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Carbon dioxide capture : an effective way to combat global warming
This topical brief summarizes the various options available for carbon capture and presents the current strategies involved in CO₂ reduction. The authors focus on current CO₂ capture technologies that facilitate the reduction of greenhouse gas (CO₂) emissions and reduce global warming. This short study will interest environmental researchers, teachers and students who have an interest in global warming.
Shortwave absorption by wildfire smoke dominated by dark brown carbon
by
Sedlacek, Arthur J
,
Liu, Chao
,
Onasch, Timothy B
in
Absorption
,
Absorption coefficient
,
Absorptivity
2023
Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth’s radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming.Atmospheric short-wave absorption due to wildfire smoke is caused predominantly by dark brown carbon particles, according to observations from smoke plumes in the United States.
Journal Article
Source-specific light absorption by carbonaceous components in the complex aerosol matrix from yearly filter-based measurements
by
Modini, Robin L
,
Costa, Camilla
,
Danelli, Silvia G
in
Absorption
,
Absorption cross sections
,
Aerosol absorption
2021
Understanding the sources of light-absorbing organic (brown) carbon (BrC) and its interaction with black carbon (BC) and other non-refractory particulate matter (NR-PM) fractions is important for reducing uncertainties in the aerosol direct radiative forcing. In this study, we combine multiple filter-based techniques to achieve long-term, spectrally resolved, source- and species-specific atmospheric absorption closure. We determine the mass absorption efficiency (MAE) in dilute bulk solutions at 370 nm to be equal to 1.4 m² g⁻¹ for fresh biomass smoke, 0.7 m² g⁻¹ for winter-oxygenated organic aerosol (OA), and 0.13 m² g⁻¹ for other less absorbing OA. We apply Mie calculations to estimate the contributions of these fractions to total aerosol absorption. While enhanced absorption in the near-UV has been traditionally attributed to primary biomass smoke, here we show that anthropogenic oxygenated OA may be equally important for BrC absorption during winter, especially at an urban background site. We demonstrate that insoluble tar balls are negligible in residential biomass burning atmospheric samples of this study and thus could attribute the totality of the NR-PM absorption at shorter wavelengths to methanol-extractable BrC. As for BC, we show that the mass absorption cross-section (MAC) of this fraction is independent of its source, while we observe evidence for a filter-based lensing effect associated with the presence of NR-PM components. We find that bare BC has a MAC of 6.3 m² g⁻¹ at 660 nm and an absorption Ångström exponent of 0.93 ± 0.16, while in the presence of coatings its absorption is enhanced by a factor of ∼ 1.4. Based on Mie calculations of closure between observed and predicted total light absorption, we provide an indication for a suppression of the filter-based lensing effect by BrC. The total absorption reduction remains modest, ∼ 10 %–20 % at 370 nm, and is restricted to shorter wavelengths, where BrC absorption is significant. Overall, our results allow an assessment of the relative importance of the different aerosol fractions to the total absorption for aerosols from a wide range of sources and atmospheric ages. When integrated with the solar spectrum at 300–900 nm, bare BC is found to contribute around two-thirds of the solar radiation absorption by total carbonaceous aerosols, amplified by the filter-based lensing effect (with an interquartile range, IQR, of 8 %–27 %), while the IQR of the contributions by particulate BrC is 6 %–13 % (13 %–20 % at the rural site during winter). Future studies that will directly benefit from these results include (a) optical modelling aiming at understanding the absorption profiles of a complex aerosol composed of BrC, BC and lensing-inducing coatings; (b) source apportionment aiming at understanding the sources of BC and BrC from the aerosol absorption profiles; (c) global modelling aiming at quantifying the most important aerosol absorbers.
Journal Article
Evaluation of the absorption Ångström exponents for traffic and wood burning in the Aethalometer-based source apportionment using radiocarbon measurements of ambient aerosol
by
Prévôt, André S. H.
