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All sourcesNASA NTRSDOE OSTI
NASA NTRS2004

Analysis of TRMM Microphysical Measurements: Tropical Rainfall Measuring Mission (TRMM)

SPEC Incorporated participated in three of the four TRMM field campaigns (TEFLUN-A, TEFLUN-B and KWAJEX), installing and operating a cloud particle imager (CPI) and a high volume precipitation spectrometer (HVPS) on the SPEC Learjet in TEFLUN-A, the University of North Dakota Citation in TEFLUN-B and KWAJEX, and a CPI on the NASA DC-8 in KWAJEX. This report presents and discusses new software tools and algorithms that were developed to analyze microphysical data collected during these field campaigns, as well as scientific interpretations of the data themselves. Software algorithms were developed to improve the analysis of microphysical measurements collected by the TRMM aircraft during the field campaigns. Particular attention was paid to developing and/or improving algorithms used to compute particle size distributions and ice water content. Software was also developed in support of production of the TRMM Common Microphysical Product (CMP) data files. CMP data files for TEFLUN-A field campaign were produced and submitted to the DAAC. Typical microphysical properties of convective and stratiform regions from TEFLUN-A and KWAJEX clouds were produced. In general, it was found that in the upper cloud region near -20 to -25 C, stratiform clouds contain very high (greater than 1 per cubic centimeter) concentrations of small ice particles, which are suspected to be a residual from homogeneous freezing and sedimentation of small drops in a convective updraft. In the upper cloud region near -20 to -25 C, convective clouds contain aggregates, which are not found lower in the cloud. Stratiform clouds contain aggregates at all levels, with the majority in the lowest levels. Convective cloud regions contain much higher LWC and drop concentrations than stratiform regions at all levels, and higher LWC in the middle and upper regions. Stratiform clouds contain higher IWC than convective clouds only at the lowest level. Irregular shaped ice particles are found in very high concentrations throughout both convective and stratiform cloud regions. A striking difference in particle shape in cirrus formed in situ, cirrus formed from maritime anvils and cirrus formed from continental anvils. Over 50% of the mass of in situ cirrus ice particles is composed of bullet rosettes, while bullet rosettes are virtually non-existent in maritime and tropical anvils. Tropical anvils are composed of mostly singular, plates, capped columns, and blocky irregular shapes, while continental anvils have a much higher percentage of aggregates, some of which are chains of small spheroidal particles that appear to result from homogeneous freezing of drops. A correlation between high electric fields in continental anvils and the formation of aggregates is hypothesized.

Source record↗
DOE OSTI2021

Revising the Role of Cortical Cytoskeleton during Secretion: Actin and Myosin XI Function in Vesicle Tethering

In plants, secretion of cell wall components and membrane proteins plays a fundamental role in growth and development as well as survival in diverse environments. Exocytosis, as the last step of the secretory trafficking pathway, is a highly ordered and precisely controlled process involving tethering, docking, and fusion of vesicles at the plasma membrane (PM) for cargo delivery. Although the exocytic process and machinery are well characterized in yeast and animal models, the molecular players and specific molecular events that underpin late stages of exocytosis in plant cells remain largely unknown. Here, by using the delivery of functional, fluorescent-tagged cellulose synthase (CESA) complexes (CSCs) to the PM as a model system for secretion, as well as single-particle tracking in living cells, we describe a quantitative approach for measuring the frequency of vesicle tethering events. Genetic and pharmacological inhibition of cytoskeletal function, reveal that the initial vesicle tethering step of exocytosis is dependent on actin and myosin XI. In contrast, treatments with the microtubule inhibitor, oryzalin, did not significantly affect vesicle tethering or fusion during CSC exocytosis but caused a minor increase in transient or aborted tethering events. With data from this new quantitative approach and improved spatiotemporal resolution of single particle events during secretion, we generate a revised model for the role of the cortical cytoskeleton in CSC trafficking.

