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1.
Environ Sci Process Impacts ; 22(3): 719-727, 2020 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-31970349

RESUMO

Smog chamber/FTIR techniques were used to investigate the kinetics and mechanism of the Cl atom and OH radical initiated oxidation of 2,2-dichloroethanol at (296 ± 1) K. Relative rate methods were used to measure k(Cl + CHCl2CH2OH) = (5.87 ± 0.96) × 10-12 and k(OH + CHCl2CH2OH) = (5.54 ± 1.94) × 10-13 cm3 molecule-1 s-1. Chlorine atom initiated oxidation of CHCl2CH2OH in one atmosphere of air gives HCOCl, CHCl2CHO, and COCl2 in yields of (62 ± 5)%, (39 ± 10)%, and (8 ± 2)%, respectively. The rate constant k(Cl + CHCl2CHO) = (8.3 ± 16) × 10-12 cm3 molecule-1 s-1 was determined and the IR spectra of CHCl2CHO is reported for the first time. The atmospheric lifetime for CHCl2CH2OH is estimated as 21 days. The experimental results are discussed in the context of the atmospheric chemistry of chlorinated alcohols.

2.
Environ Sci Technol ; 53(18): 11013-11022, 2019 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-31415163

RESUMO

Mass adoption of electric vehicles (EVs) is widely viewed as essential to address climate change and requires a compelling case for ownership worldwide. While the manufacturing costs and technical capabilities of EVs are similar across regions, customer needs and economic contexts vary widely. Assessments of the all-electric-range required to cover day-to-day driving demand, and the climate and economic benefits of EVs, need to account for differences in regional characteristics and individual travel patterns. To meet this need travel profiles for 1681 light-duty passenger vehicles in China, the U.S., and Germany were used to make the first consistent multiregional comparison of customer and greenhouse gas (GHG) emission benefits of EVs. We show that despite differences in fuel prices, driving patterns, and subsidies, the economic benefits/challenges of EVs are generally similar across regions. Individuals who are economically most likely to adopt EVs have GHG benefits that are substantially greater than for average drivers. Such "priority" EV customers have large (32%-63%) reductions in cradle-to-grave GHG emissions. It is shown that low battery costs (below approximately $100/kWh) and a portfolio of EV offerings are required for mass adoption of electric vehicles.


Assuntos
Gasolina , Emissões de Veículos , China , Alemanha , Efeito Estufa , Humanos , Veículos Automotores , Estados Unidos
3.
Environ Sci Technol ; 53(18): 10560-10570, 2019 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-31336049

RESUMO

Electrification and lightweighting technologies are important components of greenhouse gas (GHG) emission reduction strategies for light-duty vehicles. Assessments of GHG emissions from light-duty vehicles should take a cradle-to-grave life cycle perspective and capture important regional effects. We report the first regionally explicit (county-level) life cycle assessment of the use of lightweighting and electrification for light-duty vehicles in the U.S. Regional differences in climate, electric grid burdens, and driving patterns compound to produce significant regional heterogeneity in the GHG benefits of electrification. We show that lightweighting further accentuates these regional differences. In fact, for the midsized cars considered in our analysis, model results suggest that aluminum lightweight vehicles with a combustion engine would have similar emissions to hybrid electric vehicles (HEVs) in about 25% of the counties in the US and lower than battery electric vehicles (BEVs) in 20% of counties. The results highlight the need for a portfolio of fuel efficient offerings to recognize the heterogeneity of regional climate, electric grid burdens, and driving patterns.