,
Herich, Hanna
,
Zhang, Yanlin
in
Absorption
,
Absorption coefficient
,
Absorption cross sections
2017
Equivalent black carbon (EBC) measured by a multi-wavelength Aethalometer can be apportioned to traffic and wood burning. The method is based on the differences in the dependence of aerosol absorption on the wavelength of light used to investigate the sample, parameterized by the source-specific absorption Ångström exponent (α). While the spectral dependence (defined as α values) of the traffic-related EBC light absorption is low, wood smoke particles feature enhanced light absorption in the blue and near ultraviolet. Source apportionment results using this methodology are hence strongly dependent on the α values assumed for both types of emissions: traffic αTR, and wood burning αWB. Most studies use a single αTR and αWB pair in the Aethalometer model, derived from previous work. However, an accurate determination of the source specific α values is currently lacking and in some recent publications the applicability of the Aethalometer model was questioned.Here we present an indirect methodology for the determination of αWB and αTR by comparing the source apportionment of EBC using the Aethalometer model with 14C measurements of the EC fraction on 16 to 40 h filter samples from several locations and campaigns across Switzerland during 2005–2012, mainly in winter. The data obtained at eight stations with different source characteristics also enabled the evaluation of the performance and the uncertainties of the Aethalometer model in different environments. The best combination of αTR and αWB (0.9 and 1.68, respectively) was obtained by fitting the Aethalometer model outputs (calculated with the absorption coefficients at 470 and 950 nm) against the fossil fraction of EC (ECF ∕ EC) derived from 14C measurements. Aethalometer and 14C source apportionment results are well correlated (r = 0.81) and the fitting residuals exhibit only a minor positive bias of 1.6 % and an average precision of 9.3 %. This indicates that the Aethalometer model reproduces reasonably well the 14C results for all stations investigated in this study using our best estimate of a single αWB and αTR pair. Combining the EC, 14C, and Aethalometer measurements further allowed assessing the dependence of the mass absorption cross section (MAC) of EBC on its source. Results indicate no significant difference in MAC at 880 nm between EBC originating from traffic or wood-burning emissions. Using ECF ∕ EC as reference and constant a priori selected αTR values, αWB was also calculated for each individual data point. No clear station-to-station or season-to-season differences in αWB were observed, but αTR and αWB values are interdependent. For example, an increase in αTR by 0.1 results in a decrease in αWB by 0.1. The fitting residuals of different αTR and αWB combinations depend on ECF ∕ EC such that a good agreement cannot be obtained over the entire ECF ∕ EC range using other α pairs. Additional combinations of αTR = 0.8, and 1.0 and αWB = 1.8 and 1.6, respectively, are possible but only for ECF ∕ EC between ∼ 40 and 85 %. Applying α values previously used in the literature such as αWB of ∼ 2 or any αWB in combination with αTR = 1.1 to our data set results in large residuals. Therefore we recommend to use the best α combination as obtained here (αTR = 0.9 and αWB = 1.68) in future studies when no or only limited additional information like 14C measurements are available. However, these results were obtained for locations impacted by black carbon (BC) mainly from traffic consisting of a modern car fleet and residential wood combustion with well-constrained combustion efficiencies. For regions of the world with different combustion conditions, additional BC sources, or fuels used, further investigations are needed.
Journal Article
Deriving brown carbon from multiwavelength absorption measurements: method and application to AERONET and Aethalometer observations
by
Artaxo, Paulo
,
Sedlacek, Arthur J.
,
Watson, Thomas B.
in
Absorption
,
Absorption coefficient
,
Absorptivity
2016
The radiative impact of organic aerosols (OA) is a large source of uncertainty in estimating the global direct radiative effect (DRE) of aerosols. This radiative impact includes not only light scattering but also light absorption from a subclass of OA referred to as brown carbon (BrC). However, the absorption properties of BrC are poorly understood, leading to large uncertainties in modeling studies. To obtain observational constraints from measurements, a simple absorption Ångström exponent (AAE) method is often used to separate the contribution of BrC absorption from that of black carbon (BC). However, this attribution method is based on assumptions regarding the spectral dependence of BC that are often violated in the ambient atmosphere. Here we develop a new AAE method which improves upon previous approaches by using the information from the wavelength-dependent measurements themselves and by allowing for an atmospherically relevant range of BC properties, rather than fixing these at a single assumed value. We note that constraints on BC optical properties and mixing state would help further improve this method. We apply this method to multiwavelength absorption aerosol optical depth (AAOD) measurements at AERONET sites worldwide and surface aerosol absorption measurements at multiple ambient sites. We estimate that BrC globally contributes up to 40 % of the seasonally averaged absorption at 440 nm. We find that the mass absorption coefficient of OA (OA-MAC) is positively correlated with the BC ∕ OA mass ratio. Based on the variability in BC properties and BC ∕ OA emission ratio, we estimate a range of 0.05–1.5 m2 g−1 for OA-MAC at 440 nm. Using the combination of AERONET and OMI UV absorption observations we estimate that the AAE388∕440 nm for BrC is generally ∼ 4 worldwide, with a smaller value in Europe (< 2). Our analyses of observations at two surface sites (Cape Cod, to the southeast of Boston, and the GoAmazon2014/5 T3 site, to the west of Manaus, Brazil) reveal no significant relationship between BrC absorptivity and photochemical aging in urban-influenced conditions. However, the absorption of BrC measured during the biomass burning season near Manaus is found to decrease with photochemical aging with a lifetime of ∼ 1 day. This lifetime is comparable to previous observations within a biomass burning plume but much slower than estimated from laboratory studies. Given the large uncertainties associated with AERONET retrievals of AAOD, the most challenging aspect of our analysis is that an accurate, globally distributed, multiple-wavelength aerosol absorption measurement dataset is unavailable at present. Thus, achieving a better understanding of the properties, evolution, and impacts of global BrC will rely on the future deployment of accurate multiple-wavelength absorption measurements to which AAE methods, such as the approach developed here, can be applied.
