Tuning Crystal Phase of Palladium-Selenium Nanowires for Enhanced Ethylene Glycol Electrocatalytic Oxidation.

Alcohol electrooxidation is pivotal for a sustainable energy economy. However, designing efficient electrocatalysts for this process is still a formidable challenge. Herein, palladium-selenium nanowires featuring distinct crystal phases: monoclinic Pd7Se2 and tetragonal Pd4.5Se for ethylene glycol electrooxidation reaction (EGOR) are synthesized. Notably, the supported monoclinic Pd7Se2 nanowires (m-Pd7Se2 NWs/C) exhibit superior EGOR activity, achieving a mass activity (MA) and specific activity (SA) of 10.4 A mgPd -1 (18.7 mA cm-2), which are 8.0 (6.7) and 10.4 (8.2) times versus the tetragonal Pd4.5Se and commercial Pd/C and surpass those reported in the literature. Furthermore, m-Pd7Se2 NWs/C displays robust catalytic activity for other alcohol electrooxidation. Comprehensive characterization and density functional theory (DFT) calculations reveal that the enhanced electrocatalytic performance is attributed to the increased formation of Pd0 on the high-index facets of the m-Pd7Se2 NWs, which lowers the energy barriers for the C─C bond dissociation in CHOHCHOH* and the CO* oxidation to CO2*. This study provides palladium-based alloy electrocatalysts exhibiting the highest mass activity reported to date for the electrooxidation of ethylene glycol, achieved through the crystalline phase engineering strategy.

Bacterial-derived sialidases inhibit porcine rotavirus OSU replication by interfering with the early steps of infection.

Rotavirus infections in suckling and weaning piglets cause severe dehydration and death, resulting in significant economic losses in the pig breeding industry. With the continuous emergence of porcine rotavirus (PoRV) variants and poor vaccine cross-protection among various genotypes, there is an urgent need to develop alternative strategies such as seeking effective antiviral products from nature, microbial metabolites and virus-host protein interaction. Sialidases play a crucial role in various physiopathological processes and offer a promising target for developing antivirus drugs. However, the effect of bacterial-derived sialidases on the infection of PoRVs remains largely unknown. Herein, we investigated the impact of bacterial-derived sialidases (sialidase Cp and Vc) on PoRV strain OSU(Group A) infection, using differentiated epithelial monkey kidney cells (MA104) as a model. Our results indicated that the pretreatment of MA104 with exogenous sialidases effectively suppressed PoRV OSU in a concentration-dependent manner. Notably, even at a concentration of 0.01 µU/mL, sialidases significantly inhibited the virus (MOI = 0.01). Meanwhile, we found that sialidase Vc pretreatment sharply reduced the binding rate of PoRV OSU. Last, we demonstrated that PoRV OSU might recognize α-2,3-linked sialic acid as the primary attachment factor in MA104. Our findings provide new insights into the underlying mechanism of PoRV OSU infections, shedding lights on the development of alternative antivirus approaches based on bacteria-virus interaction.

Association between home and community-based services utilization and self-rated health among Chinese older adults with chronic diseases: evidence from the 2018 China Health and Retirement Longitudinal Study.

BACKGROUND: As global aging intensifies, older adults with chronic diseases are of increasing concern. Home and community-based services (HCBSs) have been proven to promote self-rated health (SRH) in older adults, but no research explored the associations between the use of overall HCBSs, three different types of HCBSs (health care, daily care, and social support services) and SRH among older adults with chronic diseases. Consequently, this study applies a national publicly available database to examine these associations among older adults with chronic diseases. METHODS: 8,623 older adults with chronic diseases (≥ 60 years old) were included in this study. SRH was evaluated applying a concise question with a 1 - 5 scale. HCBSs utilization was assessed through the question, "What kind of HCBSs were used in the community?". Univariate general linear regression models aimed to compare the mean values of SRH in terms of HCBSs utilization in each group. This study is a cross-sectional study design and the relationship between HCBSs utilization and SRH was assessed by multilevel linear regression. RESULTS: The mean score for SRH among the respondents was 3.19, of whom 20.55% used one or more HCBSs, 19.47% utilized health care services, 2.44% utilized social support services, and only 0.55% utilized daily care services. The use of HCBSs was found to be linked to SRH among older adults with chronic diseases (ß = 0.085, SE = 0.025, p < 0.001). SRH among older adults with chronic diseases was strongly linked to the use of health care and social support services (ß = 0.068, SE = 0.025, p < 0.001; ß = 0.239, SE = 0.063, p < 0.001, respectively). However, there was no significant association between the use of daily care services and SRH among older adults with chronic diseases. CONCLUSION: This study revealed that HCBSs utilization was positively and significantly linked to SRH in Chinese older adults with chronic diseases. Furthermore, this study supposes the low utilization of social support and daily care services may be due to a mismatch between supply and demand. The government should offer the targeted HCBSs for older adults with chronic diseases according to their unique features to enhance their health status.

