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1.
Phys Chem Chem Phys ; 25(45): 30761-30784, 2023 Nov 22.
Artículo en Inglés | MEDLINE | ID: mdl-37830239

RESUMEN

Batteries and electrochemical capacitors (ECs) are of critical importance for applications such as electric vehicles, electric grids, and mobile devices. However, the performance of existing battery and EC technologies falls short of meeting the requirements of high energy/high power and long durability for increasing markets such as the automotive industry, aerospace, and grid-storage utilizing renewable energies. Therefore, improving energy storage materials performance metrics is imperative. In the past two decades, radiation has emerged as a new means to modify functionalities in energy storage materials. There exists a common misconception that radiation with energetic ions and electrons will always cause radiation damage to target materials, which might potentially prevent its applications in electrochemical energy storage systems. But in this review, we summarize recent progress in radiation effects on materials for electrochemical energy storage systems to show that radiation can have both beneficial and detrimental effects on various types of energy materials. Prior work suggests that fundamental understanding toward the energy loss mechanisms that govern the resulting microstructure, defect generation, interfacial properties, mechanical properties, and eventual electrochemical properties is critical. We discuss radiation effects in the following categories: (1) defect engineering, (2) interface engineering, (3) radiation-induced degradation, and (4) radiation-assisted synthesis. We analyze the significant trends and provide our perspectives and outlook on current research and future directions in research seeking to harness radiation as a method for enhancing the synthesis and performance of battery materials.

2.
J Am Chem Soc ; 145(30): 16538-16547, 2023 Aug 02.
Artículo en Inglés | MEDLINE | ID: mdl-37466049

RESUMEN

Solid-electrolyte interphases (SEIs) in advanced rechargeable batteries ensure reversible electrode reactions at extreme potentials beyond the thermodynamic stability limits of electrolytes by insulating electrons while allowing the transport of working ions. Such selective ion transport occurs naturally in biological cell membranes as a ubiquitous prerequisite of many life processes and a foundation of biodiversity. In addition, cell membranes can selectively open and close the ion channels in response to external stimuli (e.g., electrical, chemical, mechanical, and thermal), giving rise to "gating" mechanisms that help manage intracellular reactions. We wondered whether the chemistry and structure of SEIs can mimic those of cell membranes, such that ion gating can be replicated. That is, can SEIs realize a reversible switching between two electrochemical behaviors, i.e., the ion intercalation chemistry of batteries and the ion adsorption of capacitors? Herein, we report such SEIs that result in thermally activated selective ion transport. The function of open/close gate switches is governed by the chemical and structural dynamics of SEIs under different thermal conditions, with precise behaviors as conducting and insulating interphases that enable battery and capacitive processes within a finite temperature window. Such an ion gating function is synergistically contributed by Arrhenius-activated ion transport and SEI dissolution/regrowth. Following the understanding of this new mechanism, we then develop an electrochemical method to heal the SEI layer in situ. The knowledge acquired in this work reveals the possibility of hitherto unknown biomimetic properties of SEIs, which will guide us to leverage such complexities to design better SEIs for future battery chemistries.

3.
ACS Energy Lett ; 6(11): 4023-4054, 2021 Nov 12.
Artículo en Inglés | MEDLINE | ID: mdl-34805527

RESUMEN

As a promising alternative to the market-leading lithium-ion batteries, low-cost sodium-ion batteries (SIBs) are attractive for applications such as large-scale electrical energy storage systems. The energy density, cycling life, and rate performance of SIBs are fundamentally dependent on dynamic physiochemical reactions, structural change, and morphological evolution. Therefore, it is essential to holistically understand SIBs reaction processes, degradation mechanisms, and thermal/mechanical behaviors in complex working environments. The recent developments of advanced in situ and operando characterization enable the establishment of the structure-processing-property-performance relationship in SIBs under operating conditions. This Review summarizes significant recent progress in SIBs exploiting in situ and operando techniques based on X-ray and electron analyses at different time and length scales. Through the combination of spectroscopy, imaging, and diffraction, local and global changes in SIBs can be elucidated for improving materials design. The fundamental principles and state-of-the-art capabilities of different techniques are presented, followed by elaborative discussions of major challenges and perspectives.

4.
Small ; 17(52): e2105292, 2021 Dec.
Artículo en Inglés | MEDLINE | ID: mdl-34716757

RESUMEN

The presence and stability of solid electrolyte interphase (SEI) on graphitic electrodes is vital to the performance of lithium-ion batteries (LIBs). However, the formation and evolution of SEI remain the least understood area in LIBs due to its dynamic nature, complexity in chemical composition, heterogeneity in morphology, as well as lack of reliable in situ/operando techniques for accurate characterization. In addition, chemical composition and morphology of SEI are not only affected by the choice of electrolyte, but also by the nature of the electrode surface. While introduction of defects into graphitic electrodes has promoted their electrochemical properties, how such structural defects influence SEI formation and evolution remains an open question. Here, utilizing nondestructive operando electrochemical atomic force microscopy (EChem-AFM) the dynamic SEI formation and evolution on a pair of representative graphitic materials with and without defects, namely, highly oriented pyrolytic and disordered graphite electrodes, are systematically monitored and compared. Complementary to the characterization of SEI topographical and mechanical changes during electrochemical cycling by EChem-AFM, chemical analysis and theoretical calculations are conducted to provide mechanistic insights underlying SEI formation and evolution. The results provide guidance to engineer functional SEIs through design of carbon materials with defects for LIBs and beyond.

