Professional Documents
Culture Documents
PII: S2950-1555(23)00031-9
DOI: https://doi.org/10.1016/j.greenca.2023.12.002
Reference: GREENC25
Weichao Dong a,c,d,f,1, Lina Huang b,1, Xiangju Song a,c,d*, Yan Zhang a,c,d, Mengke Liu
a,c,d,f
, Zhenzhen Ren e, Long Pang a,c,d, Hui Peng a,c,d, Heqing Jiang a,c,d*
a
Key Laboratory of Biobased Materials, Qingdao Institute of Bioenergy and Bioprocess
Technology, Chinese Academy of Sciences, Qingdao, 266101, China
b
School of Material Science and Engineering, Henan Polytechnic University, Jiaozuo,
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454003, China
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c
Shandong Energy Institute, Qingdao, 266101, China
e
d
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Qingdao New Energy Shandong Laboratory, Qingdao, 266101, China
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College of Chemistry and Pharmaceutical Engineering, HuangHuai University, Zhumadian,
463000, China
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f
University of Chinese Academy of Sciences, Beijing, 101408, China
*Corresponding authors:
a
jianghq@qibebt.ac.cn(HJ); +532-80662716;
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song_xj@qibebt.ac.cn(XS)
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Author contributions:
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1
ZR2021QB111), the Taishan Scholars Program of Shandong Province (No. tstq20221151), and
the Innovation Funds of Shandong Energy Institute (SEI I202140).
Declaration of Interest: The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence the work reported in
this paper.
Abstract
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Indoor heating results in high energy consumption and severe atmospheric pollution.
Although the development of solar air heaters provides a sustainable route for indoor thermal
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comfort, such heaters still face challenges in terms of adequate heat exchange and filtering of
atmospheric pollutants. Inspired by solar-driven interfacial evaporation, we propose a
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multifunctional carbon nanotube-based photothermal membrane for efficient cold air heating
and purification via ventilation. Carbon nanotubes endow the membrane with high light
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absorption and thermal conversion capabilities, thereby sufficiently heating the approaching
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cold air. With the hierarchical structure formed by phase inversion, the thin upper skin of the
composite membrane intercepts micropollutants via the size-sieving effect, whereas the finger-
like pores and interpenetrating macrovoids inside the membrane ensure that the heated clear air
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across the membrane, yielding a temperature increase of ca. 37 °C as well as a PM 2.5 rejection
always higher than 93%. Further antibacterial experiments demonstrated that the membrane
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photothermal membrane with specific microstructures not only improves the indoor living
quality but also provides a sustainable development scheme to coordinate the relationship
among energy utilization, building heating, and air purification.
1. Introduction
Because people spend the majority of their lives indoors, a comfortable and healthy indoor
environment must be provided [1, 2]. However, in cold regions, space heating in winter, even
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during shoulder seasons, leads to significant energy consumption and severe air pollution [3-6].
The atmosphere is exposed to various pollutants, including bacteria and fine particulate matter
(PM 2.5), that often cause long-lasting haze weather. With improvements in the airtightness of
modern buildings, ventilation is often required to avoid the wanton spread of microorganisms
in a relatively closed indoor environment [7-9], which is evidently not feasible on haze days.
Abundant and clean solar energy provides a sustainable route for indoor heating. However, for
the traditional solar air heater, the cold air entering the system only contacts the surface of the
absorber plate, resulting in extremely limited heat transfer [10]. MesgarPour et al. [11]
increased the air–absorber contact area and retention time to enhance the heat transfer efficiency
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by optimizing the geometry of the absorber. Nevertheless, further promotion of cold air heating
and efficient filtering of PM 2.5 or other pollutants in outdoor cold air are major challenges [12,
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13].
The recently developed solar-driven interfacial water evaporation method utilizes the
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surface of a photothermal membrane as the evaporation interface, where the heat obtained from
sunlight conversion is further localized and concentrated, thus selectively heating the
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evaporation portion of water instead of the entire body of water. The corresponding energy
utilization efficiency exceeds 90% when using the thermal localization strategy of a
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applied in many new scenarios such as wastewater purification [17, 18], atmospheric water
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harvesting [19-22], energy storage/conversion [23-25], and soil remediation [26, 27]. Recently,
Zhou et al. [28] fabricated photothermal hybrid dendritic nanosheets with well-ordered channels
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that displayed 90.9% energy efficiency under irradiation at 1 kW m-2. Li et al. [29] tailored a
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be explored to improve the indoor living environment by customizing the material and structure
of the photothermal membrane.