Diagnostic performance of computed tomography-digital subtraction angiography and conventional magnetic resonance imaging for evaluating the vascularity of osseous spinal tumors.

BACKGROUND AND PURPOSE: Patients with hypervascular spinal tumors may have severe blood loss during tumor resection, which increases the risks of perioperative morbidity and mortality. However, the preoperative evaluation of tumor vascularity may be challenging; moreover, the reliability of the data obtained in conventional preoperative noninvasive imaging is debatable. In this study, we compared conventional magnetic resonance imaging (MRI) and subtraction computed tomography angiography (CTA) in terms of their performance in vascularity evaluation. The catheter digital subtraction angiography (DSA) technique was used as a reference standard. METHODS: This study included 123 consecutive patients with spinal tumor who underwent subtraction CTA, catheter DSA, and subsequent surgery between October 2015 and October 2021. Data regarding qualitative and semiquantitative subtraction CTA parameters and conventional MRI signs were collected for comparison with tumor vascularity graded through catheter DSA. The diagnostic performance of qualitative CTA, quantitative CTA, and conventional MRI in assessing spinal tumor vascularity was analyzed. RESULTS: Qualitative subtraction CTA was the best noninvasive imaging modality in terms of diagnostic performance (area under the receiver operating characteristic curve [AUROC], 0.95). Quantitative CTA was relatively inferior (AUROC, 0.87). MRI results had low reliability (AUROC, 0.51 to 0.59). Intratumoral hemorrhage and prominent foraminal venous plexus were found to be the specific signs for hypervascularity (specificity 93.2%). CONCLUSIONS: Qualitative subtraction CTA offers the highest diagnostic value in evaluating spinal tumor vascularity, compared to quantitative CTA and MRI. Although conventional MRI may not be a reliable approach, certain MRI signs may have high specificity, which may be crucial for assessing spinal tumor vascularity.

Vacancy-induced catalytic mechanism for alcohol electrooxidation on nickel-based electrocatalyst.

Owing to outstanding performances, nickel-based electrocatalysts are commonly used in electrochemical alcohol oxidation reactions (AORs), and the active phase is usually vacancy-rich nickel oxide/hydroxide (NiOx Hy ) species. However, researchers are not aware of the catalytic role of atom vacancy in AORs. Here, we study vacancy-induced catalytic mechanisms for AORs on NiOx Hy species. As to AORs on oxygen-vacancy-poor ß-Ni(OH)2 , the only redox mediator is electrooxidation-induced electrophilic lattice oxygen species, which can only catalyze the dehydrogenation process (e.g., the electrooxidation of primary alcohol to carboxylic acid) instead of the C-C bond cleavage. Hence, vicinal diol electrooxidation reaction involving the C-C bond cleavage is not feasible with oxygen-vacancy-poor ß-Ni(OH)2 . Only through oxygen vacancy-induced adsorbed oxygen-mediated mechanism, can oxygen-vacancy-rich NiOx Hy species catalyze the electrooxidation of vicinal diol to carboxylic acid and formic acid accompanied with the C-C bond cleavage. Crucially, we examine how vacancies and vacancy-induced catalytic mechanisms work during AORs on NiOx Hy species.

Unconventional hcp/fcc Nickel Heteronanocrystal with Asymmetric Convex Sites Boosts Hydrogen Oxidation.

