Nanoscale Pore Size Research Articles

Evaporation-driven 3D CNT scaffolding for composite reinforcement

The reinforcement of composites by carbon-nanotubes (CNTs) is typically limited by agglomeration and non-uniform dispersion. Thus, achieving a nanocomposite with high density of reinforcement material is a tough challenge. In this work, rather than mixing CNTs in a matrix, we first construct a dense CNT-network scaffold, and then impregnate it by the matrix to obtain a composite. To that end, we explore an evaporation-driven self-assembly approach to form 3D CNT scaffolds on quartz fibers, which combines high CNT density and nanoscale pore size with a straightforward, efficient process. The scaffold is thicker than the fiber by more than an order of magnitude, with a typical pore size of 70 nm and porosity of 60%. The strength of a scaffold-reinforced composite is evaluated by a fragmentation test. μCT 3D-reconstruction of the fragmented scaffold reveals that the matrix-impregnated scaffold creates a multiscale structure that under load behaves much like a fibrous composite. The fragmentation results are analyzed by a mechanical model, demonstrating a scaffold-composite strength of ∼200 MPa. The improved strength and relatively high CNT volume fraction (∼20%), along with the capability of tuning the scaffold thickness and density, make the proposed structure a promising prospect for composite reinforcement, as well as for diverse nanoscale applications.

Cytotoxicity and Cellular Uptake of 5-Fluorouracil Loaded Methylcellulose Nanohydrogel for Treatment of Oral Cancer

The objective of the study was to investigate the cytotoxicity and cellular uptake of prepared 5-Fluorouracil (5-FU) nano hydrogel formulation using KB oral cancer cell line and VERO fibroblast cell line. The biodegradable thermoresponsive modified methylcellulose (MMC) polymer was used for the preparation of nano hydrogel, whereas it shows a sol-gel phase transition at 36˚C to 40˚C. The physical crosslinking method was used, followed by probe sonication for the preparation of 5-FU loaded MMC nano hydrogel. The mechanism of crosslinking was studied by FT-IR and SEM. These experimental techniques explained physical crosslinking viz. H-bonding phenomenon with the interconnected porous structure of nanoscale pore size. Cytotoxicity assay in the concentration range from 1 µg/ml to 2000µg/ml shows an IC50 value at around 250µg/ml. This nano hydrogel shows concentration-dependent toxicity to the cancer cells while they were less toxic to normal fibroblast VERO cells. Cellular uptake was confirmed by the green fluorescence inside cells by Rhodamine-B conjugation using a fluorescent microscope. These results depict that 5-FU loaded thermosensitive nano hydrogel may be a promising candidate for intratumoral targeted drug delivery to cancer cells.

Pore size distributions contributed by OM, clay and other minerals in over-mature marine shale: A case study of the Longmaxi shale from Southeast Chongqing, China

Nano-scale pores play an important role in determining the adsorption capacity of shale gas. To quantitatively evaluate the pore size distributions contributed by organic matter (OM), clay and other minerals in an over-mature shale reservoir, the Lower Silurian Longmaxi shale from Southeast Chongqing was selected as a case study and was analyzed by the pore size distributions contributed by OM, clay and other minerals (PSDCOCO) method. Based on the results of total organic carbon (TOC), carbon element content in OM, X-ray diffraction (XRD) and low temperature nitrogen adsorption/desorption (LTNA) experiments, the pore size distributions contributed by a unit mass of OM, clay and other minerals were calculated and the differences between the results of the LTNA and PSDCOCO methods were determined for the four verified samples. The average value of the difference between the experimental and calculated pore volumes is 0.154 × 10−3 cm3/g. For the Longmaxi shale from the Py1 well, the contributions of OM and other minerals to the pore volume (pore width <200 nm) are primarily distributed in the pore width ranges from 2 to 20 nm and <2 nm, respectively. The nano-scale pore size distributions (<200 nm) contributed by the clay minerals have two relatively high peak values in the pore width ranges of 20–100 nm and 2–5 nm. The pore volumes for pore widths less than 200 nm contributed by a unit mass of OM, clay and other minerals were 115.776 × 10−3 cm3/g, 10.489 × 10−3 cm3/g and 0.006 × 10−3 cm3/g, respectively. In the shale reservoir, the contributions of OM, clay and other minerals to the pore volume with pore widths less than 200 nm were 45.75%, 54.17% and 0.08%, respectively, based on the limited data available.

