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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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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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Metabolic reprogramming by Syntenin-1 directs RA FLS and endothelial cell-mediated inflammation and angiogenesis

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Cellular & Molecular Immunology 2024年第1期21卷 33-46页

作者： Anja Meyer Stephanie R.Zack Wes Nijim Adel Burgos Vishwa Patel brian Zanotti Michael V.Volin M.Asif Amin Myles j.Lewis Costantino Pitzalis Shiva Arami joseph A.Karam Nadera j.Sweiss Shiva Shahrara jesse Brown VA Medical Center ChicagoILUSA Department of Medicine Division of RheumatologyThe University of Illinois at ChicagoChicagoILUSA Department of Microbiology and Immunology Midwestern UniversityDowners GroveILUSA Division of Rheumatology and Clinical Autoimmunity Center of Excellence University of MichiganAnn ArborMIUSA Centre for Experimental Medicine and Rheumatology William Harvey Research InstituteBarts and The London School of Medicine and DentistryQueen Mary University of LondonLondonUnited Kingdom Centre for Experimental Medicine&Rheumatology William Harvey Research InstituteQueen Mary University of London and Barts NIHR BRC&NHS TrustLondonUK Department of Biomedical Sciences Humanitas Universityand Humanitas Research HospitalMilanItaly Department of Orthopedic Surgery the University of Illinois at ChicagoChicagoILUSA

A novel rheumatoid arthritis(RA)synovial fluid protein,Syntenin-1,and its receptor,Syndecan-1(SDC-1),are colocalized on RA synovial tissue endothelial cells and fibroblast-like synoviocytes(FLS).Syntenin-1 exacerbates the inflammatory landscape of endothelial cells and RA FLS by upregulating transcription of IRF1/5/7/9,IL-1β,IL-6,and CCL2 through SDC-1 ligation and HIF1α,or mTOR ***,Syntenin-1 orchestrates RA FLS and endothelial cell invasion via SDC-1 and/or mTOR *** Syntenin-1 reprogrammed endothelial cells,the dynamic expression of metabolic intermediates coincides with escalated glycolysis along with unchanged oxidative factors,AMPK,PGC-1α,citrate,and inactive oxidative ***,RA FLS rewired by Syntenin-1 displayed a modest glycolytic-ATP accompanied by a robust mitochondrial-ATP *** enriched mitochondrial-ATP detected in Syntenin-1 reprogrammed RA FLS was coupled with mitochondrial fusion and fission recapitulated by escalated Mitofusin-2 and DRP1 *** found that VEGFR1/2 and Notch1 networks are responsible for the crosstalk between Syntenin-1 rewired endothelial cells and RA FLS,which are also represented in RA *** to RA explants,morphological and transcriptome studies authenticated the importance of VEGFR1/2,Notch1,RAPTOR,and HIF1αpathways in Syntenin-1 arthritic mice and their obstruction in SDC-1 deficient ***,dysregulation of SDC-1,mTOR,and HIF1αnegated Syntenin-1 inflammatory phenotype in RA explants,while inhibition of HIF1αimpaired synovial angiogenic imprint amplified by *** conclusion,since the current therapies are ineffective on Syntenin-1 and SDC-1 expression in RA synovial tissue and blood,targeting this pathway and its interconnected metabolic intermediates may provide a novel therapeutic strategy.

关键词： Syntenin-1 Syndecan-1 RA FLS RA explants immunometabolism

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Fetal Head Compression: Its Possible Role in Neurologic Injury

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Open journal of Obstetrics and Gynecology 2024年第1期14卷 124-143页

作者： Barry S. Schifrin brian j. Koos Wayne R. Cohen Department of Obstetrics and Gynecology The Western University of Health Sciences Pomona USA The David Geffen School of Medicine at UCLA Los Angeles USA The University of Arizona College of Medicine Tucson USA

It is widely assumed that fetal ischemic brain injury during labor derives almost exclusively from severe, systemic hypoxemia with marked neonatal depression and acidemia. Severe asphyxia, however, is one of several causes of perinatal neurological injury and may not be the most common;most neonates diagnosed with hypoxic-ischemic encephalopathy do not have evidence of severe asphyxia. Sepsis, direct brain trauma, and drug or toxin exposure account for some cases, while mechanical forces of labor and delivery that increase fetal intracranial pressure sufficiently to impair brain perfusion may also contribute. Because of bony compliance and mobile suture lines, the fetal skull changes shape and redistributes cerebrospinal fluid during labor according to constraints imposed by contractions, and bony and soft tissue elements of the birth canal as the head descends. These accommodations, including the increase in intracranial pressure, are adaptive and necessary for efficient descent of the head while safeguarding cerebral blood flow. Autonomic reflexes mediated through central receptors normally provide ample protection of the brain from the considerable pressure exerted on the skull. On occasion, those forces, which are transmitted intracranially, may overcome the various adaptive anatomical, cardiovascular, metabolic, and neurological mechanisms that maintain cerebral perfusion and oxygen availability, resulting in ischemic brain injury. Accepting the notion of a potentially adverse impact of fetal head compression suggests that avoidance of excessive uterine activity and of relentless pushing without steady progress in descent may offer protection for the fetal brain during parturition. Excessive head compression should be considered in the differential diagnosis of ischemic encephalopathy.

