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918 result(s) for "Goetz, K."
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Predictive control of selective secondary alcohol oxidation of glycerol on NiOOH
Many biomass intermediates are polyols and selectively oxidizing only a primary or secondary alcohol group is beneficial for the valorization of these intermediates. For example, production of 1,3-dihydroxyacetone, a highly valuable oxidation product of glycerol, requires selective secondary alcohol oxidation. However, selective secondary alcohol oxidation is challenging due to its steric disadvantage. This study demonstrates that NiOOH, which oxidizes alcohols via two dehydrogenation mechanisms, hydrogen atom transfer and hydride transfer, can convert glycerol to 1,3-dihydroxyacetone with high selectivity when the conditions are controlled to promote hydrogen atom transfer, favoring secondary alcohol oxidation. This rational production of 1,3-dihydroxyacetone achieved by selectively enabling one desired dehydrogenation pathway, without requiring alteration of catalyst composition, demonstrates how comprehensive mechanistic understanding can enable predictive control over selectivity. While valuable chemicals can be obtained from biomass electro-oxidation, the mechanisms can be challenging to discern. Here, authors show that explicit control of electrochemical dehydrogenation mechanisms enables selective secondary alcohol oxidation of glycerol to produce 1,3-dihydroxyacetone.
Convolutional networks for supervised mining of molecular patterns within cellular context
Cryo-electron tomograms capture a wealth of structural information on the molecular constituents of cells and tissues. We present DeePiCt (deep picker in context), an open-source deep-learning framework for supervised segmentation and macromolecular complex localization in cryo-electron tomography. To train and benchmark DeePiCt on experimental data, we comprehensively annotated 20 tomograms of Schizosaccharomyces pombe for ribosomes, fatty acid synthases, membranes, nuclear pore complexes, organelles, and cytosol. By comparing DeePiCt to state-of-the-art approaches on this dataset, we show its unique ability to identify low-abundance and low-density complexes. We use DeePiCt to study compositionally distinct subpopulations of cellular ribosomes, with emphasis on their contextual association with mitochondria and the endoplasmic reticulum. Finally, applying pre-trained networks to a HeLa cell tomogram demonstrates that DeePiCt achieves high-quality predictions in unseen datasets from different biological species in a matter of minutes. The comprehensively annotated experimental data and pre-trained networks are provided for immediate use by the community. DeePiCt (deep picker in context) is a versatile, open-source deep-learning framework for supervised segmentation and localization of subcellular organelles and biomolecular complexes in cryo-electron tomography.
A modular platform for automated cryo-FIB workflows
Lamella micromachining by focused ion beam milling at cryogenic temperature (cryo-FIB) has matured into a preparation method widely used for cellular cryo-electron tomography. Due to the limited ablation rates of low Ga + ion beam currents required to maintain the structural integrity of vitreous specimens, common preparation protocols are time-consuming and labor intensive. The improved stability of new-generation cryo-FIB instruments now enables automated operations. Here, we present an open-source software tool, SerialFIB, for creating automated and customizable cryo-FIB preparation protocols. The software encompasses a graphical user interface for easy execution of routine lamellae preparations, a scripting module compatible with available Python packages, and interfaces with three-dimensional correlative light and electron microscopy (CLEM) tools. SerialFIB enables the streamlining of advanced cryo-FIB protocols such as multi-modal imaging, CLEM-guided lamella preparation and in situ lamella lift-out procedures. Our software therefore provides a foundation for further development of advanced cryogenic imaging and sample preparation protocols.
