多级钯-铜-银多孔纳米花作为高效电催化剂催化CO_(2)还原为C_(2+)产物

近年来,具有可控元素分布的铜基多金属纳米晶作为CO_(2)还原反应(CO_(2)RR)的电催化剂,受到了广泛研究。通过对铜电催化剂进行二次甚至多次的金属元素修饰,能够有效改变其整体d带结构并引起d带中心的位移。这种变化可以影响铜对关键中间体的表面亲和力,从而影响后续的催化途径。除了调整电子结构,形貌工程也成为提高CO_(2)RR电催化性能的有效手段。相对于随机形状的球形颗粒,基于二维纳米片构建的三维多孔结构有利于最大限度地暴露表面原子,为催化过程中产生的关键中间体提供丰富的扩散通道和反应中心。然而,通过设计合成路线构建这种类型的纳米结构是一项技术挑战,传统的分步自组装策略耗时且难以精确控制结构。因此,我们的研究旨在实现高纯度的合成方法,制备这种独特的纳米结构,并精确调控元素组成和电子结构,以探索结构优势与CO_(2)RR电化学性能改善之间的潜在关系,具有重要的应用价值。在此研究中,我们合理设计了钯-铜-银(Pd-Cu-Ag)纳米晶的二维-三维杂化结构,实现了可控的合成过程,并验证了其在电化学CO_(2)还原中的应用潜力。合成过程中,通过使用封装剂十八烷基三甲基氯化铵,成功地将Au@Cu_(x)O纳米球转化为层状CuAg纳米花(HNFs)。有趣的是,该过程中原位形成了作为构建单元的纳米薄片。通过对CuAg HNFs与Na_(2)PdCl_(4)进行电偶置换,除去了Ag和Cu,引入了零价的Pd,并在纳米片上形成了大量孔隙。我们对这些CuAg电催化剂进行了CO_(2)RR测试,结果显示Pd_(0.7)Cu_(40.0)Ag_(59.7)PHNs在C_(2+)产物选择性(69.5%)和C_(2+)分电流密度(-349.1mA·cm^(-2))方面表现出最佳性能。密度泛函理论(DFT)模拟表明,PdAgCu表面具有独特的电子性质,降低了C-C偶联反应的能垒,凸显了Pd掺杂对CuAg电催化剂CO_(2)还原的卓越性能。本研究为基于多孔纳米薄片构建多层次多金属纳米结构提供了一种直观方法,并验证了其在电催化方面的结构优势,为高效的CO_(2)RR催化剂的合理设计提供了依据。

Numerical studies on the radiation uniformity of Z-pinch dynamic hohlraum

Radiation uniformity is important for Z-pinch dynamic hohlraum driven fusion. In order to understand the radiation uniformity of Z-pinchdynamic hohlraum, the code MULTI-2D with a new developed magnetic field package is employed to investigate the related physical processeson Julong-I facility with drive current about 7e8 MA. Numerical simulations suggest that Z-pinch dynamic hohlraum with radiation temperaturemore than 100 eV can be created on Julong-I facility. Although some X-rays can escape out of the hohlraum from Z-pinch plasma and electrodes, the radiation field near the foam center is quite uniform after a transition time. For the load parameters used in this paper, the transitiontime for the thermal wave transports from r = 1 mm to r = 0 mm is about 2.0 ns. Implosion of a testing pellet driven by cylindrical dynamichohlraum shows that symmetrical implosion is hard to achieve due to the relatively slow propagation speed of thermal wave and the compressionof cylindrical shock in the foam. With the help of quasi-spherical implosion, the hohlraum radiation uniformity and corresponding pelletimplosion symmetry can be significantly improved thanks to the shape modulation of thermal wave front and shock wave front.

Genetic analyses in a cohort of 191 Chinese pulmonarv arterial hypertension patients

Objective Pulmonary arterial hypertension(PAH)is mainly characterized by pulmonary artery obstruction,which is diagnosed by a mean pulmonary artery pressure≥25 mm Hg at rest,and excluding other known causes of pulmonary hypertension.To identify genetic mutations and help make a precise diagnosis,we performed genetic testing in 191 probands with invasively confirmed PAH and tried to analyze the genotype-phenotype correlation.

