Controlling Emission Wavelength and Chirality of Quantum Emitters in 2D Heterostructures
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In support of Pratt & Whitney efforts to define the Rich burn/Quick mix/Lean burn (RQL) combustor for the High Speed Civil Transport (HSCT) aircraft engine, UTRC conducted a flametube-scale study of the RQL concept. Extensive combustor testing was performed at the Supersonic Cruise (SSC) condition of a HSCT engine cycle, Data obtained from probe traverses near the exit of the mixing section confirmed that the mixing section was the critical component in controlling combustor emissions. Circular-hole configurations, which produced rapidly-, highly-penetrating jets, were most effective in limiting NOx. The spatial profiles of NOx and CO at the mixer exit were not directly interpretable using a simple flow model based on jet penetration, and a greater understanding of the flow and chemical processes in this section are required to optimize it. Neither the rich-combustor equivalence ratio nor its residence time was a direct contributor to the exit NOx. Based on this study, it was also concluded that (1) While NOx formation in both the mixing section and the lean combustor contribute to the overall emission, the NOx formation in the mixing section dominates. The gas composition exiting the rich combustor can be reasonably represented by the equilibrium composition corresponding to the rich combustor operating condition. Negligible NOx exits the rich combustor. (2) At the SSC condition, the oxidation processes occurring in the mixing section consume 99 percent of the CO exiting the rich combustor. Soot formed in the rich combustor is also highly oxidized, with combustor exit SAE Smoke Number <3. (3) Mixing section configurations which demonstrated enhanced emissions control at SSC also performed better at part-power conditions. Data from mixer exit traverses reflected the expected mixing behavior for off-design jet to crossflow momentum-flux ratios. (4) Low power operating conditions require that the RQL combustor operate as a lean-lean combustor to achieve low CO and high efficiency. (5) A RQL combustor can achieve the emissions goal of EINOX = 5 at the Supersonic Cruise operating condition for a HSCT engine.
In support of Pratt & Whitney efforts to define the Rich burn/Quick mix/Lean burn (RQL) combustor for the High Speed Civil Transport (HSCT) aircraft engine, UTRC conducted a flametube-scale study of the RQL concept. Extensive combustor testing was performed at the Supersonic Cruise (SSC) condition of an HSCT engine cycle. Data obtained from probe traverses near the exit of the mixing section confirmed that the mixing section was the critical component in controlling combustor emissions. Circular-hole configurations, which produced rapidly-, highly-penetrating jets, were most effective in limiting NO(x). The spatial profiles of NO(x) and CO at the mixer exit were not directly interpretable using a simple flow model based on jet penetration, and a greater understanding of the flow and chemical processes in this section are required to optimize it. Neither the rich-combustor equivalence ratio nor its residence time was a direct contributor to the exit NO(x). Based on this study, it was also concluded that: (1) While NO(x) formation in both the mixing section and the lean combustor contribute to the overall emission, the NOx formation in the mixing section dominates. The gas composition exiting the rich combustor can be reasonably represented by the equilibrium composition corresponding to the rich combustor operating condition. Negligible NO(x) exits the rich combustor. (2) At the SSC condition, the oxidation processes occurring in the mixing section consume 99 percent of the CO exiting the rich combustor. Soot formed in the rich combustor is also highly oxidized, with combustor exit SAE Smoke Number <3. (3) Mixing section configurations which demonstrated enhanced emissions control at SSC also performed better at part-power conditions. Data from mixer exit traverses reflected the expected mixing behavior for off-design jet to crossflow momentum-flux ratios. (4) Low power operating conditions require that the RQL combustor operate as a lean-lean combustor to achieve low CO and high efficiency. (5) An RQL combustor can achieve the emissions goal of EINO(x) = 5 at the Supersonic Cruise operating condition for an HSCT engine.
