Browsing by Author "Beckham, Jacob L."

Now showing 1 - 5 of 5
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    A scientific machine learning framework to understand flash graphene synthesis
    (Royal Society of Chemistry, 2023) Sattari, Kianoosh; Eddy, Lucas; Beckham, Jacob L.; Wyss, Kevin M.; Byfield, Richard; Qian, Long; Tour, James M.; Lin, Jian; NanoCarbon Center; Welch Institute for Advanced Materials
    Flash Joule heating (FJH) is a far-from-equilibrium (FFE) processing method for converting low-value carbon-based materials to flash graphene (FG). Despite its promises in scalability and performance, attempts to explore the reaction mechanism have been limited due to the complexities involved in the FFE process. Data-driven machine learning (ML) models effectively account for the complexities, but the model training requires a considerable amount of experimental data. To tackle this challenge, we constructed a scientific ML (SML) framework trained by using both direct processing variables and indirect, physics-informed variables to predict the FG yield. The indirect variables include current-derived features (final current, maximum current, and charge density) predicted from the proxy ML models and reaction temperatures simulated from multi-physics modeling. With the combined indirect features, the final ML model achieves an average R2 score of 0.81 ± 0.05 and an average RMSE of 12.1% ± 2.0% in predicting the FG yield, which is significantly higher than the model trained without them (R2 of 0.73 ± 0.05 and an RMSE of 14.3% ± 2.0%). Feature importance analysis validates the key roles of these indirect features in determining the reaction outcome. These results illustrate the promise of this SML to elucidate FFE material synthesis outcomes, thus paving a new avenue to processing other datasets from the materials systems involving the same or different FFE processes.
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    Light-activated molecular machines are fast-acting broad-spectrum antibacterials that target the membrane
    (AAAS, 2022) Santos, Ana L.; Liu, Dongdong; Reed, Anna K.; Wyderka, Aaron M.; van Venrooy, Alexis; Li, John T.; Li, Victor D.; Misiura, Mikita; Samoylova, Olga; Beckham, Jacob L.; Ayala-Orozco, Ciceron; Kolomeisky, Anatoly B.; Alemany, Lawrence B.; Oliver, Antonio; Tegos, George P.; Tour, James M.; Smalley-Curl Institute; NanoCarbon Center; Welch Institute for Advanced Materials
    The increasing occurrence of antibiotic-resistant bacteria and the dwindling antibiotic research and development pipeline have created a pressing global health crisis. Here, we report the discovery of a distinctive antibacterial therapy that uses visible (405 nanometers) light-activated synthetic molecular machines (MMs) to kill Gram-negative and Gram-positive bacteria, including methicillin-resistant Staphylococcus aureus, in minutes, vastly outpacing conventional antibiotics. MMs also rapidly eliminate persister cells and established bacterial biofilms. The antibacterial mode of action of MMs involves physical disruption of the membrane. In addition, by permeabilizing the membrane, MMs at sublethal doses potentiate the action of conventional antibiotics. Repeated exposure to antibacterial MMs is not accompanied by resistance development. Finally, therapeutic doses of MMs mitigate mortality associated with bacterial infection in an in vivo model of burn wound infection. Visible light–activated MMs represent an unconventional antibacterial mode of action by mechanical disruption at the molecular scale, not existent in nature and to which resistance development is unlikely.
