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At least 55 records · Page 3

Automated processing of environmental transmission electron microscopy images for quantification of thin film dewetting and carbon nanotube nucleation dynamics

We report scalable production of carbon nanotubes (CNTs) requires catalysts and reaction conditions that provide high nucleation efficiency. In situ characterization methods such as environmental transmission electron microscopy (ETEM) can reveal fundamental mechanisms of synthesis, but to date have primarily provided qualitative observations on small sample sizes. Here, quantitative analysis is performed using high-resolution, high-rate video capture of ETEM experimentation coupled with automated image processing, involving computer vision algorithms and convolutional neural networks. By this approach, we detect distinct nanoparticle formation from an alumina-supported iron thin film and subsequent CNT nucleation from the nanoparticles. The statistical summary of particles in each video shows that, compared to a H 2 -only atmosphere, pretreatment of the catalyst with carbon added to the H 2 atmosphere results in a smaller average particle diameter, a 2-fold increase in particle density (to 5300 particles/μm 2 ), a 3-fold increase in CNT nucleation efficiency (to 92%), and more than a 5-fold increase in CNT density (to 4800/μm 2 ). Addition of carbon during exposure to H 2 is also more effective than NH 3 at dewetting the catalyst film and increasing the CNT nucleation efficiency, in spite of NH 3 being a stronger reducing agent for iron. Insights from this study are applicable to improving CNT yield and productivity in both batch-style and continuous processes.

25 ENERGY STORAGE↗

Competing conduction mechanisms in high performance carbon nanotube fibers

The performance of carbon nanotube (CNT) cables, a contender for copper-wire replacement, is tied to its metallic and semi-conducting-like conductivity responses with temperature; the origin of the semi-conducting-like response however is an underappreciated incongruity in literature. With controlled aspect-ratio and doping-degree, over 61 unique cryogenic experiments including anisotropy and Hall measurements, CNT cable performance is explored at extreme temperatures (65 mK) and magnetic-fields (60 T). A semi-conducting-like conductivity response with temperature becomes temperature-independent approaching absolute-zero, uniquely demonstrating for the first time the necessity of heterogeneous fluctuation induced tunneling; complete de-doping leads to localized hopping, contrasting graphite's pure metallic-like response. High-field magneto-resistance (including novel +22 % longitudinal magneto-resistance near room-temperature) is analyzed with hopping and classical two-band models, both yielding a similar parameter useful for conductor development. Varying field-orientation angle uncovers significant two- and four-fold symmetries that are shown to be from Aharonov-Bohm-like corrections to the curvature-induced bandgap, a first for macroscale CNT fibers. Tight-binding calculations using Green's Function formalism model the largest, coherent transport to-date in commensurate CNT bundles in magnetic-field, revealing non-uniform transmission across bundle cross-sections with doping restoring uniformity; independent of doping, transport in bundle-junction-bundle systems are predominantly from CNTs adjacent to the other bundle—demonstrating that smaller bundles are more efficient for electronic transport. The final impact is predicting the ultimate conductivity of heterogeneous CNT cables using temperature and field-dependent transport, surpassing conductivity of traditional metals.

36 MATERIALS SCIENCE↗

Enhancing carbon nanotube production from carbon dioxide and ethane using bimetallic catalysts

Converting CO 2 into carbon nanotubes (CNTs) offers a promising way for CO 2 utilization and sequestration, potentially mitigating environmental impacts from anthropogenic emissions. This study reports that bimetallic CoFe catalysts can increase CNT production from the reaction of CO 2 and C 2 H 6 by an order of magnitude compared to their monometallic counterparts. The active sites and CNT morphologies are composition-dependent: Co-rich catalysts (Co/Fe ratio ≥ 5) form stable face-centered cubic (fcc) CoFe alloys, producing cylindrical CNTs; Fe-containing catalysts (Co/Fe ≤ 2) favor body-centered cubic (bcc) CoFe alloy upon reduction, which transforms into carbides, resulting in bamboo-like CNTs. Experimental evidence and DFT calculations reveal that adjacent Fe and Co atoms modulate CO and C x H y adsorption, regulating CNT production pathways through the CO Boudouard reaction and C 2 H 6 decomposition. In conclusion, these results highlight the dual benefits of bimetallic catalysts in enhancing CNT yield and controlling CNT morphology through adjustment of catalyst compositions.

