Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water...Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water.Herein,a sandwich composite structure(designed as MS-Mo2C@NCNS)ofβ-Mo2C hollow nanotubes(HNT)and N-doped carbon nanosheets(NCNS)is designed and prepared using a binary NaCl–KCl molten salt(MS)strategy for HER.The temperature-dominant Kirkendall formation mechanism is tentatively proposed for such a three-dimensional hierarchical framework.Due to its attractive structure and componential synergism,MS-Mo2C@NCNS exposes more effective active sites,confers robust structural stability,and shows significant electrocatalytic activity/stability in HER,with a current density of 10 mA cm-2 and an overpotential of only 98 mV in 1 M KOH.Density functional theory calculations point to the synergistic effect of Mo2C HNT and NCNS,leading to enhanced electronic transport and suitable adsorption free energies of H*(ΔGH*)on the surface of electroactive Mo2C.More significantly,the MS-assisted synthetic methodology here provides an enormous perspective for the commercial development of highly active non-noble metal electrocatalysts toward efficient hydrogen evolution.展开更多
The sea star Asterias amurensis is widely viewed as a severe“marine pest”because of its broad feeding habits.Over the past few decades,A.amurensis undergoes massive and sporadic population outbreaks worldwide,causin...The sea star Asterias amurensis is widely viewed as a severe“marine pest”because of its broad feeding habits.Over the past few decades,A.amurensis undergoes massive and sporadic population outbreaks worldwide,causing extensive economic and ecological losses to the local aquaculture industry and marine ecosystem.Understanding the genetic diversity and population structure of A.amurensis can provide vital information for resource management.By analyzing the polymorphism of the mitochondrial cytochrome C oxidase subunit I(COI)gene and ten simple sequence repeat(SSR)microsatellites markers,the genetic diversity and population structure of A.amurensis of four populations along the northern coast of China was uncovered.A total of 36 haplotypes were identified,and a main haplotype was found in four populations.The Qingdao(QD)population displayed the highest genetic diversity among all the populations.The AMOVA and pairwise F_(st)showed that there was small but statistically significant population differentiation among the four populations,especially between QD and Weihai(WH).Moreover,the principal component analysis(PCA)and admixture analysis showed that several individuals in Yantai(YT)and Dalian(DL)had little genetic association with other individuals.Overall,this study provided useful information of the genetic diversity and population structure of A.amurensis and will contribute to the resource management of A.amurensis in China.展开更多
A brief review and analysis of two historical models of the electron, the charged spinning sphere and Goudsmit and Uhlenbeck’s concept, is presented. It is shown that the enormous potential of classical electrodynami...A brief review and analysis of two historical models of the electron, the charged spinning sphere and Goudsmit and Uhlenbeck’s concept, is presented. It is shown that the enormous potential of classical electrodynamics has been underutilized in particle physics. Such observation leads to discovery of a principal component in the electron inner structure—the charged c-ring. The intrinsic (fundamental) electron model based on the charged c-ring successfully explains the ontology of the charge fractionation in quantum chromodynamics and the formation of Cooper pairs in superconductivity. The c-ring properties are explained on the basis of