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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Artificial Intelligence for Digital Security and Protections

Proper functioning of nuclear power plants relies on a mix of well-regulated human and machine-driven workflows. This regulation supports nuclear safety through a series of processes and many of the tasks that support these processes have a repetitive nature that make artificial intelligence (AI) informed by machine learning (ML) a potential aid in a variety of tasks. AI is being evaluated for activities that include inspections, fuel processing, monitoring, and other activities. The introduction of any new technology presents a potential new attack vector. In the case of AI/ML, there are many attacks that have already been discovered and over time the attacks can be expected to follow the growth pattern observed in cyber security. While future planning is necessary, current efforts need to be established now to predict the threat emergence over the next year 10 years and mitigate potential threats. Based on these observations, AI/ML will need to become trustworthy, which corresponds to techniques and procedures that emphasize AI explainability along with resilience techniques to data, algorithms, models, and systems. This kind of system robustness is the foundation for defenses against AI/ML-specific attacks. Attempting to look forward and take a broad view of capabilities provides input to research roadmaps and the ability to distill vulnerabilities into specific use cases may provide greater assistance in understanding the technology benefits while introducing new risks. The impact of current and future AI in three areas—capabilities, challenges, and recovery strategies—represents an initial attempt at balancing both.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗
DOE OSTI2024

Impacts of photovoltaic solar energy on soil carbon: A global systematic review and framework

Globally, solar energy is anticipated to be the primary source of electricity as early as 2050, and the greatest additions in capacity are currently in the form of large, ground-mounted photovoltaic solar energy facilities (GPVs). Growing interest lies in understanding and anticipating opportunities to increase soil carbon sequestration across the footprint and perimeter of both conventional and multi-use GPVs (e.g., ecovoltaics, agrivoltaics, and rangevolatics), especially as operators increasingly deputize as land managers. To date, studies on the relationship between soils and PV solar energy are limited to unique, localized sites. This study employed a systematic review to (i) identify a global corpus of 18 studies on interactions between GPVs and soils, (ii) collect and characterize 113 soil and soil-related experimental variables interacting with GPVs from this corpus, and (iii) synthesize trends among these experimental variables. Next, this study combined data from the systematic review with an iterative, knowledge co-production approach to produce a conceptual model for the study of soil and GPV interactions that applies to multiple installation types, scales, and contexts where GPVs are deployed, and identified research opportunities, threats, and priorities. This study's baseline understanding, conceptual model, and co-produced knowledge confer unique insight into the feasibility of combining soil carbon sequestration with the climate change mitigation potential of PV solar energy.

agrivoltaics↗
NASA NTRS2018

The Influence of Mental Workload in Causes of System Degradation in Air Traffic Control

System safety and resilience is a critical concern in the air traffic domain. An important element of maintaining system safety and resilience is the ability of systems to ‘degrade gracefully’. However, previous research on the causes of system degradation in the air traffic domain are sporadic, and the potential interaction between the causes of degradation, and the resulting possible compound effect on the entire system, has been under-researched. An interview study was conducted with 12 retired controllers as participants. The results of a thematic analysis revealed the key causes of system degradation, and the associated impact on the ability of the controllers to prevent system degradation or recover the system. Findings have direct implications for identifying and mitigating potential risks of increasingly automated air traffic control systems.

Edwards, Tamsyn E.↗
NASA NTRS2018

The Influence of Mental Workload in Causes of System Degradation in Air Traffic Control

System safety and resilience is a critical concern in the air traffic domain. An important element of maintaining system safety and resilience is the ability of systems to ‘degrade gracefully'. However, previous research on the causes of system degradation in the air traffic domain are sporadic, and the potential interaction between the causes of degradation, and the resulting possible compound effect on the entire system, has been under-researched. An interview study was conducted with 12 retired controllers as participants. The results of a thematic analysis revealed the key causes of system degradation, and the associated impact on the ability of the controllers to prevent system degradation or recover the system. Findings have direct implications for identifying and mitigating potential risks of increasingly automated air traffic control systems.