Zhang, Weiwei↗
NASA NTRS2016

Particle Streak Velocimetry of Supersonic Nozzle Flows

A novel velocimetry technique to probe the exhaust flow of a laboratory scale combustor is being developed. The technique combines the advantages of standard particle velocimetry techniques and the ultra-fast imaging capabilities of a streak camera to probe high speed flows near continuously with improved spatial and velocity resolution. This "Particle Streak Velocimetry" technique tracks laser illuminated seed particles at up to 236 picosecond temporal resolution allowing time-resolved measurement of one-dimensional flows exceeding 2000 m/s as are found in rocket nozzles and many other applications. Developmental tests with cold nitrogen have been performed to validate and troubleshoot the technique with supersonic flows of much lower velocity and without background noise due to combusting flow. Flow velocities on the order of 500 m/s have been probed with titanium dioxide particles and a continuous-wave laser diode. Single frame images containing multiple streaks are analyzed to find the average slope of all incident particles corresponding to the centerline axial flow velocity. Long term objectives for these tests are correlation of specific impulse to theoretical combustion predictions and direct comparisons between candidate green fuels and the industry standard, monomethylhydrazine, each tested under identical conditions.

Willits, J. D.↗
DOE OSTI2021

Reducing Zinc Redistribution and Extending Cycle Life Via Electrochemical Synthesis of Zinc/Zinc Oxide Anodes in Rechargeable Alkaline Batteries

Redistribution of zinc over the electrode surface, also known as shape change, is a major problem and a cause of failure in alkaline zinc anode batteries. To mitigate this phenomenon, we propose a scalable approach based on an in situ formed, highly porous electrochemically synthesized ZnO matrix with uniformly electrodeposited zinc particles. This results in ∼70% improvement in cycle life performance at a rate of 10 mA cm −2 compared to control Zn anodes, which have not gone through the formation process. A quantitative electrolyte analysis revealed under-saturated zincate ion concentration in the electrochemically synthesized ZnO/Zn cells indicating reduced zincate movement. Post mortem analysis of the anodes indicated higher retention of both Zn and ZnO on the electrochemically synthesized ZnO anodes signifying reduced redistribution of active material. Image analysis of the cycled anodes revealed a narrower Zn particle size distribution (62−79 μ m) in contrast to a wider particle size distribution of 51–96 μ m observed in the control anodes. The formation approach results in electrochemically synthesized ZnO/Zn anodes providing a stable ZnO matrix in which Zn particles retain their localized distribution on cycling better than control electrodes conventionally made by pasting zinc particles together with a binder.

Kolhekar, Snehal (ORCID:0000000210321153)↗
DOE OSTI2026

Observing dark matter decays to gravitons via graviton-photon conversion

Since dark matter is only known to have gravitational interactions, it may plausibly decay to gravitons on cosmological timescales. Although such a scenario can be easily realized, there are currently no known limits on this possibility based on indirect-detection methods. We propose a new search strategy that exploits the Gertsenshtein effect, whereby the gravitons produced in dark matter decays can convert to photons in large-scale magnetic fields along the line of sight to an observer. These conversions primarily occur within cosmological filaments which occupy a large (order unity) volume fraction and contain ∼ 10 – 100 nG fields with ∼ Mpc coherence lengths. Thus, dark matter decays to gravitons predict an irreducible population of extragalactic photons, which we constrain using the extragalactic gamma-ray background measured by the Fermi-LAT telescope. Using this method, we derive the first-ever constraints on the dark matter lifetime in the 0.1 GeV - 10 8 GeV mass range, contingent on the assumed filament magnetic field strength. We also make projections for the Advanced Particle-astrophysics Telescope, which can improve sensitivity to this dark matter decay channel by an order of magnitude beyond those we set using Fermi-LAT data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRSDate not supplied

Balancing Manufacturability with Performance: Achieving Extrudable, High Thermal Conductivity, and Dielectrically Robust Thermoplastic Composites

Improved thermal management solutions for electrical insulation systems are a priority for increasing efficiency. Although polymeric electrical insulation is ubiquitous, it generally exhibits low thermal conductivities (κ ; 0.1 – 0.3 W/mK). High κ electrical insulation systems are desirable for several reasons including improved heat wicking. Polymer-ceramic composites offer a viable path towards increasing κ of electrical insulation systems. However, processing-induced anisotropic particle orientation can result in prohibitively high concentrations of high κ particles being required to achieve impactful improvements. This work evaluates the effectiveness of a double percolation approach and its impacts on extruded polymer composite insulation κ using polyimide (PI), polyphenylsulfone (PPSU), and hexagonal boron nitride (hBN). Thermoplastic composite blends of PI/PPSU exhibited a 15% improvement in composite κ at comparable loading levels of hBN relative to mono-polymer material systems. On the other hand, PI/PPSU/hBN composites exhibited lower dielectric strengths than either neat polymer/hBN composite. A trade-off between maximizing material κ and resultant processing and dielectric performances may exist when using a double percolation approach for thermoplastic composites.

