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Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries

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chinese Chemical Letters 2024年第5期35卷 434-440页

作者： Haodong Wang Xiaoxu Lai chi chen Pei Shi Houzhao Wan Hao Wang Xingguang chen Dan Sun CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Fujian Normal UniversityFuzhou 350007China Xiamen Institute of Rare Earth Materials Haixi InstitutesChinese Academy of SciencesXiamen 361021China School of Microelectronics Hubei UniversityWuhan 430062China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen 361021China

The detrimental“shuttle effect”of lithium polysulfides(LiPSs)together with sluggish multi-order reaction kinetics are the main drawbacks hindering lithium-sulfur(Li-S)batteries from commercial success.Here,we first propose the implementability of layered rare-earth hydroxides(LREHs)in Li-S batteries to optimize electrochemical performance.In this work,a two-dimensional(2D)rare-earth-based composite constructed by the layered gadolinium hydroxy chloride[Gd_(2)(OH)_(5)(H_(2)O)_(n)]Cl nanoplates(LGdH NPs)and graphene oxide(GO)was designed as a sulfur immobilizer for Li-S batteries.Combining the experimental results and density functional theory(DFT)calculations,it is revealed that the LGdH@GO composite not only provides a strong anchoring of the intermediates during cycling,but also acts as an effective catalyst to accelerate the liquid-solid conversion of polysulfides.The Li-S batteries assembled by LGdH@GO modified separators delivered a superior rate performance with a specific capacity of 605.34 mAh/g at 5 C,as well as excellent cycle stability with a decay rate of 0.087%over 500 cycles at 2 C.This study provided a deep understanding of the mechanism to suppress the“shuttle effect”by the LREHs,and a guide to design effective functional interlayers for high-performance Li-S batteries with excellent electrocatalytic activity.

关键词： Lithium-sulfur batteries Functional separator Layered rare-earth hydroxides Shuttle effect Adsorption Catalysis

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Pillar effect induced by ultrahigh phosphorous/nitrogen doping enables graphene/MXene film with excellent cycling stability for alkali metal ion storage

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Journal of Energy Chemistry 2024年第6期93卷 146-156,I0004页

作者： Meng Qin Yiwei Yao Junjie Mao chi chen Kai Zhu Guiling Wang Dianxue Cao Jun Yan Key Laboratory of Superlight Materials and Surface Technology Ministry of EducationCollege of Materials Science and Chemical EngineeringHarbin Engineering UniversityHarbin 150001HeilongjiangChina Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials and Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021FujianChina

Graphene's large theoretical surface area and high conductivity make it an attractive anode material for potassium-ion batteries(PIBs).However,its practical application is hindered by small interlayer distance and long ion transfer distance.Herein,this paper aims to address the issue by introducing MXene through a simple and scalable method for assembling graphene and realizing ultrahigh P doping content.The findings reveal that MXene and P-C bonds have a "pillar effect" on the structure of graphene,and the P-C bond plays a primary role.In addition,N/P co-doping introduces abundant defects,providing more active sites for K^(+) storage and facilitating K^(+) adsorption.As expected,the developed ultrahigh phosphorous/nitrogen co-doped flexible reduced graphene oxide/MXene(NPrGM) electrode exhibits remarkable reversible discharge capacity(554 mA hg^(-1) at 0.05 A g^(-1)),impressive rate capability(178 mA h g^(-1) at 2 A g^(-1)),and robust cyclic stability(0.0005% decay per cycle after 10,000 cycles at 2 A g^(-1)).Furthermore,the assembled activated carbon‖NPrGM potassium-ion hybrid capacitor(PIHC) can deliver an impressive energy density of 131 W h kg^(-1) and stable cycling performance with 98.1% capacitance retention after5000 cycles at 1 A g^(-1).Such a new strategy will effectively promote the practical application of graphene materials in PIBs/PIHCs and open new avenues for the scalable development of flexible films based on two-dimensional materials for potential applications in energy storage,thermal interface,and electromagnetic shielding.