Developing non-platinum group metal catalysts for the sluggish hydrogen oxidation reaction (HOR) is critical for alkaline fuel cells. To date, Ni-based materials are the most promising candidates but still suffer from insufficient performance. Herein, we report an unconventional hcp/fcc Ni (u-hcp/fcc Ni) heteronanocrystal with multiple epitaxial hcp/fcc heterointerfaces and coherent twin boundaries, generating rugged surfaces with plenty of asymmetric convex sites. Systematic analyses discover that such convex sites enable the adsorption of *H in unusual bridge positions with weakened binding energy, circumventing the over-strong *H adsorption on traditional hollow positions, and simultaneously stabilizing interfacial *H2O. It thus synergistically optimizes the HOR thermodynamic process as well as reduces the kinetic barrier of the rate-determining Volmer step. Consequently, the developed u-hcp/fcc Ni exhibits the top-rank alkaline HOR activity with a mass activity of 40.6 mA mgNi-1 (6.3 times higher than fcc Ni control) together with superior stability and high CO-tolerance. These results provide a paradigm for designing high-performance catalysts by shifting the adsorption state of intermediates through configuring surface sites.

Flexible All-in-one Quasi-Solid-State Batteries Enabled by Low-water-content Hydrogel Films.

The high conductivities and good mechanical properties of hydrogel electrolyte films are critical for energy storage devices with high flexibility, fast redox kinetics, and long life. Herein, a low water content (6.63 wt%) hydrogel film is prepared, and a favorable environment is created, with an electrochemical stability window of 2.26 V and a high ionic conductivity of 2.6 mS cm-1 . The hydrogel film exhibits good folding ability, low in-plane swelling, and anti-freezing abilities. These properties are benefitted by immobilizing free water molecules on the abundant oxygenic groups of polymer fibers in the hydrogel film, offering a unique 3D channel to allow Li+ to quickly transport along the polymer network. Therefore, the hydrogel film-based all-in-one flexible cell exhibits stable cycling performance with a retention of 81.8% of the initial capacity after 500 cycles at room temperature and 66.2% of capacity retention at -30 °C. Furthermore, the full cell with high cathode loading (≈21 mg cm-2 ) exhibits a high areal capacity of 2.5 mAh cm-2 (≈119 mAh g-1 ). The overall merits of flexible all-in-one quasi-solid-state batteries demonstrate high potential to be used for power wearable electronics.

Electronic Modulation of Metal-Organic Frameworks Caused by Atomically Dispersed Ru for Efficient Hydrogen Evolution.

Designing excellent electrocatalysts for the hydrogen evolution reaction (HER) is extremely significant in producing clean and sustainable hydrogen fuel. Herein, a rational strategy is developed to fabricate a promising electrocatalyst by introducing atomically dispersed Ru into a cobalt-based metal-organic framework (MOF), Co-BPDC (Co(bpdc)(H2 O)2 , BPDC: 4,4'-Biphenyldicarboxylic acid). The obtained CoRu-BPDC nanosheet arrays exhibit remarkable HER performance with an overpotential of 37 mV at a current density of 10 mA cm-2 in alkaline media, which is superior to most of the MOF-based electrocatalysts and comparable to the commercial Pt/C. Synchrotron radiation-based X-ray absorption fine structure (XAFS) spectroscopy studies verify that the isolated Ru atoms are dispersed in Co-BPDC nanosheets with the formation of five-coordinated Ru-O5 species. XAFS spectroscopy combined with density functional theory (DFT) calculations unravels that atomically dispersed Ru can modulate the electronic structure of the as-obtained Co-BPDC, contributing to the optimization of binding strength for H* and the enhancement of HER performance. This work opens a new avenue to rationally design highly-active single-atom modified MOF-based HER electrocatalysts via modulating electronic structures of MOF.

Synergy of Ultrathin CoOx Overlayer and Nickel Single Atoms on Hematite Nanorods for Efficient Photo-Electrochemical Water Splitting.

To solve surface carrier recombination and sluggish water oxidation kinetics of hematite (α-Fe2 O3 ) photoanodes, herein, an attractive surface modification strategy is developed to successively deposit ultrathin CoOx overlayer and Ni single atoms on titanium (Ti)-doped α-Fe2 O3 (Ti:Fe2 O3 ) nanorods through a two-step atomic layer deposition (ALD) and photodeposition process. The collaborative decoration of ultrathin CoOx overlayer and Ni single atoms can trigger a big boost in photo-electrochemical (PEC) performance for water splitting over the obtained Ti:Fe2 O3 /CoOx /Ni photoanode, with the photocurrent density reaching 1.05 mA cm-2 at 1.23 V vs. reversible hydrogen electrode (RHE), more than three times that of Ti:Fe2 O3 (0.326 mA cm-2 ). Electrochemical and electronic investigations reveal that the surface passivation effect of ultrathin CoOx overlayer can reduce surface carrier recombination, while the catalysis effect of Ni single atoms can accelerate water oxidation kinetics. Moreover, theoretical calculations evidence that the synergy of ultrathin CoOx overlayer and Ni single atoms can lower the adsorption free energy of OH* intermediates and relieve the potential-determining step (PDS) for oxygen evolution reaction (OER). This work provides an exemplary modification through rational engineering of surface electrochemical and electronic properties for the improved PEC performances, which can be applied in other metal oxide semiconductors as well.

