Cellulose-derived Carbon Aerogels Research Articles

Sustainable and low-cost cellulose aerogel-based absorber for solar steam generation

Solar steam generation is a promising technology for sustainable seawater desalination. However, its practical application is hindered by the low water evaporation rate and the high cost of materials. Carbon aerogels have demonstrated superior properties for clean water production through solar steam generation, but the complex and time-consuming preparation process inhibits their development and applications. In this study, high-performance solar steam absorbers based on cellulose-derived carbon aerogels were prepared from paper and waste paper using a simple green method. The fabricated carbon aerogels have a typical microporous structure (pore diameter: 20–250 µm), super-hydrophilic properties, good mechanical properties and efficient solar light absorption (∼96 %), which make them ideal for application in solar steam generation. Three different configurations based on cellulose and carbon aerogels were fabricated (bulk absorber, double-layer absorbers and ink-based absorber) to achieve the best design with high efficiency for steam generation. The surface temperature of the bulk absorber and dry double-layer absorbercan achieve 100 °C under 1 kWm−2irradiation. Among all configurations, the double-layer absorbers represented the highest efficiencies, 90.4 % for paper and 84.3 % for waste paper, under 1 kWm−2 irradiation, which are higher than most reported results. According to the results, the sustainable cellulose-based double-layer absorbers were promising materials for efficient solar steam generation due to their high hydrophilicity, high sunlight absorption, open porous structure, non-toxicity, biodegradability, availability and low cost.

MOF-Derived Co/C and MXene co-Decorated Cellulose-Derived Hybrid Carbon Aerogel with a Multi-Interface Architecture toward Absorption-Dominated Ultra-Efficient Electromagnetic Interference Shielding.

Exploring electromagnetic interference (EMI) shielding materials with ultra-efficient EMI shielding effectiveness (SE) and an absorption-dominated mechanism is urgently required for fundamentally tackling EMI radiation pollution. Herein, zeolitic imidazolate framework-67 (ZIF-67)/MXene/cellulose aerogels were first prepared via a simple solution mixing-regeneration and freeze-drying process. Subsequently, they are converted into electric/magnetic hybrid carbon aerogels (Co/C/MXene/cellulose-derived carbon aerogels) through a facile pyrolysis strategy. ZIF-67-derived porous Co/C could provide the additional magnetic loss capacity. The resultant electric/magnetic hybrid carbon aerogels exhibit a hierarchically porous structure, complementary electromagnetic waves (EMWs) loss mechanisms, and abundant heterointerfaces. The construction of a porous architecture and the synergy of electric/magnetic loss could greatly alleviate the impedance mismatching at the air-specimen interface, which enables more EMWs to enter into the materials for consumption. Moreover, numerous heterointerfaces among Co/C, Ti3C2Tx MXene, and cellulose-derived carbon skeleton induce the generation of multiple polarization losses containing interfacial and dipole polarization, which further dissipate the EMWs. The resultant electric/magnetic hybrid carbon aerogel with a low density (85.6 mg/cm3) achieves an ultrahigh EMI SE of 86.7 dB and a superior absorption coefficient of 0.72 simultaneously. This work not only offers a novel approach to design high-performance EMI shielding materials entailing low reflection characteristic but also broadens the applicability of electric/magnetic hybrid carbon aerogels in aerospace, precision electronic devices, and military stealth instruments.

Recent advances on the bacterial cellulose-derived carbon aerogels

This review summarizes the innovative strategies recently reported to exploit the applications of biomass-derived carbon aerogel conductors.

Synthesis of cellulose carbon aerogel via combined technology of wet ball-milling and TEMPO-mediated oxidation and its supersorption performance to ionic dyes

In this study, modified cellulose aerogels (CAs) were obtained via wet ball-milling and 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-mediated oxidation and were further applied to prepare cellulose-derived carbon aerogels (CCAs) by pyrolyzing. The results showed that the successive treatments by ball-milling and oxidation completely opened the CA fibers and converted them into plane or wrinkle structures. CCAs contained porous and graphite-like structures and its specific surface area reached up to 2825 m2/g. The maximum adsorption capacities of CCAs were 1078 mg/g for methylene blue (MB) and 644 mg/g for alizarin reds (ARS). The sorption of dyes occurred via hydrophobic partition, pore-filling, H-bonding, p/π-π electron donor–acceptor interactions. For the cationic MB, electrostatic attraction reinforced the sorption, while the electrostatic repulsion between the anionic ARS and CCAs was weakened by high salty. Besides, CCAs showed excellent salt tolerance. The present study provides an excellent CCA adsorbent by successive modification of ball-milling and oxidation of CAs.

Structuring Hierarchically Porous Architecture in Biomass-Derived Carbon Aerogels for Simultaneously Achieving High Electromagnetic Interference Shielding Effectiveness and High Absorption Coefficient.

