In-Situ Derived Defective Ru Particles Anchored on Ru-Ni Layered Double Hydroxides for Enhanced Alkaline Hydrogen Evolution.

Developing active, stable, and cost-efficient electrocatalysts to replace platinum for the alkaline hydrogen evolution reaction (HER) is highly desirable yet represents a great challenge. Here, it is reported on a facile one-pot synthesis of RuxNi layered double hydroxides (RuxNi-LDHs) that exhibit remarkable HER activity and stability after an in-situ activation treatment, surpassing most state-of-the-art Ru-based catalysts as well as commercial Ru/C and Pt/C catalysts. The structural and chemical changes triggered by in-situ activation are systematically investigated, and the results clearly show that the pristine, less-active RuxNi-LDHs are transformed into a highly active catalyst characterized by raft-like, defect-rich Ru° particles decorated on the surface of RuxNi-LDHs. Density functional theory (DFT) calculations reveal that the defective Ru sites can effectively optimize the reaction pathway and lower the free energies of the elemental steps involved, leading to enhanced intrinsic activity. This work highlights the importance of the currently understudied strategy of defect engineering in boosting the HER activity of Ru-based catalysts and offers an effective approach involving in-situ electrochemical activation for the development of high-performance alkaline HER catalysts.

Design of high performance nitrogen reduction electrocatalysts by doping defective polyoxometalate with a single atom promoter.

Single-atom catalysts (SACs) are emerging as promising candidates for electrochemical nitrogen reduction reaction (NRR). Previous studies have shown that the single-atom centers of SACs can not only serve as active sites, but also act as promoters to affect the catalytic properties. However, the use of single metal atoms as promoters in electrocatalysis has rarely been studied. In this work, the defective Keggin-type phosphomolybdic acid (PMA) is used as a substrate to support the single metal atoms. We aim to tune the electronic structures of the exposed molybdenum active sites on defective PMA by using these supported single atoms as promoters for efficient NRR. Firstly, the stability and N2 adsorption capacity were studied to screen for an effective catalyst capable of activating N2. Most of the SACs were found to have good stability and N2 adsorption capacity. Then, we compared the selectivity and NRR activity of the catalysts and found that catalysts with metal atom promoters have improved NRR selectivity and activity. Finally, electronic structure analysis was carried out to understand the promoting effect of the promoter on N2 activation and the activity of the NRR process. This work provides a new strategy for designing efficient catalysts for electrocatalytic reactions by introducing promoters.

Role of Peripheral Coordination Boron in Electrocatalytic Nitrogen Reduction over N-Doped Graphene-Supported Single-Atom Catalysts.

In this work, we investigate the effect of peripheral B doping on the electrocatalytic nitrogen reduction reaction (NRR) performance of N-doped graphene-supported single-metal atoms using density functional theory (DFT) calculations. Our results showed that the peripheral coordination of B atoms could improve the stability of the single-atom catalysts (SACs) and weaken the binding of nitrogen to the central atom. Interestingly, it was found that there was a linear correlation between the change in the magnetic moment (µ) of single-metal atoms and the change in the limiting potential (UL) of the optimum NRR pathway before and after B doping. It was also found that the introduction of the B atom suppressed the hydrogen evolution reaction, thereby enhancing the NRR selectivity of the SACs. This work provides useful insights into the design of efficient SACs for electrocatalytic NRR.

Core-Shell-Type All-Inorganic Heterometallic Nanoclusters: Record High-Nuclearity Cobalt Polyoxoniobates for Visible-Light-Driven Photocatalytic CO2 Reduction.

Only rarely have polyoxometalates been found to form core-shell nanoclusters. Here, we succeeded in isolating a series of rare giant and all-inorganic core-shell cobalt polyoxoniobates (Co-PONbs) with diverse shapes, nuclearities and original topologies, including 50-nuclearity {Co12 Nb38 O132 }, 54-nuclearity {Co20 Nb34 O128 }, 62-nuclearity {Co26 Nb36 O140 } and 87-nuclearity {Co33 Nb54 O188 }. They are the largest Co-PONbs and also the polyoxometalates containing the greatest number of Co ions and the largest cobalt clusters known thus far. These molecular Co-PONbs have intriguing and atomically precise core-shell architectures comprising unique cobalt oxide cores and niobate oxide shells. In particular, the encapsulated cobalt oxide cores with different nuclearities have identical compositions, structures and mixed-valence Co3+ /Co2+ states as the different sized Co-O moieties of the bulk cubic-spinel Co3 O4 , suggesting that they can serve as various molecular models of the cubic-spinel Co3 O4 . The successful construction of the series of the Co-PONbs reveals a feasible and versatile synthetic method for making rare core-shell heterometallic PONbs. Further, these new-type core-shell bimetal species are promising cluster molecular catalysts for visible-light-driven CO2 reduction.

Ru-polyoxometalate as a single-atom electrocatalyst for N2 reduction to NH3 with high selectivity at applied voltage: a perspective from DFT studies.

