docking computations helped guide the development of the Aβ probes. This study expands the family of N,N-dimethylaminophenyl-based Aβ-sensitive fluorophores, with NT-HTCP emerging as a highly promising imaging agent.
Antibiotic abuse now poses a grave threat to global ecology and bestirs public concerns about the residue issue in daily necessities. The traceability measurements along supply chain or logistic circulation have become increasingly essential given the labile nature of diverse synthetic residuals on site. In an attempt to answer this urgency, here a miniaturized fluorometric aptasensor prototype was contrived that catered to the point-of-care screening norm for two typical additives: chloramphenicol and enrofloxacin. The key target-indicating module worked in vitro based on the competitive binding-induced fluorescence recovery of fluorescein-labeled aptamers, which were photobleached beforehand in the format of double helix on burlike nanogold carriers. The “prickly” geometry of the latter not just enriched the capture probes at preferentially substrate-accessible spires; but also contributed to a tip-enhanced surface plasmon effect, sensitizing the signal-on during the duplex dissociation even at nanomolar threshold of the analytes. On the other hand, to encompass a full portable, a set of optical devices were mounted within a 3D-printed cartridge (adaptor) to converge the light beam and route it towards the detector, for which the smartphone camera came up in handy with a home-developed App for calibrating the emissive brightness. Enlightened by the high-dynamic-range compression, an imaging diagnostic algorithm was built in to grid and digitize each slide in the album for augmented detection performance. Thus, a novel bio-to-silico integration was invented that capable of in situ rapid reporting on the antibiotic presence with high sensitivity and selectivity. Further field practices in spiked milk on sales proved the precision and rudimentary feasibility of the well-assembled model of appliance, thus holding nice prospects in nonexpert (e.g., family and local community) utilities for foodborne antibiotic identification.
This review explores the concept of life-on-a-chip, which involves the creation of miniaturized biological systems, such as organs, tissues, and model organisms, on microscale platforms called microfluidic chips. These chips consist of intricately etched channels, wells, and chambers that enable precise control and observation of fluids, cells, and biochemical reactions, facilitating the simulation of various aspects of human or animal physiology and the study of responses to different stimuli, drugs, or disease conditions. The review highlights the application of a novel technology, "Beyond Limit Manufacturing" (BLM), in the development of sophisticated three-dimensional cell models and model organism microchips. Model-organism-on-a-chip and organ-on-a-chip (OoC) are among the thriving developments in the field of microfluidics, allowing for the reconstruction of living microenvironments and implementation of multiple stimuli. The review discusses the latest advancements in life-on-a-chip technology using BLM and outlines potential future research directions, emphasizing the significant role of these chips in studying complex biological processes in a controlled and scalable manner.
To develop efficient sensitizers for dye-sensitized solar cells (DSSCs), we recently reported doubly concerted companion (DCC) dye XW83 with a wrapped porphyrin sub-dye unit linked to an organic sub-dye unit through a flexible chain, which exhibits panchromatic absorption and excellent anti-aggregation ability. To further improve the absorption, we herein report XW87 and XW88 by inserting an ethynyl group into the organic sub-dye unit of XW83 near the donor and acceptor, respectively. For the corresponding organic dyes Z3 and Z4, the introduced ethynyl group improves their absorption, but induces aggravated charge recombination, leading to lowered power conversion efficiencies (PCEs). Similar to the organic dyes, the introduced ethynyl group improves the absorption of DCC dyes XW87 and XW88 as well. In addition, the ethynyl group near the acceptor of the organic sub-dye unit can be well protected by the long wrapping chains from the porphyrin unit. As a result, XW88 affords the highest JSC (21.84 mA/cm2), VOC (782 mV) and PCE (12.2%) among the DCC dyes. These results provide an effective method for developing efficient DSSC dyes by inserting an ethynyl group at a suitable position of a DCC dye.
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