58 GEOSCIENCES↗

Development of multifunctional nylon 6,6-based nanocomposites with high electrical and thermal conductivities by scalable melt and dry blending methods for automotive applications

With the advent of intelligent automobile technology, the demand for multifunctional composites with higher electrical and thermal conductivities is increasing. We have herein reported for the first time the effect of polyolester on the dispersion of carbon nanotube (CNT) in the short-carbon fiber (CF)/nylon 6,6 (PA66) composite using a scalable melt-mixing and dry-blending method and its subsequent improvement in electrical and thermal conductivities. Masterbatches were prepared with a higher concentration of CNT (both untreated and polyolester-treated) followed by dry blended with reference composite (30 wt% CF and 10 wt% mineral fiber filled PA66) before making coupons via injection molding. A 500% and 63% improvements in electrical (3.14 S cm -1 ) and thermal conductivities (in-plane) (1.99 W m -1 K -1 ) conductivities were observed by adding 1.5 wt% treated CNT compared to the reference composite. The improvements were even higher than that of untreated CNT due to better dispersion. Furthermore, the electromagnetic shielding effectiveness reached 61 dB for 1.5 wt% treated CNT-filled composite (39% enhancement). In conclusion, these results are significant in imparting multiple functionalities to the automotive composite parts.

36 MATERIALS SCIENCE↗

Water-Assisted Proton Transport in Confined Nanochannels

Hydrated excess protons under hydrophobic confinement are a critical component of charge transport behavior and reactivity in nanoporous materials and biomolecular systems. In this study, excess proton confinement effects are computationally investigated for sub-2 nm hydrophobic nanopores by varying the diameters (d = 0.81, 0.95, 1.09, 1.22, 1.36, 1.63, and 1.90 nm), lengths (l ~3 and ~5 nm), curvature, and chirality of cylindrical carbon nanotube (CNT) nanopores. CNTs with a combination of different diameter segments are also explored. The spatial distribution of water molecules under confinement is diameter-dependent; however, proton solvation and transport are consistently found to occur in the water layer adjacent to the pore wall, showing an “amphiphilic” character of the hydrated excess proton hydronium-like structure. The proton transport free energy barrier also decreases significantly as the nanopore diameter increases and proton transport becomes almost barrierless in the d > 1 nm nanopores. Among the nanopores studied, the Zundel cation (H 5 O 2 + ) is populated only in the d = 0.95 nm CNT (7,7) nanopore. The presence of the hydrated excess proton and K + inside the CNT (7,7) nanopore induces a water density increase by 40 and 20%, respectively. The K + transport through CNT nanopores is also consistently higher in the free energy barrier than proton transport. Interestingly, the evolution of excess protonic charge defect distribution reveals a “frozen” single water wire configuration in the d = 0.81 nm CNT (6,6) nanopore (or segment), through which hydrated excess protons can only shuttle via the Grotthuss mechanism. Vehicular diffusion becomes relevant to proton transport in the “flat” free energy regions and in the wider nanopores, where protons do not primarily shuttle in the axial direction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomically Dispersed Iron–Nitrogen Sites on Hierarchically Mesoporous Carbon Nanotube and Graphene Nanoribbon Networks for CO 2 Reduction