Assuntos
Gases de Efeito Estufa , Emissões de Veículos , Automóveis , Gasolina , Efeito Estufa , Veículos Automotores
4.
Nat Commun ; 10(1): 1555, 2019 04 09.
Artigo em Inglês | MEDLINE | ID: mdl-30967534

RESUMO

Interest and investment in electric vertical takeoff and landing aircraft (VTOLs), commonly known as flying cars, have grown significantly. However, their sustainability implications are unclear. We report a physics-based analysis of primary energy and greenhouse gas (GHG) emissions of VTOLs vs. ground-based cars. Tilt-rotor/duct/wing VTOLs are efficient when cruising but consume substantial energy for takeoff and climb; hence, their burdens depend critically on trip distance. For our base case, traveling 100 km (point-to-point) with one pilot in a VTOL results in well-to-wing/wheel GHG emissions that are 35% lower but 28% higher than a one-occupant internal combustion engine vehicle (ICEV) and battery electric vehicle (BEV), respectively. Comparing fully loaded VTOLs (three passengers) with ground-based cars with an average occupancy of 1.54, VTOL GHG emissions per passenger-kilometer are 52% lower than ICEVs and 6% lower than BEVs. VTOLs offer fast, predictable transportation and could have a niche role in sustainable mobility.

5.
Environ Sci Technol ; 53(10): 6063-6072, 2019 05 21.
Artigo em Inglês | MEDLINE | ID: mdl-31021614

RESUMO

Electrification of transportation offers clear national energy security benefits but unclear climate benefits. With the current heterogeneity of grid electricity mix in China, greenhouse gas (GHG) benefits of battery electric vehicles (BEVs) vary dramatically with location. Currently, compared to baseline conventional gasoline vehicles, BEVs in north and northeastern Chinese provinces have very modest (∼10-20%) well-to-wheel (WTW) GHG benefits, whereas BEVs in southern provinces have substantial benefits (∼50%). With the expected transition to a more renewable electricity mix documented here, regional effects will largely disappear and the benefits of BEVs will be substantial (∼60-70% lower than current internal combustion engine vehicles (ICEVs) and ∼10-40% lower than 2030 advanced hybrid electric vehicles (HEVs)) across the whole of China by 2030. GHG emissions from BEVs in Chinese cities (Beijing, Shanghai, Chongqing, and Pearl River Delta) and United States cities and regions (New York; Washington, DC; Chicago; New England; Texas; and California) in 2015 and 2030 are evaluated and compared. BEVs in Chinese cities will still have substantially higher WTW GHG emissions than those in New York, New England, and California in 2030.


Assuntos
Gases de Efeito Estufa , Pequim , California , Chicago , China , Cidades , Eletricidade , Efeito Estufa , Veículos Automotores , New England , New York , Texas , Estados Unidos , Emissões de Veículos
6.
Environ Sci Technol ; 53(4): 2199-2208, 2019 02 19.
Artigo em Inglês | MEDLINE | ID: mdl-30682256

RESUMO

Substituting conventional materials with lightweight materials is an effective way to reduce the life cycle greenhouse gas (GHG) emissions from light-duty vehicles. However, estimated GHG emission reductions of lightweighting depend on multiple factors including the vehicle powertrain technology and efficiency, lightweight material employed, and end-of-life material recovery. We developed a fleet-based life cycle model to estimate the GHG emission changes due to lightweighting the U.S. light-duty fleet from 2016 to 2050, using either high strength steel or aluminum as the lightweight material. Our model estimates that implementation of an aggressive lightweighting scenario using aluminum reduces 2016 through 2050 cumulative life cycle GHG emissions from the fleet by 2.9 Gt CO2 eq (5.6%), and annual emissions in 2050 by 11%. Lightweighting has the greatest GHG emission reduction potential when implemented in the near-term, with two times more reduction per kilometer traveled if implemented in 2016 rather than in 2030. Delaying implementation by 15 years sacrifices 72% (2.1 Gt CO2 eq) of the cumulative GHG emission mitigation potential through 2050. Lightweighting is an effective solution that could provide important near-term GHG emission reductions especially during the next 10-20 years when the fleet is dominated by conventional powertrain vehicles.


