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DOE OSTI2020

Optimization of Oxygen Electrode Combined with Soluble Catalyst to Enhance the Performance of Lithium-Oxygen Battery

Lithium-air batteries possess a high theoretical energy density among the current battery technologies, and are expected to become the driving power for electric vehicles. However, the practical application of lithium air batteries is handicapped by their poor cycle life, high over-charge potential and low energy efficiency. Numerous studies have performed to improve the kinetics of the electrochemical reaction. Making a good oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalyst system is under intense scrutiny. In this work, we report a rational design of air electrode, which derives from biomass and presents a three-dimensional porous carbon architecture with high specific surface and large volume expansion coefficient. Combining with a soluble catalyst, this oxygen electrode presents an ultrahigh areal specific capacity of 7.95 mAh/cm 2 and a long cycling life up to 1000 cycles with suppressed polarization (about 0.46 V). Finally, the greatly improved overall performance is due to the synergetic effect of the novel designed oxygen electrode capable of mediating the redox mediators to trigger the ORR and OER process.

25 ENERGY STORAGE↗

NASA NTRS2012

Modeling and Assimilating Ocean Color Radiances

Radiances are the source of information from ocean color sensors to produce estimates of biological and geochemical constituents. They potentially provide information on various other aspects of global biological and chemical systems, and there is considerable work involved in deriving new information from these signals. Each derived product, however, contains errors that are derived from the application of the radiances, above and beyond the radiance errors. A global biogeochemical model with an explicit spectral radiative transfer model is used to investigate the potential of assimilating radiances. The results indicate gaps in our understanding of radiative processes in the oceans and their relationships with biogeochemical variables. Most important, detritus optical properties are not well characterized and produce important effects of the simulated radiances. Specifically, there does not appear to be a relationship between detrital biomass and its optical properties, as there is for chlorophyll. Approximations are necessary to get beyond this problem. In this reprt we will discuss the challenges in modeling and assimilation water-leaving radiances and the prospects for improving our understanding of biogeochemical process by utilizing these signals.

Gregg, Watson↗

DOE OSTI2022

Frictional Contacts Between Individual Woody Biomass Particles under Wet and Dry Conditions

Friction between wood particles can be a critical property when designing processing equipment for creating cellulosic biofuels and similar natural products. Also, as wood processing is likely to occur year-round, understanding the friction between wet as well as dry wood particles can help design and model equipment, such as screw feeders. Here, a tribo-rheometry method was developed using a commercial rheometer that measured the torque required to rotate two contacting millimeter-scale wood chip particles. First, a range of normal forces were used to find the limits of the experimental method. Torque values were measured for seven pairs of wood chip particles at 1 N normal force under both dry and wet conditions, at both ambient conditions and in a humidity-controlled chamber. The torque required to rotate the wet particles was consistently higher than that of the dry particles, although differences were not quite statistically significant when measurements were performed at ambient conditions. Using humidity control resulted in torque values for wet particles of 1900 uNm and 900 uNm for dry particles. Finally, the friction coefficient was calculated as 0.23 for wet particles and 0.11 for dry particles when humidity was controlled. These frictions coefficients agreed with values for wood reported in the literature. Overall, controlling humidity is strongly recommended to quantify the range of friction for particles that uptake water, including granular systems from biomass to food to powders.

biomass↗

DOE OSTI2023

Iodide uptake by forest soils is principally related to the activity of extracellular oxidases

