Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “high loading”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

High-Fuel Loading Ignition Delay Time Characterization of Hydrogen/Natural Gas/Ammonia at Gas Turbine-Relevant Conditions Inside a High-Pressure Shock Tube

Abstract This study explores the combustion characterization of high-fuel percentage, air-diluted mixtures of H2 mixed with natural gas (NG) as well as mixtures of H2 and NH3 at temperatures and pressures relevant to turbine operating conditions (20–30 bar, 1000–1500 K). Lower temperatures (below 1070 K) exhibit preignition characteristics due to non-homogeneity. An attempt to mitigate these occurrences at high pressures is investigated using the constrained reaction volume (CRV) stage-filling technique. Due to the need to further refine the facility CRV stage-filling uncertainty, only higher temperature data will be interpreted at this time. The test conditions in this study closely replicate the temperatures, pressures, and mixtures that would be seen in hydrogen-powered gas turbines, making it the first to explore such conditions. The experimental IDTs were compared against the current state-of-the-art chemical kinetic models for mechanism validation. The current work will advance H2-powered turbines and aims to determine the optimum molecular ratio of H2 when mixed with natural gas.

Pierro, Michael↗
DOE OSTI2025

Enhanced Performance of Silicon Anodes through Hybrid Surface Engineering

Silicon (Si) is a promising anode material for nextgeneration lithium-ion batteries (LIBs) due to its high theoretical capacity. However, Si-containing anodes typically suffer from unacceptably short lives because of the unrestricted growth of the solid electrolyte interphase (SEI). Here, in this study, hybrid surface coatings are developed to stabilize the SEI in high loading pure Si anodes using atomic and molecular layer deposition. The coatings, consisting of LiF paired with lithicone, create an ionically conductive surface that enhances the capacity retention, rate performance, and longevity. Careful binder selection helps demonstrate the full utility of the coatings by enabling high loading electrodes to cycle continuously at current densities of 1200 mA/g Si . Uncoated controls, in comparison, fail within just 10 cycles at lower loadings. X-ray photoelectron spectroscopy and electrochemical impedance spectroscopy are used to provide supporting evidence of the coating composition and efficacy. The data indicate that our lithicone coating is converted to Li 2 CO 3 upon cycling contributing to favorable LiF/Li 2 CO 3 interfaces that enhance the space-charge effect at the active material’s surface. When applied to electrodes made with thermally stable binders and increasingly higher loadings (approaching 5 mAh/cm 2 ), ion transport through the bulk electrode, rather than SEI growth, is shown to be the limiting factor. Furthermore, data suggests a favorable interaction between lithicone precursors and poly(acrylic acid) binders mitigates thermal decomposition at higher temperatures. The work presented here represents the successful realization of composite coatings containing LiF/Li 2 CO 3 components to stabilize high-loading Si anodes. This work helps inform advanced surface engineering strategies to achieve highly reversible, high-capacity Si anodes capable of fast charging for high-performance LIBs.

atomic layer deposition↗
NASA NTRS2002

Miniature Reservoir Cathode: An Update

We report on recent work to produce a small low power, low cost reservoir cathode capable of long life (more than 100,000 hours) at high loading (> 5 A/sq cm). Our objective is a highly manufacturable, commercial device costing less than $30. Small highly loaded cathodes are needed, especially for millimeter wave tubes, where focusing becomes difficult when area convergence ratios are too high. We currently have 3 models ranging from .060-inch diameter to. 125-inch diameter. Reservoir type barium dispenser cathodes have a demonstrated capability for simultaneous high emission density and long life. Seven reservoir cathodes continue to operate on the cathode life test facility at NSWC, Crane, Indiana at 2 and 4 amps/sq cm. They have accumulated nearly 100,000 hours with practically no change in emission levels or knee temperature.