Assuntos
Gases de Efeito Estufa , Efeito Estufa , Veículos Automotores , Aço , Emissões de Veículos
7.
Environ Sci Technol ; 53(3): 1245-1251, 2019 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-30589541

RESUMO

The reaction of perfluorooctanoic acid with the smallest carbonyl oxide Criegee intermediate, CH2OO, has been measured and is very rapid, with a rate coefficient of (4.9 ± 0.8) × 10-10 cm3 s-1, similar to that for reactions of Criegee intermediates with other organic acids. Evidence is shown for the formation of hydroperoxymethyl perfluorooctanoate as a product. With such a large rate coefficient, reaction with Criegee intermediates can be a substantial contributor to atmospheric removal of perfluorocarboxylic acids. However, the atmospheric fates of the ester product largely regenerate the initial acid reactant. Wet deposition regenerates the perfluorocarboxylic acid via condensed-phase hydrolysis. Gas-phase reaction with OH is expected principally to result in formation of the acid anhydride, which also hydrolyzes to regenerate the acid, although a minor channel could lead to destruction of the perfluorinated backbone.


Assuntos
Caprilatos , Fluorcarbonetos , Compostos Orgânicos , Óxidos
8.
Phys Chem Chem Phys ; 20(44): 27949-27958, 2018 Nov 14.
Artigo em Inglês | MEDLINE | ID: mdl-30382259

RESUMO

The chemical mechanisms of the OH radical, Cl-atom and O3 initiated oxidation of (Z)-CF3CH[double bond, length as m-dash]CHCl were studied at 296 ± 1 K in 10-700 Torr air of N2/O2 diluent. Cl atoms add to the [double bond splayed left]C[double bond, length as m-dash]C[double bond splayed right] double bond: 12 ± 5% to the terminal carbon and 85 ± 5% to the central carbon. In 700 Torr of air the products are CF3CHClCHO, HCOCl, CF3COCl, CF3CHO, (E)-CF3CH[double bond, length as m-dash]CHCl, CF3C(O)CHCl2, and CF3CHClCOCl. The yield of (E) isomer was dependent on total pressure, but independent of O2 partial pressure; consistent with isomerization occurring via Cl atom elimination from the chemically activated rather than the thermalized CF3CHCHCl-Cl adduct. The rate constant for (Z)-CF3CH[double bond, length as m-dash]CHCl + Cl was measured at low pressure (10-15 Torr) and found to be indistinguishable from that determined at 700 Torr total pressure, whereas the low pressure rate constant for (E)-CF3CH[double bond, length as m-dash]CHCl was 36% smaller. G4MP2 ab initio calculations showed that the (E) isomer is 1.2 kcal mol-1 more stable than the (Z) isomer. Cl atom elimination from the adduct will preferentially form the (E) isomer and hence the rate of CF3CH[double bond, length as m-dash]CHCl loss will be more sensitive to pressure for the (Z) than the (E) isomer. Reaction of (Z)-CF3CH[double bond, length as m-dash]CHCl with OH radicals gives CF3CHO, HCOCl, (E)-CF3CH[double bond, length as m-dash]CHCl, and HCl. A significant chlorine atom elimination channel was observed experimentally, and supported by computational results. The oxidation products of the reaction of O3 with (Z)- and (E)-CF3CH[double bond, length as m-dash]CHCl were determined with no evidence of isomerization. The results are discussed with respect to the atmospheric chemistry and environmental impact of (Z)- and (E)-CF3CH[double bond, length as m-dash]CHCl.

