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1.
J Am Chem Soc ; 142(42): 17881-17886, 2020 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-33021787

RESUMO

Bottom-up-synthesized graphene nanoribbons (GNRs) with excellent electronic properties are promising materials for energy storage systems. Herein, we report bottom-up-synthesized GNR films employed as electrode materials for micro-supercapacitors (MSCs). The micro-device delivers an excellent volumetric capacitance and an ultra-high power density. The electrochemical performance of MSCs could be correlated with the charge carrier mobility within the differently employed GNRs, as determined by pump-probe terahertz spectroscopy studies.

2.
Proc Natl Acad Sci U S A ; 112(41): 12592-7, 2015 Oct 13.
Artigo em Inglês | MEDLINE | ID: mdl-26417094

RESUMO

In living organisms, color patterns, behavior, and ecology are closely linked. Thus, detection of fossil pigments may permit inferences about important aspects of ancient animal ecology and evolution. Melanin-bearing melanosomes were suggested to preserve as organic residues in exceptionally preserved fossils, retaining distinct morphology that is associated with aspects of original color patterns. Nevertheless, these oblong and spherical structures have also been identified as fossilized bacteria. To date, chemical studies have not directly considered the effects of diagenesis on melanin preservation, and how this may influence its identification. Here we use time-of-flight secondary ion mass spectrometry to identify and chemically characterize melanin in a diverse sample of previously unstudied extant and fossil taxa, including fossils with notably different diagenetic histories and geologic ages. We document signatures consistent with melanin preservation in fossils ranging from feathers, to mammals, to amphibians. Using principal component analyses, we characterize putative mixtures of eumelanin and phaeomelanin in both fossil and extant samples. Surprisingly, both extant and fossil amphibians generally exhibit melanosomes with a mixed eumelanin/phaeomelanin composition rather than pure eumelanin, as assumed previously. We argue that experimental maturation of modern melanin samples replicates diagenetic chemical alteration of melanin observed in fossils. This refutes the hypothesis that such fossil microbodies could be bacteria, and demonstrates that melanin is widely responsible for the organic soft tissue outlines in vertebrates found at exceptional fossil localities, thus allowing for the reconstruction of certain aspects of original pigment patterns.


Assuntos
Fósseis , Melaninas , Melanossomas/ultraestrutura , Animais , Bactérias , Pigmentação
3.
Nature ; 473(7347): 364-7, 2011 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-21593869

RESUMO

Amphisbaenia is a speciose clade of fossorial lizards characterized by a snake-like body and a strongly reinforced skull adapted for head-first burrowing. The evolutionary origins of amphisbaenians are controversial, with molecular data uniting them with lacertids, a clade of Old World terrestrial lizards, whereas morphology supports a grouping with snakes and other limbless squamates. Reports of fossil stem amphisbaenians have been falsified, and no fossils have previously tested these competing phylogenetic hypotheses or shed light on ancestral amphisbaenian ecology. Here we report the discovery of a new lacertid-like lizard from the Eocene Messel locality of Germany that provides the first morphological evidence for lacertid-amphisbaenian monophyly on the basis of a reinforced, akinetic skull roof and braincase, supporting the view that body elongation and limblessness in amphisbaenians and snakes evolved independently. Morphometric analysis of body shape and ecology in squamates indicates that the postcranial anatomy of the new taxon is most consistent with opportunistically burrowing habits, which in combination with cranial reinforcement indicates that head-first burrowing evolved before body elongation and may have been a crucial first step in the evolution of amphisbaenian fossoriality.


Assuntos
Fósseis , Lagartos/anatomia & histologia , Lagartos/classificação , Filogenia , Animais , Tamanho Corporal , Ecossistema , Extremidades/anatomia & histologia , Alemanha , Lagartos/fisiologia , Modelos Biológicos , Crânio/anatomia & histologia , Serpentes/anatomia & histologia , Serpentes/classificação
5.
Nat Commun ; 11(1): 1490, 2020 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-32198456

RESUMO

The vast potential of organic materials for electronic, optoelectronic and spintronic devices entails substantial interest in the fabrication of π-conjugated systems with tailored functionality directly at insulating interfaces. On-surface fabrication of such materials on non-metal surfaces remains to be demonstrated with high yield and selectivity. Here we present the synthesis of polyaromatic chains on metallic substrates, insulating layers, and in the solid state. Scanning probe microscopy shows the formation of azaullazine repeating units on Au(111), Ag(111), and h-BN/Cu(111), stemming from intermolecular homo-coupling via cycloaddition reactions of CN-substituted polycyclic aromatic azomethine ylide (PAMY) intermediates followed by subsequent dehydrogenation. Matrix-assisted laser desorption/ionization (MALDI) mass spectrometry demonstrates that the reaction also takes place in the solid state in the absence of any catalyst. Such intermolecular cycloaddition reactions are promising methods for direct synthesis of regioregular polyaromatic polymers on arbitrary insulating surfaces.