Witold K. Fuchs↗
NASA NTRS1990

Cirrus microphysics and radiative transfer: Cloud field study on October 28, 1986

The radiative properties of cirrus clouds present one of the unresolved problems in weather and climate research. Uncertainties in ice particle amount and size and, also, the general inability to model the single scattering properties of their usually complex particle shapes, prevent accurate model predictions. For an improved understanding of cirrus radiative effects, field experiments, as those of the Cirrus IFO of FIRE, are necessary. Simultaneous measurements of radiative fluxes and cirrus microphysics at multiple cirrus cloud altitudes allows the pitting of calculated versus measured vertical flux profiles; with the potential to judge current cirrus cloud modeling. Most of the problems in this study are linked to the inhomogeneity of the cloud field. Thus, only studies on more homogeneous cirrus cloud cases promises a possibility to improve current cirrus parameterizations. Still, the current inability to detect small ice particles will remain as a considerable handicap.

Kinne, Stefan↗
NASA NTRS1995

Fuzzy inference enhanced information recovery from digital PIV using cross-correlation combined with particle tracking

Particle Image Velocimetry provides a means of measuring the instantaneous 2-component velocity field across a planar region of a seeded flowfield. In this work only two camera, single exposure images are considered where both cameras have the same view of the illumination plane. Two competing techniques which yield unambiguous velocity vector direction information have been widely used for reducing the single exposure, multiple image data: cross-correlation and particle tracking. Correlation techniques yield averaged velocity estimates over subregions of the flow, whereas particle tracking techniques give individual particle velocity estimates. The correlation technique requires identification of the correlation peak on the correlation plane corresponding to the average displacement of particles across the subregion. Noise on the images and particle dropout contribute to spurious peaks on the correlation plane, leading to misidentification of the true correlation peak. The subsequent velocity vector maps contain spurious vectors where the displacement peaks have been improperly identified. Typically these spurious vectors are replaced by a weighted average of the neighboring vectors, thereby decreasing the independence of the measurements. In this work fuzzy logic techniques are used to determine the true correlation displacement peak even when it is not the maximum peak on the correlation plane, hence maximizing the information recovery from the correlation operation, maintaining the number of independent measurements and minimizing the number of spurious velocity vectors. Correlation peaks are correctly identified in both high and low seed density cases. The correlation velocity vector map can then be used as a guide for the particle tracking operation. Again fuzzy logic techniques are used, this time to identify the correct particle image pairings between exposures to determine particle displacements, and thus velocity. The advantage of this technique is the improved spatial resolution which is available from the particle tracking operation. Particle tracking alone may not be possible in the high seed density images typically required for achieving good results from the correlation technique. This two staged approach offers a velocimetric technique capable of measuring particle velocities with high spatial resolution over a broad range of seeding densities.

Wernet, Mark P.↗
NASA NTRS2016

TPSAS-NF1676L-23432-DND

The POLSTRACC (POlar STRAtosphere in a Changing Climate) field campaign was conducted in the Arctic during December 2015 - March 2016 to investigate the chemical, microphysical, and dynamical processes of the Arctic lowermost stratosphere and upper troposphere. The primary measurement platform for POLSTRACC was the German HALO (High Altitude LOng range) research aircraft carrying a large suite of in situ and remote sensing instruments to measure key chemical species, tracers, as well as aerosol and cloud particles and meteorological parameters. Two primary science objectives of POLSTRACC are to improve our understanding of polar stratospheric cloud (PSC) particle characteristics and formation processes and investigate the impact of Arctic cirrus clouds on radiative forcing and chlorine activation. To complement the more focused measurements from the POLSTRACC field campaign, we have used spaceborne lidar measurements from CALIPSO to characterize PSC occurrence and composition, as well as the occurrence of Arctic cirrus during the 2015-2016 season on vortex-wide scales. In this paper, we present a general overview of the 2015-2016 winter, examine in detail the evolution of PSCs and cirrus during the season, and explore the unique aspects of this season in attempt to understand the underlying physical mechanisms.

