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A scalable method for preparing Cu electrocatalysts that convert CO2 into C2+ products 期刊论文
NATURE COMMUNICATIONS, 2020, 11 (1)
作者:  Kim, Taehee;  Palmore, G. Tayhas R.
收藏  |  浏览/下载:4/0  |  提交时间:2020/07/21
In situ X-ray diffraction of silicate liquids and glasses under dynamic and static compression to megabar pressures 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (22) : 11981-11986
作者:  Morard, Guillaume;  Hernandez, Jean-Alexis;  Guarguaglini, Marco;  Bolis, Riccardo;  Benuzzi-Mounaix, Alessandra;  Vinci, Tommaso;  Fiquet, Guillaume;  Baron, Marzena A.;  Shim, Sang Heon;  Ko, Byeongkwan;  Gleason, Arianna E.;  Mao, Wendy L.;  Alonso-Mori, Roberto;  Lee, Hae Ja;  Nagler, Bob;  Galtier, Eric;  Sokaras, Dimosthenis;  Glenzer, Siegfried H.;  Andrault, Denis;  Garbarino, Gaston;  Mezouar, Mohamed;  Schuster, Anja K.;  Ravasio, Alessandra
收藏  |  浏览/下载:11/0  |  提交时间:2020/05/20
amorphous silicates  high pressure  shock compression  static compression  XFEL diffraction  
Phase Transition of Enstatite-Ferrosilite Solid Solutions at High Pressure and High Temperature: Constraints on Metastable Orthopyroxene in Cold Subduction 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2020, 47 (12)
作者:  Xu, Jingui;  Fan, Dawei;  Zhang, Dongzhou;  Guo, Xinzhuan;  Zhou, Wenge;  Dera, Przemyslaw K.
收藏  |  浏览/下载:8/0  |  提交时间:2020/05/13
Diagenetic to incipient metamorphic zones of the Benton Uplift, Ouachita Orogen, Arkansas, USA 期刊论文
GEOLOGICAL SOCIETY OF AMERICA BULLETIN, 2020, 132 (5-6) : 977-986
作者:  Johnson, Harold E., II;  Wiltschko, David, V;  Harris, John P.
收藏  |  浏览/下载:2/0  |  提交时间:2020/07/02
Diagenetic differences caused by gas charging with different compositions in the XF13 block of the Yinggehai Basin, South China Sea 期刊论文
AAPG BULLETIN, 2020, 104 (4) : 735-765
作者:  Duan, Wei;  Li, Chun-Feng;  Chen, Xue-Gang;  Luo, Cheng-Fei;  Tuo, Lei;  Liu, Jian-Zhang
收藏  |  浏览/下载:6/0  |  提交时间:2020/05/13
Actinide 2-metallabiphenylenes that satisfy Huckel's rule 期刊论文
NATURE, 2020, 578 (7796) : 563-+
作者:  Achar, Yathish Jagadheesh;  Adhil, Mohamood;  Choudhary, Ramveer;  Gilbert, Nick;  Foiani, Marco
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/03

Aromaticity and antiaromaticity, as defined by Huckel'  s rule, are key ideas in organic chemistry, and are both exemplified in biphenylene(1-3)-a molecule that consists of two benzene rings joined by a four-membered ring at its core. Biphenylene analogues in which one of the benzene rings has been replaced by a different (4n + 2) pi-electron system have so far been associated only with organic compounds(4,5). In addition, efforts to prepare a zirconabiphenylene compound resulted in the isolation of a bis(alkyne) zirconocene complex instead(6). Here we report the synthesis and characterization of, to our knowledge, the first 2-metallabiphenylene compounds. Single-crystal X-ray diffraction studies reveal that these complexes have nearly planar, 11-membered metallatricycles with metrical parameters that compare well with those reported for biphenylene. Nuclear magnetic resonance spectroscopy, in addition to nucleus-independent chemical shift calculations, provides evidence that these complexes contain an antiaromatic cyclobutadiene ring and an aromatic benzene ring. Furthermore, spectroscopic evidence, Kohn-Sham molecular orbital compositions and natural bond orbital calculations suggest covalency and delocalization of the uranium f(2) electrons with the carbon-containing ligand.


The synthesis of uranium- and thorium-containing metallabiphenylenes demonstrates the ability of the actinides to stabilize aromatic/antiaromatic structures where transition metals have failed.


  
High-pressure strengthening in ultrafine-grained metals 期刊论文
NATURE, 2020
作者:  Yoshida, Kenichi;  Gowers, Kate H. C.;  Lee-Six, Henry;  Chandrasekharan, Deepak P.;  Coorens, Tim;  Maughan, Elizabeth F.;  Beal, Kathryn;  Menzies, Andrew;  Millar, Fraser R.;  Anderson, Elizabeth;  Clarke, Sarah E.;  Pennycuick, Adam;  Thakrar, Ricky M.;  Butler, Colin R.
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

High-pressure diamond anvil cell experiments reveal that compression strengthening of nanocrystalline nickel increases as its grain sizes decrease to 3 nanometres, owing to dislocation hardening and suppression of grain boundary plasticity.


