Latest ArticlesResearchers engrossed in enantioseparation keep seeking for versatile chiral separation selectors. This work proposes a concept of quasi-dual-chiral-channel (QDCC) enantioseparation platform, where the surface sequentially grafted quinine (QN) and functional cyclodextrin (CD) can imitate two independent chiral channels without mutual interference to achieve wide spectrum chiral resolution. Chiral separation results combined with molecular docking simulation indicates that the different interaction mode of QN and functional CD layer renders QDCC the wide separation capability. This work provides a valuable insight into the rational design of versatile enantioseparation materials.
This work reported a facile approach to surface oxygen vacancy (OV)-enriched urchin-like TiO2 microparticles (U-TiO2), which were highly effective and durable in catalyzing selective nitrate reduction to ammonia (NO3RR). Specifically, the U-TiO2 delivered a mass activity of 1.15 min−1 mgcatalyst−1, a low yield of toxic NO2−-N intermediate (≤0.4 mg/L) and an exceptional high NH3-N selectivity of 98.1% in treating 22.5 mg/L of NO3−-N under a potential of -0.60 V vs. RHE, outperforming most of the reported oxide-based catalysts. When comparing the performance of U-TiO2 with that of the solid amorphous TiO2 counterpart (A-TiO2) that had close particle size but more OV on surfaces, we identified that the OV was the reactive sites, but rather than its content, the NO3RR kinetics were primarily limited by the electron and mass transfer at U-TiO2/water interfaces. Accordingly, the superior performance of U-TiO2 to A-TiO2 could be ascribed to the hierarchical urchin-like structure in U-TiO2. The in-situ DEMS test revealed that the NO3RR on U-TiO2 followed a pathway of *NO3− → *NO2−→ *NO → *N → *NH → *NH2 → *NH3. We also demonstrated that the U-TiO2 could keep its robust performance under a wide NO3−-N concentration range and in the presence of some co-existing ions (such as Ca2+, Cl−, Mg2+). However, the presence of humic acid and CO32− in water slowed down the NO3RR on U-TiO2. This work provides a more fundamental insight into the OV-driven NO3RR process on TiO2, which should benefit for the development of efficient TiO2-based catalysts.
The trade-off between mass-loading and cycling stability is always a big challenge for iron oxide-based electrodes. Herein, α-Fe2O3 nanoparticles uniformly anchored on nitrogen-doped wood carbons with high mass-loading have been synthesized via a facile electrodeposition method accompanied by post-heating treatment. The resultant composite delivers a high specific capacitance of 603 F/g at 0.1 A/g and superior capacitance retention of 85.5% after 10,000 cycles at 10 A/g, indicating excellent long-term cycling stability. Such excellent electrochemical performance can be attributed to the synergistic effects of α-Fe2O3 nanoparticles and the conductive matrix as well as the formation of interfacial Fe-O-C bonding, which enables the composite electrode to provide plenty of accessible redox active sites, sufficient electron transport and electrolyte ions diffusion, and robust interfacial interaction. Consequently, the asymmetrical supercapacitor exhibits a high energy density of 30.3 Wh/kg at 125 W/kg, suggesting its great potential for practical applications.