关键词： Graphene MXene Phosphorous doping Pillar effect Potassium-ion batteries

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A Systematic Analysis of Early Life Exposure to the chinese Famine(1959-1961)and the Health of Older Adults-china,2008-2023

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china CDC weekly 2024年第11期6卷 203-207,I0001-I0003页

作者： chi Shen Xi chen School of Public Policy and Administration Xi’an Jiaotong UniversityXi’an CityShaanxi ProvinceChina Department of Health Policy and Management Yale School of Public HealthNew HavenCTU.S Department of Economics Yale UniversityNew HavenCTU.S

What is already known about this topic?There is mounting evidence indicating that the aging process initiates during early life stages,with in utero the individual’s environment playing a significant role.Consequently,it is crucial to comprehend the enduring effects of early life circumstances on health in old age.What is added by this report?In this study,we conducted a meta-analysis to examine the effects of the chinese Famine(1959–1961)on the health of older adults.We also explored potential mechanisms underlying these effects.What are the implications for public health practice?The complex interplay between early life circumstances,multiple health-related sectors,and healthy aging necessitates a comprehensive life-course approach and strategic interventions to enhance public health in an aging society.

关键词： life aging mount

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Serum 25-hydroxyvitamin D, genetic susceptibility, and the risk of incident type 2 diabetes: A prospective cohort in East china

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中华医学杂志(英文版) 2024年第8期137卷 972-979页

作者： Sun Ying Zhang Haojie Wang Bin Wang Yuying chen chi chen Yi Lu Yingli Wang Ningjian West china Hospital Sichuan University chengdu Sichuan 610041 Department of Endocrinology Shuguang Hospital Affiliated to Shanghai University of Traditional chinese Medicine Shanghai 201203 Institute and Department of Endocrinology and Metabolism Shanghai Ninth People’s Hospital Shanghai JiaoTong University School of Medicine Shanghai 200011 china Department of Endocrinology and Metabolism and Department of Guideline and Rapid Recommendation Cochrane china Center MAGIC china Center chinese Evidence-Based Medicine Center

Background: The serum vitamin D level varies widely by population, and studies have linked vitamin D levels with the risk of type 2 diabetes mellitus (T2DM). However, the relationship is inconsistent and the impact of vitamin D on T2DM among East chinese adults is unclear. The study aimed to investigate the association between serum 25-hydroxyvitamin D (25[OH]D) levels and the risk of T2DM and evaluated whether the association is modified by genetic predisposition.Methods: In the Survey on Prevalence in East china for Metabolic Diseases and Risk Factors (SPECT-china) cohort, 1862 participants free of T2DM at baseline were included. A weighted genetic risk score was calculated with 28 variants associated with T2DM. Hierarchical logistic models were used to examine the association of serum 25(OH)D and genetic risk with T2DM.Results: After a 5-year follow-up, 132 cases of T2DM were documented. We observed no significant association between quartiles of serum 25(OH)D and T2DM risk after multivariable adjustment (χ2 = 0.571,Pfor trend = 0.426). Compared to those in the lowest quartile of 25(OH)D, the odds ratios (ORs) (95% confidence interval [CI]) for participants with increased quartiles were 1.29 (0.74-2.25), 1.35 (0.77-2.36), and 1.27 (0.72-2.24), respectively. We observed a positive association of glycated hemoglobin (HbA1c) with 25(OH)D at baseline (β = 1.752,P = 0.001) and after follow-up (β = 1.385,P = 0.003), and a negative association of ln conversion homeostasis model assessment (HOMA)-β with 25(OH)D at baseline (β = -0.982,P = 0.021). There was no significant interaction between 25(OH)D and diabetes genetic predisposition on the risk of T2DM (χ2 = 2.710,Pfor interaction = 0.100). The lowest OR (95% CI) of T2DM was among participants with low genetic risk and the highest quartile of 25(OH)D (0.17 [0.05–0.62]).Conclusion: Serum 25(OH)D may be irrelevant to the risk of incident T2DM among East chinese adults regardless of genetic predisposition.