9.
Phys Chem Chem Phys ; 20(45): 28796-28809, 2018 Nov 21.
Artigo em Inglês | MEDLINE | ID: mdl-30418435

RESUMO

Photochemical reactors were used to study the kinetics and mechanisms of reactions of Cl atoms and OH radicals with hexa- and penta-fluorobenzene (C6F6, C6F5H) in 700 Torr total pressure of N2, air, or O2 diluent at 296 ± 2 K. C6F6 and C6F5H undergo ring-opening following 254 nm UV irradiation, but with small quantum yields (φ < 0.03). Reaction of Cl atoms with C6F6 proceeds via adduct formation, while the reaction of Cl atoms with C6F5H proceeds via hydrogen abstraction and adduct formation. C6F6-Cl and C6F5H-Cl adducts decompose rapidly (k ∼ 105-106 s-1) reforming the reactants, and react with Cl atoms to form products. The fraction of adduct reacting with Cl atoms increases with steady state Cl atom concentration, resulting in an increasing apparent effective Cl atom rate constant. The rate constant for the H-abstraction channel for Cl + C6F5H is estimated at (7.3 ± 5.7) × 10-16 cm3 molecule-1 s-1. Establishment of the equilibrium between the adducts and the aromatic reactant + Cl occurs rapidly with equilibrium constants of K([adduct]/[aromatic][Cl]) = (1.96 ± 0.11) × 10-16 and (9.28 ± 0.11) × 10-17 cm3 molecule-1 for C6F6 and C6F5H, respectively. Reaction of the adducts with O2 occurs slowly with estimated rate constants of <7 and <4 × 10-18 cm3 molecule-1 s-1 for C6F6-Cl and C6F5H-Cl, respectively. The rate constants for reaction of OH radicals with C6F6 and C6F5H were determined to be (2.27 ± 0.49) × 10-13 and (2.56 ± 0.62) × 10-13 cm3 molecule-1 s-1, respectively. UV and IR spectra of C6F6 and C6F5H at 296 ± 1 K were collected and calibrated. Results are discussed in the context of available literature data for reactions of Cl atoms and OH radicals with halogenated aromatic compounds.

11.
Environ Pollut ; 241: 1027-1037, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-30029310

RESUMO

The increasing adoption of intelligent transportation system (ITS) data in smart-city initiatives worldwide has offered unprecedented opportunities for improving transportation air quality management. In this paper, we demonstrate the effective use of ITS and other traffic data to develop a link-level and hourly-based dynamic vehicle emission inventory. Our work takes advantage of the extensive ITS infrastructure deployed in Nanjing, China (6600 km2) that offers high-resolution, multi-source traffic data of the road network. Improved than conventional emission inventories, the ITS data empower the strength of revealing significantly temporal and spatial heterogeneity of traffic dynamics that pronouncedly impacts traffic emission patterns. Four urban districts account for only 4% of the area but approximately 30%-40% of vehicular emissions (e.g., CO2 and air pollutants). Owing to the detailed resolution of road network traffic, two types of emission hotspots are captured by the dynamic emission inventory: those in the urban area dominated by urban passenger traffic, and those along outlying highway corridors reflecting inter-city freight transportation (especially in terms of NOX). Fine-grained quantification of emissions reductions from traffic restriction scenarios is explored. ITS data-driven emission management systems coupled with atmospheric models offer the potential for dynamic air quality management in the future.


Assuntos
Poluentes Atmosféricos/análise , Poluição do Ar/estatística & dados numéricos , Monitoramento Ambiental , Transportes/estatística & dados numéricos , Emissões de Veículos/análise , Poluição do Ar/análise , Poluição do Ar/prevenção & controle , China , Cidades , Transportes/métodos
12.
Environ Sci Technol ; 52(5): 3249-3256, 2018 03 06.
Artigo em Inglês | MEDLINE | ID: mdl-29446302

RESUMO

Although recent studies of connected and automated vehicles (CAVs) have begun to explore the potential energy and greenhouse gas (GHG) emission impacts from an operational perspective, little is known about how the full life cycle of the vehicle will be impacted. We report the results of a life cycle assessment (LCA) of Level 4 CAV sensing and computing subsystems integrated into internal combustion engine vehicle (ICEV) and battery electric vehicle (BEV) platforms. The results indicate that CAV subsystems could increase vehicle primary energy use and GHG emissions by 3-20% due to increases in power consumption, weight, drag, and data transmission. However, when potential operational effects of CAVs are included (e.g., eco-driving, platooning, and intersection connectivity), the net result is up to a 9% reduction in energy and GHG emissions in the base case. Overall, this study highlights opportunities where CAVs can improve net energy and environmental performance.


