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SSRN 2023年

作者： Liu, Eric Z. Popescu, Sofia Rivalta Eden, Alexander Chung, Julia Roehrich, Brian Sepunaru, Lior Department of Chemistry and Biochemistry University of California at Santa Barbara Santa BarbaraCA93106 United States Department of Chemical Engineering University of California Santa Barbara Santa BarbaraCA93106 United States Department of Mechanical Engineering University of California Santa Barbara Santa BarbaraCA93106 United States Interdepartmental Program in Biomolecular Science and Engineering University of California at Santa Barbara Santa BarbaraCA93106 United States

Blocking electrochemistry, a subfield of single-entity electrochemistry, enables in-situ sizing of redox-inactive particles. This method exploits the adsorptive impact of individual insulating particles on a microelectrode, which decreases the electrochemically active surface area of the electrode. Against the background of an electroactive redox reaction in solution, each individual impacting particle results in a discrete current drop, with the magnitude of the drop corresponding to the size of the blocking particle. One significant limitation of this technique is "edge effects", resulting from the inhomogeneous flux of the redox species’ diffusion due to increased mass transport to the edge of the disk electrode surface. "Edge effects" cause increased errors in size detection, resulting in poor analytical precision. Here, we use computational simulations to demonstrate that inhomogeneous diffusional edge flux of quasi-reversible redox species is mitigated at lowered overpotentials. This phenomenon is further illustrated experimentally by lowering the applied potential such that the system is operating under a kinetically-controlled regime instead of a diffusion-limited regime, which mitigates edge effects and increases particle sizing precision significantly. In addition, we found this method to be generalizable, as the precision enhancement is not limited to geometrically spherical particles but also occurs for cubic particles. This work presents a simple, novel methodology for edge effect mitigation with general applicability across different particle types. © 2023, The Authors. All rights reserved.

关键词： Microelectrodes

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Controlling liquid-liquid phase behavior with an active fluid

arXiv

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arXiv 2022年

作者： Tayar, Alexandra M. Caballero, Fernando Anderberg, Trevor Saleh, Omar A. Marchetti, M. Cristina Dogic, Zvonimir Department of Physics University of California Santa BarbaraCA93106 United States Materials Department University of California Santa BarbaraCA93106 United States Biomolecular Science and Engineering Program University of California Santa BarbaraCA93106 United States

Demixing of binary liquids is a ubiquitous transition, which is explained using a well-established thermodynamic formalism that requires equality of intensive thermodynamics parameters across the phase boundaries. Demixing transitions also occur when binary fluid mixtures are driven away from equilibrium, for example, by external shear flow. Predicting demixing transition under nonequilibrium non-potential conditions remains, however, a challenge. We drive liquid-liquid phase separation of attractive DNA nanostar molecules away from equilibrium using an internally driven microtubule-based active fluid. Activity lowers the critical temperature and narrows the coexistence concentrations, but only when there are mechanical bonds between the liquid droplets and the reconfiguring active fluid. Similar behaviors are observed in numerical simulations, suggesting that activity suppression of liquid-liquid phase separation is a generic feature of active LLPS. Our work describes a platform for building soft active materials with feedback control while also providing insight into cell biology, where phase separation emerged as a ubiquitous self-organizational principle. © 2022, CC BY.

关键词： Shear flow

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Machine learning identification of organic compounds using visible light

arXiv

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arXiv 2022年

作者： Bikku, Thulasi Fritz, Rubén A. Colón, Yamil J. Herrera, Felipe Department of Physics Universidad de Santiago de Chile Av. Victor Jara 3493 Santiago Chile Computer Science and Engineering Vignan's Nirula Institute of Technology and Science for Women Andhra Pradesh Guntur India Department of Chemical and Biomolecular Engineering University of Notre Dame IN United States ANID - Millennium Science Initiative Program Millennium Institute for Research in Optics Concepción Chile

Identifying chemical compounds is essential in several areas of science and engineering. Laser-based techniques are promising for autonomous compound detection because the optical response of materials encodes enough electronic and vibrational information for remote chemical identification. This has been exploited using the fingerprint region of infrared absorption spectra, which involves a dense set of absorption peaks that are unique to individual molecules, thus facilitating chemical identification. However, optical identification using visible light has not been realized. Using decades of experimental refractive index data in the scientific literature of pure organic compounds and polymers over a broad range of frequencies from the ultraviolet to the far-infrared, we develop a machine learning classifier that can accurately identify organic species based on a single-wavelength dispersive measurement in the visible spectral region, away from absorption resonances. The optical classifier proposed here could be applied to autonomous material identification protocols or applications. Copyright © 2022, The Authors. All rights reserved.