129 I is a nuclear fission decay product of concern because of its long half-life (16 Ma) and propensity to bioaccumulate. Microorganisms impact iodine mobility in soil systems by promoting iodination (covalent binding) of soil organic matter through processes that are not fully understood. Here, we examined iodide uptake by soils collected at two depths (0–10 and 10–20 cm) from 5 deciduous and coniferous forests in Japan and the United States. Autoclaved soils, and soils amended with an enzyme inhibitor (sodium azide) or an antibacterial agent (bronopol), bound significantly less 125 I tracer (93%, 81%, 61% decrease, respectively) than the untreated control soils, confirming a microbial role in soil iodide uptake. Correlation analyses identified the strongest significant correlation between 125 I uptake and three explanatory variables, actinobacteria soil biomass ( p = 6.04E-04, 1.35E-02 for Kendall-Tau and regression analysis, respectively), soil nitrogen content ( p = 4.86E-04, 4.24E-03), and soil oxidase enzyme activity at pH 7.0 using the substrate L-DOPA ( p = 2.83E-03, 4.33E-04) and at pH 5.5 using the ABTS ( p = 5.09E-03, 3.14E-03). Together, the results suggest that extracellular oxidases, primarily of bacterial origin, are the primary catalyst for soil iodination in aerobic, surface soils of deciduous and coniferous forests, and that soil N content may be indicative of the availability of binding sites for reactive iodine species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1988

Comparison of simulation modeling and satellite techniques for monitoring ecological processes

In 1985 improvements were made in the world climatic data base for modeling and predictive mapping; in individual process models and the overall carbon-balance models; and in the interface software for mapping the simulation results. Statistical analysis of the data base was begun. In 1986 mapping was shifted to NASA-Goddard. The initial approach involving pattern comparisons was modified to a more statistical approach. A major accomplishment was the expansion and improvement of a global data base of measurements of biomass and primary production, to complement the simulation data. The main accomplishments during 1987 included: production of a master tape with all environmental and satellite data and model results for the 1600 sites; development of a complete mapping system used for the initial color maps comparing annual and monthly patterns of Normalized Difference Vegetation Index (NDVI), actual evapotranspiration, net primary productivity, gross primary productivity, and net ecosystem production; collection of more biosphere measurements for eventual improvement of the biological models; and development of some initial monthly models for primary productivity, based on satellite data.

Box, Elgene O.↗

NASA NTRSDate not supplied

Improving the Representation of Land Surface Processes using the Data Assimilation Research Testbed (DART)

The land surface is a critical part of the earth system as processes related to water, carbon, energy and nitrogen cycling have important implications for climate forcing, air quality, water availability and seasonal atmospheric forecasting. Despite advances in land surface modeling, land surface model performance is often limited because of errors related to initial and boundary conditions, model structure, and parameters. Data assimilation (DA) techniques combined with an expanding network of earth system observations present an opportunity to reduce these errors and improve simulations. Here we apply an Ensemble Kalman Filter DA system as part of the Data Assimilation Research Testbed to a variety of land surface simulations. First, we describe the use of remotely sensed biomass observations to provide improved simulations of plant phenology, carbon and water cycling for regions highly sensitive to climate change (Western US, China, and Arctic). We discuss approaches to account for systemic biases between models and observations, including the use of spatially-varying adaptive ensemble inflation as an alternative approach to re-scaling soil moisture observations. Finally, we discuss a strategy to incorporate complementary observations (snow water equivalent, solar-induced fluorescence) to better constrain the representation of carbon and water cycling across complex terrain.

DART↗

DOE OSTI2021

DOE Energy Frontier Research Centers Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio)