Developing high-performance electromagnetic interference (EMI) shielding materials with high absorption coefficient is highly desired for eliminating the secondary pollution of reflected electromagnetic wave (EMW). Nevertheless, it has long been a daunting challenge to achieve high shielding effectiveness (SE) and ultralow or no reflection SE simultaneously. Herein, highly porous and conductive carbon nanotube (CNT)-based carbon aerogel with a meticulously designed hierarchically porous structure from micro and sub-micro to nano levels is developed by specific two-stage pyrolysis and potassium hydroxide activation processes. The resultant activated cellulose-derived carbon aerogels (a-CCAs) exhibit an ultrahigh EMI SE of 96.4 dB in the frequency range of 8.2-12.4 GHz in conjunction with an exceptionally high absorption coefficient of 0.79 at a low density of 30.5 mg cm-3. The successful construction of hierarchically porous structure is responsible for the excellent "structurally absorbing" ability of a-CCAs, and the introduction of CNT-based heterogeneous conductive network can effectively dissipate the incident EMWs by interfacial polarization and microcurrent losses. Moreover, the as-prepared a-CCAs have a water contact angle of as high as 158.3°and a sliding angle of as low as 5.3°, revealing their superhydrophobic feature. The ingenious structure design proposed here provides a possible pathway to overcome the conflict between high EMI shielding performance and ultralow or no secondary reflection, and the as-prepared a-CCAs are exceedingly promising in the application of telecommunication, microelectronics, and spacecraft.

Achieving enhanced electromagnetic shielding and absorption capacity of cellulose-derived carbon aerogels via tuning the carbonization temperature

A cellulose-derived carbon aerogel with enhanced electromagnetic shielding and absorption capacity was achieved simply by tuning the carbonization temperature.

Structuring dense three-dimensional sheet-like skeleton networks in biomass-derived carbon aerogels for efficient electromagnetic interference shielding

Developing ultralight, highly conductive carbon aerogels with facilely tunable microscopic structure is still a long-standing issue to effectively shield the electromagnetic interference (EMI). Here, highly porous and conductive all biomass-derived carbon aerogels were first successfully achieved by carbonizing cellulose aerogels, which held excellent structure designability by controlling cellulose content in lithium hydroxide/urea aqueous solution, porogen composition in solvent exchange process, as well as freezing rate during freeze-drying. The as-prepared cellulose-derived carbon aerogels with optimized structure of small pore size and dense three-dimensional sheet-like skeleton network were demonstrated to be highly efficient to greatly prolong the propagation path of electromagnetic waves (EMWs) and dissipate incident EMWs into heat energy, exhibiting the dominant EMI shielding mechanism of EMW absorption. As a result, an impressive EMI shielding effectiveness of as high as 93.1 dB in the X band frequency range at a density of as low as 0.079 g cm−3 was achieved. Of more practical significance is that the new insight into the relationship between microscopic pore structure of carbon aerogels and their EMI shielding performance provides a valuable clue in developing highly efficient EMI shielding carbon aerogels in the application of microelectronics, aircraft and spacecraft.

Carbon aerogels by pyrolysis of TEMPO-oxidized cellulose

Although carbon aerogels derived from naturally occurring materials have been developed extensively, a reasonable synthetic approach using cellulose-resource remains unclear. Here, we report a strategy to prepare carbon aerogels originated from cellulose position-selectively oxidized by TEMPO-oxidized process. Contrary to non-TEMPO-oxidized cellulose-derived carbon aerogels (NCCA) with relative loose structure, TEMPO-oxidized cellulose-derived carbon aerogels (TCCA) with tight fibrillar-continuous network are monitored, suggesting the importance of TEMPO-oxidized modification towards creating the architecture of subsequently produced carbon aerogels. TCCA endows a higher BET area despite owning slightly dense bulk density comparing with that of NCCA. The structural texture of TCCA could be maintained in a way in comparison to TEMPO-oxidized cellulose-derived aerogel, due to the integration and aggregation effect by losing the electric double layer repulsion via ionization of the surface carboxyl groups. FTIR and XPS analyses signify the evidence of non-functionalized carbon-skeleton network formation in terms of TCCA. Further, the mechanism concerning the creation of carbon aerogels is also established. These findings not only provide new insights into the production of carbon aerogels but also open up a new opportunity in the field of functional carbon materials.

