Latest ArticlesIn this paper, Ni3S2 nanosheet (NS) was generated by chemical etching with sodium sulfide directly on the nickel foam (NF), which was induced by dielectric barrier discharge plasma in liquid. Compared with other chemical etching methods of nickel-based nanomaterials, this method was not only rapid (40 min) and mild (at room temperature and atmospheric pressure), but also showed consistent stability and good reproducibility. The Ni3S2 NS/NF electrode showed excellent performance in the electrochemical detection of formaldehyde under alkaline conditions. It had a good linear relationship with the concentration of formaldehyde in the range of 0.002-5.45 mmol/L (R2 = 0.9957) and the limit of detection (LOD) was 1.23 µmol/L (S/N = 3). The sensitivity was 1286.9 µA L mmol‒1 cm‒2, and the response time was about 5 s. The plasma-induced chemical etching strategy provides a simple and stable electrode preparation method, which has great application prospects in nonenzymatic electrochemical sensors.
Microfluidic devices have become a powerful tool for chemical and biologic applications. To control different functional parts on the microchip, valve plays a key role in the device. In conventional methods, physio-mechanical valves are usually used on microfluidic chip. Herein, we reported a chemo-mechanical switchable valve on microfluidic chip by using a thermally responsive block copolymer. The wettability changes of capillary with copolymer modification on inner surface were investigated to verify the function as a valve. Capillaries with modification of poly-(N-isopropylacrylamide-co-hexafluoroisopropyl acrylate) (P(NIPAAm-co-HFIPA)) with a 20% HFIPA was demonstrated capable of control aqueous solution stop or go through. Then short capillaries with copolymer modification were integrated in microchannels as valves. With the temperature changing around lower critical solution temperature (LCST), the integrated chemo-mechanical switchable valve exhibited excellent "OPEN–CLOSE'' behavior for microflow control. After optimization of the block copolymer sequences and molar ratio, a switching time as low as 20 s was achieved. The developed micro valve was demonstrated effective for flow control on microchip.
An efficient photo-Fenton catalyst (FeS2@HTCN) was designed by maximizing the synergistic effect of FeS2 nanoparticles and hollow tubular g-C3N4 (HTCN). Molecule self-assembly and molten salts-assisted calcination were used to engineering the hollow structured g-C3N4 before anchoring FeS2 nanoparticles on the walls of HTCN via reflux method. Compared to bulk g-C3N4, the unique structure of HTCN and heterojunction in the composite endowed FeS2@HTCN with more active sites and abundant channels for electron transfer and charge separation. The enriched electrons can improve the Fe3+ recycling and boost Fe2+ catalyzed •OH production via H2O2. As-prepared photo-Fenton catalyst was successfully applied to the treatment of industrial paint wastewater. The paint wastewater with its COD as high as 8200 mg/L can be effectively degraded with 0.2 mol/L H2O2 in 90 min under visible light irradiation. The photo-Fenton system was further evaluated according to the process stability and economic benefit, proving that the strategy presented in this work would be applicable to the treatment of real wastewater.
Understanding the impact of substituents on the quantum interference effect at single molecule scale is of great importance for the design of molecular devices. In this work, three platinum(Ⅱ) complexes with –H, –NH2 and –NO2 groups on conductive backbones were designed and synthesized. Single-molecule conductance, which was measured using scanning tunnelling microscope break junction (STM-BJ) technique, demonstrated a conductance freeze phenomenon under the variation of substituents. Theoretical study revealed that, despite the electronic effect of the substituents shifting the energy level of molecular orbital, the quantum interference effect vanished the influence of electronic effect on the conductance and eventually leaded to the conductance freeze.
The thermal decomposition of AgNO3 is known to produce metallic Ag, but single-atomic dispersion is hard to achieve instead of the aggregation state of nanoparticles. Herein, we develop an efficient approach to thermally generate and stabilize single Ag atoms via the coordination effect. Two desired Co-Ag phosphonates [Ag2ⅠCo2Ⅲ(notpH3)2(NO3)]X [X = NO3− (1) or ClO4− (2)] were synthesized by solid-phase grinding method or solution crystallization. Both crystal structures reveal slightly different packing arrangements of various lattice anions and identical one-dimensional (1-D) coordination chains, formed in each case by the coordination of Ag(Ⅰ) to the metalloligand Co(notpH3) and NO3− anion. The number of Ag(Ⅰ) ions connected to each NO3− anion reduces from 5 in bulk AgNO3 to 2 in compounds 1 and 2, leading to the AgNO3 component stepwise decomposition at a lower temperature (< 300 ℃). During the thermal decomposition, the changes of supermolecular structures and Ag oxidation states were monitored by PXRD, IR and XAFS measurements. The most interesting finding is that 1 and 2 can retain chain structures and harvest Ag(0) atoms in the chain by controlling decomposition temperatures (220 ℃ for 1 and 254 ℃ for 2).
