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Song, Hua

Publications and source records attributed to Song, Hua.

Self-Supervised Cloud Classification

Abstract Low-level marine clouds play a pivotal role in Earth’s weather and climate through their interactions with radiation, heat and moisture transport, and the hydrological cycle. These interactions depend on a range of dynamical and microphysical processes that result in a broad diversity of cloud types and spatial structures, and a comprehensive understanding of cloud morphology is critical for continued improvement of our atmospheric modeling and prediction capabilities moving forward. Deep learning has recently accelerated our ability to study clouds using satellite remote sensing, and machine learning classifiers have enabled detailed studies of cloud morphology. A major limitation of deep learning approaches to this problem, however, is the large number of hand-labeled samples that are required for training. This work applies a recently developed self-supervised learning scheme to train a deep convolutional neural network (CNN) to map marine cloud imagery to vector embeddings that capture information about mesoscale cloud morphology and can be used for satellite image classification. The model is evaluated against existing cloud classification datasets and several use cases are demonstrated, including training cloud classifiers with very few labeled samples, interrogation of the CNN’s learned internal feature representations, cross-instrument application, and resilience against sensor calibration drift and changing scene brightness. The self-supervised approach learns meaningful internal representations of cloud structures and achieves comparable classification accuracy to supervised deep learning methods without the expense of creating large hand-annotated training datasets. Significance Statement Marine clouds heavily influence Earth’s weather and climate, and improved understanding of marine clouds is required to improve our atmospheric modeling capabilities and physical understanding of the atmosphere. Recently, deep learning has emerged as a powerful research tool that can be used to identify and study specific marine cloud types in the vast number of images collected by Earth-observing satellites. While powerful, these approaches require hand-labeling of training data, which is prohibitively time intensive. This study evaluates a recently developed self-supervised deep learning method that does not require human-labeled training data for processing images of clouds. We show that the trained algorithm performs competitively with algorithms trained on hand-labeled data for image classification tasks. We also discuss potential downstream uses and demonstrate some exciting features of the approach including application to multiple satellite instruments, resilience against changing image brightness, and its learned internal representations of cloud types. The self-supervised technique removes one of the major hurdles for applying deep learning to very large atmospheric datasets.

54 ENVIRONMENTAL SCIENCES↗

Understanding zeolite deactivation by sulfur poisoning during direct olefin upgrading

The presence of sulfur contaminants in bitumen derived crude oils can lead to rapid catalyst deactivation and is a major problem faced by downstream refiners. Whilst expensive hydrotreating steps may remove much of the sulfur content, it is important to understand how catalyst deactivation by sulfur poisoning occurs and how it may be mitigated. Here we report a mechanistic study of sulfur poisoning over a zeolite catalyst promoted with silver and gallium Lewis acids. Olefin upgrading, an essential process in the refinement of heavy oils, is used as a model reaction. Access to the zeolite inner pores is blocked by bulky, weakly adsorbed sulfur species. Pore access and thus catalyst activity is restored by increasing the reaction temperature. We also show that a simple alkaline treatment greatly improves both the sulfur tolerance and performance of the catalyst. Furthermore, these findings may enhance the rational design of heterogenous catalysts for olefin upgrading.

09 BIOMASS FUELS↗

Subgrid variations of the cloud water and droplet number concentration over the tropical ocean: satellite observations and implications for warm rain simulations in climate models

Abstract. One of the challenges in representing warm rain processes in global climate models (GCMs) is related to the representation of the subgrid variability of cloud properties, such as cloud water and cloud droplet number concentration (CDNC), and the effect thereof on individual precipitation processes such as autoconversion. This effect is conventionally treated by multiplying the resolved-scale warm rain process rates by an enhancement factor ( E q ) which is derived from integrating over an assumed subgrid cloud water distribution. The assumed subgrid cloud distribution remains highly uncertain. In this study, we derive the subgrid variations of liquid-phase cloud properties over the tropical ocean using the satellite remote sensing products from Moderate Resolution Imaging Spectroradiometer (MODIS) and investigate the corresponding enhancement factors for the GCM parameterization of autoconversion rate. We find that the conventional approach of using only subgrid variability of cloud water is insufficient and that the subgrid variability of CDNC, as well as the correlation between the two, is also important for correctly simulating the autoconversion process in GCMs. Using the MODIS data which have near-global data coverage, we find that E q shows a strong dependence on cloud regimes due to the fact that the subgrid variability of cloud water and CDNC is regime dependent. Our analysis shows a significant increase of E q from the stratocumulus (Sc) to cumulus (Cu) regions. Furthermore, the enhancement factor E N due to the subgrid variation of CDNC is derived from satellite observation for the first time, and results reveal several regions downwind of biomass burning aerosols (e.g., Gulf of Guinea, east coast of South Africa), air pollution (i.e., East China Sea), and active volcanos (e.g., Kilauea, Hawaii, and Ambae, Vanuatu), where the E N is comparable to or even larger than E q , suggesting an important role of aerosol in influencing the E N . MODIS observations suggest that the subgrid variations of cloud liquid water path (LWP) and CDNC are generally positively correlated. As a result, the combined enhancement factor, including the effect of LWP and CDNC correlation, is significantly smaller than the simple product of E q ∙ E N . Given the importance of warm rain processes in understanding the Earth's system dynamics and water cycle, we conclude that more observational studies are needed to provide a better constraint on the warm rain processes in GCMs.