关键词： Refractive index

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Unleashing the Power of Nature: Eco-Friendly Mussel-Byssus-Inspired Pbs/Pbat Fishing Gear for Biodegradation by Marine Microbes

SSRN

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SSRN 2023年

作者： Hong, Yuri Yang, Ho-Sung Lee, Min Hee Kim, Sinyang Park, Sung Bae Hwang, Sung Yeon Park, Jeyoung Koo, Jun Mo Oh, Dongyeop Hwang, Dong Soo Gyeongsangbuk-do Pohang37673 Korea Republic of Ulsan44429 Korea Republic of Department of Plant & Environmental New Resources Graduate School of Biotechnology Kyung Hee University Gyeonggi-do 17104 Korea Republic of Department of Chemical and Biomolecular Engineering Sogang University Seoul04107 Korea Republic of Department of Organic Materials Engineering Chungnam National University Daejeon34134 Korea Republic of Department of Polymer Science and Engineering and Program in Environmental and Polymer Engineering Inha University Incheon22212 Korea Republic of

Abstract Abandoned, lost, and discarded fishing gear (ALDFG) poses global challenges for marine ecosystems as they destroy algal forests, the largest oceanic carbon dioxide sinks. Biodegradable polybutylene succinate (PBS), which has a tensile toughness similar to that of nylon, has been suggested as a potential fishing-gear material. However, its slow degradation in the marine environment and limited draping characteristics need to be addressed before it can be used in environmentally friendly fishing gear. Inspired by the mussel byssus, a mussel-thread-like holdfast known for its stiff yet extensible mechanical properties, we developed fishing gear using a mussel-byssus-mimetic fiber (artificial byssus, AB) structure. The AB was composed of poly(butylene adipate-co-butylene terephthalate) (PBAT) fibers with favorable draping characteristics coated with mechanically resilient and PBS, which demonstrated sufficient toughness and draping properties for use in fishing gear. The AB may serve as fishing-gear material capable of mitigating ALDFG issues, given its marine degradability by microbial strains that degrade PBS and PBAT. Furthermore, it could serve as a substrate for ocean afforestation, given the improved settlement and growth of seaweed spores (Pyropia yezoensis) on AB. Overall, AB-based fishing gear is expected to enhance macroalgal forest conservation and expansion, and facilitate marine carbon capture through marine afforestation. © 2023, The Authors. All rights reserved.

关键词： Butenes

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Theoretical Insights into Co2 Electroreduction on Single and Dual Heteroatom-Doped Diamonds

SSRN

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SSRN 2023年

作者： Injongkol, Yuwanda Zhang, Rui-Qin Montoya, Alejandro Rungrotmongkol, Thanyada Jungsuttiwong, Siriporn Center of Excellence in Biocatalyst and Sustainable Biotechnology Department of Biochemistry Faculty of Science Chulalongkorn University Bangkok10330 Thailand City University of Hong Kong Hong Kong School of Chemical and Biomolecular Engineering The University of Sydney SydneyNSW2006 Australia Program in Bioinformatics and Computational Biology Graduate School Chulalongkorn University Bangkok10330 Thailand Department of Chemistry Faculty of Science Ubon Ratchathani University Ubon Ratchathani34190 Thailand

We employed Periodic Density Functional Theory (DFT) to investigate the catalytic activity of single and double dopant of boron (B), nitrogen (N), and phosphorous (P) anchored on diamond surfaces for the CO2 reduction reaction (CO2RR) by analyzing reaction energy profiles. Our findings show that the double-doped catalyst exhibits lower energy barriers in CO2RR compared to the single dopants. Specifically, when considering BB and NN configurations, there is a thermodynamic preference towards the formation of formic acid (HCOOH) with overpotentials of 0.40 and 0.09 V, respectively. The co-doped catalyst comprising B and N (BN) demonstrates a tendency towards the formation of HCOOH without requiring any applied overpotentials. Notably, BN outperforms other catalysts, occupying the top position on the volcano plot, indicating the lowest limiting potential (UL), remarkable thermal stability, and the ability to suppress the competing hydrogen evolution reaction (HER). This research provides valuable insights into the product differentiation in the electroreduction of CO2. © 2023, The Authors. All rights reserved.

