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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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NASA's desire to study and characterize the solar system and small bodies like comets and asteroids will be done by in-situ robotic systems in the near term.
The project's goal is to combine high-fidelity numerical models and true-triaxial block fracturing tests at high temperatures to understand the relationship between in situ stress, thermal effects, wellbore orientations and hydraulic fracture patterns. The numerical models are calibrated against field data, such as well pressures and microseismic data, and employed to estimate the in situ stress at the FORGE site. Laboratory experiments investigate the complex physics driving hydraulic fracture nucleation in EGS, enhancing understanding of the role of parameters like temperature, well orientation, and stress. Additionally, they are employed to validate some of the numerical tools used in the project. The project will have a significant impact by: (1) improving the characterization of the in-situ stress field at FORGE; (2) demonstrating the use of high-fidelity modeling tools for EGS; (3) providing a unique set of high-temperature hydraulic fracturing results to identify key components for in-situ stress estimation, validate current theories, and propose new ones; (4) offering a validated set of numerical tools within an open-source simulation framework, GEOS, that will be available to any future user.
Characterizing catalyst stability by identifying the predominant mechanisms, timescales and driving forces of catalyst reconstruction under relevant reaction conditions is necessary for the design and commercialization of new catalysts. Here, in this paper, we study Rh/TiO 2 catalysts under CO 2 hydrogenation conditions (773 K, 75% H 2 , 25% CO 2 ) at high conversion and utilize reactivity studies along with ex-situ and in-situ spectroscopy and microscopy to characterize changes in catalyst activity and structure as a function of time on stream and the initial catalyst structure. This is a prototypical catalyst for CO 2 hydrogenation where Rh structure and Rh-TiO 2 interactions have been proposed to explain reactivity, selectivity (between CO and CH 4 formation) and catalyst stability. The influence of the initial Rh structure (varying from Rh single atoms to Rh nanoparticles), support stability, regeneration and pretreatment(s), and the chemical potential(s) of the reaction environment on reaction selectivity and catalyst stability were explored. The product selectivity between CO and CH 4 was determined to be dependent on the relative fraction of Rh single atoms and Rh nanoparticle-TiO 2 interfacial sites under reaction conditions, each exhibiting distinct stability under prolonged time on stream. Surprisingly, Rh single atoms exhibited stability for the duration of 90 h reactivity measurements, even at high Rh density (≥ 1.8 Rh atoms/nm 2 ) on the support, while Rh nanoparticles sintered under reaction conditions. As a result, all catalysts exhibited increasing selectivity to CO with increasing time on stream (> 10 h). We conclude the distribution of Rh structures evolved over time under reaction conditions through three distinct reconstruction mechanisms (Rh particle fragmentation, Ostwald ripening, and particle migration and coalescence) that occurred on varying timescales. Catalyst stability on the ~90 h time scale was ultimately controlled by the initial Rh structure.