In situ catalytic fast pyrolysis of crude and torrefied Eucalyptus globulus using carbon aerogel-supported catalysts

Nickel and iron supported on thermostable cellulose-derived carbon aerogels (CAG), were used for the catalytic fast pyrolysis (CFP) of crude and torrefied Eucalyptus globulus. Pyrolysis vapors produced from torrefied biomass under non-catalytic conditions were reduced by 70% in carboxylic acids with respect to vapors originating from crude biomass, but also were richer in ketones and aromatics. In the case of CFP of both crude and torrefied E.globulus on CAG-supported iron and nickel (Fe/CAG and Ni/CAG), the metallic clusters were activated for ketonization, while Ni0 provided additional hydrogenation sites, increasing the production of monoaromatics (c.a.18% selectivity), leading to a high acids-to-ketone (ξA-K = 1.3) and heavy-to-light (ξH-L = 1.0) ratios. Accordingly, Ni/CAG and Fe/CAG were more effective than HZSM-5 –a traditional cracking catalysts– for upgrading CFP vapors to light compounds. The combination of zeolite acid sites with the oxophilic Ni0 and Fe0 allows the deoxygenation of vapors while the ratio of polyaromatics to light aromatics (ξPAHs) was reduced by nearly 50%.

Synthesis and electromagnetic interference shielding of cellulose-derived carbon aerogels functionalized with α-Fe2O3 and polypyrrole

Eco-friendly cellulose-derived carbon aerogels (CDCA) were employed as porous substrate to integrate with α-Fe2O3 and polypyrrole (PPy) via pyrolysis and vapor-phase polymerization. The SEM and TEM observations present that the wrinkled PPy sheets and the α-Fe2O3 nanoparticles were well dispersed in CDCA. The strong interactions (such as hydrogen bonding) between the substrate and the nanomaterials were demonstrated by the FTIR and XPS analysis. When utilized as electromagnetic interference (EMI) shielding materials, the α-Fe2O3/PPy/CDCA (FPCA) composite has the highest total shielding effectiveness (SEtotal) of 39.4dB, about 2.0, 2.9, and 1.3 times that of the acid-treated CDCA (19.3dB), PPy (13.6dB), and α-Fe2O3/CDCA (29.3dB), respectively. Moreover, the shielding effectiveness due to absorption accounts for 78.2%–84.2% of SEtotal for FPCA, indicative of the absorption-dominant shielding mechanism contributing to alleviating secondary radiation. These features make the composite a useful alternative candidate for EMI shielding.

Homogeneous deposition of Ni(OH)2 onto cellulose-derived carbon aerogels for low-cost energy storage electrodes

The cellulose-derived carbon aerogel/Ni(OH)2 composites show good electrochemical performances.

Elucidating the role of ammonia-based salts on the preparation of cellulose-derived carbon aerogels

The effects of using (NH4)2SO4 as a carbonization promoter for producing cellulose-derived carbon aerogels (CAG) was studied. The effects of pretreatment on the textural, morphological, and chemical properties of pristine cellulose nanofibers (CNF) were analyzed through N2 adsorption, scanning electron microscopy (SEM), X-ray diffraction (XRD), elemental analysis, inductively coupled plasma optical emission spectrometry (ICP-OES), and Fourier transform infrared spectroscopy (FT-IR). Furthermore, the thermal behaviors of raw CNF and those impregnated with (NH4)2SO4 were investigated by coupling thermogravimetric analysis with mass spectrometry (TGA-MS). The results suggested that the pretreatment did not cause any morphological/structural changes in the nanofibers. However, the presence of (NH4)2SO4 affected their pyrolysis by favoring intermolecular dehydration, thereby reducing the formation of levoglucosan and increasing the carbon yield during pyrolysis. Interestingly, above certain impregnation level, the concentration of sulfate-derived species in the gas phase increased. This phenomenon was attributed to an excess of salt within the fiber structure and on their surfaces. Consequently, the levoglucosan-to-carbon route was inhibited, and the mechanisms of intra- and inter-molecular dehydration, chain scission, and crosslinking reactions were affected, leading to a reduced char yield. The chemical effects of ammonia-based salts is elucidated supported on the interpretation of MS signals and kinetic modeling results.

Functionalisation and chemical characterisation of cellulose-derived carbon aerogels

A series of nitrogen- and oxygen-functionalised carbon aerogels was produced from a carbon aerogel derived from cellulose acetate. Samples were oxidised by H2O2 or HNO3 and/or enriched in nitrogen by reaction with gaseous ammonia or co-heating of the carbon aerogel and melamine. Porosity variations and morphology were monitored using N2 adsorption and helium pycnometry. The surface chemistry was characterised by elemental analysis, FTIR and XPS spectroscopy, pH of the point of zero charge and acid/base titration. The prepared carbons are mainly mesoporous and show a moderate porosity development (SBET between 160 and 300m2/g). The applied chemical methods allow producing a wide range of functionalised carbon aerogels differing in terms of oxygen and nitrogen groups, their distribution and basicity. Both oxidation methods introduce a similar amount of oxygen, while the produced carbons differ in term of their acid/base character. Treatment with ammonia produces the most basic materials, which is partly due to the introduction of basic nitrogen groups, but also to the reduction of the acidic oxygen functionalities.