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11.
The long‐term success of photosynthetic organisms has resulted in their global superabundance, which is sustained by their widespread, continual mass‐production of the integral proteins that photocatalyze the chemical processes of natural photosynthesis. Here, a fast, general method to assemble multilayer films composed of one such photocatalytic protein complex, Photosystem I (PSI), onto a variety of substrates is reported. The resulting films, akin to the stacked thylakoid structures of leaves, consist of a protein matrix that is permeable to electrochemical mediators and contain a high concentration of photoelectrochemically active redox centers. These multilayer assemblies vastly outperform previously reported monolayer films of PSI in terms of photocurrent production when incorporated into an electrochemical system, and it is shown that these photocatalytic properties increase with the film thickness. These results demonstrate how the assembly of micron‐thick coatings of PSI on non‐biological substrates yields a biohybrid ensemble that manifests the photocatalytic activity of the film’s individual protein constituents, and represent significant progress toward affordable, biologically‐inspired renewable energy conversion platforms.  相似文献   
12.
Path Diversification is a new mechanism that can be used to select multiple paths between a given ingress and egress node pair using a quantified diversity measure to achieve maximum flow reliability. The path diversification mechanism is targeted at the end-to-end layer, but can be applied at any level for which a path discovery service is available. Path diversification also takes into account service requirements for low-latency or maximal reliability in selecting appropriate paths. Using this mechanism will allow future internetworking architectures to exploit naturally rich physical topologies to a far greater extent than is possible with shortest-path routing or equal-cost load balancing. We describe the path diversity metric and its application at various aggregation levels, and apply the path diversification process to 13 real-world network graphs as well as 4 synthetic topologies to asses the gain in flow reliability. Based on the analysis of flow reliability across a range of networks, we then extend our path diversity metric to create a composite compensated total graph diversity metric that is representative of a particular topology’s survivability with respect to distributed simultaneous link and node failures. We tune the accuracy of this metric having simulated the performance of each topology under a range of failure severities, and present the results. The topologies used are from national-scale backbone networks with a variety of characteristics, which we characterize using standard graph-theoretic metrics. The end result is a compensated total graph diversity metric that accurately predicts the survivability of a given network topology.  相似文献   
13.
Fast and highly efficient intramolecular singlet exciton fission in a pentacene dimer, consisting of two covalently attached, nearly orthogonal pentacene units is reported. Fission to triplet excitons from this ground state geometry occurs within 1 ps in isolated molecules in solution and dispersed solid matrices. The process exhibits a sensitivity to environmental polarity and competes with geometric relaxation in the singlet state, while subsequent triplet decay is strongly dependent on conformational freedom. The near orthogonal arrangement of the pentacene units is unlike any structure currently proposed for efficient singlet exciton fission and may lead to new molecular design rules.  相似文献   
14.
The future of green electronics possessing great strength and toughness proves to be a promising area of research in this technologically advanced society. This work develops the first fully bendable and malleable toughened polylactic acid (PLA) green composite by incorporating a multifunctional polyhydroxybutyrate rubber copolymer filler that acts as an effective nucleating agent to accelerate PLA crystallization and performs as a dynamic plasticizer to generate massive polymer chain movement. The resultant biocomposite exhibits a 24‐fold and 15‐fold increment in both elongation and toughness, respectively, while retaining its elastic modulus at >3 GPa. Mechanism studies show the toughening effect is due to an amalgamation of massive shear yielding, crazing, and nanocavitation in the highly dense PLA matrix. Uniquely distinguished from the typical flexible polymer that stretches and recovers, this biocomposite is the first report of PLA that can be “bend, twist, turn, and fold” at room temperature and exhibit excellent mechanical robustness even after a 180° bend, attributes to the highly interconnected polymer network of innumerable nanocavitation complemented with an extensively unified fibrillar bridge. This unique trait certainly opens up a new horizon to future sustainable green electronics development.  相似文献   
15.