Efficacy of preoperative embolization for metastatic spinal tumor surgery using angiographic vascularity assessment.

OBJECTIVES: Preoperative embolization (PE) for metastatic spinal tumors is a method of minimizing intraoperative blood loss during aggressive surgery. This study specified angiographic standards and investigated the influence of these and other factors on blood loss in patients with spinal metastases and various pathologies. METHODS: The cohort comprised 126 consecutive patients receiving PE from 2015 to 2021. Their clinical, surgical, and angiographic characteristics were reviewed. Standard angiographic grading was used for vascularity assessment. Degree of embolization was divided into complete (≥ 90%), near complete (67 to < 90%), and partial (< 67%). Logistic regression analysis was used to investigate factors predictive of massive blood loss (> 2500 mL). A proportional odds model was used to assess factors predictive of the degree of embolization. RESULTS: Mean intraoperative blood loss was 1676 mL. Among the patients, 62 had hypervascular tumors and 64 had nonhypervascular tumors, according to the angiographic classification. Intraoperative blood loss differed significantly with embolization degree, both overall (p < 0.001) and in the hypervascular and nonhypervascular groups (p = 0.01 and 0.03). Angiographic hypervascularity, spinal metastasis invasiveness index, and embolization degree were significant predictors of massive blood loss in univariate analysis, but only embolization degree was significant in multivariate analysis. Only the presence of the radiculomedullary artery at the target level was significant in both the univariate and multivariate analyses for embolization degree. CONCLUSIONS: In addition to pathological classification, angiographic vascularity assessment is valuable. Although complete embolization is a reasonable goal, it is challenging to achieve in cases of visible radiculomedullary artery. KEY POINTS: • Angiography has a supplementary role in vascularity assessment for spinal metastatic surgery. • Better embolization degree is associated with less intraoperative blood loss in both angiographic hypervascular and nonhypervascular groups. • Presence of radiculomedullary artery in the target level causes worse embolization outcome.

Efficacy of anti-osteoporosis treatment for men with osteoporosis: a meta-analysis.

INTRODUCTION: Osteoporosis and fracture are important healthcare problems for men worldwide, which are relevant to severe disability and mortality. This meta-analysis aimed to assess the effectiveness of pharmacological therapy in men with osteoporosis, and to provide evidence-based hints for clinical practice. MATERIALS AND METHODS: PubMed, Embase, Web of Science were searched from inception to July 31, 2022. Pooled standardized mean difference (SMD) and relative risk (RR) were calculated. Heterogeneity between included studies and publication bias were detected. RESULTS: Twenty clinical studies were enrolled in this meta-analysis. The pooled SMD for mean percentage differences of change from baseline in lumbar spine BMD between the treatment group and the control group was 4.95 (95% CI 2.48, 7.42, I2 = 99%, p < 0.0001). For mean percentage differences of change in femoral neck BMD, the overall SMD was 3.08 (95% CI 0.95, 5.20, I2 = 99%, p = 0.0045). For a change in total hip BMD, the overall SMD was 1.06 (95% CI 0.50, 1.63, I2 = 82%, p = 0.0002). The overall RR for incident vertebral fractures was 0.50 (95% CI 0.37, 0.68, I2 = 5%, p = 0.3971). The pooled RR for nonvertebral fractures and clinical fracture were 0.74 (95% CI 0.41, 1.33, I2 = 28%, p = 0.3139) and 0.81 (95% CI 0.54, 1.21, I2 = 0%, p = 0.2992). CONCLUSION: Findings in this meta-analysis indicate that pharmacological treatment increases lumbar spine, femoral neck, total hip BMD, and decreases incident vertebral fractures in men with osteoporosis.

