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- Click Step-Growth Polymerization and E/Z Stereochemistry Using Nucleophilic Thiol-yne/-ene Reactions: Applying Old Concepts for Practical Sustainable (Bio)MaterialsWorch, Joshua C.; Dove, Andrew P. (American Chemical Society, 2022-08-25)Polymer sustainability is synonymous with "bioderived polymers" and the zeitgeist of "using renewable feedstocks". However, this sentiment does not adequately encompass the requirements of sustainability in polymers. In addition to recycling considerations and mechanical performance, following green chemistry principles also needs to be maximized to improve the sustainability of polymer synthesis. The synthetic cost (i.e., maximizing atom economy, reducing chemical hazards, and lowering energy requirements) of producing polymers should be viewed as equally important to the monomer source (biomass vs petrol platform chemicals). Therefore, combining the use of renewable feedstocks with efficient syntheses and green chemistry principles is imperative to delivering truly sustainable polymers. The high efficiency, atom economy, and single reaction trajectories that define click chemistry reactions position them as ideal chemical approaches to synthesize polymers in a sustainable manner while simultaneously expanding the structural scope of accessible polymers from sustainably sourced chemicals.Click step-growth polymerization using the thiol-yne Michael addition, a reaction first reported over a century ago, has emerged as an extremely mild and atom-efficient pathway to yield high-performance polymers with controllable E/Z stereochemistry along the polymer backbone. Building on studies of aromatic thiol-yne polymers, around 10 years ago our group began investigating the thiol-yne reaction for the stereocontrolled synthesis of alkene-containing aliphatic polyesters. Our early studies established a convenient path to high-molecular-weight (>100 kDa) E-rich or Z-rich step-growth polymers by judiciously changing the catalyst and/or reaction solvent. This method has since been adapted to synthesize fast-degrading polyesters, high-performance polyamides, and resilient hydrogel biomaterials. Across several systems, we have observed dramatic differences in material properties among polymers with different alkene stereochemistry.We have also explored the analogous thiol-ene Michael reaction to create high-performance poly(ester-urethanes) with precise E/Z stereochemistry. In contrast to the stereoselective thiol-yne polymerization, here the use of monomers with predefined E/Z (geometric) isomerism (arising from either alkenes or the planar rigidity of ring units) affords polymers with total control over stereochemistry. This advancement has enabled the synthesis of tough, degradable materials that are derived from sustainable monomer feedstocks. Employing isomers of sugar-derived isohexides, bicyclic rigid-rings possessing geometric isomerism, led to degradable polymers with fundamentally opposing mechanical behavior (i.e., plastic vs elastic) simply by adjusting the stereochemistry of the isohexide. In this Account, we feature our investigation of thiol-yne/-ene click step-growth polymers and efforts to establish structure-property relationships toward degradable materials with practical mechanical performance in the context of sustainable polymers and/or biomaterials. We have paid attention to installing and controlling geometric isomerism by using these click reactions, an overarching objective of our work in this research area. The exquisite control of geometric isomerism that is possible within polymer backbones, as enabled by convenient click chemistry reactions, showcases a powerful approach to creating multipurpose degradable polymers.
- Fiber-optic SeismologyLindsey, Nathaniel J.; Martin, Eileen R. (2021)Distributed Acoustic Sensing (DAS) is an emerging technology that repurposes a fiber-optic cable as a dense array of strain sensors. This technology repeatedly pings a fiber with laser pulses, measuring optical phase changes in Rayleigh backscattered light. DAS is beneficial for studies of fine-scale processes over multi-kilometer distances, long-term time-lapse monitoring, and deployment in logistically challenging areas (e.g. high temperatures, power limitations, land access barriers). These bene fits have motivated a decade of applications in subsurface imaging and microseismicity monitoring for energy production and carbon sequestration. DAS arrays have recorded microearthquakes, regional earthquakes, teleseisms, and infrastructure signals. Analysis of these wavefields is enabling earthquake seismology where traditional sensors were sparse, as well as structural and near-surface seismology. These studies improved understanding of DAS instrument response through comparison with traditional seismometers. More recently DAS has been used to study cryosphere systems, marine geophysics, geodesy and volcanology. Further advancement of geoscience using DAS requires several community efforts related to instrument access, training, outreach and cyberinfrastructure.
