Latest ArticlesThe existence of adsorbed water and structural water in the crystal structure of attapulgite (ATP) endows it with poor capability to store lithium ions. Herein, the chloride molten salt method was developed to function ATP materials based on theoretical calculations, which exhibit ground-breaking electrochemical performance. After the modification process, the metal ions in chloride molten salt occupy the vertices of the Mg-O octahedral structure from the liberation of structural water and hydroxyl groups in ATP, forming MaMgbAlcSixOy (M = Li, Na, or K). Using LiCl molten salt-modified ATP (Li-ATP) as a proof-of-concept, the detailed phase transition, physicochemical properties, and lithium storage capacity were investigated. Compared to the original ATP, Li-ATP achieves a nearly 7-fold increase in lithium storage capacity (498 mAh/g), featuring a promising low-cost polyanionic type anode material.
Epilepsy, as a chronic neurological disease of the brain, is closely related to oxidative stress, and the peroxynitrite (ONOO−) significantly rise up in this event. Therefore, ONOO− is considered as a potential biomarker for early prediction of epilepsy. However, some potential diagnostic reagents for epilepsy are hindered by the blood-brain barrier (BBB). Meanwhile, “drug repurposing” is attracting a growing interest. Edaravone (EDA), as a first-line drug in the clinical treatment of cerebral ischemia, plays antioxidant roles in scavenging free radicals, promising potential antiepileptic activity. Thus, it is imperative to develop fluorescent probes for monitoring ONOO− fluctuations in the epileptic brain. Hence, we proposed a novel fluorescent probe with the thiocarbonate as the promising recognition unit for ONOO− and dicyanoisophorone derivative as the fluorophore. Moreover, by the “three-in-one” strategy, the introduction of trifluoromethyl into DCI-ONOO-3 can extend the emission wavelength of the fluorophore, shorten the response and increase lipophilicity. Consequently, DCI-ONOO-3 was used for monitoring ONOO− fluxes in brain of epileptic mice and evaluating the antiepileptic efficacy of EDA. It opens up a new way for the design of BBB permeable fluorescent probes, and provides a convincing new method for the diagnosis and treatment of epilepsy.
The topology of conjugated macrocycles had significant impacts on their photo-physical and photo-chemical properties. Herein, a series of π-conjugated macrocycles with diverse topology were synthesized via intramolecular McMurry coupling. Their chemical structure and macrocyclic topology were unambiguously confirmed via NMR, MALDI-TOF mass spectra, crystal analysis and scanning tunneling microscopy (STM). Depending on the structural topology and structural rigidity, these cyclic compounds display obviously distinctive emission behavior and photochemical reactions in the solution and in the solid state. Monocyclic phenylene vinylene macrocycle (denoted as MST) exhibiting aggregation-induced emission behavior, was more vulnerable to photo-cyclization in solution and triplet sensitizer promoted photo-dimerization due to lower strain and more flourishing intramolecular motions. After UV light irradiation, relatively more flexible MST could yield the anti-dimer via triplet excimer on the HOPG surface confirmed by STM investigation. By contrast, highly constrained bicyclic analogue (named as DMTPE) with central tetraphenylethene core, displayed high emission quantum yields of 68% both in solution and in the solid state, and was relatively inert to photochemical reactions and yield syn-dimer on the surface via singlet excimer involved [2 + 2] photo-dimerization. Based on the solution-mediated photo-polymerization of MST moiety, multicyclic porous carbon-rich ribbon connected with four-membered ring was successfully constructed and validated via STM imaging.
Bioelectronics have gained substantial research attention owing to their potential applications in health monitoring and diagnose, and greatly promoted the development of biomedicine. Recently, poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) hydrogels have arose as a promising candidate for the next-generation bioelectronic interface due to its high-conductivity, versatility, flexibility and biocompatibility. In this review, we highlight the recent advances of PEDOT:PSS hydrogels, including the gelation methods and modification strategies, and summarize their wide applications in different type of sensors and tissue engineering in detail. We expect that this work will provide valuable information regarding the functionalizations and applications of PEDOT:PSS hydrogels.