Vancil, Bernard K.↗
DOE OSTI2024

A High-Ceramic-Loading LATP–PVDF–Al 2 O 3 Composite Film for Lithium-Ion Batteries With Favorable Porous Microstructure and Enhanced Thermal Stability

A separator plays a crucial role in a Li-ion battery to carry liquid electrolytes while preventing short-circuiting between electrodes. Nevertheless, conventional commercial separators often exhibit poor wettability and are prone to shrink at elevated temperatures due to their limited thermal stability. Herein, we report a heat-resistant LATP–PVDF–Al 2 O 3 composite film with outstanding wetting performance. The thin film was prepared using ball mill mixing and tape-casting processes. Two solvents, NMP and glycerol, were applied to prepare the slurry, and a favorable microstructure in the film was created after drying. Here, the ionic conductivity of the film was tested at 1.39 mS cm –1 when paired with liquid electrolyte, almost double that of the commercial counterpart. The high ceramic loading of 70% improved both the thermal shrinkage resistance and dendrite inhibition of the membrane. When assembled in an NMC half-cell, the cycling capacity retentions of 92.8% and 92.1% are achieved after 50 cycles at 0.5 C and 1 C, demonstrating its capability to be used in Li-ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Synergistic Effect of High Sulfur Loading Layered Cathode, Ceramic Separator and Gel Electrolyte

Lithium sulfur (Li-S) batteries are promising candidates for next-generation energy storage devices as they are capable of providing higher energy density and lower cost in comparison to the state of the art Li-ion batteries. To gain these characteristics, there are challenges such as polysulfide crossover, large volume changes during cycling, and deposition of insulating lithium sulfide that need to be alleviated. A popular approach to address these issues is to control the structure and properties of the carbon cathode in order to influence the transport of polysulfides, surface area for reaction, and lithium sulfide deposition. Ceramic separators on the other hand can drastically affect ion diffusion and overall battery performance. Safety concerns regarding the flammable liquid electrolyte can be reduced by deploying gel electrolyte. Towards this direction, we developed a layer-on-layer cathode structure with sulfur-impregnated activated carbon alternating with graphene layer, which was fabricated by Air-assisted electrospray. A much higher sulfur loading compared to slurry cast cathodes can be provided in this method. Combining the new cathode with gel electrolyte can offer higher safety of the battery and capacity retention. Ceramic separator would compensate the reduced ion conductivity of the gel electrolyte and the combination of these variables will be very promising in improvement of battery performance and safety.

25 ENERGY STORAGE↗
DOE OSTI2025

Revisiting the Impact of Anion Selection on Sulfur Redox Reaction Kinetics for High Sulfur Loading Lithium–Sulfur Batteries

Lithium bis(trifluoromethane)sulfonimide (LiTFSI) is widely used in lithium–sulfur (Li–S) battery electrolytes due to its stability with lithium polysulfides (LiPSs) and moderate compatibility with lithium metal anodes. However, LiTFSI presents environmental concerns due to its association with per- and polyfluoroalkyl substances (PFAS), which are environmentally persistent and potentially toxic, raises sustainability concerns. This research also reveals that LiTFSI limits sulfur redox reactions (SRRs), making it less effective than other lithium salts. Additionally, some salts previously considered incompatible with Li-S systems due to their reactivity with LiPSs are demonstrated to perform effectively. For the first time, a protective, porous cathode electrolyte interphase (CEI) formed in situ through reactions between salt anions and LiPS is reported. The cells delivered a high specific capacity of 1230.8 mAh g −1 at 0.05 C with a sulfur loading of ≈6 mg cm −2 , limited lithium anode, maintaining a capacity retention of 76.2% after 100 cycles at 0.1 C. Under harsh conditions, such as high sulfur loading, lean electrolyte conditions (3 µL mg −1 ), and in anode-free cells, the cells continued to deliver outstanding capacity. This work provides valuable guidelines for understanding and selecting lithium salts to advance electrolyte design for Li–S batteries.

high loading batteries↗
DOE OSTI2026

Persistent Elevated Soot Emissions Induced by Clustered Stochastic Preignition Events