关键词： Fetal Brain Injury Fetal Head Compression Ischemic Encephalopathy Neonatal Encephalopathy

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Rodent management in Aotearoa New Zealand: approaches and challenges to landscape-scale control

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Integrative Zoology 2024年第1期19卷 8-26页

作者： john G.INNES Grant NORBURY Araceli SAMANIEGO Susan WALKER Deborah j.WILSON Manaaki Whenua-Landcare Research HamiltonNew Zealand Manaaki Whenua-Landcare Research AlexandraNew Zealand Manaaki Whenua-Landcare Research AucklandNew Zealand Manaaki Whenua-Landcare Research DunedinNew Zealand

Aotearoa—New Zealand has only four rodent species,all *** order of arrival,they are Pacific rat Rattus exulans,brown rat ***,house mouse Mus musculus,and black rat *** management in New Zealand aims mainly to conserve indigenous biodiversity rather than to protect crops or manage diseases,as is usual *** describe four major“regimes”and one major vision for rodent control in New Zealand to meet ecological restoration *** challenges for island eradications are for large islands that are remote or populated by *** 1080 is the only large-scale(tens of thousands of hectares)option for black rat control,but its application requires adjustment to counter subsequent rapid black rat ***“ecosanctuaries”(mean 720 ha)use ground-based traps and poisons to target mainly black rats and face constant *** with mammal-resistant fences(up to 3500 ha)limit reinvasion and target more pest species and have enabled the return of previously extirpated taxa to the main *** Free 2050 aims to eradicate the rat species(but not mice)plus some other introduced mammals from New Zealand by *** vision is not attainable with current tools,but research and experimental management is exploring techniques and *** large scale(to 100000 ha)at which black rats are now targeted for control to extremely low abundance seems to be unique to New Zealand.

关键词： black rat brown rat eradication house mouse rodent control

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Effect of Air Plasma Processing on the Adsorption Behaviour of Bovine Serum Albumin on Spin-Coated PMMA Surfaces

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journal of Bionic Engineering 2008年第3期5卷 204-214页

作者： Chaozong Liu brian j. Meenan Advanced Materials and Biomaterials Research Centre School of Engineering The Robert Gordon University Aberdeen ABIO 1FR UK Northern ireland Bioengineering Centre University of Ulster Newtownabbey BT37 OQB Northern Ireland UK

This paper reports the adsorption of Bovine Serum Albumin （BSA） onto Dielectric Barrier Discharge （DBD） processed Poly（methyl methacrylate）（PMMA） surfaces by a Quartz Crystal Microbalance with Dissipation monitoring （QCM-D） technique. The purpose is to study the influence of DBD processing on the nature and scale of BSA adsorption on PMMA surface in vitro. It was observed that DBD processing improves the surface wettability of PMMA film, a fact attributable to the changes in surface chemistry and topography. Exposure of the PMMA to Phosphate Buffed Saline （PBS） solution in the QCM-D system resulted in surface adsorption which reaches an equilibrium after about 30 minutes for pristine PMMA, and 90 minutes for processed PMMA surface. Subsequent injection of BSA in PBS indicated that the protein is immediately adsorbed onto the PMMA surface. It was revealed that adsorption behaviour of BSA on pristine PMMA differs from that on processed PMMA surface. A slower adsorption kinetics was observed for pristine PMMA surface, whilst a quick adsorption kinetics for processed PMMA. Moreover, the dissipation shift of protein adsorption suggested that BSA forms a more rigid structure on pristine PMMA surface that on processed surface. These data suggest that changes in wettability and attendant chemical properties and surface texture of the PMMA surface may play a significant role in BSA adsorption process.

