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Full-Text Articles in Physical Sciences and Mathematics

No Evidence For Trace Metal Limitation On Anaerobic Carbon Mineralization In Three Peatland Soils, Jason K. Keller, Jillian Wade Nov 2017

No Evidence For Trace Metal Limitation On Anaerobic Carbon Mineralization In Three Peatland Soils, Jason K. Keller, Jillian Wade

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Peatlands store roughly one-third of the terrestrial soil carbon and release the potent greenhouse gas methane (CH4) to the atmosphere, making these wetlands among the most important ecosystems in the global carbon cycle. Despite their importance, the controls of anaerobic decomposition of organic matter to carbon dioxide (CO2) and CH4 within peatlands are not well understood. It is known, however, that the enzymes responsible for CH4 production require cobalt, iron and nickel, and there is a growing appreciation for the potential role of trace metal limitation in anaerobic decomposition. To explore the possibility of …


Phase Behavior Of Binary And Polydisperse Suspensions Of Compressible Microgels Controlled By Selective Particle Deswelling, A. Scotti, U. Gasser, E. S. Herman, Jun Han, A. Menzel, L. Andrew Lyon, A. Fernandez-Nieves Sep 2017

Phase Behavior Of Binary And Polydisperse Suspensions Of Compressible Microgels Controlled By Selective Particle Deswelling, A. Scotti, U. Gasser, E. S. Herman, Jun Han, A. Menzel, L. Andrew Lyon, A. Fernandez-Nieves

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

We investigate the phase behavior of suspensions of poly(N-isopropylacrylamide) (pNIPAM) microgels with either bimodal or polydisperse size distribution. We observe a shift of the fluid-crystal transition to higher concentrations depending on the polydispersity or the fraction of large particles in suspension. Crystallization is observed up to polydispersities as high as 18.5%, and up to a number fraction of large particles of 29% in bidisperse suspensions. The crystal structure is random hexagonal close-packed as in monodisperse pNIPAM microgel suspensions.We explain our experimental results by considering the effect of bound counterions. Above a critical particle concentration, these cause deswelling of the largest …


Estimation Of Bubble-Mediated Air–Sea Gas Exchange From Concurrent Dms And Co2 Transfer Velocities At Intermediate–High Wind Speeds, Thomas G. Bell, Sebastian Landwehr, Scott D. Miller, Warren J. De Bruyn, Adrian H. Callaghan, Brian Scanlon, Brian Ward, Mingxi Yang, Eric S. Saltzman Jul 2017

Estimation Of Bubble-Mediated Air–Sea Gas Exchange From Concurrent Dms And Co2 Transfer Velocities At Intermediate–High Wind Speeds, Thomas G. Bell, Sebastian Landwehr, Scott D. Miller, Warren J. De Bruyn, Adrian H. Callaghan, Brian Scanlon, Brian Ward, Mingxi Yang, Eric S. Saltzman

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Simultaneous air–sea fluxes and concentration differences of dimethylsulfide (DMS) and carbon dioxide (CO2/ were measured during a summertime North Atlantic cruise in 2011. This data set reveals significant differences between the gas transfer velocities of these two gases (1kw/ over a range of wind speeds up to 21ms􀀀1. These differences occur at and above the approximate wind speed threshold when waves begin breaking. Whitecap fraction (a proxy for bubbles) was also measured and has a positive relationship with 1kw, consistent with enhanced bubble-mediated transfer of the less soluble CO2 relative to that of the more soluble DMS. However, the correlation …


Oligo(Ethylene Glycol)-Sidechain Microgels Prepared In Absence Of Cross-Linking Agent: Polymerization, Characterization And Variation Of Particle Deformability, Nicole Welsch, L. Andrew Lyon Jul 2017

Oligo(Ethylene Glycol)-Sidechain Microgels Prepared In Absence Of Cross-Linking Agent: Polymerization, Characterization And Variation Of Particle Deformability, Nicole Welsch, L. Andrew Lyon