Edwards, Tamsyn↗
DOE OSTI2025

Advanced Reactor Designs Security Analysis, Risk, and Recommendations: Risks, Consequences, and Possible by-Design Mitigation Approaches Associated with Select Advanced Reactors

Next-generation advanced reactors (ARs) incorporate enhanced safety systems, have smaller source terms, and feature compact modular designs, which should lessen their collective risk profiles. However, to fully evaluate risk, security needs to be a part of the equation. Without taking security into consideration, safety systems and components in the new ARs may be vulnerable to sabotage. These base attributes, coupled with enhanced security features specific to AR design through sound engineering and security-by-design (SeBD), should provide developers and operators with lower inherent security risk profiles. Building security early into the AR design may remove or passively secure potential critical targets from an adversary’s reach , thereby increasing overall safety and security. An integrated approach and diverse design team that includes engineering, operations, and security experts are fundamental to building security into the design without sacrificing fundamental operational efficiencies and principles. The objective of this project was to evaluate the security and safety interfaces for five classes of reactors, identify potential security vulnerabilities of structures, systems, and components (SSC), and underscore the need to consider security alongside safety in the design o f these concepts. The five reactor classes evaluated in this project and presented in this report are molten-salt reactors (MSR), high temperature gas reactors (HTGR), sodium-fast reactors (SFR), advanced light-water reactors (ALWR), and microreactors. These designs were selected because they reflect the concepts that are closest to market deployment and have received significant resource investments from the public and private sector. This project assesses the inherent security risks posed by common classes of ARs, provides a methodology and framework to assess security along with safety, and offers an analysis of potential mitigation strategies that could be incorporated. For each AR technology, the SSCs that relate to radionuclide source safety functions are discussed to understand the SSC contribution to safety and relative importance in the protective strategy for the design. The assumptions that went into evaluating each reactor concept originated from generic publicly available nonproprietary information and should not directly be used to qualify an absolute risk profile nor to rank specific AR designs. Instead, the purpose of the analysis is to understand and compare the generic inherent security risks of different AR technologies.

98 - NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL↗
DOE OSTI2024

Consumer Benefits of Clean Energy: The resilience value of residential solar + storage systems in the continental U.S.

Meeting national and state decarbonization goals requires a transition to clean energy technologies. Energy efficiency, demand flexibility, renewable energy and storage can reduce consumers’ electricity bills, lower total electricity system costs, and provide health and resilience benefits. Berkeley Lab developed a series of briefs that explore these consumer benefits of a clean energy transition. Clean energy resources that are located behind the meter have the potential to benefit the hosting customers by providing affordability, environmental, and reliability and resilience value. Solar plus storage systems (PVESS) are clean energy resources that can supply backup power without requiring fuel resupply or increasing local emissions. This report examines the regional value of PVESS for resilience by calculating a benefit-cost ratio (BCR) that considers the annual resiliency benefits of PVESS and the annualized cost of the investment. In addition, we estimate the expected technical mitigation potential of PVESS systems at the county-level to these expected events, and characterize the customer interruption costs by determining the value of lost load at the state level.

14 SOLAR ENERGY↗
DOE OSTI2024

Large-scale spatially explicit analysis of carbon capture at cellulosic biorefineries

The large-scale production of cellulosic biofuels would involve spatially distributed systems including biomass fields, logistics networks and biorefineries. Better understanding of the interactions between landscape-related decisions and the design of biorefineries with carbon capture and storage (CCS) in a supply chain context is needed to enable efficient systems. Here we analyse the cost and greenhouse gas mitigation potential for cellulosic biofuel supply chains in the US Midwest using realistic spatially explicit land availability and crop productivity data and consider fuel conversion technologies with detailed CCS design for their associated CO 2 streams. Optimization methods identify trade-offs and design strategies leading to systems with attractive environmental and economic performance. Strategic and operational decisions depend on underlying spatial features and are sensitive to biofuel demand and CCS incentives. US CCS incentives neglect to motivate greenhouse gas mitigation from all supply chain emission sources, which leverage spatial interactions between CCS, electricity prices and the biomass landscape.