In this study, we prepared a multifunctional carbon nanotube-based photothermal composite
membrane and applied it to interfacial air heating and purification to meet the high requirements
of the public for indoor thermal comfort and air quality. As promising photothermal
components, carbon nanotubes achieved efficient light absorption and thermal conversion, thus
rapidly heating the approaching cold air. With the unique pore structure formed by nonsolvent-
induced phase separation, the thin upper skin of the composite membrane intercepted
micropollutants in the air via the size-sieving effect. The finger-like pores and interpenetrating
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macrovoids inside the membrane ensured that the heated air stream passed through quickly.
During a continuous test for up to 32 h, the multifunctional membrane maintained the PM 2.5
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rejection always higher than 93%, and the inlet cold air with an initial temperature of
approximately 13 °C could be heated up to approximately 50 °C. The designed antibacterial
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experiment indicated that the composite membrane effectively removed airborne bacteria under
the operating conditions. Furthermore, the lightweight composite membrane possessed
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excellent mechanical properties, and the ultimate stress reached 3.11 MPa owing to the
reinforcement of the carbon nanotubes. Thus, this interfacial photothermal system with air
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2. Experimental Section
2.1. Materials
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Polysulfone (PSF, P-3500, MW = 75–81 × 103) for membrane preparation was supplied by
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Solvay SA. Multi-walled carbon nanotube (MWCNT, O.D. × L: 20–40 nm × 10–30 μm) was
purchased from Aladdin Biochemical Technology Co., Ltd. N-methyl-2-pyrrolidone (NMP,
AR) and poly (vinylpyrrolidone) (PVP, MW = 44000–54000, GR) were purchased from
Sinopharm Chemical Reagent Co., Ltd. Agar powder was obtained from Solarbio. LB broth
was purchased from MDBio Inc.
2.2. Membrane fabrication
The synthesis process for the carbon nanotube-based photothermal composite membrane,
MWCNT@PSF–PSF, is depicted in Fig. 1. A mixture consisting of 1 g of MWCNT in 81 g of
NMP was preprocessed by ultrasonication, and then 3 g of PVP and 15 g of PSF were added to
the mixed solution. The homogeneous MWCNT–PSF dope solution was obtained by overnight
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mechanical stirring at 70 °C. The PSF casting solution was prepared under the same conditions
but without adding MWCNT. Subsequently, the defoamed PSF casting solution was cast onto
a glass plate using a manual precision doctor blade. After standing in air for 30 s, the MWCNT–
PSF solution was carefully poured at one end of the formed basement membrane and then
uniformly scraped. The obtained composite was immediately immersed in deionized water to
complete the phase inversion process and then dried at 50 °C in an oven.
2.3. Material characterization
The morphologies and microstructures of the membranes were observed using a Hitachi S-
4800 scanning electron microscope and a Thermo Scientific Prisma E scanning electron
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microscope, respectively. Atomic force microscopy (AFM, Agilent 5400) was used to examine
the surface morphology and roughness of the membranes. Raman spectra were recorded using
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a Thermo DXR Raman spectrometer. To investigate the distribution of MWCNT in the
membrane, line-scanning Raman spectroscopy was performed, and 13 different positions from
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the top to the bottom surface were sampled for analysis. The mechanical properties of the as-
prepared samples were measured using a material testing machine (Instron 5982). A mercury
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injection instrument (Quantachrome, PoreMaster 33) was used to test the porosity and pore size
distribution of the MWCNT@PSF–PSF composite membrane. Diffuse reflection and
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obtained using a FLIR One infrared camera. The airflow temperature was monitored using a
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TM-902C temperature sensor. The concentration of PM 2.5 was measured using a commercial
PM meter (CEM, DT-96 B).
