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arXiv 2021年

作者： Han, Insung Wang, Kelly L. Cadotte, Andrew T. Xi, Zhucong Parsamehr, Hadi Xiao, Xianghui Glotzer, Sharon C. Shahani, Ashwin J. Department of Materials Science and Engineering University of Michigan Ann ArborMI48109 United States Macromolecular Science and Engineering Program University of Michigan Ann ArborMI48109 United States University of Michigan Ann ArborMI48109 United States National Synchrotron Light Source-II Brookhaven National Laboratory UptonNY11973 United States Department of Chemical Engineering University of Michigan Ann ArborMI48109 United States Biointerfaces Institute University of Michigan Ann ArborMI48109 United States

Quasicrystals exhibit long-range order but lack translational symmetry. When grown as single crystals, they possess distinctive and unusual properties owing to the absence of grain boundaries. Unfortunately, conventional methods such as bulk crystal growth or thin film deposition only allow us to synthesize either polycrystalline quasicrystals or quasicrystals that are at most a few centimeters in size. Here, we reveal through real-time and 3D imaging the formation of a single decagonal quasicrystal arising from a hard collision between multiple growing quasicrystals in an Al-Co-Ni liquid. Through corresponding molecular dynamics simulations, we examine the underlying kinetics of quasicrystal coalescence and investigate the effects of initial misorientation between the growing quasicrystalline grains on the formation of grain boundaries. At small misorientation, coalescence occurs following rigid rotation that is facilitated by phasons. Our joint experimental-computational discovery paves the way toward fabrication of single, large-scale quasicrystals for novel applications. Copyright © 2021, The Authors. All rights reserved.

关键词： Quasicrystals

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Bacteria-based bioactive materials for tumor immunotherapy

Precision Medicine and Engineering

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Precision Medicine and Engineering 2024年第2期1卷

作者： Yongcan Li Fangfang Cao Lie Ma Lulu Jin MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 PR China Departments of Diagnostic Radiology Surgery Chemical and Biomolecular Engineering and Biomedical Engineering Yong Loo Lin School of Medicine and College of Design and Engineering National University of Singapore 119074 Singapore Nanomedicine Translational Research Program NUS Center for Nanomedicine Yong Loo Lin School of Medicine National University of Singapore 117597 Singapore

As one of the most abundant biological populations endowed with unique properties such as specific targeting and genetic engineering vectors, bacteria with immunogenic potential have garnered significant attention for their ability to elicit immune activation against tumors. This approach has achieved substantial breakthroughs as a modality for cancer treatment and is known as bacterial immunotherapy. However, the immunosuppressive tumor microenvironment (TME) can inhibit the immune response induced by bacteria and promote tumor growth and metastasis. To overcome this challenge, recent advancements in bacteria-based bioactive materials, which are biological substances synthesized by bacteria, have not only harnessed the inherent properties of bacteria but also specifically targeted the modulation of the TME, providing a more favorable environment for immune activation and significantly enhancing the efficacy of immunotherapy for cancer treatment. This review introduces the key mechanisms of bacteria-based biomaterials as anticancer agents and reviews the latest research progress, along with their clinical applications in cancer treatment. Finally, the potential and challenges of bacteria-based biomaterials for tumor therapy are explored, aiming to provide insights into the functions of bacteria-based bioactive materials and their role in advancing cancer immunotherapy while offering recommendations for the development of new bacteria-based biomaterials.

关键词： Tumor immunotherapy Immune cells Tumor microenvironment Bioactive materials

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On sparse identification of complex dynamical systems: a study on discovering influential reactions in chemical reaction networks

arXiv

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arXiv 2020年

作者： Harirchi, Farshad Kim, Doohyun Khalil, Omar Liu, Sijia Elvati, Paolo Baranwal, Mayank Hero, Alfred Violi, Angela Department of Electrical Engineering and Computer Science University of Michigan Ann ArborMI48109–2125 United States Department of Mechanical Engineering University of Michigan Ann ArborMI48109–2125 United States Departments of Chemical Engineering Biomedical Engineering Macromolecular Science and Engineering Biophysics Program University of Michigan Ann ArborMI48109–2125 United States

