William Huang
Masters Student in Computer Science, admitted Autumn 2023
All Publications
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Resolving three-dimensional nanoscale heterogeneities in lithium metal batteries with cryoelectron tomography
MATTER
2025; 8 (7)
View details for DOI 10.1016/j.matt.2025.102266
View details for Web of Science ID 001532637500008
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Robust trigger wave speed in Xenopus cytoplasmic extracts.
Nature communications
2024; 15 (1): 5782
Abstract
Self-regenerating trigger waves can spread rapidly through the crowded cytoplasm without diminishing in amplitude or speed, providing consistent, reliable, long-range communication. The macromolecular concentration of the cytoplasm varies in response to physiological and environmental fluctuations, raising the question of how or if trigger waves can robustly operate in the face of such fluctuations. Using Xenopus extracts, we find that mitotic and apoptotic trigger wave speeds are remarkably invariant. We derive a model that accounts for this robustness and for the eventual slowing at extremely high and low cytoplasmic concentrations. The model implies that the positive and negative effects of cytoplasmic concentration (increased reactant concentration vs. increased viscosity) are nearly precisely balanced. Accordingly, artificially maintaining a constant cytoplasmic viscosity during dilution abrogates this robustness. The robustness in trigger wave speeds may contribute to the reliability of the extremely rapid embryonic cell cycle.
View details for DOI 10.1038/s41467-024-50119-0
View details for PubMedID 38987269
View details for PubMedCentralID PMC11237086
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Membrane localization accelerates association under conditions relevant to cellular signaling.
Proceedings of the National Academy of Sciences of the United States of America
2024; 121 (10): e2319491121
Abstract
Translocation of cytoplasmic molecules to the plasma membrane is commonplace in cell signaling. Membrane localization has been hypothesized to increase intermolecular association rates; however, it has also been argued that association should be faster in the cytosol because membrane diffusion is slow. Here, we directly compare an identical association reaction, the binding of complementary DNA strands, in solution and on supported membranes. The measured rate constants show that for a 10-µm-radius spherical cell, association is 22- to 33-fold faster at the membrane than in the cytoplasm. The kinetic advantage depends on cell size and is essentially negligible for typical ~1 µm prokaryotic cells. The rate enhancement is attributable to a combination of higher encounter rates in two dimensions and a higher reaction probability per encounter.
View details for DOI 10.1073/pnas.2319491121
View details for PubMedID 38427601
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Signaling reactions in 2D vs. 3D
CELL PRESS. 2024: 21A
View details for Web of Science ID 001194120700100
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Measuring Molecular Diffusion in Self-Organizing Xenopus Extracts by Fluorescence Correlation Spectroscopy.
Methods in molecular biology (Clifton, N.J.)
2024; 2740: 107-115
Abstract
The cytoplasm is densely packed with macromolecules and organelles, displaying viscoelastic properties at various scales. How biochemical reactions function efficiently enough in a seemingly jammed environment remains elusive. Cell-free Xenopus laevis extracts represent a powerful system for investigating the biochemistry and biophysics of living systems. Here we present a protocol for characterizing macromolecular diffusion in self-organizing cytoplasmic extracts using fluorescence correlation spectroscopy (FCS), which measures the motions on a distance scale of ~200nm. The method can also be used to characterize diffusion in the cytoplasm as it progresses through different phases of the cell cycle.
View details for DOI 10.1007/978-1-0716-3557-5_6
View details for PubMedID 38393471
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Constrained Diffusion with Trust Sampling
edited by Globerson, A., Mackey, L., Belgrave, D., Fan, A., Paquet, U., Tomczak, J., Zhang, C.
NEURAL INFORMATION PROCESSING SYSTEMS (NIPS). 2024
View details for Web of Science ID 001633268100205
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Robust trigger wave speed in Xenopus cytoplasmic extracts.
bioRxiv : the preprint server for biology
2023
Abstract
Self-regenerating trigger waves can spread rapidly through the crowded cytoplasm without diminishing in amplitude or speed, providing consistent, reliable, long-range communication. The macromolecular concentration of the cytoplasm varies in response to physiological and environmental fluctuations, raising the question of how or if trigger waves can robustly operate in the face of such fluctuations. Using Xenopus extracts, we found that mitotic and apoptotic trigger wave speeds are remarkably invariant. We derived a model that accounts for this robustness and for the eventual slowing at extremely high and low cytoplasmic concentrations. The model implies that the positive and negative effects of cytoplasmic concentration (increased reactant concentration vs. increased viscosity) are nearly precisely balanced. Accordingly, artificially maintaining a constant cytoplasmic viscosity during dilution abrogates this robustness. The robustness in trigger wave speeds may contribute to the reliability of the extremely rapid embryonic cell cycle.
View details for DOI 10.1101/2023.12.22.573127
View details for PubMedID 38187567
View details for PubMedCentralID PMC10769400
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Molecular Layer Deposition of Organic-Inorganic Hafnium Oxynitride Hybrid Films for Electrochemical Applications
ACS APPLIED ENERGY MATERIALS
2023; 6 (11): 5806-5816
View details for DOI 10.1021/acsaem.3c00107
View details for Web of Science ID 001005217300001
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Francis Bacon at SemEval-2023 Task 4: Ensembling BERT and GloVe for Value Identification in Arguments
edited by Ojha, A. K., Dogruoz, A. S., Madabushi, H. T., Kumar, R., Sartori, E., DaSanMartino, G.
