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1.
Chem Rev ; 122(6): 6795-6849, 2022 03 23.
Artículo en Inglés | MEDLINE | ID: mdl-35263103

RESUMEN

The development and application of trimetallic nanoparticles continues to accelerate rapidly as a result of advances in materials design, synthetic control, and reaction characterization. Following the technological successes of multicomponent materials in automotive exhausts and photovoltaics, synergistic effects are now accessible through the careful preparation of multielement particles, presenting exciting opportunities in the field of catalysis. In this review, we explore the methods currently used in the design, synthesis, analysis, and application of trimetallic nanoparticles across both the experimental and computational realms and provide a critical perspective on the emergent field of trimetallic nanocatalysts. Trimetallic nanoparticles are typically supported on high-surface-area metal oxides for catalytic applications, synthesized via preparative conditions that are comparable to those applied for mono- and bimetallic nanoparticles. However, controlled elemental segregation and subsequent characterization remain challenging because of the heterogeneous nature of the systems. The multielement composition exhibits beneficial synergy for important oxidation, dehydrogenation, and hydrogenation reactions; in some cases, this is realized through higher selectivity, while activity improvements are also observed. However, challenges related to identifying and harnessing influential characteristics for maximum productivity remain. Computation provides support for the experimental endeavors, for example in electrocatalysis, and a clear need is identified for the marriage of simulation, with respect to both combinatorial element screening and optimal reaction design, to experiment in order to maximize productivity from this nascent field. Clear challenges remain with respect to identifying, making, and applying trimetallic catalysts efficiently, but the foundations are now visible, and the outlook is strong for this exciting chemical field.


Asunto(s)
Nanopartículas , Catálisis , Hidrogenación , Nanopartículas/química , Oxidación-Reducción , Óxidos
2.
Faraday Discuss ; 242(0): 193-211, 2023 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-36189732

RESUMEN

A number of Pd based materials have been synthesised and evaluated as catalysts for the conversion of carbon dioxide and hydrogen to methanol, a useful platform chemical and hydrogen storage molecule. Monometallic Pd catalysts show poor methanol selectivity, but this is improved through the formation of Pd alloys, with both PdZn and PdGa alloys showing greatly enhanced methanol productivity compared with monometallic Pd/Al2O3 and Pd/TiO2 catalysts. Catalyst characterisation shows that the 1 : 1 ß-PdZn alloy is present in all Zn containing post-reaction samples, including PdZn/Ga2O3, with the Pd2Ga alloy formed for the Pd/Ga2O3 sample. The heat of mixing was calculated for a variety of alloy compositions with high values determined for both PdZn and Pd2Ga alloys, at ca. -0.6 eV per atom and ca. -0.8 eV per atom, respectively. However, ZnO is more readily reduced than Ga2O3, providing a possible explanation for the preferential formation of the PdZn alloy, rather than PdGa, when in the presence of Ga2O3.

3.
Lancet Microbe ; 5(4): e335-e344, 2024 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-38484748

RESUMEN

BACKGROUND: The origin of novel SARS-CoV-2 spike sequences found in wastewater, without corresponding detection in clinical specimens, remains unclear. We sought to determine the origin of one such cryptic wastewater lineage by tracking and characterising its persistence and genomic evolution over time. METHODS: We first detected a cryptic lineage, WI-CL-001, in municipal wastewater in Wisconsin, USA, in January, 2022. To determine the source of WI-CL-001, we systematically sampled wastewater from targeted sub-sewershed lines and maintenance holes using compositing autosamplers. Viral concentrations in wastewater samples over time were measured by RT digital PCR. In addition to using metagenomic 12s rRNA sequencing to determine the virus's host species, we also sequenced SARS-CoV-2 spike receptor binding domains, and, where possible, whole viral genomes to identify and characterise the evolution of this lineage. FINDINGS: We traced WI-CL-001 to its source at a single commercial building. There we detected the cryptic lineage at concentrations as high as 2·7 × 109 genome copies per L. The majority of 12s rRNA sequences detected in wastewater leaving the identified source building were human. Additionally, we generated over 100 viral receptor binding domain and whole-genome sequences from wastewater samples containing the cryptic lineage collected over the 13 consecutive months this virus was detectable (January, 2022, to January, 2023). These sequences contained a combination of fixed nucleotide substitutions characteristic of Pango lineage B.1.234, which circulated in humans in Wisconsin at low levels from October, 2020, to February, 2021. Despite this, mutations in the spike gene and elsewhere resembled those subsequently found in omicron variants. INTERPRETATION: We propose that prolonged detection of WI-CL-001 in wastewater indicates persistent shedding of SARS-CoV-2 from a single human initially infected by an ancestral B.1.234 virus. The accumulation of convergent omicron-like mutations in WI-CL-001's ancestral B.1.234 genome probably reflects persistent infection and extensive within-host evolution. People who shed cryptic lineages could be an important source of highly divergent viruses that sporadically emerge and spread. FUNDING: The Rockefeller Foundation, Wisconsin Department of Health Services, Centers for Disease Control and Prevention, National Institute on Drug Abuse, and the Center for Research on Influenza Pathogenesis and Transmission.