Silicon-based anodes including Si, SiOx and SiO2 could deliver ultra-large capacities, but degrade fast owing to huge volume change and low conductivity. Generally, large amounts of elastic binder and conductive additives were composited with nanosized silicon-based materials to yield reasonable cycling stability, which nevertheless not only decrease specific capacity but also induce inhomogeneous lithiation/delithiation as well as uneven stress variations. Artificial nanolattice has exhibited superior mechanical properties which could be ideal structure for silicon-based anodes, but yet faces challenges in integration of chemical reactivity, conductivity and mechanical stability. Herein, we fabricate artificial SiO2 honeycomb nanolattice consisting of numerous nanoscale SiO2 cells interconnected by through-holes, and conformal coating of highly graphitic carbon on the nanolattice is achieved through in situ catalytic graphitization. Moreover, the nanolattice is firmly bonded on Cu substrate through atomic interdiffusion irrespective of surface roughness. This unique structure allows fast charge transportation and homogeneous lithiation/delithiation throughout the micron-meter nanolattice, which results in excellent stability and large reversible capacity over 500 cycles at 1 A/g. The results highlight design and constructing artificial nanolattice can be an effective way to prevent chemo-mechanical degradation of silicon-based anode materials.
The development of efficient and stable bifunctional overall water-splitting is a crucial goal for clean and renewable energy, which is a challenging task. Herein, we report an Mn-incorporated RuO2 (Mn-RuO2) catalyst for highly efficient electrocatalytic oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acid and alkaline media. Benefiting from a more electrochemical active area with the incorporation of Mn, the Mn-RuO2 required an overpotential of 200 mV to attain a current density of 10 mA/cm2 for OER in acid. DFT result indicates that the doping of Mn into RuO2 can enhance the OER activity. An acidic overall water-splitting electrolyzer with good stability constructed by bifunctional Mn-RuO2 only requires a cell voltage of 1.50 V to afford 10 mA/cm2 and can operate stably for 50 h at 50 mA/cm2, which is better than the state-of-the-art Ru-based catalyst. Additionally, the Mn-RuO2 exhibits excellent HER and OER activity in alkaline media, and it shows superior activity and durability for overall water-splitting, only needing a cell voltage of 1.49 V to attain 10 mA/cm2. The present work provides an efficient approach to designing and constructing efficient Ru-based electrocatalysts for overall water-splitting.
DNA-based hydrogels are exceptional materials for biological applications because of their numerous advantages such as biodegradability, biocompatibility, hydrophilicity, super absorbency, porosity, and swelling. Among these advantages, the ability of DNA-based hydrogels to respond to specific physical and chemical triggers and undergo reversible phase transitions has garnered significant attention in the fields of disease diagnosis (biosensors) and treatment (drug delivery). This article focuses on the recent advancements in the research of DNA-based hydrogels and discusses the different types of these hydrogels, the synthetic methods, their unique properties, and their applications in biosensors and drug delivery. The types of DNA hydrogels are categorized based on their building blocks, and the process of synthesis as well as the unique characteristics of DNA-based hydrogels are described. Then, DNA-based responsive hydrogels utilized as intelligent materials for the development of biosensors are reviewed. Furthermore, this article also presents the current status of DNA-based responsive hydrogels in drug delivery for cancer treatment, wound healing, and other therapeutic applications. Ultimately, this paper discusses the current challenges in expanding the practical application of DNA-based hydrogels.