A compound heterozygous EIF2AK4 mutation cause pulmonary veno-occlusive disease

Aim Idiopathic pulmonary arterial hypertension(IPAH) and pulmonary veno-occlusive disease (PVOD) are undistinguished on clinical practice. We proposed that gene test might be a promising and feasible method in the future.Methods A 20-year-old woman was diagnosed as IPAH in 2013while a diagnosis of PVOD was also suspected. The genomic DNA was extracted from peripheral blood and gene panel testing was performed.

Machine-learning guided optimization of laser pulses for direct-drive implosions

The optimization of laser pulse shapes is of great importance and a major challenge for laser direct-drive implosions.In this paper,we propose an efficient intelligent method to perform laser pulse optimization via hydrodynamic simulations guided by the genetic algorithm and random forest algorithm.Compared to manual optimizations,the machine-learning guided method is able to efficiently improve the areal density by a factor of 63%and reduce the in-fiight-aspect ratio by a factor of 30%at the same time.A relationship between the maximum areal density and ion temperature is also achieved by the analysis of the big simulation dataset.This design method has been successfully demonstrated by the2021 summer double-cone ignition experiments conducted at the SG-II upgrade laser facility and has great prospects for the design of other inertial fusion experiments.

nvolvement of collagen-binding heat shock protein 47 in scleroderma-associated fibrosis

Uncontrolled fibrosis of skin and internal organs is the main characteristic of scleroderma, and collagen is a major extracellular matrix protein that deposits in the fibrotic organs. As the chaperone of collagen, heat shock protein 47 （HSP47） is closely related with the development of fbrosis. To explore the potential func- tion of HSP47 in the pathogenesis of scleroderma, the clinical, in vivo and in vitro studies were performed. In clinical, the increased mRNA level of HSP47 was observed in the skin fibroblasts and PBMC from scle- roderma patients, and the enhanced protein level of HSP47 was also detected in the skin biopsy and plasma of the above patients. Unexpectedly, the enhanced levels of HSP47 were positively correlated with the presence of anti-centromere antibody in scleroderma patients. Moreover, a high expression of HSP47 was found in the skin lesion of BLM-induced scleroderma mouse model. Further in vitro studies demonstrated that HSP47 knockdown could block the intracellular and extracellular collagen over-productions induced by exogenous TGF-13. Therefore, the results in this study provide direct evidence that HSP47 is involved in the pathogenesis of scleroderma. The high expression of HSP47 can be detected in the circulatory system of scleroderma patients, indicating that HSP47 maybecome a pathological marker to assess the progres- sion of scleroderma, and also explain the systemic fibrosis of scleroderma. Meanwhile, collagen over-ex- pression is blocked by HSP47 knockdown, suggesting the possibility that HSP47 can be a potential therapeutic target for scleroderma.

Machine-learning guided optimization of laser pulses for direct-drive implosions

There was a mistake in the value of V in the righthand column of Table l.A correct version of the table is below.Also,the units of this value when stated in the text were incorrectly stated as g/cm²,where they should have been stated askm/s.

Using Composite Phenotypes to Reveal Hidden Physiological Heterogeneity in High-Altitude Acclimatization in a Chinese Han Longitudinal Cohort

Altitude acclimatization is a human physiological process of adjusting to the decreased oxygen availability.Since several physiological processes are involved and their correlations are complicated,the analyses of single traits are insufficient in revealing the complex mechanism of high-altitude acclimatization.In this study,we examined these physiological responses as the composite phenotypes that are represented by a linear combination of physiological traits.We developed a strategy that combines both spectral clustering and partial least squares path modeling(PLSPM)to define composite phenotypes based on a cohort study of 883 Chinese Han males.In addition,we captured 14 composite phenotypes from 28 physiological traits of high-altitude acclimatization.Using these composite phenotypes,we applied k-means clustering to reveal hidden population physiological heterogeneity in high-altitude acclimatization.Furthermore,we employed multivariate linear regression to systematically model(Models 1 and 2)oxygen saturation(SpO_(2))changes in high-altitude acclimatization and evaluated model fitness performance.Composite phenotypes based on Model 2 fit better than single trait-based Model 1 in all measurement indices.This new strategy of using composite phenotypes may be potentially employed as a general strategy for complex traits research such as genetic loci discovery and analyses of phenomics.