关键词： Density functional theory

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Asymmetric fluctuations and self-folding of active interfaces

arXiv

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arXiv 2024年

作者： Zhao, Liang Gulati, Paarth Caballero, Fernando Kolvin, Itamar Adkins, Raymond Marchetti, M. Cristina Dogic, Zvonimir Department of Physics University of California Santa Barbara Santa BarbaraCA93106 United States Department of Physics Brandeis University WalthamMA02453 United States School of Physics Georgia Institute of Technology AtlantaGA30332 United States Department of Molecular Biophysics and Biochemistry Yale University New HavenCT06520 United States Biomolecular Science and Engineering Program University of California Santa BarbaraCA93106 United States

We study the structure and dynamics of the interface separating a passive fluid from a microtubule-based active fluid. Turbulent-like active flows power giant interfacial fluctuations, which exhibit pronounced asymmetry between regions of positive and negative curvature. Experiments, numerical simulations, and theoretical arguments reveal how the interface breaks up the spatial symmetry of the fundamental bend instability to generate local vortical flows that lead to asymmetric interface fluctuations. The magnitude of interface deformations increases with activity: In the high activity limit, the interface self-folds invaginating passive droplets and generating a foam-like phase, where active fluid is perforated with passive droplets. These results demonstrate how active stresses control the structure, dynamics, and break-up of soft, deformable, and reconfigurable liquid-liquid interfaces. Copyright © 2024, The Authors. All rights reserved.

关键词： Drop breakup

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Molecular Insights into the Structure-Property Relationships of 3d Printed Polyamide Reverse-Osmosis Membrane for Desalination

SSRN

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SSRN 2022年

作者： He, Jinlong Yang, Jason McCutcheon, Jeffrey R. Li, Ying Department of Mechanical Engineering University of Connecticut StorrsCT06269 United States Division of Chemistry and Chemical Engineering California Institute of Technology PasadenaCA91125 United States Department of Chemical & Biomolecular Engineering Center for Environmental Sciences and Engineering University of Connecticut StorrsCT06269 United States Department of Mechanical Engineering Polymer Program Institute of Materials Science University of Connecticut StorrsCT06269 United States

3D-printing is an emerging method for manufacturing polyamide (PA) reserve osmosis (RO) membranes for water treatment and desalination, which can precisely control membrane structural properties, such as thickness, roughness, and resolution. However, the synthesis-structure (i.e., degree of cross-linking (DC), m-phenylenediamine/trimesoyl chloride (MPD/TMC) ratio, and membrane thickness) to property (permeability and water-salt selectivity) relationships for these membranes has not been well understood. At the same time, a microscopic understanding of the physical mechanism of water and salt transport is needed to guide the design of high-performance 3D-printed membranes and improve printing efficiency. Thus, the atomic-scale transport features and energetics of water and salt ions are studied at high pressure for the 3D-printed PA RO membranes with the different DCs and MPD/TMC ratios through non-equilibrium molecular dynamics (NEMD) simulations. Factoring in membrane structure properties, rejection ratio of salt ions and pressure-dependent water flux, 3D-printed PA membranes having an MPD/TMC ratio of 3.0:2.0 and a DC between 80%~90% attains ideal performance: high water flux, high rejection of salt ions, and excellent structural integrity. Mechanistically, water permeability for highly cross-linked PA RO membranes depends on the temporary on-and-off channels that allow water molecules to jump from one cavity to another at high pressure. In addition, higher pressures cause a rapid compaction of PA membranes’ free volume and membrane thickness. Membrane failure at high pressure is determined by the DC and MPD/TMC ratios-dependent compressive yield strength. In short, these findings provide physical insights for optimizing existing PA membranes and designing next-generation desalination membranes at the molecular level. © 2022, The Authors. All rights reserved.