the General Compton Conditions as defined. Properties of the charged c-ring include the explanation of the boundary conditions, electro-magnetostatic field configuration, self-mass, spin, magnetic moment, and the gyromagnetic ratio. The self-mass of the intrinsic electron is 100% electro-magnetostatic and it is shown how to compute its value. The classical-quantum divide no longer exists. Relation between the intrinsic electron and the electron is fundamentally defined. The electron is the composite fermion consisting of the intrinsic electron and the neutrino. The ontology of the anomaly in the electron magnetic moment is demonstrated—it is due to the addition of the neutrino magnetic moment to the overall electron magnetic moment. The intrinsic electron replaces the W? boson in particle physics, resulting in a fundamental implication for the Standard Model.展开更多
This paper investigates the application of active mass dampers to mitigate the vibrations of building structures subjected to unknown external excitations under controller saturation conditions. By utilizing an H<s...This paper investigates the application of active mass dampers to mitigate the vibrations of building structures subjected to unknown external excitations under controller saturation conditions. By utilizing an H<sub>∞</sub> control strategy, the optimal state feedback controller is derived by solving the linear matrix inequality problem for controller saturation. Case studies show that the proposed controller is capable of stabilizing the closed-loop system with good control performance and effectively suppressing vibrations in building structures under unknown external excitation. When compared to controllers that do not consider saturation, the proposed controller requires lower gain and results in reduced energy consumption. The research findings provide valuable insights for addressing real-world building structure control problems, contributing to both theoretical significance and practical applications.展开更多
The quantum field theory (QFT) is one of branches of the Standard Model. According to QFT, quantum fields are the primary entities and particles are the excitations of these fields, coming in discrete lumps with no in...The quantum field theory (QFT) is one of branches of the Standard Model. According to QFT, quantum fields are the primary entities and particles are the excitations of these fields, coming in discrete lumps with no inner structures and with properties assigned by declaration. Such view is in conflict with the observed vacuum energy density, 140 orders of magnitudes less than required by the QFT. In addition, such view is challenged by Aphysical Quantum Mechanics (AQM), a deeper quantum theory. According to AQM, the fundamental understanding of quantum reality is expanded by the addition of two fundamental categories, aphysical and elementary consciousness of elementary particles. Based on AQM and as an example, the total ontology of the intrinsic (fundamental) electron is presented with its inner structure of perfect geometry consisting of the physical charged c-ring and aphysical cylinder, and with its properties such as self-mass, spin, magneto-electrostatic field configuration and magnetic moment. The position parameter in the inner structure demonstrates that there are no two identical intrinsic electrons in the Universe thus placing a question mark over the QFT principle of indistinguishability.展开更多
