Latest ArticlesThe 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.
A copper-catalyzed three-component reaction of alkenes, cycloketone oximes and DABCO·(SO2)2 is developed, which provides a convenient route for the synthesis of diverse (E)-cyanoalkylsulfonyl alkenes in moderate to good yields with excellent regio- and stereoselectivity. A broad substrate scope with excellent functional group tolerance is observed. A plausible radical pathway is proposed, which involves copper-catalyzed ring-opening CC bond cleavage of O-acyl oxime and insertion of sulfur dioxide. During the reaction process, cyanoalkyl radical and cyanoalkylsulfonyl radical are the key intermediates.
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.
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.
Monovalent cation perm-selective membrane (MCPMs) allow fast and selective transport of monovalent cations, and they are promisingly required for extraction of special ions, such as lithium extraction, acid recovery and sea salt production. Herein, we report a novel strategy to design the critical functional layers of MCPMs with both space charge repulsion and cross-linked dense screenability. The in-situ deposition polymerization of pyrrole was carried out on the surface of sulfonated polyphenyl sulfone (SPPSU) substrate membrane followed by cross-linking quaternization of the polypyrrole (PPy) layer with diiodinated functional molecules, thus, the membrane obtained more excellent selective permeability and stable transport properties of monovalent cations. It confirms that the designed PPy layers with charged surface and cross-linking structure improved the hydrophilicity, facilitated cation transport and increased ion flux. Meanwhile, for the dense PPy layer, the charged cross-linked structure endowed the functional layer with the synergistic characteristics of Donnan exclusion and pore size sieving for positively charged ions, which improved the monovalent cation perm-selectivity of the membranes. At a constant current density of 5.1 mA/cm2, the optimal membrane exhibited superior perm-selectivity (PMgNa) and monovalent cation flux (JNa+ = 2.80×10 -8 mol cm-2 s-1) during electrodialysis.
Applying mixed oxygen ionic and electronic conducting (MIEC) oxides as the cathode offers a promising solution to enhance the performance of solid oxide fuel cells (SOFCs). However, the phase instability in CO2-containing air and sluggish oxygen reduction activity of MIEC cathodes remain a long-term challenge for optimizing the electrochemical performance of SOFCs. Herein, a heterovalent co-doping strategy is proposed to enhance the oxygen reduction activity and CO2 tolerance of SOFCs cathodes, which can be demonstrated by developing a novel BaCo0.6Fe0.4O3-δ (BCF)-based MIEC oxide, BaCo0.6Fe0.2Sn0.1Y0.1O3-δ (BCFSY). In addition to improving the stability of BCF-based perovskites, this strategy achieves an optimized balance of ionic mobility and oxygen vacancies due to the synergies between the effects of the co-dopants. Compared with single-doped materials, BCFSY exhibits improved CO2 tolerance and considerably higher ORR activity, which is reflected in a significantly lower polarization resistance of 0.15 Ω cm2 at 600 ℃. The results of this work provide an efficient tactic for designing electrode materials for SOFCs.
Alcohol fuels oxidation plays a significant role in carbon sustainable cycling and high-performance catalyst with a strong anti-poisoning effect is desired. Herein, Pt-Ni alloy supported on the N-doped graphene aerogel synthesized by simple freeze-drying and annealing was demonstrated to have such catalytic ability for alcohol fuel oxidation. Pt-Ni alloy particles were found uniformly dispersed over the surface of 3D N-doped graphene aerogel. High anti-poisoning ability for CO-like intermediates oxidation was demonstrated by the CO-stripping experiment. The as-prepared catalyst was found to have outstanding catalytic performance for methanol and ethanol oxidation with high catalytic activity, stability and catalytic kinetics. Compared to the control samples, the improved catalytic ability could be due to the presence of oxophilic Ni species and the support effect of 3D N-doped graphene aerogel that combined multi-advantages of large surface area, facile mass transfer, and abundant defects.
