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Accelerated discovery of CO2 electrocatalysts using active machine learning 期刊论文
NATURE, 2020, 581 (7807) : 178-+
作者:  Lan, Jun;  Ge, Jiwan;  Yu, Jinfang;  Shan, Sisi;  Zhou, Huan;  Fan, Shilong;  Zhang, Qi;  Shi, Xuanling;  Wang, Qisheng;  Zhang, Linqi;  Wang, Xinquan
收藏  |  浏览/下载:89/0  |  提交时间:2020/07/03

The rapid increase in global energy demand and the need to replace carbon dioxide (CO2)-emitting fossil fuels with renewable sources have driven interest in chemical storage of intermittent solar and wind energy(1,2). Particularly attractive is the electrochemical reduction of CO2 to chemical feedstocks, which uses both CO2 and renewable energy(3-8). Copper has been the predominant electrocatalyst for this reaction when aiming for more valuable multi-carbon products(9-16), and process improvements have been particularly notable when targeting ethylene. However, the energy efficiency and productivity (current density) achieved so far still fall below the values required to produce ethylene at cost-competitive prices. Here we describe Cu-Al electrocatalysts, identified using density functional theory calculations in combination with active machine learning, that efficiently reduce CO2 to ethylene with the highest Faradaic efficiency reported so far. This Faradaic efficiency of over 80 per cent (compared to about 66 per cent for pure Cu) is achieved at a current density of 400 milliamperes per square centimetre (at 1.5 volts versus a reversible hydrogen electrode) and a cathodic-side (half-cell) ethylene power conversion efficiency of 55 +/- 2 per cent at 150 milliamperes per square centimetre. We perform computational studies that suggest that the Cu-Al alloys provide multiple sites and surface orientations with near-optimal CO binding for both efficient and selective CO2 reduction(17). Furthermore, in situ X-ray absorption measurements reveal that Cu and Al enable a favourable Cu coordination environment that enhances C-C dimerization. These findings illustrate the value of computation and machine learning in guiding the experimental exploration of multi-metallic systems that go beyond the limitations of conventional single-metal electrocatalysts.


  
A pause in Southern Hemisphere circulation trends due to the Montreal Protocol 期刊论文
NATURE, 2020, 579 (7800) : 544-548
作者:  Imai, Yu;  Meyer, Kirsten J.;  Iinishi, Akira;  Favre-Godal, Quentin;  Green, Robert;  Manuse, Sylvie;  Caboni, Mariaelena;  Mori, Miho;  Niles, Samantha;  Ghiglieri, Meghan;  Honrao, Chandrashekhar;  Ma, Xiaoyu;  Guo, Jason J.;  Makriyannis, Alexandros;  Linares-Otoya, Luis;  Boehringer, Nils;  Wuisan, Zerlina G.;  Kaur, Hundeep;  Wu, Runrun;  Mateus, Andre
收藏  |  浏览/下载:20/0  |  提交时间:2020/05/13

Observations show robust near-surface trends in Southern Hemisphere tropospheric circulation towards the end of the twentieth century, including a poleward shift in the mid-latitude jet(1,2), a positive trend in the Southern Annular Mode(1,3-6) and an expansion of the Hadley cell(7,8). It has been established that these trends were driven by ozone depletion in the Antarctic stratosphere due to emissions of ozone-depleting substances(9-11). Here we show that these widely reported circulation trends paused, or slightly reversed, around the year 2000. Using a pattern-based detection and attribution analysis of atmospheric zonal wind, we show that the pause in circulation trends is forced by human activities, and has not occurred owing only to internal or natural variability of the climate system. Furthermore, we demonstrate that stratospheric ozone recovery, resulting from the Montreal Protocol, is the key driver of the pause. Because pre-2000 circulation trends have affected precipitation(12-14), and potentially ocean circulation and salinity(15-17), we anticipate that a pause in these trends will have wider impacts on the Earth system. Signatures of the effects of the Montreal Protocol and the associated stratospheric ozone recovery might therefore manifest, or have already manifested, in other aspects of the Earth system.


