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Mapping County-Level Exposure and Vulnerability to the US Energy Transition 科技报告
来源:Resources for the Future. 出版年: 2021
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收藏  |  浏览/下载:6/0  |  提交时间:2022/01/14
Dissecting the “spice” of Dune 新闻
来源平台:CNRS News. 发布日期:2021
作者:  admin
收藏  |  浏览/下载:85/0  |  提交时间:2021/10/22
Students from around the world unite to tackle global challenges 新闻
来源平台:Imperial College London. 发布日期:2021
作者:  admin
收藏  |  浏览/下载:12/0  |  提交时间:2021/08/26
Breakthrough could lead to early detection of pregnancy complications 新闻
来源平台:EurekAlert. 发布日期:2021
作者:  admin
收藏  |  浏览/下载:24/0  |  提交时间:2021/05/13
Quantifying fluid retention due to natural vegetation in a forest floodplain analogue using the Aggregated Dead Zone (ADZ) dilution approach 期刊论文
Water Resources Research, 2020
作者:  Paul Carling;  Julian Leyland;  Maarten G. Kleinhans;  Louison Besozzi;  Pierre Duranton;  Hai Trieu;  Roy Teske
收藏  |  浏览/下载:7/0  |  提交时间:2020/06/29
A bedform phase diagram for dense granular currents 期刊论文
NATURE COMMUNICATIONS, 2020, 11 (1)
作者:  Smith, Gregory;  Rowley, Peter;  Williams, Rebecca;  Giordano, Guido;  Trolese, Matteo;  Silleni, Aurora;  Parsons, Daniel R.;  Capon, Samuel
收藏  |  浏览/下载:6/0  |  提交时间:2020/06/16
Late-stage oxidative C(sp(3))-H methylation 期刊论文
NATURE, 2020, 580 (7805) : 621-+
作者:  Fessler, Evelyn;  Eckl, Eva-Maria;  Schmitt, Sabine;  Mancilla, Igor Alves;  Meyer-Bender, Matthias F.;  Hanf, Monika;  Philippou-Massier, Julia;  Krebs, Stefan;  Zischka, Hans;  Jae, Lucas T.
收藏  |  浏览/下载:46/0  |  提交时间:2020/07/03

Frequently referred to as the '  magic methyl effect'  , the installation of methyl groups-especially adjacent (alpha) to heteroatoms-has been shown to dramatically increase the potency of biologically active molecules(1-3). However, existing methylation methods show limited scope and have not been demonstrated in complex settings(1). Here we report a regioselective and chemoselective oxidative C(sp(3))-H methylation method that is compatible with late-stage functionalization of drug scaffolds and natural products. This combines a highly site-selective and chemoselective C-H hydroxylation with a mild, functional-group-tolerant methylation. Using a small-molecule manganese catalyst, Mn(CF3PDP), at low loading (at a substrate/catalyst ratio of 200) affords targeted C-H hydroxylation on heterocyclic cores, while preserving electron-neutral and electron-rich aryls. Fluorine- or Lewis-acid-assisted formation of reactive iminium or oxonium intermediates enables the use of a mildly nucleophilic organoaluminium methylating reagent that preserves other electrophilic functionalities on the substrate. We show this late-stage C(sp(3))-H methylation on 41 substrates housing 16 different medicinally important cores that include electron-rich aryls, heterocycles, carbonyls and amines. Eighteen pharmacologically relevant molecules with competing sites-including drugs (for example, tedizolid) and natural products-are methylated site-selectively at the most electron rich, least sterically hindered position. We demonstrate the syntheses of two magic methyl substrates-an inverse agonist for the nuclear receptor RORc and an antagonist of the sphingosine-1-phosphate receptor-1-via late-stage methylation from the drug or its advanced precursor. We also show a remote methylation of the B-ring carbocycle of an abiraterone analogue. The ability to methylate such complex molecules at late stages will reduce synthetic effort and thereby expedite broader exploration of the magic methyl effect in pursuit of new small-molecule therapeutics and chemical probes.


A manganese-catalysed oxidative C(sp(3))-H methylation method allows a methyl group to be selectively installed into medicinally important heterocycles, providing a way to improve pharmaceuticals and better understand the '  magic methyl effect'  .


  
Climate Destabilization Unlikely to Cause Methane ‘Burp’ 新闻
来源平台:Scripps Institution of Oceanography. 发布日期:2020
作者:  admin
收藏  |  浏览/下载:12/0  |  提交时间:2020/02/24
Preindustrial (CH4)-C-14 indicates greater anthropogenic fossil CH4 emissions 期刊论文
NATURE, 2020, 578 (7795) : 409-+
作者:  Keener, Megan;  Hunt, Camden;  Carroll, Timothy G.;  Kampel, Vladimir;  Dobrovetsky, Roman;  Hayton, Trevor W.;  Menard, Gabriel
收藏  |  浏览/下载:25/0  |  提交时间:2020/05/13

Atmospheric methane (CH4) is a potent greenhouse gas, and its mole fraction has more than doubled since the preindustrial era(1). Fossil fuel extraction and use are among the largest anthropogenic sources of CH4 emissions, but the precise magnitude of these contributions is a subject of debate(2,3). Carbon-14 in CH4 ((CH4)-C-14) can be used to distinguish between fossil (C-14-free) CH4 emissions and contemporaneous biogenic sources  however, poorly constrained direct (CH4)-C-14 emissions from nuclear reactors have complicated this approach since the middle of the 20th century(4,5). Moreover, the partitioning of total fossil CH4 emissions (presently 172 to 195 teragrams CH4 per year)(2,3) between anthropogenic and natural geological sources (such as seeps and mud volcanoes) is under debate  emission inventories suggest that the latter account for about 40 to 60 teragrams CH4 per year(6,7). Geological emissions were less than 15.4 teragrams CH4 per year at the end of the Pleistocene, about 11,600 years ago(8), but that period is an imperfect analogue for present-day emissions owing to the large terrestrial ice sheet cover, lower sea level and extensive permafrost. Here we use preindustrial-era ice core (CH4)-C-14 measurements to show that natural geological CH4 emissions to the atmosphere were about 1.6 teragrams CH4 per year, with a maximum of 5.4 teragrams CH4 per year (95 per cent confidence limit)-an order of magnitude lower than the currently used estimates. This result indicates that anthropogenic fossil CH4 emissions are underestimated by about 38 to 58 teragrams CH4 per year, or about 25 to 40 per cent of recent estimates. Our record highlights the human impact on the atmosphere and climate, provides a firm target for inventories of the global CH4 budget, and will help to inform strategies for targeted emission reductions(9,10).


Isotopic evidence from ice cores indicates that preindustrial-era geological methane emissions were lower than previously thought, suggesting that present-day emissions of methane from fossil fuels are underestimated.


  
Natural acidification changes the timing and rate of succession, alters community structure, and increases homogeneity in marine biofouling communities 期刊论文
GLOBAL CHANGE BIOLOGY, 2018, 24 (1) : E112-E127
作者:  Brown, Norah E. M.;  Milazzo, Marco;  Rastrick, Samuel P. S.;  Hall-Spencer, Jason M.;  Therriault, Thomas W.;  Harley, Christopher D. G.
收藏  |  浏览/下载:11/0  |  提交时间:2019/04/09
climate change  community  marine biodiversity  natural analogue  Ocean acidification