6.
Adv Mater ; 29(4)2017 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-27874220

RESUMO

A facile one-step procedure for a template-assisted fabrication of hollow carbon tubes is reported, using organic halides as the carbon source. The shape-persistent tubes are obtained with arbitrary shapes as hollow replicas of the metal template. They feature a high quality of graphite, and a high conductivity of 1.31 ± 0.05 · 106 S·m-1 .

7.
Anat Rec (Hoboken) ; 298(11): 1848-63, 2015 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-26235188

RESUMO

Palaeobatrachidae are extinct frogs from Europe closely related to the Gondwanan Pipidae, which includes Xenopus. Their frontoparietal is a distinctive skeletal element which has served as a basis for establishing the genus Albionbatrachus. Because little was known about developmental and individual variation of the frontoparietal, and its usefulness in delimiting genera and species has sometimes been doubted, we investigate its structure in Palaeobatrachus and Albionbatrachus by means of X-ray high resolution computer tomography (micro-CT). To infer the scope of variation present in the fossil specimens, we also examined developmental and interspecific variation in extant Xenopus. In adults of extinct taxa, the internal structure of the frontoparietal bone consists of a superficial and a basal layer of compact bone, with a middle layer of cancellous bone between them, much as in early amphibians. In Albionbatrachus, the layer of cancellous bone, consisting of small and large cavities, was connected with the dorsal, sculptured surface of the bone by a system of narrow canals; in Palaeobatrachus, the layer of cancellous bone and the canals connecting this layer with the dorsal surface of the frontoparietal were reduced. The situation in Palaeobatrachus robustus from the lower Miocene of France is intermediate-while external features support assignment to Palaeobatrachus, the inner structure is similar to that in Albionbatrachus. It may be hypothesized that sculptured frontoparietals with a well-developed layer of cancellous (i.e., vascularized) bone may indicate adaptation to a more terrestrial way of life, whereas a reduced cancellous layer might indicate a permanent water dweller.


Assuntos
Anuros/anatomia & histologia , Anuros/classificação , Evolução Biológica , Osso Frontal/anatomia & histologia , Osso Parietal/anatomia & histologia , Animais , Feminino , Microtomografia por Raio-X
8.
J Nucl Med ; 55(6): 1023-8, 2014 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-24752674

RESUMO

UNLABELLED: Post-processing by means of a cation-exchanger-based protocol is an efficient strategy for purification and concentration of generator-derived (68)Ga. It ensures the removal of (68)Ge before (68)Ga-radiopharmaceutical preparation and high labeling yields of (68)Ga-labeled radiopharmaceuticals for routine medical application. METHODS: In an effort to overcome the problem associated with acetone in the currently applied method, we have investigated the feasibility of replacing it with ethanol. The purification of (68)Ga from coeluted metallic impurities ((68)Ge(4+), Fe(3+), Zn(2+), and Ti(4+)) on various cation-exchange columns has been investigated with a variety of post-processing solutions. As a proof of principle, the post-processed (68)Ga was used to radiolabel DOTATOC in combination with high-purity water and various buffer solutions. RESULTS: An effective protocol for the processing of generator-produced (68)Ga on the basis of cation-exchange chromatography using EtOH/HCl medium has been developed. Up to 95% of the initially eluted (68)Ga activity can be collected in a 1-mL fraction of 90% EtOH/0.9N HCl after removal of (68)Ge-breakthrough in a washing step. The post-processed eluate has been used to radiolabel DOTATOC in yields of approximately 97% ± 0.25% at 80°C in 5 min. CONCLUSION: The described novel protocol improves the radiolabeling efficiency and efficacy of DOTATOC, providing yields of greater than 99% (decay-corrected). As a result, further purification to separate the desired product from uncomplexed (68)Ga is not necessary. The developed post-processing and labeling protocols permit reliable and high-yield preparation of injectable (68)Ga-DOTATOC (or other (68)Ga-labeled radiopharmaceuticals) that are suitable for routine application. It is possible to incorporate this protocol into existing automated modules.


Assuntos
Composição de Medicamentos/métodos , Etanol/química , Radioquímica/métodos , Compostos Radiofarmacêuticos/química , Resinas de Troca de Cátion/química , Radioisótopos de Gálio/química , Ácido Clorídrico/química , Marcação por Isótopo , Octreotida/análogos & derivados , Octreotida/química , Controle de Qualidade
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