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1.
Chen Hou Jiuhui Han Pan Liu Chuchu Yang Gang Huang Takeshi Fujita Akihiko Hirata Mingwei Chen 《Liver Transplantation》2019,9(45)
The solid electrolyte interphase (SEI) spontaneously formed on anode surfaces as a passivation layer plays a critical role in the lithium dissolution and deposition upon discharge/charge in lithium ion batteries and lithium‐metal batteries. The formation kinetics and failure of the SEI films are the key factors determining the safety, power capability, and cycle life of lithium ion and lithium‐metal batteries. Since SEI films evolve with the volumetric and interfacial changes of anodes, it is technically challenging in experimental study of SEI kinetics. Here operando observations are reported of SEI formation, growth, and failure at a high current density by utilizing a mass‐sensitive Cs‐corrected scanning transmission electron microscopy. The sub‐nano‐scale observations reveal a bilayer hybrid structure of SEI films and demonstrate the radical assisted SEI growth after the SEI thickness beyond the electron tunneling regime. The failure of SEI films is associated with rapid dissolution of inorganic layers when they directly contact with the electrolyte in broken SEI films. The initiation of cracks in SEI films is caused by heterogeneous volume changes of the electrodes during delithiation. These microscopic insights have important implications in understanding SEI kinetics and in developing high‐performance anodes with the formation of robust SEI films. 相似文献
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The search for superior‐energy‐density electrode materials for rechargeable batteries is prompted by the continuously growing demand for new electric vehicles and large energy‐storage grids. The structural properties of electrode materials affect their electrochemical performance because their functionality is correlated to their structure at the atomic scale. Although challenging, a deeper and comprehensive understanding of the basic structural operating units of electrode materials may contribute to the advancement of new energy‐storage technologies and many other technologies. Therefore, we must strategically control both the structure and kinetics of electrode materials to achieve optimal electrochemical performance. In this contribution, advancements in synchrotron radiation techniques, specifically in situ/operando experiments on electrode materials for rechargeable batteries, are presented and discussed. Indeed, the latest synchrotron radiation methods offer deeper insights into pristine and chemically modified electrode materials, opening new opportunities to optimize these materials and exploit new technologies. In particular, the most recent results from in situ/operando synchrotron radiation measurements, which play a critical role in the fundamental understanding of the kinetics processes that occur in rechargeable batteries, are discussed. 相似文献
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Lukas Zielke Tobias Hutzenlaub Dean R. Wheeler Chien‐Wei Chao Ingo Manke André Hilger Nils Paust Roland Zengerle Simon Thiele 《Liver Transplantation》2015,5(5)
LiCoO2 electrodes contain three phases, or domains, each having specific‐intended functions: ion‐conducting pore space, lithium‐ion‐reacting active material, and electron conducting carbon‐binder domain (CBD). Transport processes take place in all domains on different characteristic length scales: from the micrometer scale in the active material grains through to the nanopores in the carbon‐binder phase. Consequently, more than one imaging approach must be utilized to obtain a hierarchical geometric representation of the electrode. An approach incorporating information from the micro‐ and nanoscale to calculate 3D transport‐relevant properties in a large‐reconstructed active domain is presented. Advantages of focused ion beam/scanning electron microscopy imaging and X‐ray tomography combined by a spatial stochastic model, validated with an artificially produced reference structure are used. This novel approach leads to significantly different transport relevant properties compared with previous tomographic approaches: nanoporosity of the CBD leads to up to 42% additional contact area between active material and pore space and increases ionic conduction by a factor of up to 3.6. The results show that nanoporosity within the CBD cannot be neglected. 相似文献
4.
Seoung‐Bum Son James E. Trevey Hyunchul Roh Sung‐Hwan Kim Kee‐Bum Kim Jong Soo Cho Jeong‐Tak Moon Christopher M. DeLuca Kurt K. Maute Martin L. Dunn Heung Nam Han Kyu Hwan Oh Se‐Hee Lee 《Liver Transplantation》2011,1(6):1199-1204
We report the direct observation of microstructural changes of LixSi electrode with lithium insertion. HRTEM experiments confirm that lithiated amorphous silicon forms a shell around a core made up of the unlithiated silicon and that fully lithiated silicon contains a large number of pores of which concentration increases toward the center of the particle. Chemomechanical modeling is employed in order to explain this mechanical degradation resulting from stresses in the LixSi particles with lithium insertion. Because lithiation‐induced volume expansion and pulverization are the key mechanical effects that plague the performance and lifetime of high‐capacity Si anodes in lithium‐ion batteries, our observations and chemomechanical simulation provide important mechanistic insight for the design of advanced battery materials. 相似文献
5.