Atomically dispersed metal and nitrogen co-doped carbon (M-N/C) catalysts hold great promise for electrochemical CO 2 conversion. However, there is a lack of cost-effective synthesis approaches to meet the goal of economic mass production of single-atom M-N/C with desirable carbon support architecture for efficient CO 2 reduction. Herein, we report facile transformation of commercial carbon nanotube (CNT) into isolated Fe-N 4 sites anchored on carbon nanotube and graphene nanoribbon (GNR) networks (Fe-N/CNT@GNR). The oxidization-induced partial unzipping of CNT results in the generation of GNR nanolayers attached to the remaining fibrous CNT frameworks, which reticulates a hierarchically mesoporous complex and thus enables a high electrochemical active surface area and smooth mass transport. The Fe residues originating from CNT growth seeds serve as Fe sources to form isolated Fe-N-4 moieties located at the CNT and GNR basal plane and edges with high intrinsic capability of activating CO 2 and suppressing hydrogen evolution. The Fe-N/CNT@GNR delivers a stable CO Faradaic efficiency of 96% with a partial current density of 22.6 mA cm -2 at a low overpotential of 650 mV, making it one of the most active M-N/C catalysts reported. This work presents an effective strategy to fabricate advanced atomistic catalysts and highlights the key roles of support architecture in single-atom electrocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synergistic Coupling Effect of Electronic Conductivity and Interphase Compatibility on High-Voltage Na 3 V 2 (PO 4 ) 2 F 3 Cathodes

Na 3 V 2 (PO 4 ) 2 F 3 (NVPF) has been considered an up-and-coming cathode material candidate for sodium (Na) ion batteries in light of its high specific capacity and working voltage. However, an erratic cathode/electrolyte interface layer is inevitably formed, accompanied by continuous electrolyte decomposition on the NVPF surface, when the voltage exceeds 4.2 V vs Na + /Na. Herein, the interphase features of NVPF are obviously enhanced owing to the ameliorated electronic conductivity obtained by combining it with carbon nanotubes (CNT). The NVPF with 3 wt % CNT (NVPF@3% CNT) reduces the Na + diffusion kinetic energy barrier and electron transport resistance. Furthermore, the conducting network formed by CNT with sturdy structure strength can promptly accommodate the volumetric changes during sequential Na + extraction/insertion and thus effectively improve the long-term cyclic performance of NVPF/hard carbon full cells. The initial discharge capacity approaches 105 mA h g –1 at 0.5C, and it retains 94% capacity retention after 200 cycles at the temperature of –10 °C. The cathode/electrolyte interphase characterization results further demonstrate that the interphase layer on the NVPF@3% CNT cathode is thinner and more compact compared with pristine samples. Here, this research provides a competitive strategy to facilitate the interfacial compatibility between the NVPF and electrolytes and accelerate the commercialization of high-performance Na-ion batteries.

25 ENERGY STORAGE↗

Spectroscopic signature of negative electronic compressibility from the Ti core-level of titanium carbonitride MXene

Two-dimensional transition metal carbides, carbonitrides, and nitrides called MXenes exhibit high metallic conductivity, ion intercalation capability and reversible redox activity, prompting their applications in energy storage and conversion, electromagnetic interference (EMI) shielding, and electronics, among many other fields. It has been shown that replacement of about 50% of carbon atoms in the most popular MXene family member, titanium carbide (Ti 3 C 2 T x ), by nitrogen atoms, forming titanium carbonitride (Ti 3 CNT x ), leads to drastically different properties, such as very high negative charge in solution and extreme EMI shielding effectiveness, exceeding all known materials, even metals at comparable thicknesses. Here, by using ultraviolet photoemission spectroscopy (UPS), the electronic structures of Ti 3 CNT x and Ti 3 C 2 T x are systematically investigated and compared as a function of charge carrier density. We observe that, in contrast to Ti 3 C 2 T x , the Ti 3p core-level of Ti 3 CNT x exhibits a counterintuitive shift to a lower binding energy of up to approximately 250 meV upon increasing the electron density, which is a spectroscopic signature of negative electronic compressibility (NEC). These experimentally measured chemical potential shifts are well-captured by the density functional theory (DFT) calculation. The DFT results also further suggest that the hybridization of titanium-nitrogen bonding in Ti 3 CNT x helps promoting the available states of Ti atoms for receiving more electron above the Fermi level and leads to the observed NEC. Furthermore, our findings explain the differences in electronic properties between the two very important and widely studied MXenes and also suggest a new strategy to apply the NEC effect of Ti 3 CNT x in energy and charge storage applications.