54 ENVIRONMENTAL SCIENCES↗

Co-aromatization of methane with olefins: The role of inner pore and external surface catalytic sites

The co-aromatization of methane with olefins is investigated using Ag-Ga/HZSM-5 as the catalyst at 400 degrees C. The presence of methane has a pronounced effect on the product distribution in terms of increased average carbon number and substitution index and decreased aromatic carbon fraction compared with its N2 environment counterpart. The participation of methane during the co-aromatization over the Ag-Ga/HZSM-5 catalyst diminishes as the co-fed olefin feedstock molecule becomes larger, from 1-hexene to 1-octene and 1-decene, in diameter. The effect of suppressed methane participation with larger olefinic molecules is not as significant when Ag-Ga/HY is employed as the catalyst, which might be attributed to the larger pore size of HY that gives more room to hold olefin and methane molecules within the inner pores and reduces the diffusion limitation of olefin molecules. The effect of olefin feedstock on the methane participation during the co-aromatization over Ag-Ga/HZSM-5 is experimentally evidenced by 13C and 2D NMR. The incorporation of the methane carbon atoms into the phenyl ring of product molecules is reduced significantly with larger co-fed olefins, whereas its incorporation into the substitution groups of the formed aromatic molecules is not notably affected, suggesting that the methane participation in the phenyl ring formation might preferably occur within inner pores, while its incorporation into substitution groups may mainly take place on external catalytic sites. This hypothesis is well supported by the product selectivity obtained over Ag-Ga/HZSM-5 catalysts prepared using conventional ZSM-5, ZSM-5 with the external catalytic sites deactivated, nanosize ZSM-5, ZSM-5 with a micro/meso pore structure and ZSM-5 with the inner pores blocked, and further confirmed by the isotopic labeling studies.

09 BIOMASS FUELS↗

The importance of considering sub-grid cloud variability when using satellite observations to evaluate the cloud and precipitation simulations in climate models

Abstract. Satellite cloud observations have become an indispensable tool for evaluating general circulation models (GCMs). To facilitate the satellite and GCM comparisons, the CFMIP (Cloud Feedback Model Inter-comparison Project) Observation Simulator Package (COSP) has been developed and is now increasingly used in GCM evaluations. Real-world clouds and precipitation can have significant sub-grid variations, which, however, are often ignored or oversimplified in the COSP simulation. In this study, we use COSP cloud simulations from the Super-Parameterized Community Atmosphere Model (SPCAM5) and satellite observations from the Moderate Resolution Imaging Spectroradiometer (MODIS) and CloudSat to demonstrate the importance of considering the sub-grid variability of cloud and precipitation when using the COSP to evaluate GCM simulations. We carry out two sensitivity tests: SPCAM5 COSP and SPCAM5-Homogeneous COSP. In the SPCAM5 COSP run, the sub-grid cloud and precipitation properties from the embedded cloud-resolving model (CRM) of SPCAM5 are used to drive the COSP simulation, while in the SPCAM5-Homogeneous COSP run only grid-mean cloud and precipitation properties (i.e., no sub-grid variations) are given to the COSP. We find that the warm rain signatures in the SPCAM5 COSP run agree with the MODIS and CloudSat observations quite well. In contrast, the SPCAM5-Homogeneous COSP run which ignores the sub-grid cloud variations substantially overestimates the radar reflectivity and probability of precipitation compared to the satellite observations, as well as the results from the SPCAM5 COSP run. The significant differences between the two COSP runs demonstrate that it is important to take into account the sub-grid variations of cloud and precipitation when using COSP to evaluate the GCM to avoid confusing and misleading results.

