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Oxide interfaces in disarray

Microscope image, bright blue background with bright green oxides

Atomic-scale imaging informs interface models for oxygen defect formation during disordering of oxides used in energy and computing.

| PNNL

Exploration of disorder at material interfaces could lead to better device performance

March 3, 2020
March 3, 2020
Highlight

The structure of an interface at which two materials meet helps determine the performance of the computers and other devices we use every day. However, understanding and controlling interface disorder at the atomic level is a difficult materials science challenge.

A research team at PNNL and Texas A&M University combined cutting edge imaging and numerical simulations to examine disordering processes in widely used oxide materials. They found that certain oxide interface configurations remain stable in extreme environments, suggesting ways to build better performing, more reliable devices for fuel cells, space-based electronics, and nuclear energy.

Visualizing the disordering process

As reported in Advanced Materials Interfaces (Asymmetric Lattice Disorder Induced at Oxide Interfaces,” DOI: 10.1002/admi.201901944) the team set out to examine interfaces between pyrochlore-like and perovskite oxides, two common classes of functional materials used in energy and computing technologies. While most past work has focused on individual bulk materials, less attention has been paid to interfaces connecting them, as would be the case in a device. In particular, it is not clear how interface features, such as composition, bonding, and possible defects, govern disordering processes.

Funded by PNNL’s Nuclear Process Science Initiative (NPSI), the team employed experimental and theoretical methods to study the interface at different stages of disorder introduced through ion irradiation. They imaged the local structure of the material using high-resolution scanning transmission electron microscopy and convergent beam electron diffraction, which showed that the bulk of the two materials disordered (amorphized) before the interface. After further irradiating the material, they found that a band region near the interface had remained crystalline, while the rest of the structure had become amorphous.

To understand this behavior, the team turned to a technique called electron energy loss spectroscopy, which allowed them to examine the atomic-scale chemistry and defects formed at the interface. Their measurements revealed the presence of substantial amounts of defects called oxygen vacancies, which can greatly affect properties such as magnetism and conductivity. Based on these observations, the team constructed a theoretical model of the interface and explored the effect of different interface configurations on the tendency to form vacancies.

“In our model we are able to systematically vary interface features, such as crystal structure, intermixing, and strain, to see their effect on defect formation. We found that the structure of the materials on both sides of the interface can influence where defects are likely to form first,” explained Steven R. Spurgeon, a PNNL materials scientist. “Our model suggests that by selecting appropriate crystal structures and controlling how they connect, it may be possible to dictate the sequence of defect formation, which would allow us to enhance the properties of these materials.”

The team is exploring other interface structures and chemistries, with an eye toward improving the performance of oxides used in extreme environments.

The study was conducted as part of the NPSI project, “Damage Mechanisms and Defect Formation in Irradiated Model Systems,” led by Spurgeon.

Research Team

Steven Spurgeon (PNNL), Tiffany Kaspar (PNNL), Vaithiyalingam Shutthanandan (Environmental Molecular Sciences Laboratory at PNNL), Jonathan Gigax (Texas A&M), Lin Shao (Texas A&M), Michel Sassi (PNNL).
February 20, 2020

Improving nuclear waste storage models by studying the chemistry of material interactions

A female researcher wearing a blue lab coat and heat-resistant safety gloves pours molten glass out of a metal crucible onto a metal tray.

PNNL conducts research into glass, glass-ceramic, grout, metal, and metal-ceramic wasteforms that will withstand corrosion over geologic time.

PNNL | Andrea Starr

WastePD EFRC research on the glass-steel interface was published in Nature Materials

February 3, 2020
February 3, 2020
Highlight

New research unravels the chemistry of how materials in the waste packages used for the disposal of high-level radioactive waste interact in deep geologic repository environments. Having a better understanding of the interactions between materials under various conditions provides more information to make waste storage performance models more robust.

“Many performance models use conservative approaches such as assuming that the steel canister walls don’t even exist or that they dissolve very fast. This study provides the opportunity to better incorporate the canister barrier in the models,” said Joseph Ryan, a PNNL materials scientist and coauthor on the paper, “Self-accelerated corrosion of nuclear waste forms at material interfaces,” published in Nature Materials.

The United States is converting highly radioactive nuclear waste, also known as high-level waste, into glass. The molten glass is poured into steel canisters for long-term storage and ultimate disposal in a geologic repository. The goal is to design waste storage and disposal systems that would remain safe for hundreds of thousands of years to come, even if they are exposed to water. Because of the extensive time span of waste storage, researchers turn to cutting-edge science to project what will happen during that time period. The data is used to inform extensive safety analyses—helping make sure the system is engineered to be compatible with the natural system so that waste remains separate from the environment.