Bert Conings Jeroen Drijkoningen Nicolas Gauquelin Aslihan Babayigit Jan D'Haen Lien D'Olieslaeger Anitha Ethirajan Jo Verbeeck Jean Manca Edoardo Mosconi Filippo De Angelis Hans‐Gerd Boyen 《Liver Transplantation》2015,5(15)
Organolead halide perovskites currently are the new front‐runners as light absorbers in hybrid solar cells, as they combine efficiencies passing already 20% with deposition temperatures below 100 °C and cheap solution‐based fabrication routes. Long‐term stability remains a major obstacle for application on an industrial scale. Here, it is demonstrated that significant decomposition effects already occur during annealing of a methylammonium lead triiode perovskite at 85 °C even in inert atmosphere thus violating international standards. The observed behavior supports the view of currently used perovskite materials as soft matter systems with low formation energies, thus representing a major bottleneck for their application, especially in countries with high average temperatures. This result can trigger a broader search for new perovskite families with improved thermal stability. 相似文献
6.
David S. Eastwood Vladimir Yufit Jeff Gelb Allen Gu Robert S. Bradley Stephen J. Harris Daniel J. L. Brett Nigel P. Brandon Peter D. Lee Philip J. Withers Paul R. Shearing 《Liver Transplantation》2014,4(4)
Recent advances in high‐resolution 3D X‐ray computed tomography (CT) allow detailed, non‐destructive 3D structural mapping of a complete lithium‐ion battery. By repeated 3D image acquisition (time lapse CT imaging) these investigations of material microstructure are extended into the fourth dimension (time) to study structural changes of the device in operando. By digital volume correlation (DVC) of successive 3D images the dimensional changes taking place during charge cycling are quantified at the electrode level and at the Mn2O4 particle scale. After battery discharging, the extent of lithiation of the manganese (III/IV) oxide grains in the electrode is found to be a function of the distance from the battery terminal with grains closest to the electrode/current collector interface having the greatest expansion (≈30%) and grains furthest from the current collector and closest to the counter electrode showing negligible dilation. This implies that the discharge is limited by electrical conductivity. This new CT+DVC technique is widely applicable to the 3D exploration of the microstructural degradation processes for a range of energy materials including fuel cells, capacitors, catalysts, and ceramics. 相似文献
7.
Batteries: Lithiation‐Induced Dilation Mapping in a Lithium‐Ion Battery Electrode by 3D X‐Ray Microscopy and Digital Volume Correlation (Adv. Energy Mater. 4/2014) 
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下载免费PDF全文 David S. Eastwood Vladimir Yufit Jeff Gelb Allen Gu Robert S. Bradley Stephen J. Harris Daniel J. L. Brett Nigel P. Brandon Peter D. Lee Philip J. Withers Paul R. Shearing 《Liver Transplantation》2014,4(4)
8.