An organic-inorganic hybrid FeIII–PrIII-included 2-germano-20-tungstate [Pr(H2O)8]2H2[Fe4(H2O)4 (pca)4Ge2W20O72]•34H2O (Hpca = 2-pyridinecarboxylic acid) (1) was hydrothermally prepared. Its polyoxoanion comprises one tetra-FeIII incorporated [Fe4(H2O)4(pca)4Ge2W20O72]8- hybrid entity and two [Pr(H2O)8]3+ ornamental cations. The [Fe4(H2O)4(pca)4Ge2W20O72]8- 2-germano-20-tungstate entity can be regarded as an infrequent S-type [Ge2W20O72]16- cluster pocketed by four [Fe(H2O)(pca)]2+ cations. The S-type [Ge2W20O72]16- cluster could be imagined as condensation of two divacant Keggin [α-GeW10O37]10- segments by sharing two atoms. It is of interest is that carboxyl O and pyridine N atoms on pca ligands concurrently bind with Fe3+ cations in a five-membered heterocyclic fashion to increase the stability of the whole structure. Furthermore, the electrochemical biosensing properties of 1 as the modified electrode material have been investigated for detecting norepinephrine (NPP), showing a low detection limit of 3.25 µmol/L. This work not only enriches structures of heterometallic germanotungstates (GTs), but also expands applications of polyoxometalates (POMs) in the electrochemical biosensing field.
Zinc-ion batteries (ZIBs), in particular quasi-solid-state ZIBs, occupy a crucial position in the field of energy storage devices owing to the superiorities of abundant zinc reserve, low cost, high safety and high theoretical capacity of zinc anode. However, as divalent Zn2+ ions experience strong electrostatic interactions when intercalating into the cathode materials, which poses challenges to the structural stability and higher demand in Zn2+ ions diffusion kinetics of the cathode materials. Here, a microwave-assisted hydrothermal method is adopted to prepare pre-potassiated hydrated vanadium pentoxide (K0.52V2O5·0.29H2O, abbreviated as KHVO) cathode material, in which the potassium ions pre-inserted into the interlayers can act as "pillars" to stabilize the lamellar structure, and crystal water can act as "lubricant" to improve the diffusion efficiency of Zn2+ ions. Consequently, the KHVO displays high electrochemical properties with high capacity (~300 mAh/g), superior rate capability (69 mAh/g at 5 A/g) and ultralong cycling performance (> 1500 cycles at 2 A/g) in quasi-solid-state ZIBs. These superior Zn storage properties result from the large diffusion coefficient and highly stable and reversible Zn2+ (de)intercalation reaction of KHVO.
Prostate cancer (PCa) is the second most commonly diagnosed cancer in men. The Rac1-GTP inhibitor NSC23766 has been shown to suppress PCa growth. However, these therapies have low tumor-targeting efficacy in vivo. Therefore, it is essential to produce a drug delivery system that specifically targets the tumor site. Herein, novel l-phenylalanine-based poly(ester amide) (Phe-PEA) polymers were synthesized and loaded with NSC23766 (NSC23766@8P6 NPs), which had a small particle size (162.3 ± 6.7 nm) and high NSC23766 loading (8.0% ± 1.1%) with a more rapid release of NSC23766 at pH 5.0. In vitro cellular uptake and cytotoxicity assays demonstrated that NSC23766@8P6 NPs were rapidly taken up by PC3 cells and showed significant effects of PCa cell proliferation inhibition and G2/M phase arrest. Furthermore, in vivo studies using PC3-bearing mice demonstrated that NSC23766@8P6 NPs delivered by intravenous injection not only increased the drug concentration with prolonged retention (96 h) at the tumor site, but also inhibited tumor growth and induced apoptosis. In conclusion, we have discovered that NSC23766@8P6 NPs can serve as a delivery system that targets the tumor site and is therefore a promising therapeutic approach for PCa treatment.
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