“We can’t just do a test on a material and say, ‘That material corroded this much in 30 days and extrapolate that to a million years.’ It doesn’t work that way,” Ryan said. “At the most basic level, we try to understand the underlying chemistry of corrosion. Then, we feed that information into computer models to calculate the expected release over time.”

In this study, led by the WastePD Energy Frontier Research Center based at Ohio State University, researchers unpacked the chemistry that occurs when two materials are close together, focusing on glass-steel along with ceramic-steel interactions. This chemical situation could occur when water has percolated into the repository and has breached the steel canister, exposing the glass-steel interface to water.

When water finally breaches the waste package container, it will fill the microscopic space that forms between the solid glass and the steel canister. Chemical reactions that happen in localized and tiny microenvironments such as these can be quite different than those happening in a more open setting. In this case, this localized area can have a different chemistry than the surrounding solution, causing more corrosion than would be expected.

The researchers tested their theory in the laboratory. They pressed glass and steel together in salty liquid and kept it at 90° C (194° F) for a month. At the end of the experiment, they found differences in the width of thin layers that indicated higher corrosion between the glass-steel couple interface than in a control sample.

Why it matters: This research allows scientists to improve models that project how a disposal canister could perform in a deep geologic environment. Having a better understanding of the interactions between materials under various conditions provides more information to make the models more robust. Currently, some models project what happens to waste under the assumption that the steel canister walls do not exist. Operating under this pretext can result in higher projections of waste degradation than would likely occur when taking a conservative approach. But better understanding the chemistry of how the solid waste and the steel canister interact allows a scientifically based understanding of how the canisters behave and interact with the glass to be included in performance assessment models.

Summary: High-level waste is immobilized as glass in stainless steel canisters. On cooling, a confined crevice space forms at the stainless steel-glass interface. If the disposal canister is breached and if water can enter the steel-glass interface, it could result in anodic dissolution of the stainless steel, generating metal cations, which hydrolyze to form protons and strongly increase the local acidity. This acidic environment may locally enhance the corrosion of both the stainless steel and the glass, which leads to the release of cations from the glass. Further, the coupled corrosion may trigger the precipitation of additional secondary phases that may impact subsequent canister corrosion or nuclear glass durability.

What’s Next: While this study sheds light on the chemical interactions that occur at the stainless steel-glass interface, there are more interactions to explore. Ultimately, a better understanding of different chemical mechanisms will improve the overall performance model.

Acknowledgements

Sponsors: This work was supported as part of the Center for Performance and Design of Nuclear Waste Forms and Containers, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award no. DESC0016584.

Research Team: Xiaolei Guo, Gerald S. Frankel, Gopal Viswanathan, Tianshu Li (Ohio State University); Stéphane Gin (CEA, France); Penghui Lei, Tiankai Yao, Jie Lian (Rensselaer Polytechnic Institute); Hongshen Liu, Dien Ngo, Seong H. Kim (Pennsylvania State University); Daniel K. Schreiber, John D. Vienna, Joseph V. Ryan (PNNL); Jincheng Du (University of North Texas)

January 27, 2020
DECEMBER 4, 2019
Web Feature

A More Painless Extraction

PNNL and Argonne researchers developed and tested a chemical process that successfully captures radioactive byproducts from used nuclear fuel so they could be sent to advanced reactors for destruction while also producing electrical power.

PNNL Launches Marine Renewable Energy Database

Logo of Tethys Engineering

PNNL created an online database to share information related to the marine renewable energy industry.

Tethys Engineering addresses industry’s technical and engineering challenges

November 18, 2019
November 18, 2019
Highlight

Marine renewable energy (MRE) has the potential to provide 90 gigawatts of power in the United States through waves and tidal and ocean currents.

To harness the ocean’s energy, the MRE industry needs to understand how to address technical and engineering challenges such as efficient power takeoff, device survivability, and grid integration.

PNNL developed Tethys Engineering in September 2019 to allow sharing resources around the deployment of devices in corrosive, high-energy marine environments. The recently launched Tethys Engineering online database includes collected and curated documents surrounding the technical and engineering development of MRE devices. Users can search and filter results to intuitively identify information relevant to developers, researchers, and regulators.

Tethys Engineering includes more than 3,000 journal articles, conference papers, reports, and presentations related to wave, current, salinity gradient, and ocean thermal energy conversion technologies. The database contains information from around the world.