A wide variety of real life complex networks are prohibitively large for modeling, analysis and control. Understanding the structure and dynamics of such networks entails creating a smaller representative network that preserves its relevant topological and dynamical properties. While modern machine learning methods have enabled identification of governing laws for complex dynamical systems, their inability to produce white-box models with sufficient physical interpretation renders such methods undesirable to domain experts. In this paper, we introduce a hybrid black-box, white-box approach for the sparse identification of the governing laws for complex, highly coupled dynamical systems with particular emphasis on finding the influential reactions in chemical reaction networks for combustion applications, using a data-driven sparse-learning technique. The proposed approach identifies a set of influential reactions using species concentrations and reaction rates, with minimal computational cost without requiring additional data or simulations. The new approach is applied to analyze the combustion chemistry of H2 and C3H8 in a constant-volume homogeneous reactor. The influential reactions determined by the sparse-learning method are consistent with the current kinetics knowledge of chemical mechanisms. Additionally, we show that a reduced version of the parent mechanism can be generated as a combination of the significantly reduced influential reactions identified at different times and conditions and that for both H2 and C3H8 fuel, the reduced mechanisms perform closely to the parent mechanisms as a function of the ignition delay time over a wide range of conditions. Our results demonstrate the potential of the sparse-learning approach as an effective and efficient tool for dynamical system analysis and reduction. The uniqueness of this approach as applied to combustion systems lies in the ability to identify influential reactions in specified conditions and times dur

关键词： Learning systems

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Hybrid Vesicles Enable Mechano-Responsive Hydrogel Degradation

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Angewandte Chemie 2023年第41期135卷

作者： Sung-Won Hwang Chung-Man Lim Prof. Cong Truc Huynh Hossein Moghimianavval Prof. Nicholas A. Kotov Prof. Eben Alsberg Prof. Allen P. Liu Department of Chemical Engineering University of Michigan Ann Arbor MI 48109 USA Department of Materials Science and Engineering University of Michigan Ann Arbor MI 48109 USA Department of Biomedical Engineering University of Illinois Chicago Chicago IL 60612 USA Department of Mechanical Engineering University of Michigan Ann Arbor MI 48109 USA Departments of Biomedical Engineering Macromolecular Science and Engineering Biointerfaces Institute University of Michigan Ann Arbor MI 48109 USA Departments of Orthopedic Surgery Pharmacology and Regenerative Medicine and Mechanical and Industrial Engineering University of Illinois Chicago Chicago IL 60612 USA Departments of Biomedical Engineering Biophysics Cellular and Molecular Biology Program Applied Physics Program University of Michigan Ann Arbor MI 48109 USA

Stimuli-responsive hydrogels are intriguing biomimetic materials. Previous efforts to develop mechano-responsive hydrogels have mostly relied on chemical modifications of the hydrogel structures. Here, we present a simple, generalizable strategy that confers mechano-responsive behavior on hydrogels. Our approach involves embedding hybrid vesicles, composed of phospholipids and amphiphilic block copolymers, within the hydrogel matrix to act as signal transducers. Under mechanical stress, these vesicles undergo deformation and rupture, releasing encapsulated compounds that can control the hydrogel network. To demonstrate this concept, we embedded vesicles containing ethylene glycol tetraacetic acid (EGTA), a calcium chelator, into a calcium-crosslinked alginate hydrogel. When compressed, the released EGTA sequesters calcium ions and degrades the hydrogel. This study provides a novel method for engineering mechano-responsive hydrogels that may be useful in various biomedical applications.

关键词： Block Copolymers Functional Material Stimuli-Responsive Hydrogel Stress-Induced Degradation Vesicles

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Computational Identification and Experimental Demonstration of High-Performance Methane Sorbents

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Angewandte Chemie 2022年第25期134卷

作者： Dr. Karabi Nath Dr. Alauddin Ahmed Prof. Dr. Donald J. Siegel Prof. Dr. Adam J. Matzger Department of Chemistry and Macromolecular Science and Engineering Program University of Michigan 930 North University Avenue Ann Arbor MI 48109 USA Mechanical Engineering Department University of Michigan Ann Arbor MI 48109 USA Materials Science and Engineering Applied Physics Program and University of Michigan Energy Institute University of Michigan Ann Arbor MI 48109 USA Current address: Walker Department of Mechanical Engineering Texas Materials Institute and Oden Institute for Computational Engineering and Sciences University of Texas at Austin 204 E. Dean Keeton Street ETC II 5.160 Austin TX 78712-1591 USA

Remarkable methane uptake is demonstrated experimentally in three metal-organic frameworks (MOFs) identified by computational screening: UTSA-76, UMCM-152 and DUT-23-Cu. These MOFs outperform the benchmark sorbent, HKUST-1, both volumetrically and gravimetrically, under a pressure swing of 80 to 5 bar at 298 K. Although high uptake at elevated pressure is critical for achieving this performance, a low density of high-affinity sites (coordinatively unsaturated metal centers) also contributes to a more complete release of stored gas at low pressure. The identification of these MOFs facilitates the efficient storage of natural gas via adsorption and provides further evidence of the utility of computational screening in identifying overlooked sorbents.

