Latest ArticlesThe formation of bacterial biofilms closely associates with infectious diseases. Until now, precise diagnosis and effective treatment of bacterial biofilm infections are still in great need. Herein, a novel multifunctional theranostic nanoplatform based on MnO2 nanosheets (MnO2 NSs) has been designed to achieve pH-responsive dual-mode imaging and hypoxia-relief-enhanced antimicrobial photodynamic therapy (aPDT) of bacterial biofilm infections. In this study, MnO2 NSs were modified with bovine serum albumin (BSA) and polyethylene glycol (PEG) and then loaded with chlorin e6 (Ce6) as photosensitizer to form MnO2-BSA/PEG-Ce6 nanosheets (MBP-Ce6 NSs). After being delivered into the bacterial biofilm-infected tissues, the MBP-Ce6 NSs could be decomposed in acidic biofilm microenvironment and release Ce6 with Mn2+, which subsequently activate both fluorescence (FL) and magnetic resonance (MR) signals for effective dual-mode FL/MR imaging of bacterial biofilm infections. Meanwhile, MnO2 could catalyze the decomposing of H2O2 in biofilm-infected tissues into O2 and relieve the hypoxic condition of biofilm, which significantly enhances the efficacy of aPDT. An in vitro study showed that MBP-Ce6 NSs could significantly reduce the number of methicillin-resistant Staphylococcus aureus (MRSA) in biofilms after 635 nm laser irradiation. Guided by FL/MR imaging, MRSA biofilm-infected mice can be efficiently treated by MBP-Ce6 NSs-based aPDT. Overall, MBP-Ce6 NSs not only possess biofilm microenvironment-responsive dual-mode FL/MR imaging ability but also have significantly enhanced aPDT efficacy by relieving the hypoxia habitat of biofilm, which provides a promising theranostic nanoplatform for bacterial biofilm infections.
The optimization of thermoelectric materials involves the decoupling of the transport of electrons and phonons. In this work, an increased Mg1-Mg2 distance, together with the carrier conduction network protection, has been shown as an effective strategy to increase the weighted mobility () and hence thermoelectric power factor of Mg3+δSb2-yBiy family near room temperature. Mg3+δSb0.5Bi1.5 has a high carrier mobility of 247 cm2 V-1 s-1 and a record power factor of 3470 μW m-1 K-2 at room temperature. Considering both efficiency and power density, Mg3+δSb1.0Bi1.0 with a high average ZT of 1.13 and an average power factor of 3184 μW m-1 K-2 in the temperature range of 50-250°C would be a strong candidate to replace the conventional n-type thermoelectric material Bi2Te2.7Se0.3. The protection of the transport channel through Mg sublattice means alloying on Sb sublattice has little effect on electron while it significantly reduces phonon thermal conductivity, providing us an approach to decouple electron and phonon transport for better thermoelectric materials.
Optimization problems especially in a dynamic environment is a hot research area that has attracted notable attention in the past decades. It is clear from the dynamic optimization literatures that most of the efforts have been devoted to continuous dynamic optimization problems although the majority of the real-life problems are combinatorial. Moreover, many algorithms shown to be successful in stationary combinatorial optimization problems commonly have mediocre performance in a dynamic environment. In this study, based on binary wolf pack algorithm (BWPA), combining with flexible population updating strategy, a flexible binary wolf pack algorithm (FWPA) is proposed. Then, FWPA is used to solve a set of static multidimensional knapsack benchmarks and several dynamic multidimensional knapsack problems, which have numerous practical applications. To the best of our knowledge, this paper constitutes the first study on the performance of WPA on a dynamic combinatorial problem. By comparing two state-of-the-art algorithms with the basic BWPA, the simulation experimental results demonstrate that FWPA can be considered as a feasibility and competitive algorithm for dynamic optimization problems.
With the recent advance in chemical modification of fullerenes, electrosynthesis has demonstrated increasing importance in regioselective synthesis of novel fullerene derivatives. Herein, we report successively regioselective synthesis of stable tetra- and hexafunctionalized [60]fullerene derivatives. The cycloaddition reaction of the electrochemically generated dianions from [60]fulleroindolines with phthaloyl chloride regioselectively affords 1,2,4,17-functionalized [60]fullerene derivatives with two attached ketone groups and a unique addition pattern, where the heterocycle is rearranged to a [5,6]-junction and the carbocycle is fused to an adjacent [6,6]-junction. This addition pattern is in sharp contrast with that of the previously reported biscycloadducts, where both cycles are appended to [6,6]-junctions. The obtained tetrafunctionalized compounds can be successively manipulated to 1,2,3,4,9,10-functionalized [60]fullerene derivatives with an intriguing “S”-shaped configuration via a novel electrochemical protonation. Importantly, the stability of tetrafunctionalized [60]fullerene products allows them to be applied in planar perovskite solar cells as efficient electron transport layers.
Exhaled acetone is one of the representative biomarkers for the noninvasive diagnosis of type-1 diabetes. In this work, we have applied a facile two-step chemical bath deposition method for acetone sensors based on α-Fe2O3/SnO2 hybrid nanoarrays (HNAs), where one-dimensional (1D) FeOOH nanorods are in situ grown on the prefabricated 2D SnO2 nanosheets for on-chip construction of 1D/2D HNAs. After annealing in air, ultrafine α-Fe2O3 nanorods are homogenously distributed on the surface of SnO2 nanosheet arrays (NSAs). Gas sensing results show that the α-Fe2O3/SnO2 HNAs exhibit a greatly enhanced response to acetone (3.25 at 0.4 ppm) at a sub-ppm level compared with those based on pure SnO2 NSAs (1.16 at 0.4 ppm) and pure α-Fe2O3 nanorods (1.03 at 0.4 ppm), at an operating temperature of 340°C. The enhanced acetone sensing performance may be attributed to the formation of α-Fe2O3–SnO2 n-n heterostructure with 1D/2D hybrid architectures. Moreover, the α-Fe2O3/SnO2 HNAs also possess good reproducibility and selectivity toward acetone vapor, suggesting its potential application in breath acetone analysis.