09 BIOMASS FUELS↗
DOE OSTI2021

Hydropower Cyber-Physical Configurations

The U.S. Department of Energy’s Water Power Technologies Office funded Pacific Northwest National Laboratory, Argonne National Laboratory, and the National Renewable Energy Laboratory to develop a typology to characterize the variety and pervasiveness of cyber-physical configurations across the nation’s hydropower fleet. Outreach to owners and operators returned configurations for 275 hydropower plants or approximately 12% of the fleet. Components (OT and IT), systems, and connections among systems differed among plants according to function, age, position in the river cascade, and many other factors. Seven cyber-physical configuration types labeled A through I, included from 2 to dozens of plants. They were differentiated by how pervasive data and control connections were among cyber-physical components and how frequently control signals paired with data signals in a feedback loop. The flow of data and control within each type implies what cybersecurity vulnerabilities may exist, and what mitigation actions may be most effective. A self-assessment approach allows plant operators to identify the configuration type similar to their plant and link to the lessons learned and best practices information. The cyber-physical typology reinforces the idea that hydropower facilities vary widely, but it also identifies groups that highlight similarities in how their cyber-physical components interact. This helps address fleetwide cybersecurity needs by identifying a reasonable number of configuration types that share risks, vulnerabilities, and potential mitigations.

13 HYDRO ENERGY↗
NASA NTRS2022

Near-Earth Object Surveyor Overview

The Near-Earth Object (NEO) Surveyor is designed to detect, categorize and characterize Near-Earth Objects (NEOs) using infrared imaging. The project was approved to enter the preliminary design phase (Phase B) in FY21 after an extended Concept Development Phase (Phase A). The NEO Surveyor project responds to US Public Law 109-155[1], National Research Council’s report “Defending Planet Earth: Near-Earth Object Surveys & Hazard Mitigation Strategies (2010)”[2], the U. S. National Near-Earth Object Preparedness Strategy and Action Plan (June 2018)[3], and the objectives of NASA’s Planetary Defense Coordination Office (PDCO). The goals of the NEO Surveyor project are to: (1) identify impact hazards to the Earth posed by NEOs (defined as asteroids and comets that come within 1.3 AU of the Sun) by performing a comprehensive survey of the NEO population; (2) obtain detailed physical characterization data for individual objects that are likely to pose an impact hazard; (3) characterize the entire population of potentially hazardous NEOs to inform potential mitigation strategies. The mission will make significant progress toward the George E. Brown, Jr. NEO Survey Program objective defined by the U. S. Congress of detecting, tracking, cataloging, and characterizing at least 90% of NEOs equal to or larger than 140 m in diameter. The project is a collaboration between NASA-JPL, the University of Arizona (UA) and industry, with Ball Aerospace notably providing the spacecraft and key instrument elements. This paper will describe the overall NEO Surveyor Project objectives, initial spacecraft and instrument design and development plans and mission concept.

Veto, Michael↗
DOE OSTI2022

Rye as an Energy Cover Crop: Management, Forage Quality, and Revenue Opportunities for Feed and Bioenergy

