The quantitative correlation of the catalytic activity with the microscopic structure of heterogeneous catalysts is a major challenge for the field of catalysis science. It requests synergistic capabilities to tailor the structure with atomic scale precision and to control the catalytic reaction to proceed through well-defined pathways. Here we leverage on the controlled growth of MoS2 atomically thin films to demonstrate that the catalytic activity of MoS2 for the hydrogen evolution reaction decreases by a factor of ∼ 4.47 for the addition of every one more layer. Similar layer dependence is also found in edge-riched MoS2 pyramid platelets. This layer-dependent electrocatalysis can be correlated to the hopping of electrons in the vertical direction of MoS2 layers over an interlayer potential barrier. Our experimental results suggest the potential barrier to be 0.119 V, consistent with theoretical calculations. Different from the conventional wisdom, which states that the number of edge sites is important, our results suggest that increasing the hopping efficiency of electrons in the vertical direction is a key for the development of high-efficiency two-dimensional material catalysts.

BackgroundRegional and subtype-specific mutational patterns of HIV-1 transmitted drug resistance (TDR) are essential for informing first-line antiretroviral (ARV) therapy guidelines and designing diagnostic assays for use in regions where standard genotypic resistance testing is not affordable. We sought to understand the molecular epidemiology of TDR and to identify the HIV-1 drug-resistance mutations responsible for TDR in different regions and virus subtypes.Methods and FindingsWe reviewed all GenBank submissions of HIV-1 reverse transcriptase sequences with or without protease and identified 287 studies published between March 1, 2000, and December 31, 2013, with more than 25 recently or chronically infected ARV-naïve individuals. These studies comprised 50,870 individuals from 111 countries. Each set of study sequences was analyzed for phylogenetic clustering and the presence of 93 surveillance drug-resistance mutations (SDRMs). The median overall TDR prevalence in sub-Saharan Africa (SSA), south/southeast Asia (SSEA), upper-income Asian countries, Latin America/Caribbean, Europe, and North America was 2.8%, 2.9%, 5.6%, 7.6%, 9.4%, and 11.5%, respectively. In SSA, there was a yearly 1.09-fold (95% CI: 1.05–1.14) increase in odds of TDR since national ARV scale-up attributable to an increase in non-nucleoside reverse transcriptase inhibitor (NNRTI) resistance. The odds of NNRTI-associated TDR also increased in Latin America/Caribbean (odds ratio [OR] = 1.16; 95% CI: 1.06–1.25), North America (OR = 1.19; 95% CI: 1.12–1.26), Europe (OR = 1.07; 95% CI: 1.01–1.13), and upper-income Asian countries (OR = 1.33; 95% CI: 1.12–1.55). In SSEA, there was no significant change in the odds of TDR since national ARV scale-up (OR = 0.97; 95% CI: 0.92–1.02). An analysis limited to sequences with mixtures at less than 0.5% of their nucleotide positions—a proxy for recent infection—yielded trends comparable to those obtained using the complete dataset. Four NNRTI SDRMs—K101E, K103N, Y181C, and G190A—accounted for >80% of NNRTI-associated TDR in all regions and subtypes. Sixteen nucleoside reverse transcriptase inhibitor (NRTI) SDRMs accounted for >69% of NRTI-associated TDR in all regions and subtypes. In SSA and SSEA, 89% of NNRTI SDRMs were associated with high-level resistance to nevirapine or efavirenz, whereas only 27% of NRTI SDRMs were associated with high-level resistance to zidovudine, lamivudine, tenofovir, or abacavir. Of 763 viruses with TDR in SSA and SSEA, 725 (95%) were genetically dissimilar; 38 (5%) formed 19 sequence pairs. Inherent limitations of this study are that some cohorts may not represent the broader regional population and that studies were heterogeneous with respect to duration of infection prior to sampling.ConclusionsMost TDR strains in SSA and SSEA arose independently, suggesting that ARV regimens with a high genetic barrier to resistance combined with improved patient adherence may mitigate TDR increases by reducing the generation of new ARV-resistant strains. A small number of NNRTI-resistance...

A rechargeable aluminum-ion battery exhibits outstanding perofrmance due to the rationally designed CoSe2-based cathode material.

