Nanoengineering cellulose for the selective removal of neodymium: Towards sustainable rare earth element recovery

Wamea, Patricia; Pitcher, Mica L.; Muthami, Joy; Sheikhi, Amir

doi:10.1016/j.cej.2021.131086

Cited by 19 publications

(19 citation statements)

References 66 publications

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“…This is likely a result of DAP charge screening by Na + via decreasing the electrical double layer thickness without compromising the surface charge of DAP. A similar trend has been reported for the Na + effect on the cation removal capacity of carboxylated adsorbents …”

Section: Resultssupporting

confidence: 86%

“…A similar trend has been reported for the Na + effect on the cation removal capacity of carboxylated adsorbents. 36,37 Figure 5d shows the IXB-mediated DAP removal percentage and capacity at varying Ca 2+ concentrations. The DAP removal capacity decreased more than 50% when the Ca 2+ concentration increased from 0 to 500 mM, possibly because the , respectively.…”

Section: Effects Of Ph and Ionic Strength On Ixb−dap Interactionsmentioning

confidence: 99%

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Ion Exchange Biomaterials to Capture Daptomycin and Prevent Resistance Evolution in Off-Target Bacterial Populations

Yeh

Narasimhalu

Steeg

et al. 2022

ACS Appl. Mater. Interfaces

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Daptomycin (DAP), a cyclic anionic lipopeptide antibiotic, is among the last resorts to treat multidrug-resistant Gram-positive bacterial infections, caused by vancomycin-resistant Enterococcus faecium or methicillin-resistant Staphylococcus aureus. DAP is administered intravenously, and via biliary excretion, ∼5–10% of the intravenous DAP dose arrives in the gastrointestinal (GI) tract where it drives resistance evolution in the off-target populations of E. faecium bacteria. Previously, we have shown in vivo that the oral administration of cholestyramine, an ion exchange biomaterial (IXB) sorbent, prevents DAP treatment from enriching DAP resistance in the populations of E. faecium shed from mice. Here, we investigate the biomaterial–DAP interfacial interactions to uncover the antibiotic removal mechanisms. The IXB-mediated DAP capture from aqueous media was measured in controlled pH/electrolyte solutions and in the simulated intestinal fluid (SIF) to uncover the molecular and colloidal mechanisms of DAP removal from the GI tract. Our findings show that the IXB electrostatically adsorbs the anionic antibiotic via a time-dependent diffusion-controlled process. Unsteady-state diffusion-adsorption mass balance describes the dynamics of adsorption well, and the maximum removal capacity is beyond the electric charge stoichiometric ratio because of DAP self-assembly. This study may open new opportunities for optimizing cholestyramine adjuvant therapy to prevent DAP resistance, as well as designing novel biomaterials to remove off-target antibiotics from the GI tract.

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Section: Resultssupporting

confidence: 86%

Section: Effects Of Ph and Ionic Strength On Ixb−dap Interactionsmentioning

confidence: 99%

Ion Exchange Biomaterials to Capture Daptomycin and Prevent Resistance Evolution in Off-Target Bacterial Populations

Yeh

Narasimhalu

Steeg

et al. 2022

ACS Appl. Mater. Interfaces

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“…The pK a of sulfate half-ester groups on CNC is 1.9; therefore, about 71.5% of them are protonated at pH = 1.5. The pK a1 and pK a2 of carboxylate groups on AHCNC are approximately 4.9 and 7.9, respectively, corresponding to the two distinct carboxylates on the C2 and C3 of cellulose. Therefore, more than 99.9% of them are protonated at pH = 1.5.…”

