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"Bender, Michael"
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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.
Journal Article
User's guide for the SCID-5-AMPD : structured clinical interview for the DSM-5 alternative model for personality disorders
The paramount tool for the use of SCID-5-AMPD, the User's Guide for the SCID-5-AMPD provides readers with an essential manual to effectively understand and use the three SCID-5-AMPD modules. Integrating an overview of the DSM-5 Alternative Model, this companion guide provides instructions for each SCID-5-AMPD module and features completed samples of all modules in full, with corresponding sample patient cases and commentary-- back cover
Book
Alcohol oxidation as alternative anode reactions paired with (photo)electrochemical fuel production reactions
(Photo)electrochemical cells that produce fuels have often relied on water oxidation to complete the redox cycle. Here, the authors discuss alcohol oxidation as an alternative reaction and consider general mechanistic features of oxidation electrocatalysts.
Journal Article
Two-million-year-old snapshots of atmospheric gases from Antarctic ice
Over the past eight hundred thousand years, glacial–interglacial cycles oscillated with a period of one hundred thousand years (‘100k world’
1
). Ice core and ocean sediment data have shown that atmospheric carbon dioxide, Antarctic temperature, deep ocean temperature, and global ice volume correlated strongly with each other in the 100k world
2
–
6
. Between about 2.8 and 1.2 million years ago, glacial cycles were smaller in magnitude and shorter in duration (‘40k world’
7
). Proxy data from deep-sea sediments suggest that the variability of atmospheric carbon dioxide in the 40k world was also lower than in the 100k world
8
–
10
, but we do not have direct observations of atmospheric greenhouse gases from this period. Here we report the recovery of stratigraphically discontinuous ice more than two million years old from the Allan Hills Blue Ice Area, East Antarctica. Concentrations of carbon dioxide and methane in ice core samples older than two million years have been altered by respiration, but some younger samples are pristine. The recovered ice cores extend direct observations of atmospheric carbon dioxide, methane, and Antarctic temperature (based on the deuterium/hydrogen isotope ratio δD
ice
, a proxy for regional temperature) into the 40k world. All climate properties before eight hundred thousand years ago fall within the envelope of observations from continuous deep Antarctic ice cores that characterize the 100k world. However, the lowest measured carbon dioxide and methane concentrations and Antarctic temperature in the 40k world are well above glacial values from the past eight hundred thousand years. Our results confirm that the amplitudes of glacial–interglacial variations in atmospheric greenhouse gases and Antarctic climate were reduced in the 40k world, and that the transition from the 40k to the 100k world was accompanied by a decline in minimum carbon dioxide concentrations during glacial maxima.
Analysis of two-million-year-old ice from Antarctica provides a direct comparison of atmospheric gas levels before and after the shift from glacial cycles of 100 thousand years to 40-thousand-year cycles around one million years ago.
Journal Article
Review of the state of the art and future prospects of the ground-based GNSS meteorology in Europe
Global navigation satellite systems (GNSSs) have revolutionised positioning, navigation, and timing, becoming a common part of our everyday life. Aside from these well-known civilian and commercial applications, GNSS is now an established atmospheric observing system, which can accurately sense water vapour, the most abundant greenhouse gas, accounting for 60–70 % of atmospheric warming. In Europe, the application of GNSS in meteorology started roughly two decades ago, and today it is a well-established field in both research and operation. This review covers the state of the art in GNSS meteorology in Europe. The advances in GNSS processing for derivation of tropospheric products, application of GNSS tropospheric products in operational weather prediction and application of GNSS tropospheric products for climate monitoring are discussed. The GNSS processing techniques and tropospheric products are reviewed. A summary of the use of the products for validation and impact studies with operational numerical weather prediction (NWP) models as well as very short weather prediction (nowcasting) case studies is given. Climate research with GNSSs is an emerging field of research, but the studies so far have been limited to comparison with climate models and derivation of trends. More than 15 years of GNSS meteorology in Europe has already achieved outstanding cooperation between the atmospheric and geodetic communities. It is now feasible to develop next-generation GNSS tropospheric products and applications that can enhance the quality of weather forecasts and climate monitoring. This work is carried out within COST Action ES1206 advanced global navigation satellite systems tropospheric products for monitoring severe weather events and climate (GNSS4SWEC, http://gnss4swec.knmi.nl).
Journal Article
Atmospheric composition 1 million years ago from blue ice in the Allan Hills, Antarctica
Here, we present direct measurements of atmospheric composition and Antarctic climate from the mid-Pleistocene (∼1 Ma) from ice cores drilled in the Allan Hills blue ice area, Antarctica. The 1-Ma ice is dated from the deficit in ⁴⁰Ar relative to the modern atmosphere and is present as a stratigraphically disturbed 12-m section at the base of a 126-m ice core. The 1-Ma ice appears to represent most of the amplitude of contemporaneous climate cycles and CO ₂ and CH ₄ concentrations in the ice range from 221 to 277 ppm and 411 to 569 parts per billion (ppb), respectively. These concentrations, together with measured δD of the ice, are at the warm end of the field for glacial–interglacial cycles of the last 800 ky and span only about one-half of the range. The highest CO ₂ values in the 1-Ma ice fall within the range of interglacial values of the last 400 ka but are up to 7 ppm higher than any interglacial values between 450 and 800 ka. The lowest CO ₂ values are 30 ppm higher than during any glacial period between 450 and 800 ka. This study shows that the coupling of Antarctic temperature and atmospheric CO ₂ extended into the mid-Pleistocene and demonstrates the feasibility of discontinuously extending the current ice core record beyond 800 ka by shallow coring in Antarctic blue ice areas.