ASSOC COMPUTATIONAL LINGUISTICS-ACL. 2023: 2039-2042
View details for Web of Science ID 001281001900279
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Resolving Current-Dependent Regimes of Electroplating Mechanisms for Fast Charging Lithium Metal Anodes.
Nano letters
2022
Abstract
Poor fast-charge capabilities limit the usage of rechargeable Li metal anodes. Understanding the connection between charging rate, electroplating mechanism, and Li morphology could enable fast-charging solutions. Here, we develop a combined electroanalytical and nanoscale characterization approach to resolve the current-dependent regimes of Li plating mechanisms and morphology. Measurement of Li+ transport through the solid electrolyte interphase (SEI) shows that low currents induce plating at buried Li||SEI interfaces, but high currents initiate SEI-breakdown and plating at fresh Li||electrolyte interfaces. The latter pathway can induce uniform growth of {110}-faceted Li at extremely high currents, suggesting ion-transport limitations alone are insufficient to predict Li morphology. At battery relevant fast-charging rates, SEI-breakdown above a critical current density produces detrimental morphology and poor cyclability. Thus, prevention of both SEI-breakdown and slow ion-transport in the electrolyte is essential. This mechanistic insight can inform further electrolyte engineering and customization of fast-charging protocols for Li metal batteries.
View details for DOI 10.1021/acs.nanolett.2c02792
View details for PubMedID 36214378
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Multicenter Long-Term Follow Up of Allogeneic Hematopoietic Stem Cell Transplantation With Omidubicel: A Pooled Analysis of Five Prospective Clinical Trials
CIG MEDIA GROUP, LP. 2022: S442
View details for Web of Science ID 000897948100541
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Cytoplasmic organization promotes protein diffusion in Xenopus extracts.
Nature communications
2022; 13 (1): 5599
Abstract
The cytoplasm is highly organized. However, the extent to which this organization influences the dynamics of cytoplasmic proteins is not well understood. Here, we use Xenopus laevis egg extracts as a model system to study diffusion dynamics in organized versus disorganized cytoplasm. Such extracts are initially homogenized and disorganized, and self-organize into cell-like units over the course of tens of minutes. Using fluorescence correlation spectroscopy, we observe that as the cytoplasm organizes, protein diffusion speeds up by about a factor of two over a length scale of a few hundred nanometers, eventually approaching the diffusion time measured in organelle-depleted cytosol. Even though the ordered cytoplasm contained organelles and cytoskeletal elements that might interfere with diffusion, the convergence of protein diffusion in the cytoplasm toward that in organelle-depleted cytosol suggests that subcellular organization maximizes protein diffusivity. The effect of organization on diffusion varies with molecular size, with the effects being largest for protein-sized molecules, and with the time scale of the measurement. These results show that cytoplasmic organization promotes the efficient diffusion of protein molecules in a densely packed environment.
View details for DOI 10.1038/s41467-022-33339-0
View details for PubMedID 36151204
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Electrical resistance of the current collector controls lithium morphology.
Nature communications
2022; 13 (1): 3986
Abstract
The electrodeposition of low surface area lithium is critical to successful adoption of lithium metal batteries. Here, we discover the dependence of lithium metal morphology on electrical resistance of substrates, enabling us to design an alternative strategy for controlling lithium morphology and improving electrochemical performance. By modifying the current collector with atomic layer deposited conductive (ZnO, SnO2) and resistive (Al2O3) nanofilms, we show that conductive films promote the formation of high surface area lithium deposits, whereas highly resistive films promote the formation of lithium clusters of low surface area. We reveal an electrodeposition mechanism in which radial diffusion of electroactive species is promoted on resistive substrates, resulting in lateral growth of large (150m in diameter) planar lithium deposits. Using resistive substrates, similar lithium morphologies are formed in three distinct classes of electrolytes, resulting in up to ten-fold improvement in battery performance. Ultimately, we report anode-free pouch cells using the Al2O3-modified copper that maintain 60 % of their initial discharge capacity after 100 cycles, displaying the benefits of resistive substrates for controlling lithium electrodeposition.
View details for DOI 10.1038/s41467-022-31507-w
View details for PubMedID 35821247
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Graphene coating on silicon anodes enabled by thermal surface modification for high-energy lithium-ion batteries
MRS BULLETIN
2022
View details for DOI 10.1557/s43577-021-00191-4
View details for Web of Science ID 000771066700003
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Cytoplasmic organization modulates reaction kinetics in cells
CELL PRESS. 2022: 149
View details for Web of Science ID 000759523000722
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Suspension electrolyte with modified Li+ solvation environment for lithium metal batteries.
Nature materials
1800
Abstract
Designing a stable solid-electrolyte interphase on a Li anode is imperative to developing reliable Li metal batteries. Herein, we report a suspension electrolyte design that modifies the Li+ solvation environment in liquid electrolytes and creates inorganic-rich solid-electrolyte interphases on Li. Li2O nanoparticles suspended in liquid electrolytes were investigated as a proof of concept. Through theoretical and empirical analyses of Li2O suspension electrolytes, the roles played by Li2O in the liquid electrolyte and solid-electrolyte interphases of the Li anode are elucidated. Also, the suspension electrolyte design is applied in conventional and state-of-the-art high-performance electrolytes to demonstrate its applicability. Based on electrochemical analyses, improved Coulombic efficiency (up to ~99.7%), reduced Li nucleation overpotential, stabilized Li interphases and prolonged cycle life of anode-free cells (~70 cycles at 80% of initial capacity) were achieved with the suspension electrolytes. We expect this design principle and our findings to be expanded into developing electrolytes and solid-electrolyte interphases for Li metal batteries.