54 ENVIRONMENTAL SCIENCES↗

Investigation on the light alkanes aromatization over Zn and Ga modified HZSM-5 catalysts in the presence of methane

The catalytic co-aromatization of methane and paraffin-rich raffinate oil was investigated along with hexane, heptane and octane as its model compounds over zinc and gallium modified ZSM-5 zeolite catalysts. The benzene, toluene and xylene (BTX) components derived from light alkane aromatization were highly promoted with the assistance of methane. The co-existence of Zn and Ga metal species has a positive effect on the formation of BTX components, whereas the individual metal loaded catalyst resulted in the production of heavy aromatics, suggesting that zinc and gallium have a synergistic effect on the formation of BTX under the methane environment. When concerned with gaseous analysis, the introduced methane might interact with smaller intermediates and then transform into larger hydrocarbons. From the DRIFT observation, it was witnessed that the interaction between light alkane and methane occurred on the surface of the charged Zn-Ga/ZSM-5 catalyst. According to the comprehensive catalyst characterizations, the excellent catalytic performance may be closely associated with greatly dispersed metal species on the zeolite support, improved microporous characteristic, moderate Bronsted and increased Lewis acidic sites during the paraffin-rich liquid feedstock aromatization under methane environment. This research provides a promising pathway for the highly effective and profitable utilization of petrochemical resources and natural gas.

09 BIOMASS FUELS↗

An Evaluation of Marine Boundary Layer Cloud Property Simulations in the Community Atmosphere Model Using Satellite Observations: Conventional Subgrid Parameterization versus CLUBB

This paper presents a satellite-observation-based evaluation of the marine boundary layer (MBL) cloud properties from two Community Atmosphere Model, version 5 (CAM5), simulations, one with the standard parameterization schemes (CAM5–Base) and the other with the Cloud Layers Unified by Binormals scheme (CAM5–CLUBB). When comparing the direct model outputs, the authors find that CAM5–CLUBB produces more MBL clouds, a smoother transition from stratocumulus to cumulus, and a tighter correlation between in-cloud water and cloud fraction than CAM5–Base. In the model-to-observation comparison using the COSP satellite simulators, the authors find that both simulations capture the main features and spatial patterns of the observed cloud fraction from MODIS and shortwave cloud radiative forcing (SWCF) from CERES. However, CAM5–CLUBB suffers more than CAM5–Base from a problem that can be best summarized as “undetectable” clouds (i.e., a significant fraction of simulated MBL clouds are thinner than the MODIS detection threshold). This issue leads to a smaller COSP–MODIS cloud fraction and a weaker SWCF in CAM5–CLUBB than the observations and also CAM5–Base in the tropical descending regions. Finally, the authors compare modeled radar reflectivity with CloudSat observations and find that both simulations, especially CAM5–CLUBB, suffer from an excessive drizzle problem. Further analysis reveals that the subgrid precipitation enhancement factors in CAM5–CLUBB are unrealistically large, which makes MBL clouds precipitate too excessively, and in turn results in too many undetectable thin clouds.

54 ENVIRONMENTAL SCIENCES↗

Co-aromatization of olefin and methane over Ag-Ga/ZSM-5 catalyst at low temperature

The massive exploitation of shale gas in the past decade has boosted the production of natural gas and reduced its price dramatically. The methane activation and following conversion into more valuable fuels and chemicals have thus become more and more attractive, while the introduction of hydrocarbons to enhance the methane activation at mild conditions represents a promising approach. In the present work, the co-aromatization of methane with propylene has been studied at 400 °C. The presence of methane would increase the toluene to benzene ratio as well as the average carbon number of the formed liquid aromatic products compared to its propylene alone counterpart. Among the gas products, the formations of C 3 H 8 , C 4 H 8 and C 4 H 10 also get promoted when methane is present. The incorporation of methane into the product molecules is also directly evidenced by the 1 H, 2 D and 13 C NMR spectroscopy of the liquid products obtained from the reaction between propylene (or styrene) and isotope labelled methane. Hydrogen from methane would contribute a large portion of the hydrogen in the product molecules, while the benzylic and aromatic hydrogen sites are favored compared with those on the alkyl side chains. The activation of methane is also observed in the DRIFT spectra when deuterium enriched methane is engaged as the methane source and evidenced by the escalated exothermic feature when olefin aromatization takes place under methane environment. The excellent catalytic performance of Ag-Ga/ZSM-5 might be because of the better dispersion of Ag and Ga on the ZSM-5 surface and moderate amount of strong Brosted and Lewis surface acid sites. All the observations suggest that methane might be activated nonoxidatively and converted into aromatics if suitable catalyst is charged under the assistance of co-existing olefin. In conclusion, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and petrochemical intermediates.

