Multifunctional photothermal fabrics with water repellent for efficient crude oil adsorption and seawater desalination

Abstract

Solar-driven crude oil adsorption and seawater desalination have become promising strategies for oil spill recovery and freshwater production, respectively. However, the water adsorbed into the solar absorber has negative impacts on both the oil adsorption capacity and water evaporation rate, so it is vital to restrain water from entering the solar absorber. Herein, a versatile photothermal fabric was prepared by modifying carbon cloth (CC) with polydimethylsiloxane (PDMS). The introduction of PDMS improves the light absorption and the hydrophobicity, and prevents water from being adsorbed into the absorber. Taking advantage of the above properties, CC@PDMS exhibits an outstanding crude oil adsorption capacity of 21.13 g g⁻¹ and a remarkable evaporation rate of 1.81 kg m⁻² h⁻¹. This work provides a facile strategy for solving the common issue of solar-driven crude oil adsorption and solar steam generation.

Keywords

Solar-driven crude oil adsorption solar steam generation photothermal fabrics seawater desalination photothermal conversion lipophilic and hydrophobic

The growing scarcity of energy and fresh water poses a serious threat to the production and life of human society.^1,2 To tackle this dilemma, attention has turned to the ocean, which contains a critical mass of resources, including crude oil and water.³ However, frequent crude oil leakage caused by oil exploitation, storage and transportation not only imperils marine security and ecological balance, but also leads to great energy waste.⁴ Moreover, the high viscosity of crude oil at room temperature (10³–10⁵ MPa s) restricts the efficient removal of oil spills.⁵ More recently, the photothermal effect has been utilized to heat oil components to significantly reduce their viscosities to achieve rapid crude oil cleanup.^6,7 Huang et al.⁷ measured the changes between the viscosity of the crude oil and the amount of its adsorption with temperature, in particular. When the temperature of crude oil rises from 20°C to 90°C, the viscosity decreases from 6.1 × 10⁴ to 3.6 × 10² MPa · s. When the temperature rises from 30°C to 90°C, the crude oil adsorption capacity increases from 0.84 to 6.14 kg m⁻² (within 1 min). Interestingly, interface photothermal conversion technology also displays great potential in solar-driven seawater desalination.^8–10 Therefore, it is imperative to develop a versatile solar absorber with excellent performance both in crude oil adsorption and seawater desalination.

Typically, a series of porous absorbents, such as commercial sponge^11–13 and wood-based aerogel,^5,14 are selected as the matrix, then hydrophobic polymer (e.g., polydimethylsiloxane [PDMS])^15,16 and photothermal materials (e.g., carbon tubes,^17,18 carbon dots,¹⁹ graphene,^6,7 polypyrrole²⁰ and molybdenum disulfide¹³) are introduced to endow the matrix with remarkable lipophilicity and solar-to-heat performance. Under sunlight, the obtained solar absorber floating on the oil spill could heat the crude oil in situ and reduce its viscosity.²¹ Then the oil with enhanced fluidity would be easily adsorbed into the solar absorber. However, in practice, the absorber will inevitably contact with seawater. For most solar absorbers with a developed pore structure, seawater will enter the absorber driven by capillary force and occupy the space for storing crude oil, which has an adverse effect on the adsorption efficiency. Thus, it is necessary to improve the selective adsorption of oil for solar absorbers.

For solar-driven seawater desalination, a hydrophilic porous matrix is usually chosen to ensure an adequate water supply.^22–24 Nevertheless, the excess water in the absorber caused by the rapid water supply would have negative impacts on photothermal conversion and water evaporation.^25–27 If no water enters the absorber, solar-to-steam conversion would take place at the interface between the solar absorber and the water surface, which is conducive to high-performance solar steam generation. Therefore, preventing water from entering the absorber is also important for solar desalination.