Michael C Pitts↗
NASA NTRS1993

Gas-evaporation in low-gravity field (cogelation mechanism of metal vapors) (M-14)

When metal and alloy compounds are heated and vaporized in a rare gas such as helium, argon, or xenon, the vaporized substances diffused in the rare gas are supersaturated resulting in a smoke of fine particles of the material congealing as snow or fog. The gas vaporizing method is a fine particle generation method. Though the method has a variety of applications, the material vapor flow is disturbed by gravitational convection on Earth. The inability to elucidate the fine particle generation mechanism results in an obstruction to improving the method to mass production levels. As no convection occurs in microgravity in space, the fine particle generation mechanism influenced only by diffusion can be investigated. Investigators expect that excellent particles with homogeneous diameter distribution can be obtained. Experiment data and facts will assist in improving efficiency, quality, and scale or production processes including element processes such as vaporization, diffusion, and condensation. The objective of this experiment is to obtain important information related to the mechanism of particle formation in the gas atmosphere (smoke particles) and the production of submicron powders of extremely uniform size.

Wada, N.↗
DOE OSTI2022

Forecasting dark showers at Belle II

Dark showers from strongly interacting dark sectors that confine at the GeV scale can give rise to novel signatures at e + e - colliders. In this work, we study the sensitivity of B factory experiments to dark showers produced through an effective interaction arising from a heavy off-shell mediator. We show that a prospective search for displaced vertices from GeV-scale long-lived particles at Belle II can improve the sensitivity to dark showers substantially compared to an existing search at BaBar. We compare the sensitivity of searches for displaced signals to searches for promptly produced resonances at BaBar and KLOE and calculate sensitivity projections for a single-photon search at Belle II to invisible dark showers produced through an effective interaction. The underlying structure of the effective interaction can be resolved at higher-energy experiments, where the mediator can be produced on-shell. To study the resulting constraints, we update electroweak precision bounds on kinetically mixed Z' bosons and reinterpret a search for low-mass di-muon resonances at LHCb in terms of dark showers. We find that LHCb and Belle II are most sensitive to different particle decay lengths, underscoring the complementarity of LHC and intensity frontier experiments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
NASA NTRS1980

Analysis of differential and active charging phenomena on ATS-5 and ATS-6

Spacecraft charging on the differential charging and artificial particle emission experiments on ATS 5 and ATS 6 were studied. Differential charging of spacecraft surfaces generated large electrostatic barriers to spacecraft generated electrons, from photoemission, secondary emission, and thermal emitters. The electron emitter could partially or totally discharge the satellite, but the mainframe recharged negatively in a few 10's of seconds. The time dependence of the charging behavior was explained by the relatively large capacitance for differential charging in comparison to the small spacecraft to space capacitance. A daylight charging event on ATS 6 was shown to have a charging behavior suggesting the dominance of differential charging on the absolute potential of the mainframe. Ion engine operations and plasma emission experiments on ATS 6 were shown to be an effective means of controlling the spacecraft potential in eclipse and sunlight. Elimination of barrier effects around the detectors and improving the quality of the particle data are discussed.

Olsen, R. C.↗
DOE OSTI2026

Recent advances in plasma control and physics research in the Large Helical Device

The Large Helical Device (LHD), the largest superconducting helical system in the world, is equipped with advanced heating and diagnostic tools, facilitating plasma control and physics research. Data assimilation was employed for electron temperature control using a real-time Thomson scattering system and real time prediction code. A virtual LHD environment enabled visualization of escaping high-energy tritium ions and demonstrated that these ions impact the rear side of the divertor plate. Pioneering results crucial to plasma control have also been achieved. Real-time wall conditioning using Lithium granule dropping improved bulk ion energy and particle transport while simultaneously enhancing the heavy impurity transport. Progress has also been made in the investigation of turbulence-driven transport. At the confinement bifurcation, ion-scale turbulence decreased, while electron-scale turbulence increased. A change in the anisotropy of turbulent eddies was also observed at the confinement bifurcation. Coexistence of local and non-local turbulence was identified in electron-scale turbulence. Non-local turbulence exhibited the rapid spatial propagation of perturbations throughout the plasma, while local turbulence followed the temperature gradient. A transition between drift-wave turbulence and magnetohydrodynamics (MHD) turbulence was observed with the turbulence minimized at the transition condition. Machine learning analysis was employed to evaluate the temperate and density conditions of this turbulence transition. Then, real-time control of fueling and heating was applied to maintain the turbulence transition condition, improving the energy confinement enhancement factor by 20%. In addition, evidence was obtained for collisionless ion heating by energetic-ion-driven geodesic acoustic modes and MHD bursts. These achievements represent unique contributions to the development of fusion reactors.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS2008

