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Fedorov, Alexey

Publications and source records attributed to Fedorov, Alexey.

7 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Redox dynamics and surface structures of an active palladium catalyst during methane oxidation

Catalysts based on palladium are among the most effective in the complete oxidation of methane. Despite extensive studies and notable advances, the nature of their catalytically active species and conceivable structural dynamics remains only partially understood. Here, we combine operando transmission electron microscopy (TEM) with near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) and density functional theory (DFT) calculations to investigate the active state and catalytic function of Pd nanoparticles (NPs) under methane oxidation conditions. We show that the particle size, phase composition and dynamics respond appreciably to changes in the gas-phase chemical potential. In combination with mass spectrometry (MS) conducted simultaneously with in situ observations, we uncover that the catalytically active state exhibits phase coexistence and oscillatory phase transitions between Pd and PdO. Aided by DFT calculations, we provide a rationale for the observed redox dynamics and demonstrate that the emergence of catalytic activity is related to the dynamic interplay between coexisting phases, with the resulting strained PdO having more favorable energetics for methane oxidation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Pantropical Indo-Atlantic temperature gradient modulates multi-decadal AMOC variability in models and observations

Abstract Interconnections between ocean basins are recognized as an important driver of climate variability. Recent modeling evidence suggests that the North Atlantic climate can respond to persistent warming of the tropical Indian Ocean sea surface temperature (SST) relative to the rest of the tropics (rTIO). Here, we use observational data to demonstrate that multi-decadal changes in pantropical ocean temperature gradients lead to variations of an SST-based proxy of the Atlantic Meridional Overturning Circulation (AMOC). The largest contribution to this temperature gradient-AMOCconnection comes from gradients between the Indian and Atlantic Oceans. TherTIOindex yields the strongest connection of this tropical temperature gradient to theAMOC. Focusing on the internally generated signal in three observational products reveals that an SST-basedAMOCproxy index has closely followed low-frequency changes ofrTIOtemperature with about 26-year lag since 1870. Analyzing the pre-industrial control simulations of 44 CMIP6 climate models shows that theAMOCproxy index lags simulated mid-latitudeAMOCvariations by 4 ± 4 years. These model simulations reveal the mechanism connectingAMOCvariations to pantropical ocean temperature gradients at a 27 ± 2 years lag, matching the observed time lag in 28 out of the 44 analyzed models. rTIO temperature changes affect the North Atlantic climate through atmospheric planetary waves, impacting temperature and salinity in the subpolar North Atlantic, which modifies deep convection and ultimately the AMOC. Through this mechanism, observed internalrTIOvariations can serve as a multi-decadal precursor ofAMOCchanges with important implications forAMOCdynamics and predictability.

Meteorology & Atmospheric Sciences↗
DOE OSTI2023

The Role of Bjerknes and Shortwave Feedbacks in the Tropical Pacific SST Response to Global Warming

Abstract The evolution of tropical sea surface temperatures (SSTs) in response to greenhouse warming is of great societal and scientific interest. Most state‐of‐the‐art climate models predict a mean “El Niño‐like” warming pattern by century‐end, characterized by greater warming over the Pacific cold tongue compared to the western warm pool. However, it is unclear which proposed mechanism dominates in this response. Here, we present partially coupled abrupt CO 2 doubling experiments in which surface wind stress and shortwave heating are overridden to values from a control simulation. Contrary to previous studies, we find that experiments with overriding of surface wind stress exhibit only 58% of the full reduction in east‐west SST contrast. When both surface wind stress and shortwave flux are overridden, only 34% of the full reduction remains, controlled by spatially‐varying evaporative cooling. These results underscore the importance of Bjerknes and shortwave feedbacks in the tropical Pacific SST response to global warming.

Geology↗
DOE OSTI2023

The Impacts of a Weakened Atlantic Meridional Overturning Circulation on ENSO in a Warmer Climate

This study quantifies the impacts of the Atlantic Meridional Overturning Circulation (AMOC) on the El Niño–Southern Oscillation (ENSO) under anthropogenic warming by comparing climate change model simulations with declining and fixed strengths of the overturning. After the 1980s, a weakened AMOC is shown to reduce the strength of the annual cycle of sea surface temperature (SST) in the eastern equatorial Pacific and induce anomalous cross-equatorial northerly winds there, which strengthens ENSO variability by about 11%. An analysis of the Bjerknes stability index reveals that this intensification of ENSO results mainly from enhanced Ekman upwelling feedback due to amplified atmospheric wind response to SST anomalies and oceanic upwelling response to equatorial wind stress anomalies. The weakened AMOC also promotes the occurrence of Central Pacific El Niño events and reduces ENSO skewness. These AMOC impacts on ENSO magnitude and complexity throughout the twenty-first century are however smaller than ENSO variations expected from internal climate variability.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

AMOC stability and diverging response to Arctic sea ice decline in two climate models

This study compares the impacts of Arctic sea ice decline on the Atlantic meridional overturning circulation (AMOC) in two configurations of the Community Earth System Model with different horizontal resolution. In a suite of model experiments, we impose radiative imbalance at the ice surface, replicating a loss of sea ice cover comparable to that observed during 1979–2014, and we find dramatic differences in the AMOC response between the two models. In the lower-resolution configuration, the AMOC weakens by about one-third over the first 100 years, approaching a new quasi-equilibrium. By contrast, in the higher-resolution configuration, the AMOC weakens by ~10% during the first 20–30 years followed by a full recovery driven by invigorated deep water formation in the Labrador Sea and adjacent regions. We investigate these differences using a diagnostic AMOC stability indicator, which reflects the AMOC freshwater transport in and out of the basin and hence the strength of the basin-scale salt-advection feedback. This indicator suggests that the AMOC in the lower-resolution model is less stable and more sensitive to surface perturbations, as confirmed by hosing experiments mimicking Arctic freshening due to sea ice decline. Differences between the models’ mean states, including the Atlantic Ocean mean surface freshwater fluxes, control the differences in AMOC stability. Our results demonstrate that the AMOC stability indicator is indeed useful for evaluating AMOC sensitivity to perturbations. We emphasize that, despite the differences in the long-term adjustment, both models simulate a multidecadal AMOC weakening caused by Arctic sea ice decline, relevant to climate change.

54 ENVIRONMENTAL SCIENCES↗