New capabilities to predict, design and control the chemistries of carbon could answer a global imperative to transition from fossil-based to sustainable transportation fuels. While the use of inexpensive hydrocarbons has been an unparalleled achievement and enabler of economic prosperity for many nations, singular dependence upon crude oil has given rise to systemic vulnerabilities in climate, energy, economic, and national security. Lignocellulosic biomass, a renewable and carbon-neutral resource, has the potential to displace an estimated annual equivalent of three billion barrels of oil in the U.S. alone (National Research Council 2009, U. S. Department of Energy, 2011). However, biomass has only one-third the energy density of crude oil (Agrawal and Singh 2009, Richard 2010) and lacks petroleum’s versatility as a feedstock for fuels and chemicals. These limitations keep biomass conversion below the efficiency level needed for strategic impact while the scientific challenge of routing carbon from one molecular context to another remains unmet. In 2009, the Center for Direct Catalytic Conversion of Biomass to Biofuels (C3Bio) recognized the potential of chemical catalysis and fast pyrolysis to overcome such limitations by transforming the main components of biomass (cellulose, xylan, and lignin) from grasses and trees directly to liquid hydrocarbons and aromatic co-products. Enabled by the EFRC high-risk, high-reward approach to grand challenge science, C3Bio researchers have been key national players in disrupting the conventional paradigm of the cellulosic biorefinery into a new future of “no carbon left behind”—the full utilization of carbon from plant cell walls in energy-dense fuels (Fig. 1). We identified catalytic and fast-pyrolytic pathways that utilize cellulose, xylan and, most significantly, lignin. We developed catalytic processes that deoxygenate and transform monomers and isolated polymers into useful products and tested their use with intact biomass. We gained control of lignin synthesis within plants and initiated tailoring biomass to its end-use through the tools of plant molecular biology and genetic engineering. C3Bio breakthroughs have increased the energy density of biomass-derived substrates via catalytic and pyrolytic conversions into products such as benzoquinones, furfural and hydroxymethylfurfural, levoglucosan and levulinic acid, methoxypropylphenols and propylbenzene. Such advances in biomass conversion would not have been possible without simultaneous advances in analytical instrumentation and methodologies, and imaging technologies and applications. The legacy science developed by C3Bio enables design and control strategies for achieving a targeted product portfolio of fuel and chemical feedstocks from a diverse range of native and tailored biomass. Our research provides the knowledge base required for a bio-economy with product streams as diverse in functionality as those of the petrochemical industry. Coupling targeted computational modeling with experimentation, we achieved: (1) fundamental understanding of biopolymers and cell wall architecture assembly, (2) discovery of new chemistries that allow the development of highly selective pathways to fuels and desirable chemicals, and (3) an integrated systems-level understanding to control catalytic and pyrolytic pathways.

09 BIOMASS FUELS↗

NASA NTRS1996

The Application of Remote Sensing Data to GIS Studies of Land Use, Land Cover, and Vegetation Mapping in the State of Hawaii

A land cover-vegetation map with a base classification system for remote sensing use in a tropical island environment was produced of the island of Hawaii for the State of Hawaii to evaluate whether or not useful land cover information can be derived from Landsat TM data. In addition, an island-wide change detection mosaic combining a previously created 1977 MSS land classification with the TM-based classification was produced. In order to reach the goal of transferring remote sensing technology to State of Hawaii personnel, a pilot project was conducted while training State of Hawaii personnel in remote sensing technology and classification systems. Spectral characteristics of young island land cover types were compared to determine if there are differences in vegetation types on lava, vegetation types on soils, and barren lava from soils, and if they can be detected remotely, based on differences in pigments detecting plant physiognomic type, health, stress at senescence, heat, moisture level, and biomass. Geographic information systems (GIS) and global positioning systems (GPS) were used to assist in image rectification and classification. GIS was also used to produce large-format color output maps. An interactive GIS program was written to provide on-line access to scanned photos taken at field sites. The pilot project found Landsat TM to be a credible source of land cover information for geologically young islands, and TM data bands are effective in detecting spectral characteristics of different land cover types through remote sensing. Large agriculture field patterns were resolved and mapped successfully from wildland vegetation, but small agriculture field patterns were not. Additional processing was required to work with the four TM scenes from two separate orbits which span three years, including El Nino and drought dates. Results of the project emphasized the need for further land cover and land use processing and research. Change in vegetation composition was noted in the change detection image.

Hogan, Christine A.↗

DOE OSTI2021

Economic and Environmental Sustainability of an Integrated Direct Air Capture System with Advanced Algal Biofuel Production

The presentation titled Economic and Environmental Sustainability of an Integrated Direct Air Capture System with Advanced Algal Biofuel Production. The background and motivation of the presentation will encompass promotion of decarbonization of the atmosphere, decouple algae production facilities from anthropogenic CO2 sources, identify key economic drivers, minimize cost and greenhouse gas emissions through process integration and optimization.