Underoil Superhydrophilic Metal Felt Fabricated by Modifying Ultrathin Fumed Silica Coatings for the Separation of Water-in-Oil Emulsions.

Although various superhydrophobic/superoleophilic porous materials have been developed and successfully applied to separate water-in-oil emulsions through the size-sieving mechanism, the separation performance is restricted by their nanoscale pore size severely. In this study, the wettability of underoil water on fumed silica was experimentally observed, and the underlying mechanism was investigated by carrying out theoretical analysis and molecular dynamic (MD) simulations. Further, we present a novel, facile, and an inexpensive technique to fabricate an underoil superhydrophilic metal felt with microscale pores for the separation of water-in-oil emulsions using SiO2 nanoparticles (NPs) as building blocks. The as-prepared underoil superhydrophilic coating is closed-packed and ultrathin (the thickness is approximately hundreds of nanometers), as well as capable of being coated on a metal felt with complex structures without blocking its pores. The as-prepared metal felt could adsorb water droplets directly from oil, which endowed it with the ability to separate both surfactant-free and surfactant-stabilized water-in-oil emulsions with high separation efficiency up to 99.7% even though its pore size is larger than that of the emulsified droplet. The filtration flux for the separation of span 80-stabilized emulsion is up to ∼4000 L·m-2·h-1. Its separation performance is better than most of the other traditional membranes and superwettable materials used for the separation of water-in-oil emulsions. Moreover, the as-prepared metal felt retained outstanding separation performance even after 30 cycles of use, which demonstrated its excellent reusability and durability. Additionally, the distinctive wettability of underoil superhydrophilicity endued coated metal felt with superior antifouling properties toward crude oil. Overall, this study not only provides a new perspective on separating water-in-oil emulsions but also gives a universal approach to develop unique wettability surfaces.

3D pore system reconstruction using nano-scale 2D SEM images and pore size distribution analysis for intermediate rank coal matrix

This paper comprises the analysis of scanning electron microscopy (SEM) images, nuclear magnetic resonance (NMR) and mercury injection capillary pressure (MICP) data to quantify the pore distribution in coal matrix. We first generate the 3D pore system in the coal matrix based on the statistics of pore distribution obtained from 2D SEM images, and then extract the pore network using the maximal ball method. The influence of the reconstructed cube size and the 2D image resolution on the accuracy of the reconstructed 3D coal sample was analysed when generate the 3D digital coal smaple. It was observed that the highest resolution which was achieved for the studied samples (6 nm) resulted in the underestimation of porosity of the studied sample, and it is recommended for future to create several models with different resolution to find the most representative model, instead of apriori using the highest possible resolution. The extracted pore network was then used to analyse pore size distribution and perform capillary pressure simulation using pore network modeling. A comparison of the pore network analysis with NMR and measured MICP data demonstrated that the pore network extraction method simplified the results of distribution and underestimated the size of elongated pores and microfractures. The simulated and laboratory measured MICP shows significant difference partically bucease the network extraction method was not suitable for the studied samples and this could be overcomed by our future study of model MICP using direct simulation method in the reconstructed 3D model.

Toward Improved Optical Transparency of Polyimide Aerogels.

Highly translucent polyimide aerogels were prepared by combining equimolar amounts of pyromellitic dianhydride, 4,4'-hexafluoroisopropylidene di(phthalic anhydride) (6FDA), and 2,2'-dimethylbenzidine and cross-linking with 1,3,5-benzenetricarbonyl trichloride. A multivariable statistical design of experiments was used to perform a comparison study between three variables used to fabricate the aerogels: formulated repeat unit (n) of polyimide oligomers, 6FDA fraction of total dianhydride (0-50 mol %), and total polymer concentration in solution (7-10 wt %). Polymers with 25 mol % 6FDA in the backbone structure were found to produce polyimide aerogels with high optical transmission and low haze. These aerogels also possessed higher surface areas and very narrow nanoscale pore size distribution. Because of the decreased thermal conductivity with increasing amount of 6FDA in the backbone, these aerogels may find use where the combination of high optical transparency and thermal impedance is desired, such as insulated window panes. To this end, future efforts will focus on reducing the yellow color of the polyimide aerogels.

Polyimide aerogels with novel bimodal micro and nano porous structure assembly for airborne nano filtering applications.