Assuntos
Condução de Veículo , Emissões de Veículos , Fontes de Energia Elétrica , Eletricidade , Efeito Estufa
13.
Environ Sci Technol ; 52(4): 2392-2399, 2018 02 20.
Artigo em Inglês | MEDLINE | ID: mdl-29298387

RESUMO

This article presents a cradle-to-grave (C2G) assessment of greenhouse gas (GHG) emissions and costs for current (2015) and future (2025-2030) light-duty vehicles. The analysis addressed both fuel cycle and vehicle manufacturing cycle for the following vehicle types: gasoline and diesel internal combustion engine vehicles (ICEVs), flex fuel vehicles, compressed natural gas (CNG) vehicles, hybrid electric vehicles (HEVs), hydrogen fuel cell electric vehicles (FCEVs), battery electric vehicles (BEVs), and plug-in hybrid electric vehicles (PHEVs). Gasoline ICEVs using current technology have C2G emissions of ∼450 gCO2e/mi (grams of carbon dioxide equivalents per mile), while C2G emissions from HEVs, PHEVs, H2 FCEVs, and BEVs range from 300-350 gCO2e/mi. Future vehicle efficiency gains are expected to reduce emissions to ∼350 gCO2/mi for ICEVs and ∼250 gCO2e/mi for HEVs, PHEVs, FCEVs, and BEVs. Utilizing low-carbon fuel pathways yields GHG reductions more than double those achieved by vehicle efficiency gains alone. Levelized costs of driving (LCDs) are in the range $0.25-$1.00/mi depending on time frame and vehicle-fuel technology. In all cases, vehicle cost represents the major (60-90%) contribution to LCDs. Currently, HEV and PHEV petroleum-fueled vehicles provide the most attractive cost in terms of avoided carbon emissions, although they offer lower potential GHG reductions. The ranges of LCD and cost of avoided carbon are narrower for the future technology pathways, reflecting the expected economic competitiveness of these alternative vehicles and fuels.


Assuntos
Gases de Efeito Estufa , Gasolina , Efeito Estufa , Veículos Automotores , Estados Unidos , Emissões de Veículos
14.
Environ Sci Technol ; 51(24): 14436-14444, 2017 Dec 19.
Artigo em Inglês | MEDLINE | ID: mdl-29120610

RESUMO

A comprehensive component-level assessment of several strategic and minor metals (SaMMs), including copper, manganese, magnesium, nickel, tin, niobium, light rare earth elements (LREEs; lanthanum, cerium, praseodymium, neodymium, promethium, and samarium), cobalt, silver, tungsten, heavy rare earth elements (yttrium, europium, gadolinium, terbium, dysprosium, holmium, erbium, thulium, ytterbium, and lutetium), and gold, use in the 2013 model year Ford Fiesta, Focus, Fusion, and F-150 is presented. Representative material contents in cars and light-duty trucks are estimated using comprehensive, component-level data reported by suppliers. Statistical methods are used to accommodate possible errors within the database and provide estimate bounds. Results indicate that there is a high degree of variability in SaMM use and that SaMMs are concentrated in electrical, drivetrain, and suspension subsystems. Results suggest that trucks contain greater amounts of aluminum, nickel, niobium, and silver and significantly greater amounts of magnesium, manganese, gold, and LREEs. We find tin and tungsten use in automobiles to be 3-5 times higher than reported by previous studies which have focused on automotive electronics. Automotive use of strategic and minor metals is substantial, with 2013 vehicle production in the United States, Canada, EU15, and Japan alone accounting for approximately 20% of global production of Mg and Ta and approximately 5% of Al, Cu, and Sn. The data and analysis provide researchers, recyclers, and decision-makers additional insight into the vehicle content of strategic and minor metals of current interest.


Assuntos
Automóveis , Metais , Canadá , Japão , Lantânio , Neodímio , Praseodímio
18.
Environ Sci Technol ; 51(15): 8215-8228, 2017 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-28714678