Binder-free thin film cathodes have become a critical basis for advanced high-performance lithium ion batteries for lightweight device applications such as all-solid-state batteries, portable electronics, and flexible electronics. However, these thin film electrodes generally require modifications to improve the electrochemical performance. This overview summarizes the current modification approaches on thin film cathodes, where the approaches can be classified as single-phase nanostructure designs and multiphase nanocomposite designs. Recent representative advancements of different modification approaches are also highlighted. Besides, this review discusses the existing challenges regarding the thin film cathodes. The review also discusses the future research directions and needs towards future advancement in thin film cathode designs for energy storage needs in advanced portable and personal electronics.
Designing highly active and robust platinum-free electrocatalysts for hydrogen evolution reaction is vital for large-scale and efficient production of hydrogen through electrochemical water splitting. Here, we report nonprecious intermetallic Cu5Zr clusters that are in situ anchored on hierarchical nanoporous copper (NP Cu/Cu5Zr) for efficient hydrogen evolution in alkaline medium. By virtue of hydroxygenated zirconium atoms activating their nearby Cu-Cu bridge sites with appropriate hydrogen-binding energy, the Cu5Zr clusters have a high electrocatalytic activity toward the hydrogen evolution reaction. Associated with unique architecture featured with steady and bicontinuous nanoporous copper skeleton that facilitates electron transfer and electrolyte accessibility, the self-supported monolithic NP Cu/Cu5Zr electrodes boost violent hydrogen gas release, realizing ultrahigh current density of 500 mA cm-2 at a low potential of -280 mV versus reversible hydrogen electrode, with exceptional stability in 1 M KOH solution. The electrochemical properties outperform those of state-of-the-art nonprecious metal electrocatalysts and make them promising candidates as electrodes in water splitting devices.
Electrochemical water splitting driven by clean and sustainable energy sources to produce hydrogen is an efficient and environmentally friendly energy conversion technology. Water splitting involves hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), in which OER is the limiting factor and has attracted extensive research interest in the past few years. Conventional noble-metal-based OER electrocatalysts like IrO2 and RuO2 suffer from the limitations of high cost and scarce availability. Developing innovative alternative nonnoble metal electrocatalysts with high catalytic activity and long-term durability to boost the OER process remains a significant challenge. Among all of the candidates for OER catalysis, self-supported layered double hydroxides (LDHs) have emerged as one of the most promising types of electrocatalysts due to their unique layered structures and high electrocatalytic activity. In this review, we summarize the recent progress on self-supported LDHs and highlight their electrochemical catalytic performance. Specifically, synthesis methods, structural and compositional parameters, and influential factors for optimizing OER performance are discussed in detail. Finally, the remaining challenges facing the development of self-supported LDHs are discussed and perspectives on their potential for use in industrial hydrogen production through water splitting are provided to suggest future research directions.
Rational synthesis of materials is a long-term challenging issue due to the poor understanding on the formation mechanism of material structure and the limited capability in controlling nanoscale crystallization. The emergent in situ electron microscope provides an insight to this issue. By employing an in situ scanning electron microscope, silver crystallization is investigated in real time, in which a reversible crystallization is observed. To disclose this reversible crystallization, the radicals generated by the irradiation of electron beam are calculated. It is found that the concentrations of radicals are spatiotemporally variable in the liquid cell due to the diffusion and reaction of radicals. The fluctuation of the reductive hydrated electrons and the oxidative hydroxyl radicals in the cell leads to the alternative dominance of the reduction and oxidation reactions. The reduction leads to the growth of silver crystals while the oxidation leads to their dissolution, which results in the reversible silver crystallization. A regulation of radical distribution by electron dose rates leads to the formation of diverse silver structures, confirming the dominant role of local chemical concentration in the structure evolution of materials.
Most of the existing acoustic metamaterials rely on architected structures with fixed configurations, and thus, their properties cannot be modulated once the structures are fabricated. Emerging active acoustic metamaterials highlight a promising opportunity to on-demand switch property states; however, they typically require tethered loads, such as mechanical compression or pneumatic actuation. Using untethered physical stimuli to actively switch property states of acoustic metamaterials remains largely unexplored. Here, inspired by the sharkskin denticles, we present a class of active acoustic metamaterials whose configurations can be on-demand switched via untethered magnetic fields, thus enabling active switching of acoustic transmission, wave guiding, logic operation, and reciprocity. The key mechanism relies on magnetically deformable Mie resonator pillar (MRP) arrays that can be tuned between vertical and bent states corresponding to the acoustic forbidding and conducting, respectively. The MRPs are made of a magnetoactive elastomer and feature wavy air channels to enable an artificial Mie resonance within a designed frequency regime. The Mie resonance induces an acoustic bandgap, which is closed when pillars are selectively bent by a sufficiently large magnetic field. These magnetoactive MRPs are further harnessed to design stimuli-controlled reconfigurable acoustic switches, logic gates, and diodes. Capable of creating the first generation of untethered-stimuli-induced active acoustic metadevices, the present paradigm may find broad engineering applications, ranging from noise control and audio modulation to sonic camouflage.