Article
Chemistry, Multidisciplinary
Eric N. Donders, Kai V. Slaughter, Christian Dank, Ahil N. Ganesh, Brian K. Shoichet, Mark Lautens, Molly S. Shoichet
Summary: The pK(a) of colloid-forming drugs can be manipulated to achieve endosomal disruption while avoiding phospholipidosis and minimizing toxicity, leading to the design of drug-rich nanoparticles. By synthesizing ionizable derivatives of fulvestrant analogs, which are lipid-stabilized drug colloids, the pK(a) of these ionizable colloids influenced the mechanism of endosomal and lysosomal disruption. This study establishes a tunable and generalizable strategy for endosomal disruption by manipulating the pK(a) of colloid-forming drugs.
Review
Chemistry, Multidisciplinary
Teodora Andrian, Roger Riera, Silvia Pujals, Lorenzo Albertazzi
Summary: The successful delivery of nanoparticles in cytosol is often hindered by their entrapment and degradation in endosomes. To overcome this challenge, it is crucial to accurately detect and quantify the endosomal escape process. Nanoscopy technologies have rapidly evolved in the past two decades, showcasing a diverse range of powerful techniques that can significantly impact the field of nanomedicine. This review discusses the latest insights into endosomal escape of nanoparticles obtained through nanoscopy, highlighting the potential benefits of these techniques in studying drug delivery processes.
NANOSCALE ADVANCES
(2021)
Review
Biochemistry & Molecular Biology
Shuo Huang, Rui Dai, Zhiqi Zhang, Han Zhang, Meng Zhang, Zhangjun Li, Kangrui Zhao, Wenjun Xiong, Siyu Cheng, Buhua Wang, Yi Wan
Summary: CRISPR/Cas systems are widely used in gene editing due to their accuracy, programmability, ease of use, and affordability. Additionally, they have been applied in live-cell imaging and bioanalysis, expanding the scope of their use beyond gene editing.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Article
Biochemical Research Methods
Christoffer Edlund, Timothy R. Jackson, Nabeel Khalid, Nicola Bevan, Timothy Dale, Andreas Dengel, Sheraz Ahmed, Johan Trygg, Rickard Sjoegren
Summary: The LIVECell dataset consists of annotated phase-contrast images of over 1.6 million cells, aiming to improve the training of image segmentation models through deep learning. Its creation and utilization help explore biological phenomena and conduct high-throughput quantitative imaging studies.
Review
Biochemistry & Molecular Biology
Herbert Schneckenburger
Summary: Laser plays an increasing role in live cell microscopy due to its unique properties. It is used in various techniques such as 3D microscopy, super-resolution microscopy, spectral imaging, and fluorescence lifetime imaging. Laser applications in live cell biology include fluorescence diagnosis, photodynamic therapy, and laser-assisted optoporation.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Chemistry, Multidisciplinary
Tom Baladi, Jesper R. Nilsson, Audrey Gallud, Emanuele Celauro, Cecile Gasse, Fabienne Levi-Acobas, Ivo Sarac, Marcel R. Hollenstein, Anders Dahlen, Elin K. Esbjorner, L. Marcus Wilhelmsson
Summary: The study introduces a stealth labeling strategy to efficiently generate RNA transcripts and translate them into correct proteins, providing an important tool for biological research and RNA delivery studies.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Biology
Jeremy Copperman, Sean M. Gross, Young Hwan Chang, Laura M. Heiser, Daniel M. Zuckerman
Summary: Time-lapse imaging is a powerful tool to study cell dynamics, but analyzing morphological changes over time is challenging. In this study, we use trajectory embedding to analyze cellular behavior based on multiple time points simultaneously. We apply this method to study the effects of microenvironmental perturbagens on MCF10A mammary epithelial cells. Our analysis reveals ligand-specific regulation of cell state transitions and provides descriptive models of single-cell trajectories. Incorporating trajectories improves the characterization of cell states and enables better identification of phenotypes compared to snapshot-based analysis. This approach has broad applications in live-cell imaging for studying cell responses.