5.
Front Psychol ; 12: 701189, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-34367026

RESUMEN

In adapting to remote emergency teaching modes during pandemic-imposed conditions, teachers' instruction has changed dramatically. Early research indicates that the well-being of music teachers has suffered during the COVID-19 pandemic and that high levels of depression are widespread. The purpose of this survey study was to assess the continued psychological well-being of music teachers working amid a global pandemic based upon previous research we conducted during the Spring 2020 semester when most teachers in the United States were forced into emergency remote teaching. A secondary purpose was to explore the ways that pandemic conditions have affected music teachers' sense of safety at work and their current teaching situations. Our questionnaire consisted of sections pertaining to (1) demographic and institutional information, (2) well-being and depression, (3) instructional format and preparedness, (4) teaching efficacy compared to the start of the pandemic, and (5) potential positive outcomes of the pandemic-imposed adjustments. In total, 1,325 music teachers responded to our survey. Overall, the participants reported poorer well-being than both published norms and the sample of participants in our previous study. In addition, 17% reported mild depression, 25% reported moderate depression, and 24% reported severe extremely severe levels of depression. Summaries of the participants instructional experiences and their implications for music education are discussed within.

6.
Mol Biochem Parasitol ; 142(2): 177-83, 2005 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-15876462

RESUMEN

The transcriptional repertoire of the in vivo liver stage of Plasmodium has remained largely unidentified and seemingly not amenable to traditional molecular analysis because of the small number of parasites and large number of uninfected hepatocytes. We have overcome this obstruction by utilizing laser capture microdissection to provide a high quality source of parasite mRNA for the construction of a liver stage cDNA library. Sequencing and annotation of this library demonstrated expression of 623 different Plasmodium yoelii genes during development in the hepatocyte. Of these genes, 25% appear to be unique to the liver stage. This is the first comprehensive analysis of in vivo gene expression undertaken for the liver stage of P. yoelii, and provides insights into the differential expression of P. yoelii genes during this critical stage of development.


Asunto(s)
Regulación del Desarrollo de la Expresión Génica , Hígado/parasitología , Malaria/parasitología , Plasmodium yoelii/crecimiento & desarrollo , Proteínas Protozoarias/metabolismo , Animales , Etiquetas de Secuencia Expresada , Biblioteca de Genes , Hepatocitos/parasitología , Hígado/citología , Ratones , Ratones Endogámicos BALB C , Plasmodium yoelii/genética , Plasmodium yoelii/metabolismo , Proteínas Protozoarias/genética , Reacción en Cadena de la Polimerasa de Transcriptasa Inversa , Transcripción Genética
7.
Genome Res ; 14(10B): 2076-82, 2004 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-15489329

RESUMEN

Large-scale functional genomics studies for malaria vaccine and drug development will depend on the generation of molecular tools to study protein expression. We examined the feasibility of a high-throughput cloning approach using the Gateway system to create a large set of expression clones encoding Plasmodium falciparum single-exon genes. Master clones and their ORFs were transferred en masse to multiple expression vectors. Target genes (n = 303) were selected using specific sets of criteria, including stage expression and secondary structure. Upon screening four colonies per capture reaction, we achieved 84% cloning efficiency. The genes were subcloned in parallel into three expression vectors: a DNA vaccine vector and two protein expression vectors. These transfers yielded a 100% success rate without any observed recombination based on single colony screening. The functional expression of 95 genes was evaluated in mice with DNA vaccine constructs to generate antibody against various stages of the parasite. From these, 19 induced antibody titers against the erythrocytic stages and three against sporozoite stages. We have overcome the potential limitation of producing large P. falciparum clone sets in multiple expression vectors. This approach represents a powerful technique for the production of molecular reagents for genome-wide functional analysis of the P. falciparum genome and will provide for a resource for the malaria resource community distributed through public repositories.


Asunto(s)
Antígenos de Protozoos/genética , Clonación Molecular/métodos , Vacunas contra la Malaria/genética , Plasmodium falciparum/genética , Plasmodium falciparum/inmunología , Recombinación Genética , Animales , Anticuerpos Antiprotozoarios/sangre , ADN Protozoario/genética , Genoma de Protozoos , Hígado/parasitología , Malaria/inmunología , Malaria/parasitología , Malaria/prevención & control , Vacunas contra la Malaria/administración & dosificación , Vacunas contra la Malaria/farmacología , Ratones , Plásmidos/genética , Plasmodium falciparum/crecimiento & desarrollo , Reacción en Cadena de la Polimerasa , Proteínas Recombinantes/genética , Proteínas Recombinantes/aislamiento & purificación , Proteínas Recombinantes/metabolismo , Vacunas de ADN/administración & dosificación , Vacunas de ADN/genética , Vacunas de ADN/farmacología
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