algal biofuel production↗

DOE OSTI2023

Task 2.3: Continuous Counter-Current Chromatography

This task in the Separations Consortium focuses on the development of counter-current chromatography (CCC), which is an advanced liquid-liquid chromatography method. Today, CCC is primarily practiced in batch mode operation, but continuous operation will be required for at-scale deployment in a biorefinery setting. In this task, we are developing a continuous CCC process in collaboration with a company that builds CCC units. This work will be demonstrated on the biorefining challenge of lignin valorization. Specifically, we demonstrate use of continuous CCC for both monomer-monomer and monomer-oligomer separations in multiple lignin streams of relevance to the biorefining industry. Breakthroughs in this area would be useful for BETO goals in both sustainable aviation fuel and biochemicals production, including directly contributing to BETO's 2030 lignin valorization goal. Our approach includes developing new computational modeling approaches to optimize both batch and continuous CCC processes, experimental work to determine optimal solvent systems for multiple lignin streams sourced from BETO-funded projects and industrial collaborators, and techno-economic analysis and life cycle assessment to identify the most impactful areas to ultimately enable this approach in the biorefinery. This task overall will enable high-resolution, multi-component, continuous separations at scale, demonstrated on a grand challenge biorefining problem.

BIOMASS FUELS↗

NASA NTRS2020

Influence of Dynamic Ozone Dry Deposition on Ozone Pollution

Identifying the contributions of chemistry and transport to observed ozone pollution using regional‐to‐global models relies on accurate representation of ozone dry deposition. We use a recently developed configuration of the NOAA GFDL chemistry‐climate model – in which the atmosphere and land are coupled through dry deposition—to investigate the influence of ozone dry deposition on ozone pollution over northern midlatitudes. In our model, deposition pathways are tied to dynamic terrestrial processes, such as photosynthesis and water cycling through the canopy and soil. Small increases in winter deposition due to more process‐based representation of snow and deposition to surfaces reduce hemispheric‐scale ozone throughout the lower troposphere by 5–12 ppb, improving agreement with observations relative to a simulation with the standard configuration for ozone dry deposition. Declining snow cover by the end of the 21st‐century tempers the previously identified influence of rising methane on winter ozone. Dynamic dry deposition changes summer surface ozone by −4 to +7 ppb. While previous studies emphasize the importance of uptake by plant stomata, new diagnostic tracking of depositional pathways reveals a widespread impact of nonstomatal deposition on ozone pollution. Daily variability in both stomatal and nonstomatal deposition contribute to daily variability in ozone pollution. Twenty‐first century changes in summer deposition result from a balance among changes in individual pathways, reflecting differing responses to both high carbon dioxide (through plant physiology versus biomass accumulation) and water availability. Our findings highlight a need for constraints on the processes driving ozone dry deposition to test representation in regional‐to‐global models.

dry deposition↗

DOE OSTI2024

Integrating State Data Assimilation and Innovative Model Parameterization Reduces Simulated Carbon Uptake in the Arctic and Boreal Region

Model representation of carbon uptake and storage is essential for accurate projection of the response of the arctic-boreal zone to a rapidly changing climate. Land model estimates of LAI and aboveground biomass that can have a marked influence on model projections of carbon uptake and storage vary substantially in the arctic and boreal zone, making it challenging to correctly evaluate model estimates of Gross Primary Productivity (GPP). To understand and correct bias of LAI and aboveground biomass in the Community Land Model (CLM), we assimilated the 8-day Moderate Resolution Imaging Spectroradiometer (MODIS) LAI observation and a machine learning product of annual aboveground biomass into CLM using an Ensemble Adjustment Kalman Filter (EAKF) in an experimental region including Alaska and Western Canada. Assimilating LAI and aboveground biomass reduced these model estimates by 58% and 72%, respectively. The change of aboveground biomass was consistent with independent estimates of canopy top height at both regional and site levels. The International Land Model Benchmarking system assessment showed that data assimilation significantly improved CLM's performance in simulating the carbon and hydrological cycles, as well as in representing the functional relationships between LAI and other variables. Here, to further reduce the remaining bias in GPP after LAI bias correction, we re-parameterized CLM to account for low temperature suppression of photosynthesis. The LAI bias corrected model that included the new parameterization showed the best agreement with model benchmarks. Combining data assimilation with model parameterization provides a useful framework to assess photosynthetic processes in LSMs.

