The precise control of the size, morphology, surface chemistry, and assembly process of each component is important to construction of integrated functional nanocomposites. We report here the fabrication of multifunctional microspheres which possess a core of nonporous silica-protected magnetite particles, transition layer of active gold nanoparticles, and an outer shell of ordered mesoporous silica with perpendicularly aligned pore channels. The well-designed microspheres have high magnetization (18.6 emu/g), large surface area (236 m(2)/g), highly open mesopores (approximately 2.2 nm), and stably confined but accessible Au nanoparticles and, as a result, show high performance in catalytic reduction of 4-nitrophenol (with conversion of 95% in 12 min), styrene epoxidation with high conversion (72%) and selectivity (80%), especially convenient magnetic separability, long life and good reusability. The unique nanostructure makes the microsphere to be a novel stable and approachable catalyst system for various catalytic industry processes.
Producing electrolytes with high ionic conductivity has been a critical challenge in the progressive development of solid oxide fuel cells (SOFCs) for practical applications. The conventional methodology uses the ion doping method to develop electrolyte materials, e.g., samarium-doped ceria (SDC) and yttrium-stabilized zirconia (YSZ), but challenges remain. In the present work, we introduce a logical design of non-stoichiometric CeO 2-δ based on non-doped ceria with a focus on the surface properties of the particles. The CeO 2−δ reached an ionic conductivity of 0.1 S/cm and was used as the electrolyte in a fuel cell, resulting in a remarkable power output of 660 mW/cm 2 at 550°C. Scanning transmission electron microscopy (STEM) combined with electron energy-loss spectroscopy (EELS) clearly clarified that a surface buried layer on the order of a few nanometers was composed of Ce 3+ on ceria particles to form a CeO 2−δ @CeO 2 core-shell heterostructure. The oxygen deficient layer on the surface provided ionic transport pathways. Simultaneously, band energy alignment is proposed to address the short circuiting issue. This work provides a simple and feasible methodology beyond common structural (bulk) doping to produce sufficient ionic conductivity. This work also demonstrates a new approach to progress from material fundamentals to an advanced lowtemperature SOFC technology.
We present an electrical sensor that uses rolling circle amplification (RCA) of DNA to stretch across the gap between two electrodes, interact with metal nanoparticle seeds to generate an electrically conductive nanowire, and produce electrical signals upon detection of specific target DNA sequences. RCA is a highly specific molecular detection mechanism based on DNA probe circularization. With this technique, long single-stranded DNA with simple repetitive sequences are produced. Here we show that stretched RCA products can be metalized using silver or gold solutions to form metal wires. Upon metallization, the resistance drops from TΩ to kΩ for silver and to Ω for gold. Metallization is seeded by gold nanoparticles aligned along the single-stranded DNA product through hybridization of functionalized oligonucleotides. We show that combining RCA with electrical DNA detection produces results in readout with very high signal-to-noise ratio, an essential feature for sensitive and specific detection assays. Finally, we demonstrate detection of 10 ng of Escherichia coli genomic DNA using the sensor concept.
Organophosphorus
pesticides (OPs) can inhibit the activity of acetylcholinesterase
(AChE) to induce neurological diseases. It is significant to exploit
a rapid and sensitive strategy to monitor OPs. Here, a metal–organic
framework (MOF) acted as a carrier to encapsulate AuNCs, which can
limit the molecular motion of AuNCs, trigger the aggregation-induced
emission (AIE) effect, and exhibit a strong fluorescence with a fluorescence
lifetime and quantum yield of 6.83 μs and 4.63%, respectively.
Then, the marriage of fluorescence and colorimetric signals was realized
on the basis of the dual function of the enzymolysis product from
AChE and choline oxidase (CHO) on AuNCs@ZIF-8. First, it can decompose
ZIF-8 to weaken the restraint on AuNCs, and thus the fluorescence
receded. Second, it can be used as a substrate for the peroxidase
mimics of the released AuNCs to oxidize 3,3′,5,5′-tetramethylbenzidine
(TMB) and a visible blue appeared. Thus, on the basis of the inhibition
of AChE activity by OPs, a fluorescence–colorimetric dual-signal
biosensor was established. In addition, colorimetric paper strips
were exploited to realize a visual semiquantitative detection, and
a smartphone APP was developed to make the visualization results more
precise and realize real-time supervision of pesticide contamination.
Since colossal ionic conductivity was detected in the planar heterostructures consisting of fluorite and perovskite, heterostructures have drawn great research interest as potential electrolytes for solid oxide fuel cells (SOFCs). However, so far, the practical uses of such promising material have failed to materialize in SOFCs due to the short circuit risk caused by SrTiO3. In this study, a series of fluorite/perovskite heterostructures made of Sm-doped CeO2 and SrTiO3 (SDC–STO) are developed in a new bulk-heterostructure form and evaluated as electrolytes. The prepared cells exhibit a peak power density of 892 mW cm−2 along with open circuit voltage of 1.1 V at 550 °C for the optimal composition of 4SDC–6STO. Further electrical studies reveal a high ionic conductivity of 0.05–0.14 S cm−1 at 450–550 °C, which shows remarkable enhancement compared to that of simplex SDC. Via AC impedance analysis, it has been shown that the small grain-boundary and electrode polarization resistances play the major roles in resulting in the superior performance. Furthermore, a Schottky junction effect is proposed by considering the work functions and electronic affinities to interpret the avoidance of short circuit in the SDC–STO cell. Our findings thus indicate a new insight to design electrolytes for low-temperature SOFCs.
A new approach was developed to control the size of gold nanoparticles in citrate reduction by altering the concentration of chloride ions. The size of the as-prepared gold nanoparticles could be tuned in the range 19-47 nm at a specific molar ratio of citrate and tetrachloroauric acid (5:1) by simply changing the concentration of chloride ions from 0 to 20 mM. UV-visible spectra and TEM observations showed that the increased size of the gold particles was primarily related to the promoted aggregation of the primary gold particles. The aggregation was attributed to their decreased surface charge as the chloride ion concentration in the reaction solutions increased. This approach could also be extended to other reaction systems, for example, the size of gold nanoparticles prepared by NaBH(4) reduction increased from 3 to 12 nm as the chloride ion concentration was increased from 0 to 20 mM.
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