View details for DOI 10.1038/s41563-021-01172-3
View details for PubMedID 35039645
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Capturing the swelling of solid-electrolyte interphase in lithium metal batteries.
Science (New York, N.Y.)
1800; 375 (6576): 66-70
Abstract
[Figure: see text].
View details for DOI 10.1126/science.abi8703
View details for PubMedID 34990230
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Stochasticity and positive feedback enable enzyme kinetics at the membrane to sense reaction size.
Proceedings of the National Academy of Sciences of the United States of America
2021; 118 (47)
Abstract
Here, we present detailed kinetic analyses of a panel of soluble lipid kinases and phosphatases, as well as Ras activating proteins, acting on their respective membrane surface substrates. The results reveal that the mean catalytic rate of such interfacial enzymes can exhibit a strong dependence on the size of the reaction system-in this case membrane area. Experimental measurements and kinetic modeling reveal how stochastic effects stemming from low molecular copy numbers of the enzymes alter reaction kinetics based on mechanistic characteristics of the enzyme, such as positive feedback. For the competitive enzymatic cycles studied here, the final product-consisting of a specific lipid composition or Ras activity state-depends on the size of the reaction system. Furthermore, we demonstrate how these reaction size dependencies can be controlled by engineering feedback mechanisms into the enzymes.
View details for DOI 10.1073/pnas.2103626118
View details for PubMedID 34789575
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Relating cellular signaling timescales to single-molecule kinetics: A first-passage time analysis of Ras activation by SOS.
Proceedings of the National Academy of Sciences of the United States of America
2021; 118 (45)
Abstract
Son of Sevenless (SOS) is a Ras guanine nucleotide exchange factor (GEF) that plays a central role in numerous cellular signaling pathways. Like many other signaling molecules, SOS is autoinhibited in the cytosol and activates only after recruitment to the membrane. The mean activation time of individual SOS molecules has recently been measured to be 60 s, which is unexpectedly long and seemingly contradictory with cellular signaling timescales, which have been measured to be as fast as several seconds. Here, we rectify this discrepancy using a first-passage time analysis to reconstruct the effective signaling timescale of multiple SOS molecules from their single-molecule activation kinetics. Along with corresponding experimental measurements, this analysis reveals how the functional response time, comprised of many slowly activating molecules, can become substantially faster than the average molecular kinetics. This consequence stems from the enzymatic processivity of SOS in a highly out-of-equilibrium reaction cycle during receptor triggering. Ultimately, rare, early activation events dominate the macroscopic reaction dynamics.
View details for DOI 10.1073/pnas.2103598118
View details for PubMedID 34740968
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Potentiometric Measurement to Probe Solvation Energy and Its Correlation to Lithium Battery Cyclability.
Journal of the American Chemical Society
2021
Abstract
The electrolyte plays a critical role in lithium-ion batteries, as it impacts almost every facet of a battery's performance. However, our understanding of the electrolyte, especially solvation of Li+, lags behind its significance. In this work, we introduce a potentiometric technique to probe the relative solvation energy of Li+ in battery electrolytes. By measuring open circuit potential in a cell with symmetric electrodes and asymmetric electrolytes, we quantitatively characterize the effects of concentration, anions, and solvents on solvation energy across varied electrolytes. Using the technique, we establish a correlation between cell potential (Ecell) and cyclability of high-performance electrolytes for lithium metal anodes, where we find that solvents with more negative cell potentials and positive solvation energies-those weakly binding to Li+-lead to improved cycling stability. Cryogenic electron microscopy reveals that weaker solvation leads to an anion-derived solid-electrolyte interphase that stabilizes cycling. Using the potentiometric measurement for characterizing electrolytes, we establish a correlation that can guide the engineering of effective electrolytes for the lithium metal anode.
View details for DOI 10.1021/jacs.1c03868
View details for PubMedID 34184873
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Dual-Solvent Li-Ion Solvation Enables High-Performance Li-Metal Batteries
ADVANCED MATERIALS
2021: e2008619
Abstract
Novel electrolyte designs to further enhance the lithium (Li) metal battery cyclability are highly desirable. Here, fluorinated 1,6-dimethoxyhexane (FDMH) is designed and synthesized as the solvent molecule to promote electrolyte stability with its prolonged -CF2 - backbone. Meanwhile, 1,2-dimethoxyethane is used as a co-solvent to enable higher ionic conductivity and much reduced interfacial resistance. Combining the dual-solvent system with 1 m lithium bis(fluorosulfonyl)imide (LiFSI), high Li-metal Coulombic efficiency (99.5%) and oxidative stability (6 V) are achieved. Using this electrolyte, 20 µm Li||NMC batteries are able to retain ≈80% capacity after 250 cycles and Cu||NMC anode-free pouch cells last 120 cycles with 75% capacity retention under ≈2.1 µL mAh-1 lean electrolyte conditions. Such high performances are attributed to the anion-derived solid-electrolyte interphase, originating from the coordination of Li-ions to the highly stable FDMH and multiple anions in their solvation environments. This work demonstrates a new electrolyte design strategy that enables high-performance Li-metal batteries with multisolvent Li-ion solvation with rationally optimized molecular structure and ratio.