An interpenetrating polymer network (IPN) material with controllable nanoporosity is developed for applications such as chemical protection. The IPN material is based on a conducting polymer backbone consisting of thiophene and 3,4 ethylenedioxythiophene (EDOT) repeat units–poly(thiophene‐EDOT)–formed within a soft polyurethane support. The IPN demonstrates reversible, electrochemically switchable nanoporosity in the absence of standard liquid electrolyte, with the oxidized state being the open (high porosity) state and the reduced state being the closed (low porosity) state. The switching of the IPN between its oxidized (open) and reduced (closed) states is actuated using application of ±1.0 V. The variability in the IPN porosity, induced by the electrochemical switching, is revealed by large changes in water vapor diffusivity, as well as changes in the diffusivities of the chemical agent simulants chloroethyl ethyl sulfide (CEES) and methyl salicylate (MeS). The closed state of the IPN is able to decrease CEES diffusivity by ≈99% compared to expanded Teflon (ePTFE), while the open state allows high MVT rates comparable to ePTFE. The IPN's ability to allow high MVT under non‐threat conditions (open state) and high protection from agents under threat conditions (closed state) is a unique and desirable characteristic of this novel IPN material.  相似文献   
16.
In the design of brain-machine interface (BMI) algorithms, the activity of hundreds of chronically recorded neurons is used to reconstruct a variety of kinematic variables. A significant problem introduced with the use of neural ensemble inputs for model building is the explosion in the number of free parameters. Large models not only affect model generalization but also put a computational burden on computing an optimal solution especially when the goal is to implement the BMI in low-power, portable hardware. In this paper, three methods are presented to quantitatively rate the importance of neurons in neural to motor mapping, using single neuron correlation analysis, sensitivity analysis through a vector linear model, and a model-independent cellular directional tuning analysis for comparisons purpose. Although, the rankings are not identical, up to sixty percent of the top 10 ranking cells were in common. This set can then be used to determine a reduced-order model whose performance is similar to that of the ensemble. It is further shown that by pruning the initial ensemble neural input with the ranked importance of cells, a reduced sets of cells (between 40 and 80, depending upon the methods) can be found that exceed the BMI performance levels of the full ensemble.  相似文献   
17.
A core–satellite nanotheranostic agent with pH‐dependent photothermal properties, pH‐triggered drug release, and H2O2‐induced catalytic generation of radical medicine is fabricated to give a selective and effective tumor medicine with three modes of action. The nanocomplex (core–satellite mesoporous silica–gold nanocomposite) consists of amino‐group‐functionalized mesoporous silica nanoparticles (MSN‐NH2) linked to L‐cysteine‐derivatized gold nanoparticles (AuNPs‐Cys) with bridging ferrous iron (Fe2+) ions. The AuNPs‐Cys serve as both removable caps that control drug release (doxorubicin) and stimuli‐responsive agents for selective photothermal therapy. Drug release and photothermal therapy are initiated by the cleavage of Fe2+ coordination bonds at low pH and the spontaneous aggregation of the dissociated AuNPs‐Cys. In addition, the Fe2+ is able to catalyze the decomposition of hydrogen peroxide abundant in cancer cells by a Fenton‐like reaction to generate high‐concentration hydroxyl radicals (·OH), which then causes cell damage. This system requires two tumor microenvironment conditions (low pH and considerable amounts of H2O2) to trigger the three therapeutic actions. In vivo data from mouse models show that a tumor can be completely inhibited after two weeks of treatment with the combined chemo‐photothermal method; the data directly demonstrate the efficiency of the MSN–Fe–AuNPs for tumor therapy.  相似文献   
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19.
文章介绍了两种移植和可控纳米沉积荧光粉颗粒和纳米铁电体颗粒的载体.第一种载体是一种可以悬浮和沉积合成的具有亚微米级尺寸大小的荧光粉颗粒的油墨.解决了该油墨的聚集和沉降问题,并发现该油墨具有良好的液流学性能,从而可用于印刷高分辨率的荧光粉.测量了相关的单个象素的阴极发光密度以评定这种丝网印刷油墨的可重复性.第二种载体是一种粘结剂,这种粘结剂不仅可以携带 30 μm 以及更大的尺寸的电致发光的荧光粉,还可以携带纳米铁电体颗粒.这种新型的粘结剂可应用于不需要额外的绝缘反射层的低造价的 EL 显示器.从衬底按要求将发射层剥下来就形成了柔性薄膜,将该薄膜置于两电极之间,仍可保持其电致发光的活性.该粘结剂薄膜可以很容易地印刷和定型制成显示屏.  相似文献   
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