The nanoscale mechanisms of localized corrosion in low carbon steels have remained elusive due to the complexity of studying the degradative material behavior at nanoscale solid-liquid interfaces. We identified various steps in the nanogalvanic corrosion processes using in-situ liquid-cell scanning transmission electron microscopy (STEM) using a microfluidic holder by Hummingbird Scientific. Initial work, performed at low magnification, identified the initiation point on a 1018 low-carbon steel surface. This initiation point was determined to be a triple junction of two ferrite grains bridging a cementite grain in contact with a baseline electrolyte of 6 uM CO2 dissolved in a buffered (2.78 uM Na2SO4) aqueous solution, pH 6.1. The pre-etched low-carbon steel surface was prepared using focused ion beam lift-out procedures to extract a cross-section of the low-carbon steel surface, which then was thinned to about 150 nm and transferred to a SiN membrane microfluidic window. The transfer was made using a lift-out needle to attach the low-carbon steel lamella to the corner of the SiN window, and then Pt/C deposition held the lamella in contact with the window while it was released from the lift out needle. To identify the triple point on the low carbon steel lamella, prior to attachment on the SiN window, the sample was characterized for compositional variations with energy dispersive x-ray spectroscopy mapping, grain orientation and phase mapping with precession electron diffraction, and thickness mapping with energy filtered transmission electron microscopy. This pre-characterization prior to the in-situ experiment provided a map of the multiphase and multigrain structure, where the in-situ liquid cell imaging provided a clear understanding of the initiation point on the sample. These data were cross-correlated to paint a holistic picture of the triple junction site, enabling low electron-fluence in-situ snapshot imaging to avoid dominating the native corrosion reactions with effects from the incident electron beam. This initial result identified that localized, nanogalvanic corrosion at the phase interface was the dominant corrosion process in the low-carbon steel, so we next targeted the observation of an array of these nanogalvanic features phase boundaries in a pearlite grain. Near-surface ferrite/cementite phase interfaces that typify pearlitic low-carbon steel were extracted, pre-characterized, and imaged for the in-situ corrosion processes. The sample was a cross-section from a pearlite grain, with alternating ferrite and cementite grains that extended microns down from the pre-etched low-carbon steel pipe surface. After contact with a buffered aqueous solution, the phase boundaries between the ferrite and cementite began to dissolve, with observable material loss and thickness changes in the dark-field and bright-field STEM images. Within minutes, the corrosion front proceeded deeper into the material, claiming a thin layer of ferrite around all exposed phase boundaries before progressing laterally into the ferrite matrix, converting the ferrite to corrosion product normal to each buried cementite grain. Formation of the corrosion product causes a volumetric expansion, creating a lateral wedging force that mechanically ejects the cementite grains from their grooves and leaves behind percolation channels into the steel substructure. Rapid and deleterious, this nanogalvanic corrosion pathway represents an important target for understanding and preventing run-away degradation in this common building material. Observation of this corrosion mechanism was enabled by the combination of pre-characterization using standard structural, grain, and compositional analysis in the TEM, which provides maps for understanding the reaction propagation captured in low-dose, in-situ, liquid-cell STEM.
Atomically dispersed catalysts have drawn great interest lately, as they showcase a high density of active sites, selectivity, and high turnover frequencies in oxidation chemistry due to labile oxygen activation. In contrast, the applications of these catalysts have lagged in reduction reactions due to the ambiguity caused by the sintering and restructuring of active sites. To bridge this gap, the evolution of Pt 4+ isomorphically substituted into an octahedral molecular sieve structure (OMS-2) under reductive conditions was correlatively characterized using multiple in-situ analytical techniques such as ambient pressure X-ray photoelectron spectroscopy, environmental transmission electron microscopy, and solid-state nuclear magnetic resonance. The surface dynamics of the Pt single atoms were revealed during the Reverse Water Gas Shift (RWGS) reaction, where the active sites were identified as two-coordinated platinum single atoms. Under reaction, we show nonbinding atoms adjacent to the single atoms restructured the motif of the single atoms to Pt 2+ via ion mobility of potassium, increasing the activation energy by 25.6 kJ/mol. Here, this work also highlights the potential for increased stability of the single atom sites via isomorphic substitution of the metal oxide support, since the Pt-OMS-2 catalyst retained activity for about 33 h before deactivation, after which nanoparticles were observed in TEM images. This work offers a new perspective in single atom synthesis using the metal oxide as the host for the single atom site, instead of adatoms on the surface
The Twente region in the east of the Netherlands has a network with twenty soil monitoring stations that has been utilized for validation of the Soil Moisture Active/Passive (SMAP) passive-only soil moisture products. Over the period from April 2015 until December 2018, seven stations covered by the SMAP reference pixels 15 have fairly complete data records. Spatially distributed soil moisture simulations with the Dutch national hydrological model have been utilized for the development of upscaling functions to translate the spatial mean of point measurements to the domain of the SMAP reference pixels. The native and upscaled spatial soil moisture means computed using the in-situ measurements have been adopted as references to assess the performance of the SMAP i) Single Channel Algorithm at Horizontal Polarization (SCA-H), ii) Single Channel Algorithm at Vertical Polarization (SCA-V), and iii) Dual Channel Algorithm (DCA) soil moisture estimates. In the case of the Twente network it was found that the SCA-V soil moisture retrieved SMAP observations collected in the afternoon had the best agreement with the native spatial mean leading to an unbiased Root Mean Squared Error (uRMSE) of 0.059 m3 m-3, whereas for the upscaled in-situ references primarily larger biases were found. These error levels are larger than the mission’s target accuracy of 0.04 m3 m-3, which can be attributed to large over- and underestimation errors (>0.08 m3 m-3) in particular at the end of dry spells and during freezing, respectively. The strong vertical dielectric gradients associated with rapid soil freezing and wetting causes the disparity in soil depth characterized by SMAP and in situ that leads to the large mismatches. Once filtered for frozen conditions and antecedent rainfall the uRMSE improves to 0.043 m3 m-3.