Previous studies demonstrated that global warming can lead to deteriorated air quality even when anthropogenic emissions were kept constant, which has been called a climate change penalty on air quality. It is expected that anthropogenic emissions will decrease significantly in the future considering the aggressive emission control actions in China. However, the dependence of climate change penalty on the choice of emission scenario is still uncertain. To fill this gap, we conducted multiple independent model simulations to investigate the response of PM2.5 to future (2050) climate warming (RCP8.5) in China but with different emission scenarios, including the constant 2015 emissions, the 2050 CLE emissions (based on Current Legislation), and the 2050 MTFR emissions (based on Maximum Technically Feasible Reduction). For each set of emissions, we estimate climate change penalty as the difference in PM2.5 between a pair of simulations with either 2015 or 2050 meteorology. Under 2015 emissions, we find a PM2.5 climate change penalty of 1.43 μg m−3 in Eastern China, leading to an additional 35,000 PM2.5-related premature deaths [95% confidence interval (CI), 21,000-40,000] by 2050. However, the PM2.5 climate change penalty weakens to 0.24 μg m−3 with strict anthropogenic emission controls under the 2050 MTFR emissions, which decreases the associated PM2.5-related deaths to 17,000. The smaller MTFR climate change penalty contributes 14% of the total PM2.5 decrease when both emissions and meteorology are changed from 2015 to 2050, and 24% of total health benefits associated with this PM2.5 decrease in Eastern China. This finding suggests that controlling anthropogenic emissions can effectively reduce the climate change penalty on PM2.5 and its associated premature deaths, even though a climate change penalty still occurs even under MTFR. Strengthened controls on anthropogenic emissions are key to attaining air quality targets and protecting human health in the context of future global climate change.
An electron emission control circuit of the switching regulator type operating at 100 kHz has been developed which maintains a constant emission current within 0.1% for a cathode power demand variation of approximately 100%. The power output stage has an efficiency of 67%, and the overall efficiency is 45% when driving a thoria-coated iridium cathode having a nominal resistance at operating temperature of 2.5 ohms. Under optimum conditions, the bus power demand is 1.75 W. The circuit is useful in controlling the electron emission current of ion sources in applications which involve a substantial variation of the cathode work function, such as oxygen partial pressure measurements over a large dynamic range.
Previous studies demonstrated that global warming can lead to deteriorated air quality even when anthropogenic emissions were kept constant, which has been called a climate change penalty on air quality. It is expected that anthropogenic emissions will decrease significantly in the future considering the aggressive emission control actions in China. However, the dependence of climate change penalty on the choice of emission scenario is still uncertain. To fill this gap, we conducted multiple independent model simulations to investigate the response of PM2.5 to future (2050) climate warming (RCP8.5) in China but with different emission scenarios, including the constant 2015 emissions, the 2050 CLE emissions (based on Current Legislation), and the 2050 MTFR emissions (based on Maximum Technically Feasible Reduction). For each set of emissions, we estimate climate change penalty as the difference in PM2.5 between a pair of simulations with either 2015 or 2050 meteorology. Under 2015 emissions, we find a PM2.5 climate change penalty of 1.43 µg m-3 in Eastern China, leading to an additional 35,000 PM2.5-related premature deaths [95% confidence interval (CI), 21,000-40,000] by 2050. However, the PM2.5 climate change penalty weakens to 0.24 µg m-3 with strict anthropogenic emission controls under the 2050 MTFR emissions, which decreases the associated PM2.5-related deaths to 17,000. The smaller MTFR climate change penalty contributes 14% of the total PM2.5 decrease when both emissions and meteorology are changed from 2015 to 2050, and 24% of total health benefits associated with this PM2.5 decrease in Eastern China. This finding suggests that controlling anthropogenic emissions can effectively reduce the climate change penalty on PM2.5 and its associated premature deaths, even though a climate change penalty still occurs even under MTFR. Strengthened controls on anthropogenic emissions is key to attaining air quality targets and protecting human health in the context of future global climate change.