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The membrane was fixed in a custom-made sealed chamber to investigate its ability to heat
the cold air. An air pump insufflated the ambient air into a precooling device, and after sufficient
heat exchange, a stable cold air flow was obtained. Cold air could undergo a slight heat
exchange with the atmosphere before entering the photothermal and separation system.
Subsequently, the cold air in the sealed chamber permeated from the upper surface of the
membrane to the lower side of the membrane, completed the heating process, and exited the
chamber. A schematic representation of this process is shown in Fig. S1. Two thermocouples
were placed near the inlet and outlet of the chamber to measure the real-time airflow
temperature. Unless specified, the light intensity was always set to 1 kW m-2. For the PM 2.5
interception test, an NaCl nanoparticle generator module (provided by Suzhou Huada Filer
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Technology Co., Ltd., China) was added in front of the pre-cooling device, and the dispersed
NaCl aerosols were used as the model PM particles, whose concentrations were detected in the
inlet and permeate air flows.
2.5. Antibacterial tests
To verify the antibacterial performance of the composite membrane under the operating
conditions, a pre-sterilized container was simulated as an indoor space, and a clean agar plate
was placed in it. The air passing through the membrane was continuously introduced into the
container for 8 h. Subsequently, the agar plate was removed and cultured in a constant
temperature incubator (37 °C, running at 20 rpm), and the colony growth was monitored
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regularly. In addition, a control experiment was set up, in which ambient air was directly
introduced into the closed container to contact the agar plate and then cultured under the same
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conditions after 8 h.
3. Results and Discussion
3.1. Structural properties -p
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an important parameter for practical applications; in particular, ensuring light weight and good
mechanical properties in parallel would facilitate the installation and usage of solar air heating
membranes. Therefore, tensile stress–strain tests were conducted on the membranes. As
illustrated in the inset of Fig. 1, for the pure PSF and MWCNT@PSF–PSF photothermal
composite membranes with similar thicknesses, the reinforcement effects of the MWCNT [31]
enabled the composite membrane to hold higher tensile rate (from 8.2% to 20.3%) and ultimate
stress value (2.527 MPa to 3.11 MPa).
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macropores (Fig. S2(b)). The entire cross section of the MWCNT@PSF–PSF membrane had a
finger-like macrovoid structure (Fig. 2(c)), and the local magnification images clearly showed
the existence of the MWCNT photothermal component in the upper layer of the membrane
(Fig. 2(d)). Compared with the line-scanning Raman spectra of the pure PSF membrane (Fig.
S3, 13 Raman spectra spanned the cross section of the film from top to bottom), the Raman
scanning of the MWCNT@PSF–PSF membrane (Fig. 2(b)) further revealed that the MWCNT
existed in the upper part of the membrane, according to the typical D peak (≈1340 cm-1) and
2D peak (≈2700 cm-1) [33, 34]. A mercury pressure test was conducted to investigate pore size
distribution. As shown in Figs. 3(a) and 3(b), the pore size was mainly concentrated in three
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ranges, and the corresponding peaks were 170 nm, 12 μm and 42 μm. Among the different
pores, the small nanopores distributed on the membrane surface can prevent micropollutants in
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cold air from entering the membrane; this may ensure relatively low internal pollution of the
membrane. Large pores can accelerate the transport of air owing to decreased mass transfer
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resistance. Therefore, the unique architecture of the photothermal composite membrane
allowed outdoor cold air to undergo sufficient heat exchange with the porous membrane to
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obtain adequate heat. Subsequently, it can quickly pass through the membrane for indoor
heating and ventilation (Fig. 2(a)).
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Fig. 3. (a) Pore size distribution of the MWCNT@PSF–PSF membrane. (b) Local magnified
image of the blue region.
