Recyclable Joule heated low shrinkage carbon nanofiber aerogels for microscale oil/water separation

doi:10.1016/j.jmst.2022.03.025

Abstract

Abstract:

Aerogels have shown great potential as oil adsorbents but their application to the removal of microscale oil from water and their recycling remains problematic. The present work proposed a freeze-shaping method for fabricating carbon nanofiber aerogels (CNFAs) based on the direct use of one-dimensional (1D) carbon nanofibers (CNF) rather than carbonization of polymer aerogels. This technique greatly reduces volume shrinkage and increases the three-dimensional (3D) structural stability of the material. Carbon nanotubes (CNT) and gelatinized starch were incorporated in these aerogels as a conductive enhancement agent and binder, respectively, forming a “vine (CNT)-wrapped tree (CNF)” structure that improved mechanical and Joule-heating performance. The effects of glutaraldehyde added to aerogels as a cross-linking agent on mechanical properties and microstructure were also systematically investigated. The optimized CNFAs combined with low density, high porosity, good elasticity, and superior Joule-heating efficiency along with suitable adsorption capacity, excellent selectivity, and cycling stability. This material was able to selectively remove 87% and 92% of microscale acetone and dimethylformamide (DMF), respectively, from the water after nine cycles of adsorption and Joule-heating. The present work demonstrates a novel means of designing and fabricating a low shrinkage CNFA with outstanding Joule-heating performance having potential practical applications in the remediation of organic pollution.

Key words: Electrospinning, Carbon nanofiber aerogel, Volume shrinkage, Joule-heating, Chemical oxygen demand

Guangkai Hu, Dong Liu, Sidi Yin, Bin Yu, Tao Huang, Hao Yu, Meifang Zhu. Recyclable Joule heated low shrinkage carbon nanofiber aerogels for microscale oil/water separation[J]. J. Mater. Sci. Technol., 2022, 127: 89-97.

Figures/Tables 6

Fig. 1. (a) Schematic illustration of the synthetic steps of CNFA and (b) corresponding optical photographs.

Fig. 2. Mechanical compression performance of the CNFA. (a) Compressive stress-strain curves for the CNFA-0, CNFA-50, CNFA-75, and CNFA-100 at a strain of 50%, (b) comparison of the specific strengths of the CNFA-0, CNFA-50, CNFA-75, and CNFA-100, (c) plastic deformation of the CNFA-0, CNFA-50, CNFA-75, and CNFA-100 after 10 cycles at 50% strain, and (d) stress-strain curves obtained from the CNFA-75 after 10 cycles at 30%, 50%, and 70% strain.

Fig. 3. SEM images of the (a1-a3) CNFA-0, (b1-b3) CNFA-50, (c1-c3) CNFA-75, and (d1-d3) CNFA-100 aerogels. (a1-d1) Surfaces perpendicular to the growth direction of ice crystals and (a2-d2) surfaces parallel to the growth direction of ice crystals. (a3-d3) are enlarged views of (a2-d2), respectively.

Fig. 4. (a) Diagram of the aerogel Joule-heating setup, (b) I-V curve obtained from the CNFA, (c) diagram of the resistance heating mechanism, (d) Joule-heating cycling performance of the CNFA at a power input of 14 W, (e) diagram and photographic image of simulated electrical heated clothing (57 mm diameter, 6 mm height, approximately 360 mg), (f) infrared thermal images acquired a different power inputs, (g) infrared thermal imaging of a commercial hair dryer (rated power: 1200 W) operating at an alternating current (AC) voltage of 220 V and a photograph showing its internal structure, (h) photograph of the custom-made Joule-heating device and its infrared thermal image acquired at 9 W power input (inset: an infrared thermal image of the CNFA with diameter: 23.5 mm, height: 9 mm, density: 20.58 mg cm-3), and (i) plots of temperature against time for the hair dryer and CNFA according to Videos S1 and S2 after power-on and power-off, operating at AC 220 V and 1200 W for the hair dryer, direct current (DC) 11 V and 9 W (actual calculated power) for the CNFA. Test conditions: open system and ambient temperature (21.3 °C).

Fig. 5. (a) Schematic diagram of the separator apparatus, (b) saturated adsorption capacities of the CNFA for different solvents at room temperature (RT: 20 °C), (c) times required for different solvents to reach saturated adsorption capacity at RT and 70 °C. Photographic images showing the adsorption of organic solvents ((d1-d4) for H2O (dyed with copper nitrate) + blend oil, (e1-e4) for H2O (dyed with copper nitrate) + CCl4 (stained with methyl red)), using an H2O: blend oil or CCl4vol ratio of 2:1; (f1) diagram showing the separation process, (f2) photographic images of the removal process; and (g) removal percentages of acetone and DMF (3 g L-1) from water over repeated treatment using open systems at ambient temperature (20 °C).

Table 1. Removal characteristics of microscale organic matter and comparison of its parameters.

Materials	Source of contaminated water	Initial COD (mg L^-1)	Removal percentage of COD/%	Refs.
Carbon nanofiber aerogel (CNFA)	Acetone + Water	4990	87	This work
Carbon nanofiber aerogel (CNFA)	DMF + Water	4351	92	This work
Single chamber microbial fuel cell (SCMFC)	Wastewater treatment plant	210-220	80	2004 [45]
Cellulose acetate - polyethersulphone blend membrane (CA-PES)	Permeated palm oil mill effluent	15,000	41	2007 [46]
Closed, cylindrical acrylic reactor	Supernatant of livestock wastewater	100-800	O₃: 54 O₃/H₂O₂: 62 O₃/UV: 78 O₃/H₂O₂/UV: 88	2011 [47]
Bio-trickling filter (volcanic rock + polyvinyl chloride)	DMF wastewater	300-400	80-90	2016 [48]
Composite of nano-MgO, CNT and Graphite	Pesticide-laden wastewater	6173	82	2020 [49]
Hybrid system combining Floating, Vertical, and Horizontal Flow Constructed Wetlands (gravel + pebble)	Urban wastewater	-^a	77	2020 [33]
Bacterial community	Acetone, propionic and hexanoic acids-components of wastewater	4000-6000 8000-10,000	5 g COD/L: 89 9.53 g COD/L: 82	2020 [50]
Lectin protein isolated	Coffee cherry pulping wastewater	29,460	80	2021 [51]
Micro-packed bed reactor (Zirconia ceramic beads, g-Al₂O₃ pellets)	Organic pollutants (including phenols, antibiotics, and dyes)	1450	70-80	2021 [52]
TiO₂, boron carbon nitride (BCN) nanosheets	Gasfield produced water	9500	81	2021 [53]
Multiple phenyl iron tetraamino ligand	Dye wastewater	-	catalyst A: 52-61 catalyst B: 45-58	2021 [54]
Microflora in hybrid constructed wetland	Landfill leachate treatment	640-984	55-76	2021 [55]

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