关键词： Molecular dynamics

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Advanced glycation end-product crosslinking activates a type VI secretion system phospholipase effector protein

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Nature Communications 2024年第1期15卷 8804页

作者： Jensen, Steven J. Cuthbert, Bonnie J. Garza-Sánchez, Fernando Helou, Colette C. de Miranda, Rodger Goulding, Celia W. Hayes, Christopher S. Department of Molecular Cellular and Developmental Biology University of California Santa Barbara Santa Barbara 93106 United States Department of Molecular Biology & amp Biochemistry University of California Irvine Irvine 92697 United States Department of Pharmaceutical Sciences University of California Irvine Irvine 92697 United States Biomolecular Science and Engineering Program University of California Santa Barbara Santa Barbara 93106 United States

Advanced glycation end-products (AGE) are a pervasive form of protein damage implicated in the pathogenesis of neurodegenerative disease, atherosclerosis and diabetes mellitus. Glycation is typically mediated by reactive dicarbonyl compounds that accumulate in all cells as toxic byproducts of glucose metabolism. Here, we show that AGE crosslinking is harnessed to activate an antibacterial phospholipase effector protein deployed by the type VI secretion system of Enterobacter cloacae. Endogenous methylglyoxal reacts with a specific arginine-lysine pair to tether the N- and C-terminal α-helices of the phospholipase domain. Substitutions at these positions abrogate both crosslinking and toxic phospholipase activity, but in vitro enzyme function can be restored with an engineered disulfide that covalently links the N- and C-termini. Thus, AGE crosslinking serves as a bona fide post-translation modification to stabilize phospholipase structure. Given the ubiquity of methylglyoxal in prokaryotic and eukaryotic cells, these findings suggest that glycation may be exploited more generally to stabilize other proteins. This alternative strategy to fortify tertiary structure could be particularly advantageous in the cytoplasm, where redox potentials preclude disulfide bond formation. © The Author(s) 2024.

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Mammalian Fuel Cells Produce Clean Energy

SSRN

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SSRN 2023年

作者： Shlosberg, Yaniv Faynus, Mohamed A. Huang, Ailun Carlini, Andrea Sylvia Clegg, Dennis O. Kaner, Richard B. Department of Chemistry and Biochemistry University of California at Santa Barbara Santa BarbaraCA93106 United States Center for Polymers and Organic Solids University of California at Santa Barbara Santa BarbaraCA93106 United States Center for Stem Cell Biology and Engineering Neuroscience Research Institute University of California Santa Barbara Santa BarbaraCA United States Program for Biomolecular Science and Engineering University of California Santa BarbaraCA93106 United States Department of Chemistry and Biochemistry Department of Materials Science and Engineering California Nano Systems Institute University of California Los AngelesCA United States

The increasing concern about climate change has led scientists around the world to develop clean energy technologies that may replace the traditional use of fossil fuels. A promising approach is the utilization of unicellular organisms as electron donors in bio-fuel cells. To date, this method has been limited to microorganisms such as bacteria, yeast, and microalgae. In this work, we show for the first time the concept of using mammalian cell cultures and organoids as electron donors in biofuel cells. We apply cyclic voltammetry to show that upon association of ARPE19 cells with the anode, they release reducing molecules to produce electricity. Furthermore, we apply 2D-fluorescence measurements and show that upon illumination, photosensitive stem cell derived retinal organoids that consists of rod photoreceptors and interneurons, secrete NADH and NADPH molecules that can donate electrons at the anode to produce photocurrent. © 2023, The Authors. All rights reserved.

关键词： Supercapacitor

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Publisher's Note: "Physically interpretable performance metrics for clustering" [J. Chem. Phys. 161, 244106 (2024)]

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The Journal of chemical physics 2025年第6期162卷 069902页

作者： Kinjal Mondal Jeffery B Klauda Institute for Physical Science and Technology Biophysics Program University of Maryland College Park Maryland 20742 USA. Department of Chemical and Biomolecular Engineering University of Maryland College Park Maryland 20742 USA.

This article was originally published online on 26 December 2024 with errors on page 12 and Refs. 23 and 24. On page 12, last paragraph in the left column, the

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