View details for DOI 10.1002/adma.202008619
View details for Web of Science ID 000648495100001
View details for PubMedID 33969571
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Corrosion of lithium metal anodes during calendar ageing and its microscopic origins
NATURE ENERGY
2021
View details for DOI 10.1038/s41560-021-00787-9
View details for Web of Science ID 000631480700002
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Organic wastewater treatment by a single-atom catalyst and electrolytically produced H2O2.
Nature sustainability
2021; 4: 233-241
Abstract
The presence of organic contaminants in wastewater poses considerable risks to the health of both humans and ecosystems. Although advanced oxidation processes that rely on highly reactive radicals to destroy organic contaminants are appealing treatment options, substantial energy and chemical inputs limit their practical applications. Here we demonstrate that Cu single atoms incorporated in graphitic carbon nitride can catalytically activate H2O2 to generate hydroxyl radicals at pH 7.0 without energy input, and show robust stability within a filtration device. We further design an electrolysis reactor for the on-site generation of H2O2 from air, water and renewable energy. Coupling the single-atom catalytic filter and the H2O2 electrolytic generator in tandem delivers a wastewater treatment system. These findings provide a promising path toward reducing the energy and chemical demands of advanced oxidation processes, as well as enabling their implementation in remote areas and isolated communities.
View details for DOI 10.1038/s41893-020-00635-w
View details for PubMedID 34355066
View details for PubMedCentralID PMC8330436
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Efficient Lithium Metal Cycling over a Wide Range of Pressures from an Anion-Derived Solid-Electrolyte Interphase Framework
ACS ENERGY LETTERS
2021; 6 (2): 816–25
View details for DOI 10.1021/acsenergylett.0c02533
View details for Web of Science ID 000619803400061
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Cathode-Electrolyte Interphase in Lithium Batteries Revealed by Cryogenic Electron Microscopy
MATTER
2021; 4 (1)
View details for DOI 10.1016/j.matt.2020.10.021
View details for Web of Science ID 000608248900009
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Underpotential lithium plating on graphite anodes caused by temperature heterogeneity.
Proceedings of the National Academy of Sciences of the United States of America
2020
Abstract
Rechargeability and operational safety of commercial lithium (Li)-ion batteries demand further improvement. Plating of metallic Li on graphite anodes is a critical reason for Li-ion battery capacity decay and short circuit. It is generally believed that Li plating is caused by the slow kinetics of graphite intercalation, but in this paper, we demonstrate that thermodynamics also serves a crucial role. We show that a nonuniform temperature distribution within the battery can make local plating of Li above 0 V vs. Li0/Li+ (room temperature) thermodynamically favorable. This phenomenon is caused by temperature-dependent shifts of the equilibrium potential of Li0/Li+ Supported by simulation results, we confirm the likelihood of this failure mechanism during commercial Li-ion battery operation, including both slow and fast charging conditions. This work furthers the understanding of nonuniform Li plating and will inspire future studies to prolong the cycling lifetime of Li-ion batteries.
View details for DOI 10.1073/pnas.2009221117
View details for PubMedID 33168752
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Organic wastewater treatment by a single-atom catalyst and electrolytically produced H2O2
NATURE SUSTAINABILITY
2020
View details for DOI 10.1038/s41893-020-00635-w
View details for Web of Science ID 000588002700001
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Revealing and Elucidating ALD-Derived Control of Lithium Plating Microstructure
ADVANCED ENERGY MATERIALS
2020
View details for DOI 10.1002/aenm.202002736
View details for Web of Science ID 000578514900001
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Microclusters of Kinked Silicon Nanowires Synthesized by a Recyclable Iodide Process for High-Performance Lithium-Ion Battery Anodes
ADVANCED ENERGY MATERIALS
2020
View details for DOI 10.1002/aenm.202002108
View details for Web of Science ID 000573081400001
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Nickel Impurities in the Solid-Electrolyte Interphase of Lithium-Metal Anodes Revealed by Cryogenic Electron Microscopy
CELL REPORTS PHYSICAL SCIENCE
2020; 1 (9)
View details for DOI 10.1016/j.xcrp.2020.100188
View details for Web of Science ID 000658752300015
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Coupled Membrane Lipid Miscibility and Phosphotyrosine-Driven Protein Condensation Phase Transitions.
Biophysical journal
2020
Abstract
Lipid miscibility phase separation has long been considered to be a central element of cell membrane organization. More recently, protein condensation phase transitions, into three-dimensional droplets or in two-dimensional lattices on membrane surfaces, have emerged as another important organizational principle within cells. Here, we reconstitute the linker for activation of Tcells (LAT):growth-factor-receptor-bound protein 2 (Grb2):son of sevenless (SOS) protein condensation on the surface of giant unilamellar vesicles capable of undergoing lipid phase separations. Our results indicate that the assembly of the protein condensate on the membrane surface can drive lipid phase separation. This phase transition occurs isothermally and is governed by tyrosine phosphorylation on LAT. Furthermore, we observe that the induced lipid phase separation drives localization of the SOS substrate, K-Ras, into the LAT:Grb2:SOS protein condensate.
View details for DOI 10.1016/j.bpj.2020.09.017
View details for PubMedID 33080222
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Opportunities for Cryogenic Electron Microscopy in Materials Science and Nanoscience.