Asunto(s)
COVID-19 , Aguas Residuales , Estados Unidos , Humanos , SARS-CoV-2/genética , COVID-19/epidemiología , Centers for Disease Control and Prevention, U.S.
4.
Mar Genomics ; 37: 1-17, 2018 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-28970064

RESUMEN

The biodiversity, ecosystem services and climate variability of the Antarctic continent and the Southern Ocean are major components of the whole Earth system. Antarctic ecosystems are driven more strongly by the physical environment than many other marine and terrestrial ecosystems. As a consequence, to understand ecological functioning, cross-disciplinary studies are especially important in Antarctic research. The conceptual study presented here is based on a workshop initiated by the Research Programme Antarctic Thresholds - Ecosystem Resilience and Adaptation of the Scientific Committee on Antarctic Research, which focussed on challenges in identifying and applying cross-disciplinary approaches in the Antarctic. Novel ideas and first steps in their implementation were clustered into eight themes. These ranged from scale problems, through risk maps, and organism/ecosystem responses to multiple environmental changes and evolutionary processes. Scaling models and data across different spatial and temporal scales were identified as an overarching challenge. Approaches to bridge gaps in Antarctic research programmes included multi-disciplinary monitoring, linking biomolecular findings and simulated physical environments, as well as integrative ecological modelling. The results of advanced cross-disciplinary approaches can contribute significantly to our knowledge of Antarctic and global ecosystem functioning, the consequences of climate change, and to global assessments that ultimately benefit humankind.


Asunto(s)
Organismos Acuáticos/fisiología , Ecosistema , Investigación Interdisciplinaria , Regiones Antárticas , Biodiversidad , Cambio Climático , Congresos como Asunto , Ecología , Genómica
5.
Puesta día urgenc. emerg. catastr ; 9(2): 67-77, abr.-jun. 2009. ilus
Artículo en Español | IBECS (España) | ID: ibc-74864

RESUMEN

Los sanitarios que asisten heridos en medios hostiles ,como cuevas, precisan de una formación específica que sumen tres aspectos fundamentales: uno es la práctica de una medicina de urgencia de calidad a realizar en la cavidad, sin apoyos y en un medio totalmente ajeno al sanitario habitual que se define como 'difícil, hostil y aislado', otro la capacidad física y los conocimientos técnicos necesarios para poder acceder, por difícil que sea hasta el lugar donde se encuentra el accidentado, para prestarle asistencia sanitaria y, finalmente, la formación necesaria para colaborar con los equipos de rescate, plenamente integrado en ellos, haciéndose cargo al completo de los aspectos médicos y colaborando eficazmente en las tareas de rescate, sin suponer un estorbo, ni un peligro añadido para sus operativos. Es decir, que estos sanitarios deben ser buenos especialistas en medicina de urgencia, acreditados espeleólogos y aceptables rescatadores en los operativos de rescate. Algo que no es fácil de conseguir, pero que es necesario si pretendemos asumir con garantías el reto de la medicalización del rescate en cavidades(AU)


The sanitary staff that assists injured men in hostile enviroments as caves, need a specific formation that should add three fundamental aspects: one is the practice of a medicine of quality urgency to practice in the cavity, without supports and in a way completely foreign to the sanitary habitual one that is defined as 'difficult, hostile and outlying', another one is the physical capacity and the necessary technical knowledge to be able to gain access, for difficult that is up to the place where the eventful one is it, not even a danger added for his operative ones gives him sanitary and, assistance finally, the necessary formation to collaborate with the rescue teams, fully integrated to them, taking charge to the finished one of the medical aspects and collaborating effectively in therescue works, without supposing an obstacle. That is to say, that sanitary staff must be good specialists in medicine of urgency, accredited speleologists and acceptable rescuers. Something that is not easy to obtain, but that is necessary if we try to assume with guarantees the challenge of the medicalization of the rescue in cavities(AU)


Asunto(s)
Humanos , Masculino , Femenino , Medicina de Emergencia/métodos , Servicio de Urgencia en Hospital , Trabajo de Rescate/tendencias , Trabajo de Rescate , Personal de Rescate , Búsqueda y Rescate
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