Bamboo charcoal-based activated carbon cloth (CC) with high porosity is widely used in the adsorption of dye and heavy metal wastewater. However, its inherent photothermal property and hydrophobicity have rarely been deeply explored and applied. Herein, a versatile photothermal fabric was prepared by modifying CC with PDMS. The CC modified by PDMS (CC@PDMS) displays a splendid overall light absorption of 99.1% and a notable hydrophobicity (the water contact angle is 140°). Moreover, the introduction of PDMS prevents water from being adsorbed into the absorber, avoiding the adverse effects of water in crude oil adsorption and solar steam generation. Taking advantage of the above properties, CC@PDMS exhibits an outstanding crude oil adsorption capacity of 21.13 g g⁻¹ and a remarkable evaporation rate of 1.81 kg m⁻² h⁻¹. This work provides a facile strategy for solving the common issue of solar-driven crude oil adsorption and solar steam generation.

Materials and methods

Materials

CC was purchased from Alibaba. Crude oil was purchased from Sinopec Zhongyuan Oilfield. PDMS and petroleum ether were purchased from Shanghai Aladdin Biochemical Technology Co., Ltd. Acetic acid, ethyl acetate, ethanol absolute and silicone oil were purchased from Tianjin FengChuan Chemical Reagent Technology Co., Ltd.

Preparation of CC@PDMS

As shown in Figure 1, CC was washed by ethanol and then heated at 102°C for 2 h. Next, 20 mg prepolymer of PDMS, 1 mg hardener, 7.5 mL ethyl acetate and 2.5 mL ethanol were put into a beaker and stirred to obtain a mixture. Then, CC was soaked in the mixture and stirred for 3 h. Finally, the resultant product was dried at 120°C for 4 h to obtain CC modified by PDMS (denoted as CC@PDMS).

Figure 1.
Schematic diagram of the preparation of carbon cloth (CC)@polydimethylsiloxane (PDMS) for solar-driven oil adsorption and solar steam generation.

Characterization

The morphology was observed by a field-emission scanning electron microscope (SEM, JSM-7500F) at an accelerating voltage of 10 kV. The surface elemental distribution was analyzed using an energy-dispersive X-ray spectrometer (EDX, Empyrean Panalytical Cu). The phase structure was analyzed by X-ray diffraction (XRD, Empyrean) in the range of 10–50° with a scan rate of 5°/min. Raman spectra were recorded by a confocal Raman microscope (DXRxi) at the range of 50–3400 cm⁻¹. The absorption spectra were tested using an ultraviolet-visible near-infrared (UV-Vis-NIR) spectrophotometer (UV-3600i Plus) in the range of 200–2500 nm with an integrating sphere. Water contact angle measurement was carried out on a standard type contact angle meter (JC-2000A) using a 2 µL droplet of water as an indicator.

Photothermal conversion experiment

A solar light simulator (PLS-SXE300D) was used as the light source. The surface temperatures of CC and CC@PDMS in air and water were monitored using an infrared thermal imaging camera (UNI-T, UTi260B) at a distance of 20 cm. All photothermal conversion experiments were carried out under the conditions of air temperature of 20–22°C and humidity of 16%, and the intensity of simulated sunlight was 1 kW m⁻² (one sun).

Solar-driven oil adsorption experiment

Various types of oils and organic solvents, including silicone oil, vegetable oil, petroleum ether, ethanol, chloroform and crude oil, were used to determine the adsorption capacities of the samples. The tested sample was uniformly cut into a cuboid (1 cm × 1 cm × 0.3 cm). After being weighed, the sample was immersed in a solvent. Then, the sample was removed from the solvent for subsequent weight measurement. The oil adsorption capacity (Q_t, g g⁻¹) was calculated by Equation (1)
$Q_{t} = (W_{t} - W_{0}) / W_{0}$
(1)
where W₀ (g) and W_t (g) are the weight of the CC and CC@PDMS before and after adsorption, respectively. All solar-driven oil adsorption experiments were carried out under the conditions of air temperature of 20–22°C and humidity of 16%, and the intensity of simulated sunlight was 1 kW m⁻² (one sun). Besides, all solar-driven oil adsorption experiments were performed more than three times.