Stochastic Preignition (SPI) is an abnormal combustion phenomenon that can occur in spark-ignition engines particularly under high-load operation. SPI is characterized by uncontrolled initiation of combustion prior to spark discharge, an abnormal combustion process that can lead to severe knock events and significant engine damage. SPI has been associated with fuel properties, lubricant composition, and engine design and operation. Here, in this work, a single-cylinder test engine with a dry-sump oil system was utilized to study the SPI response of E10 and E25 fuels with a range of Reid Vapor Pressure (RVP). An automated test procedure was employed, consisting of ten square-waved load profile segments, with each segment composed of 5 min of low-load operation followed by 25 min of sustained high-load operation. These tests were replicated across multiple days of testing including a lubricant triple flush between tests, and an online Fuel in Oil diagnostic measurement. Exhaust particulate emissions were continuously measured by an AVL microsoot sensor (MSS). Elevated particulate matter emissions were observed to occur concurrently with SPI events as blooms of soot. Particularly after clustered events (i.e., multiple SPI cycles occurring within 10 consecutive engine cycles), high soot emissions were observed to persist over several days of sequential operation despite daily lubricant changes, a complete warm-up procedure, and sustained low-load operation between test segments. This result implies that the particulate emissions trends may be dominated by deposit-based effects, where higher load operation is needed to alter deposition and formation processes. The observed soot blooms were also found to correspond to a reduction in the engine fueling and the fuel engine oil dilution rate despite the engine exhaust remaining at stoichiometric exhaust operation. These observations suggest that post-SPI events, pathways for lubricant migration and consumption into the combustion chamber may occur until these pathways are closed from deposit formation or ring dynamics during extended operation. These observed sooting propensity persisted with all fuels tests, but a linear correlation was observed between the summation of soot and particulate matter index (PMI) value for each fuel as well as SPI events, proving that PMI is a crucial fuel property for reducing SPI.

Splitter, Derek [Oak Ridge National Laboratory (OR↗
NASA NTRS2015

Tribological Evaluation of Candidate Gear Materials Operating Under Light Loads in Highly Humid Conditions

A series of pin-on-disk sliding wear tests were undertaken to identify candidate materials for a pair of lightly loaded timing gears operating under highly humid conditions. The target application involves water purification and thus precludes the use of oil, grease and potentially toxic solid lubricants. The baseline sliding pair is austenitic stainless steel operating against a carbon filled polyimide. The test load and sliding speed (4.9N, 2.7ms) were chosen to represent average contact conditions of the meshing gear teeth. In addition to the baseline materials, the hard superelastic NiTiNOL 60 (60NiTi) was slid against itself, against the baseline polyimide, and against 60NiTi onto which a commercially deposited dry film lubricant (DFL) was applied. The alternate materials were evaluated as potential replacements to achieve a longer wear life and improved dimensional stability for the timing gear application. An attempt was also made to provide solid lubrication to self-mated 60NiTi by rubbing the polyimide against the disk wear track outside the primary 60NiTi-60NiTi contact, a method named stick or transfer-film lubrication. The selected test conditions gave repeatable friction and wear data and smooth sliding surfaces for the baseline materials similar to those in the target application. Friction and wear for self-mated stainless steel were high and erratic. Self-mated 60NiTi gave acceptably low friction (0.2) and modest wear but the sliding surfaces were rough and potentially unsuitable for the gear application. Tests in which 60NiTi pins were slid against DFL coated 60NiTi and DFL coated stainless steel gave low friction and long wear life. The use of stick lubrication via a secondary polyimide pin provided effective transfer film lubrication to self-mated 60NiTi tribological specimens. Using this approach, friction levels were equal or lower than the baseline polyimide-stainless combination and wear was higher but within data scatter observed in these preliminary tests. Based upon these results, self-mated 60NiTi gear teeth utilizing solid lubrication, is a reasonable approach for the target application.

tribology↗
NASA NTRS2015

Tribological Evaluation of Candidate Gear Materials Operating Under Light Loads in Highly Humid Conditions