Many highly active electrocatalysts for the reduction of N2 to NH3 (NRR) have been synthesized but suffer from poor selectivity. One crucial reason is that the adsorption of hydrogen often dominates at the active centers at applied voltage, which leads to the competitive hydrogen evolution reaction. This work used density functional theory (DFT) calculations to develop a class of stable polyoxometalate-based electrocatalysts including phosphomolybdic-, phosphotungstic-, silicotungstic-, and silicomolybdic-acid supported Ru single atoms to efficiently catalyze the NRR process with an overpotential lower than 0.25 V. More importantly, phosphomolybdic- and phosphotungstic acid-supported Ru electrocatalysts can achieve high selectivity at applied voltage. This work offers useful insights into designing high-performance polyoxometalate-based electrocatalysts for the NRR.

Hepatitis D virus isolates with low replication and epithelial-mesenchymal transition-inducing activity are associated with disease remission.

Clearance of hepatitis D virus (HDV) viremia leads to disease remission. Large hepatitis delta antigen (L-HDAg) has been reported to activate transforming growth factor ß, which may induce epithelial-mesenchymal transition (EMT) and fibrogenesis. This study analyzed serum HDV RNA "quasispecies" in HDV-infected patients at two stages of infection: before and after alanine aminotransferase (ALT) elevations. Included in the study were four patients who went into remission after ALT elevation and three patients who did not go into remission and progressed to cirrhosis or hepatocellular carcinoma. Full-length HDV cDNA clones were obtained from the most abundant HDV RNA species at the pre- and post-ALT elevation stages. Using an in vitro model consisting of Huh-7 cells transfected with cloned HDV cDNAs, the pre- or post-ALT elevation dominant HDV RNA species were characterized for (i) their replication capacity by measuring HDV RNA and HDAg levels in transfected cells and (ii) their capacity to induce EMT by measuring the levels of the mesenchymal-cell-specific protein vimentin, the EMT regulators twist and snail, and the epithelial-cell-specific protein E-cadherin. Results show that in patients in remission, the post-ALT elevation dominant HDV RNA species had a lower replication capacity in vitro and lower EMT activity than their pre-ALT elevation counterparts. This was not true of patients who did not go into remission. The expression of L-HDAg, but not small HDAg, increased the expression of the EMT-related proteins. It is concluded that in chronically infected patients, HDV quasispecies with a low replication capacity and low EMT activity are associated with disease remission.

Health literacy and its socio-demographic risk factors in Hebei: A cross-sectional survey.

ABSTRACT: This study aimed to evaluate the prevalence of low health literacy in Hebei Province of China, and to investigate its socio-demographic risk factors.This study was a community-based, cross-sectional questionnaire survey with a multiple-stage randomization design and a sample size of 10,560. Participants' health literacy status was evaluated by a questionnaire based on the 2012 Chinese Resident Health Literacy Scale. Meanwhile, participants' socio-demographic characteristics were also collected by the questionnaire.A total of 9952 participants provided valid questionnaires and were included in the final analyses. The mean health literacy score was 63.1 ±â€Š17.1 points; for its subscales, the mean basic knowledge and concepts score, lifestyle score, health-related skills score were 31.7 ±â€Š9.0, 17.2 ±â€Š4.8, 14.3 ±â€Š4.1, respectively. Meanwhile, low health literacy prevalence was 81.0%; for its subscales, low basic knowledge and concepts prevalence (70.6%) was numerically reduced compared to low lifestyle prevalence (87.4%) and low health-related skills prevalence (86.1%). Further analyses showed that age, male, and rural area were positively associated, but education level and annual household income were negatively associated with low health literacy prevalence. Further multivariate logistic regression analyses showed that higher age, male, lower education level, lower annual household income, and rural area were closely correlated with the risks of low total health literacy or low health literacy in subscales in Hebei Province.The prevalence of low health literacy is 81.0% in Hebei Province. Meanwhile, higher age, male, lower education level, lower annual household income, and rural area closely associate with low health literacy risk.

PGBL inhibits the RAW 264.7 cells to express inflammatory factor.

Polysaccharides derived from Ginkgo biloba leaf (PGBL) is a kind of active ingredient came out from ginkgo biloba leaf extractions. Previous studies have shown that PGBL has a good anti-inflammatory effect. However, the mechanism is not clear. This study is to investigate the modulated immunity effect of PGBL on RAW264.7 cells. Here we showed that lipopolysaccharide (LPS) induces the expression of tumor necrosis factor-α (TNF-α) and interleukin-6 (IL-6), and this induction can be repressed by PGBL treatment both in protein level and mRNA level, and PGBL strongly reduced the translocation of nuclear factor (NF)-κB to the cell nucleus. These findings demonstrate that PGBL can decrease the sensitivity of monocytes to LPS, and PGBL has applications in systemic inflammation and immune diseases.