COMMUNICATIONS BIOLOGY
(2023)
Article
Oncology
Dilan Khalili, Martin Kunc, Sarah Herbrich, Anna M. M. Muller, Ulrich Theopold
Summary: Chitinase-like proteins (CLPs) are associated with tissue-remodeling and inflammation, but their role in tumors is not clear. In this study, using Drosophila melanogaster and molecular genetics, the researchers found that one member of CLPs, Idgf3, is transcriptionally induced in a JNK-dependent manner via a positive feedback loop mediated by reactive oxygen species (ROS). Through disrupting cytoskeletal organization via enlarged endosomal vesicles (EnVs), Idgf3 promotes tumor progression. These findings provide new insights into the function of CLPs in tumors and identify potential targets for tumor control.
FRONTIERS IN ONCOLOGY
(2023)
Article
Chemistry, Applied
Rosita Diana, Ugo Caruso, Francesco Silvio Gentile, Luigi Di Costanzo, David Turra, Stefania Vitale, Barbara Panunzi
Summary: In this study, we designed three novel fluorescent brightening agents based on a benzodifuran skeleton, which have improved water solubility and the ability to interact with living cells. A complete understanding of the emission mechanisms was achieved through Density Functional Theory study and X-ray crystallographic analysis. The fluorescence quantum yields were measured in different solvents and at different pH values. Through fluorescence microscopy technique, two probes with different functionalized branching chains were found to be efficient stains for plant root cell wall.
Article
Optics
Zewei Luo, Ge Wu, Mengting Kong, Zhi Chen, Zhengfei Zhuang, Junchao Fan, Tongsheng Chen
Summary: Forster resonance energy transfer (FRET) microscopy is a valuable tool for studying biological systems, but super-resolution FRET imaging in living cells is challenging. In this study, we propose a SR FRET method called SIM-FRET that combines SR structured illumination microscopy (SIM) imaging and acceptor sensitized emission FRET imaging to achieve live-cell quantitative SR FRET imaging. Our method provides enhanced spatial resolution and maintains the advantages of quantitative FRET analysis. We validate the effectiveness of SIM-FRET through simulated models and live-cell samples, and demonstrate its ability to reveal the intricate structure of FRET signals.
PHOTONICS RESEARCH
(2023)
Article
Cell Biology
Joanna W. Pylvanainen, Estibaliz Gomez-de-Mariscal, Ricardo Henriques, Guillaume Jacquemet
Summary: Live imaging, particularly when combined with fluorescence microscopy, is a powerful tool for observing cellular components in real time. However, implementing live imaging and analyzing the resulting datasets is challenging due to issues such as drift, phototoxicity, and dataset size. Recent advances in bioimage analysis, including deep learning, are revolutionizing how live imaging is performed. Important computational methods for live imaging include drift correction, denoising, super-resolution imaging, artificial labeling, tracking, and time series analysis. Self-driving microscopy has also seen recent advancements.
CURRENT OPINION IN CELL BIOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Ze Huang, Aixiang Ding, Jiaxiang Yang, Chengyuan Wang, Fang Tang
Summary: Dual-state emission luminogens (DSEgens) are attracting research interest for their high emission efficiency in both solution and solid states. This study demonstrates the synthesis of bright DSEgens through tuning the molecular electronic structures and conformations. The synthesized molecules show strong dual-state emission and display reversible mechanofluorochromism, allowing for applications in rewritable information storage and live-cell imaging.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Review
Biochemistry & Molecular Biology
Yang Zhang, Yeting Zheng, Andrea Tomassini, Ambarish Kumar Singh, Francisco M. Raymo
Summary: PALM uses fluorescence photoactivation and single-molecule localization to overcome optical diffraction and achieve nanoscale spatial resolution in imaging biological samples. Synthetic modifications of the BODIPY chromophore allow for photoactivation and precise localization of single molecules. In combination with targeting ligands, photoactivatable BODIPYs can label subcellular components and enable sub-diffraction imaging of live cells using PALM, making them valuable probes for bioimaging applications.
Article
Biotechnology & Applied Microbiology
Andreas Boden, Francesca Pennacchietti, Giovanna Coceano, Martina Damenti, Michael Ratz, Ilaria Testa
Summary: A new 3D pRESOLFT microscope method with sub-80-nm resolution has been developed to visualize the volumetric architecture of organelles and molecules inside whole living cells, allowing for targeted 3D confinement of fluorescence and observation of dynamic structural alterations in cells.
