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Switching O-O bond formation mechanism between WNA and I2M pathways by modifying the Ru-bda backbone ligands of water-oxidation catalysts

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journal of Energy Chemistry 2021年第3期30卷 815-821页

作者： Biaobiao Zhang Shaoqi Zhan Tianqi Liu Linqin Wang A.Ken Inge Lele Duan Brian j.j.Timmer Oleksandr Kravchenko Fei Li Marten S.G.Ahlquist Licheng Sun Department of Chemistry KTH Royal Institute of Technology10044 StockholmSweden Department of Theoretical Chemistry&Biology School of Engineering Sciences in Chemistry Biotechnology and HealthKTH Royal Institute of Technology10691 StockholmSweden Department of Materials and Environmental Chemistry Stockholm University10691 StockholmSweden Department of Chemistry Southern University of Science and Technology(SUSTech)Shenzhen 518055GuangdongChina State Key Laboratory of Fine Chemicals Institute of Artificial PhotosynthesisDUT–KTH Joint Education and Research Center on Molecular DevicesDalian University of Technology(DUT)Dalian 116024LiaoningChina

Understanding the seven coordination and O-O coupling pathway of the distinguished Ru-bda catalysts is essential for the development of next generation efficient water-oxidation catalysts based on earthabundant *** work reports the synthesis,characterization and catalytic properties of a monomeric ruthenium catalyst Ru-bnda(H2 bnda=2,2’-bi(nicotinic acid)-6,6’-dicarboxylic acid)featuring steric hindrance and enhanced hydrophilicity on the *** experimental evidence with systematic density functional theory calculations on the Ru-bnda and related catalysts Ru-bda(H_(2)bda=2,2’-bipyridine-6,6’-dicarboxylic acid),Ru-pda(H_(2)pda=1,10-phenanthroline-2,9-dicarboxylic acid),and Ru-biqa(H_(2)biqa=(1,1’-biisoquinoline)-3,3’-dicarboxylic acid),we emphasized that seven coordination clearly determines presence of Ru^(Ⅴ)=O with high spin density on the ORu^(Ⅴ)=O atom,*** with radical properties,which is one of the necessary conditions for reacting through the O-O coupling ***,an additional factor to make the condition sufficient is the favorable intermolecular faceto-face interaction for the generation of the pre-reactive[Ru^(Ⅴ)=O…O=Ru^(Ⅴ)],which may be significantly influenced by the secondary coordination *** work provides a new understanding of the structure-activity relationship of water-oxidation catalysts and their potential to adopt I2M pathway for O-O bond formation.

关键词： Water oxidation Oxygen evolution Ruthenium O-O bond formation

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Creatine supplementation in exercised rats: Effects on the aerobic capacity

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Open journal of Animal Sciences 2013年第1期3卷 21-26页

作者： Michel Barbosa de Araújo Roberto C. Vieira junior Leandro P. Moura Marcelo Costa junior Rodrigo A. Dalia Amanda Christine da Silva Sponton Carla Ribeiro Maria alice R. Mello Biosciences Institute Department of Physical Education Universidade Estadual Paulista Júlio de Mesquita Filho Rio Claro Brazil Biosciences Institute Department of Physical Education Universidade Estadual Paulista Júlio de Mesquita Filho Rio Claro Brazil Faculty of Nutrition Universidade Federal de Mato Grosso Cuiabá Brazil

This study aimed to analyze the possible metabolic disturbances caused by creatine supplementation on aerobic capacity of rats, inferred by the maximal lactate steady state. Forty male Wistar rats (90 days old) were distributed into two groups for eight weeks: trained group (T): rats that were submitted to a training protocol, and supplemented-trained group (TCr): rats that were submitted to a training protocol and received balanced diet supplemented with 2% creatine. The blood lactate concentrations equivalent to maximal lactate steady state during treadmill running were analyzed at the beginning and also at the end of the experiment. At the end of the experiment were done comparing the test results MLSS between the two groups. At the beginning of the experiment, prior to groups division, the majority of animals obtained MLSS at a speed of26 m/min, blood lactate concentration of 3.79 ± 0.76 mmol/L. At the end of the experiment, most of trained rats in T presented MLSS at the speed of28 m/min, blood lactate concentration of 3.37 ± 0.68 mmol/L. Most TCr had MLSS at the speed of28 m/min, blood lactate concentration of 3.52 ± 0.69 mmol/L. We conclude that creatine supplementation was not the cause of the improvement in the aerobic capacity of rats in the tread-mill exercise.