ACS nano
2020
Abstract
Cryogenic electron microscopy (cryo-EM) was the basis for the 2017 Nobel Prize in Chemistry for its profound impact on the field of structural biology by freezing and stabilizing fragile biomolecules for near atomic-resolution imaging in their native states. Beyond life science, the development of cryo-EM for the physical sciences may offer access to previously inaccessible length scales for materials characterization in systems that would otherwise be too sensitive for high-resolution electron microscopy and spectroscopy. Weakly bonded and reactive materials that typically degrade under electron irradiation and environmental exposure can potentially be stabilized by cryo-EM, opening up exciting opportunities to address many central questions in materials science. New discoveries and fundamental breakthroughs in understanding are likely to follow. In this Perspective, we identify six major areas in materials science that may benefit from the interdisciplinary application of cryo-EM: (1) batteries, (2) soft polymers, (3) metal-organic frameworks, (4) perovskite solar cells, (5) electrocatalysts, and (6) quantum materials. We highlight long-standing questions in each of these areas that cryo-EM can potentially address, which would firmly establish the powerful tool's broad scope and utility beyond biology.
View details for DOI 10.1021/acsnano.0c05020
View details for PubMedID 32806083
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Molecular design for electrolyte solvents enabling energy-dense and long-cycling lithium metal batteries
NATURE ENERGY
2020
View details for DOI 10.1038/s41560-020-0634-5
View details for Web of Science ID 000542060100001
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AUTHOR REPLY.
Urology
2020; 140: 121
View details for DOI 10.1016/j.urology.2020.01.051
View details for PubMedID 32456860
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Tortuosity Effects in Lithium-Metal Host Anodes
JOULE
2020; 4 (4): 938–52
View details for DOI 10.1016/j.joule.2020.03.008
View details for Web of Science ID 000527264500022
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Improving Lithium Metal Composite Anodes with Seeding and Pillaring Effects of Silicon Nanoparticles.
ACS nano
2020
Abstract
Metallic lithium (Li) anodes are crucial for the development of high specific energy batteries yet are plagued by their poor cycling efficiency. Electrode architecture engineering is vital for maintaining a stable anode volume and suppressing Li corrosion during cycling. In this paper, a reduced graphene oxide "host" framework for Li metal anodes is further optimized by embedding silicon (Si) nanoparticles between the graphene layers. They serve as Li nucleation seeds to promote Li deposition within the framework even without prestored Li. Meanwhile, the LixSi alloy particles serve as supporting "pillars" between the graphene layers, enabling a minimized thickness shrinkage after full stripping of metallic Li. Combined with a Li compatible electrolyte, a 99.4% Coulombic efficiency over 600 cycles is achieved, and stable cycling of a Li||NMC532 full cell for 380 cycles with negligible capacity decay is realized.
View details for DOI 10.1021/acsnano.0c00184
View details for PubMedID 32271533
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Resolving Nanoscopic and Mesoscopic Heterogeneity of Fluorinated Species in Battery Solid-Electrolyte Interphases by Cryogenic Electron Microscopy
ACS ENERGY LETTERS
2020; 5 (4): 1128–35
View details for DOI 10.1021/acsenergylett.0c00194
View details for Web of Science ID 000526315900015
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Scalable synthesis of nanoporous silicon microparticles for highly cyclable lithium-ion batteries
NANO RESEARCH
2020
View details for DOI 10.1007/s12274-020-2770-4
View details for Web of Science ID 000524406500005
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Transient Voltammetry with Ultramicroelectrodes Reveals the Electron Transfer Kinetics of Lithium Metal Anodes
Adv. Energy Lett.
2020; 5: 701-709
View details for DOI 10.1021/acsenergylett.0c00031
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Alvimopan is Associated with a Reduction in Length of Stay and Hospital Costs for Patients Undergoing Radical Cystectomy.
Urology
2020
Abstract
To evaluate the impact of alvimopan in patient undergoing radical cystectomy (RC) for bladder cancer. We hypothesize that alvimopan can decrease cost for RC by reducing length of stay (LOS).We identified patients who underwent elective RC for bladder cancer from 2009 to 2015 in the Premier Healthcare Database, a nationwide, all-payer hospital-based database, and compared patients who received and did not receive alvimopan in the perioperative period. Hospitals that had no record of administering alvimopan for patients undergoing RC were excluded. The primary outcomes were LOS and the direct hospital costs. The secondary outcomes were 90-day readmission for ileus and major complications.After applying the inclusion criteria, the study cohort consisted of 1087 patients with 511 patients receiving perioperative alvimopan. Alvimopan was associated with a reduction in hospital costs by -$2,709 (95%CI: -$4,507 to -$912, p=0.003), decreased median LOS (7 vs 8 days, p<0.001), and lower likelihood of readmission for ileus (adjusted OR: 0.63, p=0.041). While alvimopan use led to higher pharmacy costs, this was outweighed by lower room and board costs due to the reduced LOS. There was no significant difference between two groups regarding major complications. These results were robust across multiple adjusted regression models.Our data show that alvimopan is associated with a substantial cost-saving in patients undergoing radical cystectomy, and suggest that routine use of alvimopan may be a potential cost-effective strategy to reduce the overall financial burden of bladder cancer.
