Abstract
Copper electrocatalysts have been shown to selectively reduce carbon dioxide to hydrocarbons. Nevertheless, the absence of a systematic study based on time-resolved spectroscopy renders the ...functional agent—either metallic or oxidative Copper—for the selectivity still undecidable. Herein, we develop an operando seconds-resolved X-ray absorption spectroscopy to uncover the chemical state evolution of working catalysts. An oxide-derived Copper electrocatalyst is employed as a model catalyst to offer scientific insights into the roles metal states serve in carbon dioxide reduction reaction (CO
2
RR). Using a potential switching approach, the model catalyst can achieve a steady chemical state of half-Cu(0)-and-half-Cu(I) and selectively produce asymmetric C
2
products - C
2
H
5
OH. Furthermore, a theoretical analysis reveals that a surface composed of Cu-Cu(I) ensembles can have dual carbon monoxide molecules coupled asymmetrically, which potentially enhances the catalyst’s CO
2
RR product selectivity toward C
2
products. Our results offer understandings of the fundamental chemical states and insights to the establishment of selective CO
2
RR.
We report the discovery of tidal structures around the intermediate-aged (∼700-800 Myr), nearby (∼85 pc) star cluster Coma Berenices. The spatial and kinematic grouping of stars is determined with ...the Gaia DR2 parallax and proper motion data, by a clustering analysis tool, StarGO, to map 5D parameters (X, Y, Z, ) onto a 2D neural network. Leading and trailing tails, each with an extension of ∼50 pc are revealed for the first time around this disrupting star cluster. The cluster members, totaling , are clearly mass-segregated, and exhibit a flat mass function with ∼ 0.79 0.16, in the sense of dN/dm ∝ m− , where N is the number of member stars and m is stellar mass, in the mass range of m = 0.25-2.51 M☉. Within the tidal radius of ∼6.9 pc, there are 77 member candidates with an average position, i.e., the cluster center, of R.A. = 186 8110, and decl. = 25 8112, and an average distance of 85.8 pc. Additional 120 member candidates reside in the tidal structures, i.e., outnumbering those in the cluster core. The expansion of escaping members lead to an anisotropy in the velocity field of the tidal tails. Our analysis also serendipitously uncovers an adjacent stellar group, part of which has been cataloged in the literature. We identify 218 member candidates, 10 times more than previously known. This star group is some 65 pc away from, and ∼400 Myr younger than, Coma Ber, but is already at the final stage of disruption.
Improvements in the performance of electrocatalysts, along with continuing advances in selective pathway for target reaction, have great potential to offer opportunities in designing competitive ...reactions especially for using a photophysical process owing to its tunable properties. Herein, we demonstrated a first empirical evidence of suppressing the formation of undesired peroxide intermediate through plasmonic effects, in which plasmonic Ag–Pt bimetallic nanocages were synthesized with an edgeless feature, and a custom-made RDE/RRDE working station was designed to provide unique means by which to in situ realize the plasmon-induced effects toward the target reaction. The edgeless Ag–Pt bimetallic nanocages with hollow interior performed newly plasmon-induced effects, which was characteristic of photodependent nature to suppress the formation of undesired peroxide intermediate. We concluded that the plasmon-induced hot electron transfer governed the suppression of peroxide formation instead of plasmon-induced heating that would cause a negative effect (i.e., increase of peroxide yield), in which the hot electron transfer of Ag nanostructure offered a sufficient energy to populate the antibonding orbital of O2 as illustrated by in situ X-ray absorption approach. This rapid light-dependent nature corresponding to localized surface plasmon resonance in present nanocages can potentially offer synergetic strategies toward altering the chemical reactions or reaction pathways in various fields.
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IJS, KILJ, NUK, PNG, UL, UM
Distinct phylogeny and substrate specificities suggest that 12 Arabidopsis Ovarian Tumor domain-containing (OTU) deubiquitinases participate in conserved or plant-specific functions. The
null mutant ...displayed a pleiotropic phenotype, including early flowering, mimicking that of mutants harboring defects in subunits (e.g., ARP6) of the SWR1 complex (SWR1c) involved in histone H2A.Z deposition. Transcriptome and RT-qPCR analyses suggest that downregulated
and
are responsible for the early flowering of
. qChIP analyses revealed a reduction and increase in activating and repressive histone marks, respectively, on
and
in
. Subcellular fractionation, GFP-fusion expression, and MNase treatment of chromatin showed that OTU5 is nucleus-enriched and chromatin-associated. Moreover, OTU5 was found to be associated with
and
. The OTU5-associated protein complex(es) appears to be distinct from SWR1c, as the molecular weights of OTU5 complex(es) were unaltered in
plants. Furthermore, the
double mutant exhibited synergistic phenotypes, and H2A.Z levels on
were reduced in
but not
. Our results support the proposition that Arabidopsis OTU5, acting independently of SWR1c, suppresses flowering by activating
and
through histone modification. Double-mutant analyses also indicate that
acts independently of the HUB1-mediated pathway, but it is partially required for
-mediated flowering suppression in autonomous pathway mutants and
-Col.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
After obtaining written consent, we performed bloodletting acupuncture using a sterile 22-gauge (0.40 × 32 mm) disposable stainless steel injection needle to puncture the patient's engorged venules ...around the posterior inferior side of the right lateral ankle (Figure 1C). According to the meridian theory, this area belongs to the bladder meridian and all the engorged venules are located between BL60 and BL61. Following this, she received the 2nd bloodletting acupuncture on the same place and VAS-pain decreased to 0/10. ...she was able to perform housekeeping tasks and rotate her back smoothly.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Carbon@titania yolk–shell nanostructures are successfully synthesized at different calcination conditions. These unique structure nanomaterials can be used as a photocatalyst to degrade the emerging ...water pollutant, acetaminophen (paracetamol). The photodegradation analysis studies have shown that the samples with residual carbon nanospheres have improved the photocatalytic efficiency. The local electronic and atomic structure of the nanostructures are analyzed by X‐ray absorption spectroscopy (XAS) measurements. The spectra confirm that the hollow shell has an anatase phase structure, slight lattice distortion, and variation in Ti 3d orbital orientation. In situ XAS measurements reveal that the existence of amorphous carbon nanospheres inside the nano spherical shell inhibit the recombination of electron–hole pairs; more mobile holes are formed in the p–d hybridized bands near the Fermi surface and enables the acceleration of the carries that significantly enhance the photodegradation of paracetamol under UV–visible irradiation. The observed charge transfer process from TiO2 hybridized orbital to the carbon nanospheres reduces the recombination rate of electrons and holes, thus increasing the photocatalytic efficiency.