Significance Bubbles of ancient air trapped in ice cores permit the direct reconstruction of atmospheric composition and allow us to link greenhouse gases and global climate over the last 800 ky. Here, we present new ice core records of atmospheric composition roughly 1 Ma from a shallow ice core drilled in the Allan Hills blue ice area, Antarctica. These records confirm that interglacial CO ₂ concentrations decreased by 800 ka. They also show that the link between CO ₂ and Antarctic temperature extended into the warmer world of the mid-Pleistocene.
Journal Article
Reconstructing the last interglacial at Summit, Greenland
The Eemian (last interglacial, 130–115 ka) was likely the warmest of all interglacials of the last 800 ka, with summer Arctic temperatures 3–5 °C above present. Here, we present improved Eemian climate records from central Greenland, reconstructed from the base of the Greenland Ice Sheet Project 2 (GISP2) ice core. Our record comes from clean, stratigraphically disturbed, and isotopically warm ice from 2,750 to 3,040 m depth. The age of this ice is constrained by measuring CH₄ and δ18O of O₂, and comparing with the historical record of these properties from the North Greenland Ice Core Project (NGRIP) and North Greenland Eemian Ice Drilling (NEEM) ice cores. The δ18Oice, δ15N of N₂, and total air content for samples dating discontinuously from 128 to 115 ka indicate a warming of ∼6 °C between 127–121 ka, and a similar elevation history between GISP2 and NEEM. The reconstructed climate and elevation histories are compared with an ensemble of coupled climate-ice-sheet model simulations of the Greenland ice sheet. Those most consistent with the reconstructed temperatures indicate that the Greenland ice sheet contributed 5.1 m (4.1–6.2 m, 95% credible interval) to global eustatic sea level toward the end of the Eemian. Greenland likely did not contribute to anomalously high sea levels at ∼127 ka, or to a rapid jump in sea level at ∼120 ka. However, several unexplained discrepancies remain between the inferred and simulated histories of temperature and accumulation rate at GISP2 and NEEM, as well as between the climatic reconstructions themselves.
Journal Article
Individual and societal risk factors of attitudes justifying intimate partner violence against women: a multilevel cross-sectional study
ObjectivesAttitudes justifying intimate partner violence against women (IPVAW) can play an essential role in explaining the prevalence of such public health problem. The study aim was to explain attitudes justifying IPVAW identifying individual and societal risk factors.Design and settingA multilevel cross-sectional study of the World Values Survey (WVS) in 54 global countries.ParticipantsA representative transnational community-based sample of 81 516 participants (47.8% male, 52.1% female), aged mean of 42.41.MeasuresAttitudes justifying IPVAW, sociodemographic, sexism, self-transcendence and conservation values were measured using questions from WVS. Country and regional gender inequality were assessed by Gender Inequality Index.ResultsAround 16% (intraclass correlation=0.16) of individual differences in attitudes justifying IPVAW are explained by countries. Statistically significant predictors at individual and country level were: sex (B=−0.24, 95% CI −0.27 to −0.22), age (B=−0.08 to −0.25, 95% CI −0.34 to −0.03), marital status (B=0.09 to 0.23, 95% CI 0.002 to 0.33), educational level (B=−0.10 to −0.14, 95% CI −0.20 to −0.04), self-transcendence values (B=−0.10, 95% CI −0.20 to −0.12), sexism (B=0.21, 95% CI 0.15 to 0.28), country (B=2.18, 95% CI 1.09 to 3.26) and regional (B=2.23, 95% CI 1.04 to 3.42) gender inequality. Country gender inequality (B=−0.18, p=0.12) and regional gender inequality (B=−0.21, p=0.10) did not moderate the associations between self-transcendence values and attitudes justifying IPVAW. In the same way for sexism, data did not provide support for a moderating role of country gender inequality (B=0.22, p=0.26) and regional gender inequality (B=0.10, p=0.66).ConclusionsIndividual and country predictors accounted for differences in attitudes justifying IPVAW. However, neither gender inequality of country nor gender inequality of region interacted with sexism and self-transcendence values. Theoretical and methodological implications are discussed.
Journal Article
A potent and broad neutralization of SARS-CoV-2 variants of concern by DARPins
We report the engineering and selection of two synthetic proteins—FSR16m and FSR22—for the possible treatment of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) infection. FSR16m and FSR22 are trimeric proteins composed of DARPin SR16m or SR22 fused with a T4 foldon. Despite selection by a spike protein from a now historical SARS-CoV-2 strain, FSR16m and FSR22 exhibit broad-spectrum neutralization of SARS-CoV-2 strains, inhibiting authentic B.1.351, B.1.617.2 and BA.1.1 viruses, with respective IC
50
values of 3.4, 2.2 and 7.4 ng ml
−1
for FSR16m. Cryo-EM structures revealed that these DARPins recognize a region of the receptor-binding domain (residues 456, 475, 486, 487 and 489) overlapping a critical portion of the angiotensin-converting enzyme 2 (ACE2)-binding surface. K18-hACE2 transgenic mice inoculated with B.1.617.2 and receiving intranasally administered FSR16m showed less weight loss and 10–100-fold lower viral burden in upper and lower respiratory tracts. The strong and broad neutralization potency makes FSR16m and FSR22 promising candidates for the prevention and treatment of infection by SARS-CoV-2.
Homotrimeric DARPin molecules neutralize SARS-CoV-2 variants of concern by targeting a critical ACE2-binding interface.
Journal Article