关键词： Computational Screening Deliverable Capacity Interatomic Potentials Metal Organic Framework (MOF) Methane Storage

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Terahertz time-domain polarimetry for generalized anistropic and chiral materials 12

Terahertz time-domain polarimetry for generalized anistropic...

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Terahertz, RF, Millimeter, and Submillimeter-Wave Technology and Applications XII 2019

作者： Cheng, Gong Choi, Won Jin Jang, Hee-Jeong Kotov, Nicholas A. Norris, Theodore B. Department of Physics University of Michigan Ann ArborMI48109 United States Center for Ultrafast Optical Science University of Michigan Ann ArborMI48109 United States Department of Materials Science and Engineering University of Michigan Ann ArborMI48109 United States Department of Chemical Engineering University of Michigan Ann ArborMI48109 United States Biointerfaces Institute University of Michigan Ann ArborMI48109 United States Program in Macromolecular Science and Engineering University of MI Ann ArborMI48109 United States Department of Electrical Engineering and Computer Science University of Michigan Ann ArborMI48109 United States

ISBN: (纸本)9781510624764

We have developed two terahertz (THz) polarimetric methodologies based on terahertz time-domain spectroscopy (THz-TDS) incorporating three wire-grid polarizers. They require no change to existing THz-TDS setups and are free of any complicated electronic controls and synchronizations. In addition to the standard quantities measured by THz-TDS such as transmission and optical constants, they provide complete information on the anisotropy and chirality for a generalized material through measurements of the full electric field vector and hence the Jones matrix, and calculating specific quantities. Thus terahertz time-domain polarimetry (THz-TDP) can be considered as an upgrade of the conventional THz-TDS, needed for full characterization of anisotropic and chiral materials. In this paper, we describe the details of the experimental settings, mathematical procedures and property quantifications in these methodologies. We present experimental results on an anisotropic polymer sheet showing the effectiveness of the methods, and preliminary data for chiral DNA molecules for the first time in the THz frequency range. © 2019 SPIE.

关键词： Polarimeters

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Chiral Phonons in Biocrystals

Research Square

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Research Square 2021年

作者： Choi, Won Jin Yano, Keiichi Cha, Minjeong Colombari, Felippe M. Wang, Yichun Lee, Sang Hyun Kruger, John M. de Moura, André F. Kotov, Nicholas A. Department of Materials Science and Engineering University of Michigan Ann ArborMI48109 United States Biointerfaces Institute University of Michigan Ann ArborMI48109 United States Department of Chemical Engineering University of Michigan Ann ArborMI48109 United States SP Campinas13.083-100 Brazil Department of Biomedical Engineering University of Michigan Ann ArborMI48109 United States Department of Chemical and Biochemical Engineering University of Notre Dame South BendIN46556 United States Department of Electrical Engineering and Computer Science University of Michigan Ann ArborMI48109 United States Department of Small Animal Clinical Sciences Michigan State University East LansingMI48824 United States Department of Chemistry Federal University of São Carlos SP São Carlos13565-905 Brazil Program in Macromolecular Science and Engineering University of Michigan Ann ArborMI48109 United States

Chiral phonons are concerted mirror-symmetric movements of atomic groups connected by covalent and intermolecular bonds. Finding chiral phonons in biocrystals is fundamentally and technologically important because these lattice vibrations should be highly specific to their short- and long-range organizations. Based on theoretical and experimental data they might be expected but not identified or utilized. Here we show that terahertz chiroptical spectroscopy enables registration and attribution of chiral phonons in microcrystals of numerous amino acids and dipeptides. Theoretical analysis and computer simulations confirm that sharp mirror-symmetric bands observed for left and right enantiomers originate from collective vibrations of biomolecules interconnected by hydrogen bonds into helical chains. Structure-property relationships for strong phonons with rotatory components in biocrystals were also identified. Bladder stones and health supplements display strong spectral signatures of chiral phonons indicating their immediate importance for biomedicine. © 2021, CC BY.