A change in the unoccupied states and a charge transfer under UV–visible illumination for the carbon@titania yolk–shell nanostructures enhance the photocatalytic activity.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Standard inactivated influenza vaccines are poorly immunogenic in immunologically naive healthy young children, who are particularly vulnerable to complications from influenza. For them, there is an ...unmet need for better influenza vaccines. Oil-in-water emulsion-adjuvanted influenza vaccines are promising candidates, but clinical trials yielded inconsistent results. Here, we meta-analyze randomized controlled trials with efficacy data (3 trials, n = 15,310) and immunogenicity data (17 trials, n = 9062). Compared with non-adjuvanted counterparts, adjuvanted influenza vaccines provide a significantly better protection (weighted estimate for risk ratio of RT-PCR-confirmed influenza: 0.26) and are significantly more immunogenic (weighted estimates for seroprotection rate ratio: 4.6 to 7.9) in healthy immunologically naive young children. Nevertheless, in immunologically non-naive children, adjuvanted and non-adjuvanted vaccines provide similar protection and are similarly immunogenic. These results indicate that oil-in-water emulsion adjuvant improves the efficacy of inactivated influenza vaccines in healthy young children at the first-time seasonal influenza vaccination.
Introduction
Many risk prediction models of diabetes remission after bariatric and metabolic surgery have been proposed. Most models have been created using Roux-en-Y gastric bypass cohorts. However, ...validation of these models in sleeve gastrectomy (SG) is limited. The objective of our study is to validate the performance of risk prediction models of diabetes remission in obese patients with diabetes who underwent SG.
Method
This retrospective cohort study included 128 patients who underwent SG with at least 1 year follow-up from Dec 2011 to Sep 2016 as the validation cohort. A literature review revealed total 11 models with 2 categories (scoring system and logistic regression), which were validated by our study dataset. Discrimination was evaluated by area under the receiver operating characteristic (AUC) while calibration by Hosmer–Lemeshow test and predicted versus observed remission ratio.
Results
At 1 year after surgery, 71.9% diabetes remission (HbA1c < 6.0 off medication) and 61.4% excess weight loss were observed. Individual metabolic surgery, ABCD, DiaRem, Advanced-DiaRem, DiaBetter, Ana et al., and Dixon et al. models showed excellent discrimination power (AUC > 0.8). In calibration, all models overestimated diabetes remission from 5 to 30% but did not lose their goodness of fit.
Conclusion
This is the first comprehensive external validation of current risk prediction models of diabetes remission at 1 year after SG. Seven models showed excellent predicting power, and scoring models were recommended more because of their easy utility.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OBVAL, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
Cortico-basal ganglia circuits are critical for speech and language and are implicated in autism spectrum disorder, in which language function can be severely affected. We demonstrate that in the ...mouse striatum, the gene Foxp2 negatively interacts with the synapse suppressor gene Mef2c. We present causal evidence that Mef2c inhibition by Foxp2 in neonatal mouse striatum controls synaptogenesis of corticostriatal inputs and vocalization in neonates. Mef2c suppresses corticostriatal synapse formation and striatal spinogenesis, but can itself be repressed by Foxp2 through direct DNA binding. Foxp2 deletion de-represses Mef2c, and both intrastriatal and global decrease of Mef2c rescue vocalization and striatal spinogenesis defects of Foxp2-deletion mutants. These findings suggest that Foxp2-Mef2C signaling is critical to corticostriatal circuit formation. If found in humans, such signaling defects could contribute to a range of neurologic and neuropsychiatric disorders.
Altered sensation (including paresthesia, dysesthesia and hypoesthesia) after mandibular implant surgery may indicate transient or permanent injury of the inferior alveolar nerve and the mental ...branch, and considerably lower patients' satisfaction about the therapy. Previous studies have shown a great degree of variability on the incidence of altered sensation. We here reported the incidence of altered sensation after mandibular implant surgery based on a meta-analysis of 26 articles published between 1990.1.1 and 2016.1.1. Study quality and risk of bias was assessed and the studies with a lower score were excluded in the meta-analysis. Data synthesis was performed using the logistic-normal random-effect model. The meta-analyses revealed that the short-term (10 days after implant placement) and long-term (1 year after implant placement) incidence was 13% (95% CI, 6%-25%) and 3% (95% CI, 1%-7%), respectively. (2) For the patients who initially reported altered sensation, 80% (95% CI, 52%-94%) of them would return to normal sensation within 6 months after surgery, and 91% (95% CI, 78%-96%) of them would return to normal sensation one year after surgery. We concluded that dentist-patient communication about the risk of altered sensation is critical to treatment planning, since the short-term incidence of altered sensation is substantial (13%). When a patient reports altered sensation, regular assessment for 6 months would help tracing the changes of symptoms. In terms of long-term follow-up (1 year after surgery), the incidence is much lower (3%) and most patients (91%) would return to normal sensation.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
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