2D materials↗

Field emission microscopy of carbon nanotube fibers: Evaluating and interpreting spatial emission

In this work, the authors quantify field emission properties of cathodes made from carbon nanotube (CNT) fibers. The cathodes were arranged in different configurations to determine the effect of cathode geometry on the emission properties. Various geometries were investigated including (1) flat cut fiber tip, (2) folded fiber, (3) looped fiber, and (4) fibers wound around a cylinder. The authors employ a custom field emission microscope to quantify I-V characteristics in combination with laterally resolved field-dependent electron emission area. Additionally, they look at the very early emission stages, first when a CNT fiber is turned on for the first time, which is then followed by multiple ramp-up/down runs. Upon the first turn on, all fibers demonstrated limited and discrete emission area. During ramping runs, all CNT fibers underwent multiple (minor and/or major) breakdowns, which improved emission properties in that turn-on field decreased and field enhancement factor and emission area both increased. It is proposed that breakdowns are responsible for removing initially undesirable emission sites caused by stray fibers higher than average. This initial breakdown process gives way to a larger emission area that is created when the CNT fiber subcomponents unfold and align with the electric field. Overall, the authors' results form the basis for careful evaluation of CNT fiber cathodes for dc or low frequency pulsed power systems in which large uniform area emission is required or for narrow beam high frequency applications in which high brightness is a must.

Image processing↗

Customization for Current Market Applications of the Carbon Nanotubes Produced by PNNL’s Regenerable Catalytic Pyrolysis (ReCaP) for Scaled Hydrogen Production

Here, we demonstrated the Regenerative Catalytic Pyrolysis (ReCaP) process that generates carbon dioxide-free hydrogen (CO 2 -free H 2 ) from inexpensive and domestically abundant natural gas (NG), while simultaneously producing H 2 at net production cost of $1.0/kg through the sale of valuable carbon nanotube (CNT) co-product. The specific goal of this project is to 1) scale up the production of CNT, 2) correlate the properties of the CNT with the reaction conditions, 3) perform a techno-economic analysis to obtain minimum selling price of H 2 and CNT, and 4) identify industrial partners interested in the CNT co-product.

03 NATURAL GAS↗

Development of a self-lubricating high-efficiency hybrid seal composed of carbon nanotube-coated metal meshes for CSP turbomachinery (SETO CPS #36333 Final Report)

In turbomachinery, internal leakage flow accounts for up to 3% of the total thermodynamic cycle energy loss. Tradeoff must be made between the sealing efficiency (smaller clearance) and the friction and wear issues for interfering with the shaft (larger clearance). This ORNL-Danfoss joint effort developed a novel hybrid seal composed of carbon nanotube (CNT)-coated metal meshes. The CNT growth process was based on a self-catalyzing chemical vapor deposition and these multiwall CNTs were well aligned with high crystallinity. This hybrid material structure takes advantage of the CNT’s low-friction nature and uses the metal mesh as an extendable backbone. Full-scale experimental seals were designed, fabricated, and optimized for sealing performance and durability. The CNT-coated metal mesh seal demonstrated superior gas sealing efficiency to the baseline labyrinth seal and significantly improved shaft surface protection compared with the state-of-the-art superalloy brush seal on the static rig and full-scale compressor dynamometer tests. The CNT-metal mesh seal is low-cost and scalable and can potentially benefit wide applications, including CSP and other power generation, marine, automotive, and HVAC.

