Future Automotive Aftertreatment Solutions: The 150?C Challenge Workshop Report

With future fuel economy standards enacted, the U.S. automotive manufacturers (OEMs) are committed to pursuing a variety of high risk/highly efficient stoichiometric and lean combustion strategies to achieve superior performance. In recognition of this need, the U.S. Department of Energy (DOE) has partnered with domestic automotive manufacturers through U.S. DRIVE to develop these advanced technologies. However, before these advancements can be introduced into the U.S. market, they must also be able to meet increasingly stringent emissions requirements. A significant roadblock to this implementation is the inability of current catalyst and aftertreatment technologies to provide the required activity at the much lower exhaust temperatures that will accompany highly efficient combustion processes and powertrain strategies. Therefore, the goal of this workshop and report is to create a U.S. DRIVE emission control roadmap that will identify new materials and aftertreatment approaches that offer the potential for 90% conversion of emissions at low temperature (150°C) and are consistent with highly efficient combustion technologies currently under investigation within U.S. DRIVE Advanced Combustion and Emission Control (ACEC) programs

Final Report of a CRADA Between Pacific Northwest National Laboratory and the Ford Motor Company (CRADA No. PNNL/265): ?Deactivation Mechanisms of Base Metal/Zeolite Urea Selective Catalytic Reduction Materials, and Development of Zeolite-Based Hydrocarbon Adsorber Materials?

Reducing NOx emissions and particulate matter (PM) are primary concerns for diesel vehicles required to meet current LEV II and future LEV III emission standards which require 90+% NOx conversion. Currently, urea SCR as the NOx reductant and a Catalyzed Diesel Particulate Filter (CDPF) are being used for emission control system components by Ford Motor Company for 2010 and beyond diesel vehicles. Because the use of this technology for vehicle applications is new, the relative lack of experience makes it especially challenging to satisfy durability requirements. Of particular concern is being able to realistically simulate actual field aging of the catalyst systems under laboratory conditions. This is necessary both as a rapid assessment tool for verifying improved performance and certifiability of new catalyst formulations, and to develop a good understanding of deactivation mechanisms that can be used to develop improved catalyst materials. In addition to NOx and PM, the hydrocarbon (HC) emission standards are expected to become much more stringent during the next few years. Meanwhile, the engine-out HC emissions are expected to increase and/or be more difficult to remove. Since HC can be removed only when the catalyst becomes warm enough for its oxidation, three-way catalyst (TWC) and diesel oxidation catalyst (DOC) formulations often contain proprietary zeolite materials to hold the HC produced during the cold start period until the catalyst reaches its operating temperature (e.g., >200°C). Unfortunately, much of trapped HC tends to be released before the catalyst reaches the operating temperature. Among materials effective for trapping HC during the catalyst warm-up period, siliceous zeolites are commonly used because of their high surface area and high stability under typical operating conditions. However, there has been little research on the physical properties of these materials related to the adsorption and release of various hydrocarbon species found in the engine exhaust. For these reasons, automakers and engine manufacturers have difficulty improving their catalytic converters for meeting the stringent HC emission standards. In this collaborative program, scientists and engineers in the Institute for Integrated Catalysis at Pacific Northwest National Laboratory and at Ford Motor Company have investigated laboratory- and engine-aged SCR catalysts, containing mainly base metal zeolites. These studies are leading to a better understanding of various aging factors that impact the long-term performance of SCR catalysts and improve the correlation between laboratory and engine aging, saving experimental time and cost. We have also studied materials effective for the temporary storage of HC species during the cold-start period. In particular, we have examined the adsorption and desorption of various HC species produced during the combustion with different fuels (e.g., gasoline, E85, diesel) over potential HC adsorber materials, and measured the kinetic parameters to update Ford’s HC adsorption model. Since this CRADA has now been completed, in this final report we will provide brief summaries of most of the work carried out on this CRADA over the last several years

EMSL and Institute for Integrated Catalysis (IIC) Catalysis Workshop

Within the context of significantly accelerating scientific progress in research areas that address important societal problems, a workshop was held in November 2010 at EMSL to identify specific and topically important areas of research and capability needs in catalysis-related science

Advanced Resources for Catalysis Science; Recommendations for a National Catalysis Research Institute

