17 research outputs found
Characterization of Nb Superconducting Radio Frequency Cavities Based On In-Situ STEM And EELS
Various impurities of Nb are investigated with atomic resolution. Methodologies
for quantifying Nb oxides and hydrides are developed. Direct observation of hydrogen atoms
is realized in ABF images at room temperature, and can also serve as a promising method to
identify diff erent hydrides in Nb bulk at LN2 temperature if the cold stage is stable enough.
My work on the local strain of Nb cavities points out that Nb carbides play a signi ficant role
in the performance of SRF cavities at low temperature and intermediate to high fields
Direct Atomic-Scale Imaging of Hydrogen and Oxygen Interstitials in Pure Niobium Using Atom-Probe Tomography and Aberration-Corrected Scanning Transmission Electron Microscopy
Imaging the three-dimensional atomic-scale structure of complex interfaces has been the goal of many recent studies, due to its importance to technologically relevant areas. Combining atom-probe tomography and aberration-corrected scanning transmission electron microscopy (STEM), we present an atomic-scale study of ultrathin (âŒ5 nm) native oxide layers on niobium (Nb) and the formation of ordered niobium hydride phases near the oxide/Nb interface. Nb, an elemental type-II superconductor with the highest critical temperature (<i>T</i><sub>c</sub> = 9.2 K), is the preferred material for superconducting radio frequency (SRF) cavities in next-generation particle accelerators. Nb exhibits high solubilities for oxygen and hydrogen, especially within the RF-field penetration depth, which is believed to result in SRF quality factor losses. STEM imaging and electron energy-loss spectroscopy followed by ultraviolet laser-assisted local-electrode atom-probe tomography on the same needle-like sample reveals the NbO<sub>2</sub>, Nb<sub>2</sub>O<sub>5</sub>, NbO, Nb stacking sequence; annular bright-field imaging is used to visualize directly hydrogen atoms in bulk ÎČ-NbH
Atomic-scale observation of lithiation reaction front in nanoscale SnO \u3c inf\u3e 2 materials
In the present work, taking advantage of aberration-corrected scanning transmission electron microscopy, we show that the dynamic lithiation process of anode materials can be revealed in an unprecedented resolution. Atomically resolved imaging of the lithiation process in SnO2 nanowires illustrated that the movement, reaction, and generation of b = [1Ă...1Ă...1] mixed dislocations leading the lithiated stripes effectively facilitated lithium-ion insertion into the crystalline interior. The geometric phase analysis and density functional theory simulations indicated that lithium ions initial preference to diffuse along the [001] direction in the {200} planes of SnO2 nanowires introduced the lattice expansion and such dislocation behaviors. At the later stages of lithiation, the Li-induced amorphization of rutile SnO2 and the formation of crystalline Sn and LixSn particles in the Li2O matrix were observed. © 2013 American Chemical Society
Lithiation-induced shuffling of atomic stacks
© 2014 American Chemical Society. In rechargeable lithium-ion batteries, understanding the atomic-scale mechanism of Li-induced structural evolution occurring at the host electrode materials provides essential knowledge for design of new high performance electrodes. Here, we report a new crystalline-crystalline phase transition mechanism in single-crystal Zn-Sb intermetallic nanowires upon lithiation. Using in situ transmission electron microscopy, we observed that stacks of atomic planes in an intermediate hexagonal (h-)LiZnSb phase are shuffled to accommodate the geometrical confinement stress arising from lamellar nanodomains intercalated by lithium ions. Such atomic rearrangement arises from the anisotropic lithium diffusion and is accompanied by appearance of partial dislocations. This transient structure mediates further phase transition from h-LiZnSb to cubic (c-)Li2ZnSb, which is associated with a nearly zero-strain coherent interface viewed along the [001]h/[111]c directions. This study provides new mechanistic insights into complex electrochemically driven crystalline-crystalline phase transitions in lithium-ion battery electrodes and represents a noble example of atomic-level structural and interfacial rearrangements
Structural and Chemical Evolution of Amorphous Nickel Iron Complex Hydroxide upon Lithiation/Delithiation
Development of novel electrode materials
is essential to achieve
high-performance lithium ion batteries. Here, we demonstrate that
amorphous nickel iron complex hydroxides (NiâFeâOH)
synthesized by a laserâchemical method can be used as a potential
conversion anode material for lithium storage. Complementary characterizations,
including ensemble-averaged X-ray absorption spectroscopy, spatially
resolved electron energy-loss spectroscopy, and energy dispersive
X-ray spectroscopy in a scanning transmission electron microscope,
were performed to reveal the chemical and structural evolutions of
the active hydroxide particles undergoing electrochemical cycling.
The solidâelectrolyte interphase (SEI) layer with a primary
component of lithium fluoride (LiF) was found and remained robust
on the particle surface during the charge/discharge processes, which
suggests that the LiF-containing SEI layer plays a critical role in
maintaining the stable capacity retention and good reversibility of
the NiâFeâOH anode
Highly porous non-precious bimetallic electrocatalysts for efficient hydrogen evolution.