饱和的碳氢键氧化是合成化学和化学工业中一类重要的化学反应.然而,饱和C(sp^(3))−H键离解能(BDEs)较高、极性较弱,导致了底物难以活化和催化转化效率较低等问题.在过去的几十年,C(sp^(3))−H键的定向活化转化取得了重要的进展.其中,关于...饱和的碳氢键氧化是合成化学和化学工业中一类重要的化学反应.然而,饱和C(sp^(3))−H键离解能(BDEs)较高、极性较弱,导致了底物难以活化和催化转化效率较低等问题.在过去的几十年,C(sp^(3))−H键的定向活化转化取得了重要的进展.其中,关于C(sp^(3))−H键催化氧化的研究主要涉及一些键能低的、预活化的C−H键,包括苄基型、亚甲基型、脂肪族X−CH_(2)(X=O,N)和甲苯等,含有未活化C(sp^(3))−H键的复杂化合物的选择性氧化仍具有挑战性.例如,芳基醚C(sp^(3))−H键功能化通常采用计量的过氧化物氧化剂,或者通过单电子氧化和碱促进的去质子化进一步构建C−C/C−N键,产物选择性较低,也带来了一些不利的环境影响.因此,有必要开发高效、温和的芳基醚C(sp^(3))−H键选择氧化方法,并将其应用于有机合成和药物开发.近年来,光催化C(sp^(3))−H键氧化因其操作简便、氧化还原中性等优点,已发展成为一种有用且多样的催化研究工具.本文发展了一种利用氧气作为氧化剂,在可见光驱动下选择性地将芳基醚C(sp^(3))−H键氧化成为甲酸苯酯类产物的新方法.使用Mes-10-phenyl-Acr^(+)−BF_(4)^(-)光催化剂,高效活化多种氯源(如盐酸、无机氯盐和有机氯化物)得到氯自由基,由于其具有较高的氧化能力(+2.03 V vs.SCE)和对氢原子的亲和力,能够通过氢原子转移过程活化芳基醚C(sp^(3))−键,攫取氢自由基得到相应的烷基碳自由基(•CH_(2)OPh)中间体,进一步被分子氧选择氧化得到酯类目标产物.研究结果表明,多种链状芳基醚和不同取代(如给电子基和吸电子基)芳基醚均可发生氧化反应,高收率地合成了一系列官能团丰富的甲酸苯酯类化合物.本文方法具有反应条件温和、操作简单、官能团耐受性好以及可规模化放大等优点,并且少量的水对反应没有明显影响.机理实验研究结果表明,芳基醚C(sp^(3))−H键的断裂是反应过程的决速步骤.紫外可见吸收光谱结果表明,氯离子与催化剂之间的相互作用强于底物,并且自由基捕获实验证实反应体系中存在氯自由基和烷基碳自由基物种,表明反应经历自由基路径.此外,电子顺磁共振测试结果表明,反应过程中存在单线态氧物种,可能是激发态的光催化剂直接与氧气发生能量转移得到;同位素实验(18O)揭示了甲酸苯酯类化合物氧的来源.综上,本文实现了温和条件下光催化芳基醚C(sp^(3))−H键选择氧化反应,高收率合成了一系列甲酸苯酯类化合物.该方法避免了化学计量的过氧化物和碱等添加剂的使用以及底物的过度氧化,阐明了催化反应机制,为其他醚类化合物的C(sp^(3))−H键氧化功能化提供了新思路,为后续化学合成和药物开发提供了参考和启示.展开更多
目的研究交趾黄檀Dalbergia cochinchinensis Pierre ex Laness的新黄酮类成分及其抗H9c2心肌细胞缺氧/复氧损伤活性。方法交趾黄檀70%乙醇提取物采用硅胶、Sephadex LH-20、反相制备HPLC进行分离纯化,根据理化性质及波谱数据鉴定所得...目的研究交趾黄檀Dalbergia cochinchinensis Pierre ex Laness的新黄酮类成分及其抗H9c2心肌细胞缺氧/复氧损伤活性。方法交趾黄檀70%乙醇提取物采用硅胶、Sephadex LH-20、反相制备HPLC进行分离纯化,根据理化性质及波谱数据鉴定所得化合物的结构。采用CCK-8法检测其对H9c2心肌细胞的活性及对H9c2细胞缺氧/复氧损伤的保护作用,并分析其构效关系。结果从中分离得到12个化合物,分别鉴定为阔叶黄檀酚(1)、5-O-methyllatifolin(2)、mimosifoliol(3)、5-O-methydalbergiphenol(4)、dalbergiphenol(5)、cearoin(6)、2,4-dihydroxy-5-methoxy-benzophenone(7)、2-hydroxy-4,5-dimethoxybenzophenone(8)、melannoin(9)、2,2′,5-trihydroxy-4-methoxybenzophenone(10)、黄檀素(11)、4-甲氧基黄檀醌(12)。黄檀酚及黄檀内酯类化合物对H9c2细胞毒性较小,黄檀酚类化合物抗H9c2心肌细胞缺氧/复氧损伤活性较强。结论化合物8为新天然产物,化合物4、9为首次从该植物中分离得到。黄檀酚类化合物可能是抗H9c2细胞缺氧/复氧损伤的主要新黄酮类成分。展开更多
Non-alcoholic fatty liver disease(NAFLD)is associated with mutations in lipopolysaccharide-binding protein(LBP),but the underlying epigenetic mechanisms remain understudied.Herein,LBP^(-/-)rats with NAFLD were establi...Non-alcoholic fatty liver disease(NAFLD)is associated with mutations in lipopolysaccharide-binding protein(LBP),but the underlying epigenetic mechanisms remain understudied.Herein,LBP^(-/-)rats with NAFLD were established and used to conduct integrative targetingactive enhancer histone H3 lysine 27 acetylation(H3K27ac)chromatin immunoprecipitation coupled with high-throughput and transcriptomic sequencing analysis to explore the potential epigenetic pathomechanisms of active enhancers of NAFLD exacerbation upon LBP deficiency.Notably,LBP^(-/-)reduced the inflammatory response but markedly aggravated high-fat diet(HFD)-induced NAFLD in rats,with pronounced alterations in the histone acetylome and regulatory transcriptome.In total,1128 differential enhancer-target genes significantly enriched in cholesterol and fatty acid metabolism were identified between wild-type(WT)and LBP^(-/-)NAFLD rats.Based on integrative analysis,CCAAT/enhancer-binding proteinβ(C/EBPβ)was identified as a pivotal transcription factor(TF)and contributor to dysregulated histone acetylome H3K27ac,and the lipid metabolism gene SCD was identified as a downstream effector exacerbating NAFLD.This study not only broadens our understanding of the essential role of LBP in the pathogenesis of NAFLD from an epigenetics perspective but also identifies key TF C/EBPβand functional gene SCD as potential regulators and therapeutic targets.展开更多
基金the National Natural Science Foundation of China(Nos.52072151,52171211,52102253,52271218,U22A20145)the Jinan Independent Innovative Team(2020GXRC015)+1 种基金the Major Program of Shandong Province Natural Science Foundation(ZR2021ZD05)the Science and Technology Program of University of Jinan(XKY2119).