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

We present a systematic study of self-cross-linked microgels formed by precipitation polymerization of oligo ethylene glycol methacrylates. The cross-linking density of these microgels and, thus, the network flexibility can be easily tuned through the modulation of the reaction temperature during polymerization. Microgels prepared in absence of any difunctional monomer, i.e. cross-linker, show enhanced deformability and particle spreading on solid surfaces as compared to microgels cross-linked with varying amounts of poly(ethylene glycol diacrylate) (PEG-DA) in addition to self-crosslinking. Particles prepared at low reaction temperatures exhibit the highest degree of spreading due to the lightly cross-linked and flexible polymer network. Moreover, AFM …


Hydrogenation Of Organic Matter As A Terminal Electron Sink Sustains High Co2:Ch4 Production Ratios During Anaerobic Decomposition, Rachel M. Wilson, Malak M. Tfaily, Virginia I. Rich, Jason K. Keller, Scott D. Bridgham, Cassandra Medvedeff Zalman, Laura Meredith, Paul J. Hanson, Mark Hines, Laurel Pfeifer-Meister, Scott R. Saleska, Patrick Crill, William T. Cooper, Jeff P. Chanton, Joel E. Kostka Jul 2017

Hydrogenation Of Organic Matter As A Terminal Electron Sink Sustains High Co2:Ch4 Production Ratios During Anaerobic Decomposition, Rachel M. Wilson, Malak M. Tfaily, Virginia I. Rich, Jason K. Keller, Scott D. Bridgham, Cassandra Medvedeff Zalman, Laura Meredith, Paul J. Hanson, Mark Hines, Laurel Pfeifer-Meister, Scott R. Saleska, Patrick Crill, William T. Cooper, Jeff P. Chanton, Joel E. Kostka

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Once inorganic electron acceptors are depleted, organic matter in anoxic environments decomposes by hydrolysis, fermentation, and methanogenesis, requiring syntrophic interactions between microorganisms to achieve energetic favorability. In this classic anaerobic food chain, methanogenesis represents the terminal electron accepting (TEA) process, ultimately producing equimolar CO2 and CH4 for each molecule of organic matter degraded. However, CO2:CH4 production in Sphagnum-derived, mineral-poor, cellulosic peat often substantially exceeds this 1:1 ratio, even in the absence of measureable inorganic TEAs. Since the oxidation state of C in both cellulose-derived organic matter and acetate is 0, and CO2 has …


Application Of Bottlebrush Block Copolymers As Photonic Crystals, Allegra L. Liberman-Martin, Crystal K. Chu, Robert H. Grubbs May 2017

Application Of Bottlebrush Block Copolymers As Photonic Crystals, Allegra L. Liberman-Martin, Crystal K. Chu, Robert H. Grubbs

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

Brush block copolymers are a class of comb polymers that feature polymeric side chains densely grafted to a linear backbone. These polymers display interesting properties due to their dense functionality, low entanglement, and ability to rapidly self-assemble to highly ordered nanostructures. The ability to prepare brush polymers with precise structures has been enabled by advancements in controlled polymerization techniques. This Feature Article highlights the development of brush block copolymers as photonic crystals that can reflect visible to near-infrared wavelengths of light. Fabrication of these materials relies on polymer self-assembly processes to achieve nanoscale ordering, which allows for the rapid preparation …


Catalysis In Real Time Using X-Ray Lasers, A. Nilsson, Jerry L. Larue, H. Öberg, H. Ogasawara, M. Dell’Angela, M. Beye, H. Öström, J. Gladh, J. K. Nørskov, W. Wurth, F. Abild-Pedersen, L. G. M. Pettersson Feb 2017

Catalysis In Real Time Using X-Ray Lasers, A. Nilsson, Jerry L. Larue, H. Öberg, H. Ogasawara, M. Dell’Angela, M. Beye, H. Öström, J. Gladh, J. K. Nørskov, W. Wurth, F. Abild-Pedersen, L. G. M. Pettersson

Biology, Chemistry, and Environmental Sciences Faculty Articles and Research

We describe how the unique temporal and spectral characteristics of X-ray free-electron lasers (XFEL) can be utilized to follow chemical transformations in heterogeneous catalysis in real time. We highlight the systematic study of CO oxidation on Ru(0001), which we initiate either using a femtosecond pulse from an optical laser or by activating only the oxygen atoms using a THz pulse. We find that CO is promoted into an entropy-controlled precursor state prior to desorbing when the surface is heated in the absence of oxygen, whereas in the presence of oxygen, CO desorbs directly into the gas phase. We monitor the …