A robust and efficient non-precious metal catalyst for hydrogen evolution reaction is one of the key components for carbon dioxide-free hydrogen production. Here we report that a hierarchical nanoporous copper-titanium bimetallic electrocatalyst is able to produce hydrogen from water under a mild overpotential at more than twice the rate of state-of-the-art carbon-supported platinum catalyst. Although both copper and titanium are known to be poor hydrogen evolution catalysts, the combination of these two elements creates unique copper-copper-titanium hollow sites, which have a hydrogen-binding energy very similar to that of platinum, resulting in an exceptional hydrogen evolution activity. In addition, the hierarchical porosity of the nanoporous copper-titanium catalyst also contributes to its high hydrogen evolution activity, because it provides a large-surface area for electrocatalytic hydrogen evolution, and improves the mass transport properties. Moreover, the catalyst is self-supported, eliminating the overpotential associated with the catalyst/support interface
Revealing cation-exchange-induced phase transformations in multielemental chalcogenide nanoparticles
To control the process of cation exchange (CE) in a multielemental system, a detailed understanding of structural changes at the microscopic level is imperative. However, the synthesis of a multielemental system has so far relied on the CE phenomenon of a binary system, which does not necessarily extend to the higher-order systems. Here, direct experimental evidence supported by theoretical calculations reveals a growth model of binary CuâS to ternary CuâSnâS to quaternary CuâZnâSnâS, which shows that cations preferentially diffuse along a specific lattice plane with the preservation of sulfuric anionic framework. In addition, we also discover that, unlike the commonly accepted structure (P63mc), the metastable crystal structure of CuâZnâSnâS phase possesses fixed Sn occupancy sites. By revealing the preferential nature of cations diffusion and growth mechanism, our work provides insight into controlling the stoichiometry and phase purity of novel multielemental materials.Ministry of Education (MOE)National Research Foundation (NRF)Accepted versionWe acknowledge financial support from National Research Foundation (NRF), Singapore, through the Singapore-Berkeley Research Initiative for Sustainable Energy (SinBeRISE) and Nanomaterials for Energy and Water Management (SHARE NEW) CREATE program. L.H.W. thanks the funding support from Singapore Ministry of Education, Tier 2 (2016-T2-1-030). S.L. acknowledges the funding support from Singapore Ministry of Education Tier 1 (107/15). H.Z. thanks the funding support from U.S. DOE BES Materials Sciences and Engineering Division Under Contract No. KC22ZH. X.Y.L. thanks the funding support from Singapore Ministry of Education, Tier 1 (RG21/16) and Tier 2 (MOE2016-T2-1- 043) grants.. The work at the Molecular Foundry was supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. We thank Fiona Doyle for lending us her synthetic laboratory in University of California Berkeley (UCB), Song Chengyu and Karen Bustilo for their help and assistance on TEM, and Matthew P. Sherburne for nanoparticle growth discussion
Lithiation-Induced Shuffling of Atomic Stacks
In rechargeable lithium-ion batteries,
understanding the atomic-scale
mechanism of Li-induced structural evolution occurring at the host
electrode materials provides essential knowledge for design of new
high performance electrodes. Here, we report a new crystallineâcrystalline
phase transition mechanism in single-crystal ZnâSb intermetallic
nanowires upon lithiation. Using in situ transmission electron microscopy,
we observed that stacks of atomic planes in an intermediate hexagonal
(<i>h</i>-)ÂLiZnSb phase are âshuffledâ to
accommodate the geometrical confinement stress arising from lamellar
nanodomains intercalated by lithium ions. Such atomic rearrangement
arises from the anisotropic lithium diffusion and is accompanied by
appearance of partial dislocations. This transient structure mediates
further phase transition from <i>h</i>-LiZnSb to cubic (c-)ÂLi<sub>2</sub>ZnSb, which is associated with a nearly âzero-strainâ
coherent interface viewed along the [001]<sub><i>h</i></sub>/[111]<sub><i>c</i></sub> directions. This study provides
new mechanistic insights into complex electrochemically driven crystallineâcrystalline
phase transitions in lithium-ion battery electrodes and represents
a noble example of atomic-level structural and interfacial rearrangements
Revealing the Atomic Restructuring of PtâCo Nanoparticles
We studied PtâCo bimetallic
nanoparticles during oxidation
in O<sub>2</sub> and reduction in H<sub>2</sub> atmospheres using
an aberration corrected environmental transmission electron microscope.
During oxidation Co migrates to the nanoparticle surface forming a
strained epitaxial CoO film. It subsequently forms islands via strain
relaxation. The atomic restructuring is captured as a function of
time. During reduction cobalt migrates back to the bulk, leaving a
monolayer of platinum on the surface