文摘Focused exploration of earth-abundant and cost-efficient non-noble metal electrocatalysts with superior hydrogen evolution reaction(HER)performance is very important for large-scale and efficient electrolysis of water.Herein,a sandwich composite structure(designed as MS-Mo2C@NCNS)ofβ-Mo2C hollow nanotubes(HNT)and N-doped carbon nanosheets(NCNS)is designed and prepared using a binary NaCl–KCl molten salt(MS)strategy for HER.The temperature-dominant Kirkendall formation mechanism is tentatively proposed for such a three-dimensional hierarchical framework.Due to its attractive structure and componential synergism,MS-Mo2C@NCNS exposes more effective active sites,confers robust structural stability,and shows significant electrocatalytic activity/stability in HER,with a current density of 10 mA cm-2 and an overpotential of only 98 mV in 1 M KOH.Density functional theory calculations point to the synergistic effect of Mo2C HNT and NCNS,leading to enhanced electronic transport and suitable adsorption free energies of H*(ΔGH*)on the surface of electroactive Mo2C.More significantly,the MS-assisted synthetic methodology here provides an enormous perspective for the commercial development of highly active non-noble metal electrocatalysts toward efficient hydrogen evolution.
基金Supported by the International Science Partnership Program of the Chinese Academy of Sciences(No.133137KYSB20200002)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA23050304)the Natural Science Foundation of Shandong Province(Nos.ZR2021MC151,ZR2021QD158)。
文摘The sea star Asterias amurensis is widely viewed as a severe“marine pest”because of its broad feeding habits.Over the past few decades,A.amurensis undergoes massive and sporadic population outbreaks worldwide,causing extensive economic and ecological losses to the local aquaculture industry and marine ecosystem.Understanding the genetic diversity and population structure of A.amurensis can provide vital information for resource management.By analyzing the polymorphism of the mitochondrial cytochrome C oxidase subunit I(COI)gene and ten simple sequence repeat(SSR)microsatellites markers,the genetic diversity and population structure of A.amurensis of four populations along the northern coast of China was uncovered.A total of 36 haplotypes were identified,and a main haplotype was found in four populations.The Qingdao(QD)population displayed the highest genetic diversity among all the populations.The AMOVA and pairwise F_(st)showed that there was small but statistically significant population differentiation among the four populations,especially between QD and Weihai(WH).Moreover,the principal component analysis(PCA)and admixture analysis showed that several individuals in Yantai(YT)and Dalian(DL)had little genetic association with other individuals.Overall,this study provided useful information of the genetic diversity and population structure of A.amurensis and will contribute to the resource management of A.amurensis in China.
文摘A brief review and analysis of two historical models of the electron, the charged spinning sphere and Goudsmit and Uhlenbeck’s concept, is presented. It is shown that the enormous potential of classical electrodynamics has been underutilized in particle physics. Such observation leads to discovery of a principal component in the electron inner structure—the charged c-ring. The intrinsic (fundamental) electron model based on the charged c-ring successfully explains the ontology of the charge fractionation in quantum chromodynamics and the formation of Cooper pairs in superconductivity. The c-ring properties are explained on the basis of the General Compton Conditions as defined. Properties of the charged c-ring include the explanation of the boundary conditions, electro-magnetostatic field configuration, self-mass, spin, magnetic moment, and the gyromagnetic ratio. The self-mass of the intrinsic electron is 100% electro-magnetostatic and it is shown how to compute its value. The classical-quantum divide no longer exists. Relation between the intrinsic electron and the electron is fundamentally defined. The electron is the composite fermion consisting of the intrinsic electron and the neutrino. The ontology of the anomaly in the electron magnetic moment is demonstrated—it is due to the addition of the neutrino magnetic moment to the overall electron magnetic moment. The intrinsic electron replaces the W? boson in particle physics, resulting in a fundamental implication for the Standard Model.
