Browsing by Author "Zetterholm, Sarah Grace"

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    Adsorption of aqueous insensitive munitions compounds by graphene nanoplatelets
    (Elsevier, 2024) Gurtowski, Luke A.; McLeod, Sheila J.; Zetterholm, Sarah Grace; Allison, Cleveland D.; Griggs, Chris S.; Gramm, Josh; Wyss, Kevin; Tour, James M.; Sanchez, Florence; Rice Advanced Materials Institute; Smalley-Curl Institute
    Mitigation strategies for potential environmental impacts of insensitive munition (IM) compounds, including 2,4-dinitroanisole (DNAN), 3-nitro-1,2,4-triazol-5-one (NTO), nitroguanidine (NQ), and methylnitroguanidine, (MeNQ) are being considered to enhance sustainability of current or potential IM formulations. Graphene nanoplatelets (GnPs) were investigated for adsorptive removal of each compound. GnPs were characterized to determine surface areas, along with particle size and zeta potential at different pH and ionic strength conditions. Adsorption kinetics and isotherm studies were conducted, comparing results against granular activated carbon (GAC). Ionic strength, pH, and temperature were adjusted to inform impacts on adsorptive behaviors and performance. The results indicated that GnPs adsorbed IM compounds more rapidly than GAC. Additionally, GnPs removed DNAN with greater capacity compared to GAC, likely due to π-π interactions. GnPs removed other compounds via van der Waals forces, while GAC exhibited greater adsorption capacities due to higher surface area. Although negative charges associated with GnPs and dissociated NTO species hindered adsorption, pH and ionic strength did not impact other compounds. Moreover, this study reports the first environmental treatment technique for MeNQ. Overall, these findings suggest that GnPs are a promising treatment technology for IM-laden waters, particularly those with compounds like DNAN where specific interactions enhance removal efficiency.
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    Graphene as a rational interface for enhanced adsorption of microcystin-LR from water
    (Elsevier, 2023) Roberts, Jesse L.; Zetterholm, Sarah Grace; Gurtowski, Luke; Fernando, PU Ashvin I.; Evans, Angela; Puhnaty, Justin; Wyss, Kevin M.; Tour, James M.; Fernando, Brianna; Jenness, Glen; Thompson, Audie; Griggs, Chris; Rice Advanced Materials Institute; Welch Institute for Advanced Materials; Smalley-Curl Institute
    Cyanotoxins such as microcystin-LR (MC-LR) represent a global environmental threat to ecosystems and drinking water supplies. The study investigated the direct use of graphene as a rational interface for removal of MC-LR via interactions with the aromatic ring of the ADDA1 chain of MC-LR and the sp2 hybridized carbon network of graphene. Intra-particle diffusion model fit indicated the high mesoporosity of graphene provided significant enhancements to both adsorption capacities and kinetics when benchmarked against microporous granular activated carbon (GAC). Graphene showed superior MC-LR adsorption capacity of 75.4 mg/g (Freundlich model) compared to 0.982 mg/g (Langmuir model) for GAC. Sorption kinetic studies showed graphene adsorbs 99% of MC-LR in 30 min, compared to zero removal for GAC after 24 hr using the same MC-LR concentration. Density functional theory (DFT), calculations showed that postulated π-based interactions align well with the NMR-based experimental work used to probe primary interactions between graphene and MC-LR adduct. This study proved that π-interactions between the aromatic ring on MC-LR and graphene sp2 orbitals are a dominant interaction. With rapid kinetics and adsorption capacities much higher than GAC, it is anticipated that graphene will offer a novel molecular approach for removal of toxins and emerging contaminants with aromatic systems.