Catalysis is one of the most valuable contributors to our economy and historically an area where the United States has enjoyed, but is now losing, international leadership. While other countries are stepping up their work in this area, support for advanced catalysis research and development in the U.S. has diminished. Yet, more than ever, innovative and improved catalyst technologies are imperative for new energy production processes to ease our dependence on imported resources, for new energy-efficient and environmentally benign chemical production processes, and for new emission reduction technologies to minimize the environmental impact of an active and growing economy. Addressing growing concerns about the future direction of U.S. catalysis science, experts from the catalysis community met at a workshop to determine and recommend advanced resources needed to address the grand challenges for catalysis research and development. The workshop's primary conclusion: To recapture our position as the leader in catalysis innovation and practice, and promote crucial breakthroughs, the U.S. must establish one or more well-funded and well-equipped National Catalysis Research Institutes competitively selected, centered in the national laboratories and, by charter, networked to other national laboratories, universities, and industry. The Institute(s) will be the center of a national collaboratory that gives catalysis researchers access to the most advanced techniques available in the scientific enterprise. The importance of catalysis to our energy, economic, and environmental security cannot be overemphasized. Catalysis is a vital part of our core industrial infrastructure, as it is integral to chemical processing and petroleum refining, and is critical to proposed advances needed to secure a sustainable energy future. Advances in catalysis could reduce our need for foreign oil by making better use of domestic carbon resources, for example, allowing cost-effective and zero emission conversion of coal into transportation fuels. No matter what energy sources are being considered (oil, natural gas, coal, biomass, solar, or nuclear based), a clean, sustainable energy future will involve catalysis to improve energy efficiency and storage and use options, and to mitigate environmental impacts. Recent revolutionary advances in nanotechnology and high-performance computing are enabling the breakthroughs in catalysis science and technology essential for a secure energy future. Thus, the time is right for substantially increased investments in catalysis science and technology

Mid- and Far-Infrared Reflection/Absorption Spectroscopy (IRAS) Studies of NO on Rh Single Crystal Surfaces

The NO/CO reaction over Rh metal in automobile catalytic converters is critical to the control of emissions of these pollutant molecules. As part of a program to determine the elementary mechanism(s) of this reaction, we have been performing mid- and far-infrared reflection/absorption spectroscopic (IRAS) measurements of the adsorption and co-adsorption and co-adsorption of NO and CO on Rh single crystal surfaces. Of particular interest is the low-frequency range of the IRAS spectra where we hoped to observe features due to metal-N stretching and/or bending vibrational motions. In particular, we hoped to obtain information regarding the site-requirements for the dissociation of the NO molecule on various Rh single crystal surfaces. An important result from our earlier work is that the selectivity of the reaction for the two nitrogen-containing products, N2 and N2O, is a strong function of the Rh surface structure. On the basis of ancillary data, we suggested that the location of adsorbed NO and N-atoms (formed from dissociation of adsorbed NO) on various Rh surfaces could, perhaps account for the selectivity differences

Final Report of a CRADA Between Pacific Northwest National Laboratory and the General Motors Company (CRADA No. PNNL/271): “Degradation Mechanisms of Urea Selective Catalytic Reduction Technology”

Diesel engines can offer substantially higher fuel efficiency, good driving performance characteristics, and reduced carbon dioxide (CO2) emission compared to stoichiometric gasoline engines. Despite the increasing public demand for higher fuel economy and reduced dependency on imported oil, however, meeting the stringent emission standards with affordable methods has been a major challenge for the wide application of these fuel-efficient engines in the US market. The selective catalytic reduction of NOx by urea (urea-SCR) is one of the most promising technologies for NOx emission control for diesel engine exhausts. To ensure successful NOx emission control in the urea-SCR technology, both a diesel oxidation catalyst (DOC) and a urea-SCR catalyst with high activity and durability are critical for the emission control system. Because the use of this technology for light-duty diesel vehicle applications is new, the relative lack of experience makes it especially challenging to satisfy the durability requirements. Of particular concern is being able to realistically simulate actual field aging of the catalyst systems under laboratory conditions, which is necessary both as a rapid assessment tool for verifying improved performance and certifiability of new catalyst formulations. In addition, it is imperative to develop a good understanding of deactivation mechanisms to help develop improved catalyst materials. In this CRADA program, General Motors Company and PNNL have investigated fresh, laboratory- and vehicle-aged DOC and SCR catalysts. The studies have led to a better understanding of various aging factors that impact the long-term performance of catalysts used in the urea-SCR technology, and have improved the correlation between laboratory and vehicle aging for reduced development time and cost. This Final Report briefly highlights many of the technical accomplishments and documents the productivity of the program in terms of peer-reviewed scientific publications (2 total), reports (3 total including this Final Report), and presentations (5 total)

Final Report of a CRADA Between Pacific Northwest National Laboratory and the General Motors Company (CRADA No. PNNL/271): ?Degradation Mechanisms of Urea Selective Catalytic Reduction Technology?