Viruses can alter the abundance, evolution, and metabolism of microorganisms in the ocean, playing a key role in water column biogeochemistry and global carbon cycles. Large efforts to measure the contribution of eukaryotic microorganisms (e.g., protists) to the marine food web have been made, yet the in situ activities of the ecologically relevant viruses that infect these organisms are not well characterized. Viruses within the phylum Nucleocytoviricota (“giant viruses”) are known to infect a diverse range of ecologically relevant marine protists, yet how these viruses are influenced by environmental conditions remains under-characterized. By employing metatranscriptomic analyses of in situ microbial communities along a temporal and depthresolved gradient, we describe the diversity of giant viruses at the Southern Ocean Time Series (SOTS), a site within the subpolar Southern Ocean. Using a phylogeny-guided taxonomic assessment of detected giant virus genomes and metagenome-assembled genomes, we observed depth-dependent structuring of divergent giant virus families mirroring dynamic physicochemical gradients in the stratified euphotic zone. Analyses of transcribed metabolic genes from giant viruses suggest viral metabolic reprogramming of hosts from the surface to a 200-m depth. Lastly, using on-deck incubations reflecting a gradient of iron availability, we show that modulating iron regimes influences the activity of giant viruses in the field. Specifically, we show enhanced infection signatures of giant viruses under both iron-replete and iron-limited conditions. Collectively, these results expand our understanding of how the water column’s vertical biogeography and chemical surroundings affect an important group of viruses within the Southern Ocean
The goal of this project is to develop a highly efficient low-temperature ex-situ Group V diffusion doping approach in the CdCl 2 treated polycrystalline CdTe film using the group V chlorides (i.e., PCl 3 , AsCl 3 , SbCl 3 , and BiCl 3 ) as dopants source. For the first time, our innovative doping strategies through the low-temperature ex-situ Group V doping process in polycrystalline CdSeTe successfully demonstrated a promising power conversion efficiency of ~19% compared to the Cu-doped counterparts. Our newly developed low-temperature ex-situ group V doping allows dedicated control of group V diffusion amount, generates a desirable depth profile, and is completely compatible with commercial CdTe module manufacturing. We built the partnership with the largest CdTe solar module manufacturing in the US, e.g., First Solar, Inc to further develop these low-temperature diffusion doped CdSeTe solar cells. Our technology was granted US Patent No. US11257977B2. In this project, we systematically investigate and characterize the new ex-situ group V doping mechanisms, defect chemistry, microstructure, and device physics in CdTe solar cells by combining experimental and theoretical means to pave the way to achieve lower cost toward $\$$0.02/kWh and higher power conversion efficiency (PCE) toward 25% in polycrystalline CdTe solar technology. This project will benefit the public by providing more affordable solar electricity and provide an effective way to address climate change.
