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Enzymatic and chemo-enzymatic strategies to produce highly valuable chiral amines from biomass with ω-transaminases on 2D zeolites

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National Science Review 2022年第9期9卷 10-18页

作者： J.Miguel Carceller Karen S.Arias Maria J.Climent Sara Iborra Avelino Corma Instituto de Tecnologia Química (UPV-CSIC) Universitat Politècnica de València

Amino transaminases(ATAs) have been supported on a 2D ITQ-2 zeolite through electrostatic interactions, resulting in a highly stable active biocatalyst to obtain a variety of valuable chiral amines starting from prochiral ketones derived from biomass. We have extended the biocatalyst applications by designing a chemo-enzymatic process that allows, as the first step, prochiral ketones to be obtained from biomass-derived compounds through an aldol condensation–reduction step using a bifunctional metal/base catalyst. The prochiral ketone is subsequently converted into the chiral amine using the immobilized ATA. We show that it is feasible to couple both steps in a semi-continuous process to produce industrially relevant chiral amines with yields of >95% and ～100% enantiomer excess.

关键词： amino transaminase ITQ-2 zeolite chemo-enzymatic process biomass semi-continuous process Pd/MgO

Coping with drought?Effects of extended drought conditions on soil invertebrate prey and diet selection by a fossorial amphisbaenian reptile

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Current Zoology 2023年第4期69卷 367-376页

作者： José Martín Jesús Ortega Roberto García-Roa Gonzalo Rodríguez-Ruiz Ana Pérez-Cembranos Valentín Pérez-Mellado Departamento de Ecología Evolutiva Museo Nacional de Ciencias NaturalesCSICMadridSpain Institute of Evolutionary Biology CSIC-Universitat Pompeu FabraBarcelonaSpain Ethology Lab Cavanilles Institute of Biodiversity and Evolutionary BiologyUniversity of ValenciaValenciaSpain Departamento de Biología Animal Universidad de SalamancaSalamancaSpain

Arid climates are characterized by a summer drought period to which animals seem ***,in some years,the drought can extend for unusually longer *** the effects of these current extreme weather events on biodiversity can help to understand the effects of climate change,as models predict an increase in drought ***,we examined the effects of“unusual”extended drought on soil invertebrate prey availability and on diet composition(based on fecal contents)and diet selection of a fossorial amphisbaenian,the checkerboard worm lizard Trogonophis *** data show interannual variations in summer drought *** abundance and diversity of soil invertebrates in spring were high,and similar to those found in a“normal”early autumn,after some rain had ended with the summer *** contrast,in years with“unusual”extended drought,abundance,and diversity of soil invertebrates in early autumn were very ***,there were seasonal changes in amphisbaenians’diet;in autumn with drought,prey diversity,and niche breadth decreased with respect to spring and autumns after some rain had *** did not eat prey at random in any season,but made some changes in prey selection that may result from drought-related restrictions in prey ***,in spite that amphisbaenians showed some feeding flexibility,their body condition was lower in autumn than in spring,and much lower in autumn with *** extended drought became the norm in the future,amphisbaenians might suffer important negative effects for their health state.

关键词： amphisbaenians drought feeding ecology soil invertebrates Trogonophis wiegmanni weather conditions

Relationships between soil pollution by heavy metals and melanin-dependent coloration of a fossorial amphisbaenian reptile

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Integrative Zoology 2022年第4期17卷 596-607页

作者： JoséMARTÍN Pablo RECIO Gonzalo RODRÍGUEZ-RUIZ Isabel BARJA Eduardo GUTIÉRREZ Luis VGARCÍA Departamento de Ecología Evolutiva Museo Nacional de Ciencias NaturalesCSICMadridSpain Departamento de Zoología Facultad de BiologíaUniversidad Autónoma de MadridMadridSpain Centro de Investigación en Biodiversidad y Cambio Global(CIBC-UAM) Universidad Autónoma de MadridMadridSpain Departamento de Biogeoquímica Ecología Vegetal y MicrobianaInstituto de Recursos Naturales y Agrobiología de SevillaCSICSevillaSpain