- Fortune Tellers: The Story of America's First Economic Forecasters [Book review]Spanos, Aris (Cambridge University Press, 2015-11-12)
- Hotspot swells revisitedKing, Scott D.; Adam, Claudia (Elsevier, 2014-10-01)The first attempts to quantify the width and height of hotspot swells were made more than 30. years ago. Since that time, topography, ocean-floor age, and sediment thickness datasets have improved considerably. Swell heights and widths have been used to estimate the heat flow from the core-mantle boundary, constrain numerical models of plumes, and as an indicator of the origin of hotspots. In this paper, we repeat the analysis of swell geometry and buoyancy flux for 54. hotspots, including the 37 considered by Sleep (1990) and the 49 considered by Courtillot et al. (2003), using the latest and most accurate data. We are able to calculate swell geometry for a number of hotspots that Sleep was only able to estimate by comparison with other swells. We find that in spite of the increased resolution in global bathymetry models there is significant uncertainty in our calculation of buoyancy fluxes due to differences in our measurement of the swells' width and height, the integration method (volume integration or cross-sectional area), and the variations of the plate velocities between HS2-Nuvel1a (Gripp and Gordon, 1990) and HS3-Nuvel1a (Gripp and Gordon, 2002). We also note that the buoyancy flux for Pacific hotspots is in general larger than for Eurasian, North American, African and Antarctic hotspots. Considering that buoyancy flux is linearly related to plate velocity, we speculate that either the calculation of buoyancy flux using plate velocity over-estimates the actual vertical flow of material from the deep mantle or that convection in the Pacific hemisphere is more vigorous than the Atlantic hemisphere. © 2014 Elsevier B.V.
- A problematic animal fossil from the early Cambrian Hetang Formation, South China - A replyTang, Qing; Hu, Jie; Xie, Guwei; Yuan, Xunlai; Wan, Bin; Zhou, Chuanming; Dong, Xu; Cao, Guohua; Lieberman, Bruce S.; Leys, Sally P.; Xiao, Shuhai (Cambridge University Press, 2019-11-01)We recently reported Cambrowania ovata Tang and Xiao in Tang et al., 2019, from the early Cambrian Hetang Formation in South China and interpreted it as a problematic animal fossil, possibly related to either sponges or bivalved arthropods (Tang et al., 2019). Slater and Budd (2019) contested our taxonomic identification and phylogenetic interpretation; instead, they claimed that Cambrowania ovata is a large acritarch referable to morphotaxon Leiosphaeridia Eisenack, 1958, and thus is not an animal. Here we refute their criticisms, clarify the differences between Cambrowania and Leiosphaeridia and other acritarchs, and reiterate why an animal affinity for Cambrowania cannot be ruled out.
- The viability of SARS-CoV-2 on solid surfacesHosseini, Mohsen; Behzadinasab, Saeed; Benmamoun, Zachary; Ducker, William A. (Elsevier, 2021-10-01)The COVID-19 pandemic had a major impact on life in 2020 and 2021. One method of transmission occurs when the causative virus, SARS-CoV-2, contaminates solids. Understanding and controlling the interaction with solids is thus potentially important for limiting the spread of the disease. We review work that describes the prevalence of the virus on common objects, the longevity of the virus on solids, and surface coatings that are designed to inactivate the virus. Engineered coatings have already succeeded in producing a large reduction in viral infectivity from surfaces. We also review work describing inactivation on facemasks and clothing and discuss probable mechanisms of inactivation of the virus at surfaces.
- What Foundations for Statistical Modeling and Inference?Spanos, Aris (Association Oeconomia, 2019-12-01)