  
Nightside condensation of iron in an ultrahot giant exoplanet 期刊论文
NATURE, 2020, 580 (7805) : 597-+
作者:  Lu, Zhihao;  Zou, Jianling;  Li, Shuang;  Topper, Michael J.;  Tao, Yong;  Zhang, Hao;  Jiao, Xi;  Xie, Wenbing;  Kong, Xiangqian;  Vaz, Michelle;  Li, Huili;  Cai, Yi;  Xia, Limin;  Huang, Peng;  Rodgers, Kristen;  Lee, Beverly;  Riemer, Joanne B.;  Day, Chi-Ping;  Yen, Ray-Whay Chiu;  Cui, Ying;  Wang, Yujiao;  Wang, Yanni;  Zhang, Weiqiang;  Easwaran, Hariharan;  Hulbert, Alicia;  Kim, KiBem;  Juergens, Rosalyn A.;  Yang, Stephen C.;  Battafarano, Richard J.;  Bush, Errol L.;  Broderick, Stephen R.;  Cattaneo, Stephen M.;  Brahmer, Julie R.;  Rudin, Charles M.;  Wrangle, John;  Mei, Yuping;  Kim, Young J.;  Zhang, Bin;  Wang, Ken Kang-Hsin;  Forde, Patrick M.;  Margolick, Joseph B.;  Nelkin, Barry D.;  Zahnow, Cynthia A.;  Pardoll, Drew M.;  Housseau, Franck;  Baylin, Stephen B.;  Shen, Lin;  Brock, Malcolm V.
收藏  |  浏览/下载:58/0  |  提交时间:2020/07/03

Ultrahot giant exoplanets receive thousands of times Earth'  s insolation(1,2). Their high-temperature atmospheres (greater than 2,000 kelvin) are ideal laboratories for studying extreme planetary climates and chemistry(3-5). Daysides are predicted to be cloud-free, dominated by atomic species(6) and much hotter than nightsides(5,7,8). Atoms are expected to recombine into molecules over the nightside(9), resulting in different day and night chemistries. Although metallic elements and a large temperature contrast have been observed(10-14), no chemical gradient has been measured across the surface of such an exoplanet. Different atmospheric chemistry between the day-to-night ('  evening'  ) and night-to-day ('  morning'  ) terminators could, however, be revealed as an asymmetric absorption signature during transit(4,7,15). Here we report the detection of an asymmetric atmospheric signature in the ultrahot exoplanet WASP-76b. We spectrally and temporally resolve this signature using a combination of high-dispersion spectroscopy with a large photon-collecting area. The absorption signal, attributed to neutral iron, is blueshifted by -11 +/- 0.7 kilometres per second on the trailing limb, which can be explained by a combination of planetary rotation and wind blowing from the hot dayside(16). In contrast, no signal arises from the nightside close to the morning terminator, showing that atomic iron is not absorbing starlight there. We conclude that iron must therefore condense during its journey across the nightside.


Absorption lines of iron in the dayside atmosphere of an ultrahot giant exoplanet disappear after travelling across the nightside, showing that the iron has condensed during its travel.


  
Untangling the formation and liberation of water in the lunar regolith 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (23) : 11165-11170
作者:  Zhu, Cheng;  Crandall, Parker B.;  Gillis-Davis, Jeffrey J.;  Ishii, Hope A.;  Bradley, John P.;  Corley, Laura M.;  Kaiser, Ralf I.
收藏  |  浏览/下载:7/0  |  提交时间:2019/11/27
solar wind  water  Moon  
Precession modulation of the South Pacific westerly wind belt over the past million years 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (47) : 23455-23460
作者:  Frank Lamy;  John C. H. Chiang;  Gema Martínez-Méndez;  Mieke Thierens;  Helge W. Arz;  Joyce Bosmans;  Dierk Hebbeln;  Fabrice Lambert;  Lester Lembke-Jene;  and Jan-Berend Stuut
收藏  |  浏览/下载:11/0  |  提交时间:2019/11/27
orbital cycles  southern westerly wind belt  quaternary  paleoclimate  
Geophysical potential for wind energy over the open oceans 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2017, 114 (43) : 11338-11343
作者:  Possner, Anna;  Caldeira, Ken
收藏  |  浏览/下载:8/0  |  提交时间:2019/11/27
wind power  geophysical generation limits  offshore wind  atmosphere-turbine interactions  storm tracks  
Katabatic winds diminish precipitation contribution to the Antarctic ice mass balance 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2017, 114 (41) : 10858-10863
作者:  Grazioli, Jacopo;  Madeleine, Jean-Baptiste;  Gallee, Hubert .;  Forbes, Richard M.;  Genthon, Christophe;  Krinner, Gerhard;  Berne, Alexis
收藏  |  浏览/下载:8/0  |  提交时间:2019/11/27
Antarctica  precipitation sublimation  katabatic wind  
Role of co-occurring competition and facilitation in plant spacing hydrodynamics in water-limited environments 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2017, 114 (35) : 9379-9384
作者:  Trautz, Andrew C.;  Illangasekare, Tissa H.;  Rodriguez-Iturbe, Ignacio
收藏  |  浏览/下载:15/0  |  提交时间:2019/11/27
plant-plant interactions  plant spacing hydrodynamics  soil-plant-atmosphere continuum  porous media-wind tunnel experimentation