09 BIOMASS FUELS↗

Methane Upgrading of Acetic Acid as a Model Compound for a Biomass-Derived Liquid over a Modified Zeolite Catalyst

The technical feasibility of coaromatization of acetic acid derived from biomass and methane was investigated under mild reaction conditions (400 °C and 30 bar) over silver-, zinc-, and/or gallium-modified zeolite catalysts. On the basis of GC-MS, Micro-GC, and TGA analysis, more light aromatic hydrocarbons, less phenol formation, lower coke production, and higher methane conversion are observed over 5%Zn-1%Ga/ZSM-5 catalyst in comparison with catalytic performance over the other catalysts. Direct evidence of methane incorporation into aromatics over 5%Zn-1%Ga/ZSM-5 catalyst is witnessed in 1 H, 2 H, and 13 C NMR spectra, revealing that the carbon from methane prefers to occupy the phenyl carbon sites and the benzylic carbon sites, and the hydrogen of methane favors the aromatic and benzylic substitutions of product molecules. In combination with the 13 C NMR results for isotopically labeled acetic acid ( 13 CH 3 COOH and CH 3 13 COOH), it can be seen that the methyl and carbonyl carbons of acetic acid are equally involved in the formation of ortho, meta and para carbons of the aromatics, whereas the phenyl carbons directly bonded with alkyl substituent groups and benzylic carbons are derived mainly from the carboxyl carbon of acetic acid. After various catalyst characterizations by using TEM, XRD, DRIFT, NH 3 -TPD, and XPS, the excellent catalytic performance might be closely related to the highly dispersed zinc and gallium species on the zeolite support, moderate surface acidity, and an appropriate ratio of weak acidic sites to strong acidic sites as well as the fairly stable oxidation state during acetic acid conversion under a methane environment. Two mechanisms of the coaromatization of acetic acid and methane have also been proposed after consulting all the collected data in this study. In conclusion, the results reported in this paper could potentially lead to more cost-effective utilization of abundant natural gas and biomass.

09 BIOMASS FUELS↗

Catalytic co-aromatization of ethanol and methane

This study demonstrates the technical feasibility of simultaneously converting ethanol and methane into liquid hydrocarbons at mild reaction conditions (400 °C and 1 atm) over silver and/or zinc modified zeolite catalysts. After GC-MS analysis, it is worth noting that aromatics are the major compounds contained in the liquid product collected from the run when 1%Ag/ZSM-5, particularly after H 2 pretreatment, is charged. Compared to the performance exhibited from the run with pure HZSM-5 support engaged, Ag addition into the HZSM-5 framework favors aromatics formation, which might be closely associated with better Ag dispersion and more abundance of strong surface acidic sites where aromatization might take place while Zn loading exerts a detrimental effect on the production of aromatics but promotes the ether generation possibly through dehydration reaction. Referred to that from its N 2 counterpart, the increased aromatics formation of the collected liquid product when methane is present indicates that methane existence might facilitate ethanol aromatization. Moreover, combined with the increased carbon number in the formed aromatics from CH 4 run when H 2 run is referred and zero liquid formation from CH 4 -alone test as well as more prominent endothermic feature of methane run and more importantly the notably increased 13 C signals in 13 C NMR spectra of the liquid product collected during ethanol conversion under 13 CH 4 environment, all the observations suggest that methane might be activated nonoxidatively and converted into higher hydrocarbons, preferentially into aromatics if suitable catalyst is charged under the assistance of co-existing oxygenated hydrocarbon. Lastly, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and cellulosic ethanol.

09 BIOMASS FUELS↗

RACORO continental boundary layer cloud investigations. 3. Separation of parameterization biases in single-column model CAM5 simulations of shallow cumulus

Climatically important low-level clouds are commonly misrepresented in climate models. The FAst-physics System TEstbed and Research (FASTER) project has constructed case studies from the Atmospheric Radiation Measurement (ARM) Climate Research Facility's Southern Great Plain site during the RACORO aircraft campaign to facilitate research on model representation of boundary-layer clouds. This paper focuses on using the single-column Community Atmosphere Model version 5 (SCAM5) simulations of a multi-day continental shallow cumulus case to identify specific parameterization causes of low-cloud biases. Consistent model biases among the simulations driven by a set of alternative forcings suggest that uncertainty in the forcing plays only a relatively minor role. In-depth analysis reveals that the model's shallow cumulus convection scheme tends to significantly under-produce clouds during the times when shallow cumuli exist in the observations, while the deep convective and stratiform cloud schemes significantly over-produce low-level clouds throughout the day. The links between model biases and the underlying assumptions of the shallow cumulus scheme are further diagnosed with the aid of large-eddy simulations and aircraft measurements, and by suppressing the triggering of the deep convection scheme. It is found that the weak boundary layer turbulence simulated is directly responsible for the weak cumulus activity and the simulated boundary layer stratiform clouds. Increased vertical and temporal resolutions are shown to lead to stronger boundary layer turbulence and reduction of low-cloud biases.