The key challenge for the development of highperformance molybdenum sulfide HER catalysts lies in the limited fundamental understanding for the correlation between the catalytic activities and physical features of the materials.Here we have demonstrated an unambiguous correlation between the catalytic performance and the composition/ crystallinity of molybdenum sulfide. The results indicate that the crystallinity plays an overwhelming role in determining the catalytic performance, while the composition does not matter much. The crystallinity can affect the three figures of merit of the catalytic performance (Tafel slope, turnover frequency (TOF), and stability) in opposite directions. Generally, the materials with low crystalline quality may provide low Tafel slopes (∼40 mV/dec), while highly crystalline molybdenum sulfide shows higher TOFs (by 2 orders of magnitude) and better stability. DFT calculations suggest that the terminal disulfur complex S 2 2− , which may exist in MoS 3 and also likely MoS 2 of low crystalline quality due to its structural disorder, could be the true catalytically active site responsible for the low Tafel slope. Our results indicate that one key issue for the rational design of high-performance molybdenum sulfide HER catalysts is to engineer the crystallinity such that balancing its contradictory effects on the different aspects of the catalytic performance. We show that nanocrystalline MoS 2 with few-layer nanoclusters in a lateral size of 5−30 nm provides a more promising platform than either amorphous or highly crystalline molybdenum sulfide due to its combination of low Tafel slopes and good stability. As a way to illustrate this notion, we have developed a MoS 2 catalyst by engineering the crystallinity that shows Tafel slopes of 40 mV/dec, exchange current densities of 3.5 μA/cm 2 , and extraordinary stability with constant performance over >10000 cycles, which are among the best values ever reported. The performance of this catalyst could be further improved by using rougher substrates or doping to improve the relatively low exchange current density.

A colloidal chemical strategy has been developed for the synthesis of ultrathin 1T′-MoTe2 nanosheets, showing an enhanced supercapacitor performance.

No abstract

An unexplained outbreak of feline diarrhea and vomiting, negative for common enteric viral and bacterial pathogens, was subjected to viral metagenomics and PCR. We characterized from fecal samples the genome of a novel chapparvovirus we named fechavirus that was shed by 8/17 affected cats and identified three different feline bocaviruses shed by 9/17 cats. Also detected were nucleic acids from attenuated vaccine viruses, members of the normal feline virome, viruses found in only one or two cases, and viruses likely derived from ingested food products. Epidemiological investigation of disease signs, time of onset, and transfers of affected cats between three facilities support a possible role for this new chapparvovirus in a highly contagious feline diarrhea and vomiting disease.

This work reports a mechanistic study of template-directed synthesis of silica nanomaterials utilizing self-assembled peptide nanotubes as scaffolds. An ultrashort amphiphilic peptide (I3K) underwent self-assembly in aqueous solution under ambient conditions to form long and uniform nanotubes. The assembled peptide nanotubes then were used as templates for the subsequent fabrication of silica nanotubes from tetraethoxysilane (TEOS), also under ambient conditions. In order to gain better insight into the mediation of peptide self-assembly on the formation of silica nanostructures, we have carefully investigated environmental influences including the concentrations of peptide and silica precursor, solution pH, and reaction time, with the full screening of the processes by TEM, SEM, 29Si MAS NMR, FTIR, and TG-MS. The results revealed that, while peptide nanotubes worked as scaffolds for the formation of tubular silica structures, the surfaces of these peptide nanotubes served as catalytic sites for both hydrolysis and condensation of TEOS, thereby working as templates for directing silica deposition. Because the electrostatic attraction of the negatively charged silica intermediates onto the positively charged surface of peptide nanotubes drove the templating process, tuning of such an interaction by adjusting the solution conditions (such as pH) affected silica morphological structures. Silica tended to deposit along the exterior surface of the template at undersaturation over weak acidic and neutral pH ranges, while silica intermediates overcame diffusion resistance and moved inside the tubular template over mild basic pH ranges, enabling silica precipitation along the interior surface. This work has thus demonstrated that the morphological nanostructures of silica can be controlled by adjusting the silicification conditions (such as peptide concentration and solution pH) under an ambient environment, thus avoiding harsh chemicals or extreme reaction conditions.