Diesel engines can offer substantially higher fuel efficiency, good driving performance characteristics, and reduced carbon dioxide (CO2) emission compared to stoichiometric gasoline engines. Despite the increasing public demand for higher fuel economy and reduced dependency on imported oil, however, meeting the stringent emission standards with affordable methods has been a major challenge for the wide application of these fuel-efficient engines in the US market. The selective catalytic reduction of NOx by urea (urea-SCR) is one of the most promising technologies for NOx emission control for diesel engine exhausts. To ensure successful NOx emission control in the urea-SCR technology, both a diesel oxidation catalyst (DOC) and a urea-SCR catalyst with high activity and durability are critical for the emission control system. Because the use of this technology for light-duty diesel vehicle applications is new, the relative lack of experience makes it especially challenging to satisfy the durability requirements. Of particular concern is being able to realistically simulate actual field aging of the catalyst systems under laboratory conditions, which is necessary both as a rapid assessment tool for verifying improved performance and certifiability of new catalyst formulations. In addition, it is imperative to develop a good understanding of deactivation mechanisms to help develop improved catalyst materials. In this CRADA program, General Motors Company and PNNL have investigated fresh, laboratory- and vehicle-aged DOC and SCR catalysts. The studies have led to a better understanding of various aging factors that impact the long-term performance of catalysts used in the urea-SCR technology, and have improved the correlation between laboratory and vehicle aging for reduced development time and cost. This Final Report briefly highlights many of the technical accomplishments and documents the productivity of the program in terms of peer-reviewed scientific publications (2 total), reports (3 total including this Final Report), and presentations (5 total)

Final Report of a CRADA Between Pacific Northwest National Laboratory and the Ford Motor Company (CRADA No. PNNL/265): “Deactivation Mechanisms of Base Metal/Zeolite Urea Selective Catalytic Reduction Materials, and Development of Zeolite-Based Hydrocarbon Adsorber Materials”

Reducing NOx emissions and particulate matter (PM) are primary concerns for diesel vehicles required to meet current LEV II and future LEV III emission standards which require 90+% NOx conversion. Currently, urea SCR as the NOx reductant and a Catalyzed Diesel Particulate Filter (CDPF) are being used for emission control system components by Ford Motor Company for 2010 and beyond diesel vehicles. Because the use of this technology for vehicle applications is new, the relative lack of experience makes it especially challenging to satisfy durability requirements. Of particular concern is being able to realistically simulate actual field aging of the catalyst systems under laboratory conditions. This is necessary both as a rapid assessment tool for verifying improved performance and certifiability of new catalyst formulations, and to develop a good understanding of deactivation mechanisms that can be used to develop improved catalyst materials. In addition to NOx and PM, the hydrocarbon (HC) emission standards are expected to become much more stringent during the next few years. Meanwhile, the engine-out HC emissions are expected to increase and/or be more difficult to remove. Since HC can be removed only when the catalyst becomes warm enough for its oxidation, three-way catalyst (TWC) and diesel oxidation catalyst (DOC) formulations often contain proprietary zeolite materials to hold the HC produced during the cold start period until the catalyst reaches its operating temperature (e.g., >200°C). Unfortunately, much of trapped HC tends to be released before the catalyst reaches the operating temperature. Among materials effective for trapping HC during the catalyst warm-up period, siliceous zeolites are commonly used because of their high surface area and high stability under typical operating conditions. However, there has been little research on the physical properties of these materials related to the adsorption and release of various hydrocarbon species found in the engine exhaust. For these reasons, automakers and engine manufacturers have difficulty improving their catalytic converters for meeting the stringent HC emission standards. In this collaborative program, scientists and engineers in the Institute for Integrated Catalysis at Pacific Northwest National Laboratory and at Ford Motor Company have investigated laboratory- and engine-aged SCR catalysts, containing mainly base metal zeolites. These studies are leading to a better understanding of various aging factors that impact the long-term performance of SCR catalysts and improve the correlation between laboratory and engine aging, saving experimental time and cost. We have also studied materials effective for the temporary storage of HC species during the cold-start period. In particular, we have examined the adsorption and desorption of various HC species produced during the combustion with different fuels (e.g., gasoline, E85, diesel) over potential HC adsorber materials, and measured the kinetic parameters to update Ford’s HC adsorption model. Since this CRADA has now been completed, in this final report we will provide brief summaries of most of the work carried out on this CRADA over the last several years

EMSL and Institute for Integrated Catalysis (IIC) Catalysis Workshop

Within the context of significantly accelerating scientific progress in research areas that address important societal problems, a workshop was held in November 2010 at EMSL to identify specific and topically important areas of research and capability needs in catalysis-related science

Genetic studies of body mass index yield new insights for obesity biology

Note: A full list of authors and affiliations appears at the end of the article. Obesity is heritable and predisposes to many diseases. To understand the genetic basis of obesity better, here we conduct a genome-wide association study and Metabochip meta-analysis of body mass index (BMI), a measure commonly used to define obesity and assess adiposity, in up to 339,224 individuals. This analysis identifies 97 BMI-associated loci (P 20% of BMI variation. Pathway analyses provide strong support for a role of the central nervous system in obesity susceptibility and implicate new genes and pathways, including those related to synaptic function, glutamate signalling, insulin secretion/action, energy metabolism, lipid biology and adipogenesis.</p