Ultrathin Carbon Nitride Nanosheets Exfoliated and In Situ Modified with a Nickel Bis(Chelate) Complex for Boosting Photocatalytic Performances.

Exfoliation and interfacial modification of two-dimensional (2D) polymeric carbon nitride (CN) are considerably vital for applications in photo/electrocatalysis fields. Here, a grinding-ultrasonic route was designed to construct nickel bis(chelate) complex (Ni(abt)2, abt = 2-aminobenzenethiolate)-modified CN ultrathin nanosheets. Under the assistance of the shear force derived from the grinding process, Ni(abt)2 was implanted into the interlamination of bulk CN, resulting in the formation of ultrathin CN (UCN) nanosheets. Simultaneously, Ni(abt)2 molecules were anchored on the surfaces of as-formed UCN nanosheets due to the π-π stacking interaction. Interestingly, compared with single Ni(abt)2 and UCN, the as-obtained Ni(abt)2/UCN nanosheets exhibited excellent photocatalytic hydrogen evolution capability. A molecule-semiconductor internal electron transmission mechanism was suggested for explaining the separation and transfer of electron-hole pairs. Density functional theory (DFT) calculations demonstrated that the interface-induced electron redistribution tuned the electron density and hydrogen adsorption of the active centers, thus enhancing the photocatalytic performance of the hybrid catalyst. In addition, the as-obtained Ni(abt)2/UCN nanosheets could also catalyze the reduction of nitroaromatics in the presence of NaBH4. It was found that under the simulated sunlight irradiation, the conversion efficiency of nitroaromatic compounds to amino aromatic ones was up to 97.3%, far higher than that under the condition without light irradiation (51.7%), suggesting that the photocatalytic-produced hydrogen took part in the reduction of nitroaromatic compounds.

Fine mapping and characterisation of a PV-PUR mediating anthocyanin synthesis in snap bean (Phaseolus vulgaris L.).

Anthocyanin makes snap bean (Phaseolus vulgaris L.) pods purple, which helps seed dispersal and protects against environmental stress. In this study, we characterised the snap bean purple mutant pv-pur, which has purple cotyledon, hypocotyl, stem, leaf vein, flower and pod tissues. Total anthocyanin, delphinidin and malvidin levels in mutant pods were significantly higher than in wild-type plants. We constructed two populations for fine mapping of the PV-PUR purple mutation gene, located in the 243.9-kb region of chromosome 06. We identified Phvul.006g018800.3, encoding F3'5'H, as a candidate gene for PV-PUR. Six single-base mutations occurred in the coding region of this gene, altering protein structure. PV-PUR and pv-pur genes were transferred into Arabidopsis, respectively. Compared with the wild-type, the leaf base and internode of T-PV-PUR plant were purple, and the phenotype of T-pv-pur plant remained unchanged, which verified the function of the mutant gene. The results demonstrated that PV-PUR is a crucial gene for anthocyanin biosynthesis in snap bean, resulting in purple colouration. The findings lay a foundation for future breeding and improvement of snap bean. Supplementary Information: The online version contains supplementary material available at 10.1007/s11032-023-01362-8.

Association between home and community-based services and depressive symptoms in Chinese older adults: a multilevel analysis.

BACKGROUND: As the phenomenon of ageing continues to intensify, home and community-based services (HCBSs) have been increasingly important in China. However, the association between HCBSs utilization and depressive symptoms in older adults in China is unclear. Consequently, this study aimed to examine the association between HCBSs utilization and depressive symptoms in Chinese older adults. METHODS: This study included 7,787 older adults (≥ 60 years old) who were recruited within the framework of the 2018 China Health and Retirement Longitudinal Study (CHARLS). Depressive symptoms were assessed using the 10-item Center for Epidemiological Studies Depression Scale (CES-D-10). HCBSs utilization was assessed via the question, "What kind of HCBSs were being utilized in their community?". Data were analyzed using binary logistic regression models and generalized hierarchical linear models (GHLM). RESULTS: Of the 7,787 participants, 20.0% (n = 1,556) reported that they utilized HCBSs, and 36.7% (n = 2,859) were evaluated that they had depressive symptoms. After adjusting for individual- and province-level covariates, the HCBSs utilization was found to be associated with depressive symptoms (OR = 1.180, 95% CI: 1.035-1.346, p < 0.05). Additionally, the depressive symptoms were significantly associated with gender, residence, educational level, marital status, number of chronic diseases, self-rated health (SRH), smoking, and provincial Gross Domestic Product (GDP) per capita. CONCLUSIONS: This study found HCBSs utilization might be a protective factor against depressive symptoms in Chinese older adults. It is of utmost significance for the government to provide targeted HCBSs at the community level to address the unmet care needs of older adults, which can reduce the occurrence of negative emotions, consequently contributing to less severe depressive symptoms.