NATURE BIOTECHNOLOGY
(2021)
Review
Optics
Herbert Schneckenburger, Verena Richter
Summary: This short overview discusses 3D live cell imaging, relevant samples, challenges like optical sectioning and phototoxicity, and enhanced microscopy methods with some examples and applications. Future advancements may involve increasing microscopic resolution and utilizing molecular sensing techniques.
Article
Chemistry, Physical
Yierpan Aierken, Ankit Agrawal, Meiling Sun, Marko Melander, Ethan J. Crumlin, Brett A. Helms, David Prendergast
Summary: This paper proposes a method of applying charge constraints to study the charge transfer mechanisms in electrochemical systems, particularly beneficial for conversion electrodes, effectively separating electronic and nuclear degrees of freedom. Through studying sulfur cathodes and Li-S cells, the necessity of restricting electronic degrees of freedom is demonstrated. This approach will be vital for understanding dynamics at electrified interfaces, whether deliberately created or spontaneously occurring.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Multidisciplinary Sciences
Nemi Vora, Peter R. Christensen, Jeremy Demarteau, Nawa Raj Baral, Jay D. Keasling, Brett A. Helms, Corinne D. Scown
Summary: Mechanical recycling of polymers downgrades their usability, while chemical recycling offers a more sustainable way to recover chemical feedstocks. The cost and carbon footprint of chemically recycled PDKs are significantly lower than producing virgin resin, providing a strong incentive for recovering and recycling future polymer waste.
Review
Multidisciplinary Sciences
LaShanda T. J. Korley, Thomas H. Epps, Brett A. Helms, Anthony J. Ryan
Summary: Chemical recycling and polymer upcycling offer solutions to the challenges of plastic waste heterogeneity and property reductions, enabling circularity and reducing energy consumption and environmental impacts. The industrial adoption of these approaches is encouraging and plays a critical role in addressing the fate of plastics and advancing next-generation materials design.
Article
Nanoscience & Nanotechnology
Eric Schreiber, Rachel E. Garwick, Miranda J. Baran, Michael A. Baird, Brett A. Helms, Ellen M. Matson
Summary: This study investigates the size-dependent crossover behavior of redox-active vanadium compounds and polyoxovanadate-alkoxide clusters in separators derived from polymers of intrinsic microporosity (PIMs) in nonaqueous electrolyte. The results show that increasing the size of the vanadium species and restricting the pore swelling of PIMs can effectively block active species crossover and improve the efficiency of the battery.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Ganhua Xie, Pei Li, Paul Y. Kim, Pei-Yang Gu, Brett A. Helms, Paul D. Ashby, Lei Jiang, Thomas P. Russell
Summary: Water-walking insects use capillary forces to climb or descend the meniscus between water surface and a solid object by changing body posture, which inspired the development of autonomous aquatic synthetic systems that can shuttle cargo underground between landing and drop-off sites. By controlling the contact angle of a coacervate sac or hydrogel droplet, cyclic cargo shuttling can occur continuously as long as reactants from the surrounding aqueous phase are not depleted, potentially leading to applications in autonomously driven reaction or delivery systems and micro-/milli-robotics.