Cheng Ma Yongqiang Cheng Kai Chen Juchuan Li Bobby G. Sumpter Ce‐Wen Nan Karren L. More Nancy J. Dudney Miaofang Chi 《Liver Transplantation》2016,6(11)
Li‐ion‐conducting solid electrolytes can simultaneously overcome two grand challenges for Li‐ion batteries: the severe safety concerns that limit the large‐scale application and the poor electrolyte stability that forbids the use of high‐voltage cathodes. Nevertheless, the ionic conductivity of solid electrolytes is typically low, compromising the battery performances. Precisely determining the ionic transport mechanism(s) is a prerequisite for the rational design of highly conductive solid electrolytes. For decades, the research on this subject has primarily focused on the atomic and microscopic scales, where the main features of interest are unit cells and microstructures, respectively. Here, it is shown that the largely overlooked mesoscopic scale lying between these extremes could be the key to fast ionic conduction. In a prototype system, (Li0.33La0.56)TiO3, a mesoscopic framework is revealed for the first time by state‐of‐the‐art scanning transmission electron microscopy. Corroborated by theoretical calculations and impedance measurements, it is demonstrated that such a unique configuration maximizes the number of percolation directions and thus most effectively improves the ionic conductivity. This discovery reconciles the long‐standing structure–property inconsistency in (Li0.33La0.56)TiO3 and also identifies mesoscopic ordering as a promising general strategy for optimizing Li+ conduction. 相似文献
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Qiang Fu Shuoqi Liu Angelina Sarapulova Lihua Zhu Martin Etter Edmund Welter Peter G. Weidler Michael Knapp Helmut Ehrenberg Sonia Dsoke 《Liver Transplantation》2019,9(33)
In this work, the effect of Li+ substitution in Li3V2(PO4)3 with a large divalent ion (Ca2+) toward lithium insertion is studied. A series of materials, with formula Li3?2xCaxV2(PO4)3/C (x = 0, 0.5, 1, and 1.5) is synthesized and studied in the potential region 3–0.01 V versus Li+/Li. Synchrotron diffraction demonstrates that Li3V2(PO4)3/C has a monoclinic structure (space group P21/n), while Ca1.5V2(PO4)3/C possesses a rhombohedral structure (space group R‐3c). The intermediate compounds, Li2Ca0.5V2(PO4)3/C and LiCaV2(PO4)3/C, are composed of two main phases, including monoclinic Li3V2(PO4)3/C and rhombohedral Ca1.5V2(PO4)3/C. Cyclic voltammetry reveals five reduction and oxidation peaks on Li3V2(PO4)3/C and Li2Ca0.5V2(PO4)3/C electrodes. In contrast, LiCaV2(PO4)3/C and Ca1.5V2(PO4)3/C have no obvious oxidation and reduction peaks but a box‐type voltammogram. This feature is the signature for capacitive‐like mechanism, which involves fast electron transfer on the surface of the electrode. Li3V2(PO4)3/C undergoes two solid‐solution and a short two‐phase reaction during lithiation and delithiation processes, whereas Ca1.5V2(PO4)3/C only goes through capacitive‐like mechanism. In operando X‐ray absorption spectroscopy confirms that, in both Li3V2(PO4)3/C and Ca1.5V2(PO4)3/C, V ions are reduced during the insertion of the first three Li ions. This study demonstrates that the electrochemical characteristic of polyanionic phosphates can be easily tuned by replacing Li+ with larger divalent cations. 相似文献
10.
Growth of Collagen Fibril Seeds from Embryonic Tendon: Fractured Fibril Ends Nucleate New Tip Growth
Collagen fibrils are the principal tensile element of vertebrate tissues where they occur in the extracellular matrix as spatially organised arrays. A major challenge is to understand how the mechanisms of nucleation, growth and remodelling yield fibrils of tissue-specific diameter and length. Here we have developed a seeding system whereby collagen fibrils were isolated from avian embryonic tendon and added to purified collagen solution, in order to characterise fibril surface nucleation and growth mechanisms. Fragmentation of tendon in liquid nitrogen followed by Dounce homogenisation generated fibril length fragments. Most (> 94%) of the fractured ends of fibrils, which show an abrupt square profile, were found to act as nucleation sites for further growth by molecular accretion. The mechanism of this nucleation and growth process was investigated by transmission electron microscopy, atomic force microscopy and scanning transmission electron microscopy mass mapping. Typically, a single growth spur occurred on the N-terminal end of seed fibrils whilst twin spurs frequently formed on the C-terminal end before merging into a single tip projection. The surface nucleation and growth process generated a smoothly tapered tip that achieved maximum diameter when the axial extension reached ∼ 13 μm. Lateral growth also occurred along the entire length of all seed fibrils that contained tip projections. The data support a model of collagen fibril growth in which the broken ends of fibrils are nucleation sites for propagation in opposite axial directions. The observed fibril growth behaviour has direct relevance to tendon matrix remodelling and repair processes that might involve rupture of collagen fibrils. 相似文献
11.