36 MATERIALS SCIENCE↗

Enhancing the Electrode Gravimetric Capacity of Li 1.2 Mn 0.4 Ti 0.4 O 2 Cathode Using Interfacial Carbon Deposition and Carbon Nanotube-Mediated Electrical Percolation

Mn-based cation disordered rocksalt oxides (Mn-DRX) are emerging as promising cathode materials for next-generation Li-ion batteries due to their high specific capacities and cobalt and nickel free characteristic. However, to reach the theoretical capacity, solid-state method synthesized Mn-DRX materials require activation via post-synthetic ball milling, typically incorporating more than 20 wt.% conductive carbon that adversely reduces the electrode level gravimetric capacity. To solve this issue, we firstly deposit amorphous carbon on the surface of the Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO) particles to increase the electrical conductivity by a five order of magnitude. Although the cathode material gravimetric first charge capacity reaches 180 mAh/g, its highly irreversible behavior leads to a 70 mAh/g first discharge capacity. Subsequently, to ensure a good electrical percolation network, the LMTO material is ball milled with multi-wall carbon nanotube (CNT) to obtain a 78.7 wt.% LMTO active material loading in the cathode electrode (LMTO-CNT). As a result, a 210 mAh/g cathode electrode gravimetric first charge and 165 mAh/g first discharge capacity are obtained, compared to the respective capacity values of 222 mAh/g and 155 mAh/g for the LMTO ball milled with 20 wt.% SuperP C65 electrode (LMTO-SP). After 50 cycles, the LMTO-CNT delivers a 121 mAh/g electrode gravimetric discharge capacity, largely outperforming the 44 mAh/g value of the LMTO-SP. In conclusion, our study demonstrates that while ball milling is necessary to achieve the theoretical capacity of LMTO, a careful selection of the additive, such as CNT, effectively reduces the required carbon quantity to achieve a higher electrode gravimetric discharge capacity.

25 ENERGY STORAGE↗

Multilayered Cu-Carbon Nanotube Composites for Advanced Conductors

Improving the efficiency of electrical components is critical in reducing energy consumption for various industrial and residential applications, ranging from rotating machinery to all electric devices and electric vehicle (EV) components to power grid systems. Substituting Cu wires with reduced resistance conductors that incorporate carbon nanotubes (CNTs) into Cu─ultraconductive Cu (UCC) composites─has recently been considered a promising strategy to improve energy efficiency, power density, and/or performance across various applications. Here, in this study, we created stable material formulations [CNT-containing polyvinylpyrrolidone (PVP) in dimethylformamide (DMF) solution] and utilized commercially viable fabrication approaches (electrospinning and magnetron sputtering) that produced high-performance multilayered tape-based UCC composite architectures. Increasing the CNT volume fraction by sequential layering of the structure with additional Cu-CNT layers showed a nearly stepwise improved performance in electrical and mechanical properties. This study also provides valuable insight into the effectiveness of nitrogen doping in modifying the conductivity of the CNT matrix. Fabricated prototypes demonstrated a >10% increase in current carrying capacity and >10% improvement in mechanical strength compared to those obtained on pure Cu. We believe that the properties demonstrated here, combined with the scalable manufacturing pathway of our approach, pave the way in designing future advanced conductors for diverse energy efficient and high-performance electrical systems and applications.