A series of pin-on-disk sliding wear tests were undertaken to identify candidate materials for a pair of lightly loaded timing gears operating under highly humid conditions. The target application involves water purification and thus precludes the use of oil, grease and potentially toxic solid lubricants. The baseline sliding pair is austenitic stainless steel operating against a carbon filled polyimide. The test load and sliding speed (4.9 N, 2.7 m/s) were chosen to represent average contact conditions of the meshing gear teeth. In addition to the baseline materials, the hard superelastic NiTiNOL 60 (60NiTi) was slid against itself, against the baseline polyimide, and against 60NiTi onto which a commercially deposited dry film lubricant (DFL) was applied. The alternate materials were evaluated as potential replacements to achieve a longer wear life and improved dimensional stability for the timing gear application. An attempt was also made to provide solid lubrication to self-mated 60NiTi by rubbing the polyimide against the disk wear track outside the primary 60NiTi-60NiTi contact, a method named stick or transfer-film lubrication. The selected test conditions gave repeatable friction and wear data and smooth sliding surfaces for the baseline materials similar to those in the target application. Friction and wear for self-mated stainless steel were high and erratic. Self-mated 60NiTi gave acceptably low friction (approx. 0.2) and modest wear but the sliding surfaces were rough and potentially unsuitable for the gear application. Tests in which 60NiTi pins were slid against DFL coated 60NiTi and DFL coated stainless steel gave low friction and long wear life. The use of stick lubrication via the secondary polyimide pin provided effective transfer film lubrication to self-mated 60NiTi tribological specimens. Using this approach, friction levels were equal or lower than the baseline polyimide-stainless combination and wear was higher but within data scatter observed in these preliminary tests. Based upon these results, self-mated 60NiTi gear teeth utilizing solid lubrication, is a reasonable approach for the target application.

tribology↗
NASA NTRS1995

Factors in Daily Physical Activity Related to Calcaneal Mineral Density in Men

To determine the factors in daily physical activity that influence the mineral density of the calcaneus, we recorded walking steps and the type and duration of exercise in 43 healthy 26-to 51-yr-old men. Areal (g/sq cm) calcaneal bone mineral density (CBMD) was measured by single energy x-ray densitometry. Subjects walked a mean (+/- SD) of 7902(+/-2534) steps per day or approximately 3.9(+/-1.2) miles daily. Eight subjects reported no exercise activities. The remaining 35 subjects spent 143(2-772) (median and range) min/wk exercising. Twenty-eight men engaged in exercise activities that generate single leg peak vertical ground reaction forces (GRF(sub z)) of 2 or more body weights (high loaders, HL), and 15 reported exercise or daily activities that typically generate GRF(sub z) less than 1.5 body weights (low loaders, LL). CBMD was 12% higher in HL than LL (0.668 +/- 0.074 g/sq cm vs 0.597 +/- 0.062 g/sq cm, P less than 0.004). In the HL group, CBMD correlated to reported minutes of high load exercise (r = 0.41, P less than 0.03). CBMD was not related to the number of daily walking steps (N = 43, r = 0.03, NS). The results of this study support the concept that the dominant factor in daily physical activity relating to bone mineral density is the participation in site specific high loading activities, i.e., for the calcaneus, high calcaneal loads.

Hutchinson, Teresa M.↗
NASA NTRS1989

Static aeroelastic analysis and tailoring of missile control fins

A concept for enhancing the design of control fins for supersonic tactical missiles is described. The concept makes use of aeroelastic tailoring to create fin designs (for given planforms) that limit the variations in hinge moments that can occur during maneuvers involving high load factors and high angles of attack. It combines supersonic nonlinear aerodynamic load calculations with finite-element structural modeling, static and dynamic structural analysis, and optimization. The problem definition is illustrated. The fin is at least partly made up of a composite material. The layup is fixed, and the orientations of the material principal axes are allowed to vary; these are the design variables. The objective is the magnitude of the difference between the chordwise location of the center of pressure and its desired location, calculated for a given flight condition. Three types of constraints can be imposed: upper bounds on static displacements for a given set of load conditions, lower bounds on specified natural frequencies, and upper bounds on the critical flutter damping parameter at a given set of flight speeds and altitudes. The idea is to seek designs that reduce variations in hinge moments that would otherwise occur. The block diagram describes the operation of the computer program that accomplishes these tasks. There is an option for a single analysis in addition to the optimization.

