“Several birds with one stone” strategy of pH/thermoresponsive flame-retardant/photothermal bactericidal oil-absorbing material for recovering complex spilled oil

doi:10.1016/j.jmst.2022.05.002

Abstract

Abstract:

Although many material designs or strategic methods have been proposed for treating oil spills and oily wastewater, the complex oily state, dealing with the harsh operating conditions of oil-water separation (such as the recovery of viscous spilled crude oil, bacteria-containing oily wastewater, and removal of spilled oil under fire), and the autorecycling of oil and absorption materials remain a great challenge. This work proposed an ingenious design strategy of “several birds with one stone” to prepare pH/thermoresponsive flame-retardant/photothermal bactericidal P-Fe₃O₄-polydopamine (PDA)@melamine-formaldehyde (MF) foams. This design makes the foams remarkably effective in the recovery of spilled viscous crude oil as well as in the separation of bacteria-containing oily emulsions, particularly for instant fire extinguishing by magnetically controlled oil absorption as well as for fire alarms. The photothermal effect and pH response induce a change in the surface wettability of the foams, facilitating excellent autoadsorption/desorption of the spilled oil. The photothermal bactericidal activity and fouling resistance of the foam are beneficial to the separation of bacteria-containing oily wastewater. Outstanding flame-retardant properties and maneuverable magnetic control enable the foam to rapidly recover the spilled oil in a large range of fires, extinguish fires instantly, and facilitate early fire warning. The proposed strategy is expected to inspire further research on treating oil spills under complex conditions.

Key words: Oil-absorbing material, pH-responsive, Thermoresponsive, Photothermal, Bactericidal, Fire warning

Chen Ya, Lin Jing, A.M. Mersal Gaber, Zuo Jianliang, Li Jialin, Wang Qiying, Feng Yuhong, Liu Jianwei, Liu Zili, Wang Bin, Bin Xu Ben, Guo Zhanhu. “Several birds with one stone” strategy of pH/thermoresponsive flame-retardant/photothermal bactericidal oil-absorbing material for recovering complex spilled oil[J]. J. Mater. Sci. Technol., 2022, 128: 82-97.

Figures/Tables 9

Fig. 1. (a) Schematic diagram of the preparation process of multiresponse oil-absorbing foam and (b) application of P-Fe3O4-PDA@MF foam in complex oil spill treatment.

Fig. 2. SEM images of (a) MF, (b) PDA@MF, (c) Fe3O4-PDA@MF, and (d) P-Fe3O4-PDA@MF; (e) ATR-FTIR and (f) XRD of foams at different preparation stages; (g) SEM-EDS mapping distribution of various elements on P-Fe3O4-PDA@MF. (h) XPS spectra of P-Fe3O4-PDA@MF.

Fig. 3. (a) Schematic diagram of the absorption process of oil on water and underwater before and after the thermo-response of P-Fe3O4-PDA@MF. (b) Differential scanning calorimetry (DSC) of P-Fe3O4-PDA@MF. (c) Water contact angles (WCAs) of P-Fe3O4-PDA@MF at 50 °C. (d) Oil contact angles (OCAs) on water and (e) underwater oil contact angles (UWOCAs) of P-Fe3O4-PDA@MF. P-Fe3O4-PDA@MF adsorption photos of (f) light oil (cyclohexane) and (g) heavy oil (1,2-dichloroethane) at 50 °C. (h) Oil absorption capacities of various oily substances. (i) Mechanism diagram of the thermoresponsive oil absorption process of P-Fe3O4-PDA@MF.

Fig. 4. (a) WCAs of P-Fe3O4-PDA@MF at pH = 1. UWOCA diagrams of (b) light oil (cyclohexane) and (c) heavy oil (1,2-dichloroethane) on the P-Fe3O4-PDA@MF surface. Photographs of the P-Fe3O4-PDA@MF desorption process of (d) underwater light oil (cyclohexane) and (e) heavy oil (1,2-dichloroethane). (f) Oil absorption and desorption efficiency diagram of different oily substances (CYH: cyclohexane, DCE: 1, 2-dichloroethane, TL: toluene, NHD: n-hexadecane, PE: petroleum ether). (g) Cyclic oil absorption-desorption tests diagram of P-Fe3O4-PDA@MF. (h) Mechanism diagram of oil desorption process of P-Fe3O4-PDA@MF. (i) XPS spectrum of P-Fe3O4-PDA@MF at pH = 1. XPS spectra of N1s at (j) pH = 1 and (k) pH = 7. (l) Thermodynamic infused-liquid-switchable models.

Table 1. Feasibility evaluation of the oil autodesorption process according to the interfacial energy difference.