Guisheng Liang Liting Yang Qing Han Guanyu Chen Chunfu Lin Yongjun Chen Lijie Luo Xianhu Liu Yuesheng Li Renchao Che 《Liver Transplantation》2020,10(20)
“Zero‐strain” compounds are ideal energy‐storage materials for long‐term cycling because they present negligible volume change and significantly reduce the mechanically induced deterioration during charging–discharging. However, the explored “zero‐strain” compounds are very limited, and their energy densities are low. Here, γ phase Li3.08Cr0.02Si0.09V0.9O4 (γ‐LCSVO) is explored as an anode compound for lithium‐ion batteries, and surprisingly its “zero‐strain” Li+ storage during Li+ insertion–extraction is found through using various state‐of‐the‐art characterization techniques. Li+ sequentially inserts into the 4c(1) and 8d sites of γ‐LCSVO, but its maximum unit‐cell volume variation is only ≈0.18%, the smallest among the explored “zero‐strain” compounds. Its mean strain originating from Li+ insertion is only 0.07%. Consequently, both γ‐LCSVO nanowires (γ‐LCSVO‐NW) and micrometer‐sized particles (γ‐LCSVO‐MP) exhibit excellent cycling stability with 90.1% and 95.5% capacity retention after as long as 2000 cycles at 10C, respectively. Moreover, γ‐LCSVO‐NW and γ‐LCSVO‐MP respectively deliver large reversible capacities of 445.7 and 305.8 mAh g?1 at 0.1C, and retain 251.2 and 78.4 mAh g?1 at 10C. Additionally, γ‐LCSVO shows a suitably safe operating potential of ≈1.0 V, significantly lower than that of the famous “zero‐strain” Li4Ti5O12 (≈1.6 V). These merits demonstrate that γ‐LCSVO can be a practical anode compound for stable, high‐energy, fast‐charging, and safe Li+ storage. 相似文献
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Operando X‐ray diffraction (XRD) and X‐ray absorption spectroscopy (XAS) studies of Ge anodes are carried out to understand the effect of cycling rate on Ge phase transformation during charge/discharge process and to relate that effect to capacity. It is discovered that the formation of crystalline Li15Ge4 (c‐Li15Ge4) during lithiation is suppressed beyond a certain cycling rate. A very stable and reversible high capacity of ≈1800 mAh g?1 can be attained up to 100 cycles at a slow C‐rate of C/21 when there is complete conversion of Ge anode into c‐Li15Ge4. When the C‐rate is increased to ≈C/10, the lithiation reaction is more heterogeneous and a relatively high capacity of ≈1000 mAh g?1 is achieved with poorer electrochemical reversibility. An increase in C‐rate to C/5 and higher reduces the capacity (≈500 mAh g?1) due to an impeded transformation from amorphous LixGe to c‐Li15Ge4, and yet improves the electrochemical reversibility. A proposed mechanism is presented to explain the C‐rate dependent phase transformations and the relationship of these to capacity fading. The operando XRD and XAS results provide new insights into the relationship between structural changes in Ge and battery capacity, which are important for guiding better design of high‐capacity anodes. 相似文献
16.
Feng Wang Lijun Wu Baris Key Xiao‐Qing Yang Clare P. Grey Yimei Zhu Jason Graetz 《Liver Transplantation》2013,3(10):1324-1331
Silicon‐based anodes are an appealing alternative to graphite for lithium‐ion batteries because of their extremely high capacity. However, poor cycling stability and slow kinetics continue to limit the widespread use of silicon in commercial batteries. Performance improvement has been often demonstrated in nanostructured silicon electrodes, but the reaction mechanisms involved in the electrochemical lithiation of nanoscale silicon are not well understood. Here, in‐situ synchrotron X‐ray diffraction is used to monitor the subtle structural changes occurring in Si nanoparticles in a Si‐C composite electrode during lithiation. Local analysis by electron energy‐loss spectroscopy and transmission electron microscopy is performed to interrogate the nanoscale morphological changes and phase evolution of Si particles at different depths of discharge. It is shown that upon lithiation, Si nanoparticles behave quite differently than their micrometer‐sized counterparts. Although both undergo an electrochemical amorphization, the micrometer‐sized silicon exhibits a linear transformation during lithiation, while a two‐step process occurs in the nanoscale Si. In the first half of the discharge, lithium reacts with surfaces, grain boundaries and planar defects. As the reaction proceeds and the cell voltage drops, lithium consumes the crystalline core transforming it into amorphous LixSi with a primary particle size of just a few nanometers. Unlike the bulk silicon electrode, no Li15Si4 or other crystalline LixSi phases were formed in nanoscale Si at the fully‐lithiated state. 相似文献
17.