Interplanetary dust detection by radio antennas: Mass calibration and fluxes measured by STEREO/WAVES
We analyze dust impacts recorded by the S/WAVES radio instrument onboard the two STEREO spacecraft near 1 A.U. during the period 2007–2010. The impact of a dust particle on a spacecraft produces a plasma cloud whose associated electric field can be detected by on‐board electric antennas. For this study we use the electric potential time series recorded by the waveform sampler of the instrument. The high time resolution and long sampling times of this measurement enable us to deduce considerably more information than in previous studies based on the dynamic power spectra provided by the same instrument or by radio instruments onboard other spacecraft. The large detection area compared to conventional dust detectors provides flux data with a better statistics. We show that the dust‐generated signals are of two kinds, corresponding to impacts of dust from distinctly different mass ranges. We propose calibration formulas for these signals and show that we are able to use S/WAVES as a dust detector with convincing results both in the nanometer and micrometer size ranges. In the latter, the orbital motion of the spacecraft enables us to distinguish between interstellar and interplanetary dust components. Our measurements cover the mass intervals ∼10−22–10−20 kg and ∼10−17 − 5 × 10−16 kg. The flux of the larger dust agrees with measurements of other instruments on different spacecraft. Key Points We expose a technique to use radio instruments as dust detectors We analyze the data from the STEREO/WAVES radio and plasma wave instrument We obtain results in agreement with current interplanetary dust flux models
Observations of electromagnetic whistler precursors at supercritical interplanetary shocks
We present observations of electromagnetic precursor waves, identified as whistler mode waves, at supercritical interplanetary shocks using the Wind search coil magnetometer. The precursors propagate obliquely with respect to the local magnetic field, shock normal vector, solar wind velocity, and they are not phase standing structures. All are right‐hand polarized with respect to the magnetic field (spacecraft frame), and all but one are right‐hand polarized with respect to the shock normal vector in the normal incidence frame. They have rest frame frequencies fci < f ≪ fce and wave numbers 0.02 ≲ kρce ≲ 5.0. Particle distributions show signatures of specularly reflected gyrating ions, which may be a source of free energy for the observed modes. In one event, we simultaneously observe perpendicular ion heating and parallel electron acceleration, consistent with wave heating/acceleration due to these waves. Although the precursors can have δB/Bo as large as 2, fluxgate magnetometer measurements show relatively laminar shock transitions in three of the four events. Key Points Whistler precursors observed at supercritical interplanetary shocks They can have amplitudes >/=20 nT and/or dB/B up to 2 They cause perpendicular (parallel) ion (electron) heating (acceleration)
Large-amplitude electrostatic waves observed at a supercritical interplanetary shock
We present the first observations at an interplanetary shock of large-amplitude (> 100 mV/m pk-pk) solitary waves and large-amplitude (approx.30 mV/m pk-pk) waves exhibiting characteristics consistent with electron Bernstein waves. The Bernstein-like waves show enhanced power at integer and half-integer harmonics of the cyclotron frequency with a broadened power spectrum at higher frequencies, consistent with the electron cyclotron drift instability. The Bernstein-like waves are obliquely polarized with respect to the magnetic field but parallel to the shock normal direction. Strong particle heating is observed in both the electrons and ions. The observed heating and waveforms are likely due to instabilities driven by the free energy provided by reflected ions at this supercritical interplanetary shock. These results offer new insights into collisionless shock dissipation and wave-particle interactions in the solar wind.
Switching to Lowercase Messaging: A Capital Idea
It's not just what you say; it's how you type it. Capitalizing every letter in a water utility's billing statement might turn out to be a turn-off for customers and could obscure a utility's good intentions.
Why Surveys Work and How They Can Disappoint
Not only can a carefully written survey retrieve a wealth of information and customer sentiment; it is a way for a utility to control how a message is communicated.
Freezing-in orientational disorder induces crossover from thermally-activated to temperature-independent transport in organic semiconductors
The crystalline structure of organic materials dictates their physical properties, but while significant research effort is geared towards understanding structure–property relationships in such materials, the details remain unclear. Many organic crystals exhibit transitions in their electrical properties as a function of temperature. One example is the 1:1 charge-transfer complex trans -stilbene—2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane. Here we show that the mobility and resistivity of this material undergo a transition from being thermally activated at temperatures above 235 K to being temperature independent at low temperatures. On the basis of our experimental and theoretical results, we attribute this behaviour to the presence of a glass-like transition and the accompanied freezing-in of orientational disorder of the stilbene molecule. The electronic properties of organic charge-transfer complexes are highly coupled to their crystallographic structures. Goetz et al. show that the librational motion can mediate a glass-like transition, resulting in a transition from temperature-activated to temperature-independent charge transport.
Secrets, Rumors, and the Cost-Effectiveness of Truth
Rumors can have a detrimental effect if a water utility does not effectively and proactively dispel them before they spread.