Harvesting a winter rye energy cover crop (Secale cereale L.) could help sustain growing food and energy demand, provide new revenue streams, and enhance ecosystem services without inducing land-use change. A two-year field experiment with three planting methods and three N fertilization rates (0, 60, and 120 kg N ha -1 ) that produced >5.0 Mg ha -1 yr -1 of biomass was evaluated for (1) fresh and anaerobically digested rye forage quality; (2) revenue potential from renewable bioenergy, carbon markets, and digestate feed protein; and (3) potential greenhouse gas (GHG) offsets. We showed that rye can be harvested as forage for animals or anaerobically digested to produce renewable natural gas (RNG), with the residue after digestion (digestate) still available as a feed protein concentrate. Anaerobically digesting rye improved forage quality indicators. Digestion significantly decreased acid- and neutral-detergent fiber (ADF and NDF) by 5.2% and 17.8%, respectively, while significantly increasing crude protein (CP) (33.6%), total digestible nutrients (TDN) (2.0%), relative feed value (RFV) (23.6%), net energy for lactation (8.3%), maintenance (7.5%), and gain (20.0%). Using market prices for RNG, high protein feed, and GHG mitigation, potential on-farm revenue ranged from USD 307 Mg -1 and USD 502 Mg -1 dry matter with an average of USD 402 Mg -1 . However, there are substantial costs associated with RNG and the revenue potential does not represent the profitability of this system. Evaluation of the integrated system showed GHG emissions associated with rye fertilization were more than offset by the benefits of increasing yield in the 60 kg N ha -1 treatment. The overall carbon footprint of the integrated system was strongly carbon negative, confirming the potential of this strategy to sustainably intensify land use in the Midwestern United States.

09 BIOMASS FUELS↗
NASA NTRS2017

Using Information from Rendezvous Missions for Best-Case Appraisals of Impact Damage to Planet Earth Caused by Natural Objects

The Asteroid Threat Assessment Project (ATAP), a part of NASAs Planetary Defense Coordination Office (PDCO) has the responsibility to appraise the range of surface damage by potential asteroid impacts on land or water. If a threat is realized, the project will provide appraisals to officials empowered to make decisions about potential mitigation actions. This paper describes a scenario for assessment of surface damage when characterization of an asteroid had been accomplished by a rendezvous mission that would be conducted by the international planetary defense community. It is shown that the combination of data from ground and in-situ measurements on an asteroid provides knowledge that can be used to pin-point its impact location and predict the level of devastation it would cause. The hypothetical asteroid 2017 PDC with a size range of 160 to 290 m in diameter to be discussed at the PDC 2017 is used as an example. In order of importance for appraising potential damage, information required is: (1) where will the surface impact occur? (2) what is the mass, shape and size of the asteroid and what is its entry state (speed and entry angle) at the 100 km atmospheric pierce point? And (3) is the asteroid a monolith or a rubble pile? If it is a rubble pile, what is its structure and heterogeneity from the surface and throughout its interior? Item (1) is of first order importance to determine levels of devastation (loss of life and infrastructure damage) because it varies strongly on the impact location. Items (2) and (3) are used as inputs for ATAPs simulations to define the level of surface hazards: winds, overpressure, thermal exposure; all created by the deposition of energy during the objects atmospheric flight, andor cratering. Topics presented in this paper include: (i) the devastation predicted by 2017 PDCs impact on land based on initial observations using ATAPs risk assessment capability, (ii) how information corresponding to items (1) to (3) could be obtained from a rendezvous mission, and (iii) how information from a rendezvous mission could be used, along with that from ground observations and data from the literature to provide input for a new risk analysis capability that is emerging from ATAPs research. It is concluded that this approach would result in the creation of an appraisal of the threat from 2017 PDC with the least uncertainty possible, herein called the best-case.

Asteroid Impact Appraisals↗
NASA NTRS1991

An RF interference mitigation methodology with potential applications in scheduling

Software tools for interference analysis and mitigation were developed in the Communications Link Analysis and Simulation System (CLASS) environment for: communications performance evaluation; and mission planning. Potential applications are seen in analysis, evaluation, and optimization of user schedules. Tools producing required separation angles and potential interference intervals can be used as an aid to mutual interference mitigation within a scheduling system.