Aggregation-induced emission (AIE) based luminescent materials are generating intensive interest due to their unique fluorescence in the aggregation state. Herein we report a strategy of dynamic covalent chemistry (DCC) controlled AIE luminogens for the regulation of multicolor emission in reversible covalent polymer networks. Tetraphenylethene derived ring-chain tautomers were prepared, and the emission was readily controlled through multimode, such as changing the solvent, adding the base, and dynamic covalent reactions with amines. Moreover, the construction of dynamic covalent cross-linked luminescent hydrogels with tunable fluorescent, self-healing, and mechanical properties, was realized. The combination of AIE and aggregation-caused quenching (ACQ) fluorophores in the polymer network further enabled the realization of a multicolor modulator, including white emission, in both solution and gel states. The strategies and results presented should find utility in dynamic assemblies, polymer networks, chemical sensing, and responsive materials.
Two-dimensional (2D) covalent organic framework nanosheets (CONs) are attracting increasing research attention because of their unique properties derived from their ultrathin thickness, high surface-to-volume atomic ratio, and extremely large surface area. 2D CONs can provide high transport pathways for charge carriers (e.g., electrons, holes and ions) through either the conjugated skeletons or the open channels. Therefore, they have shown great potential in energy related applications. In this review, we firstly introduce the recent developments and characteristics of 2D CONs by focusing on the two typical synthetic methods, i.e., top-down and bottom-up methods. Then, the energy-related applications in energy storage and conversion of 2D CONs are summarized. Finally, we give our personal views on the challenges and perspectives for the future research of 2D CONs and their composites.
Ammonia borane (NH3BH3, AB) has been considered to be a promising chemical hydrogen storage material. Based on density functional theory, a series of transition metal atoms supported P3C (P3C_O) sheet is systematically investigated to screen out the most promising catalyst for dehydrogenation of AB. The results indicate that the Os/P3C and Os/P3C_O could be an efficient single atom catalyst (SACs) and the stepwise reaction pathway with free energy barrier of 2.07 and 1.54 eV respectively. Remarkably, the rate constant further quantitatively confirmed the real situation of the first step of dehydrogenation of AB on the Os/P3C and Os/P3C_O substrates. We found that kf1 at 400 K is equivalent to kf2 at 800 K, which greatly improves the temperature of the first step of AB dehydrogenation on P3C_O. We hope this work can provide a promising method for the design of catalysts for AB dehydrogenation reactions on the surface of two-dimensional materials (2D).
The selection and development of cathode of alkaline zinc batteries (AZBs) is still hindered and often leads to poor rate capability and short cycle life. Here, amorphous hollow nickel-cobalt-based sulfides nanocages with nanosheet arrays (AM-NCS) are designed and constructed with ZIF-67 as the self-template to exchange with Ni2+ and S2− by using a two-step ion exchange method. The synthesized AM-NCS possess the high specific capacity (160 mAh/g at 2 A/g), and the assembled battery has excellent rate performance (146 mAh/g reversible capacity at 5 A/g). The assembled device has excellent rate performance (155 mAh/g at 2 A/g) and long cycling stability (7000 cycles, 62.5% of initial capacity). The excellent electrochemical properties of the electrode materials are mainly attributed to the unique structure, in particular, polyhedron structure with hollow structure can improve the cyclic stability, and the amorphous structure can expose more reactive sites on the surfaces of nickel, cobalt and sulfur. This work provides a new strategy for the design and fabrication of high performance cathode materials for AZBs.
The simplification of localized surface plasmon resonance (LSPR) detection can further promote the development of optical biosensing application in point-of-care testing. In this study, we proposed a simple light emitting diode (LED) based single-wavelength LSPR sensor modulated with bio-electron transfers for the detection of electroactive biomolecules. Indium tin oxide electrode loaded with nanocomposites of polyaniline coated gold nanorod was used as LSPR chip, and the applied electric potential was scanned at the LSPR chip for single-wavelength LSPR biosensing. Under the scanning of applied potentials, biological electron transfer of redox reaction was employed to demonstrate the bioelectronic modulation of single-wavelength LSPR for selective electroactive biomolecule detection. Without any additional recognition material, electroactive biomolecules uric acid and dopamine were detected directly with a sensitivity of 5.05 μmol/L and 7.11 μmol/L at their specific oxidation potentials, respectively. With the simplified optical configuration and selective bioelectronic modulation, the single-wavelength LSPR sensor is promising for the development of simple, low-cost, and high specificity optical biosensor for point-of-care testing of electroactive biomolecules.
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