Aerogels have presented a very high potential to be utilized as airborne nanoparticles' filtration media due to their nanoscale pore size and extremely high porosity. The filtering performance of aerogels, such as air permeability and filtration efficiency, is highly related to the configuration of aerogels' nanostructure assembly. However, as aerogel morphology is formed with respect to the intermolecular forces during the gelation stage, tailoring the aerogel nanostructure assembly is still a challenge. In this work, a novel strategy for tailoring polyimide aerogel nanostructure assembly is proposed by controlled disturbing of the intermolecular forces. From the results, the nanostructure assembly of the 4,4′-oxydianiline (ODA)–biphenyl-tetracarboxylic acid dianhydride (BPDA) polyimide aerogel is tailored to a uniform bimodal micro and nano porous structure. This was achieved by introducing the proper fraction of thermoplastic polyurethane (TPU) chains to the polyimide chains in the solution state and through a controlled process. The fabricated polyimide/TPU aerogels with bimodal morphology presented enhanced filtration performance, with 30% improved air permeability and reduced cell size of 3.51 nm over the conventional ODA–BPDA polyimide aerogels. Moreover, the fabricated bimodal aerogels present the reduced shrinkage, density, and effective thermal conductivity of 6.3% and 0.063 g cm−3, 28.7 mW m−1 K−1, respectively. Furthermore, the bimodal polyimide/TPU aerogels show the higher porosity of 96.5 vol% along with increased mechanical flexibility over the conventional polyimide aerogel with comparable backbone chemistry.

Laminated superwetting aerogel/membrane composite with large pore sizes for efficient separation of surfactant-stabilized water-in-oil emulsions

Although superwetting filtration membranes have been widely used, they suffer from the disadvantages of low flux and membrane fouling caused by the nanoscale pore size. Herein, a laminated cellulose aerogel/membrane composite with large pore size is fabricated via combining facile freeze-drying and hydrophobic modification using cellulose fibers as building blocks. An ultrathin silanization coating layer on cellulose fibers surface is constructed via directly coupling alkoxysilane and endows the composite with excellent superhydrophobicity (161°) and superoleophilicity (0°). Upon contact with a water-in-oil emulsion, the aerogel layer causes the micrometer-sized water droplets to coalesce. The coalesced water droplets are then repelled by the membrane layer with large pore size, achieving ultrafast gravity-driven separation with high separation efficiency (99.5%) and separation flux (12890 L m−2 h−1). Moreover, the composite exhibits ease to cycle and good usability. The outstanding performance of composite highlights its potential applications in the field of oil related industry.

NANOSCALE PORE SIZE DISTRIBUTION EFFECTS ON GAS PRODUCTION FROM FRACTAL SHALE ROCKS

Effect of nanoscale pore size distribution (PSD) on shale gas production is one of the challenges to be addressed by the industry. An improved approach to study multi-scale real gas transport in fractal shale rocks is proposed to bridge nanoscale PSD and gas filed production. This approach is well validated with field tests. Results indicate the gas production is underestimated without considering a nanoscale PSD. A PSD with a larger fractal dimension in pore size and variance yields a higher fraction of large pores; this leads to a better gas transport capacity; this is owing to a higher free gas transport ratio. A PSD with a smaller fractal dimension yields a lower cumulative gas production; this is because a smaller fractal dimension results in the reduction of gas transport efficiency. With an increase in the fractal dimension in pore size and variance, an apparent permeability-shifting effect is less obvious, and the sensitivity of this effect to a nanoscale PSD is also impaired. Higher fractal dimensions and variances result in higher cumulative gas production and a lower sensitivity of gas production to a nanoscale PSD, which is due to a better gas transport efficiency. The shale apparent permeability-shifting effect to nanoscale is more sensitive to a nanoscale PSD under a higher initial reservoir pressure, which makes gas production more sensitive to a nanoscale PSD. The findings of this study can help to better understand the influence of a nanoscale PSD on gas flow capacity and gas production.

Uso de las nuevas tecnologías para estimar la calidad de vida en lactantes con enfermedades infecciosas prevenibles o potencialmente prevenibles mediante vacunación

A hierarchical structure featuring both nano- and macro- structure has emerged as prospective candidates for the application requiring high flow rates and specific surface area. A unique physical and mechanical behavior could be discovered by designing a special structure. A random orientated nanoporous copper thin film coated on a three-dimensional (3D) microporous periodical octet-truss lattice was utilized as a hierarchical structure to evaluate the mechanical and catalytic behaviors. Nanoporous copper films with ligament size ranging from 16 to 28 nm were synthesized using magnetron co-sputtering CuAl alloy films and subsequent dealloying process, while the octet-truss with a pore size of 120 μm was fabricated by digital light processing. The yield strengths of the octet-truss lattice with nanoporous Cu (L-NPC) films are 3 times higher than those of low-density bulk Cu or Cu films predicted by the Gibson-Ashby equation. The current densities and electrochemical surface area of the l-NPC films are also 10 times higher than those of octet-truss lattice with solid Cu films or NPC films coating on a two-dimensional substrate. In addition to the nano-scale pore size effect, the 3D polymer structure produced a high curly surface for NPC films to attach on the truss which could be the reason for the different mechanical and electrochemical behaviors.