3.2. Light absorption and light-thermal conversion
To ensure reliable ability to heat cold air, the light absorption performance of the materials
was carefully evaluated using a UV-Vis-NIR spectrophotometer. As shown in Figs. 4(a) and
4(b), the MWCNT@PSF–PSF composite membrane had a significantly lower diffuse
reflectance and transmission than the pure PSF membrane mainly owing to the excellent
intrinsic light absorption characteristic of the MWCNT. AFM was used to examine the surface
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roughness of the membranes. Owing to the introduction of the MWCNT, the composite
membrane exhibited a rougher top surface (Fig. S4) that was beneficial for multiple reflections
of the incident light, thus increasing light capture [35, 36]. Specifically, the light absorbance of
the composite membrane was approximately 89% that was calculated by the following equation:
Absorption (%) = 1 − reflectance (%) − transmittance (%) [37]. Owing to its high light-
harvesting capacity, the MWCNT@PSF–PSF composite membrane has the potential to achieve
efficient light-to-heat conversion. Therefore, the surface temperatures of the two samples were
tracked by infrared imaging under identical conditions (Fig. 4(c)). The average surface
temperature of the MWCNT@PSF–PSF membrane significantly increased from
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ambient temperature to 66.76 °C within 1 min, and finally stabilized at 68.51 °C after 30 min.
However, the surface temperature of the PSF membrane was elevated to only 32.11 °C within
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30 min. The faster heat response and higher equilibrium surface temperature indicated that the
as-prepared MWCNT@PSF–PSF composite membrane could be employed as a high-efficiency
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air heater. Meanwhile, the measured high thermal conductivity of 0.9347 W m-1 K-1 of the
composite membrane further ensured rapid and sufficient heat exchange between the membrane
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and the passing cold air.
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Fig. 4. (a) UV-Vis-NIR diffuse reflection and (b) transmission spectra of pure PSF and
MWCNT@PSF–PSF membranes. (c) Time-dependent surface temperature of the membranes
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Fig. 5. (a) Schematic shows the multifunctional photothermal composite membrane for efficient
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interfacial air heating and purification via ventilation mode. (b) Temperature differences
between the inlet and the permeate side of different membranes. The permeation flux is
controlled at 0.35 L/min, the area of membrane used is 50 cm2, the light intensity is set to 1 kW
m-2, and the inlet air temperature and permeate side temperature are measured in real-time by
thermometers. (c) Heating cold air performance of the photothermal composite membrane
under different permeate outlet flow rates. (d) Performance of the photothermal composite
membrane for long-term heating of cold air and intercepting PM 2.5. (e) SEM image and
corresponding EDX analyses of the upper surface of the composite membrane after intercepting
PM 2.5.
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The actual capacity of the membrane to heat cold air was tested online to reduce fossil fuel
energy consumption and accelerate clean energy heating. At the beginning of all the tests, the
air temperature at the inlet of the membrane was maintained relatively low and stable to more
closely reflect the heating performance of the membrane. As shown in Fig. S5(a), owing to the
excellent photothermal conversion characteristics of the MWCNT, the MWCNT@PSF–PSF
composite membrane exhibited remarkable cold-air heating performance. Specifically, the cold
air with an inlet temperature of 11.9 °C was rapidly heated; the air temperature at the permeate
side of the membrane reached 24 °C only after 3 min, and then increased further, reaching 31.3
°C after 15 min. For the blank PSF membrane, the air temperature slowly increased over 15
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min (Fig. S5(b)), and the temperature difference between the inlet and permeate sides gradually
decreased, whereas it increased for the composite membrane (Fig. 5(b)). Notably, the slight
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increase in the inlet air temperature in both cases may be attributed to the heating effect of the
simulated light source under light conditions. The heating performance of the MWCNT@PSF–
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PSF membrane under different airflow conditions was investigated (Figs. 5(c) and S6). As the
flow discharge increased, the average air temperature difference between the inlet and permeate
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sides of the membrane decreased. When the flow rate was set at 2.25 L/min, the permeate-side
temperature of the membrane could be rapidly increased to 21.3 °C after 12 min, maintaining
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harmful micropollutants, particularly during central heating in cold climatic regions, and haze
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weather seriously affects human life and health [38, 39]. Therefore, a test on the composite
membrane heating cold air while intercepting PM was performed. As a common model PM
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particle [40-42], NaCl nanoparticles were first fully mixed with cold air and then continuously
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supplied to the membrane. When the test began, the concentration of PM 2.5 at the inlet side of
the membrane was as high as 1744 μg/m3, whereas it immediately dropped to 11 μg/m3 at the
permeate side of the membrane, and the rejection efficiency exceeded 99%. During the
continuous test for 32 h, the rejection of the membrane remained at 93%-99%, and the PM 2.5
concentration on the permeate side of the membrane was always lower than 70 μg/m3 (Fig.
