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Molecular engineering binuclear copper catalysts for selective CO_(2) reduction to C_(2) products

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Journal of Energy Chemistry 2024年第6期93卷 166-173,I0005页

作者： Qi zhao Kai Lei Bao Yu xia Rachel Crespo-Otero Devis Di Tommaso Department of Chemistry School of Physical and Chemical SciencesQueen Mary University of LondonLondonE14NSUK Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureState Key Laboratory of Materials Processing and Die&Mould TechnologySchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074HubeiChina Department of Chemistry University College LondonLondonWC1H 0AJUK Digital Environment Research Institute Queen Mary University of LondonEmpire HouseLondon E11HHUK

Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal *** investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular *** modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)*** findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R *** rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular *** placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) *** research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.

关键词： Molecular catalyst design Selective CO_(2)reduction C_(2)products Density functional theory calculations

Application of CFD and FEA Coupling to Predict Structural Dynamic Responses of A Trimaran in Uni-and Bi-Directional Waves

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China Ocean Engineering 2024年第1期38卷 81-92页

作者： LIAO Xi-yu xia Jin-song CHEN Zhan-yang TANG Qin zhao Nan zhao Wei-dong GUI Hong-bin Marine Design&Research Institute of China Shanghai 200011China Ship Structure Division China Ship Scientific Research CenterWuxi 214082China College of Ocean Engineering Harbin Institute of TechnologyWeihaiWeihai 264209China State Key Laboratory of Structural Analysis Optimization and CAE Software for Industrial EquipmentDalian University of TechnologyDalian 116024China School of Foreign Studies Jiangnan UniversityWuxi 214122China

To predict the wave loads of a flexible trimaran in different wave fields,a one-way interaction numerical simulation method is proposed by integrating the fluid solver(Star-CCM+)and structural solver(Abaqus).Differing from the existing coupled CFD-FEA method for monohull ships in head waves,the presented method equates the mass and stiffness of the whole ship to the hull shell so that any transverse and longitudinal section stress of the hull in oblique waves can be ***,verification study and sensitivity analysis are carried out by comparing the trimaran motions using different mesh sizes and time step *** on the wave elevation of uni-and bi-directional waves is also carried *** a comprehensive analysis on the structural responses of the trimaran in different uni-directional regular wave and bi-directional cross sea conditions is carried out,***,the differences in structural response characteristics of trimaran in different wave fields are *** results show that the present method can reduce the computational burden of the two-way fluid-structure interaction simulations.

关键词： CFD-FEA fluid-structure coupling structural responses trimaran bi-directional cross sea

Insight into the Role of Isolated Gold Atoms-Ceria Conjunction in Catalyzing the Water-Gas Shift Reaction

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Chinese Journal of Chemistry 2024年第6期42卷 636-644页

作者： Xin-Pu Fu Hui-zhao Wei-Wei Wang chun-Jiang Jia Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinanShandong250100 China

As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au *** reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was ***,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),*** on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) *** CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) *** work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.

关键词： Isolated Au atoms Ceria-based catalysts Water-gas shift reaction Defect Adsorption

Construction of a Metallacyclopentadiene Ring through the Attack of Carbanions to M≡C Bond Followed by C—H Activation

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Chinese Journal of Chemistry 2024年第3期42卷 235-242页

作者： chun Tang Shengjie Zhang Zhengyu Lu Qian Li Ming Luo Dafa Chen Haiping xia State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringCollaborative Innovation Center of Chemistry for Energy MaterialsXiamen UniversityXiamenFujian361005 China Shenzhen Grubbs Institute and Guangdong Provincial Key Laboratory of Catalysis Department of ChemistrySouthern University of Science and TechnologyShenzhenGuangdong518055 China

Metallacyclopentadienes are important metallacycles and regarded as intermediates in many reactions,therefore,new methods to achieve them are *** this study,a formal[3+2]method,through the reactions of an osmapentalyne with benzyl carbanions,was *** reactions underwent a nucleophilic attack of carbanions to the Os≡C bond,followed by C—H activation to form the five-membered osmacyclopentadiene *** of the reactions were carried out at room temperature,the substituents on the aromatic rings of benzyl carbanions are diverse,and the resulting products contain an Os—H bond,representing a novel type of 10C-carbolong *** work provides a new convenient route to construct metallacyclopentadienes,which is expected to further promote the development of such a type of substances.