Ricinuleid functional mouthparts are the cucullus, the chelicerae, the pedipalps, and the labrum. These structures are movably jointed to the rest of the prosoma, most likely protruded upon hydrostatic hemolymph pressure and retracted by prosomal muscles. Seta‐like protrusions from the labrum and the pedipalpal coxae form a sieve‐like filter inside the preoral cavity and the mouth. Although the tip of the labrum can be elevated upon muscle constriction, ingestion of large, solid food particles is unlikely. The mouth has a crescent‐shaped cross section. The cuticle‐lined, also crescent‐shaped pharynx is equipped with a large dilator muscle but lacks antagonistic constrictor muscles. It represents a precerebral sucking pump. The triangular to Y‐shaped, cuticle‐lined esophagus is equipped with constrictor and dilator muscles. Its posterior part represents a postcerebral sucking pump. Four blind ending diverticula ramify from the anterior prosomal part of the entodermal midgut tube. Two of these diverticula remain inside the prosoma and form few short branches. The other two extend through the pedicel into the opisthosoma and ramify and coil there. A stercoral pocket protrudes ventrally out of the midgut tube. The most distal part of the midgut tube is modified into a contractile rectal gland. Its secretions may have defensive or physiological functions. A short anal atrium is formed by the cuticle‐lined ectodermal hindgut which opens at the end of the three‐segmented metasoma. The telescoping segments of the metasoma are protruded by hemolymph pressure and retracted by muscles. J. Morphol., 2011. © 2010 Wiley‐Liss, Inc. 相似文献
18.
DANIELA N. SCHMIDT EMILY J. RAYFIELD ALEXANDRA COCKING FEDERICA MARONE 《Palaeontology》2013,56(4):741-749
Abstract: Making the link between evolutionary processes and development in extinct organisms is usually hampered by the lack of preservation of ontogenetic stages in the fossil record. Planktic foraminifers, which grow by adding chambers, are an ideal target organism for such studies as their test incorporates all prior developmental stages. Previously, studies of development in these organisms were limited by the small size of their early chambers. Here, we describe the application of synchrotron radiation X‐ray tomographic microscopy (SRXTM) to document the ontogenetic history of the foraminifers Globigerinoides sacculifer and Globorotalia menardii. Our SRXTM scans permit resolution at submicrometre scale, thereby displaying additional internal structures such as pores, dissolution patterns and complexity of the wall growth. Our methods provide a powerful tool to pick apart the developmental history of these microfossils and subsequently assist in inferring phylogenetic relationships and evolutionary processes. 相似文献
19.
Patrick E. Hayes Peta L. Clode Rafael S. Oliveira Hans Lambers 《Plant, cell & environment》2018,41(3):605-619
Plants allocate nutrients to specific leaf cell types; eudicots are thought to predominantly allocate phosphorus (P) to epidermal/bundle sheath cells. However, three Proteaceae species have been shown to preferentially allocate P to mesophyll cells instead. These Proteaceae species are highly adapted to P‐impoverished habitats, with exceptionally high photosynthetic P‐use efficiencies (PPUE). We hypothesized that preferential allocation of P to photosynthetic mesophyll cells is an important trait in species adapted to extremely P‐impoverished habitats, contributing to their high PPUE. We used elemental X‐ray mapping to determine leaf cell‐specific nutrient concentrations for 12 Proteaceae species, from habitats of strongly contrasting soil P concentrations, in Australia, Brazil, and Chile. We found that only species from extremely P‐impoverished habitats preferentially allocated P to photosynthetic mesophyll cells, suggesting it has evolved as an adaptation to their extremely P‐impoverished habitat and that it is not a family‐wide trait. Our results highlight the possible role of soil P in driving the evolution of ecologically relevant nutrient allocation patterns and that these patterns cannot be generalized across families. Furthermore, preferential allocation of P to photosynthetic cells may provide new and exciting strategies to improve PPUE in crop species. 相似文献