Triaxial compression experiments are commonly used to characterize the elastic and inelastic behavior of geomaterials. In situ measurements of grain kinematics, particle breakage, stresses, and other microscopic phenomena have seldom been made during such experiments, particularly at high pressures relevant to many geologic and man-made processes, limiting our fundamental understanding. To address this issue, we developed a new triaxial compression device called HP-TACO (High-Pressure TriAxial COmpression Apparatus). HP-TACO is a miniaturized, conventional triaxial compression apparatus permitting confining pressures up to 50 MPa and deviatoric straining of materials, while also allowing in situ x-ray measurements of grain-scale kinematics and stresses. Here, in this study, we present the design of and first results from HP-TACO during its use in laboratory and synchrotron settings to study grain-scale kinematics and stresses in triaxially compressed sands subjected to 15 and 30 MPa confining pressures. The data highlight the unique capabilities of HP-TACO for studying the high-pressure mechanics of sands, providing new insight into micromechanical processes occurring during geologic and man-made processes.
Future in-situ lunar/martian resource utilization and characterization, as well as the scientific search for life on Mars, will require access to the subsurface and hence drilling. Drilling on Earth is hard - an art form more than an engineering discipline. Human operators listen and feel drill string vibrations coming from kilometers underground. Abundant mass and energy make it possible for terrestrial drilling to employ brute-force approaches to failure recovery and system performance issues. Space drilling will require intelligent and autonomous systems for robotic exploration and to support human exploration. Eventual in-situ resource utilization will require deep drilling with probable human-tended operation of large-bore drills, but initial lunar subsurface exploration and near-term ISRU will be accomplished with lightweight, rover-deployable or standalone drills capable of penetrating a few tens of meters in depth. These lightweight exploration drills have a direct counterpart in terrestrial prospecting and ore-body location, and will be designed to operate either human-tended or automated. NASA and industry now are acquiring experience in developing and building low-mass automated planetary prototype drills to design and build a pre-flight lunar prototype targeted for 2011-12 flight opportunities. A successful system will include development of drilling hardware, and automated control software to operate it safely and effectively. This includes control of the drilling hardware, state estimation of both the hardware and the lithography being drilled and state of the hole, and potentially planning and scheduling software suitable for uncertain situations such as drilling. Given that Humans on the Moon or Mars are unlikely to be able to spend protracted EVA periods at a drill site, both human-tended and robotic access to planetary subsurfaces will require some degree of standalone, autonomous drilling capability. Human-robotic coordination will be important, either between a robotic drill and humans on Earth, or a human-tended drill and its visiting crew. The Mars Analog Rio Tinto Experiment (MARTE) is a current project that studies and simulates the remote science operations between an automated drill in Spain and a distant, distributed human science team. The Drilling Automation for Mars Exploration (DAME) project, by contrast: is developing and testing standalone automation at a lunar/martian impact crater analog site in Arctic Canada. The drill hardware in both projects is a hardened, evolved version of the Advanced Deep Drill (ADD) developed by Honeybee Robotics for the Mars Subsurface Program. The current ADD is capable of 20m, and the DAME project is developing diagnostic and executive software for hands-off surface operations of the evolved version of this drill. The current drill automation architecture being developed by NASA and tested in 2004-06 at analog sites in the Arctic and Spain will add downhole diagnosis of different strata, bit wear detection, and dynamic replanning capabilities when unexpected failures or drilling conditions are discovered in conjunction with simulated mission operations and remote science planning. The most important determinant of future 1unar and martian drilling automation and staffing requirements will be the actual performance of automated prototype drilling hardware systems in field trials in simulated mission operations. It is difficult to accurately predict the level of automation and human interaction that will be needed for a lunar-deployed drill without first having extensive experience with the robotic control of prototype drill systems under realistic analog field conditions. Drill-specific failure modes and software design flaws will become most apparent at this stage. DAME will develop and test drill automation software and hardware under stressful operating conditions during several planned field campaigns. Initial results from summer 2004 tests show seven identifi distinct failure modes of the drill: cuttings-removal issues with low-power drilling into permafrost, and successful steps at executive control and initial automation.