文摘This paper investigates the application of active mass dampers to mitigate the vibrations of building structures subjected to unknown external excitations under controller saturation conditions. By utilizing an H<sub>∞</sub> control strategy, the optimal state feedback controller is derived by solving the linear matrix inequality problem for controller saturation. Case studies show that the proposed controller is capable of stabilizing the closed-loop system with good control performance and effectively suppressing vibrations in building structures under unknown external excitation. When compared to controllers that do not consider saturation, the proposed controller requires lower gain and results in reduced energy consumption. The research findings provide valuable insights for addressing real-world building structure control problems, contributing to both theoretical significance and practical applications.
文摘The quantum field theory (QFT) is one of branches of the Standard Model. According to QFT, quantum fields are the primary entities and particles are the excitations of these fields, coming in discrete lumps with no inner structures and with properties assigned by declaration. Such view is in conflict with the observed vacuum energy density, 140 orders of magnitudes less than required by the QFT. In addition, such view is challenged by Aphysical Quantum Mechanics (AQM), a deeper quantum theory. According to AQM, the fundamental understanding of quantum reality is expanded by the addition of two fundamental categories, aphysical and elementary consciousness of elementary particles. Based on AQM and as an example, the total ontology of the intrinsic (fundamental) electron is presented with its inner structure of perfect geometry consisting of the physical charged c-ring and aphysical cylinder, and with its properties such as self-mass, spin, magneto-electrostatic field configuration and magnetic moment. The position parameter in the inner structure demonstrates that there are no two identical intrinsic electrons in the Universe thus placing a question mark over the QFT principle of indistinguishability.
文摘饱和的碳氢键氧化是合成化学和化学工业中一类重要的化学反应.然而,饱和C(sp^(3))−H键离解能(BDEs)较高、极性较弱,导致了底物难以活化和催化转化效率较低等问题.在过去的几十年,C(sp^(3))−H键的定向活化转化取得了重要的进展.其中,关于C(sp^(3))−H键催化氧化的研究主要涉及一些键能低的、预活化的C−H键,包括苄基型、亚甲基型、脂肪族X−CH_(2)(X=O,N)和甲苯等,含有未活化C(sp^(3))−H键的复杂化合物的选择性氧化仍具有挑战性.例如,芳基醚C(sp^(3))−H键功能化通常采用计量的过氧化物氧化剂,或者通过单电子氧化和碱促进的去质子化进一步构建C−C/C−N键,产物选择性较低,也带来了一些不利的环境影响.因此,有必要开发高效、温和的芳基醚C(sp^(3))−H键选择氧化方法,并将其应用于有机合成和药物开发.近年来,光催化C(sp^(3))−H键氧化因其操作简便、氧化还原中性等优点,已发展成为一种有用且多样的催化研究工具.本文发展了一种利用氧气作为氧化剂,在可见光驱动下选择性地将芳基醚C(sp^(3))−H键氧化成为甲酸苯酯类产物的新方法.使用Mes-10-phenyl-Acr^(+)−BF_(4)^(-)光催化剂,高效活化多种氯源(如盐酸、无机氯盐和有机氯化物)得到氯自由基,由于其具有较高的氧化能力(+2.03 V vs.SCE)和对氢原子的亲和力,能够通过氢原子转移过程活化芳基醚C(sp^(3))−键,攫取氢自由基得到相应的烷基碳自由基(•CH_(2)OPh)中间体,进一步被分子氧选择氧化得到酯类目标产物.研究结果表明,多种链状芳基醚和不同取代(如给电子基和吸电子基)芳基醚均可发生氧化反应,高收率地合成了一系列官能团丰富的甲酸苯酯类化合物.本文方法具有反应条件温和、操作简单、官能团耐受性好以及可规模化放大等优点,并且少量的水对反应没有明显影响.机理实验研究结果表明,芳基醚C(sp^(3))−H键的断裂是反应过程的决速步骤.紫外可见吸收光谱结果表明,氯离子与催化剂之间的相互作用强于底物,并且自由基捕获实验证实反应体系中存在氯自由基和烷基碳自由基物种,表明反应经历自由基路径.此外,电子顺磁共振测试结果表明,反应过程中存在单线态氧物种,可能是激发态的光催化剂直接与氧气发生能量转移得到;同位素实验(18O)揭示了甲酸苯酯类化合物氧的来源.综上,本文实现了温和条件下光催化芳基醚C(sp^(3))−H键选择氧化反应,高收率合成了一系列甲酸苯酯类化合物.该方法避免了化学计量的过氧化物和碱等添加剂的使用以及底物的过度氧化,阐明了催化反应机制,为其他醚类化合物的C(sp^(3))−H键氧化功能化提供了新思路,为后续化学合成和药物开发提供了参考和启示.