Fluorescence microscopy of biophysical protein dynamics in nanoporous hydrogels

Proteins within nanoporous hydrogels have important biotechnological applications in pharmaceutical purification, tissue engineering, water treatment, biosensors, and medical implants. Yet, oftentimes proteins that are functional in solution lose activity when in contact with soft, nanostructured, condensed phase materials due to perturbations in the folded state, conformation, diffusion, and adsorption dynamics of the protein by the material. Fluorescence microscopy experimentally measures the biophysical dynamics of proteins within hydrogels at the nanoscale and can overcome the limitations of conventional ensemble techniques. An explanation of the benefits of fluorescence is provided, and principles of fluorescence microscope instrumentation and analysis are discussed. Then several nanoscale fluorescence microscopies that image nanoscale protein dynamics within hydrogels are introduced. First, location-based super-resolution imaging resolves the adsorption kinetics of proteins to charged ligands within hydrogels used in pharmaceutical separations. Next, correlation-based super-resolution techniques image the heterogeneity of the nanoscale pore size of the hydrogels and the diffusion of analytes within the pores simultaneously. Finally, fluorescence resonance energy transfer imaging combined with temperature jump perturbations determines the folding and stability of a protein within hydrogels. A common finding with all three fluorescence microscopies is that heterogeneous nanoporous hydrogel materials cause variability of protein behavior dependent on gel sterics and/or interfacial electrostatic forces. Overall, in situ observations of proteins in hydrogels using fluorescence microscopies can inform and inspire soft nanomaterial design to improve the performance, shelf life, and cost of biomaterials.

ZnO nanoparticles coated mesh with switchable wettability for on-demand ultrafast separation of emulsified oil/water mixtures

Due to frequent discharge of oily wastewater and oils spill accident, oil/water separation has attracted worldwide attention. Nowadays, the on-demand separation of emulsified oil/water mixtures is urgent. Herein, the ZnO nanoparticles (NPs) coated mesh was prepared successfully by a simple spraying method. Reversible wettability conversion of the coated mesh between superhydrophobicity/superoleophilicity and superhydrophilicity/underwater superhydrophobicity was rapidly achieved by the alternation treated the coated mesh with stearic acid ethanol and NaOH solution for 15 min. Combined with the nanoscale pore size (smaller than the emulsion), the coated mesh could separate various kinds of emulsions whether water or oil is the continuous phase. Gravity is the only driving force for the entire separation process. The separation efficiency of emulsified oil/water mixtures was larger than 99.0%. Moreover, the coated mesh still showed high separation efficiency greater than 98.0% after 8 times cycle operations of wettability transition and separation, indicating a good stability and excellent recyclability. The developed ZnO NPs coated mesh should be a potential candidate for on-demand emulsions separation.

New results of Boda Claystone research: Genesis, mineralogy, geochemistry, petrophysics

Abstract Boda Claystone is a very tight clayey rock with extreme low porosity and permeability, nano-size pores and small amounts of swelling clays. Due to this character it is ideal as a potential host rock for research into the possibilities of high-level waste deposition in geological formation. Though the research started more than 30 years ago, the genesis, the geotectonic history of the Boda Claystone Formation (BCF) and the geology of surrounding areas has only been sketched out recently. On the basis of research of the past few years the process of sedimentation of different blocks was able to be reconstructed. Equipment and methodological developments were needed for the investigation of reservoir geological and hydrodynamic behaviour of this rock, which began in the early 2000s. Based on them the pore structure and reservoir could be characterized in detail. Only theoretical approaches were available for the chemical composition of free porewater. Traditional water-extracting methods were not adaptable because of excessively low porosity and nano-scale pore size distribution. Hence, new ways have to be found for getting enough water for analysis. These new results of BCF research help to prepare more sophisticated and directed experiments, in which there is a great interest internationally.