View details for DOI 10.1016/j.urology.2020.01.049
View details for PubMedID 32268172
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A Water Stable, Near-Zero-Strain O3-Layered Titanium-Based Anode for Long Cycle Sodium-Ion Battery
ADVANCED FUNCTIONAL MATERIALS
2019
View details for DOI 10.1002/adfm.201907023
View details for Web of Science ID 000502900800001
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Monolithic solid-electrolyte interphases formed in fluorinated orthoformate-based electrolytes minimize Li depletion and pulverization
NATURE ENERGY
2019; 4 (9): 796–805
View details for DOI 10.1038/s41560-019-0464-5
View details for Web of Science ID 000486098400014
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Preventing Li depletion and pulverization by monolithic SEI layer generated in fluorinated orthoformate based electrolytes
AMER CHEMICAL SOC. 2019
View details for Web of Science ID 000525055505258
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Cryo-EM Structures of Atomic Surfaces and Host-Guest Chemistry in Metal-Organic Frameworks
MATTER
2019; 1 (2): 428–38
View details for DOI 10.1016/j.matt.2019.06.001
View details for Web of Science ID 000519688200015
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Cryo-EM structures of atomic surfaces and host-guest chemistry in metal-organic frameworks.
Matter
2019; 1 (2): 428-438
Abstract
Host-guest interactions govern the chemistry of a broad range of functional materials, but direct imaging using conventional transmission electron microscopy (TEM) has not been possible. This problem is exacerbated in metal-organic framework (MOF) materials, which are easily damaged by the electron beam. Here, we use cryogenic-electron microscopy (cryo-EM) to stabilize the host-guest structure and resolve the atomic surface of zeolitic imidazolate framework (ZIF-8) and its interaction with guest CO2 molecules. We image step-edge sites on the ZIF-8 surface that provides insight to its growth behavior. Furthermore, we observe two distinct binding sites for CO2 within the ZIF-8 pore, which are predicted by density functional theory (DFT) to be energetically favorable. This CO2 insertion induces an apparent ~3% lattice expansion along the <002> and <011> directions of the ZIF-8 unit cell. The ability to stabilize and preserve host-guest chemistry opens a rich materials space for scientific exploration and discovery using cryo-EM.
View details for DOI 10.1016/j.matt.2019.06.001
View details for PubMedID 34104881
View details for PubMedCentralID PMC8184120
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Improving cyclability of Li metal batteries at elevated temperatures and its origin revealed by cryo-electron microscopy
NATURE ENERGY
2019; 4 (8): 664–70
View details for DOI 10.1038/s41560-019-0413-3
View details for Web of Science ID 000481484400014
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Stochastic geometry sensing and polarization in a lipid kinase-phosphatase competitive reaction.
Proceedings of the National Academy of Sciences of the United States of America
2019
Abstract
Phosphorylation reactions, driven by competing kinases and phosphatases, are central elements of cellular signal transduction. We reconstituted a native eukaryotic lipid kinase-phosphatase reaction that drives the interconversion of phosphatidylinositol-4-phosphate [PI(4)P] and phosphatidylinositol-4,5-phosphate [PI(4,5)P2] on membrane surfaces. This system exhibited bistability and formed spatial composition patterns on supported membranes. In smaller confined regions of membrane, rapid diffusion ensures the system remains spatially homogeneous, but the final outcome-a predominantly PI(4)P or PI(4,5)P2 membrane composition-was governed by the size of the reaction environment. In larger confined regions, interplay between the reactions, diffusion, and confinement created a variety of differentially patterned states, including polarization. Experiments and kinetic modeling reveal how these geometric confinement effects arise from a mechanism based on stochastic fluctuations in the copy number of membrane-bound kinases and phosphatases. The underlying requirements for such behavior are unexpectedly simple and likely to occur in natural biological signaling systems.
View details for DOI 10.1073/pnas.1901744116
View details for PubMedID 31278151
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Surface-engineered mesoporous silicon microparticles as high-Coulombic-efficiency anodes for lithium-ion batteries
NANO ENERGY
2019; 61: 404–10
View details for DOI 10.1016/j.nanoen.2019.04.070
View details for Web of Science ID 000471201800048
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Fast galvanic lithium corrosion involving a Kirkendall-type mechanism
NATURE CHEMISTRY
2019; 11 (4): 382–89
View details for DOI 10.1038/s41557-018-0203-8
View details for Web of Science ID 000462046600017
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Fast galvanic lithium corrosion involving a Kirkendall-type mechanism.
Nature chemistry
2019
Abstract
Developing a viable metallic lithium anode is a prerequisite for next-generation batteries. However, the low redox potential of lithium metal renders it prone to corrosion, which must be thoroughly understood for it to be used in practical energy-storage devices. Here we report a previously overlooked mechanism by which lithium deposits can corrode on a copper surface. Voids are observed in the corroded deposits and a Kirkendall-type mechanism is validated through electrochemical analysis. Although it is a long-held view that lithium corrosion in electrolytes involves direct charge-transfer through the lithium-electrolyte interphase, the corrosion observed here is found to be governed by a galvanic process between lithium and the copper substrate-a pathway largely neglected by previous battery corrosion studies. The observations are further rationalized by detailed analyses of the solid-electrolyte interphase formed on copper and lithium, where the disparities in electrolyte reduction kinetics on the two surfaces can account for the fast galvanic process.