关键词： Diet Lactate Maximal Lactate Steady State Treadmill Running

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Prevalence of intestinal schistosomiasis in pre-school aged children: a pilot survey in Marolambo District, Madagascar

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Infectious Diseases of Poverty 2021年第3期10卷 124-124页

作者： Caitlin Sheehy Heather Lawson Emmanuel H.Andriamasy Hannah j.Russell alice Reid Gina U.Raderalazasoa Graham Dodge Robbie Kornitschky james M.StjPenney Tahiry N.Ranaivoson Antsa Andria niaina jenny S.Emmanoela Amaya L.Bustinduy jRussell Stothard Louis Andrianjaka Stephen A.Spencer The University of Man Chester Medical School University of Man ChesterManchester M139NTUK 不详

School-aged children(SAC)have a considerable burden of intestinal schistosomiasis in Madagascar yet its burden in pre-school aged children(PSAC)is currently *** assess the at-risk status of PSAC,we undertook a pilot epidemiological survey in june 2019 examining children(n=89),aged 2-4-years of balanced gender,in six remote villages in Marolambo District,*** included use of urine-circulating cathodic antigen(CCA)dipsticks and coproscopy of stool with duplicate Kato-Katz(K-K)thick smears.

关键词： Schistosoma mansoni Soil-transmitted helminthiasis Paediatric Praziquantel Mass drug administration

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Efects of topographic variability and forest attributes on fne-scale soil fertility in late-secondary succession of Atlantic Forest

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Ecological Processes 2021年第1期10卷 853-861页

作者： alice Cristina Rodrigues Pedro Manuel Villa Walnir Gomes Ferreira‑júnior Carlos Ernesto RGSchaefer Andreza Viana Neri Laboratory of Ecology and Evolution of Plants‑LEEP Departamento de Biologia VegetalPrograma de Pós-Graduação em Botânica-Universidade Federal de ViçosaViçosaMinas Gerais CEP:36570‑900Brazil. Fundación Para la Conservación de la Biodiversidad MéridaEstado Mérida CEP 5101Venezuela. Departamento de Engenharia Florestal Universidade Federal de ViçosaViçosaMinas Gerais CEP:36570‑900Brazil. Laboratório de Botânica eEcologia Setor de Biologia e Meio AmbienteInstituto Federal do Sul de Minas Gerais(IFSULDEMINAS)Campus MachadoRodovia Machado‑Paraguaçukm 3MachadoMinas Gerais CEP 37750‑000Brazil. Departamento de Solos Universidade Federal de ViçosaViçosaMinas Gerais CEP:36570‑900Brazil.

Background:Understanding how soil fertility changes due to topographical conditions and forest attributes is an essential premise for local-scale forest management *** evaluated the efects of topographic variables and forest attributes on soil fertility along a local topographical gradient in a Brazilian Atlantic *** hypothesised that soil fertility is positively afected by topographic variability and forest attributes(structure and diversity).We used tree species richness,composition,abundance,and aboveground biomass as forest *** analysed two 1-ha for‑est patches with contrasting topographical *** used diferent linear mixed efects models(LMMs)to test the main efects of diferent forest attributes and topography variables on soil ***:The results showed that higher topographic variability determines soil fertility along a fne-scale *** frst two axes of the PCA explained 66.8%of the variation in soil data,with the frst axis(PCA_(1))explaining 49.6%of the variation in soil data and positively correlating with fertility-related soil *** second axis(PCA_(2))explained 17.2%of the variation in topographical data and positively correlated with convexity(the elevation of a plot minus the average elevation of all immediate neighbour plots)and *** best models showed that topo‑graphic variables(elevation and convexity)are the main predictors that afect fne-scale soil ***:Our study demonstrates that the topographic variability,mainly elevation and convexity,determines fne-scale soil fertility in an Atlantic *** results advance our understanding that context-dependent condi‑tions based on topography and soil properties have a high variability at a fne scale,which can infuence variations in forest attributes(i.e.,species distribution,diversity and structure of tree communities).In addition,the information generated in this research may be important for planning forest restorat