关键词： Vitamin D Diabetes mellitus, Type 2 Genetic predisposition to disease Prospective cohort Glycated hemoglobin SPECT-china

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Causal roles of gut microbiota in cholangiocarcinoma etiology suggested by genetic study

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World Journal of Gastrointestinal Oncology 2024年第4期16卷 1319-1333页

作者： Zhi-Tao chen chen-chen Ding Kai-Lei chen Yang-Jun Gu chi-cheng Lu Qi-Yong Li Division of Hepatobiliary and Pancreatic Surgery Shulan(Hangzhou)Hospital Affiliated to Zhejiang Shuren University Shulan International Medical CollegeHangzhou 310000Zhejiang ProvinceChina Pediatric Psychology The Affiliated Mental Health Centre&Hangzhou Seventh People’s HospitalZhejiang University School of MedicineHangzhou 310000Zhejiang ProvinceChina School of Medicine Zhejiang Shuren UniversityHangzhou 310000Zhejiang ProvinceChina School of Medicine Zhejiang Chinese Medical University Zhejiang Shuren CollegeHangzhou 310000Zhejiang ProvinceChina

BACKGROUND Cholangiocarcinoma(CCA)is a highly malignant biliary tract cancer with poor prognosis.Previous studies have implicated the gut microbiota in CCA,but evidence for causal mechanisms is lacking.AIM To investigate the causal relationship between gut microbiota and CCA risk.METHODS We performed a two-sample mendelian randomization study to evaluate potential causal associations between gut microbiota and CCA risk using genome-wide association study summary statistics for 196 gut microbial taxa and CCA.Genetic variants were used as instrumental variables.Multiple sensitivity analyses assessed result robustness.RESULTS Fifteen gut microbial taxa showed significant causal associations with CCA risk.Higher genetically predicted abundance of genus Eubacteriumnodatum group,genus Ruminococcustorques group,genus Coprococcus,genus Dorea,and phylum Actinobacteria were associated with reduced risk of gallbladder cancer and extrahepatic CCA.Increased intrahepatic CCA risk was associated with higher abundance of family Veillonellaceae,genus Alistipes,order Enterobacteriales,and phylum Firmicutes.Protective effects against CCA were suggested for genus Collinsella,genus Eisenbergiella,genus Anaerostipes,genus Paraprevotella,genus Parasutterella,and phylum Verrucomicrobia.Sensitivity analyses indicated these findings were reliable without pleiotropy.CONCLUSION This pioneering study provides novel evidence that specific gut microbiota may play causal roles in CCA risk.Further experimental validation of these candidate microbes is warranted to consolidate causality and mechanisms.

关键词： Cholangiocarcinoma Mendelian randomization Gut microbiota Instrumental variables Sensitivity analyses

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Cobalt-nitrogen co-doped porous carbon sphere as highly efficient catalyst for liquid-phase cyclohexane oxidation with molecular oxygen and the active sites investigation

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Frontiers of Chemical Science and Engineering 2024年第3期18卷 101-112页

作者： Lei chen Yuan Sun Jinshan chi Wei Xiong Pingle Liu Fang Hao College of Chemical Engineering National&Local United Engineering Research Centre for Chemical Process Simulation and IntensificationXiangtan UniversityXiangtan411105China

The selective oxidation of cyclohexane to cyclohexanone and cyclohexanol(KA oil)is a challenging issue in the chemical industry.At present the industrial conversion of cyclohexane to cyclohexanone and cyclohexanol is normally controlled at less than 5%selectivity.Thus,the development of highly active and stable catalysts for the aerobic oxidation of cyclohexane is necessary to overcome this low-efficiency process.Therefore,we have developed a cobalt-nitrogen co-doped porous sphere catalyst,Co-NC-x(x is the Zn/Co molar ratio,where x=0,0.5,1,2,and 4)by pyrolyzing resorcinol-formaldehyde resin microspheres.It achieved 88.28%cyclohexanone and cyclohexanol selectivity and a cyclohexane conversion of 8.88%under Co-NC-2.The results showed that the introduction of zinc effectively alleviated the aggregation of Co nanoparticles and optimized the structural properties of the material.In addition,Co0 and pyridinic-N are proposed to be the possible active species,and their proportion efficiently increased in the presence of Zn^(2+)species.In this study,we developed a novel strategy to design highly active catalysts for cyclohexane oxidation.