Solar steam generation and seawater desalination experiment

The mass change of evaporation is measured by an electronic balance (Jinping, FA2004). The evaporation rate (m, kg m⁻² h⁻¹) was calculated by Equation (2)
$m = Δ m / (S \times t)$
(2)
where Δm is the mass of water evaporation in 1 h (kg), S is the area of the cross-section of the CC@PDMS (m²) and t is the time of solar irradiation (1 h). For seawater desalination experiments, the main ion concentrations of the seawater and the condensed water were tested using inductively coupled plasma-optical emission spectrometry (ICP-OES, JY200-2). All solar steam generation and seawater desalination experiments were carried out under the conditions of air temperature of 20–22°C and humidity of 16%, and the intensity of simulated sunlight was 1 kW m⁻² (one sun).

Results and discussion

As shown in the SEM images (Figure 2(a)), CC is composed of randomly arranged micron-scale fibers, and a large number of holes formed by interlaced fibers are advantageous for the adsorption of oil. With the modification of PDMS, the aforementioned morphology and microstructure could be still observed (Figure 2(b)). High-magnification SEM images (Figures 2(c) and (d)) show that the mean diameter of carbon fibers in CC@PDMS (10.1 ± 0.7 µm) is slightly larger than that of CC (8.9 ± 0.9 µm). It is conjectured that the diameter change is caused by the attachment of PDMS in the face of carbon fibers. Furthermore, the elemental mappings based on EDX portray the homogeneous distribution of the silicon element, aside from carbon and oxygen elements, in CC@PDMS (Figures 2(e)–(g)). In addition, the characteristic peaks of PDMS could be observed from the Fourier transform infrared (FTIR) spectrum of CC@PDMS (Figure S1). The results above show that PDMS attaches to the surface of carbon fibers successfully.

Figure 2.
Scanning electron microscope images of (a) carbon cloth (CC), (b) CC@polydimethylsiloxane (PDMS), (c) enlarged view of CC and (d) enlarged view of CC@PDMS. The dashed box shows the selected section for energy-dispersive X-ray spectrometer (EDX) observation. EDX maps of (e) C, (f) O and (g) Si of CC@PDMS.

XRD patterns of CC and CC@PDMS are displayed in Figure 3(a). Characteristic diffraction peaks of graphite (2θ = 24.6 (002) and 2θ = 44.7 (101))²⁸ are observed. Meanwhile, the intensities of the diffraction peaks at (002) and (101) in CC@PDMS are almost consistent with those of CC. Figure 3(b) shows the Raman spectra of CC and CC@PDMS. The peak at ca. 1340 cm⁻¹ (D band) is due to the vibration of carbon atoms with dangling bonds in the plane terminations of disordered graphite. The G band at ca. 1592 cm⁻¹ is related to an E_2g mode of hexagonal graphite and associated with the vibration of sp²-bonded carbon atoms in a graphite layer.^29,30 The I_D/I_G ratio of CC@PDMS is close to that of CC, which means that they possess similar order degrees of the graphite structure. The above results show that PDMS sticks to the surface of carbon fibers only, and does not alter its inherent structure.

Figure 3.
(a) X-ray diffraction patterns, (b) Raman spectra and (c) ultraviolet-visible near-infrared absorption spectra of carbon cloth (CC) and CC@polydimethylsiloxane (PDMS). (d) Surface temperatures of CC and CC@PDMS under one solar irradiation in air. Infrared images of (e) CC and (f) CC@PDMS under one solar irradiation.