Probe material choice for nuclear magnetic resonance cryoporometry (NMRC) measurements of the nano-scale pore size distribution of unconventional reservoirs

Nuclear magnetic resonance cryoporometry is a newly developed technique that can characterize the pore size distribution of nano-scale porous materials. To date, this technique has scarcely been used for the testing of unconventional oil and gas reservoirs; thus, their micro- and nano-scale pore structures must still be investigated. The selection of the probe material for this technique has a key impact on the quality of the measurement results during the testing of geological samples. In this paper, we present details on the nuclear magnetic resonance cryoporometric procedure. Several types of probe materials were compared during the nuclear testing of standard nano-scale porous materials and unconventional reservoir geological samples from Sichuan Basin, Southwest China. Gas sorption experiments were also carried out on the same samples simultaneously. The KGT values of the probe materials octamethylcyclotetrasiloxane and calcium chloride hexahydrate were calibrated using standard nano-scale porous materials to reveal respective values of 149.3 Knm and 184 Knm. Water did not successfully wet the pore surfaces of the standard controlled pore glass samples; moreover, water damaged the pore structures of the geological samples, which was confirmed during two freeze-melting tests. The complex phase transition during the melting of cyclohexane introduced a nuclear magnetic resonance signal in addition to that from liquid in the pores, which led to an imprecise characterization of the pore size distribution. Octamethylcyclotetrasiloxane and calcium chloride hexahydrate have been rarely employed as nuclear magnetic resonance cryoporometric probe materials for the testing of an unconventional reservoir. Both of these materials were able to characterize pore sizes up to 1 μm, and they were more applicable than either water or cyclohexane.

Fabrication and adsorption performance for CO2 capture of advanced nanoporous microspheres enriched with amino acids

Advanced porous organic materials with high gas storage capacity and high selectivity have been rapidly developed for CO2 adsorbents in the recent decade, due to extremely high surface area and nanoscale pore size. Here, novel amino acids-incorporated solid adsorbents based on porous hypercrosslinked polymers were fabricated by a dispersion polymerization of an aromatic monomer and quaternary ammonium salt comonomer, subsequently a hypercrosslinked reaction and an ion-exchange step. The developed adsorbents presented mesopores structure with BET surface area up to 864 m2/g and an extremely high CO2 capturing capacity up to 60.7 wt% (13.8 mmol/g) at 273 K/1 bar. The results also showed the adsorbent had an excellent recycling ability over repetitive adsorption-desorption cycles. All the results suggest that the amino acids-modified porous sorbents are promising CO2 sorbents that can meet the challenges of the current CO2 capture and storage technology.

Carbon dioxide adsorption through carbon adsorbent structures: Effect of the porosity size, chemical potential and temperature

In the present paper, the carbon dioxide molecule adsorption through nanoporous carbons has been studied at 248 [K], 298 [K] and 323 [K]. The 3-stage graphite, turbostratic carbon and activated carbon have been taken into account as nanoporous carbon structures with nearly the same simulation box size, i.e. 30 × 30 × 30 [Å]. The numerical experiments of the adsorption phenomenon of CO2 molecule have been successfully achieved by user-written massively parallel codes via MPI paradigm which has been carefully examined and evaluated including electrostatic charges, 3-site CO2 molecule and linear scalability issues for the parallel programming purposes. By taking advantage of the parallel programming and efficient algorithm paradigm, very accurate outcomes and highly portable implementations for High Performance Computing (HPC) have been obtained. The effect of nanoscale pore size and its distribution for the above-mentioned nanoporous carbons which are generated via user-written C++ codes, have been studied by means of scalable parallel code. In the first stage, the carbon dioxide at bulk state has been investigated. Afterwards, the adsorption simulations have been achieved on regular and nearly regular nanoporous structures, i.e. 3-stage graphite including 6 [Å] and 12 [Å] interlayer distances (pore width), receptively. The activated carbon structure which is generated via Reverse Monte Carlo in Pikunic et al. (2003), has been considered for numerical experiments of adsorption as well. The comparison among these nanoporous carbons reveals a cross-over trend beyond a specific Adams constant value and this issue can be found out for the above-mentioned carbons as well as bulk case.