The Hall-Petch relationship, according to which the strength of a metal increases as the grain size decreases, has been reported to break down at a critical grain size of around 10 to 15 nanometres(1,2). As the grain size decreases beyond this point, the dominant mechanism of deformation switches from a dislocation-mediated process to grain boundary sliding, leading to material softening. In one previous approach, stabilization of grain boundaries through relaxation and molybdenum segregation was used to prevent this softening effect in nickel-molybdenum alloys with grain sizes below 10 nanometres(3). Here we track in situ the yield stress and deformation texturing of pure nickel samples of various average grain sizes using a diamond anvil cell coupled with radial X-ray diffraction. Our high-pressure experiments reveal continuous strengthening in samples with grain sizes from 200 nanometres down to 3 nanometres, with the strengthening enhanced (rather than reduced) at grain sizes smaller than 20 nanometres. We achieve a yield strength of approximately 4.2 gigapascals in our 3-nanometre-grain-size samples, ten times stronger than that of a commercial nickel material. A maximum flow stress of 10.2 gigapascals is obtained in nickel of grain size 3 nanometres for the pressure range studied here. We see similar patterns of compression strengthening in gold and palladium samples down to the smallest grain sizes. Simulations and transmission electron microscopy reveal that the high strength observed in nickel of grain size 3 nanometres is caused by the superposition of strengthening mechanisms: both partial and full dislocation hardening plus suppression of grain boundary plasticity. These insights contribute to the ongoing search for ultrastrong metals via materials engineering.


  
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:15/0  |  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.


  
Quantum crystal structure in the 250-kelvin superconducting lanthanum hydride 期刊论文
NATURE, 2020, 578 (7793) : 66-+
作者:  Gate, David;  Saligrama, Naresha;  Leventhal, Olivia;  Yang, Andrew C.;  Unger, Michael S.;  Middeldorp, Jinte;  Chen, Kelly;  Lehallier, Benoit;  Channappa, Divya;  De Los Santos, Mark B.;  McBride, Alisha;  Pluvinage, John;  Elahi, Fanny;  Tam, Grace Kyin-Ye;  Kim, Yongha;  Greicius, Michael;  Wagner, Anthony D.;  Aigner, Ludwig;  Galasko, Douglas R.;  Davis, Mark M.;  Wyss-Coray, Tony
收藏  |  浏览/下载:19/0  |  提交时间:2020/07/03

The discovery of superconductivity at 200 kelvin in the hydrogen sulfide system at high pressures(1) demonstrated the potential of hydrogen-rich materials as high-temperature superconductors. Recent theoretical predictions of rare-earth hydrides with hydrogen cages(2,3) and the subsequent synthesis of LaH10 with a superconducting critical temperature (T-c) of 250 kelvin(4,5) have placed these materials on the verge of achieving the long-standing goal of room-temperature superconductivity. Electrical and X-ray diffraction measurements have revealed a weakly pressure-dependent T-c for LaH10 between 137 and 218 gigapascals in a structure that has a face-centred cubic arrangement of lanthanum atoms(5). Here we show that quantum atomic fluctuations stabilize a highly symmetrical Fm (3) over barm crystal structure over this pressure range. The structure is consistent with experimental findings and has a very large electron-phonon coupling constant of 3.5. Although ab initio classical calculations predict that this Fm (3) over barm structure undergoes distortion at pressures below 230 gigapascals(2,3,) yielding a complex energy landscape, the inclusion of quantum effects suggests that it is the true ground-state structure. The agreement between the calculated and experimental Tc values further indicates that this phase is responsible for the superconductivity observed at 250 kelvin. The relevance of quantum fluctuations calls into question many of the crystal structure predictions that have been made for hydrides within a classical approach and that currently guide the experimental quest for room-temperature superconductivity(6-8). Furthermore, we find that quantum effects are crucial for the stabilization of solids with high electron-phonon coupling constants that could otherwise be destabilized by the large electron-phonon interaction(9), thus reducing the pressures required for their synthesis.


  
Intragranular three-dimensional stress tensor fields in plastically deformed polycrystals 期刊论文
SCIENCE, 2019, 366 (6472) : 1492-+
作者:  Hayashi, Yujiro;  Setoyama, Daigo;  Hirose, Yoshiharu;  Yoshida, Tomoyuki;  Kimura, Hidehiko
收藏  |  浏览/下载:8/0  |  提交时间:2020/02/17