The light absorption capacity is significant for photothermal conversion. Thereby, the UV-Vis-NIR absorption spectra of samples are measured (Figure 3(c)). CC exhibits a splendid overall light absorption of 97.6% due to the inherent black color and the porous structure of carbon fibers. However, the light absorption of CC@PDMS reaches 99.1%. It is speculated that the PDMS coating reduces the reflection loss and enhances the light absorption.^31,32 Subsequently, the photothermal conversion abilities of CC and CC@PDMS in air were investigated. As shown in Figures 3(d)–(f), the surface temperature of CC@PDMS rises to 97.4°C within 300 s, then it maintains a stable temperature upon extending the irradiation time. The maximum temperature of CC@PDMS exceeds that of CC (95.0°C), suggesting the obvious advantage of CC@PDMS in efficient photothermal conversion.

As shown in Figures 4(a) and S2, CC with high specific surface area (1256.8 m² g⁻¹) has a good adsorption performance for silicon oil (18.60 g g⁻¹), vegetable oil (17.60 g g⁻¹), ethanol (13.98 g g⁻¹), petroleum ether (12.89 g g⁻¹) and chloroform (24.66 g g⁻¹), while the adsorption capabilities of CC@PDMS are 17.89, 16.83, 13.24, 12.40 and 24.12 g g⁻¹, respectively. The introduction of PDMS increases the density of fabric, so both the specific surface area (968.3 m² g⁻¹) and oil adsorption capability of CC@PDMS decrease slightly.

Figure 4.
(a) Adsorption capabilities of carbon cloth (CC) and CC@polydimethylsiloxane (PDMS) for different organic solvents and oils. Photographs of the dynamic processes of a water droplet on the surface of (b) CC and (c) CC@PDMS. (d) Oil adsorption capabilities of CC and CC@PDMS in silicon oil–water mixtures with different contents of silicon oil. The adsorption behaviors of (e) CC and (f) CC@PDMS in chloroform (dyed with red oil–water mixture).

The water contact angles of CC and CC@PDMS are shown in Figures 4(b) and (c), respectively. The instant contact angle of CC is 137.5°, and the water droplet quickly permeates inside the CC under capillary action. Comparatively, the water droplet keeps a high contact angle of 140.8° on the surface of CC@PDMS for a long time, suggesting that the introduction of PDMS enhanced the water repellency of CC.

Figure 4(d) shows that the oil adsorption capabilities of CC and CC@PDMS in the silicon oil–water mixture. Due to the poor selective adsorption capability of CC, a large amount of water in the mixture is adsorbed into the CC, bringing about a low adsorption of oil. Although the proportion of oil increased, its oil adsorption capability is only 3.01 g g⁻¹ (the content of silicon oil is 50%). In contrast, CC@PDMS can reject the entry of the water and selectively adsorb oil in the oil–water mixture. With the content of oil, its oil adsorption capability increases to 14.63 g g⁻¹ (the amount of oil is 50%), which is almost equal to the oil adsorption capability in pure silicone oil. To explain the selective adsorption capabilities of CC and CC@PDMS more clearly, we hold the CC (Figure 4(e), Movie S1) and CC@PDMS (Figure 4(f), Movie S2) with tweezers to adsorb chloroform (dyed with oil red) at the bottom of the water. It can be observed that CC hardly adsorbs chloroform since it has been filled with water before approaching chloroform at the bottom. In contrast, CC@PDMS cleans up chloroform at the bottom of the water within 12 s. Collectively, the introduction of PDMS improves the selective adsorption performance of CC@PDMS to oil, which is conducive to realize efficient oil recovery in practical scenarios, such as offshore crude oil leakage.