58 GEOSCIENCES↗

NASA NTRS2004

Response of graywater recycling systems based on hydroponic plant growth to three classes of surfactants

Anionic (sodium laureth sulfate, SLES), amphoteric (cocamidopropyl betaine, CAPB) and nonionic (alcohol polyethoxylate, AE) surfactants were added to separate nutrient film technique (NFT) hydroponic systems containing dwarf wheat (Triticum aestivum cv. USU Apogee) in a series of 21 day trials. Surfactant was added either in a (1). temporally dynamic mode (1-3 g surfactant m(-2) growing area d(-1)) as effected by automatic addition of a 300 ppm surfactant solution to meet plant water demand, or (2). continuous mode (2 g surfactant m(-2) growing area d(-1)) as effected by slow addition (10 mLh(-1)) of a 2000 ppm surfactant solution beginning at 4d after planting. SLES showed rapid primary degradation in both experiments, with no accumulation 24 h after initial addition. CAPB and AE were degraded less rapidly, with 30-50% remaining 24 h after initial addition, but CAPB and AE levels were below detection limit for the remainder of the study. No reductions in vegetative growth of wheat were observed in response to SLES, but biomass was reduced 20-25% with CAPB and AE. Microbial communities associated with both the plant roots and wetted hardware surfaces actively degraded the surfactants, as determined by monitoring surfactant levels following pulse additions at day 20 (with plants) and day 21 (after plant removal). In order to test whether the biofilm communities could ameliorate phytotoxicity by providing a microbial community acclimated for CAPB and AE decay, the continuous exposure systems were planted with wheat seeds after crop removal at day 21. Acclimation resulted in faster primary degradation (>90% within 24h) and reduced phytotoxicity. Overall, the studies indicate that relatively small areas (3-5m(2)) of hydroponic plant systems can process per capita production of mixed surfactants (5-10 g x person(-1)d(-1)) with minimal effects on plant growth.

Hydroponics↗

DOE OSTI2024

Lignin molecular weights of Populus trichocarpa residues after CELF pretreatment

Here we present a dataset of molecular weights of lignin from a woody energy crop (Populus trichocarpa) residues after a series of co-solvent enhanced lignocellulosic fractionation (CELF) pretreatment. The natural poplar variant GW-9947 from the Center for Bioenergy Innovation (CBI) was used. The poplar was knife milled and passed through a 1 mm sieve and CELF pretreatment was performed in a Parr autoclave reactor with 7.5 wt % solids loading, 0.5 wt% H2SO4 as catalyst at 150°C with various time. Tetrahydrofuran was added in a 1:1 mass ratio with water as the pretreatment solvent. Lignin was isolated from the pretreated samples after ball-milling in a porcelain jar with ceramic balls via Retsch PM 200 at 580 rpm for 2.5 h followed by enzymatic hydrolysis in acetate buffer (pH 4.8, 50 °C) for 48 h. The solid residue was isolated by centrifugation and hydrolyzed again with freshly added buffer and enzymes for another 48 h. After filtration, the solid residue was extracted twice with 96% (v/v) 1,4-dioxane/water mixture at room temperature overnight. The extracts were combined, rotary evaporated, and freeze-dried to recover lignin. The lignin samples were then derivatized in an acetic anhydride/pyridine (1:1, v/v) mixture and stirred at room temperature for 24 h. Ethanol was added to the reaction mixture, left for 30 min and then removed with a rotary evaporator. The addition and removal of ethanol was repeated at least 3 times until all traces of acetic acid were removed. Acetylated lignin samples were then dissolved in tetrahydrofuran (THF) at a concentration of 1.0 mg/mL. The molecular weight of acetylated lignin was measured by a gel permeation chromatography (GPC) on a PSS-Polymer Standards Service (Warwick, RI, USA) GPC SECurity 1200 system featuring Agilent HPLC 1200 components equipped with four Waters Styragel columns (HR1, HR2, HR4 and HR6) and an UV detector (270 nm). Tetrahydrofuran was used as the mobile phase and flow rate was 0.3 mL/min. The Polymer Standards Service WinGPC Unity software (Build 6807) was used for data processing for all the samples. The data provides information about the effects of CELF pretreatment time at 150 ºC on lignin molecular weights.

