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Revealing enigmatic mucus structures in the deep sea using DeepPIV 期刊论文
NATURE, 2020, 583 (7814) : 78-+
作者:  Nguyen, Ngoc Uyen Nhi;  Canseco, Diana C.;  Xiao, Feng;  Nakada, Yuji;  Li, Shujuan;  Lam, Nicholas T.;  Muralidhar, Shalini A.;  Savla, Jainy J.;  Hill, Joseph A.;  Le, Victor;  Zidan, Kareem A.;  El-Feky, Hamed W.;  Wang, Zhaoning;  Ahmed, Mahmoud Salama;  Hubbi, Maimon E.;  Menendez-Montes, Ivan
收藏  |  浏览/下载:13/0  |  提交时间:2020/06/09

Advanced deep-sea imaging tools yield insights into the structure and function of mucus filtration houses built by midwater giant larvaceans.


Many animals build complex structures to aid in their survival, but very few are built exclusively from materials that animals create (1,2). In the midwaters of the ocean, mucoid structures are readily secreted by numerous animals, and serve many vital functions(3,4). However, little is known about these mucoid structures owing to the challenges of observing them in the deep sea. Among these mucoid forms, the '  houses'  of larvaceans are marvels of nature(5), and in the ocean twilight zone giant larvaceans secrete and build mucus filtering structures that can reach diameters of more than 1 m(6). Here we describe in situ laser-imaging technology(7) that reconstructs three-dimensional models of mucus forms. The models provide high-resolution views of giant larvacean houses and elucidate the role that house structure has in food capture and predator avoidance. Now that tools exist to study mucus structures found throughout the ocean, we can shed light on some of nature'  s most complex forms.


  
Pore-scale investigation of the use of reactive nanoparticles for in situ remediation of contaminated groundwater source 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (24) : 13366-13373
作者:  Pak, Tannaz;  de Lima Luz, Luiz Fernando, Jr.;  Tosco, Tiziana;  Ruiz Costa, Gabriel Schubert;  Rangel Rosa, Paola Rodrigues;  Archilha, Nathaly Lopes
收藏  |  浏览/下载:10/0  |  提交时间:2020/06/09
NAPL in situ degradation  groundwater remediation  nanoremediation  zero-valent iron nanoparticle  X-ray-computed microtomography  
Relaxation of Wind Stress Drives the Abrupt Onset of Biological Carbon Uptake in the Kerguelen Bloom: A Multisensor Approach 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2020, 47 (9)
作者:  Pellichero, Violaine;  Boutin, Jacqueline;  Claustre, Herve;  Merlivat, Liliane;  Sallee, Jean-baptiste;  Blain, Stephane
收藏  |  浏览/下载:6/0  |  提交时间:2020/07/02
onset of the phytoplankton bloom  mixing-layer depth  in situ high-resolution data  mixed-layer depth  air-sea heat flux  wind stress  
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:11/0  |  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


  
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:88/0  |  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.


  
The first dinosaur egg was soft 期刊论文
NATURE, 2020
作者:  Rodstrom, Karin E. J.;  Kiper, Aytug K.;  Zhang, Wei;  Rinne, Susanne;  Pike, Ashley C. W.;  Goldstein, Matthias;  Conrad, Linus J.;  Delbeck, Martina;  Hahn, Michael G.;  Meier, Heinrich;  Platzk, Magdalena;  Quigley, Andrew;  Speedman, David;  Shrestha, Leela;  Mukhopadhyay, Shubhashish M. M.
收藏  |  浏览/下载:47/0  |  提交时间:2020/07/03

Molecular analyses of newly discovered, embryo-bearing ornithischian and sauropod dinosaur eggs suggest that the ancestral dinosaur egg was soft-shelled, and that hard-shelled eggs evolved independently at least three times in the major dinosaur lineages.


Calcified eggshells protect developing embryos against environmental stress and contribute to reproductive success(1). As modern crocodilians and birds lay hard-shelled eggs, this eggshell type has been inferred for non-avian dinosaurs. Known dinosaur eggshells are characterized by an innermost membrane, an overlying protein matrix containing calcite, and an outermost waxy cuticle(2-7). The calcitic eggshell consists of one or more ultrastructural layers that differ markedly among the three major dinosaur clades, as do the configurations of respiratory pores. So far, only hadrosaurid, a few sauropodomorph and tetanuran eggshells have been discovered  the paucity of the fossil record and the lack of intermediate eggshell types challenge efforts to homologize eggshell structures across all dinosaurs(8-18). Here we present mineralogical, organochemical and ultrastructural evidence for an originally non-biomineralized, soft-shelled nature of exceptionally preserved ornithischianProtoceratopsand basal sauropodomorphMussauruseggs. Statistical evaluation of in situ Raman spectra obtained for a representative set of hard- and soft-shelled, fossil and extant diapsid eggshells clusters the originally organic but secondarily phosphatizedProtoceratopsand the organicMussauruseggshells with soft, non-biomineralized eggshells. Histology corroborates the organic composition of these soft-shelled dinosaur eggs, revealing a stratified arrangement resembling turtle soft eggshell. Through an ancestral-state reconstruction of composition and ultrastructure, we compare eggshells fromProtoceratopsandMussauruswith those from other diapsids, revealing that the first dinosaur egg was soft-shelled. The calcified, hard-shelled dinosaur egg evolved independently at least three times throughout the Mesozoic era, explaining the bias towards eggshells of derived dinosaurs in the fossil record.


