Hydrogen energy-based electrochemical energy conversion technologies offer the promise of enabling a transition of the global energy landscape from fossil fuels to renewable energy. Here, we present ...a comprehensive review of the fundamentals of electrocatalysis in alkaline media and applications in alkaline-based energy technologies, particularly alkaline fuel cells and water electrolyzers. Anion exchange (alkaline) membrane fuel cells (AEMFCs) enable the use of nonprecious electrocatalysts for the sluggish oxygen reduction reaction (ORR), relative to proton exchange membrane fuel cells (PEMFCs), which require Pt-based electrocatalysts. However, the hydrogen oxidation reaction (HOR) kinetics is significantly slower in alkaline media than in acidic media. Understanding these phenomena requires applying theoretical and experimental methods to unravel molecular-level thermodynamics and kinetics of hydrogen and oxygen electrocatalysis and, particularly, the proton-coupled electron transfer (PCET) process that takes place in a proton-deficient alkaline media. Extensive electrochemical and spectroscopic studies, on single-crystal Pt and metal oxides, have contributed to the development of activity descriptors, as well as the identification of the nature of active sites, and the rate-determining steps of the HOR and ORR. Among these, the structure and reactivity of interfacial water serve as key potential and pH-dependent kinetic factors that are helping elucidate the origins of the HOR and ORR activity differences in acids and bases. Additionally, deliberately modulating and controlling catalyst-support interactions have provided valuable insights for enhancing catalyst accessibility and durability during operation. The design and synthesis of highly conductive and durable alkaline membranes/ionomers have enabled AEMFCs to reach initial performance metrics equal to or higher than those of PEMFCs. We emphasize the importance of using membrane electrode assemblies (MEAs) to integrate the often separately pursued/optimized electrocatalyst/support and membranes/ionomer components.
methods, at multiscales, and
simulations provide a mechanistic understanding of electron, ion, and mass transport at catalyst/ionomer/membrane interfaces and the necessary guidance to achieve fuel cell operation in air over thousands of hours. We hope that this Review will serve as a roadmap for advancing the scientific understanding of the fundamental factors governing electrochemical energy conversion in alkaline media with the ultimate goal of achieving ultralow Pt or precious-metal-free high-performance and durable alkaline fuel cells and related technologies.
Transfusion-related acute lung injury is suggested to be a “2-hit” event resulting from priming and activation of pulmonary neutrophils. Activation may result from infusion of ...lysophosphatidylcholines (LysoPCs), which accumulate during storage of blood products. In the present study, we developed a syngeneic in vivo transfusion model to test whether storage of platelet concentrates (PLTs) results in lung injury in healthy rats as well as in a “2-hit” model using lipopolysaccharide-pretreated rats. In addition, the effect of washing of platelets was studied. In healthy rats, transfusion of aged PLTs caused mild lung inflammation. In LPS-pretreated rats, transfusion of aged PLTs, but not fresh PLTs, augmented pulmonary systemic coagulopathy. When PLTs components were transfused separately, supernatant of aged PLTs, but not washed aged platelets, induced pulmonary injury in the “2-hit” model. Supernatants of aged PLTs contained increased concentrations of LysoPCs compared with fresh PLTs, which enhanced neutrophil priming activity in vitro. We conclude that transfusion of aged PLTs induces lung inflammation in healthy rats. In a “2-hit” model, aged PLTs contribute to pulmonary and systemic coagulopathy, which may be mediated by LysoPCs, which accumulate in the supernatant of PLTs during storage.
