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Molecular tuning of CO2-to-ethylene conversion 期刊论文
NATURE, 2020, 577 (7791) : 509-+
作者:  Li, Fengwang;  39;Brien, Colin P.
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

The electrocatalytic reduction of carbon dioxide, powered by renewable electricity, to produce valuable fuels and feedstocks provides a sustainable and carbon-neutral approach to the storage of energy produced by intermittent renewable sources(1). However, the highly selective generation of economically desirable products such as ethylene from the carbon dioxide reduction reaction (CO2RR) remains a challenge(2). Tuning the stabilities of intermediates to favour a desired reaction pathway can improve selectivity(3-5), and this has recently been explored for the reaction on copper by controlling morphology(6), grain boundaries(7), facets(8), oxidation state(9) and dopants(10). Unfortunately, the Faradaic efficiency for ethylene is still low in neutral media (60 per cent at a partial current density of 7 milliamperes per square centimetre in the best catalyst reported so far(9)), resulting in a low energy efficiency. Here we present a molecular tuning strategy-the functionalization of the surface of electrocatalysts with organic molecules-that stabilizes intermediates for more selective CO2RR to ethylene. Using electrochemical, operando/in situ spectroscopic and computational studies, we investigate the influence of a library of molecules, derived by electro-dimerization of arylpyridiniums(11), adsorbed on copper. We find that the adhered molecules improve the stabilization of an '  atop-bound'  CO intermediate (that is, an intermediate bound to a single copper atom), thereby favouring further reduction to ethylene. As a result of this strategy, we report the CO2RR to ethylene with a Faradaic efficiency of 72 per cent at a partial current density of 230 milliamperes per square centimetre in a liquid-electrolyte flow cell in a neutral medium. We report stable ethylene electrosynthesis for 190 hours in a system based on a membrane-electrode assembly that provides a full-cell energy efficiency of 20 per cent. We anticipate that this may be generalized to enable molecular strategies to complement heterogeneous catalysts by stabilizing intermediates through local molecular tuning.


Electrocatalytic reduction of CO2 over copper can be made highly selective by '  tuning'  the copper surface with adsorbed organic molecules to stabilize intermediates for carbon-based fuels such as ethylene


  
Fluid Surface Coverage Showing the Controls of Rock Mineralogy on the Wetting State 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2020, 47 (8)
作者:  Garfi, Gaetano;  John, Cedric M.;  Lin, Qingyang;  Berg, Steffen;  Krevor, Samuel
收藏  |  浏览/下载:17/0  |  提交时间:2020/07/02
wettability  mineralogy  X-ray micro-CT  fluid surface coverage  wettability alteration  multiphase flow  
Resistance Formulations in Shallow Overland Flow Along a Hillslope Covered With Patchy Vegetation 期刊论文
WATER RESOURCES RESEARCH, 2020, 56 (5)
作者:  Crompton, Octavia;  Katul, Gabriel G.;  Thompson, Sally
收藏  |  浏览/下载:20/0  |  提交时间:2020/05/13
surface roughness  overland flow  hydraulic resistance  hillslope hydrology  friction coefficients  
Liquid flow and control without solid walls 期刊论文
NATURE, 2020, 581 (7806) : 58-+
作者:  Hellmuth, Susanne;  Stemmann, Olaf
收藏  |  浏览/下载:51/0  |  提交时间:2020/07/03

Wall-free liquid channels surrounded by an immiscible magnetic liquid can be used to create liquid circuitry or to transport human blood without damaging the blood cells by moving permanent magnets.


When miniaturizing fluidic circuitry, the solid walls of the fluid channels become increasingly important(1) because they limit the flow rates achievable for a given pressure drop, and they are prone to fouling(2). Approaches for reducing the wall interactions include hydrophobic coatings(3), liquid-infused porous surfaces(4-6), nanoparticle surfactant jamming(7), changes to surface electronic structure(8), electrowetting(9,10), surface tension pinning(11,12) and use of atomically flat channels(13). A better solution may be to avoid the solid walls altogether. Droplet microfluidics and sheath flow achieve this but require continuous flow of the central liquid and the surrounding liquid(1,14). Here we demonstrate an approach in which aqueous liquid channels are surrounded by an immiscible magnetic liquid, both of which are stabilized by a quadrupolar magnetic field. This creates self-healing, non-clogging, anti-fouling and near-frictionless liquid-in-liquid fluidic channels. Manipulation of the field provides flow control, such as valving, splitting, merging and pumping. The latter is achieved by moving permanent magnets that have no physical contact with the liquid channel. We show that this magnetostaltic pumping method can be used to transport whole human blood with very little damage due to shear forces. Haemolysis (rupture of blood cells) is reduced by an order of magnitude compared with traditional peristaltic pumping, in which blood is mechanically squeezed through a plastic tube. Our liquid-in-liquid approach provides new ways to transport delicate liquids, particularly when scaling channels down to the micrometre scale, with no need for high pressures, and could also be used for microfluidic circuitry.