Despite intensive research exploring how aerosols respond to emission control over Northern China, efforts mostly focus on the environmental benefit, especially in winter. Here we found that unlike the most substantial PM 2.5 concentration reduction in winter, aerosol optical depth (AOD) declines more than 2 times faster in summer, causing an increase in aerosol radiative effects of 1.2 (5.7)Wm -2 on all-sky (clear-sky) conditions over 2013–2019 and largely shaping the climate impact. Low-level aerosols are shown to be the prime contributor under the synergetic effects of aerosol composition and ambient relative humidity (RH). The dominance of the highly hygroscopic sulfate combined with high RH enables a strong extinction efficiency of the reduced summertime aerosols, while the insignificant AOD decline in wintertime result from the dominance of organic aerosols with weak hygroscopicity, and is further offset by the increased frequencies of extremely high RH. We show the environmental and climatic responses of aerosols to emission control exhibit distinctively different seasonality.
The responses of secondary organic aerosols (SOA) to emission controls remain uncertain due to the limited continuous long‐term measurements. Measurements of detailed carbonaceous aerosol composition in the New York City metropolitan region during the summers of 2001, 2009, 2011, and 2018 provide a look at the changes in summertime SOA over the past two decades when significant pollution reduction and emission controls occurred in the northeastern United States. Here, we show that the averaged nighttime SOA, especially the fresh local SOA, extreme mass concentrations resulted from anthropogenic volatile organic compounds reductions, while there is a little trend for the regional aged SOA. Meanwhile, these fresh SOA extremes occurred most often under conditions of high relative humidity during nighttime. The analysis presented here provides a comprehensive evaluation of the evolution of the increasingly important organic component of the submicron ambient aerosols in this major metropolitan area.
Tropospheric ozone and black carbon (BC), a component of fine particulate matter (PM < or = 2.5 microns in aerodynamic diameter; PM2.5), are associated with premature mortality and they disrupt global and regional climate. Objectives: We examined the air quality and health benefits of 14 specific emission control measures targeting BC and methane, an ozone precursor, that were selected because of their potential to reduce the rate of climate change over the next 20-40 years. Methods: We simulated the impacts of mitigation measures on outdoor concentrations of PM2.5 and ozone using two composition-climate models, and calculated associated changes in premature PM2.5‑ and ozone-related deaths using epidemiologically derived concentration-response functions. Results: We estimated that, for PM2.5 and ozone, respectively, fully implementing these measures could reduce global population-weighted average surface concentrations by 23-34% and 7-17% and avoid 0.6-4.4 and 0.04-0.52 million annual premature deaths globally in 2030. More than 80% of the health benefits are estimated to occur in Asia. We estimated that BC mitigation measures would achieve approximately 98% of the deaths that would be avoided if all BC and methane mitigation measures were implemented, due to reduced BC and associated reductions of nonmethane ozone precursor and organic carbon emissions as well as stronger mortality relationships for PM2.5 relative to ozone. Although subject to large uncertainty, these estimates and conclusions are not strongly dependent on assumptions for the concentration-response function. Conclusions: In addition to climate benefits, our findings indicate that the methane and BC emission control measures would have substantial co-benefits for air quality and public health worldwide, potentially reversing trends of increasing air pollution concentrations and mortality in Africa and South, West, and Central Asia. These projected benefits are independent of carbon dioxide mitigation measures. Benefits of BC measures are underestimated because we did not account for benefits from reduced indoor exposures and because outdoor exposure estimates were limited by model spatial resolution.
The present disclosure relates to a thermal emissivity control system. The system may have a segmented array that makes use of a thermally conductive base layer configured to be connectable to an external heat generating subsystem, with the base layer including a thermally emissive surface. The array may also have a plurality of actuation elements at least one of positioned on or adjacent to the thermally emissive surface. A plurality of movable shutter elements is disposed adjacent one another in a grid pattern, and controlled in movement by the actuation elements to create gaps of controllably varying dimension therebetween. The shutter elements control at least one of a magnitude of, or direction of, thermal radiation through the gaps.