Melanin is the basis of coloration in many animals,and although it is often used in communication,thermoregulation,or camouflage,melanin has many other physiological *** example,in polluted habitats,melanin can have a detoxifying *** coloration would help to sequester in the skin the heavy metal contaminants from inside the body,which will be expelled to the exterior when the skin is ***,animals should have evolved more melanic colorations in more polluted habitats(“industrial melanism”hypothesis).We examined whether the fossorial amphisbaenian reptile,Trogonophis wiegmanni,is able to eliminate heavy metals,derived from soil pollution by seagull depositions,through sloughing its *** results suggest a covariation between levels of soil pollution by heavy metals and the concentration of heavy metals in the sloughed skins of *** suggests that amphisbaenians may expel heavy metals from their bodies when they slough the *** also tested whether amphisbaenians inhabiting soils with higher levels of heavy metal pollution had darker(melanin-dependent)body ***,contrary to predictions from the“industrial melanization”hypothesis,we found a negative relationship between soil pollution and proportions of melanic *** contradictory result could,however,be explained because heavy metals have endocrine disruption effects that increase physiological stress,and higher stress levels could result in decreased *** suggest that although amphisbaenians might have some detoxifying mechanism linked to melanin in the skin,this process might be negatively affected by stress and result ineffective under conditions of high soil pollution.

关键词： amphisbaenians coloration fossorial reptiles heavy metals melanin soil pollution

Development and screening of(Ca-P-Si-F)-PEO coatings for biodegradability control of Mg-Zn-Ca alloys

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Journal of Magnesium and Alloys 2022年第8期10卷 2220-2237页

作者： Lara Moreno Marta Mohedano Raul Arrabal Endzhe Matykina Departamento de Ingeniería Química y de Materiales Facultad de Ciencias QuímicasUniversidad Complutense de Madrid28040 MadridSpain

PEO coatings were developed on MgZnxCayalloys for biomedical applications using different treatment times and a novel transparent electrolyte containing Ca,P,Si and *** characteristics and chemical composition of studied materials were evaluated using scanning electron microscopy,X-ray diffraction and optical *** investigations were performed for uncoated and coated materials using potentiodynamic polarization,electrochemical impedance spectroscopy and hydrogen evolution measurements in three media(0.9wt.%NaCl,α-MEM and inorganic part ofα-MEM).Findings revealed that Zn-rich intermetallics favour the formation of large voids in the ***,P,F and Si are successfully incorporated into the *** consist of crystalline phases(Mg O,Mg F_(2)and Ca,Si-rich compounds)and amorphous *** and organic components ofα-MEM solution accelerate corrosion of the bare substrates but have no significant influence on the corrosion resistance of coated ***,inorganicα-MEM can be considered as an appropriate medium for fast screening of PEO *** relatively small amount of F content in the barrier layer facilitates early failure of the coatings,which show undercoating ***-rich intermetallic particles in the undercoating crevice induce a more aggressive corrosive environment and enhanced micro-galvanic couple effect with the Mg *** leads to faster degradation of the coated alloys compared to the bare substrates.

关键词： Magnesium Biomaterials Plasma electrolytic oxidation Corrosion

Differential effects of environmental climatic variables on parasite abundances in blue tit nests during a decade

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Integrative Zoology 2022年第4期17卷 511-529页

作者： Francisco CASTAÑO-VÁZQUEZ Santiago MERINO Evolutionary Ecology Museo Nacional de Ciencias Naturales CSICMadridSpain

Models on climate change have predicted an increase of temperature over the earth’s surface with potential drastic effects on living *** analyzed the relationships between climatic conditions(temperature,rainfall,and wind speed)and the abundance of blood-sucking flying insects(biting midges and blackflies)and nest-dwelling ectoparasites(mites,fleas,and blowflies)collected from blue tit nests during bird breeding seasons for a period of 10 *** temperature,rainfall,and wind speed showed significant differences among *** and wind speed increased during the period of study while rainfall *** midge,blackfly,and blowfly abundances increased across years but not flea and mite *** date decreased and brood size increased across *** of year variation,parasites were related to climatic *** example,biting midge,blowfly,mite,and flea abundances were positive and significantly related to average *** also found a positive and significant relationship between abundances of Haemoproteus infections and biting midge abundances during the first year of life of birds out of ***,abundance and prevalence of Lankesterella infections in yearlings were positive and significantly related to mite abundances during the year of birth of *** and Lankesterella infections were also significantly related to climatic variables and Haemoproteus and Lankesterella infections increased across *** addition,body condition of adult females and males were negatively related to flea larvae and blowfly abundance *** body condition was also negatively related to biting midge *** in climatic conditions across years could therefore affect several parasites of birds but also to birds themselves.