  
Estimating meltwater retention and associated nitrate redistribution during snowmelt in an Arctic tundra landscape 期刊论文
ENVIRONMENTAL RESEARCH LETTERS, 2020, 15 (3)
作者:  Westergaard-Nielsen, Andreas;  Balstrom, Thomas;  Treier, Urs A.;  Normand, Signe;  Elberling, Bo
收藏  |  浏览/下载:34/0  |  提交时间:2020/07/02
nitrate  arctic  snow water equivalents  UAV  hydrology  surface flow  snow volume  
Filling the Void: The Effect of Stream Bank Soil Pipes on Transient Hyporheic Exchange During a Peak Flow Event 期刊论文
WATER RESOURCES RESEARCH, 2020, 56 (2)
作者:  Lotts, William Seth;  Hester, Erich T.
收藏  |  浏览/下载:23/0  |  提交时间:2020/07/02
riparian  floodplains  surface-groundwater interaction  groundwater modeling  preferential flow  saturated flow  
The guidance receptor plexin D1 is a mechanosensor in endothelial cells 期刊论文
NATURE, 2020, 578 (7794) : 290-+
作者:  Ma, Wenchuan;  Lutsko, James F.;  Rimer, Jeffrey D.;  Vekilov, Peter G.
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

PLXND1 is a mechanosensor that is required for endothelial cells to respond to shear stress both in vitro and in vivo by regulating the site-specific distribution of atherosclerotic lesions.


Shear stress on arteries produced by blood flow is important for vascular development and homeostasis but can also initiate atherosclerosis(1). Endothelial cells that line the vasculature use molecular mechanosensors to directly detect shear stress profiles that will ultimately lead to atheroprotective or atherogenic responses(2). Plexins are key cell-surface receptors of the semaphorin family of cell-guidance signalling proteins and can regulate cellular patterning by modulating the cytoskeleton and focal adhesion structures(3-5). However, a role for plexin proteins in mechanotransduction has not been examined. Here we show that plexin D1 (PLXND1) has a role in mechanosensation and mechanically induced disease pathogenesis. PLXND1 is required for the response of endothelial cells to shear stress in vitro and in vivo and regulates the site-specific distribution of atherosclerotic lesions. In endothelial cells, PLXND1 is a direct force sensor and forms a mechanocomplex with neuropilin-1 and VEGFR2 that is necessary and sufficient for conferring mechanosensitivity upstream of the junctional complex and integrins. PLXND1 achieves its binary functions as either a ligand or a force receptor by adopting two distinct molecular conformations. Our results establish a previously undescribed mechanosensor in endothelial cells that regulates cardiovascular pathophysiology, and provide a mechanism by which a single receptor can exhibit a binary biochemical nature.


  
Mass balance of the Greenland Ice Sheet from 1992 to 2018 期刊论文
NATURE, 2020, 579 (7798) : 233-+
作者:  Scudellari, Megan
收藏  |  浏览/下载:31/0  |  提交时间:2020/04/16

The Greenland Ice Sheet has been a major contributor to global sea-level rise in recent decades(1,2), and it is expected to continue to be so(3). Although increases in glacier flow(4-6) and surface melting(7-9) have been driven by oceanic(10-12) and atmospheric(13,14) warming, the magnitude and trajectory of the ice sheet'  s mass imbalance remain uncertain. Here we compare and combine 26 individual satellite measurements of changes in the ice sheet'  s volume, flow and gravitational potential to produce a reconciled estimate of its mass balance. The ice sheet was close to a state of balance in the 1990s, but annual losses have risen since then, peaking at 345 +/- 66 billion tonnes per year in 2011. In all, Greenland lost 3,902 +/- 342 billion tonnes of ice between 1992 and 2018, causing the mean sea level to rise by 10.8 +/- 0.9 millimetres. Using three regional climate models, we show that the reduced surface mass balance has driven 1,964 +/- 565 billion tonnes (50.3 per cent) of the ice loss owing to increased meltwater runoff. The remaining 1,938 +/- 541 billion tonnes (49.7 per cent) of ice loss was due to increased glacier dynamical imbalance, which rose from 46 +/- 37 billion tonnes per year in the 1990s to 87 +/- 25 billion tonnes per year since then. The total rate of ice loss slowed to 222 +/- 30 billion tonnes per year between 2013 and 2017, on average, as atmospheric circulation favoured cooler conditions(15) and ocean temperatures fell at the terminus of Jakobshavn Isbr AE(16). Cumulative ice losses from Greenland as a whole have been close to the rates predicted by the Intergovernmental Panel on Climate Change for their high-end climate warming scenario(17), which forecast an additional 70 to 130 millimetres of global sea-level rise by 2100 compared with their central estimate.


  
Influence of December snow cover over North America on January surface air temperature over the midlatitude Asia 期刊论文
INTERNATIONAL JOURNAL OF CLIMATOLOGY, 2019
作者:  Li, Jingyi;  Li, Fei;  He, Shengping;  Wang, Huijun;  Orsolini, Yvan J.
收藏  |  浏览/下载:25/0  |  提交时间:2019/11/27
eddy-mean flow interaction  midlatitude Asia surface air temperature  North American snow cover  Rossby wave train  
Theoretical Analysis of Groundwater Flow Patterns Near Stagnation Points 期刊论文
WATER RESOURCES RESEARCH, 2019, 55 (2) : 1624-1650
作者:  Bresciani, Etienne;  Kang, Peter K.;  Lee, Seunghak
收藏  |  浏览/下载:13/0  |  提交时间:2019/11/26
groundwater flow patterns  stagnation point  dividing streamline  dividing stream surface  Darcy flow  flow topology