Minimizing the environmental impacts of amine-based post-combustion carbon capture technologies is essential for regulatory compliance and public acceptance. Experimental campaigns at RWE's CO 2 capture pilot plant in Niederaussem using CESAR1 demonstrated that combining existing emission abatement technologies can substantially reduce the concentration of amines and degradation products in the CO 2 -depleted flue gas to below the detection limit of an infrared spectrometer. The campaign confirmed that a proprietary dry bed technology (OEASE aerozone™) or a second water wash can reduce AMP and PZ emissions to below 1 mg/Nm 3 . However, an acid or chemically active wash downstream of the water wash is necessary to reduce NH 3 emissions to very low levels (<2 mg/Nm 3 ). Combining a dry bed with an acid wash significantly reduces both the required acid solution and the resulting acid waste. The techno-economic analysis indicates that implementing emission mitigation technologies provides substantial environmental benefits for the CESAR1 process, with only a marginal increase (<1 €/tCO 2 ) in both the carbon capture cost (CCC) and CO 2 avoidance cost (CAC). The additional capital cost associated with extra column packing is offset by operational cost savings from reduced solvent losses. For stringent emission permits targeting NH 3 , a configuration combining a dry bed upstream of the water wash followed by an acid wash achieves the best balance between emission control and cost efficiency. This configuration results in a Levelized Cost of Electricity (LCOE) of 143 €/MWh, a CCC of 45.4 €/tCO 2 , and a CAC of 88.4 €/tCO 2 .
N-Nitrosamines are one of the environmentally significant byproducts from aqueous amine-based post-combustion carbon capture systems (CCS) due to their potential risk to human health. Safely mitigating nitrosamines before they are emitted from these CO 2 capture systems is therefore a key concern before widescale deployment of CCS can be used to address worldwide decarbonization goals. Electrochemical decomposition is one viable route to neutralize these harmful compounds. The circulating emission control waterwash system, commonly installed at the end of the flue gas treatment trains to minimize amine solvent emissions, plays an important role to capture N-nitrosamines and control their emission into the environment. The waterwash solution is the last point where these compounds can be properly neutralized before becoming an environmental hazard. In this study, the decomposition mechanisms of N-nitrosamines in a simulated CCS waterwash with residual alkanolamines was investigated using several laboratory-scale electrolyzers utilizing carbon xerogel (CX) electrodes. Hcell experiments revealed that N-nitrosamines were decomposed through a reduction reaction and are converted into their corresponding secondary amines thereby neutralizing their environmental impact. Batch-cell experiments statistically examined the kinetic models of N-nitrosamine removal by a combined adsorption and decomposition processes. The cathodic reduction of the N-nitrosamines statistically obeyed the first-order reaction model. Finally, a prototype flow-through reactor using an authentic waterwash was used to successfully target and decompose N-nitrosamines to below the detectable level without degrading the amine solvent compounds allowing them to be return to the CCS and lower the system operating costs. Furthermore, the developed electrolyzer was able to efficiently remove greater than 98% of N-nitrosamines from the waterwash solution without producing any additional environmentally harmful compounds and offers an effective and safe route to mitigate these compounds from CO 2 capture systems.
The CRADA between Cummins and Battelle will focus on: advanced emission control for high-efficiency engines. It will specifically focus on the following three areas: 1. Passive NOx absorbers - The purpose is to develop next generation materials that can be efficiently used to address the cold-operation, as driven by improved engine efficiency. 2. Oxidation of methane and short alkanes – The purpose is to address cold-operation emissions arising from CNG vehicles. 3. Improved understanding of particulates – The purpose is to understand how particulates are formed which will be used to develop strategies to address the tightening regulations and their enforcement for exhaust particulate matter. The first two areas will be based on PNNL’s technical leadership in the area of zeolite-based materials. The third area will have a shorter time scope to leverage the unique SPLAT capabilities at PNNL to help address Cummins’ needs in improving the understanding of particulates
Nanosized cerium oxide (CeO 2 ) has been extensively used as the oxygen storage component in automotive emission control systems. However, the possible influence of atomically dispersed Ce in these catalysts has not been recognized. Here, in this study, we demonstrate the controllable transformation of ceria nanoparticles into isolated cerium cations on γ-Al 2 O 3 via reductive atom trapping in 10% H 2 at 800 °C, achieving over half-monolayer coverage. Dispersed Ce 1 ions anchored by surface penta- and octa-coordinated Al sites exhibit outstanding thermal stability in air up to 500 °C, enabling further loading of active metals with well-defined catalyst structures. With this strategy, supported single-atom Rh 1 surrounded by dispersed Ce 1 is confirmed to exhibit much superior performance to Rh 1 on bare Al 2 O 3 or nanocrystalline CeO 2 in catalyzing NO reduction by CO, exhibiting a striking one-order-of-magnitude increase in activity. Dispersed Ce 1 exhibits greatly enhanced oxygen transfer capability compared to ceria nanoparticles and introduces a modified reaction mechanism that involves an adjacent Rh 1 –Ce 1 motif, resulting in a greatly decreased activation barrier (from 192 to 96 kJ/mol). The reactivity enhancements are also seen with Ce 1 -promoted Pt nanoparticles for oxidation of CO and hydrocarbons.