5(d)). This excellent rejection performance could be attributed to the nanopores in the skin layer
of the membrane that could effectively block micropollutants. As shown in the SEM image in
Fig. 5(e), the aggregated PM 2.5 particles (marked with yellow circles) were deposited on the
surface of the composite membrane. The elemental mapping analysis revealed the composition
of the retentate compared with that of the initial membrane, and the newly appearing Na and Cl
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elements indicated that the PM particles were effectively captured. No NaCl particles were
observed on the lower surface of the membrane, and no corresponding elements were identified
by energy dispersive X-ray spectroscopy (EDX) (Fig. S7). The real-time monitoring of the flux
on the permeate side of the membrane revealed that the rejected pollutants did not cause the
membrane flux to decrease that might be due to the abundant connected macrovoids and finger-
like pores in the membrane [43]. The flux was always maintained at approximately 1 L/min
during the test (Fig. S8). Under long-term illumination, the photothermal membrane
continuously converted light to heat. Thus, the air temperature on the permeate side persistently
increased at first and then tended to approach a stable value (nearly 50 °C). However, owing to
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the weak heat radiation loss, the inlet temperature increased only slightly.
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Fig. 6. Photographs of colony growth, using culture times between 24 h and 60 h, after (a)
ambient air directly contacted with agar plate and (b) clean hot air passing through the
membrane contacted with agar plate.
The antibacterial performance of the composite membrane under the operating conditions
was examined considering the adverse effects of airborne bacteria on human health. A pre-
sterilized container was simulated as an indoor space, and the air passing through the membrane
was continuously introduced into the container to ensure full contact with the clean agar plate
placed therein. After 8 h, the agar plate was removed and cultured in a constant temperature
incubator. Correspondingly, a control experiment was set up in which ambient air was directly
introduced into the container to contact the agar plate and then cultured under the same
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conditions. As shown in Fig. 6(a), colonies appeared in the control group with increasing culture
time, indicating that the ambient air contained harmful bacteria. In contrast, the bacteria were
effectively removed when air passed through the composite membrane and no evident colonies
were observed on the agar plate (Fig. 6(b)); this might be attributed to the size-sieving effect
and photothermal antibacterial ability of the composite membrane.
4. Conclusions
In summary, a convenient phase inversion method was employed to prepare multifunctional
carbon nanotube-based composite membranes for simultaneous cold air heating, ventilation,
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and purification, thus meeting the requirements of indoor thermal comfort and air quality. As
an excellent photothermal material incorporating specific microstructures, carbon nanotubes
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rapidly heated the oncoming cold air via highly efficient light absorption and thermal
conversion. Owing to the unique architecture formed by the nonsolvent-induced phase
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separation, the thin skin of the composite membrane intercepted PM 2.5 in the cold air via the
size-sieving effect, whereas the finger-shaped pores and macropores inside the membrane
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facilitated the heated air stream to pass through quickly. Consequently, the inlet cold air could
be heated to ca. 50 °C to further warm the indoor environment, maintaining the interception of
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PM 2.5 higher than 93%. Further antibacterial experiments demonstrated that the composite
membrane effectively removed airborne bacteria under the operating conditions. In addition,
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the reinforcement effects of carbon nanotubes enabled the lightweight membrane to have an
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excellent ultimate stress of 3.11 MPa. We anticipate that the obtained carbon nanotube-based
photothermal membrane will provide a sustainable and positive approach for improving indoor
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living quality.
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Data availability
Data will be made available on request.
Acknowledgements
This study was supported by the National Natural Science Foundation of China (No.
22205252), the Natural Science Foundation of Shandong Province (No. ZR2021QB111), the
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Taishan Scholars Program of Shandong Province (No. tstq20221151), and the Innovation
Funds of Shandong Energy Institute (SEI I202140).
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Declaration of interests
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☒ The authors declare that they have no known competing financial interests or personal
relationships that could have appeared to influence the work reported in this paper.
☐ The authors declare the following financial interests/personal relationships which may be
a
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