Host Invasion Type Is a Phylogenetically Conserved Characteristic of Cephaleuros.

Cephaleuros species cause algal spot diseases, also known as red rust diseases, on many plants, including fruit crops. Most algal species are defined based on their morphological characteristics. Recent phylogenetic studies of Cephaleuros species showed that morphological determination was not congruent with phylogeny. Our study examined the phylogenetic congruence of the host invasion types (or growth habits), which are the most critical characteristics in the taxonomy of Cephaleuros. To ensure that host invasion types and phylogenetic characteristics could be inferred from the same isolate, host invasion types were assessed using microanatomical observation, and rRNA sequences from the same algal spot and/or the derived algal cultures were compared. Host invasion types were found to be conserved classification traits and were congruent with Cephaleuros phylogeny. The results also indicated that more than one Cephaleuros species commonly grew on the same leaf or, in a few cases, the same algal spot, suggesting that identification using different algal spots could result in misidentification. The Cephaleuros isolates were separated into two species complexes by host invasion types: the C. virescens species complex (CVSC) with subcuticular host invasion type and the C. parasiticus species complex (CPSC) with intercellular host invasion type. Molecular phylogenetic analysis indicated that Cephaleuros isolates clustered into 14 clades of CVSC and three clades of CPSC. This study also identified 16 and eight new hosts of CVSC and CPSC in Taiwan, respectively.

Decrypting the Controlled Product Selectivity over Ag-Cu Bimetallic Surface Alloys for Electrochemical CO2 Reduction.

Electrochemical CO2 reduction reaction (ECO2 RR) with controlled product selectivity is realized on Ag-Cu bimetallic surface alloys, with high selectivity towards C2 hydrocarbons/alcohols (≈60 % faradaic efficiency, FE), C1 hydrocarbons/alcohols (≈41 % FE) and CO (≈74 % FE) achieved by tuning surface compositions and applied potentials. In situ spectral investigations and theoretical calculations reveal that surface-composition-dependent d-band center could tune *CO binding strengths, regulating the *CO subsequent reaction pathways and then the product selectivity. Further adjusting the applied potentials will alter the energy of participated electrons, which leads to controlled ECO2 RR selectivity towards desired products. A predominant region map, with an indicator proposed to evaluate the thermodynamic predominance of the *CO subsequent reactions, is then provided as a reliable theoretical guidance for the controllable ECO2 RR product selectivity over bimetallic alloys.

Reducing the Ir-O Coordination Number in Anodic Catalysts based on IrOx Nanoparticles towards Enhanced Proton-exchange-membrane Water Electrolysis.

Due to the robust oxidation conditions in strong acid oxygen evolution reaction (OER), developing an OER electrocatalyst with high efficiency remains challenging in polymer electrolyte membrane (PEM) water electrolyzer. Recent theoretical research suggested that reducing the coordination number of Ir-O is feasible to reduce the energy barrier of the rate-determination step, potentially accelerating the OER. Inspired by this, we experimentally verified the Ir-O coordination number's role at model catalysts, then synthesized low-coordinated IrOx nanoparticles toward a durable PEM water electrolyzer. We first conducted model studies on commercial rutile-IrO2 using plasma-based defect engineering. The combined in situ X-ray absorption spectroscopy (XAS) analysis and computational studies clarify why the decreased coordination numbers increase catalytic activity. Next, under the model studies' guidelines, we explored a low-coordinated Ir-based catalyst with a lower overpotential of 231 mV@10 mA cm-2 accompanied by long durability (100 h) in an acidic OER. Finally, the assembled PEM water electrolyzer delivers a low voltage (1.72 V@1 A cm-2 ) as well as excellent stability exceeding 1200 h (@1 A cm-2 ) without obvious decay. This work provides a unique insight into the role of coordination numbers, paving the way for designing Ir-based catalysts for PEM water electrolyzers.