As shown in Figure 5(a), the crude oil is hardly adsorbed into CC@PDMS due to its high viscosity and poor liquidity at normal temperature. However, as shown in Figure S3, the viscosity of crude oil decreases with increasing temperature, so the crude oil on the water surface is fully removed by CC@PDMS within 3 min under one sun irradiation (Figure 5(b)), demonstrating that the photothermal conversion effect plays a critical role in the adsorption of crude oil. The maximum oil adsorption capacity for CC@PDMS in pure oil is displayed in Figure 5(c). Under one irradiation, the oil adsorption of CC@PDMS rapidly increases and approaches adsorption saturation at 8 min. Moreover, its maximum oil adsorption capacity (21.13 g g⁻¹) is 6.8 times that without solar irradiation (3.10 g g⁻¹). To explore its recyclability, CC@PDMS is used for oil adsorption and release multiple times (Figure 5(d)). In the process of crude oil release, repeated extrusion makes the arrangement of fibers denser and causes the decrease of porosity. Therefore, the oil adsorption capacity slightly decreases as the number of squeezes increases. Nonetheless, the recovery of crude oil is efficient (up to 95.6%) and stable. The results indicate that an excellent photo-to-thermal conversion of CC@PDMS allows rapid cleaning and efficient recovery of crude oil.

Figure 5.
Photographs of the crude oil removal experiments (a) without and (b) with solar irradiation. (c) The oil absorption capacities for carbon cloth@polydimethylsiloxane with time under dark and under irradiation and (d) Mass of crude oil in oil absorption–recovery cycles under one sun irradiation.

Consistent with the results in Figures 4(b) and (c), most of the CC immerses in water due to its poor water repellency, while CC@PDMS floats on the water stably (Figure 6(a)). The above difference directly affects the photo-to-thermal conversion capabilities of the samples. Figure 6(b) displays the surface temperatures of CC and CC@PDMS under solar irradiation on water within 60 min. The surface temperature of CC@PDMS rapidly reaches 79.2°C within 5 min, then it maintains the temperature of 88.2°C steadily upon extending the irradiation time. However, the temperature of CC is only 54.9°C after 60 min. To study the influence of the floating state on photo-to-thermal conversion, COMSOL software simulation models of the temperature distribution of samples were established. As shown in Figure 6(c), due to the difference of thermal conductivity in the structure caused by the permeation of water, the surface temperature of CC presents gradient distribution. The temperature of CC filled with water drops sharply from top to bottom since plenty of heat generated by photothermal conversion is consumed by the adsorbed water and bulk water. Without adsorbed water, most of the energy harvested from solar power is concentrated on CC@PDMS, endowing it with a high temperature (Figure 6(d)). Thus, most energy generated by CC@PDMS will be used to heat a small amount of water in contact with the bottom of the fabric, which is conducive to the realization of high-efficiency solar-to-steam conversion.

Figure 6.
(a) The floating states of carbon cloth (CC) and CC@polydimethylsiloxane (PDMS) in water. (b) Surface temperatures of CC and CC@PDMS under one solar irradiation in water. COMSOL software simulation models of the temperature distribution of (c) CC and (d) CC@PDMS under one solar irradiation in water.

In addition, the desalination performance of the solar steam generator is investigated. As shown in Figure 7(a), the water mass decreases approximately linearly with irradiation time. CC@PDMS displays an extremely high evaporation rate of 1.81 kg m⁻² h⁻¹ by virtue of its local heating effect, which is 2.55, 1.36 and 7.51 times that of seawater (0.71 kg m⁻² h⁻¹), CC (1.33 kg m⁻² h⁻¹) and dark (0.24 kg m⁻² h⁻¹), respectively. The long-term stability of CC@PDMS is evaluated by measuring the water evaporation rate under cyclic solar irradiation conditions. Figure 7(b) shows that there is no considerable difference in the evaporation rate after 10 cycles. In addition, the evaporation rate is stably above 1.75 kg m⁻² h⁻¹, demonstrating the good stability of CC@PDMS. Evaporation is caused by the thermal movement of molecules, while ions are not evaporated, so only water vapor could pass through the pores of the evaporator. Fresh water is obtained by condensing water vapor, the concentration of freshwater ions obtained is much lower than that of seawater and the concentrated salt would fall back into the seawater under the action of gravity during solar steam generation.^33–37 Thus, no accumulated salt is observed on the surface of CC@PDMS during long-lasting solar desalination (Figure 7(d)). In addition, CC@PDMS works well in removing many types of heavy metal ions from seawater, and the ion rejections of Na⁺, K⁺, Mg²⁺ and Ca²⁺ are above 99.9%. It is clear that the purification result of seawater meet the criteria for the standard of drinkable water as defined by the World Health Organization (WHO).³⁸ To demonstrate the scalable capability for the practical desalination application of CC@PDMS, a large-scale solar steam generation system (Figure 7(e)) including an evaporation chamber, CC@PDMS evaporator, steam condenser and water collecting layer was employed. The device was placed on the campus of Zhengzhou University for one day. Figure 7(f) shows that maximum outdoor temperature and solar irradiation on that day were 21°C and 0.72 kW m⁻², respectively; CC@PDMS displayed a water production of 3.92 kg m⁻² (Figure 7(g)), exhibiting a robust water production ability in outdoor conditions.