关键词： Phonons

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Superior Metal-Organic Framework Activation with Dimethyl Ether

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Angewandte Chemie 2022年第52期134卷

作者： Keenan R. Wright Dr. Karabi Nath Prof. Dr. Adam J. Matzger Department of Chemistry Institution University of Michigan 930 North University Avenue Ann Arbor MI 48109-1055 USA Contribution: Conceptualization (lead) Data curation (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Methodology (supporting) Writing - review & editing (supporting) Department of Chemistry and Macromolecular Science and Engineering Program University of Michigan 930 North University Avenue Ann Arbor MI 48109-1055 USA

Metal–organic frameworks (MOFs) are demonstrated to be readily activated by treatment with the low surface tension, low boiling point solvent dimethyl ether (DME). The mildness of the method enables access to high surface areas by avoiding structural changes in the framework that often plague thermal activation methods. A distinction from previous methods is that DME activation succeeds for materials with coordinatively unsaturated sites (CUS) and non-CUS MOFs as well. DME displaces solvent molecules occupying the pores of the MOF as well as those coordinated to metal centers; reducing evacuation temperature by using a coordinating, yet highly volatile guest enables low temperature activation with structural retention as demonstrated surface area measurements that match or exceed existing activation protocols.

关键词： Coordination Chemistry Metal–Organic Frameworks Microporous Materials Structural Collapse Surface Area

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Sequestered Cell-Secreted Extracellular Matrix Proteins Improve Folliculogenesis and Oocyte Maturation for Fertility Preservation

SSRN

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SSRN 2020年

作者： Tomaszewski, Claire E. DiLillo, Katarina M. Baker, Brendon M. Arnold, Kelly B. Shikanov, Ariella Department of Biomedical Engineering University of Michigan University of Michigan 1101 Beal Ave Ann ArborMI48109 United States Department of Obstetrics and Gynecology University of Michigan 1101 Beal Ave Ann ArborMI48109 United States Cellular and Molecular Biology Program University of Michigan 1101 Beal Ave Ann ArborMI48109 United States Macromolecular Science and Engineering University of Michigan 1101 Beal Ave Ann ArborMI48109 United States

Synthetic matrices offer a high degree of control and tunability for mimicking extracellular matrix functions of native tissue, allowing the study of disease and development in vitro. In this study, we functionalized degradable poly(ethylene glycol) hydrogels with extracellular matrix (ECM)-sequestering peptides aiming to recapitulate the native ECM composition for culture and maturation of ovarian follicular organoids. We hypothesized that ECM-sequestering peptides would facilitate deposition and retention of cell-secreted ECM molecules, thereby recreating cell-matrix interactions in otherwise bioinert PEG hydrogels. Specifically, heparin-binding peptide from antithrombin III (HBP), heparan sulfate binding peptide derived from laminin (AG73), basement membrane binder peptide (BMB), and heparan sulfate binding region of placental growth factor 2 (RRR) tethered to a PEG hydrogel significantly improved follicle survival, growth and maturation compared to PEG-Cys, a mechanically similar but biologically inert control. Immunohistochemical analysis of the hydrogel surrounding cultured follicles confirmed sequestration and retention of laminin, collagen I, perlecan and fibronectin in ECM-sequestering hydrogels but not in bioinert PEG-Cys hydrogels. The media from follicles cultured in PEG-AG73, PEG-BMB, and PEG-RRR also had significantly higher concentrations of factors known to regulate follicle development compared to PEG-Cys. PEG-AG73 and PEG-BMB were the most beneficial for promoting follicle maturation, likely because AG73 and BMB mimic basement membrane interactions which are crucial for follicle development. Here we have shown that functionalizing PEG with ECM-sequestering peptides allows cell-secreted ECM to be retained within the hydrogels, restoring critical cell-matrix interactions and promoting healthy organoid development in a fully synthetic culture system. © 2020, The Authors. All rights reserved.

关键词： Polyethylene glycols

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Enhanced Drug Delivery by Dissolution of Amorphous Drug Encapsulated in a Water Unstable Metal–Organic Framework (MOF)

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Angewandte Chemie 2019年第47期131卷

作者： Kuthuru Suresh Adam J. Matzger Department of Chemistry and the Macromolecular Science and Engineering Program University of Michigan 930 North University Avenue Ann Arbor MI 48109-1055 USA

Encapsulating a drug molecule into a water‐reactive metal–organic framework (MOF) leads to amorphous drug confined within the nanoscale pores. Rapid release of drug occurs upon hydrolytic decomposition of MOF in dissolution media. Application to improve dissolution and solubility for the hydrophobic small drug molecules curcumin, sulindac, and triamterene is demonstrated. The drug@MOF composites exhibit significantly enhanced dissolution and achieves high supersaturation in simulated gastric and/or phosphate buffer saline media. This combination strategy where MOF inhibits crystallization of the amorphous phase and then releases drug upon MOF irreversible structural collapse represents a novel and generalizable approach for drug delivery of poorly soluble compounds while overcoming the traditional weakness of amorphous drug delivery: physical instability of the amorphous form.

关键词： Amorphe Wirkstoffe Metall-organische Gerüste Sofortige Wirkstofffreisetzung Stabilität Wirkstofftransport

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