Tetracycline (TC) as a typical emerging pollutant is becoming a serious threat to the environment and human health. A combined advanced oxidation technology of UV/Ozone (O3)/peroxydisulfate (PDS) process was developed to explore an efficient and economic treatment process of TC in wastewater. Furthermore, the reactive sites and transformation pathways of TC were explored and the toxicity of the intermediates was quantified with a quantitative structure-activity relationship (QSAR) assessment. The degradation performance of TC was substantially enhanced in UV/O3/PDS process with a kobs of 0.0949 min−1, which was 2.3 times higher than UV/O3 and 3.2 times than sole UV. The results demonstrated that there was a superior synergistic effect of PDS on UV/O3 processes for the degradation of TC. Electron paramagnetic resonance (EPR) analysis and quenching experiments show that •OH, SO4•−, O2•− and 1O2 all contributed to TC degradation in the UV/O3/PDS process and exhibited a synergistic effect, which inhibited the generation of harmful products. In addition, the UV/O3/PDS system can effectively degrade TC in a wide range of substrate concentrations and pH, and also showed excellent adaptability to various concentrations of anions (Cl− and HCO3−). This study proves the feasibility of UV/O3/PDS process for treating TC contaminated wastewater with complicated water matrix.
Activated pancreatic stellate cells (PSCs) are the main source of collagen layer deposition and the key target in pancreatic fibrosis. However, no effective treatment specific to pancreatic fibrosis clinically, owing to the drug accumulation blocked by the collagen barrier and thus it is difficult to inhibit activated PSCs precisely. Herein, a PSCs-targeting nano-system based on “nanodrill” strategy (LA-PC) was designed to enhance the accumulation of all-trans retinoic acid (ATRA) in PSCs, relying on the platelet-derived growth factor receptor beta (PDGFRβ)-targeting peptide (pPB: C*SRNLIDC*) and collagenase (Col). After being injected into fibrotic mice via tail vein, the Col modified on LA-PC can remove the excess collagen layer, and the drug delivery efficiency through pPB targeting peptide was more than 5 times higher than that of free ATRA, as well as the degree of fibrosis significantly reduced. Notably, this nano-system effectively inhibited platelet-derived growth factor subunit B (PDGF-BB)/PDGFRβ axis on PSCs via a down-regulated extracellular signal-regulated protein kinase (ERK) pathway, and accordingly reduced the level of PDGF-BB. Thus, the smart platform provided a promising strategy for the treatment of pancreatic fibrosis to achieve the precise regulation of PSCs.
Charge-transfer (CT) stoichiometric cocrystals are promising choice of organic materials for unveiling the structure-property relationship. However, due to the contradiction between large CT degree required for strong NIR absorption and flexible molecular stacking, construction of stoichiomorphism-based cocystals with near-infrared (NIR) photothermal property remains challenging. Herein, the first example of stoichiomorphism-based photothermal cocrystals were accomplished through the adaptive assembly of 3,3′,5,5′-tetramethylbenzidine (TMB) donor and 1,2,4,5-tetracyanobenzene (TCNB) acceptor. The selective cocrystallization could be controlled by varying the donor-acceptor stoichiometries via a surfactant-assisted method, resulting in two cocrystals with 1:1 (T1C1) and 1:2 (T2C1) stoichiometries. The absorbance intensity of T1C1 at 808 nm was nearly twice that of T2C1, while the photothermal conversion efficiency (PCE) of the former was 60.3% ± 0.6%, approximately 80% of that for the latter (75.5% ± 2.6%), which might be caused by the different intermolecular interactions in distinct molecular stacking patterns. Notably, both excellent PCEs of stoichiometric cocrystals were attributed to the nonradiative transition process, including internal conversion and charge dissociation processes, as elucidated by femtosecond transient absorption spectroscopy measurements. Furthermore, T1C1 was used as an NIR heater for preparing agarose-based photothermal hydrogel, showing great potential for light-controlled in-situ gelation. This strategy of balancing the CT degree and molecular packing orientation not only uncovered the relationship between stoichiometric stacking and photothermal property, but also provided an opportunity to develop advanced organic optoelectronic materials.
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