Wong, Yen F.↗
NASA NTRS2017

Using Information from Rendezvous Missions For Best-Case Appraisals of Impact Damage to Planet Earth Caused By Natural Objects

The Asteroid Threat Assessment Project (ATAP), a part of NASAs Planetary Defense Coordination Office (PDCO) has the responsibility to appraise the range of surface damage by potential asteroid impacts on land or water. If a threat is realized, the project will provide appraisals to officials empowered to make decisions on potential mitigation actions. This paper describes a scenario for assessment of surface damage when characterization of an asteroid had been accomplished by a rendezvous mission that would be conducted by the international planetary defense community. It is shown that the combination of data from ground and in-situ measurements on an asteroid provides knowledge that can be used to pin-point its impact location and predict the level of devastation it would cause. The hypothetical asteroid 2017 PDC with a size of 160 to 290 m in diameter to be discussed at the PDC 2017 meeting is used as an example. In order of importance for appraising potential damage, information required is: (1) where will the surface impact occur? (2) What is the mass, shape and size of the asteroid and what is its entry state (speed and entry angle) at the 100 km atmospheric pierce point? And (3) is the asteroid a monolith or a rubble pile? If it is a rubble pile, what is its sub and interior structure? Item (1) is of first order importance to determine levels of devastation (loss of life and infrastructure damage) because it varies strongly on the impact location. Items (2) and (3) are used as input for ATAPs simulations to define the level of surface hazards: winds, overpressure, thermal exposure; all created by the deposition of energy during the objects atmospheric flight, and/or cratering. Topics presented in this paper include: (i) The devastation predicted by 2017 PDCs impact based on initial observations using ATAPs risk assessment capability, (ii) How information corresponding to items (1) to (3) could be obtained from a rendezvous mission, and (iii) How information from a rendezvous mission could be used, along with that from ground observations and data from the literature, could provide input for an new risk analysis capability that is emerging from ATAPs research. It is concluded that this approach would result in appraisal with the least uncertainty possible (herein called the best-case) using simulation capabilities that are currently available or will be in the future.

Arnold, James O.↗
NASA NTRS2017

Using Information from Rendezvous Missions For Best-Case Appraisals of Impact Damage to Planet Earth Caused By Natural Objects

The Asteroid Threat Assessment Project (ATAP), a part of NASAs Planetary Defense Coordination Office (PDCO) has the responsibility to appraise the range of surface damage by potential asteroid impacts on land or water. If a threat is realized, the project will provide appraisals to officials empowered to make decisions on potential mitigation actions. This paper describes a scenario for assessment of surface damage when characterization of an asteroid had been accomplished by a rendezvous mission that would be conducted by the international planetary defense community. It is shown that the combination of data from ground and in-situ measurements on an asteroid provides knowledge that can be used to pin-point its impact location and predict the level of devastation it would cause. The hypothetical asteroid 2017 PDC with a size of 160 to 290 m in diameter to be discussed at the PDC 2017 meeting is used as an example. In order of importance for appraising potential damage, information required is: (1) where will the surface impact occur? (2) What is the mass, shape and size of the asteroid and what is its entry state (speed and entry angle) at the 100 km atmospheric pierce point? And (3) is the asteroid a monolith or a rubble pile? If it is a rubble pile, what is its sub and interior structure? Item (1) is of first order importance to determine levels of devastation (loss of life and infrastructure damage) because it varies strongly on the impact location. Items (2) and (3) are used as input for ATAPs simulations to define the level of surface hazards: winds, overpressure, thermal exposure; all created by the deposition of energy during the objects atmospheric flight, andor cratering. Topics presented in this paper include: (i) The devastation predicted by 2017 PDCs impact based on initial observations using ATAPs risk assessment capability, (ii) How information corresponding to items (1) to (3) could be obtained from a rendezvous mission, and (iii) How information from a rendezvous mission could be used, along with that from ground observations and data from the literature, could provide input for an new risk analysis capability that is emerging from ATAPs research. It is concluded that this approach would result in appraisal with the least uncertainty possible (herein called the best-case) using simulation capabilities that are currently available or will be in the future.