Nine years of summertime ozone data from the Atlanta metropolitan area are analyzed and compared to local emissions of volatile organic carbon and nitrogen oxides. Trends from 1979 to 1987 were studied for the number of days per year ozone exceeded the NAAQS standard, the second-highest ozone level observed per year, and the first quartile summertime average ozone observed, as well as the mean difference between the ozone level observed downwind and upwind of the city. Because this last parameter is sensitive to chemical factors but relatively insensitive to the number of days each year with meteorological conditions conducive to ozone formation, its trend may be best suited for determining how effective emission controls have been in reducing O3 in the Atlanta area. In spite of the fact that sizeable reductions have been claimed for volatile organic carbon emissions over the past several years, the data give no indication that ozone levels have decreased and in fact, imply that summertime ozone production may have increased. The results imply that either emissions have not decreased as much as has been claimed or that ozone is not sensitive to anthropogenic volatile organic carbon emissions.
We show that Aura Ozone Monitoring Instrument (OMI) nitrogen dioxide (NO2) tropospheric column data may be used to assess changes of the emissions of nitrogen oxides (NOx) from power plants in the United States, though careful interpretation of the data is necessary. There is a clear response for OMI NO2 data to NOx emission reductions from power plants associated with the implementation of mandated emission control devices (ECDs) over the OMI record (2005e2011). This response is scalar for all intents and purposes, whether the reduction is rapid or incremental over several years. However, it is variable among the power plants, even for those with the greatest absolute decrease in emissions. We document the primary causes of this variability, presenting case examples for specific power plants.
We report the demonstration of optical compression of an electron beam and the production of controllable trains of femtosecond, soft x-ray pulses with the Linac Coherent Light Source (LCLS) freeelectron laser (FEL). This is achieved by enhanced self-amplified spontaneous emission with a 2 μm laser and a dechirper device. Optical compression was achieved by modulating the energy of an electron beam with the laser and then compressing with a chicane, resulting in high current spikes on the beam which we observe to lase. A dechirper was then used to selectively control the lasing region of the electron beam. Field autocorrelation measurements indicate a train of pulses, and we find that the number of pulses within the train can be controlled (from 1 to 5 pulses) by varying the dechirper position and undulator taper. These results are a step toward attosecond spectroscopy with x-ray FELs as well as future FEL schemes relying on optical compression of an electron beam.
Magnetic fields offer a powerful means to control molecular emission, enabling quantum sensing and spin-level control of chemical reactions. Here, we demonstrate a strategy to magnetically control red to near-infrared phosphorescence via triplet–triplet energy transfer (TTET) from donor–chiral bridge–acceptor (D−χ–A) molecules that generate spin-correlated radical pairs (SCRPs) upon photoexcitation. These SCRPs yield non-emissive triplet excited states whose formation is sensitive to magnetic fields. Here, by transferring this energy to emissive Pt- and Pd-based π-extended porphyrins, we enable magnetic control over phosphorescence that would otherwise be unresponsive to weak magnetic fields (<1 T). This approach establishes a platform for quantifying magnetic field effects on silent triplet states while extending magnetically responsive emission into the near-infrared. Coupling SCRP-based molecular magnetic switches to long-wavelength emissive acceptors offers a new way for probing and modulating spin-dependent processes and triplet-state populations in molecular systems.