We investigate the dependence of black hole accretion rate (BHAR) on host-galaxy star formation rate (SFR) and stellar mass (M*) in the CANDELS/GOODS-South field in the redshift range of . Our sample ...consists of galaxies, allowing us to probe galaxies with and/or . We use sample-mean BHAR to approximate long-term average BHAR. Our sample-mean BHARs are derived from the Chandra Deep Field-South 7 Ms observations, while the SFRs and M* have been estimated by the CANDELS team through spectral energy distribution fitting. The average BHAR is correlated positively with both SFR and M*, and the BHAR-SFR and BHAR-M* relations can both be described acceptably by linear models with a slope of unity. However, BHAR appears to be correlated more strongly with M* than SFR. This result indicates that M* is the primary host-galaxy property related to supermassive black hole (SMBH) growth, and the apparent BHAR-SFR relation is largely a secondary effect due to the star-forming main sequence. Among our sources, massive galaxies ( ) have significantly higher BHAR/SFR ratios than less massive galaxies, indicating that the former have higher SMBH fueling efficiency and/or higher SMBH occupation fraction than the latter. Our results can naturally explain the observed proportionality between and M* for local giant ellipticals and suggest that their is higher than that of local star-forming galaxies. Among local star-forming galaxies, massive systems might have higher compared to dwarfs.
The French Revolution brought principles of “liberty, equality, fraternity” to bear on the day-to-day challenges of governing what was then the largest country in Europe. Its experiments provided a ...model for future revolutions and democracies across the globe, but this first modern revolution had no model to follow. Using reconstructed transcripts of debates held in the Revolution’s first parliament, we present a quantitative analysis of how this body managed innovation. We use information theory to track the creation, transmission, and destruction of word-use patterns across over 40,000 speeches and a thousand speakers. The parliament as a whole was biased toward the adoption of new patterns, but speakers’ individual qualities could break these overall trends. Speakers on the left innovated at higher rates, while speakers on the right acted to preserve prior patterns. Key players such as Robespierre (on the left) and Abbé Maury (on the right) played information-processing roles emblematic of their politics. Newly created organizational functions—such as the Assembly president and committee chairs—had significant effects on debate outcomes, and a distinct transition appears midway through the parliament when committees, external to the debate process, gained new powers to “propose and dispose.” Taken together, these quantitative results align with existing qualitative interpretations, but also reveal crucial information-processing dynamics that have hitherto been overlooked. Great orators had the public’s attention, but deputies (mostly on the political left) who mastered the committee system gained new powers to shape revolutionary legislation.
Abstract
Mass communication over social media can drive rapid changes in our sense of collective identity. Hashtags in particular have acted as powerful social coordinators, playing a key role in ...organizing social movements like the Gezi park protests, Occupy Wall Street,
#metoo
, and
#blacklivesmatter
. Here we quantify collective identity from the use of hashtags as self-labels in over 85,000 actively-maintained Twitter user profiles spanning 2017–2019. Collective identities emerge from a graph model of individuals’ overlapping self-labels, producing a hierarchy of graph clusters. Each cluster is bound together and characterized semantically by specific hashtags key to its formation. We define and apply two information-theoretic measures to quantify the strength of identities in the hierarchy. First we measure collective identity coherence to determine how integrated any identity is from local to global scales. Second, we consider the conspicuousness of any identity given its vocabulary versus the global identity map. Our work reveals a rich landscape of online identity emerging from the hierarchical alignment of uncoordinated self-labeling actions.
There is increasing evidence that many risk loci found using genome-wide association studies are molecular quantitative trait loci (QTLs). Here we introduce a new set of functional annotations based ...on causal posterior probabilities of fine-mapped molecular cis-QTLs, using data from the Genotype-Tissue Expression (GTEx) and BLUEPRINT consortia. We show that these annotations are more strongly enriched for heritability (5.84× for eQTLs; P = 1.19 × 10
) across 41 diseases and complex traits than annotations containing all significant molecular QTLs (1.80× for expression (e)QTLs). eQTL annotations obtained by meta-analyzing all GTEx tissues generally performed best, whereas tissue-specific eQTL annotations produced stronger enrichments for blood- and brain-related diseases and traits. eQTL annotations restricted to loss-of-function intolerant genes were even more enriched for heritability (17.06×; P = 1.20 × 10
). All molecular QTLs except splicing QTLs remained significantly enriched in joint analysis, indicating that each of these annotations is uniquely informative for disease and complex trait architectures.
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