关键词： in vitro test protein adsorption surface modification polymethylmethacrylate QCM-D

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Crystalline compounds for remediation of rare-earth fission products:A review

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journal of Rare Earths 2022年第3期40卷 365-380,I0001页

作者： Saehwa Chong brian j.Riley Zayne j.Nelson Pacific Northwest National Laboratory RichlandWA99352USA

Rare earth(RE)-containing crystals have been investigated as media for the immobilization of RE fission products from nuclear waste *** reprocessing of spent nuclear fuel,fission products including REs,alkalis,and alkaline earths released from the *** viable option to immobilize the RE fission products is to incorporate them into chemically durable crystalline phases in specific waste *** study summarizes the crystal structures and synthesis methods of six RE-containing compounds that have applications in remediation of RE fission *** compounds include oxyapatite(AE_(2)RE_(8)(SiO_(4))_(6)O_(2)),oxychloride(REOCl),borosilicate(RE_(3)BSi_(2)O_(10)),pyrochlore(RE_(2)M_(2)O_(7)),monazite(REPO_(4)),and perovskite(REMO_(3))where AE denotes alkaline earth metals and M denotes transition *** review provides an overview of literature on the usage of these six compounds for immobilizing RE fission products and summarizes different synthesis methods for producing these *** of structural parameters with different REs in each compound are also discussed.

关键词： Rare-earth compounds Nuclear waste forms Crystal structures Synthesis of rare-earth compounds

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Trees are rarely most abundant where they grow best

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journal of Plant Ecology 2012年第1期5卷 46-51页

作者： brian j.McGill School of Biology and Ecology and Sustainability Solutions Initiative 303 Deering HallUniversity of MaineOronoME 04469USA

Aims A common assumption in ecology is that where a species is found to be most abundant must correspond to the environmental context in which the species performs the best(*** niche space).This assumption is central to common conservation and management tools such as habitat suitability assessment and species distribution modeling.I test this *** I use the US Forest Inventory Assessment data for the abundance of trees across eastern North America.I use the FORAST tree-ring dataset for ontogenetic growth rate(tree-ring increment),a measure of niche performance and correlated with intrinsic rate of increase,*** Findings I find that across 15 species,there are significantly more negative correlations than expected by *** negative correlation between abundance and performance across space contradicts common assumptions but is consistent with an inclusive niche structuring of the community.

关键词： tree rings biogeography inclusive niche climate change

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The impact of seasonality on multi-scale feature extraction techniques

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International journal of Digital Earth 2020年第1期13卷 9-21页

作者： brian Moore jacob j.McKee Geographic Information Science and Technology Group Computational Sciences and Engineering DivisionOak Ridge National LaboratoryOak RidgeTNUSA

A key component in constructing a broad-scale,gridded population dataset is fine resolution geospatial data accurately depicting the extent of human *** datasets are often developed using a wide range of methods and classification techniques,including the use of spatial features,spectral features,or the coupling of both to identify the presence of man-made structures from high-resolution satellite *** using spatial and textural-based descriptors to generate highresolution settlement layers for two dissimilar regions at the peak of seasonal disparity,this study attempts to quantify the influence of seasonality on the accuracy of a supervised,multi-scale,feature extraction framework for automated delineation of human *** generated by numerous models are evaluated against a reference dataset allowing for assessment of seasonal and feature differences in the context of *** or regional mapping of human settlement requires the assemblage of high-resolution satellite images with variegated acquisition characteristics(season,sun elevation,off-nadir,etc.)to produce a cloud-free composite image from which features are *** of this study suggest an emphasis on imagery criteria,in particular acquisition date,could improve classification accuracy when mapping human settlement at scale.

关键词： Remote sensing highresolution imagery image processing human settlement accuracy

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The endogenous progenitor response following traumatic brain injury:a target for cell therapy paradigms

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Neural Regeneration Research 2022年第11期17卷 2351-2354页

作者： Anna Badner brian j.Cummings Department of Psychiatry and Behavioral Sciences Stanford UniversityPalo AltoCAUSA Sue and Bill Gross Stem Cell Center University of California-IrvineIrvineCAUSA Institute for Memory Impairments and Neurological Disorders University of California-IrvineIrvineCAUSA Physical Medicine and Rehabilitation University of California-IrvineIrvineCAUSA Department of Anatomy and Neurobiology University of California-IrvineIrvineCAUSA

Although there is ample evidence that central nervous system progenitor pools respond to traumatic brain injury,the reported effects are variable and likely contribute to both recovery as well as *** a better understanding of the diverse progenitor populations in the adult brain and their niche-specific reactions to traumatic insult,treatments can be tailo red to enhance the benefits and dampen the deleterious effects of this *** review provides an overview of endogenous precursors,the associated effects on cognitive recovery,and the potential of exogenous cell therapeutics to modulate these endogenous repair *** the hippocampal dentate gyrus and subventricular zone of the lateral ventricles,more recently identified sites of adult neurogenesis,the meninges,as well as circumventricular organs,are also discussed as targets for endogenous ***,this review highlights that progenitor prolife ration alone is no longer a meaningful outcome and studies must strive to better chara cterize precursor spatial localization,transcriptional profile,morphology,and functional synaptic *** improved insight and a more targeted approach,the stimulation of endogenous neurogenesis remains a promising strategy for recovery following traumatic brain injury.

关键词： cell therapy endogenous repair neurogenic niche progenitors traumatic brain injury

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