Herein, we focus on understanding the microstructure-fracture correlations in a Ti–6Al– 4 V alloy additively manufactured via electron beam melting (EBM) and subjected to various post-process heat-treatments. Specifically, the as fabricated material is subjected to a sub-transus heat-treatment followed by air-cooling and a super-transus heat-treatment followed by either air- or furnace-cooling. Next, a series of in-situ single edge notch tension (SENT) tests are carried out under a high-resolution digital optical microscope. The panoramic high-resolution images captured during the in-situ tests are then used to characterize the planar deformation on the specimen surface using microstructure-based digital image correlation (DIC). Additionally, the results of the in-situ SENT tests together with DIC and post-mortem fractographic analyses provided us with a better understanding of the microstructure-fracture correlations in these materials. Our results show that the fracture mechanism of the as fabricated and sub-transus heat-treated materials is essentially the same, while the changes in the microstructure following the super-transus heat-treatments significantly affects the fracture mechanism. In this case, several microcracks of hundreds of microns in length first nucleate away from the deformed notch following extreme plastic deformation at discrete locations. Furthermore, the location of these microcracks in the super-transus heat-treated materials is extremely sensitive to the details of the underlying microstructure.
Sodium-ion batteries have attracted renewed interest in recent years and are widely studied as a complementary power source to Li-ion batteries for large-scale stationary energy storage and small electric vehicles. Compared with Li-ion batteries, Na-ion batteries offer several advantages, including elemental abundance, lower cost, improved safety, and better low-temperature performance. An in-depth understanding of Na-ion batteries across multiple length and time scales has further accelerated the rapid development of this technology. Among the various advanced characterization techniques used to study Na-ion batteries, neutron scattering has gained significant traction in recent years. It has become a powerful and versatile tool for probing structure, morphology, and sodium-ion dynamics over a wide range of length and time scales. In this article, we will briefly review the development of neutron scattering technology and highlight recent advances in applying neutron-based techniques—including neutron diffraction, total scattering, small-angle scattering, quasi-elastic/inelastic scattering, and neutron imaging—to Na-ion battery materials. We also provide perspectives on future technique developments, particularly in the realm of in situ and operando neutron scattering characterization, and discuss how these approaches could further enhance our understanding of Na-ion battery systems.
The forthcoming Near-Earth Object (NEO) Surveyor space telescope is a foundational asset designed to complete NASA’s congressionally-mandated goal of cataloging ≥90% of NEOs ≥140 meters in size as soon as practical, and discover Earth impactors far in advance. NEO Surveyor is also critical to near-Earth asteroid (NEA) exploration because it will find suitable low-Δv NEAs for robotic and human missions, often on Earth-like orbits with long synodic periods. Such NEAs have usually not been detected until imminent Earth launch opportunities because they were not observable until close to Earth. Discovering them far enough in advance to deploy missions requires a deep-space infrared survey telescope such as NEO Surveyor. In addition to posing hazards and being scientifically important, NEAs contain resources, such as water (OH), that could be utilized off-Earth. They also offer unique opportunities for the most ambitious human voyages ever undertaken. The Apollo program forever changed humanity’s perspective by showing us Earthrise from our Moon through human eyes. Crewed missions to NEAs will forever change our perspective again by showing us Earth as a distant point of light in the heavens as seen from an asteroid by astronauts. Planetary defense endeavors to understand asteroid and comet impact risks and develop mitigation capabilities. NEA exploration is synergistic in multiple ways. NEO Surveyor will discover and help characterize Earth impactors and accessible NEAs. Heavy-lift launch is highly enabling for both human NEA missions