RESUMO

The literature analyzing the fuel saving, life cycle greenhouse gas (GHG) emission, and ownership cost impacts of lightweighting vehicles with different powertrains is reviewed. Vehicles with lower powertrain efficiencies have higher fuel consumption. Thus, fuel savings from lightweighting internal combustion engine vehicles can be higher than those of hybrid electric and battery electric vehicles. However, the impact of fuel savings on life cycle costs and GHG emissions depends on fuel prices, fuel carbon intensities and fuel storage requirements. Battery electric vehicle fuel savings enable reduction of battery size without sacrificing driving range. This reduces the battery production cost and mass, the latter results in further fuel savings. The carbon intensity of electricity varies widely and is a major source of uncertainty when evaluating the benefits of fuel savings. Hybrid electric vehicles use gasoline more efficiently than internal combustion engine vehicles and do not require large plug-in batteries. Therefore, the benefits of lightweighting depend on the vehicle powertrain. We discuss the value proposition of the use of lightweight materials and alternative powertrains. Future assessments of the benefits of vehicle lightweighting should capture the unique characteristics of emerging vehicle powertrains.


Assuntos
Fontes de Energia Elétrica , Veículos Automotores , Emissões de Veículos , Custos e Análise de Custo , Eletricidade , Gasolina , Propriedade
19.
Faraday Discuss ; 200: 453-474, 2017 08 24.
Artigo em Inglês | MEDLINE | ID: mdl-28649687

RESUMO

Evaluating technology options to mitigate the climate impacts of road transportation can be challenging, particularly when they involve a tradeoff between long-lived emissions (e.g., carbon dioxide) and short-lived emissions (e.g., methane or black carbon). Here we present trends in short- and long-lived emissions for light- and heavy-duty transport globally and in the U.S., EU, and China over the period 2000-2030, and we discuss past and future changes to vehicle technologies to reduce these emissions. We model the tradeoffs between short- and long-lived emission reductions across a range of technology options, life cycle emission intensities, and equivalency metrics. While short-lived vehicle emissions have decreased globally over the past two decades, significant reductions in CO2 will be required by mid-century to meet climate change mitigation targets. This is true regardless of the time horizon used to compare long- and short-lived emissions. The short-lived emission intensities of some low-CO2 technologies are higher than others, and thus their suitability for meeting climate targets depends sensitively on the evaluation time horizon. Other technologies offer low intensities of both short-lived emissions and CO2.

20.
Sci Total Environ ; 574: 332-349, 2017 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-27639470

RESUMO

The large (26-fold over the past 25years) increase in the on-road vehicle fleet in China has raised sustainability concerns regarding air pollution prevention, energy conservation, and climate change mitigation. China has established integrated emission control policies and measures since the 1990s, including implementation of emission standards for new vehicles, inspection and maintenance programs for in-use vehicles, improvement in fuel quality, promotion of sustainable transportation and alternative fuel vehicles, and traffic management programs. As a result, emissions of major air pollutants from on-road vehicles in China have peaked and are now declining despite increasing vehicle population. As might be expected, progress in addressing vehicle emissions has not always been smooth and challenges such as the lack of low sulfur fuels, frauds over production conformity and in-use inspection tests, and unreliable retrofit programs have been encountered. Considering the high emission density from vehicles in East China, enhanced vehicle, fuel and transportation strategies will be required to address vehicle emissions in China. We project the total vehicle population in China to reach 400-500 million by 2030. Serious air pollution problems in many cities of China, in particular high ambient PM2.5 concentration, have led to pressure to accelerate the progress on vehicle emission reduction. A notable example is the draft China 6 emission standard released in May 2016, which contains more stringent emission limits than those in the Euro 6 regulations, and adds a real world emission testing protocol and a 48-h evaporation testing procedure including diurnal and hot soak emissions. A scenario (PC[1]) considered in this study suggests that increasingly stringent standards for vehicle emissions could mitigate total vehicle emissions of HC, CO, NOX and PM2.5 in 2030 by approximately 39%, 57%, 59% and 79%, respectively, compared with 2013 levels. With additional actions to control the future light-duty passenger vehicle population growth and use, and introduce alternative fuels and new energy vehicles, the China total vehicle emissions of HC, CO, NOX and PM2.5 in 2030 could be reduced by approximately 57%, 71%, 67% and 84%, respectively, (the PC[2] scenario) relative to 2013. This paper provides detailed policy roadmaps and technical options related to these future emission reductions for governmental stakeholders.

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