Symmetric Phase-Only Filtering in Particle-Image Velocimetry

Symmetrical phase-only filtering (SPOF) can be exploited to obtain substantial improvements in the results of data processing in particle-image velocimetry (PIV). In comparison with traditional PIV data processing, SPOF PIV data processing yields narrower and larger amplitude correlation peaks, thereby providing more-accurate velocity estimates. The higher signal-to-noise ratios associated with the higher amplitude correlation peaks afford greater robustness and reliability of processing. SPOF also affords superior performance in the presence of surface flare light and/or background light. SPOF algorithms can readily be incorporated into pre-existing algorithms used to process digitized image data in PIV, without significantly increasing processing times. A summary of PIV and traditional PIV data processing is prerequisite to a meaningful description of SPOF PIV processing. In PIV, a pulsed laser is used to illuminate a substantially planar region of a flowing fluid in which particles are entrained. An electronic camera records digital images of the particles at two instants of time. The components of velocity of the fluid in the illuminated plane can be obtained by determining the displacements of particles between the two illumination pulses. The objective in PIV data processing is to compute the particle displacements from the digital image data. In traditional PIV data processing, to which the present innovation applies, the two images are divided into a grid of subregions and the displacements determined from cross-correlations between the corresponding sub-regions in the first and second images. The cross-correlation process begins with the calculation of the Fourier transforms (or fast Fourier transforms) of the subregion portions of the images. The Fourier transforms from the corresponding subregions are multiplied, and this product is inverse Fourier transformed, yielding the cross-correlation intensity distribution. The average displacement of the particles across a subregion results in a displacement of the correlation peak from the center of the correlation plane. The velocity is then computed from the displacement of the correlation peak and the time between the recording of the two images. The process as described thus far is performed for all the subregions. The resulting set of velocities in grid cells amounts to a velocity vector map of the flow field recorded on the image plane. In traditional PIV processing, surface flare light and bright background light give rise to a large, broad correlation peak, at the center of the correlation plane, that can overwhelm the true particle- displacement correlation peak. This has made it necessary to resort to tedious image-masking and background-subtraction procedures to recover the relatively small amplitude particle-displacement correlation peak. SPOF is a variant of phase-only filtering (POF), which, in turn, is a variant of matched spatial filtering (MSF). In MSF, one projects a first image (denoted the input image) onto a second image (denoted the filter) as part of a computation to determine how much and what part of the filter is present in the input image. MSF is equivalent to cross-correlation. In POF, the frequency-domain content of the MSF filter is modified to produce a unitamplitude (phase-only) object. POF is implemented by normalizing the Fourier transform of the filter by its magnitude. The advantage of POFs is that they yield correlation peaks that are sharper and have higher signal-to-noise ratios than those obtained through traditional MSF. In the SPOF, these benefits of POF can be extended to PIV data processing. The SPOF yields even better performance than the POF approach, which is uniquely applicable to PIV type image data. In SPOF as now applied to PIV data processing, a subregion of the first image is treated as the input image and the corresponding subregion of the second image is treated as the filter. The Fourier transforms from both the firs and second- image subregions are normalized by the square roots of their respective magnitudes. This scheme yields optimal performance because the amounts of normalization applied to the spatial-frequency contents of the input and filter scenes are just enough to enhance their high-spatial-frequency contents while reducing their spurious low-spatial-frequency content. As a result, in SPOF PIV processing, particle-displacement correlation peaks can readily be detected above spurious background peaks, without need for masking or background subtraction.

Wemet, Mark P.↗
DOE OSTI2021

Parallelizing the Unpacking and Clustering of Detector Data for Reconstruction of Charged Particle Tracks on Multi-core CPUs and Many-core GPUs

We present results from parallelizing the unpacking and clustering steps of the raw data from the silicon strip modules for reconstruction of charged particle tracks. Throughput is further improved by concurrently processing multiple events using nested OpenMP parallelism on CPU or CUDA streams on GPU. The new implementation along with earlier work in developing a parallelized and vectorized implementation of the combinatoric Kalman filter algorithm has enabled efficient global reconstruction of the entire event on modern computer architectures. We demonstrate the performance of the new implementation on Intel Xeon and NVIDIA GPU architectures.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Ice Nucleating Particles, Aerosols and Clouds over the Higher Latitude Southern Ocean