View details for PubMedID 30664717
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Nanostructural and Electrochemical Evolution of the Solid-Electrolyte Interphase on CuO Nanowires Revealed by Cryogenic-Electron Microscopy and Impedance Spectroscopy
ACS NANO
2019; 13 (1): 737–44
Abstract
Battery performance is critically dependent on the nanostructure and electrochemical properties of the solid-electrolyte interphase (SEI) - a passivation film that exists on most lithium battery anodes. However, knowledge of how the SEI nanostructure forms and its impact on ionic transport remains limited due to its sensitivity to transmission electron microscopy and difficulty in accurately probing the SEI impedance. Here, we track the voltage-dependent, stepwise evolution of the nanostructure and impedance of the SEI on CuO nanowires using cryogenic-electron microscopy (cryo-EM) and electrochemical impedance spectroscopy (EIS). In carbonate electrolyte, the SEI forms at 1.0 V vs Li/Li+ as a 3 nm-thick amorphous SEI and grows to 4 nm at 0.5 V; as the potential approaches 0.0 V vs Li/Li+, the SEI on the CuO nanowires forms an 8 nm-thick inverted multilayered nanostructure in ethylene carbonate/diethyl carbonate (EC/DEC) electrolyte with 10 vol. % fluoroethylene carbonate (FEC) and a mosaic nanostructure in EC/DEC electrolyte. Upon Li deposition, the total SEI thickness grows to 16 nm and significant growth of the inner amorphous layer takes place in the inverted multilayered nanostructure, indicating electrolyte permeates the SEI. Using a refined EIS methodology, we isolate the SEI impedance on Cu and find that the SEI nanostructure directly correlates to macroscopic Li-ion transport through the SEI. The inverted layered nanostructure decreases the interfacial impedance upon formation, whereas the mosaic nanostructure continually increases the interfacial impedance during growth. These structural and electrochemical findings illustrate a more complete portrait of SEI formation and guide further improvements in engineered SEI.
View details for DOI 10.1021/acsnano.8b08012
View details for Web of Science ID 000456749900075
View details for PubMedID 30589528
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Dynamic Structure and Chemistry of the Silicon Solid-Electrolyte Interphase Visualized by Cryogenic Electron Microscopy
Matter
2019; 1 (5)
View details for DOI 10.1016/j.matt.2019.09.020
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Evolution of the Solid-Electrolyte Interphase on Carbonaceous Anodes Visualized by Atomic-Resolution Cryogenic Electron Microscopy.
Nano letters
2019
Abstract
The stability of modern lithium-ion batteries depends critically on an effective solid-electrolyte interphase (SEI), a passivation layer that forms on the carbonaceous negative electrode as a result of electrolyte reduction. However, a nanoscopic understanding of how the SEI evolves with battery aging remains limited due to the difficulty in characterizing the structural and chemical properties of this sensitive interphase. In this work, we image the SEI on carbon black negative electrodes using cryogenic transmission electron microscopy (cryo-TEM) and track its evolution during cycling. We find that a thin, primarily amorphous SEI nucleates on the first cycle, which further evolves into one of two distinct SEI morphologies upon further cycling: (1) a compact SEI, with a high concentration of inorganic components that effectively passivates the negative electrode; and (2) an extended SEI spanning hundreds of nanometers. This extended SEI grows on particles that lack a compact SEI and consists primarily of alkyl carbonates. The diversity in observed SEI morphologies suggests that SEI growth is a highly heterogeneous process. The simultaneous emergence of these distinct SEI morphologies highlights the necessity of effective passivation by the SEI, as large-scale extended SEI growths negatively impact lithium-ion transport, contribute to capacity loss, and may accelerate battery failure.
View details for DOI 10.1021/acs.nanolett.9b01515
View details for PubMedID 31322896
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A molecular assembly phase transition and kinetic proofreading modulate Ras activation by SOS.
Science (New York, N.Y.)
2019; 363 (6431): 1098–1103
Abstract
The guanine nucleotide exchange factor (GEF) Son of Sevenless (SOS) is a key Ras activator that is autoinhibited in the cytosol and activates upon membrane recruitment. Autoinhibition release involves structural rearrangements of the protein at the membrane and thus introduces a delay between initial recruitment and activation. In this study, we designed a single-molecule assay to resolve the time between initial receptor-mediated membrane recruitment and the initiation of GEF activity of individual SOS molecules on microarrays of Ras-functionalized supported membranes. The rise-and-fall shape of the measured SOS activation time distribution and the long mean time scale to activation (~50 seconds) establish a basis for kinetic proofreading in the receptor-mediated activation of Ras. We further demonstrate that this kinetic proofreading is modulated by the LAT (linker for activation of T cells)-Grb2-SOS phosphotyrosine-driven phase transition at the membrane.
View details for DOI 10.1126/science.aau5721
View details for PubMedID 30846600
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Proceedings of the fifth international RASopathies symposium: When development and cancer intersect
AMERICAN JOURNAL OF MEDICAL GENETICS PART A
2018; 176 (12): 2924–29
View details for DOI 10.1002/ajmg.a.40632
View details for Web of Science ID 000454612700060
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Correlating Structure and Function of Battery Interphases at Atomic Resolution Using Cryoelectron Microscopy
JOULE
2018; 2 (10): 2167–77
View details for DOI 10.1016/j.joule.2018.08.004
View details for Web of Science ID 000447735000021
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Proceedings of the fifth international RASopathies symposium: When development and cancer intersect.