关键词： Convexity Soil variability Succession Topographical gradient Tropical forests

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p53 as a hub in cellular redox regulation and therapeutic target in cancer

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journal of Molecular Cell Biology 2019年第4期11卷 330-341页

作者： Sofi E.Eriksson Sophia Ceder Vladimir j.N.Bykov Klas G.Wiman Karolinska Institutet Department of Oncology-Pathology BioClinicum Stockholm Sweden

The TP53 tumor suppressor gene encodes a DNA-binding transcription factor that regulates multiple cellular processes including cell growth and cell death. The ability of p53 to bind to DNA and activate transcription is tightly regulated by post-translational modifications and is dependent on a reducing cellular environment. Some p53 transcriptional target genes are involved in regulation of the cellular redox homeostasis, e.g. TIGAR and GLS2. A large fraction of human tumors carry TP53 mutations, most commonly missense mutations that lead to single amino acid substitutions in the core domain. Mutant p53 proteins can acquire so called gain-of-function activities and influence the cellular redox balance in various ways, for instance by binding of the Nrf2 transcription factor, a major regulator of cellular redox state. The DNA-binding core domain of p53 has 10 cysteine residues, three of which participate in holding a zinc atom that is critical for p53 structure and function. Several novel compounds that refold and reactivate missense mutant p53 bind to specific p53 cysteine residues. These compounds can also react with other thiols and target components of the cellular redox system, such as glutathione. Dual targeting of mutant p53 and redox homeostasis may allow more efficient treatment of cancer.

关键词： p53 redox regulation mutation oxidative stress Nrf2 thiols cancer therapy

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Predictive factors for survival and score application in liver retransplantation for hepatitis C recurrence

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World journal of Gastroenterology 2016年第18期22卷 4547-4558页

作者： alice Tung Wan Song Rodolphe Sobesky Carmen Vinaixa jérome Dumortier Sylvie Radenne Francois Durand Yvon Calmus Géraldine Rousseau Marianne Latournerie Cyrille Feray Valérie Delvart Bruno Roche Stéphanie Haim-Boukobza Anne-Marie Roque-Afonso Denis Castaing Edson Abdala Luiz Augusto Carneiro D’Albuquerque jean-Charles Duclos-Vallée Marina Berenguer Didier Samuel INSERM Unit 785 Villejuif 94800France Liver and Digestive Organ Transplantation Division Gastroenterology DepartmentUniversity of Sao Paulo Medical SchoolSao Paulo 05403-900Brazil Universite Paris-Sud Villejuif 94800France Liver Transplantation Laboratory LIM-37 Sao Paulo 01246-903Brazil AP-HP Hopital Paul Brousse Villejuif 94800France La Fe Hospital University of Valencia and CiberehdValencia 46026Spain Hopital Edouard Herriot Lyon 69003France Hopital Croix Rousse Lyon 69004France AP-HP Hopital Beaujon Clichy 92110France AP-HP Hopital St Antoine Paris 75011France AP-HP Hopital Salpetriere Paris 75013France CHU Pontchaillou Rennes 35000France AP-HP Hopital Henri Mondor Creteil 94010France Viral Hepatitis Laboratory LIM-47 Sao Paulo 01246-903Brazil

AIM: To identify risk factors associated with survival in patients retransplanted for hepatitis C virus(HCV) recurrence and to apply a survival score to this ***: We retrospectively identified 108 patients retransplanted for HCV recurrence in eight European liver transplantation centers(seven in France, one in Spain). Data collection comprised clinical and laboratory variables, including virological and antiviral treatment data. We then analyzed the factors associated with survival in this population. A recently published score that predicts survival in retransplantation in patients with hepatitis C was applied. Because there are currently no uniform recommendations regarding selection of the best candidates for retransplantation in this setting, we also described the clinical characteristics of 164 patients not retransplanted, with F3, F4, or fibrosing cholestatic hepatitis(FCH) post-first graft presenting with hepatic decompensation. RESULTS: Overall retransplantation patient survival rates were 55%, 47%, and 43% at 3, 5, and 10 years, respectively. Patients who were retransplanted for advanced cirrhosis had survival rates of 59%, 52%, and 49% at 3, 5, and 10 years, while those retransplanted for FCH had survival rates of 34%, 29%, and 11%, respectively. Under multivariate analysis, and adjusting for the center effect and the occurrence of FCH, factors associated with better survival after retransplantation were: negative HCV viremia before retransplantation, antiviral therapy after retransplantation, non-genotype 1, a Model for End-stage Liver Disease(MELD) score < 25 when replaced on the waiting list, and a retransplantation donor age < 60 years. Although the numbers were small, in the context of the new antivirals era, we showed that outcomes in patientswho underwent retransplantation with undetectable HCV viremia did not depend on donor age and MELD score. The Andrés score was applied to 102 patients for whom all score variables were available,