Mcintosh, S. C., Jr.↗
DOE OSTI2022

Fuel Effects on Multimode Engine Operation (Sandia National Laboratories) (DOE VTO Annual Progress Report for FY21)

In total, light-duty vehicles in the United States travel on the order of 3 trillion miles annually, providing tremendous societal and personal benefits. However, the environmental burden is excessive, prompting Co-Optimization of Fuel and Engines (Co-Optima) program efforts to provide the science needed to increase engine efficiency and produce non-fossil fuels with reduced greenhouse gas emissions. Boosted spark-ignition (SI) engines provide high power density by offering high loads and engine speeds, making them light-weight and attractive for light-duty vehicles. Unfortunately, the engine efficiency drops off at lower loads and speeds, where the engine spends most time during typical driving. Multimode SI engines can use a more efficient advanced lean combustion mode at lower loads and speeds, while reverting to boosted SI under high-load conditions. Within Co-Optima, multiple advanced lean combustion modes have been explored; these include stratified-charge SI, pre-chamber lean SI, and advanced compression ignition (ACI) techniques such as spark-assisted compression ignition (SACI). For these combustion modes, focus has been on determining fuel properties that enable higher engine efficiency, clean and stable combustion, and effective exhaust aftertreatment. This report highlights recent efforts funded by the Vehicle Technologies Office at multiple National Laboratories that supported the multimode project in Co-Optima. It also includes a brief summary of biofuel production research funded by the Bioenergy Technologies Office.

33 ADVANCED PROPULSION SYSTEMS↗
NASA NTRSDate not supplied

Aerodynamic loss generation in a low-pressure turbine stage with high lift blading

The present work aims to investigate the loss generation mechanisms in a highly loaded low-pressure turbine (LPT) stage. The turbine employs high-lift airfoils to reduce the number of blades and therefore the overall engine weight. Large Eddy Simulation (LES) is applied to study the detailed flow fields at two representative Reynolds numbers (150,000 and 40,000). The calculated flow fields are compared with available measured data. LES calculates the measured aerodynamic performance of the current turbine stage well. Both the measurements and the CFD simulations indicate that most of the aerodynamic loss is generated by the development of secondary flows near the rotor hub. An area of low momentum and high aerodynamic loss forms at roughly 25 % span above the hub downstream of the rotor. Formation and migration of a vortex system near the hub is the primary source of the loss generation. The hub wall vortex system in this highly loaded turbine stage is quite different from the horse-shoe vortex system in a typical stationary turbine cascade. Calculated instantaneous and time-averaged flow fields at two Reynolds numbers are examined in detail to study Reynolds number effects on the turbine stage performance. Steady and unsteady flow separation on the rotor suction side is calculated at both high and low Reynolds numbers. At the lower Reynolds number of 40,000, thicker blade boundary layers increase the area of flow separation on the rotor suction side, resulting in a 1.9 % increase in aerodynamic loss compared to the higher Reynolds number case.

low pressure turbine↗
NASA NTRS1986

Unsteady design-point flow phenomena in transonic compressors

High-frequency response probes which had previously been used exclusively in the MIT Blowndown Facility were successfully employed in two conventional steady state axial flow compressor facilities to investigate the unsteady flowfields of highly loaded transonic compressors at design point operation. Laser anemometry measurements taken simultaneously with the high response data were also analyzed. The time averaged high response data of static and total pressure agreed quite well with the conventional steady state instrumentation except for flow angle which showed a large spread in values at all radii regardless of the type of instrumentation used. In addition, the time resolved measurements confirmed earlier test results obtained in the MIT Blowdown Facility for the same compressor. The results of these tests have further revealed that the flowfields of highly loaded transonic compressors are heavily influenced by unsteady flow phenomena. The high response measurements exhibited large variations in the blade to blade flow and in the blade passage flow. The observed unsteadiness in the blade wakes is explained in terms of the rotor blades' shed vorticity in periodic vortex streets. The wakes were modeled as two-dimensional vortex streets with finite size cores. The model fit the data quite well as it was able to reproduce the average wake shape and bi-modal probability density distributions seen in the laser anemometry data. The presence of vortex streets in the blade wakes also explains the large blade to blade fluctuations seen by the high response probes which is simply due to the intermittent sampling of the vortex street as it is swept past a stationary probe.