5f Covalency Synergistically Boosting Oxygen Evolution of UCoO4 Catalyst.

Electronic structure modulation among multiple metal sites is key to the design of efficient catalysts. Most studies have focused on regulating 3d transition-metal active ions through other d-block metals, while few have utilized f-block metals. Herein, we report a new class of catalyst, namely, UCoO4 with alternative CoO6 and 5f-related UO6 octahedra, as a unique example of a 5f-covalent compound that exhibits enhanced electrocatalytic oxygen evolution reaction (OER) activity because of the presence of the U 5f-O 2p-Co 3d network. UCoO4 exhibits a low overpotential of 250 mV at 10 mA cm-2, surpassing other unitary cobalt-based catalysts ever reported. X-ray absorption spectroscopy revealed that the Co2+ ion in pristine UCoO4 was converted to high-valence Co3+/4+, while U6+ remained unchanged during the OER, indicating that only Co was the active site. Density functional theory calculations demonstrated that the OER activity of Co3+/4+ was synergistically enhanced by the covalent bonding of U6+-5f in the U 5f-O 2p-Co 3d network. This study opens new avenues for the realization of electronic structure manipulation via unique 5f involvement.

Unusual High-Frequency Mechanical Properties of Polymer-Grafted Nanoparticle Melts.

Brillouin light spectroscopy is used to measure the elastic moduli of spherical polymer-grafted nanoparticle (GNP) melts as a function of chain length at fixed grafting density (0.47 chains/nm^{2}) and nanoparticle radius (8 nm). While the moduli follow a rule of mixtures (Wood's law) for long chains, they display enhanced elasticity and anomalous dissipation for graft chains <100 kDa. GNP melts with long polymers at high σ have a dry zone near the GNP core, surrounded by a region where the grafts can interpenetrate with chain fragments from adjacent GNPs. We propose that the departures from Wood's law for short chains are due to the effectively larger silica volume fraction in the region where sound propagates-this is caused by the short, interpenetrated chain fragments being pushed out of the way. We thus conclude that transport mechanisms (of gas, ions, sound, thermal phonons) in GNP melts are radically different if interpenetrated chain segments can be "pushed out of the way" or not. This provides a facile new means for manipulating the properties of these materials.

Effects of calorie intake and sampling time on thyroid stimulating hormone concentration.

BACKGROUND: This study aimed to investigate the effects of blood sampling after calorie intake on thyroid stimulating hormone (TSH) level, compared with blood sampling in fasting state. METHODS: This was a prospective, randomized, controlled study. Subjects from the outpatients in the department of endocrinology without evidence of thyroid diseases were included and then randomized into the fasting group, diet intake group, and glucose intake group, respectively. Fasting blood was collected from all subjects at 7:00 am for the measurement of TSH and free thyroxine (FT4) concentrations. Afterwards, the subjects were maintained at fasting state (fasting group), had an intake of the mixed diet with 400 kcal calories (diet intake group), and had an intake of 75 g glucose (glucose intake group), respectively, and blood was collected again 2 h later (9:00 am on the same day) for TSH and FT4 level measurement and comparison. RESULTS: A total of 150 subjects were enrolled, of whom 146 met the inclusion criteria, with 48, 48, and 50 in the diet intake group, glucose intake group, and fasting group, respectively. The TSH in the diet intake group was significantly lower at 9:00 am (TSH9am) than the level at 7:00 am (TSH7am) (P < 0.001), with a median variation of -0.71 mU/L, and a median variation rate of -32.4%. In the glucose intake group, TSH9am was also significantly lower than TSH7am (P < 0.001), with a median variation of -0.73 mU/L, and a median variation rate of -31.5%. For the fasting group, TSH9am decreased slightly but was significantly lower than TSH7am (P < 0.001), with a median variation of -0.1 mU/L, and a median variation rate of -5.2%. According to TSH7am measurements, 9 subjects (3 subjects in each group) met the diagnostic criteria of subclinical hypothyroidism. However, according toTSH9am measurements, only 2 patients in the fasting group met the diagnostic criteria of subclinical hypothyroidism. CONCLUSION: Compared with the fasting state, the TSH level at 2 h after the calorie intake was decreased by about 30%, which might influence the diagnosis of subclinical hypothyroidism. TRIAL REGISTRATION: ChiCTR2100047454 (18/06/2021).