文摘目的研究交趾黄檀Dalbergia cochinchinensis Pierre ex Laness的新黄酮类成分及其抗H9c2心肌细胞缺氧/复氧损伤活性。方法交趾黄檀70%乙醇提取物采用硅胶、Sephadex LH-20、反相制备HPLC进行分离纯化,根据理化性质及波谱数据鉴定所得化合物的结构。采用CCK-8法检测其对H9c2心肌细胞的活性及对H9c2细胞缺氧/复氧损伤的保护作用,并分析其构效关系。结果从中分离得到12个化合物,分别鉴定为阔叶黄檀酚(1)、5-O-methyllatifolin(2)、mimosifoliol(3)、5-O-methydalbergiphenol(4)、dalbergiphenol(5)、cearoin(6)、2,4-dihydroxy-5-methoxy-benzophenone(7)、2-hydroxy-4,5-dimethoxybenzophenone(8)、melannoin(9)、2,2′,5-trihydroxy-4-methoxybenzophenone(10)、黄檀素(11)、4-甲氧基黄檀醌(12)。黄檀酚及黄檀内酯类化合物对H9c2细胞毒性较小,黄檀酚类化合物抗H9c2心肌细胞缺氧/复氧损伤活性较强。结论化合物8为新天然产物,化合物4、9为首次从该植物中分离得到。黄檀酚类化合物可能是抗H9c2细胞缺氧/复氧损伤的主要新黄酮类成分。
基金supported by the National Natural Science Foundation of China(81971875,82300661)Natural Science Foundation of Anhui province(2308085QH246)+3 种基金Natural Science Foundation of the Anhui Higher Education Institutions(KJ2021A0205)Basic and Clinical Cooperative Research Program of Anhui Medical University(2019xkjT002,2019xkjT022,2022xkjT013)Talent Training Program,School of Basic Medical Sciences,Anhui Medical University(2022YPJH102)National College Students Innovation and Entrepreneurship Training Program of China(202210366024)。
文摘Non-alcoholic fatty liver disease(NAFLD)is associated with mutations in lipopolysaccharide-binding protein(LBP),but the underlying epigenetic mechanisms remain understudied.Herein,LBP^(-/-)rats with NAFLD were established and used to conduct integrative targetingactive enhancer histone H3 lysine 27 acetylation(H3K27ac)chromatin immunoprecipitation coupled with high-throughput and transcriptomic sequencing analysis to explore the potential epigenetic pathomechanisms of active enhancers of NAFLD exacerbation upon LBP deficiency.Notably,LBP^(-/-)reduced the inflammatory response but markedly aggravated high-fat diet(HFD)-induced NAFLD in rats,with pronounced alterations in the histone acetylome and regulatory transcriptome.In total,1128 differential enhancer-target genes significantly enriched in cholesterol and fatty acid metabolism were identified between wild-type(WT)and LBP^(-/-)NAFLD rats.Based on integrative analysis,CCAAT/enhancer-binding proteinβ(C/EBPβ)was identified as a pivotal transcription factor(TF)and contributor to dysregulated histone acetylome H3K27ac,and the lipid metabolism gene SCD was identified as a downstream effector exacerbating NAFLD.This study not only broadens our understanding of the essential role of LBP in the pathogenesis of NAFLD from an epigenetics perspective but also identifies key TF C/EBPβand functional gene SCD as potential regulators and therapeutic targets.