A Comparative Study on the Pore Size Distribution of Different Indian Shale Gas Reservoirs for Gas Production and Potential CO2 Sequestration

A thorough knowledge on pore size distribution (PSD) is one of the fundamental requirements for characterization of shale gas reservoirs and for accurate estimation of their gas storage potential. However, being an important future source of energy need in India, the pore size distribution of Indian shale gas systems is not scientifically well understood. In the present study, the nanoscale pore size distributions of prospective Indian shale basins, viz., Cambay, Cauvery, Krishna-Godavari (K-G), and Damodar valley (DV), were investigated using mercury injection porosimetry (MIP) and low-pressure gas adsorption (LP-N2 and LP-CO2) techniques. The study focused on identifying the priority basins for shale gas production which can be substituted for sequestration of CO2 based on their PSDs. The samples exhibited higher thermal maturity with increasing organic content. The chemical composition of the shale samples was inferred from XRD data, which depicted higher clay content. The prominent clay minerals ident...

Proton Conductive Channel Optimization in Methanol Resistive Hybrid Hyperbranched Polyamide Proton Exchange Membrane.

Based on a previously developed polyamide proton conductive macromolecule, the nano-scale structure of the self-assembled proton conductive channels (PCCs) is adjusted via enlarging the nano-scale pore size within the macromolecules. Hyperbranched polyamide macromolecules with different size are synthesized from different monomers to tune the nano-scale pore size within the macromolecules, and a series of hybrid membranes are prepared from these two micromoles to optimize the PCC structure in the proton exchange membrane. The optimized membrane exhibits methanol permeability low to 2.2 × 10−7 cm2/s, while the proton conductivity of the hybrid membrane can reach 0.25 S/cm at 80 °C, which was much higher than the value of the Nafion 117 membrane (0.192 S/cm). By considering the mechanical, dimensional, and the thermal properties, the hybrid hyperbranched polyamide proton exchange membrane (PEM) exhibits promising application potential in direct methanol fuel cells (DMFC).

Grand canonical Monte Carlo simulations of pore structure influence on methane adsorption in micro-porous carbons with applications to coal and shale systems

Coal and shale are strong heterogeneous anisotropic media involving nanoscale pore size and variance of microstructure. The complexity of methane adsorption is expressed both in diverse chemical properties and confined pore structures. In this study, Grand canonical Monte Carlo simulations were carried out to assess the influence of pore structure on methane adsorption at temperature 318 K, 333 K and pressure up to 20 MPa. The pore radii of physical carbon-based model range from 0.55 nm to 1.15 nm at the step of 0.1 nm. Simulated results indicate that the excess adsorption isotherms and maximum excess adsorption density are notably different for different pore structures. The triangle pore exhibits largest value of maximum excess adsorption density followed by the slit pore, circle pore and square pore. The maximum excess adsorption density is larger than 6 × 103 mol/m3 at simulated temperatures for triangle pore with pore radius less than 1 nm. The excess adsorption amount first increases with the increase of pressure and then decreases when the pressure is larger than 7.5 MPa for slit pore and 5 MPa for the circle pore, triangle pore and square pore. The excess adsorption amount for circle pore and square pore drops down to negative value when the pressure is larger than 12.5 MPa while the excess adsorption amount stays above zero across simulated pressure for the slit pore and triangle pore. The adsorption isotherms of micro-porous carbons were obtained by superposition of simulated adsorption isotherms based on the pore size distribution and were compared with coal samples experimental data gathered from the same temperature. The experimental isotherm is more close to slit pore excess isotherm and predicted excess isotherms based on circle pore and square pore under-estimate excess adsorption capacity.

Gravity-directed separation of both immiscible and emulsified oil/water mixtures utilizing coconut shell layer

Pressure-driven and lower flux of superwetting ultrafiltration membranes in various emulsions separation are long-standing issues and major barriers for their large-scale utilization. Even though currently reported membranes have achieved great success in emulsions separeation, they still suffer from low flux and complex fabrication process resulting from their smaller nanoscale pore size. Herein, utilizition of coconut shell as a novel biomaterial for developing into a layer through the simple smashing, cleaning and stacking procedures, which not only could avoid the complexity of film making process, but also could realize efficient gravity-directed separation of both immiscible oil/water mixtures and water-in-oil emulsions with high flux. Specifically, the layer acted as “water-removing” type filtrate material with excellent underwater superoleophobicity, exhibiting high efficiency for various immiscible oil/water mixtures separation and larger oil intrusion pressure. More importantly, the layer could also serve as adsorbent material with underoil superhydrophilicity, achieving gravity-directed kinds of water-in-oil emulsions separation with high separation efficiency (above 99.99%) and higher flux (above 1620L/m2h), even when their pore sizes are larger than that of emulsified droplets. We deeply believe that this study would open up a new strategy for both immiscible oil/water mixtures and water-in-oil emulsions separation.