Bacterial infection of wounds is an escalating medical problem, issuing threats to both global public health and personal health. Photothermal antibacterial technology as a novel sterilization strategy has outstanding sterilization efficiency, high safety and low risk of emergence of drug-resistant bacteria. By combining inherent antibacterial activity and light-assisted antibacterial treatment, developing novel multifunctional dressings with synergistic high-efficiency antibacterial effects and also promoting wound healing possesses attractive advantages in the field of treating bacterial wound infections in clinical care. Herein, a multifunctional hydrogel formed by in situ photo-cross linking was designed and prepared by first grafting methacrylic anhydride as a photosensitizer onto chitosan, and then introducing oxidatively synthesized polydopamine (PDA). The physicochemical characterizations of the synthesized hydrogels demonstrated their tunability certainly associated with PDA concentration, including pore size, water swelling, rheological properties and in vitro degradability. In addition, the composite hydrogels exhibited good adhesion, anti-oxidation and photothermal properties due to the existence of PDA. Within 10 min upon exposure to 808 nm near-infrared (NIR) light irradiation, this hydrogel system displayed outstanding antibacterial activity against Staphylococcus aureus with almost 100% killing efficiency, of which rapid efficient sterilization plays a significant role in wound healing. Moreover, the hydrogel is capable of cytocompatibility and has low toxicity to murine fibroblasts (L929 and NIH/3T3). In the full-thickness wound defect infection model in mice, the wound closure ratio, inflammatory response, fibroblasts, neovascularization and epithelialization were measured. Animal experiments also reveal that the hydrogel assisted with NIR laser irradiation can inhibit effectively infection at an early stage and accelerate the wound healing process. In summary, this novel multifunctional injectable hydrogel exhibits excellent swelling capacity, bio-adhesion, antioxidant property, photothermal activity, efficient antibacterial property and facilitates skin healing, which has great promising application as a medical dressing biomaterial in infected wound care fields.
There are some critical issues hindering the practical applications of aqueous zinc-ion batteries (ZIBs), although they possess high safety and low cost as one of promising energy storge devices, such as the Zn dendrite growth and the by-product of Zn4SO4(OH)6·xH2O (ZHS) resulted from some side reactions in a mild electrolyte. Herein, a compact and self-repairing solid electrolyte interface (SEI) film, as labeled the PVDF-Zn(TFSI)2-ZHS coating [The PVDF and Zn(TFSI)2 are polyvinylidene fluoride and zinc bis(trifluoromethanesulfonyl)imide, respectively], which turns the in-situ generated ZHS into a beneficial ingredient onto the pre-coated PVDF-based composite coating layer containing Zn(TFSI)2, was designed and fabricated by a simple doctor blade method. It is shown that the SEI layer can effectively isolate Zn from the electrolyte and homogenize the Zn2+ flux, and thus effectively suppress side reactions and dendrites growth. Benefiting from the hybrid SEI layer, a symmetric cell exhibits a high cycling stability over 750 h at 2.0 mA/cm2 and 2.0 mAh/cm2, and meanwhile, a full-cell, coupled with K+ pre-intercalation α-MnO2 (KMO) cathode, displays excellent rate performance, stable coulombic efficiency and an acceptable cycle life. This work provides a feasible approach for simple and scalable modification of Zn anodes to achieve high performance.
Herein, we review the significant of ordered macroporous (OM) TiO2-based catalysts for boosting photocatalytic CO2 reduction. Based on the need to improve the three key factors of photogenerated charge separation efficiency, solar energy utilization and CO2 adsorption rate during the conversion of CO2 to H2O, we summarized five modification measures: including doping ions into OM TiO2, introducing second semiconductor coupling and noble metal nanoparticles for fabricating multiple Z-scheme heterojunctions, constructing hierarchical pore and carbon-loaded OM TiO2 materials, which effectively enhance the absorption rate of visible light, the separation rate of electrons-hole pairs and the selection of multiple active sites. The OM structured TiO2-based photocatalysts solve the single or multiple key factors for enhancing photocatalytic performances during CO2 conversion. The catalytic mechanism and pathways of OM structured TiO2-based photocatalysts for CO2 reduction are discussed and summarized. It provides new insights on the development of high-efficient catalyst for photocatalytic CO2 conversion to solar fuels.
Ammonia borane (NH3BH3, AB) is an ideal raw material of hydrogen production with higher hydrogen storage capacity. In this paper, the catalytic processes of AB dehydrogenation were described from different ways, including thermal dehydrogenation, hydrolysis, methanolysis, photocatalysis and photo-piezoelectric synergy catalysis with experimental research and theoretical calculations. Catalyst models include bulk materials, two-dimensional materials, nanocluster particles and single/diatomic structures. Among them, the proportion of H2 released is different, and the reaction conditions are also different, which are suitable for different application scenarios. Through this review, we could have a preliminary comprehensive understanding of AB dehydrogenation reaction.