Journal Article
Atmospheric evolution of molecular-weight-separated brown carbon from biomass burning
by
Mihalopoulos, Nikolaos
,
Tsiodra, Irini
,
Kanakidou, Maria
in
Absorption
,
Absorption coefficient
,
Absorptivity
2019
Biomass burning is a major source of atmospheric brown carbon (BrC), and through its absorption of UV/VIS radiation, it can play an important role in the planetary radiative balance and atmospheric photochemistry. The considerable uncertainty of BrC impacts is associated with its poorly constrained sources, transformations, and atmospheric lifetime. Here we report laboratory experiments that examined changes in the optical properties of the water-soluble (WS) BrC fraction of laboratory-generated biomass burning particles from hardwood pyrolysis. Effects of direct UVB photolysis and OH oxidation in the aqueous phase on molecular-weight-separated BrC were studied. Results indicated that the majority of low-molecular-weight (MW) BrC (<400 Da) was rapidly photobleached by both direct photolysis and OH oxidation on an atmospheric timescale of approximately 1 h. High MW BrC (≥400 Da) underwent initial photoenhancement up to ∼15 h, followed by slow photobleaching over ∼10 h. The laboratory experiments were supported by observations from ambient BrC samples that were collected during the fire seasons in Greece. These samples, containing freshly emitted to aged biomass burning aerosol, were analyzed for both water- and methanol-soluble BrC. Consistent with the laboratory experiments, high-MW BrC dominated the total light absorption at 365 nm for both methanol and water-soluble fractions of ambient samples with atmospheric transport times of 1 to 68 h. These ambient observations indicate that overall, biomass burning BrC across all molecular weights has an atmospheric lifetime of 15 to 28 h, consistent with estimates from previous field studies – although the BrC associated with the high-MW fraction remains relatively stable and is responsible for light absorption properties of BrC throughout most of its atmospheric lifetime. For ambient samples of aged (>10 h) biomass burning emissions, poor linear correlations were found between light absorptivity and levoglucosan, consistent with other studies suggesting a short atmospheric lifetime for levoglucosan. However, a much stronger correlation between light absorptivity and total hydrous sugars was observed, suggesting that they may serve as more robust tracers for aged biomass burning emissions. Overall, the results from this study suggest that robust model estimates of BrC radiative impacts require consideration of the atmospheric aging of BrC and the stability of high-MW BrC.
Journal Article
Interfacial water engineering boosts neutral water reduction
2022
Hydrogen evolution reaction (HER) in neutral media is of great practical importance for sustainable hydrogen production, but generally suffers from low activities, the cause of which has been a puzzle yet to be solved. Herein, by investigating the synergy between Ru single atoms (RuNC) and RuSe
x
cluster compounds (RuSe
x
) for HER using ab initio molecular dynamics, operando X-ray absorption spectroscopy, and operando surface-enhanced infrared absorption spectroscopy, we establish that the interfacial water governs neutral HER. The rigid interfacial water layer in neutral media would inhibit the transport of H
2
O*/OH* at the electrode/electrolyte interface of RuNC, but the RuSe
x
can promote H
2
O*/OH* transport to increase the number of available H
2
O* on RuNC by disordering the interfacial water network. With the synergy of RuSe
x
and RuNC, the resulting neutral HER performance in terms of mass-specific activity is 6.7 times higher than that of 20 wt.% Pt/C at overpotential of 100 mV.
