Engineering topics
Zhang, Shuo
Publications and source records attributed to Zhang, Shuo.
Poly(4-vinylbenzoic acid): A Re-Engineered Binder for Improved Performance from Water-Free Slurry Processing for Silicon Graphite Composite Electrodes
In silicon-based lithium-ion batteries, polymeric binders play the crucial role of “gluing” the electrode matrix together, providing strong adhesion between the active silicon (Si) and conductive carbon particles and keeping them in electrical contact, despite considerable volumetric changes during cycling. While remarkable progress has been seen in the development of binders, improved cycling performance is still needed to fully enable Si anodes. Achieving that end requires in turn a better understanding of the relationship between binder properties and cell cycling performance. Here, we describe a novel polymer binder, poly(4-vinylbenzoic acid) (P4VBA), developed by re-engineering the widely used poly(acrylic acid) (PAA) binder to explore that relationship. The modified structure produces a binder that is more compatible with 1-methyl-2-pyrrolidinone (NMP) slurries and affords much improved cycling performance of the fabricated cells. Compared with PAA binders, P4VBA provides higher initial and average capacities and better capacity retention. While P4VBA offers an interesting alternative to wet processing of the Si-based electrodes, this re-engineered binder is an initial effort to develop a better binder material by exploring the relationship between binder and cell cycling performance.
Rational Design of a Multifunctional Binder for High-Capacity Silicon-Based Anodes
Although several principles have been recognized to fabricate a nominal "better" binder, there continues to be a lack of a rational design and synthesis approach that would meet the robust criteria required for silicon (Si) anodes. Herein, we report a synthetic polymer binder, i.e., catechol-functionalized chitosan cross-linked by glutaraldehyde (CS-CG+GA), that serves dual functionalities: (a) wetness-resistant adhesion capability via catechol grafting and (b) mechanical robustness via in situ formation of a three-dimensional (3D) network. A SiNP-based anode with a designed functional polymer network (CS-CG10%+6%GA) exhibits a capacity retention of 91.5% after 100 cycles (2144 +/- 14 mAh/g). Properties that are traditionally considered to be advantageous, including stronger adhesion strength and higher mechanical robustness, do not always improve the binder performance. A clear relationship between these properties and ultimate electrochemical performance is established by assessing the rheological behavior, mechanical property, adhesion force, peel stress, morphology evolution, and semiquantitative evaluation. This study provides a clear path for the rational design of high-performance functional polymer binders for not only Si-based electrodes but also other types of alloy and conversion-based electrodes.
Guiding Synthesis of Polymorphs of Materials Using Nanometric Phase Diagrams
Conventionally, phase diagrams serve as road maps for the design and synthesis of materials. However, bulk phase diagrams are often not as predictive for the synthesis of nanometric materials, mainly due to the increased significance of surface energy. The change of surface energy can drastically alter the total energy of the nanocrystals thus yield a polymorph or meta-stable phase different than the stable phase in bulk, providing a means for controlling the synthesis of metastable phases. To achieve a theoretical and systematical understanding on the polymorphism of nanomaterials, metallic cobalt was chosen as a model system, where the two polymorphs, fcc and hcp phases, can be tuned with 100% selectivity in a solvothermal reaction. Advanced in situ synchrotron X-ray diffraction (XRD) technique and density functionals theory (DFT) were complementary employed to reveal the size and surface dependent polymorphism at nanometer scale. Furthermore, the nanometric phase diagram provides a general predictive approach to guide the synthesis of metastable materials.
A fast marine sewage detection method for remote-sensing image
This paper presents an effective method for marine sewage detection from a remote-sensing image. It is inspired by the Grab-Cut mechanism that iterative estimation and incomplete labeling allow a considerably reduced degree of user interaction for a given quality of result. By establishing the relationship between the color feature and the object seeds, we first model object and background with Gaussian mixture model, respectively, followed by iteratively updating the parameter of model to decline the energy function. To improve the computation efficiency, we propose to extend the region of interest as background. The proposed method accounts for not only the effect of color feature, but also the geographical information. The experimental results demonstrate that the proposed method is more reliable in marine sewage detection compared to other state-of-the-art methods.
