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Rapid growth of new atmospheric particles by nitric acid and ammonia condensation 期刊论文
NATURE, 2020, 581 (7807) : 184-+
作者:  Liang, Guanxiang;  Zhao, Chunyu;  Zhang, Huanjia;  Mattei, Lisa;  Sherrill-Mix, Scott;  Bittinger, Kyle;  Kessler, Lyanna R.;  Wu, Gary D.;  Baldassano, Robert N.;  DeRusso, Patricia;  Ford, Eileen;  Elovitz, Michal A.;  Kelly, Matthew S.;  Patel, Mohamed Z.;  Mazhani, Tiny;  Gerber, Jeffrey S.;  Kelly, Andrea;  Zemel, Babette S.;  Bushman, Frederic D.
收藏  |  浏览/下载:41/0  |  提交时间:2020/05/20

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog(1,2), but how it occurs in cities is often puzzling(3). If the growth rates of urban particles are similar to those found in cleaner environments (1-10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below -15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid-base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms(4,5).


  
Quantitative detection of iodine in the stratosphere 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (4) : 1860-1866
作者:  Koenig, Theodore K.;  Baidar, Sunil;  Campuzano-Jost, Pedro;  Cuevas, Carlos A.;  Dix, Barbara;  Fernandez, Rafael P.;  Guo, Hongyu;  Hall, Samuel R.;  Kinnison, Douglas;  Nault, Benjamin A.;  Ullmann, Kirk;  Jimenez, Jose L.;  Saiz-Lopez, Alfonso;  Volkamer, Rainer
收藏  |  浏览/下载:24/0  |  提交时间:2020/05/13
iodine  UTLS  stratospheric ozone  gas phase  heterogeneous chemistry  
Hidden diversity of vacancy networks in Prussian blue analogues 期刊论文
NATURE, 2020, 578 (7794) : 256-+
作者:  Hendrickx, N. W.;  Franke, D. P.;  Sammak, A.;  Scappucci, G.;  Veldhorst, M.
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

Prussian blue analogues (PBAs) are a diverse family of microporous inorganic solids, known for their gas storage ability(1), metal-ion immobilization(2), proton conduction(3), and stimuli-dependent magnetic(4,5), electronic(6) and optical(7) properties. This family of materials includes the double-metal cyanide catalysts(8,9) and the hexacyanoferrate/ hexacyanomanganate battery materials(10,11). Central to the various physical properties of PBAs is their ability to reversibly transport mass, a process enabled by structural vacancies. Conventionally presumed to be random(12,13), vacancy arrangements are crucial because they control micropore-network characteristics, and hence the diffusivity and adsorption profiles(14,15). The long-standing obstacle to characterizing the vacancy networks of PBAs is the inaccessibility of single crystals(16). Here we report the growth of single crystals of various PBAs and the measurement and interpretation of their X-ray diffuse scattering patterns. We identify a diversity of non-random vacancy arrangements that is hidden from conventional crystallographic powder analysis. Moreover, we explain this unexpected phase complexity in terms of a simple microscopic model that is based on local rules of electroneutrality and centrosymmetry. The hidden phase boundaries that emerge demarcate vacancynetwork polymorphs with very different micropore characteristics. Our results establish a foundation for correlated defect engineering in PBAs as a means of controlling storage capacity, anisotropy and transport efficiency.


  
Shale Gas Well, Hydraulic Fracturing, and Formation Data to Support Modeling of Gas and Water Flow in Shale Formations 期刊论文
WATER RESOURCES RESEARCH, 2018, 54 (4) : 3196-3206
作者:  Edwards, Ryan W. J.;  Celia, Michael A.
收藏  |  浏览/下载:15/0  |  提交时间:2019/04/09
shale gas  hydraulic fracturing  fracking  two-phase flow  numerical modeling  groundwater  
Hourly composition of gas and particle phase pollutants at a central urban background site in Milan, Italy 期刊论文
ATMOSPHERIC RESEARCH, 2017, 186
作者:  Bigi, A.;  Bianchi, F.;  De Gennaro, G.;  Di Gilio, A.;  Fermo, P.;  Ghermandi, G.;  Prevot, A. S. H.;  Urbani, M.;  Valli, G.;  Vecchi, R.;  Piazzalunga, A.
收藏  |  浏览/下载:13/0  |  提交时间:2019/04/09
PM2.5  Hourly ionic composition  Gas-phase pollutants  Po valley