Section: Resultsmentioning

confidence: 97%

Nanoengineering the Redispersibility of Cellulose Nanocrystals

2022

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Enhancing the redispersibility of dried colloidal particles to yield stable dispersions after rehydration is a persistent challenge in the sustainable processing of nanocelluloses due to hydrogen bonding-induced irreversible aggregation. Programming nanocelluloses, such as cellulose nanocrystals (CNC), with moieties that enable colloidal repulsion after rehydration may address this challenge and contribute to the United Nation (UN)'s sustainable development goals (SDGs) of urban development and sustainable living (SDGs 9 and 11) and cradle-to-cradle processing (SDG 12). We hypothesize that imparting electrosteric repulsion to CNC via polyanionic disordered cellulose chains (hairs) protruding from each end may render the dried nanocrystals highly redispersible in aqueous media. Anionic hairy CNC (AHCNC), that is, CNC decorated with dicarboxylated cellulose (DCC) chains, were synthesized by the preferential, successive periodate/chlorite oxidation of the disordered regions of cellulose fibrils, bearing >5 mmol of carboxylate groups per gram. The colloidal properties of AHCNC were compared with those of sulfate half-ester groupfunctionalized CNC and TEMPO-oxidized CNC (TOCNC) after redispersion in aqueous media, followed by comparing the redispersibility of AHCNC and CNC in aqueous solutions containing monovalent or divalent cations and at varying pH. The AHCNC had remarkable aqueous redispersibility even at high ionic strengths and extreme pH. The unique redispersibility mechanism of dried AHCNC relies on the synergistic steric and electrostatic repulsion forces, recuperated upon the rehydration of DCC. This work may open new opportunities for more sustainable and cost-effective handling and processing of nanocelluloses.

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“…This is likely a result of the DAP charge screening by Na + via decreasing the electrical double layer thickness without comprimsing the surface charge of DAP. 36…”

Section: Resultsmentioning

confidence: 99%

Ion exchange biomaterials to capture daptomycin and prevent resistance evolution in off-target bacterial populations

Yeh

Narasimhalu

Steeg

et al. 2022

Preprint

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Daptomycin (DAP), a cyclic anionic lipopeptide antibiotic, is among the last resorts to treat multidrug resistant (vancomycin resistant Enterococcus faecium or methicillin resistant Staphylococcus aureus) Gram-positive bacterial infections. DAP is administered intravenously and biliary excretion results in the introduction of DAP (~5-10 % of the intravenous DAP dose) arriving in the gastrointestinal (GI) tract where it drives resistance evolution in off-target populations of Enterococcus faecium bacteria. Previously, we have shown that the oral administration of cholestyramine, an ion exchange biomaterial (IXB) sorbent, prevents DAP treatment from enriching DAP-resistance in populations of E. faecium shed from mice. Here, we engineer the biomaterial-DAP interfacial interactions to uncover the antibiotic removal mechanisms. The IXB-mediated DAP capture from aqueous media was measured in both controlled pH/electrolyte solutions and in simulated intestinal fluid (SIF) to uncover the molecular and colloidal mechanisms of DAP removal from the GI tract. Our findings show that the IXB electrostatically adsorbs the anionic antibiotic via a time-dependent diffusion-controlled process. Unsteady-state diffusion-adsorption mass balance describes the dynamics of adsorption well, and the maximum removal capacity is beyond the electric charge stoichiometric ratio because of DAP self-assembly. This study may open new opportunities for optimizing cholestyramine adjuvant therapy to prevent DAP resistance, as well as designing novel biomaterials to remove off-target antibiotics from the GI tract.

show abstract

Nanoengineering cellulose for the selective removal of neodymium: Towards sustainable rare earth element recovery

Cited by 19 publications

References 66 publications

Ion Exchange Biomaterials to Capture Daptomycin and Prevent Resistance Evolution in Off-Target Bacterial Populations

Ion Exchange Biomaterials to Capture Daptomycin and Prevent Resistance Evolution in Off-Target Bacterial Populations

Nanoengineering the Redispersibility of Cellulose Nanocrystals

Ion exchange biomaterials to capture daptomycin and prevent resistance evolution in off-target bacterial populations

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