| 1. |
- Khaliha, Sara, et al.
(författare)
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Defective graphene nanosheets for drinking water purification : Adsorption mechanism, performance, and recovery
- 2021
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Ingår i: FlatChem. - : Elsevier. - 2452-2627. ; 29
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Tidskriftsartikel (refereegranskat)abstract
- Defect-rich graphene oxide (dGO) was used as sorbent for organic contaminants of emerging concern in tap water, including drugs and dyes, and the performance compared to those of lower-defects graphene types. The role of holes and carbonyl- carboxylic groups on graphene nanosheets surface on the adsorption mechanism and efficiency was investigated. dGO showed enhanced adsorption capacity toward two fluoroquinolone antibiotics (ofloxacin, OFLOX, and ciprofloxacin, CIPRO) in tap water with a maximum capacity of 650 mg/g, compared to 204 mg/g for Hummers derived commercial GO (hGO) and 125 mg/g for less defected Brodie derived GO (bGO) for OFLOX. The role of defects on the selective adsorption of OFLOX was also modelled by MD simulations, highlighting a mechanism mainly driven by the shape complementarity between the graphene holes and the molecules. Adsorption isotherms revealed different adsorption model for dGO, with a Langmuir fitting for dGO and BET fitting for all the other investigated samples. The maximum adsorption capacity of dGO for OFLOX was about six times higher than that of Granular Activated Carbon (95 mg/g), the industrial adsorption standard technology. Finally, it was also demonstrated that dGO can be recovered from treated water by ultrafiltration, this preventing secondary contamination risks and enabling safe use of graphene nanosheets for water purification.
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| 2. |
- Kovtun, Alessandro, et al.
(författare)
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Core-shell graphene oxide-polymer hollow fibers as water filters with enhanced performance and selectivity
- 2021
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Ingår i: Faraday Discussions. - : Royal Society of Chemistry (RSC). - 1359-6640 .- 1364-5498. ; 227, s. 274-290
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Tidskriftsartikel (refereegranskat)abstract
- Commercial hollow fiber filters for micro- and ultrafiltration are based on size exclusion and do not allow the removal of small molecules such as antibiotics. Here, we demonstrate that a graphene oxide (GO) layer can be firmly immobilized either inside or outside polyethersulfone-polyvinylpyrrolidone hollow fiber (Versatile PES (R), hereafter PES) modules and that the resulting core-shell fibers inherits the microfiltration ability of the pristine PES fibers and the adsorption selectivity of GO. GO nanosheets were deposited on the fiber surface by filtration of a GO suspension through a PES cartridge (cut-off 0.1-0.2 mu m), then fixed by thermal annealing at 80 degrees C, rendering the GO coating stably fixed and unsoluble. The filtration cut-off, retention selectivity and efficiency of the resulting inner and outer modified hollow fibers (HF-GO) were tested by performing filtration on water and bovine plasma spiked with bovine serum albumin (BSA, 66 kDa, approximate to 15 nm size), monodisperse polystyrene nanoparticles (52 nm and 303 nm sizes), with two quinolonic antibiotics (ciprofloxacin and ofloxacin) and rhodamine B (RhB). These tests showed that the microfiltration capability of PES was retained by HF-GO, and in addition the GO coating can capture the molecular contaminants while letting through BSA and smaller polystyrene nanoparticles. Combined XRD, molecular modelling and adsorption experiments show that the separation mechanism does not rely only on physical size exclusion, but involves intercalation of solute molecules between the GO layers.
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| 3. |
- Kovtun, Alessandro, et al.
(författare)
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Multiscale Charge Transport in van der Waals Thin Films: Reduced Graphene Oxide as a Case Study
- 2021
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Ingår i: ACS Nano. - : American Chemical Society (ACS). - 1936-086X .- 1936-0851. ; 15:2, s. 2654-2667
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Tidskriftsartikel (refereegranskat)abstract
- Large area van der Waals (vdW) thin films are assembled materials consisting of a network of randomly stacked nanosheets. The multiscale structure and the two-dimensional (2D) nature of the building block mean that interfaces naturally play a crucial role in the charge transport of such thin films. While single or few stacked nanosheets (i.e., vdW heterostructures) have been the subject of intensive works, little is known about how charges travel through multilayered, more disordered networks. Here, we report a comprehensive study of a prototypical system given by networks of randomly stacked reduced graphene oxide 2D nanosheets, whose chemical and geometrical properties can be controlled independently, permitting to explore percolated networks ranging from a single nanosheet to some billions with room-temperature resistivity spanning from 10-5 to 10-1 ω·m. We systematically observe a clear transition between two different regimes at a critical temperature T*: Efros-Shklovskii variable-range hopping (ES-VRH) below T∗ and power law behavior above. First, we demonstrate that the two regimes are strongly correlated with each other, both depending on the charge localization length ζ, calculated by the ES-VRH model, which corresponds to the characteristic size of overlapping sp2 domains belonging to different nanosheets. Thus, we propose a microscopic model describing the charge transport as a geometrical phase transition, given by the metal-insulator transition associated with the percolation of quasi-one-dimensional nanofillers with length ζ, showing that the charge transport behavior of the networks is valid for all geometries and defects of the nanosheets, ultimately suggesting a generalized description on vdW and disordered thin films.
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| 4. |
- Quintano, Vanesa, et al.
(författare)
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Long-range selective transport of anions and cations in graphene oxide membranes, causing selective crystallization on the macroscale
- 2021
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Ingår i: Nanoscale Advances. - : Royal Society of Chemistry (RSC). - 2516-0230. ; 3:2, s. 353-358
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Tidskriftsartikel (refereegranskat)abstract
- Monoatomic nanosheets can form 2-dimensional channels with tunable chemical properties, for ion storage and filtering applications. Here, we demonstrate transport of K+, Na+, and Li+ cations and F- and Cl- anions on the centimeter scale in graphene oxide membranes (GOMs), triggered by an electric bias. Besides ion transport, the GOM channels foster also the aggregation of the selected ions in salt crystals, whose composition is not the same as that of the pristine salt present in solution, highlighting the difference between the chemical environment in the 2D channels and in bulk solutions.
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