09 BIOMASS FUELS↗

DOE OSTI2021

Higher Energy-Content Jet Blending Components Derived from Ethanol (CRADA 467)

This project aims to develop a new sustainable aviation fuel (SAF) that comprises favorable properties, such as high energy density, excellent thermal stability, and favorable cold fold properties. Through catalyst development, this work will provide a route to control the cycloalkane/n-alkane/iso alkane content of a next-generation fuel with minimal or no aromatic content. Combining n-alkane and iso-alkane streams (high specific energy, MJ/kg) with cycloalkanes (higher energy density, MJ/L), is expected to enable at least a 4% net increase in combined (specific (MJ/kg) and volumetric (MJ/L)) energy content without impacting ‘drop-in’ fuel requirements, such as seal swelling. PNNL and LanzaTech have already demonstrated a sustainable, non-petroleum, route to isoalkanes. However, economically attractive cycloalkane production from waste and biomass is challenged by large hydrogen requirements, preferential selectivity to aromatic compounds and low yields to jet fuel range components. Many gaps in understanding cycloalkane properties and performance in complex jet fuel mixtures remain. The close tie and integration of Purdue’s fuel property analysis, with PNNL’s process development, can lead to an economically attractive process. The fuel analysis and testing by Purdue will enable a robust understanding of the properties and behavior of the cycloalkanes produced to inform process development. Additionally, seal-swelling analysis will quantify the ability of fuel blends with zero or minimal aromatics content to satisfy the seal swell requirement of O rings. Lastly, Purdue’s system-level analysis will lead to the development of a roadmap for deployment in key regions that considers system pressures such as hydrogen, water, energy efficiency, and ease of infrastructure access.

10 SYNTHETIC FUELS↗

DOE OSTI2020

Nucleophilic Thiols Reductively Cleave Ether Linkages in Lignin Model Polymers and Lignin

Lignin may serve as a renewable feedstock for the production of chemicals and fuels if mild, scalable processes for its depolymerization can be devised. The use of small organic thiols represents a bioinspired strategy to cleave the β–O–4 bond, the most common linkage in lignin. In the present study, synthetic β–O–4 linked polymers were treated with organic thiols, yielding up to 90 % cleaved monomer products. Lignin extracted from poplar was also treated with organic thiols resulting in molecular weight reductions as high as 65 % (Mn) in oxidized lignin. Thiol–based cleavage of other lignin linkages was also explored in small–molecule model systems to uncover additional potential pathways by which thiols might depolymerize lignin. The success of thiol–mediated cleavage on model dimers, polymers, and biomass–derived lignin illustrates the potential utility of small redox–active molecules to penetrate complex polymer matrices for depolymerization and subsequent valorization of lignin into fuels and chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Rewetting of soil: Revisiting the origin of soil CO 2 emissions

Rewetting dry soils is associated with a burst of microbial activity and mineralization, which manifests itself as a pulse in soil CO 2 emissions, long-known as the Birch effect. In arid and semi-arid systems, soil CO 2 losses upon rewetting at the end of extended dry periods can contribute a significant fraction to the overall carbon (C) budget. Microbial biomass is one of the sources of mineralized C, as was demonstrated over 30 years ago (Kieft et al., 1987). The present paper offers a perspective on how the field has progressed since the 1987 paper was published in Soil Biology & Biochemistry, what it means in terms of current concerns about global climate change, and the needs and potential emphases of future research. Many studies since 1987 have addressed the origin of this CO 2 pulse, finding multiple possible C sources involving both biotic and abiotic processes. We propose that the magnitude of the rewetting event (Δψ) determines the relative contribution from the array of substrates that contribute to the soil CO 2 pulse upon rewetting. The magnitude of the CO 2 pulse is likely related to soil physical characteristics and to the size of the available C pool, which is partly controlled by plants. Further, the relative contributions of the mechanisms generating soil CO 2 pulses upon rewetting are likely to be modified by climate change. To understand and predict the magnitude of soil CO 2 pulses upon rewetting, we advocate continued cross-disciplinary research involving soil microbial ecology, soil physics, soil chemistry, as well as increased integration and recognition of the importance of plant-soil interactions in controlling the soil C pools contributing to soil CO 2 pulses.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2013