Carbon nanotubes↗

Activation of Transition Metal (Fe, Co and Ni)-Oxide Nanoclusters by Nitrogen Defects in Carbon Nanotube for Selective CO 2 Reduction Reaction

The electrochemical carbon dioxide reduction reaction (CO2RR), which can produce value-added chemical feedstocks, is a proton-coupled-electron process with sluggish kinetics. Thus, highly efficient, cheap catalysts are urgently required. Transition metal oxides such as CoO x , FeO x , and NiO x are low-cost, low toxicity, and abundant materials for a wide range of electrochemical reactions, but are almost inert for CO 2 RR. Here, we report for the first time that nitrogen doped carbon nanotubes (N-CNT) have a surprising activation effect on the activity and selectivity of transition metal-oxide (MO x where M = Fe, Ni, and Co) nanoclusters for CO 2 RR. MO x supported on N-CNT, MOx/N-CNT, achieves a CO yield of 2.6–2.8 mmol cm -2 min -1 at an overpotential of -0.55V, which is two orders of magnitude higher than MO x supported on acid treated CNTs (MOx/O-CNT) and four times higher than pristine N-CNT. The faraday efficiency for electrochemical CO 2 -to-CO conversion is as high as 90.3% at overpotential of 0.44V. Both in-situ XAS measurements and DFT calculations disclose that MO x nanoclusters can be hydrated in CO 2 saturated KHCO 3 , and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions, which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.

36 MATERIALS SCIENCE↗

Monolayer Films of Binary Metal Oxide Nanoparticles for Carbon Nanotube Synthesis

Binary metal oxide nanoparticles (biMO-NPs) combining transition and main-group metals with well-organized atomic architectures have unique potential as robust and economical heterogeneous catalysts. Herein, metal oxide nanoparticles (CoAlxOy) using cobalt and aluminum were synthesized, and their structure, morphology, and chemical composition were investigated using various characterization techniques. The biMO-NPs, which had a Gaussian-type size distribution (∼6 nm), were assembled on plain silicon substrates modified chemically with linker molecules bearing suitable end groups. Surface analysis revealed an ordered, uniform, close-packed arrangement of biMO-NPs forming a monolayer architecture with nanoscale thickness (∼12 nm), high surface uniformity, and negligible defects. The nanoparticle monolayer film (NP-MF) was employed as a catalyst to grow carbon nanotube (CNT) forests via the thermal chemical vapor deposition (CVD) method, similar to those grown from catalyst thin films deposited by physical vapor deposition. Structural characterization confirmed the growth of a dense, uniform, high-quality vertically aligned carbon nanotube (VA-CNT) forest with a length of ∼125 µm, which is comparable to the VA-CNTs grown from expensive thin films. Thus, CNT growth was successfully catalyzed by the biMO-NPs, highlighting a simple and inexpensive alternative for catalyst deposition. In this innovative wet-chemistry approach, the catalyst and catalyst support are combined within a single nanoparticle before NP-MF assembly. Interestingly, this approach provides a scalable and cost-effective pathway for CNT growth, eliminating the need for expensive thin deposition techniques.

Regmi, Bishow [University of Cincinnati]↗

Evaluating the Lightning Strike Damage Tolerance for CFRP Composite Laminates Containing Conductive Nanofillers

Conductive nanofillers, such as carbon nanotube, graphene nanoplatelets, and carbon black particles (with diameters in nanometers) have been shown to enhance the electrical conductivity of fiber reinforced polymer matrix composites in many existing studies. The motivation is primarily for lightning strike protection, electromagnetic interference shielding, de-icing, and the manufacturing of lightweight electronic components. Here, we evaluate the lightning strike damage tolerance of carbon fiber reinforced polymer (CFRP) matrix composite laminates containing conductive nanofillers with varying weight fractions, including carbon black (CB), carbon nanotubes (CNT), and a mix of CB and CNT, through simulated lightning strike tests, followed by both non-destructive ultrasonic inspection and destructive sectioning to characterize the damage inflicted by the simulated lightning strike. Three-point flexural tests are performed to evaluate the residual strength retained by all CFRP specimens. Results show that lightning strike damage experienced varying levels of reduction for CFRP composite specimens containing conductive fillers in comparison to the baseline specimen without fillers. Notably, the delamination only penetrated to the interface between the 1st and 2nd layer for the specimen with 0.25 wt.% CNT in comparison to the baseline CFRP specimen for which the delamination penetrated to the interface between the 5th and 6th layer. Moreover, the retention of the flexural modulus increased from 26.5% to a maximum of 95.0% for the specimen with 0.25 wt.% hybrid CB and CNT. Yet, we show that using our chosen conductive fillers cannot fully eliminate lightning strike damage. Additionally, adding conductive fillers could compromise the flexural properties. We provide discussions on future recommendations on using conductive fillers for the lightning strike protection of CFRP composites.