关键词： Metallacyclopentadiene Carbolong chemistry Osmium C–H activation Nucleophilic addition

A high-performance lithium anode based on N-doped composite graphene

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Rare Metals 2024年第3期43卷 1030-1036页

作者： Can Jiao Hao-Bo Sun Li Zhang Shang-Qian zhao Guo-Yao Pang chun-Rong zhao Shi-Gang Lu General Research Institute for Nonferrous Metals Beijing100088China China Automotive Battery Research Institute Co.Ltd Beijing101407China

Lithium(Li)metal is the most promising electrode for next-gene ration rechargeable *** order to push the commercialization of the lithium metal batteries,a kind of nitrogen(N)-doped composite graphene(NCG)adopted as the Li plating host was prepared to regulate Li metal nucleation and suppress dendrite ***,a new kind of sandwich-type composite lithium metal(STCL)electrode was developed to improve its *** STCL electrode can be used as convenient as a piece of Li foil but no dendrite *** a symmetric battery,the STCL electrode cycled for more than 4500 h with the overpotential of less than 40 *** due to the creative design,the STCL promises the Li-S battery with a prolonged cycling lifespan.

关键词： Lithium metal anode Lithiophilic N-doped composite graphene Sandwich-type composite lithium metal electrode

Acoustofluidic scanning fluorescence nanoscopy with a large field of view

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Microsystems & Nanoengineering 2024年第3期10卷 159-167页

作者： Geonsoo Jin Neil Upreti Joseph Rich Jianping xia Chenglong zhao Tony Jun Huang Thomas Lord Department of Mechanical Engineering and Materials Science Duke UniversityDurhamNC 27708USA Department of Biomedical Engineering Duke UniversityDurhamNC 27708USA The MITRE Corporation McLeanVA 22102USA

Large-field nanoscale fluorescence imaging is invaluable for many applications,such as imaging subcellular structures,visualizing protein interactions,and high-resolution tissue ***,conventional fluorescence microscopy requires a trade-off between resolution and field of view due to the nature of the optics used to form the *** overcome this barrier,we developed an acoustofluidic scanning fluorescence nanoscope that simultaneously achieves superior resolution,a large field of view,and strong fluorescent *** acoustofluidic scanning fluorescence nanoscope utilizes the superresolution capabilities of microspheres that are controlled by a programmable acoustofluidic device for rapid fluorescence enhancement and *** acoustofluidic scanning fluorescence nanoscope resolves structures that cannot be resolved with conventional fluorescence microscopes with the same objective lens and enhances the fluorescent signal by a factor of~5 without altering the field of view of the *** improved resolution realized with enhanced fluorescent signals and the large field of view achieved via acoustofluidic scanning fluorescence nanoscopy provides a powerful tool for versatile nanoscale fluorescence imaging for researchers in the fields of medicine,biology,biophysics,and biomedical engineering.

关键词： field resolution utilize

Toward a rapid and convenient nanoplastic quantification method in laboratory-scale study based on fluorescence intensity

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Frontiers of Environmental Science & Engineering 2024年第5期18卷 117-126页

作者： Ruiqi Yan Sen Lin Qian Ding Lei Zhang xia Yu Wentao zhao Qian Sui State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process School of Resources and Environmental EngineeringEast China University of Science and TechnologyShanghai200237China State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai200092China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

The thorough investigation of nanoplastics(NPs)in aqueous environments requires efficient and expeditious quantitative analytical methods that are sensitive to environmentally relevant NP concentrations and convenient to *** analysis-based quantitative methods have been acknowledged as effective and rapid approaches for quantifying NP concentrations in laboratory-scale ***,we compared three commonly used optical response indicators,namely fluorescence intensity(FI),ultraviolet absorbance,and turbidity,to assess their performance in quantifying ***,orthogonal experiments were conducted to evaluate the influence of various water quality parameters on the preferred indicator-based quantification *** results revealed that FI exhibits the highest correlation coefficient(>0.99)with NP ***,the limit of quantification(LOQ)for various types of NPs is exceptionally low,ranging from 0.0089 to 0.0584 mg/L in ultrapure water,well below environmentally relevant *** variations in water quality parameters such as pH,salinity,suspended solids(SS),and humic acid,a robust relationship between detectable FI and NP concentration was ***,an increased matrix,especially SS in water samples,results in an enhanced LOQ for ***,the quantitative method remains applicable in real water bodies,especially in drinking water,with NP LOQ as low as 0.0157–0.0711 mg/*** exceeds the previously reported detectable concentration for 100 nm NPs at 40µg/mL using surface-enhanced Raman *** study confirms the potential of FI as a reliable indicator for the rapid quantification of NPs in aqueous environments,offering substantial advantages in terms of both convenience and cost-effectiveness.