American journal of medical genetics. Part A
2018: e40632
Abstract
This report summarizes and highlights the fifth International RASopathies Symposium: When Development and Cancer Intersect, held in Orlando, Florida in July 2017. The RASopathies comprise a recognizable pattern of malformation syndromes that are caused by germ line mutations in genes that encode components of the RAS/mitogen-activated protein kinase (MAPK) pathway. Because of their common underlying pathogenetic etiology, there is significant overlap in their phenotypic features, which includes craniofacial dysmorphology, cardiac, cutaneous, musculoskeletal, gastrointestinal and ocular abnormalities, neurological and neurocognitive issues, and a predisposition to cancer. The RAS pathway is a well-known oncogenic pathway that is commonly found to be activated in somatic malignancies. As in somatic cancers, the RASopathies can be caused by various pathogenetic mechanisms that ultimately impact or alter the normal function and regulation of the MAPK pathway. As such, the RASopathies represent an excellent model of study to explore the intersection of the effects of dysregulation and its consequence in both development and oncogenesis.
View details for PubMedID 30302932
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Core-Shell Nanofibrous Materials with High Particulate Matter Removal Efficiencies and Thermally Triggered Flame Retardant Properties.
ACS central science
2018; 4 (7): 894–98
Abstract
Dust filtration is a crucial process for industrial waste gas treatment. Great efforts have been devoted to improve the performance of dust filtration filters both in industrial and fundamental research. Conventional air-filtering materials are limited by three key issues: (1) Low filtration efficiency, especially for particulate matter (PM) below 1 mum; (2) large air pressure drops across the filter, which require a high energy input to overcome; and (3) safety hazards such as dust explosions and fires. Here, we have developed a "smart" multifunctional material which can capture PM with high efficiency and an extremely low pressure drop, while possessing a flame retardant design. This multifunctionality is achieved through a core-shell nanofiber design with the polar polymer Nylon-6 as the shell and the flame retardant triphenyl phosphate (TPP) as the core. At 80% optical transmittance, the multifunctional materials showed capture efficiency of 99.00% for PM2.5 and >99.50% for PM10-2.5, with a pressure drop of only 0.25 kPa (0.2% of atmospheric pressure) at a flow rate of 0.5 m s-1. Moreover, during direct ignition tests, the multifunctional materials showed extraordinary flame retardation; the self-extinguishing time of the filtrate-contaminated filter is nearly instantaneous (0 s/g) compared to 150 s/g for unmodified Nylon-6.
View details for PubMedID 30062118
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Core-Shell Nanofibrous Materials with High Particulate Matter Removal Efficiencies and Thermally Triggered Flame Retardant Properties
ACS CENTRAL SCIENCE
2018; 4 (7): 894–98
View details for DOI 10.1021/acscentsci.8b00285
View details for Web of Science ID 000439816200016
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Engineering stable interfaces for three-dimensional lithium metal anodes.
Science advances
2018; 4 (7): eaat5168
Abstract
Lithium metal has long been considered one of the most promising anode materials for advanced lithium batteries (for example, Li-S and Li-O2), which could offer significantly improved energy density compared to state-of-the-art lithium ion batteries. Despite decades of intense research efforts, its commercialization remains limited by poor cyclability and safety concerns of lithium metal anodes. One root cause is the parasitic reaction between metallic lithium and the organic liquid electrolyte, resulting in continuous formation of an unstable solid electrolyte interphase, which consumes both active lithium and electrolyte. Until now, it has been challenging to completely shut down the parasitic reaction. We find that a thin-layer coating applied through atomic layer deposition on a hollow carbon host guides lithium deposition inside the hollow carbon sphere and simultaneously prevents electrolyte infiltration by sealing pinholes on the shell of the hollow carbon sphere. By encapsulating lithium inside the stable host, parasitic reactions are prevented, resulting in impressive cycling behavior. We report more than 500 cycles at a high coulombic efficiency of 99% in an ether-based electrolyte at a cycling rate of 0.5 mA/cm2 and a cycling capacity of 1 mAh/cm2, which is among the most stable Li anodes reported so far.
View details for PubMedID 30062125
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Engineering stable interfaces for three-dimensional lithium metal anodes
SCIENCE ADVANCES
2018; 4 (7)
View details for DOI 10.1126/sciadv.aat5168
View details for Web of Science ID 000443176100058
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Importin-beta modulates the permeability of the nuclear pore complex in a Ran-dependent manner
ELIFE
2015; 4
Abstract
Soluble karyopherins of the importin-β (impβ) family use RanGTP to transport cargos directionally through the nuclear pore complex (NPC). Whether impβ or RanGTP regulate the permeability of the NPC itself has been unknown. In this study, we identify a stable pool of impβ at the NPC. A subpopulation of this pool is rapidly turned-over by RanGTP, likely at Nup153. Impβ, but not transportin-1 (TRN1), alters the pore's permeability in a Ran-dependent manner, suggesting that impβ is a functional component of the NPC. Upon reduction of Nup153 levels, inert cargos more readily equilibrate across the NPC yet active transport is impaired. When purified impβ or TRN1 are mixed with Nup153 in vitro, higher-order, multivalent complexes form. RanGTP dissolves the impβ•Nup153 complexes but not those of TRN1•Nup153. We propose that impβ and Nup153 interact at the NPC's nuclear face to form a Ran-regulated mesh that modulates NPC permeability.
View details for DOI 10.7554/eLife.04052
View details for Web of Science ID 000351864100002
View details for PubMedID 25748139
View details for PubMedCentralID PMC4375889