关键词： Antivirals Hepatitis C Mortality Prognosis Retransplantation Risk factors

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When will it end? Long-lived intracontinental reactivation in central Australia

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Geoscience Frontiers 2019年第1期10卷 149-164页

作者： Raphael Quentin de Gromard Christopher L.Kirkland Heather M.Howard Michael T.D.Wingate Fred jourdan Brent I.A.Mc Innes Martin Danisik Noreen j.Evans Bradley j.McDonald R.Hugh Smithies Geological Survey of Western Australia Department of Mines Industry Regulation and Safety School of Earth and Planetary Science/john de Laeter Centre/TIGeR Curtin University

The post-Mesoproterozoic tectonometamorphic history of the Musgrave Province, central Australia, has previously been solely attributed to intracontinental compressional deformation during the 580 -520 Ma Petermann Orogeny. However, our new structurally controlled multi-mineral geochronology results,from two north-trending transects, indicate protracted reactivation of the Australian continental interior over ca. 715 million years. The earliest events are identified in the hinterland of the orogen along the western transect. The first tectonothermal event, at ca. 715 Ma, is indicated by40 Ar/39 Ar muscovite and U e Pb titanite ages. Another previously unrecognised tectonometamorphic event is dated at ca. 630 Ma by Ue Pb analyses of metamorphic zircon rims. This event was followed by continuous cooling and exhumation of the hinterland and core of the orogen along numerous faults, including the Woodroffe Thrust,from ca. 625 Ma to 565 Ma as indicated by muscovite, biotite, and hornblende40 Ar/39 Ar cooling ages. We therefore propose that the Petermann Orogeny commenced as early as ca. 630 Ma. Along the eastern transect,40 Ar/39 Ar muscovite and zircon(Ue Th)/He data indicate exhumation of the foreland fold and thrust system to shallow crustal levels between ca. 550 Ma and 520 Ma, while the core of the orogen was undergoing exhumation to mid-crustal levels and cooling below 600-660℃. Subsequent cooling to 150 -220℃ of the core of the orogen occurred between ca. 480 Ma and 400 Ma(zircon [Ue Th]/He data)during reactivation of the Woodroffe Thrust, coincident with the 450 -300 Ma alice Springs *** of the footwall of the Woodroffe Thrust to shallow depths occurred at ca. 200 Ma. More recent tectonic activity is also evident as on the 21 May, 2016(Sydney date), a magnitude 6.1 earthquake occurred, and the resolved focal mechanism indicates that compressive stress and exhumation along the Woodroffe Thrust is continuing to the present day. Overall, these results

关键词： Intracontinental deformation Thermochronology Petermann orogen Musgrave Province Plate tectonics Cratonization

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汉语发展性深层阅读障碍的个案研究

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心理学报 2002年第4期34卷 338-343页

作者：栾辉舒华黎程正家林薇北京师范大学心理学系北京100875 香港理工大学护理与医疗科学系北京金色雨林学习能力研究中心北京100045

报告了一个发展性阅读障碍个案j,j的语音技能存在缺陷 ,音位、声调意识差 ,语音短时记忆能力弱 ,在汉字命名中产生大量语义错误、视觉错误和选择错误 ,表现出一系列深层阅读障碍症候群 ,是一例典型的深层阅读障碍个案。还讨论了汉语发... 详细信息