Figure 7.
(a) Cumulative mass changes of seawater versus time under different conditions: seawater under dark (dark), seawater (blank), seawater with carbon cloth (CC) and CC@polydimethylsiloxane (PDMS). (b) The evaporation cycle performance of CC@PDMS in seawater. (c) Concentrations of Na⁺, K⁺, Mg²⁺ and Ca²⁺ in seawater and the World Health Organization (WHO) standard for healthy drinking water. (d) Self-desalting performance of CC@PDMS during desalination for 10 h. (e) Schematic diagram of the outdoor seawater desalination device. (f) Changes of solar power density and outdoor temperature with time and (g) Accumulated clean water production and water production rate with time.

Conclusion

In summary, a versatile photothermal fabric was obtained by modifying CC with PDMS. CC@PDMS displays splendid overall light absorption of 99.1% and notable hydrophobicity (the water contact angle is 140°). CC@PDMS exhibits an outstanding crude oil adsorption capacity of 21.13 g g⁻¹ and a remarkable evaporation rate of 1.81 kg m⁻² h⁻¹. In addition, the introduction of PDMS prevents water from being adsorbed into the absorber, avoiding the adverse effects of water in crude oil adsorption and solar steam generation. We provide a facile method to enhance the performances of solar-driven crude oil adsorption and solar steam generation at the same time, which has important practical significance to handle the issues of oil spills and freshwater shortages. In addition, the two-in-one design of sewage treatment and freshwater production driven by clean energy is also an important exploration direction that can be widely used in rivers or lakes polluted by industry in addition to sea surface crude oil adsorption and seawater desalination. It not only makes full use of the absorber/evaporator, but also greatly improves the efficiency of water purification. It is especially suitable for remote, arid and energy-poor areas.

Supplemental Material

sj-pdf-1-trj-10.1177_00405175221147252 - Supplemental material for Multifunctional photothermal fabrics with water repellent for efficient crude oil adsorption and seawater desalination

Supplemental material, sj-pdf-1-trj-10.1177_00405175221147252 for Multifunctional photothermal fabrics with water repellent for efficient crude oil adsorption and seawater desalination by Xiangyi Gu, Xuying Chen, Li na Wang, Changyuan Song, Junhua Hu and Wentao Liu in Textile Research Journal

Footnotes

Authors Note

Lina Wong is now affiliated with College of Materials Engineering, Henan University of Engineering, China. Junhua Hu is also affiliated with State Center for International Cooperation on Designer Low-carbon & Environmental Materials (CDLCEM), China.

Declaration of conflicting interests

The author(s) declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.

Funding

The author(s) disclosed receipt of the following financial support for the research, authorship and/or publication of this article: This work was supported by the National Natural Science Foundation of China (51872266, 51672253, 51571182 and 52171082), the National Key Research and Development Program of China grant (2018YFD0400702), the Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN003) and the Henan Provincial Key Laboratory for Metal Fuel Battery.

ORCID iD

Changyuan Song

Supplemental material

Supplemental material for this article is available online.

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