关键词： KA oil production cyclohexane selective oxidation cobalt-nitrogen co-doped porous carbon spheres metal-organic framework

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Theoretical screening of cooperative N-bridged dual-atom sites for efficient electrocatalytic nitrogen reduction with remolding insight

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Nano Research 2024年第4期17卷 3413-3422页

作者： Huimei chen Yan Yang chi Jiao Zhiwen Zhuo Junjie Mao Yan Liu Key Laboratory of Functional Molecular Solids Ministry of EducationCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China

The electrocatalytic nitrogen reduction reaction(e-NRR)is a promising alternative method for the Haber–Bosch process.However,it still faces many challenges in searching for high activity,stability,and selectivity catalysts and ascertaining the catalytic mechanism with complete insight.Here,a series of graphene-based N-bridged dual-atom catalysts(M1-N-M2/NC)are systematically investigated via first-principle calculation and a high-throughput screening strategy.The result unveils that N_(2) adsorption on M1-N-M2/NC in bridge-on adsorption mode can effectively break the scaling relationship on single-atom catalysts(SACs).Moreover,V-N-Ru/NC and V-N-Os/NC are systematically screened out as promising e-NRR catalysts,with extremely low limiting potentials of-0.20 and-0.18 V,respectively.Furthermore,the adsorption site competition between*N_(2) and*H,as well as the competitive twin reactions of hydrogen evolution reaction(HER)on intermediates(N_(n)H_(m))during the e-NRR process,is systematically evaluated to form a remodeling insight for the reactions in mechanism,and the e-NRR of new proposed dual-atom catalysts(DACs)is strategically optimized for its high-efficiency performance potential via our remolding insight in e-NRR mechanism.This work provides new ideas and insights for the design and mechanism of e-NRR catalysts and an effective strategy for rapidly screening highly efficient e-NRR catalysts.

关键词： nitrogen reduction dual-atom catalysts high-throughput screening hydrogen evolution reaction density functional theory calculations

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Nonlinear Impact Damage Evolution of Charpy Type and Analysis of Its Key Influencing Factors

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chinese Journal of Mechanical Engineering 2024年第1期37卷 254-264页

作者： Jianfeng Mao Qian Xu Jiadong Yang chi Cao Dasheng Wang Fengping Zhong Mingya chen Institute of Process Equipment and Control Engineering Zhejiang University of TechnologyHangzhou 310032China Taizhou Key Laboratory of Advanced Manufacturing Technology Taizhou InstituteZhejiang University of TechnologyTaizhou 318014China State Key Laboratory of Nuclear Power Safety Monitoring Technology and Equipment Shenzhen 518172China Zhejiang Academy of Special Equipment Science Hangzhou 310020China Suzhou Nuclear Power Research Institute Suzhou 215004China

The current research of Charpy impact mainly focuses on obtaining the ductile brittle transition temperature of materials by experiments.Compared with experiments,numerical simulation can study many problems with harsh conditions.However,there are still few studies on the influence of geometric factors such as side grooves.In this paper,the geometry of standard Charpy impact test is designed.Specimens with different widths and side grooves are tested.The finite element model of Charpy impact was established by ABAQUS software.Use test results and simulation results to verify each other.The effects of sample width,side groove depth and side groove bottom fillet on the impact fracture resistance of the sample were studied.The results show that the specimen width is positively correlated with the impact toughness of the specimen.The side groove greatly reduces the impact toughness of the material;the toughness of side groove decreases with the increase of depth;the fracture toughness of side groove decreases with the increase of fillet at the bottom of side groove.The proportion of toughness energy to impact energy of samples was analyzed.The results show that the toughness energy accounts for about 70%of the impact energy of the sample,which has little to do with the geometric characteristics of the sample.This study presents a reliable method for studying Charpy impact tests.The influence of geometric parameters is obtained,which provides a reference method for the study of impact toughness of high toughness materials.