Gertz, J. B.↗
DOE OSTI2023

Scalable Hybrid Classification-Regression Solution for High-Frequency Nonintrusive Load Monitoring

Residential buildings with the ability to monitor and control their net-load (sum of load and generation) can provide valuable flexibility to power grid operators. We present a novel multiclass nonintrusive load monitoring (NILM) approach that enables effective net-load monitoring capabilities at high-frequency with minimal additional equipment and cost. The proposed machine learning based solution provides accurate multiclass state predictions while operating at a faster timescale (able to provide a prediction for each 60- Hz ac cycle used in US power grid) without relying on event-detection techniques. We also introduce an innovative hybrid classification-regression method that allows for the prediction of not only load on/off states but also individual load operating power levels. A test bed with eight residential appliances is used for validating the NILM approach. Results show that the overall method has high accuracy, good scaling and generalization properties.

feature extraction↗
DOE OSTI2020

Ultra-thermostable RNA nanoparticles for solubilizing and high-yield loading of paclitaxel for breast cancer therapy

Paclitaxel is widely used in cancer treatments, but poor water-solubility and toxicity raise serious concerns. Here we report an RNA four-way junction nanoparticle with ultra-thermodynamic stability to solubilize and load paclitaxel for targeted cancer therapy. Each RNA nanoparticle covalently loads twenty-four paclitaxel molecules as a prodrug. The RNA-paclitaxel complex is structurally rigid and stable, demonstrated by the sub-nanometer resolution imaging of cryo-EM. Using RNA nanoparticles as carriers increases the water-solubility of paclitaxel by 32,000-fold. Intravenous injections of RNA-paclitaxel nanoparticles with specific cancer-targeting ligand dramatically inhibit breast cancer growth, with nearly undetectable toxicity and immune responses in mice. No fatalities are observed at a paclitaxel dose equal to the reported LD 50 . The use of ultra-thermostable RNA nanoparticles to deliver chemical prodrugs addresses issues with RNA unfolding and nanoparticle dissociation after high-density drug loading. This finding provides a stable nano-platform for chemo-drug delivery as well as an efficient method to solubilize hydrophobic drugs.

60 APPLIED LIFE SCIENCES↗
NASA NTRS2017

Toward Understanding Tip Leakage Flows in Small Compressor Cores Including Stator Leakage Flow

The focus of this work was to provide additional data to supplement the work reported in NASA/CR-2015-218868 (Berdanier and Key, 2015b). The aim of that project was to characterize the fundamental flow physics and the overall performance effects due to increased rotor tip clearance heights in axial compressors. Data have been collected in the three-stage axial research compressor at Purdue University with a specific focus on analyzing the multistage effects resulting from the tip leakage flow. Three separate rotor tip clearances were studied with nominal tip clearance gaps of 1.5 percent, 3.0 percent, and 4.0 percent based on a constant annulus height. Overall compressor performance was previously investigated at four corrected speedlines (100 percent, 90 percent, 80 percent, and 68 percent) for each of the three tip clearance configurations. This study extends the previously published results to include detailed steady and time-resolved pressure data at two loading conditions, nominal loading (NL) and high loading (HL), on the 100 percent corrected speedline for the intermediate clearance level (3.0 percent). Steady detailed radial traverses of total pressure at the exit of each stator row are supported by flow visualization techniques to identify regions of flow recirculation and separation. Furthermore, detailed radial traverses of time-resolved total pressures at the exit of each rotor row have been measured with a fast-response pressure probe. These data were combined with existing three-component velocity measurements to identify a novel technique for calculating blockage in a multistage compressor. Time-resolved static pressure measurements have been collected over the rotor tips for all rotors with each of the three tip clearance configurations for up to five loading conditions along the 100 percent corrected speedline using fast-response piezoresistive pressure sensors. These time-resolved static pressure measurements reveal new knowledge about the trajectory of the tip leakage flow through the rotor passage. Further, these data extend previous measurements identifying a modulation of the tip leakage flow due to upstream stator wake propagation. Finally, a novel instrumentation technique has been implemented to measure pressures in the shrouded stator cavities. These data provide boundary conditions relating to the flow across the shrouded stator knife seal teeth. Moreover, the utilization of fast-response pressure sensors provides a new look at the time-resolved pressure field, leading to instantaneous differential pressures across the seal teeth. Ultimately, the data collected for this project represent a unique data set which contributes to build a better understanding of the tip leakage flow field and its associated loss mechanisms. These data will facilitate future engine design goals leading to small blade heights in the rear stages of high pressure compressors and aid in the development of new blade designs which are desensitized to the performance penalties attributed to rotor tip leakage flows.

Berdanier, Reid A.↗
DOE OSTI2021

General synthesis of single-atom catalysts with high metal loading using graphene quantum dots

Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO 2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