Liquid A	Liquid B	${{\gamma }_{\text{L}}}$ ($\text{mJ}\ {{\text{m}}^{-2}}$)		${{\gamma }_{\text{AB}}}$ ($\text{mJ}\ {{\text{m}}^{-2}}$)	θ*(°)		∆E		Autodesorption
Liquid A	Liquid B	${{\gamma }_{\text{A}}}$	${{\gamma }_{\text{B}}}$		$\theta _{\text{A}}^{*}$	$\theta _{\text{B}}^{*}$	$\text{ }\!\!\Delta\!\!\text{ }{{E}_{1}}$	$\text{ }\!\!\Delta\!\!\text{ }{{E}_{2}}$	Theory	Exp.^a
CYH^b	Aqueous solution (pH = 1)	24.94	66.48	17.59	154.5	0	> 0	> 0	Y^d	Y
DCE^c	Aqueous solution (pH = 1)	30.85	66.48	42.87	153.8	0	> 0	> 0	Y	Y

Fig. 5. (a) Infrared thermal image of foams at different modification stages after illumination (1.0 kW m?2). (b) Viscosity of crude oil at different temperatures. (c) Crude oil absorption state on the P-Fe3O4-PDA@MF without illumination, and (d) with illumination. (e) Curves of the temperature of P-Fe3O4-PDA@MF and pristine MF during crude oil absorption. (f) Absorption process of simulated offshore crude oil on water. (g) Continuous absorption process and infrared thermal image of crude oil using a peristaltic pump under no illumination or (h) with illumination. (i) Recovery percentage of crude oil and 1,2-dichloroethane.

Fig. 6. (a) Mechanism diagram of filtration and photothermal sterilization for bacteria-containing emulsion. (b) Images and particle size distribution of an emulsion containing S. aureus and E. coli coated on an agar plate before and after filtration. (c) Infrared thermal image of filter device load with P-Fe3O4-PDA@MF, fluorescence microscopy, colonies on the agar plate, and micromorphology of bacteria after illumination and no illumination. (d) UWOCA and (e) adhesion force of oil (1,2-dichloroethane) on P-Fe3O4-PDA@MF.

Fig. 7. (a) Combustion of foam (PU and P-Fe3O4-PDA@MF) after oil absorption. (b) Photographs of oil absorption and flame-retardancy of P-Fe3O4-PDA@MF. Diagrams of (c) TG, (d) DTG of PU foam and P-Fe3O4-PDA@MF. (e) Photographs of magnetic oil absorption and fire extinguishing of P-Fe3O4-PDA@MF. (f) Hysteresis loop diagram of Fe3O4 NPs and their modified foam. (g) Mechanism diagram of oil absorption and flame-retardancy of P-Fe3O4-PDA@MF. (h) Resistance changes of P-Fe3O4-PDA@MF with temperature. (i) Fire alarm response of P-Fe3O4-PDA@MF.

Table 2. Comparison of various porous sorbent materials (-, ×, and √ stand for Unknown, No, and Yes, respectively.)

Porous materials	Absorbates	Absorptioncapacity (g g^-1)	Oil/adsorbent recovery method	Oil recovery efficiency (%)	Antibacterial	Magnetic control	Flame retardant	Fire warning	Refs.
PDMS/PDA coated sponge	Crude oil	∼11	Be compressed	-	×	×	×	×	[53]
Silylated wood sponge	Silicone oil, olive oil, motor oil, and organic solvents	16-41	Be compressed	∼70	×	×	×	×	[54]
Fe₃O₄@OA @GO-PU^a	Olive oil, canola oil, kerosene, and organic solvents	80-150	Be compressed	> 99	×	√	√	×	[89]
Fe₃O₄/HDPE^b PU sponge	Cook oil and organic solvents	15-52	Be compressed	-	×	√	×	×	[90]
Silica/graphene oxide wide ribbon@MF	Petrol oil, tetrachloromethane	-	Be compressed	-	×	×	√	√	[88]
Tannic acid-graphene aerogel	Kerosene, liquid paraffin, maize oil, soybean oil, and organic solvents	15-30	Combustion	-	√	×	√	×	[91]
MF-OTS^c/ PNIPAAm sponge	Pump oil, peanut oil, and organic solvents	35-70	Thermoresponsive desorption	-	×	×	×	×	[71]
PNIPAm/PPy@MS	Crude oil, silicone oil, mineral oil, paraffin oil, bitumen	∼32	Thermoresponsive desorption	> 87	×	×	×	×	[92]
Porous polyHIPE^d monoliths	Pump oil, edible oil, crude oil, and organic solvents	6.7-18.2	pH-responsive desorption	∼100	×	×	×	×	[93]
pH-responsive SiO₂@MF	Silicone oil, soybean oil, and organic solvents	20-50	pH-responsive desorption	-	×	×	×	×	[94]
P-Fe₃O₄-PDA@MF	Crude oil, pump oil, silicone oil, and organic solvents	12.8-43.8	pH-responsive desorption	88.7-98.4	√	√	√	√	This work

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