报告了一个发展性阅读障碍个案j,j的语音技能存在缺陷 ,音位、声调意识差 ,语音短时记忆能力弱 ,在汉字命名中产生大量语义错误、视觉错误和选择错误 ,表现出一系列深层阅读障碍症候群 ,是一例典型的深层阅读障碍个案。还讨论了汉语发展性阅读障碍亚类型的分类标准以及分布特点。

关键词：发展性深层阅读障碍生理年龄对照组语音缺陷语义错误

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Isolation and Identification of Pseudo Seven-Coordinate Ru(Ⅲ)Intermediate Completing the Catalytic Cycle of Ru-bda Type of Water Oxidation Catalysts

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CCS Chemistry 2022年第7期4卷 2481-2490页

作者： Tianqi Liu Ge Li Nannan Shen Linqin Wang Brian j.j.Timmer Shengyang Zhou Biaobiao Zhang Alexander Kravchenko Bo Xu Marten S.G.Ahlquist Licheng Sun Department of Chemistry School of Engineering Sciences in ChemistryBiotechnologyand HealthKTH Royal Institute of TechnologyStockholm 10044 Department of Theoretical Chemistry and Biology School of Engineering Sciences in ChemistryBiotechnologyand HealthKTH Royal Institute of TechnologyStockholm 10691 State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences(RAD-X)Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow UniversitySuzhou 215123 Center of Artificial Photosynthesis for Solar Fuels School of ScienceWestlake UniversityHangzhou 310024 Nanotechnology and Functional Materials Department of Materials Sciences and EngineeringThe Angstrom LaboratoryUppsala UniversityUppsala 75103 Institute of Artificial Photosynthesis(IAP) State Key Laboratory of Fine ChemicalsDalian University of Technology(DUT)Dalian 116024

Isolation of RuⅢ-bda(17-electron specie)complex with an aqua ligand(2-electron donor)is challenging due to violation of the 18-electron *** considerable efforts have been dedicated to mechanistic studies of water oxidation by the Ru-bda family,the structure and initial formation of the Ru^(Ⅲ)-bda aqua complex are still ***,we challenge this often overlooked step by designing a pocketshape Ru-based complex *** computational studies showed that 1 possesses the crucial hydrophobicity at the Ru^(V)(O)state as well as similar probability of access of terminal O to solvent water molecules when compared with classic Ru-bda *** characterization of single-crystal structures at the Ru^(Ⅱ) and Ru^(Ⅲ) states,a pseudo seven-coordinate“ready-togo”aqua ligand with Ru^(Ⅲ)…O distance of 3.62A was *** aqua ligand was also found to be part of a formed hydrogen-bonding network,providing a good indication of how the Ru^(Ⅲ)-OH_(2)complex is formed.

关键词： Ru-bda water oxidation pseudo seven-coordinate Ru^(Ⅲ)-OH_(2)intermediate water preorganization

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Predicting elastic properties of hard-coating alloys using ab-initio and machine learning methods

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npj Computational Materials 2022年第1期8卷 139-148页

作者： H.Levämäki F.Tasnádi D.G.Sangiovanni L.j.S.johnson R.Armiento I.A.Abrikosov Department of Physics Chemistry and BiologyLinköping UniversitySE-58183LinköpingSweden Sandvik Coromant S-12680StockholmSweden Materials Modeling and Development Laboratory National University of Science and Technology‘MISIS’119049MoscowRussia

Accelerated design of hard-coating materials requires state-of-the-art computational tools,which include data-driven techniques,building databases,and training machine learning *** develop a heavily automated high-throughput workflow to build a database of industrially relevant hard-coating materials,such as binary and ternary *** use the high-throughput toolkit to automate the density functional theory calculation *** present results,including elastic constants that are a key parameter determining mechanical properties of hard-coatings,for X_(1−x)Y_(x)N ternary nitrides,where X,Y∈{Al,Ti,Zr,Hf}and fraction x=0,1/4,1/2,3/4,*** also explore ways for machine learning to support and complement the designed *** find that the crystal graph convolutional neural network trained on ordered lattices has sufficient accuracy for the disordered nitrides,suggesting that existing databases provide important data for predicting mechanical properties of qualitatively different types of materials,in our case disordered hard-coating alloys.

关键词： coating alloys ternary

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