54 ENVIRONMENTAL SCIENCES↗

RACORO Continental Boundary Layer Cloud Investigations: 3. Separation of Parameterization Biases in Single-Column Model CAM5 Simulations of Shallow Cumulus

Climatically important low-level clouds are commonly misrepresented in climate models. The FAst-physics System TEstbed and Research (FASTER) Project has constructed case studies from the Atmospheric Radiation Measurement Climate Research Facility's Southern Great Plain site during the RACORO aircraft campaign to facilitate research on model representation of boundary-layer clouds. This paper focuses on using the single-column Community Atmosphere Model version 5 (SCAM5) simulations of a multi-day continental shallow cumulus case to identify specific parameterization causes of low-cloud biases. Consistent model biases among the simulations driven by a set of alternative forcings suggest that uncertainty in the forcing plays only a relatively minor role. In-depth analysis reveals that the model's shallow cumulus convection scheme tends to significantly under-produce clouds during the times when shallow cumuli exist in the observations, while the deep convective and stratiform cloud schemes significantly over-produce low-level clouds throughout the day. The links between model biases and the underlying assumptions of the shallow cumulus scheme are further diagnosed with the aid of large-eddy simulations and aircraft measurements, and by suppressing the triggering of the deep convection scheme. It is found that the weak boundary layer turbulence simulated is directly responsible for the weak cumulus activity and the simulated boundary layer stratiform clouds. Increased vertical and temporal resolutions are shown to lead to stronger boundary layer turbulence and reduction of low-cloud biases.

parameterization↗

Study on the energy band structure and photoelectrochemical performances of spinel Li{sub 4}Ti{sub 5}O{sub 12}

Highlights: • Spinel Li{sub 4}Ti{sub 5}O{sub 12} possesses more positive potential of valence band and wider band gap than TiO{sub 2}. • Spinel Li{sub 4}Ti{sub 5}O{sub 12} displays typical n-type semiconductor characteristic and excellent UV-excitateded photocatalysis activity. • Our preliminary study will open new perspectives in investigation of other lithium-based compounds for new photocatalysts. - Abstract: Energy band structure, photoelectrochemical performances and photocatalysis activity of spinel Li{sub 4}Ti{sub 5}O{sub 12} are investigated for the first time in this paper. Li{sub 4}Ti{sub 5}O{sub 12} possesses more positive valence band potential and wider band gap than TiO{sub 2} due to its valence band consisting of Li{sub 1s} and Ti{sub 3d} orbitals mixed with O{sub 2p}. Li{sub 4}Ti{sub 5}O{sub 12} shows typical photocatalysis material characteristics and excellent photocatlytic activity under UV irradiation.

36 MATERIALS SCIENCE↗

Evaluation of Precipitation Simulated by Seven SCMs against the ARM Observations at the SGP Site

This study evaluates the performances of seven single-column models (SCMs) by comparing simulated surface precipitation with observations at the Atmospheric Radiation Measurement Program Southern Great Plains (SGP) site from January 1999 to December 2001. Results show that although most SCMs can reproduce the observed precipitation reasonably well, there are significant and interesting differences in their details. In the cold season, the model-observation differences in the frequency and mean intensity of rain events tend to compensate each other for most SCMs. In the warm season, most SCMs produce more rain events in daytime than in nighttime, whereas the observations have more rain events in nighttime. The mean intensities of rain events in these SCMs are much stronger in daytime, but weaker in nighttime, than the observations. The higher frequency of rain events during warm-season daytime in most SCMs is related to the fact that most SCMs produce a spurious precipitation peak around the regime of weak vertical motions but rich in moisture content. The models also show distinct biases between nighttime and daytime in simulating significant rain events. In nighttime, all the SCMs have a lower frequency of moderate-to-strong rain events than the observations for both seasons. In daytime, most SCMs have a higher frequency of moderate-to-strong rain events than the observations, especially in the warm season. Further analysis reveals distinct meteorological backgrounds for large underestimation and overestimation events. The former occur in the strong ascending regimes with negative low-level horizontal heat and moisture advection, whereas the latter occur in the weak or moderate ascending regimes with positive low-level horizontal heat and moisture advection.

Model comparison↗