Bounding the Role of Black Carbon in the Climate System: a Scientific Assessment

Black carbon aerosol plays a unique and important role in Earth's climate system. Black carbon is a type of carbonaceous material with a unique combination of physical properties. This assessment provides an evaluation of black-carbon climate forcing that is comprehensive in its inclusion of all known and relevant processes and that is quantitative in providing best estimates and uncertainties of the main forcing terms: direct solar absorption; influence on liquid, mixed phase, and ice clouds; and deposition on snow and ice. These effects are calculated with climate models, but when possible, they are evaluated with both microphysical measurements and field observations. Predominant sources are combustion related, namely, fossil fuels for transportation, solid fuels for industrial and residential uses, and open burning of biomass. Total global emissions of black carbon using bottom-up inventory methods are 7500 Gg/yr in the year 2000 with an uncertainty range of 2000 to 29000. However, global atmospheric absorption attributable to black carbon is too low in many models and should be increased by a factor of almost 3. After this scaling, the best estimate for the industrial-era (1750 to 2005) direct radiative forcing of atmospheric black carbon is +0.71 W/sq m with 90% uncertainty bounds of (+0.08, +1.27)W/sq m. Total direct forcing by all black carbon sources, without subtracting the preindustrial background, is estimated as +0.88 (+0.17, +1.48) W/sq m. Direct radiative forcing alone does not capture important rapid adjustment mechanisms. A framework is described and used for quantifying climate forcings, including rapid adjustments. The best estimate of industrial-era climate forcing of black carbon through all forcing mechanisms, including clouds and cryosphere forcing, is +1.1 W/sq m with 90% uncertainty bounds of +0.17 to +2.1 W/sq m. Thus, there is a very high probability that black carbon emissions, independent of co-emitted species, have a positive forcing and warm the climate. We estimate that black carbon, with a total climate forcing of +1.1 W/sq m, is the second most important human emission in terms of its climate forcing in the present-day atmosphere; only carbon dioxide is estimated to have a greater forcing. Sources that emit black carbon also emit other short-lived species that may either cool or warm climate. Climate forcings from co-emitted species are estimated and used in the framework described herein. When the principal effects of short-lived co-emissions, including cooling agents such as sulfur dioxide, are included in net forcing, energy-related sources (fossil fuel and biofuel) have an industrial-era climate forcing of +0.22 (0.50 to +1.08) W/sq m during the first year after emission. For a few of these sources, such as diesel engines and possibly residential biofuels, warming is strong enough that eliminating all short-lived emissions from these sources would reduce net climate forcing (i.e., produce cooling). When open burning emissions, which emit high levels of organic matter, are included in the total, the best estimate of net industrial-era climate forcing by all short-lived species from black-carbon-rich sources becomes slightly negative (0.06 W/sq m with 90% uncertainty bounds of 1.45 to +1.29 W/sq m). The uncertainties in net climate forcing from black-carbon-rich sources are substantial, largely due to lack of knowledge about cloud interactions with both black carbon and co-emitted organic carbon. In prioritizing potential black-carbon mitigation actions, non-science factors, such as technical feasibility, costs, policy design, and implementation feasibility play important roles. The major sources of black carbon are presently in different stages with regard to the feasibility for near-term mitigation. This assessment, by evaluating the large number and complexity of the associated physical and radiative processes in black-carbon climate forcing, sets a baseline from which to improve future climate forcing estimates.

black carbon↗