Improved understanding of aerosol-cloud-precipitation interactions is a key goal of the DOE-ASR program. Ice Nucleating Particles (INPs) are rare aerosol particles that trigger ice formation in clouds. By doing so they may initiate precipitation in clouds, and this impacts cloud lifetime. Nowhere may the role of INPs be manifested so dramatically as in the Southern Ocean (SO). This vast region was the focus of the DOE-ARM MARCUS (Measurement of Aerosols, Radiation and CloUds over the Southern Oceans) and MICRE (Macquarie Island Cloud and Radiation Experiment) campaigns. In the SO, a deficit of INPs has been a leading hypothesis for why liquid clouds persist, which underlays the bias of global climate models in predicting excess shortwave radiation reaching the ocean surface between 55°S and Antarctica. In this study, we used the 6-month acquisition of INP data on four MARCUS cruises from Hobart, Tasmania, to Antarctica, and the single-location full annual INP cycle observed in MICRE, to gain a holistic, quantitative picture of the INP number concentrations as a function of temperature and their variability over SO latitudes from 43°S to Antarctica. Augmenting initial processing of filter collections of aerosol particles during MARCUS and MICRE, additional freezing studies following thermal treatment (to removes INPs associated with microbes) and peroxide treatment (to remove all organics), as well as ionic chemistry and total organic carbon analysis, were applied to samples to improve time and space resolution, and differentiate marine from terrestrial contributions. We also performed Next Generation Sequencing to determine that bacterial composition can tag periods of enhanced and degraded marine organic INPs and the relative lack of occurrence of land-sourced bio-particles. Through these and other analyses, INP data were categorized into representative source types (e.g., marine versus terrestrially-influenced). The products of our analyses are being used to parameterize ice formation for use in numerical modeling studies to determine if, and when, ocean-derived INPs control the microphysical composition and radiative balance of SO clouds in a manner not presently captured by global models. The specific objectives and approaches proposed were largely accomplished, including: 1) Additional and value-added chemical and biological analyses of archived samples of aerosols were completed to categorize and quantify INP types and concentrations over the SO. 2) Analyses were completed to place INP data in meteorological and aerosol context. 3) Sea spray aerosol INPs were demonstrated to dominate the SO region in all but episodic events. 4) New parameterizations for INP sources relevant to the SO were constructed. 5) Collaborative modeling studies demonstrating the crucial role of INPs in determining cloud radiative and precipitation properties were conducted with MARCUS and MICRE partners. Collaborative publication submissions in this regard ensued within the two year study. This work will advance the science of interactions of aerosols, clouds and precipitation, to improve their representation in regional and global climate models. Results have informed representation of primary ice crystal nucleation, give inference to the role of secondary processes, and improve investigations of aerosol influences on clouds via ice nucleation over SO high latitudes and similar vast ocean regions. Application will improve representation of such interactions for clouds in both regional and global climate models. The data base and analyses methods applied will continue to serve research studies in the future.

58 GEOSCIENCES↗
DOE OSTI2025

Optimization of Ag Electrocatalyst Performance for CO2 to CO Conversion: Pairing Atomic Simulations with Experiments

Density-functional theory- based calculations that complement our series of experimental efforts on optimizing Ag electrocatalyst performance for CO2 to CO conversion were presented. Three key findings are drawn out from the combined UHV surface science, STM and electrochemical measurements: (1) Using a series of Ag nanoparticles with 2-6 nm average diameters, CO2 reduction reaction (CO2RR) activity increases, with particle between 2 nm and ∼4 nm demonstrating the highest combination of activity and selectivity; (2) Electronic metal−support interactions (EMSIs) between Ag and C dramatically improve CO2RR performance as evidenced by a scaling relationship between particle size and the relative Ag−C EMSIs strength, which improves the CO2-to-CO Faradaic efficiency of sub-2 nm Ag particles from 2 to ∼100% and increases the CO turnover frequency ∼15-fold compared with similarly sized bare Ag particles; (3) The performance Ag electrocatalysts is improved when supported on S-doped C materials. Computational modeling of 1−10 nm Ag particles predicts a nearly identical size-dependent trend with maximum CO2RR activity predicted for 3.7nm particles. The calculations support the promotional effect of C materials, showing a large charge transfer of 1.02 e from Ag clusters to defective C and a 0.41 eV less endergonic step of forming COOH intermediate on Ag/defective-C compared to the Ag/C system. Calculations indicate a more favorable energetic pathway of CO2-to-CO at the C-S-Ag interface, consistent with experiments.

CO2 utilization↗