关键词： Nanoplastic quantification Fluorescence intensity Drinking water Limit of quantification(LOQ) Matrix effects

Study on cumulative effects of biological craniocerebral trauma under repeated blast

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Theoretical & Applied Mechanics Letters 2024年第3期14卷 174-183页

作者： Xingyuan Huang Bingchen xia Lijun Chang Zhikang Liao Hui zhao Zhihua Cai Hunan Provincial Key Laboratory of Health Maintenance for Mechanical Equipment Hunan University of Science and TechnologyXiangtan 411201China School of Mechanical and Electrical Engineering Foshan UniversityFoshan 528231China Institute for Traffic Medicine PLA Army Characteristic Medical CenterChongqing 400042China

Repeated blast impacts on personnel in explosive environments can exacerbate craniocerebral *** existing studies focus on the injury effects of a single blast,lacking in-depth analysis on the injury effects and cumulative effects of repeated ***,rats were used as the experimental samples to suffer from explosion blasts with different peak air overpressures(167 kPa~482 kPa)and varying number of repeated *** cumulative effect of craniocerebral trauma was most pronounced for moderate repeated blast,showing approximately 95%increase of trauma severity with penta blast,and an approximately 85%increase of trauma severity with penta minor *** cumulative effect of craniocerebral trauma from severe,repeated blast has a smaller rate of change compared to the other two *** severity of trauma from penta blast increased by approximately 69%compared to a single *** physiological,pathological and biochemical analysis show that the degree of neurological trauma caused by repeated blasts is higher than that of single blasts,and the pathological trauma to brain tissue is more extensive and *** trauma degree remains unchanged after double blast,increases by one grade after triple or quadruple blast,and increases by two grades after penta blast.

关键词： Repeated blast Craniocerebral trauma Trauma severity grade Cumulative effects

Ginsenoside Rd Induces Differentiation of Myeloid Leukemia Cells via Regulating ERK/GSK-3βSignaling Pathway

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Chinese Journal of Integrative Medicine 2024年第7期30卷 588-599页

作者： JIANG Yu-xia zhao Yan-na YU xiao-ling YIN Li-ming Department of Hematology Tongde Hospital of Zhejiang ProvinceHangzhou310012China Institute of Hematology Research the First Affiliated Hospital of Zhejiang Chinese Medical University(Zhejiang Provincial Hospital of Chinese Medicine)Hangzhou310006China

Objective To investigate the role of ginsenoside Rd(GRd)in acute myeloid leukemia(AML)cell *** AML cells were treated with GRd(25,50,100 and 200µg/mL),retinoic acid(RA,0.1g/L)and PD98059(20 mg/mL)for 72 h,cell survival was detected by methylthiazolyldiphenyl-tetrazolium bromide and colony formation assays,and cell cycle was detected by flow *** morphology and differentiation were observed by Wright-Giemsa staining,peroxidase chemical staining and cellular immunochemistry assay,*** protein expression levels of GATA binding protein 1(GATA-1),purine rich Box-1(PU.1),phosphorylated-extracellular signal-related kinase(p-ERK),ERK,phosphorylated-glycogen synthase kinase-3β(p-GSK3β),GSK3βand signal transducer and activator of transcription 1(STAT1)were detected by Western ***-six mice were randomly divided into 3 groups using a random number table:model control group(non-treated),GRd group[treated with 200 mg/(kg·d)GRd]and homoharringtonine(HTT)group[treated with 1 mg/(kg·d)HTT].A tumor-bearing nude mouse model was established,and tumor weight and volume were *** of subcutaneous tumor tissue were observed after hematoxylin and eosin ***1 and GATA-1 expressions were detected by immunohistochemical *** The cell survival was inhibited by GRd in a dose-dependent manner and GRd caused G0/G1 cell arrest(p<0.05).GRd treatment induced leukemia cell differentiation,showing increased expressions of peroxidase and specific proteins concerning erythrogenic or granulocytic differentiation(p<0.05).GRd treatment elicited upregulation of p-ERK,p-GSK-3βand STAT1 expressions in cells,and reversed the effects of PD98059 on inhibiting the expressions of peroxidase,GATA-1 and PU.1(P<0.05).After GRd treatment,tumor weight and volume of mice were decreased,and tumor cells underwent massive apoptosis and necrosis(P<0.05).WT1 level was decreased,and GATA-1 level was significantly increased in subcutaneous tumor ti

关键词： ginsenoside Rd myeloid leukemia survival differentiation extracellular signal-related kinase signaling pathway