and planetary defense. Reconnaissance missions for planetary defense can also characterize NEAs prior to crewed missions. In situ resource utilization (ISRU) systems may be applicable to deflecting or destroying hazardous NEAs. NEA characterization data critically inform planetary defense efforts and indicate NEA types suitable for human exploration or ISRU. In 2010, NASA performed the Near-Earth Object (NEO) Human Space Flight (HSF) Accessible Targets Study (NHATS), creating an automated online system monitoring mission accessibility of NEAs 2 . NHATS database NEAs meet criteria that require less total mission Δv and/or round-trip mission duration than the Martian surface or even Mars orbit. There are currently 4,658 NHATS NEAs, and many rival or exceed lunar orbit/surface accessibility. Thus, NHATS NEAs could be explored by humans prior to attempting a Mars mission. Human missions to NEAs would test human-rated spacecraft systems with less cost and risk than Mars missions. Thus, human missions to NEAs are compelling in their own right while also providing prudent preparation for more demanding Mars missions. Lunar missions can offer similar opportunities, but they differ from NEA missions in important ways. Lunar missions pose less demanding psychological challenges to crew and ground staff. Earth light-time delay for communications is significantly longer during NEA missions. NEA missions are available that require more propulsion system consumables than lunar missions but less than Mars missions. In this paper, we summarize NEA accessibility for human missions, discuss motivations for such missions, survey knowledge about NEAs that informs future human missions, present exemplar mission opportunities to the currently known NHATS NEAs, and describe future work towards enabling human NEA missions.
Advanced battery characterization using in situ/operando neutron imaging is critical for uncovering degradation modes such as lithium (Li) plating in Li-ion batteries (LIBs). However, conventional LIBs hinder operando neutron radiography (NR) and in situ neutron micro-computed tomography (N-μCT) for visualizing Li plating near the graphite-separator interface due to strong attenuation from hydrogen-rich components like PP–PE–PP separators, electrolyte, and Fe-based spacers. In this work, we designed and tested a neutron-friendly battery (NFB) optimized for in situ Li detection during extreme fast charging (XFC). Guided by neutron attenuation cross-sections and material transmission, the NFB enables clear visualization at the graphite–separator interface, which is typically opaque in standard LIBs. Electrochemical tests show the NFB exhibits voltage/current responses like standard cells for up to 50 XFC cycles. However, its lower reversibility and capacity are likely due to Cu-coated Al spacer degradation from delamination or corrosion. We propose titanium spacers as a more stable alternative, albeit requiring custom machining. Using this optimized cell, we achieved simultaneous neutron tomography of multiple cells, capturing in situ 3D images of dead Li accumulation, particularly near graphite edges. These heterogeneous deposits and disconnected Li clusters suggest localized current density hotspots during XFC.
Atmospheric aerosol backscatter, beta, variability gives a direct indication of aerosol loading. Since aerosol variability is governed by regional sources and sinks as well as affected by its transport due to meteorological conditions, it is important to characterize this loading at different locations and times. Lidars are sensitive instruments that can effectively provide high-resolution, large-scale sampling of the atmosphere remotely by measuring aerosol beta, thereby capturing detailed temporal and spatial variability of aerosol loading, Although vertical beta profiles are usually obtained by pulsed lidars, airborne-focused CW lidars, with high sensitivity and short time integration, can provide higher resolution sampling in the vertical, thereby revealing detailed structure of aerosol layers. During the 1995 NASA Multicenter Airborne Coherent Atmospheric Wind Sensor (MACAWS) mission, NASA MSFC airborne-focused CW CO2 Doppler lidars, operating at 9.1 and 10.6-micrometers wavelength, obtained high resolution in situ aerosol beta measurements to characterize aerosol variability. The observed variability in beta at 9.1-micrometers wavelength with altitude is presented as well as comparison with some pulsed lidar profiles.