Authigenic carbonate formation rates in marine sediments and implications for the marine δ 13 C record
Carbon isotope (δ 13 C) variations measured in carbonates have been attributed to large-scale phenomena throughout Earth history, such as changes in atmospheric oxygen or global glaciations. Additionally, these interpretations follow from a model wherein the δ 13 C of marine dissolved inorganic carbon (DIC) is controlled by the relative sedimentary burial rates of biogenic carbonate (BC) and organic carbon (OC). A new model proposes authigenic carbonate (AC) as a third major sedimentary C pool, implying that δ 13 C anomalies are not necessarily indicative of extreme changes in the global carbon cycle and/or atmospheric oxygen. Two conditions are required for AC formation to significantly alter bulk carbonate δ 13 C: the AC isotopic composition must be at least ~3‰ different from that of BC and the AC/BC ratio must be >0.1. We use pore fluid Ca and Sr concentrations to estimate rates of AC formation in Late Cenozoic marine sediments, then calculate relative fractions of AC, OC, and BC. Today AC is not expected to constitute a significant fraction of total sedimentary carbon (AC+OC+BC) globally; however, there are modern sites where local conditions promote elevated AC/BC and anaerobic metabolisms can alter the δ 13 C of pore fluids. We investigate these sites to determine what conditions might enable AC to alter δ 13 C of marine DIC. Here, we find there is very little net addition of AC relative to BC, but large quantities of AC form today across many settings via recrystallization. In settings where remineralization of organic matter causes recrystallized carbonate to form with modified δ 13 C, AC/BC is generally too low for this recrystallization to significantly shift the δ 13 C of the bulk carbonate. However, exceptions are found in sites with very low BC and extensive methane oxidation, suggesting that this environment type would need to be globally extensive in the past in order for AC formation to change the δ 13 C of marine DIC.
The existence of optimal molecular weight for poly(acrylic acid) binders in silicon/graphite composite anode for lithium-ion batteries
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Coupled electronic and atomic effects on defect evolution in silicon carbide under ion irradiation
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Effect of the Hydrofluoroether Cosolvent Structure in Acetonitrile-Based Solvate Electrolytes on the Li+ Solvation Structure and Li-S Battery Performance.
We evaluate hydrofluoroether (HFE) cosolvents with varying degrees of fluorination in the acetonitrile-based solvate electrolyte to determine the effect of the HFE structure on the electrochemical performance of the Li-S battery. Solvates or sparingly solvating electrolytes are an interesting electrolyte choice for the Li-S battery due to their low polysulfide solubility. The solvate electrolyte with a stoichiometric ratio of LiTFSI salt in acetonitrile, (MeCN)(2)-LiTFSI, exhibits limited polysulfide solubility due to the high concentration of LiTFSI. We demonstrate that the addition of highly fluorinated HFEs to the solvate yields better capacity retention compared to that of less fluorinated HFE cosolvents. Raman and NMR spectroscopy coupled with ab initio molecular dynamics simulations show that HFEs exhibiting a higher degree of fluorination coordinate to Li+ at the expense of MeCN coordination, resulting in higher free MeCN content in solution. However, the polysulfide solubility remains low, and no crossover of polysulfides from the S cathode to the Li anode is observed.
Quantum phase transition and destruction of Kondo effect in pressurized SmB 6
SmB 6 has been a well-known Kondo insulator for decades, but recently attracts extensive new attention as a candidate topological system. Studying SmB 6 under pressure provides an opportunity to acquire the much-needed understanding about the effect of electron correlations on both the metallic surface state and bulk insulating state. Here we do so by studying the evolution of two transport gaps (low temperature gap E l and high temperature gap E h ) associated with the Kondo effect by measuring the electrical resistivity under high pressure and low temperature (0.3 K) conditions. We associate the gaps with the bulk Kondo hybridization, and from their evolution with pressure we demonstrate an insulator-to-metal transition at ~4 GPa. At the transition pressure, a large change in the Hall number and a divergence tendency of the electron-electron scattering coefficient provide evidence for a destruction of the Kondo entanglement in the ground state. In conclusion, our results raise the new prospect for studying topological electronic states in quantum critical materials settings.