Arnold, J. O.↗
DOE OSTI2024

Mitigating municipal solid waste fouling in biofuel conversion via screw surface modifications

Here, municipal solid waste (MSW)'s 40–60 % carbon content makes it a feedstock for biofuel production via pyrolysis. One challenge in the conversion process is MSW fouling due to thermal decomposition. The accumulated deposit on the injection screw often leads to plugging and constriction. This study examined the morphology and composition of the MSW fouling deposit and conducted a thermal simulation to understand the temperature gradience of the injection screw. Surface modifications including smoothening and anti-adhesion coating were proposed for the injection screw to address the deposit problem. For evaluating the candidate mitigations, a bench-scale fouling test was developed with the gas environment, temperature, and sliding speed relevant to the contact interface between the MSW particles and the screw. Results suggested that a smoother screw surface could reduce the grip and a non-metallic coating with a lower surface energy could decrease adhesion, consequently leading to less fouling. Specifically, reducing the roughness from 2 to 0.6 and then to 0.2 μm proportionally decreased the amount of deposit, and the diamond-like-carbon, CrN, and NiCr–CrC composite coatings effectively hindered the fouling process. This study provides fundamental insights into the MSW fouling and proof-of-concept of potential mitigations through the screw surface modification.

09 BIOMASS FUELS↗
DOE OSTI2026

Augmenting Molecular Graphs with Geometries via Machine Learning Interatomic Potentials

Accurate molecular property predictions require 3D geometries, which are typically obtained using expensive methods such as density functional theory (DFT). Here, we attempt to obtain molecular geometries by relying solely on machine learning interatomic potential (MLIP) models. To this end, we first curate a large-scale molecular relaxation dataset comprising 3.5 million molecules and 300 million snapshots. Then MLIP pre-trained models are trained with supervised learning to predict energy and forces given 3D molecular structures. Once trained, we show that the pre-trained models can be used in different ways to obtain geometries either explicitly or implicitly. First, it can be used to obtain approximate low-energy 3D geometries via geometry optimization. While these geometries do not consistently reach DFT-level chemical accuracy or convergence, they can still improve downstream performance compared to non-relaxed structures. To mitigate potential biases and enhance downstream predictions, we introduce geometry fine-tuning based on the relaxed 3D geometries. Second, the pre-trained models can be directly fine-tuned for property prediction when ground truth 3D geometries are available. Our results demonstrate that MLIP pre-trained models trained on relaxation data can learn transferable molecular representations to improve downstream molecular property prediction and can provide practically valuable but approximate molecular geometries that benefit property predictions. Our code is publicly available at: https://github.com/divelab/AIRS/.

Fu, Cong [Texas A & M Univ., College Station, TX (↗
DOE OSTI2022

Scaling Sustainable Biochar Research & Commercialization for Agriculture & Conservation: A Summary from a Stakeholder Convening