关键词： biting midges blackfly blowfly Haemoproteus Lankesterella rainfall temperature

Using compositional data analysis to explore accumulation of sedentary behavior,physical activity and youth health

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Journal of Sport and Health Science 2022年第2期11卷 234-243页

作者： Simone J.J.M.Verswijveren Karen E.Lamb Josep A.Martín-Fernández Elisabeth Winkler Rebecca M.Leech Anna Timperio Jo Salmon Robin M.Daly Ester Cerin David W.Dunstan Rohan M.Telford Richard D.Telford Lisa S.Olive Nicola D.Ridgers Institute for Physical Activity and Nutrition School of Exercise and Nutrition SciencesDeakin UniversityGeelongVIC 3216Australia Melbourne School of Population and Global Health University of MelbourneParkvilleVIC 3053Australia Department of Computer Science Applied Mathematics and StatisticsUniversity of GironaGirona 17003Spain School of Public Health University of QueenslandHerstonQLD 4006Australia Mary MacKillop Institute for Health Research Australian Catholic UniversityFitzroyVIC 3065Australia School of Public Health University of Hong KongHong KongChina Baker Heart and Diabetes Institute MelbourneVIC 3004Australia Research Institute for Sport and Exercise University of CanberraBruceACT 2617Australia School of Psychology Deakin UniversityBurwoodVIC 3125Australia IMPACT Research Institute Deakin UniversityBurwoodVIC 3125Australia ANU Medical School Australian National UniversityGarranACT 2605Australia

Purpose:The study aimed to describe youth time-use compositions,focusing on time spent in shorter and longer bouts of sedentary behavior and physical activity(PA),and to examine associations of these time-use compositions with cardiometabolic ***:Accelerometer and cardiometabolic biomarker data from 2 Australian studies involving youths 7-13 years old were pooled(complete cases with accelerometry and adiposity marker data,n=782).A 9-component time-use composition was formed using compositional data analysis:time in shorter and longer bouts of sedentary behavior;time in shorter and longer bouts of light-,moderate-,or vigorous-intensity PA;and"other time"(i.e.,non-wear/sleep).Shorter and longer bouts of sedentary time were defined as5 min,*** bouts of light-,moderate-,and vigorous-intensity PA were defined as<1 min;longer bouts were defined as≥1 *** models examined associations between overall time-use composition and cardiometabolic ***,associations were derived between ratios of longer activity patterns relative to shorter activity patterns,and of each intensity level relative to the other intensity levels and"other time",and cardiometabolic ***:Confounder-adjusted models showed that the overall time-use composition was associated with adiposity,blood pressure,lipids,and the summary ***,more time in longer bouts of light-intensity PA relative to shorter bouts of light-intensity PA was significantly associated with greater body mass index z-score(zBMI)(β=1.79;SE=0.68)and waist circumference(β=18.35,SE=4.78).When each activity intensity was considered relative to all higher intensities and"other time",more time in light-and vigorous-intensity PA,and less time in sedentary behavior and moderate-intensity PA,were associated with lower waist ***:Accumulating PA,particularly light-intensity PA,in frequent short bursts may be more beneficial for limiting adi

关键词： Accumulation patterns Cardiometabolic health Children Compositional data analysis Time-use

Evaluation of a crop rotation with biological inhibition potential to avoid N_(2)O emissions in comparison with synthetic nitrification inhibition

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Journal of Environmental Sciences 2023年第5期127卷 222-233页

作者： Adrián Bozal-Leorri Mario Corrochano-Monsalve Luis M.Arregui Pedro M.Aparicio-Tejo Carmen González-Murua Department of Plant Biology and Ecology University of the Basque Country(UPV/EHU)Apdo.644E-48080Bilbao 48940Spain Institute for Innovation and Sustainable Development in Food Chain(ISFOOD) Public University of NavarrePamplona 31006Spain Institute for Multidisciplinary Research in Applied Biology(IMAB) Public University of NavarrePamplona 31006Spain

Agriculture has increased the release of reactive nitrogen to the environment due to crops’low nitrogen-use efficiency(NUE)after the application of *** like the use of stabilized-fertilisers with nitrification inhibitors such as DMPP(3,4-dimethylpyrazole phosphate)have been adopted to reduce nitrogen ***,cover crops can be used in crop-rotation-strategies to reduce soil nitrogen pollution and benefit the following ***(Sorghum bicolor)could be a good candidate as it is drought tolerant and its culture can reduce nitrogen losses derived from nitrification because it exudates biological nitrification inhibitors(BNIs).This work aimed to evaluate the effect of fallow-wheat and sorghum cover crop-wheat rotations on N_(2)O emissions and the grain yield of winter wheat *** addition,the suitability of DMPP addition was also *** use of sorghum as a cover crop might not be a suitable option to mitigate nitrogen losses in the subsequent *** sorghum–wheat rotation was able to reduce 22%the abundance of amoA,it presented an increment of 77%in cumulative N_(2)O emissions compared to fallow–wheat rotation,which was probably related to a greater abundance of heterotrophic-denitrification *** the other hand,the application of DMPP avoided the growth of ammonia-oxidizing bacteria and maintained the N_(2)O emissions at the levels of unfertilized-soils in both *** a conclusion,the use of DMPP would be recommendable regardless of the rotation since it maintains NH_(4)^(+)in the soil for longer and mitigates the impact of the crop residues on nitrogen soil dynamics.