NuSTAR Hard X-Ray Observation of the Gamma-Ray Binary Candidate HESS J1832–093
We present a hard X-ray observation of the TeV gamma-ray binary candidate HESS J1832−093, which is coincident with the supernova remnant G22.7−0.2, using the Nuclear Spectroscopic Telescope Array. Non-thermal X-ray emission from XMMU J183245−0921539, the X-ray source associated with HESS J1832−093, is detected up to ∼30 keV and is well-described by an absorbed power-law model with a best-fit photon index Γ=1.5±0.1. A re-analysis of archival Chandra and XMM-Newton data finds that the long-term X-ray flux increase of XMMU J183245−0921539 is 50{sub −20}{sup +40}% (90% C.L.), much less than previously reported. A search for a pulsar spin period or binary orbit modulation yields no significant signal to a pulse fraction limit of f{sub p}<19% in the range 4 ms < P<40 ks. No red noise is detected in the FFT power spectrum to suggest active accretion from a binary system. While further evidence is required, we argue that the X-ray and gamma-ray properties of XMMU J183245−0921539 are most consistent with a non-accreting binary generating synchrotron X-rays from particle acceleration in the shock formed as a result of the pulsar and stellar wind collision. We also report on three nearby hard X-ray sources, one of which may be associated with diffuse emission from a fast-moving supernova fragment interacting with a dense molecular cloud.
Rates of CO 2 Mineralization in Geological Carbon Storage
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Sagittarius A∗ High-energy X-Ray Flare Properties during NuStar Monitoring of the Galactic Center from 2012 to 2015
Understanding the origin of the flaring activity from the Galactic center supermassive black hole Sagittarius A* is a major scientific goal of the NuSTAR Galactic plane survey campaign. We report on the data obtained between 2012 July and 2015 April, including 27 observations on Sgr A*, with a total exposure of ≃1 Ms. We found a total of 10 X-ray flares detected in the NuSTAR observation window, with luminosities in the range of L{sub 3--79keV}∼(0.2–4.0)×10{sup 35} erg s{sup −1}. With this largest hard X-ray Sgr A* flare data set to date, we studied the flare spectral properties. Seven flares are detected above 5σ significance, showing a range of photon indices (Γ ∼ 2.0–2.8) with typical uncertainties of ±0.5 (90% confidence level). We found no significant spectral hardening for brighter flares, as indicated by a smaller sample. The accumulation of all of the flare spectra in 1–79 keV can be well fit with an absorbed power-law model with Γ=2.2±0.1, and does not require the existence of a spectral break. The lack of variation in the X-ray spectral index with luminosity would point to a single mechanism for the flares and is consistent with the synchrotron scenario. Lastly, we present the quiescent-state spectrum of Sgr A*, and derive an upper limit on the quiescent luminosity of Sgr A* above 10 keV to be L{sub Xq,10--79keV}⩽(2.9±0.2)×10{sup 34} erg s{sup −1}.
Naphthodipyrrolidone (NDP) based conjugated polymers with high electron mobility and ambipolar transport properties
Two novel donor–acceptor π-conjugated polymers based on naphthodipyrrolidone (NDP) were synthesized and characterized. The polymers possess low band gaps and suitable molecular orbital levels as ambipolar semiconductors. The thin film organic field effect transistor of NDP polymers exhibited ambipolar transport properties with a high electron mobility up to 0.67 cm 2 V –1 s –1 . The grazing-incidence wide-angle X-ray scattering (GIWAXS) studies demonstrated that the polymer molecules pack into a long-range-ordered lamellar structure with isotropically oriented crystalline domains. Thermal annealing promoted edge-on lamellar stacking as evidenced by the increased diffraction intensity along the out-of-plane direction. In conclusion, the polymer with NDP and bithiophene units achieved the best edge-on lamellar stacking after thermal annealing, which yielded the best electron transport performance in this work.