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    Oxidized Activated Charcoal Nanozymes: Synthesis, and Optimization for In Vitro and In Vivo Bioactivity for Traumatic Brain Injury
    (Wiley, 2024) McHugh, Emily A.; Liopo, Anton V.; Mendoza, Kimberly; Robertson, Claudia S.; Wu, Gang; Wang, Zhe; Chen, Weiyin; Beckham, Jacob L.; Derry, Paul J.; Kent, Thomas A.; Tour, James M.; Smalley-Curl Institute;NanoCarbon Center;Welch Institute for Advanced Materials
    Carbon-based superoxide dismutase (SOD) mimetic nanozymes have recently been employed as promising antioxidant nanotherapeutics due to their distinct properties. The structural features responsible for the efficacy of these nanomaterials as antioxidants are, however, poorly understood. Here, the process–structure–property–performance properties of coconut-derived oxidized activated charcoal (cOAC) nano-SOD mimetics are studied by analyzing how modifications to the nanomaterial's synthesis impact the size, as well as the elemental and electrochemical properties of the particles. These properties are then correlated to the in vitro antioxidant bioactivity of poly(ethylene glycol)-functionalized cOACs (PEG-cOAC). Chemical oxidative treatment methods that afford smaller, more homogeneous cOAC nanoparticles with higher levels of quinone functionalization show enhanced protection against oxidative damage in bEnd.3 murine endothelioma cells. In an in vivo rat model of mild traumatic brain injury (mTBI) and oxidative vascular injury, PEG-cOACs restore cerebral perfusion rapidly to the same extent as the former nanotube-derived PEG-hydrophilic carbon clusters (PEG-HCCs) with a single intravenous injection. These findings provide a deeper understanding of how carbon nanozyme syntheses can be tailored for improved antioxidant bioactivity, and set the stage for translation of medical applications.
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    Sustainable valorization of asphaltenes via flash joule heating
    (AAAS, 2022) Saadi, M.A.S.R.; Advincula, Paul A.; Thakur, Md Shajedul Hoque; Khater, Ali Zein; Saad, Shabab; Shayesteh Zeraati, Ali; Nabil, Shariful Kibria; Zinke, Aasha; Roy, Soumyabrata; Lou, Minghe; Bheemasetti, Sravani N.; Bari, Md Abdullah Al; Zheng, Yiwen; Beckham, Jacob L.; Gadhamshetty, Venkataramana; Vashisth, Aniruddh; Kibria, Md Golam; Tour, James M.; Ajayan, Pulickel M.; Rahman, Muhammad M.
    The refining process of petroleum crude oil generates asphaltenes, which poses complicated problems during the production of cleaner fuels. Following refining, asphaltenes are typically combusted for reuse as fuel or discarded into tailing ponds and landfills, leading to economic and environmental disruption. Here, we show that low-value asphaltenes can be converted into a high-value carbon allotrope, asphaltene-derived flash graphene (AFG), via the flash joule heating (FJH) process. After successful conversion, we develop nanocomposites by dispersing AFG into a polymer effectively, which have superior mechanical, thermal, and corrosion-resistant properties compared to the bare polymer. In addition, the life cycle and technoeconomic analysis show that the FJH process leads to reduced environmental impact compared to the traditional processing of asphaltene and lower production cost compared to other FJH precursors. Thus, our work suggests an alternative pathway to the existing asphaltene processing that directs toward a higher value stream while sequestering downstream emissions from the processing.
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    Visible-Light-Activated Molecular Machines Kill Fungi by Necrosis Following Mitochondrial Dysfunction and Calcium Overload
    (Wiley, 2023) Santos, Ana L.; Beckham, Jacob L.; Liu, Dongdong; Li, Gang; van Venrooy, Alexis; Oliver, Antonio; Tegos, George P.; Tour, James M.; Smalley-Curl Institute; NanoCarbon Center; Welch Institute for Advanced Materials
    Invasive fungal infections are a growing public health threat. As fungi become increasingly resistant to existing drugs, new antifungals are urgently needed. Here, it is reported that 405-nm-visible-light-activated synthetic molecular machines (MMs) eliminate planktonic and biofilm fungal populations more effectively than conventional antifungals without resistance development. Mechanism-of-action studies show that MMs bind to fungal mitochondrial phospholipids. Upon visible light activation, rapid unidirectional drilling of MMs at ≈3 million cycles per second (MHz) results in mitochondrial dysfunction, calcium overload, and ultimately necrosis. Besides their direct antifungal effect, MMs synergize with conventional antifungals by impairing the activity of energy-dependent efflux pumps. Finally, MMs potentiate standard antifungals both in vivo and in an ex vivo porcine model of onychomycosis, reducing the fungal burden associated with infection.