Understanding the slow kinetics of hydrogen evolution reaction in neutral media is of fundamental importance for the rational design of high-performance electrocatalysts for hydrogen energy. Here, by studying Ru single atom and RuSe
x
cluster, the authors report how the rate of hydrogen evolution reaction activity in neutral media is governed by interfacial water.
Journal Article
High performance from extraordinarily thick organic light-emitting diodes
by
Sandanayaka, Atula S. D.
,
Leyden, Matthew R.
,
Bencheikh, Fatima
in
639/301/1005/1007
,
639/301/923/3931
,
Absorption
2019
Organic light-emitting diode (OLED) technology is promising for applications in next-generation displays and lighting. However, it is difficult—especially in large-area mass production—to cover a large substrate uniformly with organic layers, and variations in thickness cause the formation of shunting paths between electrodes
1
,
2
, thereby lowering device production yield. To overcome this issue, thicker organic transport layers are desirable because they can cover particles and residue on substrates, but increasing their thickness increases the driving voltage because of the intrinsically low charge-carrier mobilities of organics. Chemical doping of organic layers increases their electrical conductivity and enables fabrication of thicker OLEDs
3
,
4
, but additional absorption bands originating from charge transfer appear
5
, reducing electroluminescence efficiency because of light absorption. Thick OLEDs made with organic single crystals have been demonstrated
6
, but are not practical for mass production. Therefore, an alternative method of fabricating thicker OLEDs is needed. Here we show that extraordinarily thick OLEDs can be fabricated by using the organic–inorganic perovskite methylammonium lead chloride, CH
3
NH
3
PbCl
3
(MAPbCl
3
), instead of organics as the transport layers. Because MAPbCl
3
films have high carrier mobilities and are transparent to visible light, we were able to increase the total thickness of MAPbCl
3
transport layers to 2,000 nanometres—more than ten times the thickness of standard OLEDs—without requiring high voltage or reducing either internal electroluminescence quantum efficiency or operational durability. These findings will contribute towards a higher production yield of high-quality OLEDs, which may be used for other organic devices, such as lasers, solar cells, memory devices and sensors.
Extraordinarily thick organic light-emitting diodes can be fabricated using hybrid organic–inorganic perovskites as the transport layers, thus relaxing fabrication constraints without affecting their efficiency, voltage requirement or durability.
Journal Article
Impacts of biomass burning and photochemical processing on the light absorption of brown carbon in the southeastern Tibetan Plateau
by
Wang, Jin
,
Wang, Qiyuan
,
Tian, Jie
in
Absorption
,
Absorption coefficient
,
Absorption cross sections
2023
Brown carbon (BrC) in the atmosphere can greatly influence aerosol's radiative forcing over the Tibetan Plateau (TP) because it has the non-negligible capacity of light absorption compared to black carbon (BC); however, our understanding of optical properties, sources, and atmospheric processes of BrC in this region remains limited. In this study, a multiple-wavelength Aethalometer coupled with a quadrupole aerosol chemical speciation monitor was deployed to investigate the highly time resolved BrC in the submicron aerosol at the southeastern edge of the TP during the pre-monsoon season. The results showed that BrC made substantial contributions (20.0 %–40.2 %) to the light absorption of submicron aerosol from 370 to 660 nm. Organic aerosol (OA), an alternative to BrC, was split into a biomass burning OA (BBOA) with aging processes and a photochemical-oxidation-processed oxygenated OA (po-OOA) by a hybrid environmental receptor model analysis. Combined with the light absorption coefficient of BrC (babs-BrC), the source-specific mass absorption cross sections of BBOA (0.61–2.78 m2 g−1) and po-OOA (0.30–1.43 m2 g−1) at 370–660 nm were retrieved. On average, babs-BrC from po-OOA (1.3–6.0 Mm−1) was comparable to that from BBOA (1.3–6.0 Mm−1) at all wavelengths. The concentration-weighted trajectory analysis showed that the most important potential source regions for babs-BrC values from BBOA and po-OOA were located in northern Myanmar and along the China–Myanmar border, indicating the cross-border transport of BrC from Southeast Asia. A “simple forcing efficiency” evaluation further illustrated the importance of the BrC radiative effect with the high fractional radiative forcing by two OAs relative to BC (48.8 ± 15.5 %). This study highlights a significant influence of BrC of biomass burning origin and secondary formation on climate change over the TP region during the pre-monsoon season.
