Pacific Northwest National Laboratory

About: Pacific Northwest National Laboratory is a facility organization based out in Richland, Washington, United States. It is known for research contribution in the topics: Catalysis & Aerosol. The organization has 11581 authors who have published 27934 publications receiving 1120489 citations. The organization is also known as: PNL & PNNL.

Radiative forcing of the direct aerosol effect from AeroCom Phase II simulations

Abstract: We report on the AeroCom Phase II direct aerosol effect (DAE) experiment where 16 detailed global aerosol models have been used to simulate the changes in the aerosol distribution over the industrial era. All 16 models have estimated the radiative forcing (RF) of the anthropogenic DAE, and have taken into account anthropogenic sulphate, black carbon (BC) and organic aerosols (OA) from fossil fuel, biofuel, and biomass burning emissions. In addition several models have simulated the DAE of anthropogenic nitrate and anthropogenic influenced secondary organic aerosols (SOA). The model simulated all-sky RF of the DAE from total anthropogenic aerosols has a range from −0.58 to −0.02 Wm−2, with a mean of −0.27 Wm−2 for the 16 models. Several models did not include nitrate or SOA and modifying the estimate by accounting for this with information from the other AeroCom models reduces the range and slightly strengthens the mean. Modifying the model estimates for missing aerosol components and for the time period 1750 to 2010 results in a mean RF for the DAE of −0.35 Wm−2. Compared to AeroCom Phase I (Schulz et al., 2006) we find very similar spreads in both total DAE and aerosol component RF. However, the RF of the total DAE is stronger negative and RF from BC from fossil fuel and biofuel emissions are stronger positive in the present study than in the previous AeroCom study. We find a tendency for models having a strong (positive) BC RF to also have strong (negative) sulphate or OA RF. This relationship leads to smaller uncertainty in the total RF of the DAE compared to the RF of the sum of the individual aerosol components. The spread in results for the individual aerosol components is substantial, and can be divided into diversities in burden, mass extinction coefficient (MEC), and normalized RF with respect to AOD. We find that these three factors give similar contributions to the spread in results.

Toward a Minimal Representation of Aerosols in Climate Models: Description and Evaluation in the Community Atmosphere Model CAM5

Abstract: . A modal aerosol module (MAM) has been developed for the Community Atmosphere Model version 5 (CAM5), the atmospheric component of the Community Earth System Model version 1 (CESM1). MAM is capable of simulating the aerosol size distribution and both internal and external mixing between aerosol components, treating numerous complicated aerosol processes and aerosol physical, chemical and optical properties in a physically-based manner. Two MAM versions were developed: a more complete version with seven lognormal modes (MAM7), and a version with three lognormal modes (MAM3) for the purpose of long-term (decades to centuries) simulations. In this paper a description and evaluation of the aerosol module and its two representations are provided. Sensitivity of the aerosol lifecycle to simplifications in the representation of aerosol is discussed. Simulated sulfate and secondary organic aerosol (SOA) mass concentrations are remarkably similar between MAM3 and MAM7. Differences in primary organic matter (POM) and black carbon (BC) concentrations between MAM3 and MAM7 are also small (mostly within 10%). The mineral dust global burden differs by 10% and sea salt burden by 30–40% between MAM3 and MAM7, mainly due to the different size ranges for dust and sea salt modes and different standard deviations of the log-normal size distribution for sea salt modes between MAM3 and MAM7. The model is able to qualitatively capture the observed geographical and temporal variations of aerosol mass and number concentrations, size distributions, and aerosol optical properties. However, there are noticeable biases; e.g., simulated BC concentrations are significantly lower than measurements in the Arctic. There is a low bias in modeled aerosol optical depth on the global scale, especially in the developing countries. These biases in aerosol simulations clearly indicate the need for improvements of aerosol processes (e.g., emission fluxes of anthropogenic aerosols and precursor gases in developing countries, boundary layer nucleation) and properties (e.g., primary aerosol emission size, POM hygroscopicity). In addition, the critical role of cloud properties (e.g., liquid water content, cloud fraction) responsible for the wet scavenging of aerosol is highlighted.

Nanoscaffold Mediates Hydrogen Release and the Reactivity of Ammonia Borane

Abstract: One of the imposing barriers to realizing the promise of an energy economy based on hydrogen is onboard hydrogen storage for fuel-cell-powered vehicles. New materials that enable the release of dense, plentiful and pure hydrogen at temperatures less than 85 oC are necessary to move the world from an oil-based economy to a hydrogen economy. We report a novel approach in which we deposit a hydrogen-rich material into a nanoporous scaffold. The role of the scaffold is to impose a nano-phase structure on the hydrogen-rich material thus providing an additional handle on the kinetics and thermodynamics of hydrogen release. We demonstrate on the example of ammonia borane infused in the nanoporous silica that the kinetics of hydrogen release is improved while the purity of hydrogen is increased in comparison with the release from bulk ammonia borane. These findings suggest that hydrogen rich materials infused in nanoscaffolds offer the most promising approach to date for onboard hydrogen storage

Production of levulinic acid and use as a platform chemical for derived products

Abstract: Levulinic acid (LA) can be produced cost effectively and in high yield from renewable feedstocks in a new industrial process. The technology is being demonstrated on a 1 ton/day scale at a facility in South Glens Falls, New York. Low cost LA can be used as a platform chemical for the production of a wide range of value-added products. This research has demonstrated that LA can be converted to methyltetrahydrofuran (MTHF), a solvent and fuel extender. MTHF is produced in >80% molar yield via a single stage catalytic hydrogenation process. A new preparation of δ-aminolevulinic acid (DALA), a broad spectrum herbicide, from LA has also been developed. Each step in this new process proceeds in high (>80%) yield and affords DALA (as the hydrochloride salt) in >90% purity, giving a process that could be commercially viable. LA is also being investigated as a starting material for the production of diphenolic acid (DPA), a direct replacement for bisphenol A.