36 MATERIALS SCIENCE↗

Ultra-selective membrane composed of charge-stabilized fixed carrier and amino acid-based ionic liquid mobile carrier for highly efficient carbon capture

Membrane technology has been extensively studied for CO 2 capture applications, especially for flue gas sources. In the past decades, facilitated transport membranes (FTMs) have made breakthroughs overcoming the permeance-selectivity trade-off upper bound restricting traditional CO 2 separation membranes, but are still facing challenges towards practical applications, including limited performance, such as insufficient CO 2 /N 2 selectivity to achieve 95 % CO 2 dry-base purity by one step separation, and long-term stability. Herein, we designed and fabricated a novel FTM structure containing an ionic liquid (1-ethyl-3-methylimidazolium aminoacetate, [Emim][Gly]) as mobile CO 2 -carrier and a polymeric amine (polyethyleneimine, PEI) as fixed CO 2 -carrier. In this study, the fixed carrier is confined within a carbon nanotube (CNT) framework of 230 nm thickness via electrostatic forces adjusted by a polyelectrolyte (polystyrene sulfonate, PSS), while the mobile carrier diffuses freely within the CNT framework. After optimization of the membrane recipe and spray-coating fabrication procedure, following our previous work, the resulting CNT-PSS-PEI ~ IL membranes demonstrated an ultra-high CO 2 /N 2 selectivity up to 1,000 with CO 2 permeance up to 2,400 GPU (Gas Permeation Unit, 1 GPU = 3.348 × 10 -10 mol·s -1 ·m -2 ·Pa -1 ) under vacuum operation condition. Furthermore, one 100-cm 2 flat sheet membrane sample was prepared and exhibited one-stage CO 2 enrichment from 15 % to 95 % purity (dry-base) for the first time amongst all reported CO 2 separation membranes. The membrane retained a stable performance over 50-h operation period under vacuum condition. The extraordinary CO 2 separation performance illustrates the great potential of the CNT-PSS-PEI ~ IL membranes for flue gas carbon capture application.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Favorable morphology and electronic conductivity of functional sublayers for highly efficient water splitting electrodes

Low electronic conductivities and improper morphologies of anode electrodes greatly limit the reaction area, catalyst utilization and efficiency in proton exchange membrane water electrolyzers. In this study, conductive sublayers with different conductivities and morphologies were introduced into anode electrodes in membrane-based water electrolyzers. In-situ and ex-situ investigation results showed that conductive sublayers (Au mesh and carbon nanotube (CNT) film) augmented the sheet conductivity of anode electrodes by up to 4000 times (from 2000 to 0.5 ohm square -1 ), and the ohmic resistance of water electrolyzers was reduced to 1/3 when inserting conductive sublayers. In addition, CNT film provided a higher electrochemical active area than Au mesh, because of favorable morphologies (large porosity and surface area) of CNT fibers on CNT films. Therefore, the current density of water splitting was increased by 3 times (from 4.55 mA cm -2 to 14.83 mA cm -2 ) at 2.5 V compared to a conventional anode electrode. Visualizations on bubble dynamics showed improved performances with conductive sublayers; this was mainly due to greatly increased number of reaction sites, highly spread reaction area (from 50 to 1000 um), and reduced activation overpotential. Therefore, a balance between high electronic conductivity and nanoporous morphology is essential to the anode electrode for larger reaction sites and areas in highly efficient water electrolyzers.

25 ENERGY STORAGE↗