Space Resources and Their Uses: The idea of using resources in space to support human exploration and settlement or for economic development and profit beyond the surface of Earth has been proposed and discussed for decades. Work on developing a method to extract oxygen from lunar regolith started even before humans set foot on the Moon for the first time. The use of space resources, commonly referred to as In Situ Resource Utilization (ISRU), involves the processes and operations to harness and utilize resources in space (both natural and discarded) to create products for subsequent use. Potential space resources include water, solar wind implanted volatiles (hydrogen, helium, carbon, nitrogen, etc.), vast quantities of metals and minerals in extraterrestrial soils, atmospheric constituents, unlimited solar energy, regions of permanent light and darkness, the vacuum and zero-gravity of space itself, trash and waste from human crew activities, and discarded hardware that has completed its primary purpose. ISRU covers a wide variety of concepts, technical disciplines, technologies, and processes. When considering all aspects of ISRU, there are 5 main areas that are relevant to human space exploration and the commercialization of space: 1. Resource Characterization and Mapping, 2. In Situ Consumables Production, 3. Civil Engineering and Construction, 4. In Situ Energy Production and Storage, and 5. In Situ Manufacturing.
In this work, we describe 3D characterization of an additively manufactured Inconel 625 nickel-base superalloy specimen conducted during a uniaxial tension test using a suite of nondestructive x-ray techniques. High-energy diffraction microscopy in both near- and far-field modalities are employed in situ to track evolution of the material orientation and stress–strain fields at six points during the mechanical test, and these data streams are registered with micro-computed tomography reconstructions which probe the material density. This data volume was matched to a multi-modal serial sectioning characterization of the specimen taken after loading, described in this article’s companion. Twenty-eight grains which were monitored throughout the experiment were selected to form the basis for AFRL AM Modeling Series Challenge 4, Microscale Structure-to-Properties.
The overarching goal of this research program, as originally delineated in the proposal “Tuning anisotropic bonding via chemistry and pressure in layered pnictides and chalcogenides” was to develop a predictive, chemistry-driven understanding of the impact of the phonon behavior on thermal properties of bulk layered materials. At finite temperatures, atomic vibrations (phonons) strongly impact the thermodynamics, thermal and electrical transport, and phase-switching properties of functional materials. In particular, soft phonon modes and strongly anharmonic potentials can have spectacular consequences, including structural phase transitions (for example in ferroelectrics and phase-change memory materials), metal-insulator transitions, and extreme thermal resistance preventing heat propagation. Bulk materials with highly-anisotropic bonding may provide unique strategies to induce soft-phonon modes and lattice instabilities. Recently, increasingly detailed investigations of the lattice dynamics in layered materials have been made possible by the advent of first-principles phonon calculations and advanced characterization techniques based on neutron and X-ray scattering. However, due to the lack of studies in which composition and bonding character are systematically varied, there are still fundamental questions regarding the impacts of anisotropic bonding and anharmonicity on lattice stability and thermal transport. One of the major goals of this research program is therefore to address this gap by coherently tuning bonding anisotropy and anharmonicity across families of related compounds. Such approaches have revealed new strategies for exploiting structural anisotropy in quasi-1D and 2D bulk materials to obtain tailored functional properties. This project systematically explored the lattice dynamics, phase stability, and transport properties in bulk layered materials by using both composition and applied pressure to tune the degree of bonding anisotropy and anharmonicity. To accomplish this work, we combined i) single-crystal growth of key material systems with tunable anisotropy, ii) in-situ high-temperature/high-pressure characterization of structure and phonons to probe bonding anisotropy and anharmonicity, including state-of-the-art inelastic X-ray scattering (IXS) and inelastic neutron scattering (INS), and iii) first-principles simulations leveraging large-scale computing to identify the fundamental origins of the observed effects, by relating atomic structure and dynamics to electronic orbital interactions. Finally, we modeled and verified the impact of the phonon behavior on thermal transport to identify new strategies for a-priori design of thermal conductivity. Our integrated collaborative approach helped to systematically unravel the effects of anisotropy and bonding anharmonicity on phonon transport, thermodynamics, and thermal properties of complex anisotropic materials.