Journal Article
Determination of the multiple-scattering correction factor and its cross-sensitivity to scattering and wavelength dependence for different AE33 Aethalometer filter tapes: a multi-instrumental approach
by
Valentini, Sara
,
Rigler, Martin
,
Ivančič, Matic
in
Absorption
,
Absorption coefficient
,
Absorptivity
2021
Providing reliable observations of aerosol particles' absorption properties at spatial and temporal resolutions suited to climate models is of utter importance to better understand the effects that atmospheric particles have on climate. Nowadays, one of the instruments most widely used in international monitoring networks for in situ surface measurements of light absorption properties of atmospheric aerosol particles is the multi-wavelength dual-spot Aethalometer, AE33. The AE33 derives the absorption coefficients of aerosol particles at seven different wavelengths from the measurements of the optical attenuation of light through a filter where particles are continuously collected. An accurate determination of the absorption coefficients from the AE33 instrument relies on the quantification of the non-linear processes related to the sample collection on the filter. The multiple-scattering correction factor (C), which depends on the filter tape used and on the optical properties of the collected particles, is the parameter with both the greatest uncertainty and the greatest impact on the absorption coefficients derived from the AE33 measurements. Here we present an in-depth analysis of the AE33 multiple-scattering correction factor C and its wavelength dependence for two different and widely used filter tapes, namely the old, and most referenced, TFE-coated glass, or M8020, filter tape and the currently, and most widely used, M8060 filter tape. For performing this analysis, we compared the attenuation measurements from AE33 with the absorption coefficients measured with different filter-based techniques. On-line co-located multi-angle absorption photometer (MAAP) measurements and off-line PP_UniMI polar photometer measurements were employed as reference absorption measurements for this work. To this aim, we used data from three different measurement stations located in the north-east of Spain, namely an urban background station (Barcelona, BCN), a regional background station (Montseny, MSY) and a mountaintop station (Montsec d'Ares, MSA). The median C values (at 637 nm) measured at the three stations ranged between 2.29 (at BCN and MSY, lowest 5th percentile of 1.97 and highest 95th percentile of 2.68) and 2.51 (at MSA, lowest 5th percentile of 2.06 and highest 95th percentile of 3.06). The analysis of the cross-sensitivity to scattering, for the two filter tapes considered here, revealed a large increase in the C factor when the single-scattering albedo (SSA) of the collected particles was above a given threshold, up to a 3-fold increase above the average C values. The SSA threshold appeared to be site dependent and ranged between 0.90 to 0.95 for the stations considered in the study. The results of the cross-sensitivity to scattering displayed a fitted constant multiple-scattering parameter, Cf, of 2.21 and 1.96, and a cross-sensitivity factor, ms, of 1.8 % and 3.4 % for the MSY and MSA stations, respectively, for the TFE-coated glass filter tape. For the M8060 filter tape, Cf values of 2.50, 1.96 and 1.82 and ms values of 1.6 %, 3.0 % and 4.9 % for the BCN, MSY and MSA stations, respectively, were obtained. SSA variations also influenced the spectral dependence of C, which showed an increase with wavelength when SSA was above the site-dependent threshold. Below the SSA threshold, no statistically significant dependence of C on the wavelength was observed. For the measurement stations considered here, the wavelength dependence of C was to some extent driven by the presence of dust particles during Saharan dust outbreaks that had the potential to increase the SSA above the average values. At the mountaintop station, an omission of the wavelength dependence of the C factor led to an underestimation of the absorption Ångström exponent (AAE) by up to 12 %. Differences in the absorption coefficient determined from AE33 measurements at BCN, MSY and MSA of around 35 %–40 % can be expected when using the site-dependent experimentally obtained C value instead of the nominal C value. Due to the fundamental role that the SSA of the particles collected on the filter tape has in the multiple-scattering parameter C, we present a methodology that allows the recognition of the conditions upon which the use of a constant and wavelength-independent C is feasible.
Journal Article