Biochar is a carbon-rich substance with the potential to increase soil carbon sequestration, reduce greenhouse gas (GHG) emissions and improve soil health. When used as part of soil health management systems, biochar can provide multiple synergistic benefits for the agricultural sector and society, while also supporting the production of renewable, climate-neutral biofuels. Establishing a pyrolysis biochar bioenergy industry (PBBI) is necessary to harness the environmental benefits of biochar. To galvanize the necessary coordination to support a PBBI, the Foundation for Food & Agriculture Research (FFAR), the National Center for Appropriate Technology (NCAT), and American Farmland Trust (AFT) co-hosted a virtual convening event on biochar research and commercialization in March 2022. Participants represented a diverse set of stakeholders, including biochar producers, agricultural producers, and members of nonprofit, industry and government agencies. This whitepaper offers a summary of the convening, as well as insights from subsequent stakeholder engagement. Sustainably sourced, fit-for-purpose biochar can be a powerful tool in the soil health management systems and climate-smart toolbox, with decades of research supporting the soil, environment, production, and climate benefits. However, because biochar represents a range of feedstocks, processes and products, there is a critical need to: • Coordinate efforts to characterize and test the application of biochar types across locations with diverse soil and management conditions • Address research and decision-support gaps • Support the growing industry These objectives can be addressed or advanced through a coordinated strategy. To support establishment of this strategy, the convening participants identified key gaps in implementation and research. The experiences of foresters, ranchers, and farmers already using biochar, some of whom participated in the convening, helped inform priorities. Key gaps include: • Practical, applied on-farm research • Supporting management for agricultural productivity • Maximum benefits for conservation • Decision support • Life Cycle Assessment (LCA) • Quantification of climate mitigation potential Existing research gaps include: • Potential synergies among biochar, soil organic matter, and enhanced rock weathering • Development of new storage reservoirs for biochar in industrial products Convening participants further provided next steps for rapidly developing a PBBI to produce sustainable, fit-for-purpose biochars that increase soil health and mitigate climate change. Participants also stressed the need for actionable, coordinated, large-scale research relevant to commercial production in the next five years. To have a chance to reduce greenhouse gas emissions, we need an array of tools that would aid in mitigation; a coordinated strategy to enable biochar to be an effective tool in the climate-smart toolbox must be created; We cannot wait 50 years.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

ESI-MS Identification of the Cationic Phosphine-Ligated Gold Clusters Au1-Au22: Insight into the Gold-Ligand Ratio and Abundance of Larger Clusters

Triphenylphosphine (PPh3)-ligated gold clusters offer promising potential applications due to their relative ease of synthesis and usefulness in forming advanced cluster architectures. While previous studies reported cationic PPh3-ligated gold clusters with core sizes of Au1 - Au4, Au6 - Au11, and Au¬13 - Au14, there has not been definitive identification by mass spectrometry of larger clusters in the Au12 - Au25¬ range. Herein, we survey a polydisperse solution of cationic PPh3-ligated gold clusters using high mass-resolution (M/?M = 60,000) electrospray ionization mass spectrometry (ESI-MS). To improve the sensitivity and mass resolution of larger clusters for unambiguous identification, we increased the number of scan averages and reduced the range of mass collection windows to 200 m/z, thereby mitigating potential mass and ion abundance bias resulting from smaller “building block” gold clusters and other solution components present in higher abundance. In addition to the previously reported clusters, we identified several new species including Au5(PPh3)5+, Au12(PPh3)9HCl2+, Au15(PPh3)9Cl2+, Au16(PPh3)10Cl22+, Au17(PPh3)113+, Au18(PPh3)102+, Au19(PPh3)10Cl2+, Au20(PPh3)12H33+, Au21(PPh3)10Cl2+, and Au22(PPh3)10Cl22+, indicating that a full range of clusters between Au1 - Au22 may be observed in a single polydisperse solution. Considering all of the observed clusters, our findings provide evidence that the “magic number” icosahedral Au13 may be the transition point in cluster growth between smaller clusters, exhibiting a 1:1 gold-to-ligand ratio, and larger clusters, wherein subsequent gold atoms are added to the core without an equal number of accompanying ligands. Our method demonstrates that reducing the range of m/z collection windows and increasing the number of scan averages can improve instrument sensitivity for cationic gold clusters and enable a more complete survey of polydisperse solutions, thereby providing new insights to guide and validate the results of other characterization methods and theoretical calculations. This work was supported by the US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. MH acknowledges support from the DOE Science Undergraduate Laboratory Internship (SULI) program. HH acknowledges support from the DOE Office of Workforce Development for Teachers and Scientist (WDTS) under the Visiting Faculty Program (VFP). This work was performed using EMSL, a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is a multiprogram national laboratory operated for DOE by Battelle.

Hewitt, Michael↗