Rho-associated coiled-coil-containing protein kinase (ROCK) belongs to the serine-threonine family, and ROCK is involved in a variety of biological processes including cell migration, adhesion, proliferation and differentiation through phosphorylation of different downstream substrates. The aberrant activation of ROCK is associated with the pathological conditions in different systems including various diseases, including cancer, neurological diseases, inflammation, cardiovascular diseases and glaucoma. Therefore, the ROCK inhibitors have potential applicability for treating the aforementioned diseases. Four small molecule ROCK inhibitors have been approved for clinical use: fasudil, ripasudil, netarsudil and belumosudil. In recent years, more small molecule ROCK inhibitors have been identified. This paper reviews the ROCK inhibitors reported in past seven years. We mainly focused on the summarization of the structure–activity relationships, inhibitory efficacy, pharmacological mechanisms and the relevant clinical studies of the reported ROCK inhibitors. Besides the small molecular inhibitors, the peptides and biological extracts which exhibit ROCK inhibitory effects are also included. We also provide suggestions for the future development of the potent ROCK inhibitors.
Electrochemistry with antifouling sensing interfaces that effectively resist the adsorption of nonspecific biomolecules provides a powerful mean for the accurate and sensitive detection of disease biomarkers in complex biofluids. However, there are few strategies to acquire a stable and solid antifouling coating on any substrate by a simple way. Herein, a simple one-step assembly method has been adopted to construct phase-transited bovine serum albumin (PTB) antifouling layers. Prior to construction of the antifouling layers, the poly(3,4-ethylenedioxythiophene) (PEDOT) doped with 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (ionic liquid, IL) were firstly electrodeposited on bare electrodes, endowing good conductivity and catalytic capability for the developed sensor. Subsequently, with the assist of tris(2-carboxyethyl)phosphine (TCEP), the disulfide bonds of bovine serum albumin (BSA) were reduced to form PTB, which can be coated on the PEDOT-IL modified electrode to construct an antifouling electrochemical senor (PTB/PEDOT-IL/GCE) for the detection of uric acid (UA) in human serum. The UA sensor demonstrated a good linear range from 1.11 µmol/L to 798.9 µmol/L, with a high sensitivity of 0.556 µA µmol L−1 cm−2. The combination of conducting polymers with one-step assembly of PTB offers a universal and reliable method for the modification of various electrodes to determine target molecules in complex human body fluids.
Photo-catalytic oxidation of intracellular nicotinamide adenine dinucleotide (2′-phosphate) (NAD(P)H) has attracted much attention for cancer therapy. However, the general oxygen-dependent mechanism heavily depresses the efficacy in hypoxic tumors. To solve this problem, herein platinum nanoparticles (Pt NPs) with catalase-like (CAT-like) and catalytic H2 evolution activities were introduced as a powerful assistant to enhance the photo-catalytic NAD(P)H oxidation of Ru1 ([Ru(phen)2(PIP-OCH3)]2+, phen = 1,10-phenanthroline, PIP-OCH3 = 2-(4–methoxy phenyl)-1H-imidazo[4,5-f][1,10]phenanthroline) under hypoxic and even oxygen-free conditions. Firstly, Pt NPs can transform the original and in situ formed H2O2 once again into O2 by the CAT-like activity, thus relieving tumor hypoxia and realizing cyclic utilization (at least in part) of the precious oxygen in hypoxia. Secondly, Pt NPs can also be served as H2 evolution catalysts while using Ru1 as the photosensitizer and NAD(P)H as the electron and proton donor. In this process, NAD(P)H is oxidized without the participation of oxygen, which can provide an effective way even under oxygen-free conditions. Via co-encapsulation of Ru1 and Pt NPs in bovine serum albumin (BSA) with tumor targeting ability, the resultant Ru/Pt@BSA could photo-catalyze intracellular NAD(P)H oxidation under hypoxic conditions (3% O2), and exhibited an efficient and selective anticancer activity both in vitro and in vivo. Our results may provide new sights for efficient and targeted cancer treatment under hypoxic conditions.
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