Correlation of DNA methylation patterns to the phenotypic features of Tibetan elite alpinists in extreme hypoxia

High altitude is an extreme environment that imposes hypoxic pressure on physiological processes,and natives living at high altitudes are more adaptive in certain physiological processes.So far,epigenetic modifications under extreme changes in hypoxic pressures are relatively less understood.Here,we recruit 32 Tibetan elite alpinists(TEAs),who have successfully mounted Everest(8848 m)at least five times.Blood samples and physiological phenotypes of TEAs and 32 matched non-alpinist Tibetan volunteers(non-TEAs)are collected for analysis.Genome-wide DNA methylation analysis identifies 23,202 differentially methylated CpGs(P_(adj)<0.05,|β|>0.1)between the two groups.Some differentially methylated CpGs are in hypoxia-related genes such as PPP1R13L,MAP3K7CL,SEPTI-9,and CUL2.In addition,Gene ontology enrichment analysis reveals several inflammation-related pathways.Phenotypic analysis indicates that 12 phenotypes are significantly different between the two groups.In particular,TEAs exhibit higher blood oxygen saturation levels and lower neutrophil count,platelet count,and heart rate.For DNA methylation association analysis,we find that two CpGs(cg16687447,cg06947206)upstream of PTEN were associated with platelet count.In conclusion,extreme hypoxia exposure leads to epigenetic modifications and phenotypic alterations of TEA,providing us clues for exploring the molecular mechanism underlying changes under extreme hypoxia conditions.

The HuaBiao project:whole-exome sequencing of 5000 Han Chinese individuals

Next-generation sequencing technologies have significantly accelerated the identification of disease-causing mutations and facilitated the emergence of personalized medicine(Genomes Project Consortium et al.,2015;Goodwin et al.,2016;Sirugo et al.,2019).In comparison with whole-genome sequencing,whole-exome sequencing(WES),which covers the coding regions of the genome,offers a cost-efficacy balance.WES provides deeper sequencing depth(>100)and allows the more accurate detection of rare variants that are tailored for clinical applications(Lek et al.,2016).

Contradictory effect of gold nanoparticle-decorated molybdenum sulfide nanocomposites on amyloid-β-40 aggregation

The effect of gold nanoparticle-decorated molybdenum sulfide(AuNP-MoS2)nanocomposites on amyloid-β-40(Aβ40)aggregation was investigated.The interesting discovery was that the effect of AuNPMoS2 nanocomposites on Aβ40 aggregation was contradictory.Low concentration of AuNP-MoS2 nanocomposites could enhance the nucleus formation of Aβ40 peptides and accelerate Aβ40 fibrils aggregation.However,although high concentration of AuNP-MoS2 nanocomposites could enhance the nucleus formation of Aβ40 peptides,it eventually inhibited Aβ40 aggregation process.It might be attributed to the interaction between AuNP-MoS2 nanocomposites and Aβ40 peptides.For low concentration of AuNP-MoS2 nanocomposites,it was acted as nuclei,resulting in the acceleration of the nucleation process.However,the structural flexibility of Aβ40 peptides was limited as the concentration of AuNP-MoS2 nanocomposites was increased,resulting in the inhibition of Aβ40aggregation.These findings suggested that AuNP-MoS2 nanocomposites might have a great potential to design new multifunctional material for future treatment of amyloid-related diseases.

Anisotropic Plasmon Resonance Enables Spatially Controlled Photothermal and Photochemical Effects in Hot Carrier-Driven Catalysis

Localized surface plasmon resonance has been demonstrated to provide effective photophysical enhancement mechanisms in plasmonic photocatalysis.However,it remains highly challenging for distinct mechanisms to function in synergy for a collective gain in catalysis due to the lack of spatiotemporal control of their effect.Herein,the anisotropic plasmon resonance nature of Au nanorods was exploited to achieve distinct functionality towards synergistic photocatalysis.Photothermal and photochemical effects were enabled by the longitudinal and transverse plasmon resonance modes,respectively,and were enhanced by partial coating of silica nanoshells and epitaxial growth of a reactor component.Resonant excitation leads to a synergistic gain in photothermal-mediated hot carrier-driven hydrogen evolution catalysis.Our approach provides important design principles for plasmonic photocatalysts in achieving spatiotemporal modulation of distinct photophysical enhancement mechanisms.It also effectively broadens the sunlight response range and increases the efficacy of distinct plasmonic enhancement pathways towards solar energy harvesting and conversion.