Article
Chemistry, Multidisciplinary
Jeremy Demarteau, Nemi Vora, Jay D. Keasling, Brett A. Helms, Corinne D. Scown
Summary: The efficiency of monomer recovery in the chemical recycling of plastic waste has been a major consideration for sustainability. However, this study also highlights the costs, energy consumption, and carbon emissions associated with resin production. By applying systems analysis, a less intensive process for the production of polydiketoenamine (PDK) resins is proposed, resulting in cost reduction and lower greenhouse gas emissions. The study emphasizes the importance of targeted collection and sorting for achieving practical savings.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Jiajun Yan, Michael A. Baird, Derek C. Popple, Alex Zettl, Thomas P. Russell, Brett A. Helms
Summary: This study demonstrates the development of rechargeable structured-liquid batteries by compartmentalizing redox-active molecules in multiphasic liquid devices. These batteries can be integrated with soft electronics and have potential applications in smart textiles, medical implants, and wearables.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Multidisciplinary
Brett A. Helms
Summary: Mismanagement of plastic waste leads to the leakage of microplastics into the environment, causing harm to ecosystems and health. Circular plastic recycling is an important method to address the waste problem and promote sustainability.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Article
Chemistry, Physical
Michael A. Baird, Junhua Song, Ran Tao, Youngmin Ko, Brett A. Helms
Summary: This study explores locally superconcentrated electrolytes that reduce viscosity for fast-charging and extended battery life. The research identifies divergent failure mechanisms at different charge rates and depths of discharge, which has implications for future electrolyte designs.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Allison M. Green, Sanket Kadulkar, Zachary M. Sherman, Thomas M. Fitzsimons, Charles K. Ofosu, Jiajun Yan, David Zhao, Jan Ilavsky, Adrianne M. Rosales, Brett A. Helms, Venkat Ganesan, Thomas M. Truskett, Delia J. Milliron
Summary: This study investigates how wrapping colloidal tin-doped indium oxide nanocrystals with polymers affects their depletion induced interactions and assembly. The results show that the molecular weight of the depletant, as well as the surface density and molecular weight of the polymer grafts, play a crucial role in determining assembly thresholds. These findings are unique to depletion-driven assembly at the nanoscale and mirror the phase behavior of grafted nanoparticle-polymer composites. Optical and rheological responses of different polymer shell architectures were studied to understand how structural differences impact properties. This research discusses the potential for designing responsive depletion interactions and dynamically reconfigurable materials at the nanoscale.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Correction
Chemistry, Multidisciplinary
Alexander R. Epstein, Jeremy Demarteau, Brett A. Helms, Kristin A. Persson
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Alexander R. Epstein, Jeremy Demarteau, Brett A. Helms, Kristin A. Persson
Summary: The design of circular polymers is necessary due to the lack of efficient recycling methods for many commodity plastics. Polydiketoenamines (PDKs) stand out for their ability to undergo selective depolymerization in strong acid, allowing monomers to be recovered. The chemistry of the cross-linker, far from the reaction center, has been found to affect the depolymerization rate of PDKs, with a proximal amine in the cross-linker significantly accelerating the process.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jake X. Shi, Nicodemo R. Ciccia, Subhajit Pal, Diane D. Kim, John N. Brunn, Carlos Lizandara-Pueyo, Martin Ernst, Alexander M. Haydl, Phillip B. Messersmith, Brett A. Helms, John F. Hartwig
Summary: In this study, strategies for derivatizing oxidized polyethylene with functional groups were described. The presence of ketones and alcohols in the polyethylene were controlled through different catalytic reactions. The introduction of esters and oximes onto the polymer improved its surface and bulk properties. The functionalized polymers were separated from plastic blends through selective dissolution, demonstrating the potential for novel approaches in polymer separation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Wenhao Zhang, Ryan Walser-Kuntz, Jacob S. Tracy, Tim K. Schramm, James Shee, Martin Head-Gordon, Gan Chen, Brett A. Helms, Melanie S. Sanford, F. Dean Toste
Summary: Redox flow batteries (RFBs) are a promising technology for energy storage. This study introduces a new organic scaffold, indolo[2,3-b]quinoxaline, as a stable and high-performance anolyte for nonaqueous RFBs. When paired with MEEPT, it achieves a 2.3 V all-organic RFB.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Jiwoong Bae, Zhuoying Zhu, Jiajun Yan, Dong-Min Kim, Youngmin Ko, Anubhav Jain, Brett A. Helms
Summary: We designed supramolecular organo-ionic (ORION) electrolytes to separate the cathode and solid-electrolyte particles in solid-state batteries (SSBs) and enable the recycling of cathodes from the recovered materials. SSBs implementing ORION electrolytes showed less than 20% capacity fade after hundreds of cycles at 45 degrees C. Refurbished cells using a low-temperature solvent process recovered 90% of their initial capacity and sustained it for an additional 100 cycles with 84% capacity retention in their second life.