关键词： Fallow Sorghum Crop rotation Nitrification inhibitor N-cycling genes Soil mineral nitrogen

As-cast and extruded Mg-Zn-Ca systems for biodegradable implants:Characterization and corrosion behavior

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Journal of Magnesium and Alloys 2023年第3期11卷 1102-1120页

作者： Lara Moreno Endzhe Matykina Kiryl A.Yasakau Carsten Blawert Raul Arrabal Marta Mohedano Departamento de Ingeniería Química y de Materiales Facultad de Ciencias QuímicasUniversidad Complutense de Madrid28040 MadridSpain Department of Materials and Ceramic Engineering CICECO-Aveiro institute of materialsUniversity of Aveiro3810-193 AveiroPortugal Institute of Surface Science Helmholtz-Zentrum HereonMax-Planck Strasse 1Geesthacht 21502Germany

The aim of the present study is to evaluate the effect of alloy processing and composition as well as the pH control and testing medium on the in vitro corrosion performance of Mg-Zn-Ca systems for biodegradable *** grain size and secondary phases were analyzed by optical microscopy,scanning electron microscopy,transmission electron microscopy,and X-ray *** kelvin probe force microscopy(SKPFM)was used to analyze the Volta potential values of the second *** corrosion performance of the three alloys was evaluated by electrochemical and hydrogen evolution methods inα-MEM with and without organic species(*** and inorganicα-MEM).Two strategies were followed to evaluate the influence of the pH on the corrosion behavior:daily solution replacement and CO_(2)flow based pH *** all the materials,the organic medium accelerates the corrosion *** pH maintained by CO_(2)flow through the medium results in considerably higher corrosion rates for all *** impact of pH is lesser on the as-cast alloys due to the barrier effect of the secondary phases,particularly pronounced in the Mg1Zn1Ca alloy which showed the lowest corrosion *** wrought Mg0.5Zn0.2Ca alloy that lacks the refined secondary phase network and exhibits high number of twins undergoes accelerated uniform corrosion under constant pH conditions.

关键词： MgZnCa Magnesium Biomaterials Characterization Corrosion

LDH conversion films for active protection of AZ31 Mg alloy

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Journal of Magnesium and Alloys 2023年第1期11卷 201-216页

作者： B.Pillado B.Mingo R.del Olmo E.Matykina A.M.Kooijman Y.Gonzalez−Garcia R.Arrabal M.Mohedano Departamento de Ingeniería Química y de Materiales Facultad de Ciencias QuímicasUniversidad ComplutenseMadrid 28040Spain Department of Materials University of ManchesterOxford RoadManchester M139PLUK Institute of Optoelectronics Military University of Technology2 Kaliskiego Str.Warsaw 00-908Poland Materials Science and Engineering Department Delft University of TechnologyMekelweg 2Delft 2628 CDthe Netherlands

Zinc aluminium(Zn-Al)and lithium aluminium(Li-Al)–layered double hydroxides(LDH)coatings with incorporated inhibitors(Li-,Mo-and W-based)were successfully synthesized on AZ31 Mg ***-Al LDH W and Li-Al LDH Li showed the highest corrosion resistance and were selected for further *** cross-section examination revealed a bi-layer structure composed of an outer part with loose flakes and a denser inner ***,FTIR,and XPS analysis confirmed the incorporation of the ***-treatments with corrosion inhibitors containing solutions resulted in the selective dissolution of the most external layer of the LDH coating,reducing the surface roughness,hydrophilicity and paint adhesion of the *** corrosion properties were confirmed by SVET evaluation for the Zn-Al LDH W *** proposed active corrosion mechanism involves the ion-exchange of aggressive Cl-ions,deposition of hydroxides and competitive adsorption of W-rich corrosion inhibitors.

关键词： AZ31 Magnesium Layered double hydroxides Corrosion inhibitors Active corrosion protection