The Tethys Engineering database was created as a companion to the already established Tethys website, which focuses on the environmental effects of the MRE industry.

November 18, 2019

Understanding the Grid Value Proposition of Marine Energy: A Literature Review

July 1, 2019
November 1, 2019
Report

Summary 

In 2018, the US Department of Energy’s Water Power Technologies Office Marine Hydrokinetics Program directed two national laboratories, Pacific Northwest National Laboratory and National Renewable Energy Laboratory, to investigate the potential of marine renewable resources to contribute the U.S. electric system. Due to the innovative nature of marine renewable energy and the transformation of the US electric system resource mix, there is a lack of insight about the future potential role and grid value proposition of marine energy.

An initial step in this technical project is to review available literature to inform and help characterize the portfolio of potential marine energy resource contributions. This literature review summarizes the energy fundamentals of marine resources; the performance and operational characteristics of energy conversion devices; grid opportunities and integration challenges most applicable to marine energy; storage coupling to achieve grid opportunities; and offshore wind energy competition and collaboration. It provides the context and the state of knowledge in which the grid value proposition of marine energy should be further researched and explored.

Notable findings from the review include the following:

  • Very little work has been conducted to connect the grid and fundamental marine energy development. Few technical papers attempt to demonstrate grid value from marine energy or, conversely, illustrate how grid applications may have an effect on device size and scale, convergence of device types, and location of marine energy technologies. Those that have done so relied on numerous estimations and assumptions and target very specific potential benefits.
  • Aggregation of tidal generation for baseload—the concept of distributing tidal generators to accomplish complementary phase shifts in generation that, when summed, would provide relatively stable power—faces challenges from a cost perspective. One study evaluated three geographically separate, complementary locations off the Scottish coast. The study concluded that aggregate power generated from sites with varying resources is sensitive to the characteristics of the individual sites and some irregularity should be expected in aggregate power output due to natural variation in successive tides. Ultimately, the study suggests that using complementary sites and limiting the capacity of the turbines, particularly during neap tides, could create baseload power, or a constant power output; but the research team expressed concerns regarding whether such a deployment would be cost effective. Decreasing the turbines’ rated capacity and therefore not capturing the resource to its fullest extent would cause economic losses.
  • Tidal energy-generating profiles may be well matched for storage. Energy storage is a fast-growing resource in the energy industry. It can provide value in a multitude of grid situations, including supporting marine energy technologies. One report suggests that because tides are predictable, tidal technologies are ideal for pairing with energy storage to create a steady output of power. In fact, Nova Innovation recently integrated a Tesla battery storage system with the Shetland Tidal Array in Scotland and expanded the generating capacity and enabled dispatchability at the site.
  • There is a potential match between resource peak and electric demand. When considering a seasonally peaking resource, like wave energy, there is an opportunity for the generation patterns to be well matched with energy demand. For example, one study noted that British Columbia’s energy consumption peaks in the winter when the available wave resource is also at its strongest; this same characteristic is true along the rest of North America’s Pacific Northwest coast.
  • Co-location may deliver grid benefits. A study evaluating a portion of the North Sea showed that there could be significant benefits to co-locating wave devices and offshore wind turbines. When wind and waves are negatively correlated, this decreases variability and can help mitigate grid integration concerns that are sometimes associated with variable generation. Being proactive in the siting process and performing quantitative spatial planning can avoid potential conflicts between sea uses, while harnessing the most useful energy.
  • The availability and cost of land was used in utility decision-making for resource selection and resulted in a portfolio selection that included marine energy development. In a 2017 Integrated Resource Plan for the Caribbean Utilities Company (the public electric utility for Grand Cayman in the Grand Cayman Islands), a contractor evaluated land use associated with different generation technologies and found a significant advantage to using marine energy, specifically ocean thermal energy conversion (OTEC). Accordingly, and despite a higher capital cost for OTEC relative to other resource options, the resource plan containing OTEC was among the two recommended portfolios. In the portfolio, OTEC resources replaced onshore solar development, which requires a relatively high land commitment proportional to total generation, as well as natural gas-fired backup generation and battery storage. Although OTEC is not considered in this report, connections can be drawn to the technology, and research from that field is applicable to other marine energy resources in particular instances.

As the marine energy industry grows, there is a corresponding increase in the body of literature about both the potential value of harnessing marine resources as well as the requisite technical work to integrate the resource into the grid. Due to the unique aspects of marine energy resources, especially their offshore location, volume, and predictability, there are many reasons to consider marine energy a viable potential renewable resource in the future electric system.

July 1, 2019