  
The Effects of Viewing Geometry on the Spectral Analysis of Lunar Regolith as Inferred by in situ Spectrophotometric Measurements of Chang'E-4 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2020, 47 (8)
作者:  Yang, Yazhou;  Lin, Honglei;  Liu, Yang;  Lin, Yangting;  Wei, Yong;  Hu, Sen;  Yang, Wei;  Xu, Rui;  He, Zhiping;  Zou, Yongliao
收藏  |  浏览/下载:10/0  |  提交时间:2020/07/02
lunar regolith  Chang'  E-4  in situ spectrophotometric measurement  viewing geometry  spectral features  visible and near-infrared  
Noninvasive 2D and 3D Mapping of Root Zone Soil Moisture Through the Detection of Coarse Roots With Ground-Penetrating Radar 期刊论文
WATER RESOURCES RESEARCH, 2020, 56 (5)
作者:  Liu, X.;  Chen, J.;  Butnor, J. R.;  Qin, G.;  Cui, X.;  Fan, B.;  Lin, H.;  Guo, L.
收藏  |  浏览/下载:13/0  |  提交时间:2020/05/13
ecohydrology  in situ  near-surface geophysics  soil mapping  soil-plant-water relationships  subsoil  
Temperate rainforests near the South Pole during peak Cretaceous warmth 期刊论文
NATURE, 2020, 580 (7801) : 81-+
作者:  Johann P. Klages;  Ulrich Salzmann;  Torsten Bickert;  Claus-Dieter Hillenbrand;  Karsten Gohl;  Gerhard Kuhn;  Steven M. Bohaty;  ;  rgen Titschack;  Juliane Mü;  ller;  Thomas Frederichs;  Thorsten Bauersachs;  Werner Ehrmann;  Tina van de Flierdt;  Patric Simõ;  es Pereira;  Robert D. Larter;  Gerrit Lohmann;  Igor Niezgodzki;  Gabriele Uenzelmann-Neben;  Maximilian Zundel;  Cornelia Spiegel;  Chris Mark;  David Chew;  Jane E. Francis;  Gernot Nehrke;  Florian Schwarz;  James A. Smith;  Tim Freudenthal;  Oliver Esper;  Heiko Pä;  like;  Thomas A. Ronge;  Ricarda Dziadek
收藏  |  浏览/下载:12/0  |  提交时间:2020/05/13

The mid-Cretaceous period was one of the warmest intervals of the past 140 million years(1-5), driven by atmospheric carbon dioxide levels of around 1,000 parts per million by volume(6). In the near absence of proximal geological records from south of the Antarctic Circle, it is disputed whether polar ice could exist under such environmental conditions. Here we use a sedimentary sequence recovered from the West Antarctic shelf-the southernmost Cretaceous record reported so far-and show that a temperate lowland rainforest environment existed at a palaeolatitude of about 82 degrees S during the Turonian-Santonian age (92 to 83 million years ago). This record contains an intact 3-metre-long network of in situ fossil roots embedded in a mudstone matrix containing diverse pollen and spores. A climate model simulation shows that the reconstructed temperate climate at this high latitude requires a combination of both atmospheric carbon dioxide concentrations of 1,120-1,680 parts per million by volume and a vegetated land surface without major Antarctic glaciation, highlighting the important cooling effect exerted by ice albedo under high levels of atmospheric carbon dioxide.


  
A general carbonyl alkylative amination for tertiary amine synthesis 期刊论文
NATURE, 2020
作者:  Ouyang, David;  He, Bryan;  Ghorbani, Amirata;  Yuan, Neal;  Ebinger, Joseph;  Langlotz, Curtis P.;  Heidenreich, Paul A.;  Harrington, Robert A.;  Liang, David H.;  Ashley, Euan A.;  Zou, James Y.
收藏  |  浏览/下载:12/0  |  提交时间:2020/07/03

The ubiquity of tertiary alkylamines in pharmaceutical and agrochemical agents, natural products and small-molecule biological probes(1,2) has stimulated efforts towards their streamlined synthesis(3-9). Arguably the most robust method for the synthesis of tertiary alkylamines is carbonyl reductive amination(3), which comprises two elementary steps: the condensation of a secondary alkylamine with an aliphatic aldehyde to form an all-alkyl-iminium ion, which is subsequently reduced by a hydride reagent. Direct strategies have been sought for a '  higher order'  variant of this reaction via the coupling of an alkyl fragment with an alkyl-iminium ion that is generated in situ(10-14). However, despite extensive efforts, the successful realization of a '  carbonyl alkylative amination'  has not yet been achieved. Here we present a practical and general synthesis of tertiary alkylamines through the addition of alkyl radicals to all-alkyl-iminium ions. The process is facilitated by visible light and a silane reducing agent, which trigger a distinct radical initiation step to establish a chain process. This operationally straightforward, metal-free and modular transformation forms tertiary amines, without structural constraint, via the coupling of aldehydes and secondary amines with alkyl halides. The structural and functional diversity of these readily available precursors provides a versatile and flexible strategy for the streamlined synthesis of complex tertiary amines.


The synthesis of tertiary amines is achieved through a carbonyl alkylative amination reaction facilitated by visible light, in which an aldehyde and an amine condense to form an iminium ion that subsequently reacts with alkyl radical.