关键词： Johnson-Cook model Impact toughness Charpy impact

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Unraveling engineering disturbance effects on deformation in red-bed mudstone railway cuttings:incorporating crack-facilitated moisture diffusion

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Journal of Mountain Science 2024年第5期21卷 1663-1682页

作者： HUANG Kang DAI Zhangjun YAN chengzeng YAO Junkai chi Zecheng chen Shanxiong State Key Laboratory of Geomechanics and Geotechnical Engineering Institute of Rock and Soil MechanicsChinese Academy of SciencesWuhan 430071China University of chinese Academy of Sciences Beijing 100049China Faculty of Engineering China University of GeosciencesWuhan 430074China International Joint Research Center for Deep Earth Drilling and Resource Development China University of GeosciencesWuhan 430074China china Academy of Railway Sciences Corporation Limited Beijing 100081China

Red-bed mudstone, prevalent in southwest china, poses a formidable challenge due to its hydrophilic clay minerals, resulting in expansion, deformation, and cracking upon exposure to moisture. This study addresses uplift deformation disasters in high-speed railways by employing a moisture diffusion-deformation-fracture coupling model based on the finite-discrete element method(FDEM). The model integrates the influence of cracks on moisture diffusion. The investigation into various excavation depths reveals a direct correlation between depth and the formation of tensile cracks at the bottom of the railway cutting. These cracks expedite moisture migration, significantly impacting the temporal and spatial evolution of the moisture field. Additionally, crack expansion dominates hygroscopic deformation, with the lateral coordinate of the crack zone determining peak vertical displacement. Furthermore, key factors influencing deformation in railway cuttings, including the swelling factor and initial moisture content at the bottom of the cutting, are explored. The number of tensile and shear cracks increases with greater excavation depth, particularly concerning shear cracks. Higher swelling factors and initial moisture contents result in an increased total number of cracks, predominantly shear cracks. Numerical calculations provide valuable insights, offering a scientific foundation and directional guidance for the precise prevention, control, prediction, and comprehensive treatment of mudstone-related issues in high-speed railways.

关键词： Red-bed mudstone Railway cutting FDEM Moisture diffusion Deformation Crack

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Heterogeneous expression of stearoyl-acyl carrier protein desaturase genes SAD1 and SAD2 from Linum usitatissimum enhances seed oleic acid accumulation and seedling cold and drought tolerance in Brassica napus

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Journal of Integrative Agriculture 2024年第6期23卷 1864-1878页

作者： Jianjun Wang Yanan Shao Xin Yang chi Zhang Yuan Guo Zijin Liu Mingxun chen State Key Laboratory of Crop Stress Biology for Arid Areas/National Yangling Agricultural Biotechnology&Breeding Center/Shaanxi Key Laboratory of Crop Heterosis/College of Agronomy Northwest A&F UniversityYangling 712100China

Flax(Linum usitatissimum L.)is a versatile crop and its seeds are a major source of unsaturated fatty acids.Stearoyl-acyl carrier protein desaturase(SAD)is a dehydrogenase enzyme that plays a key role in oleic acid biosynthesis as well as responses to biotic and abiotic stresses.However,the function of SAD orthologs from L.usitatissimum has not been assessed.Here,we found that two LuSAD genes,LuSAD1 and LuSAD2,are present in the genome of L.usitatissimum cultivar‘Longya 10’.Heterogeneous expression of either LuSAD1 or LuSAD2 in Arabidopsis thaliana resulted in higher contents of total fatty acids and oleic acid in the seeds.Interestingly,ectopic expression of LuSAD2 in A.thaliana caused altered plant architecture.Similarly,the overexpression of either LuSAD1 or LuSAD2 in Brassica napus also resulted in increased contents of total fatty acids and oleic acid in the seeds.Furthermore,we demonstrated that either LuSAD1 or LuSAD2 enhances seedling resistance to cold and drought stresses by improving antioxidant enzyme activity and nonenzymatic antioxidant levels,as well as reducing membrane damage.These findings not only broaden our knowledge of the LuSAD functions in plants,but also offer promising targets for improving the quantity and quality of oil,and the abiotic stress tolerance of oil-producing crops,through molecular manipulation.

关键词： LuSAD oleic acid cold tolerance drought tolerance Linum usitatissimum Brassica napus

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