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At least 1,027 records · Page 57
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

How Do Ionic Liquids “Fold” Ionenes? Computational and Experimental Analysis of Imidazolium Polymers Based on Ether and Alkyl Chain Variations Dissolved in an Ionic Liquid

Molecular dynamics (MD) simulations and complementary experiments are used here to understand the inter- and intramolecular structure and conformational properties of ionenes (i.e., cationic polymers formed from condensation reactions) dissolved in an ionic liquid (IL), 1-ethyl-3-methylimidazolium bistriflimide [C 2 mim + ][Tf 2 N - ]. The simulated structural properties are benchmarked against experimental analyses of these same polymers, mainly using dynamic light scattering (DLS) experiments. Four different imidazolium ionenes are considered, corresponding to variations in the chemistry and structure of the repeat units including: (1) poly (decylimidazolium) (PD 10 ); (2) poly (tetraethyleneglycolimidazolium) (PE 10 ); (3) alternating copolymer (P(ED) 5 ); and (4) a block copolymer (PE 5 D 5 ). Detailed computational analyses of the polymer structure and conformational properties were performed, including the radius of gyration, end-to-end distance, torsional distributions, and site-site and spatial distribution functions. Overall, there is a competition between intramolecular associations between the imidazolium groups and the ether sites in the polymers versus the intermolecular interactions of the polymer imidazolium groups with the surrounding anion molecules. The polymer with only ether linkages (PE 10 ) results in the most intramolecular interactions, leading to significant coiling behavior and chain contraction. These strong interactions reduce chain flexibility, but they also result in much more linear chain configurations and alignment of the imidazolium groups. The polymer structure is strongly affected as the concentration of alkyl groups is increased, and we find that the polymer architecture (alternating versus block copolymer) also has an important influence. Furthermore, these detailed observations are important for understanding the connection between the molecular design of imidazolium polymers and their emergent structural properties, which could lead to unique opportunities for creating polymer composites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Doping Effects on Multivalence States, Electronic Structure, and Optical Band Gap in LaCrO 3 under Varied Atmospheres: An Integrated Experimental and Density Functional Theory Study

Doping effects on the valence state, electronic structure, and optical band and the effects on electrical conductivity were studied on the doped lanthanum chromite (LaCrO 3 ) system. The specific compositions studied were La 1–x Ca x CrO 3 (LCCx), La 1–x Sr x CrO 3 (LSCx), and La 0.8 Sr 0.2 Cr 1–x Mn x O 3 (LSCMx) (0.1 ≤ x ≤ 0.4). The powders were synthesized using a modified Pechini sol–gel method, and the ceramic samples were densified using a reactive sintering method resulting in densities >96% theoretical. X-ray photoelectron spectroscopy (XPS) was completed to characterize the defect states and cationic valence compensation as a result of divalent (Ca 2+ or Sr 2+ ) and trivalent (Mn 3+ ) substitutions. XPS was completed for samples tested in oxidizing and reducing atmospheres (up to 1500 °C), which provided insights into the oxidation state transitions induced by the Ca 2+ and Sr 2+ dopants. The work notably demonstrated, for the first time, the oxidation/reduction transitions of Cr 4+ to Cr 3+ in Sr 2+ /Mn 3+ co-doped samples under reducing atmospheres. Reflectance UV–vis spectrophotometry optical band gap measurements were also completed for the same materials; a decrease in the optical band gap (2.81–3.12 eV) was shown with increased substitution, suggesting electronic structure modifications in the LaCrO 3 perovskite. Density functional theory calculations validated experimental trends, predicting a diminishing band gap with a rising dopant concentration. The transition in Cr oxidation states was attributed to the presence of divalent/trivalent cations. These findings contribute some insights into methods to tune the LaCrO 3 electrical properties for various low- and high-temperature applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Curated Collection of More than 20,000 Experimentally Reported One-Dimensional Metal–Organic Frameworks

Herein, a collection of more than 20,000 experimentally derived crystal structures for metal–organic frameworks (MOFs) that do not have two- or three-dimensional covalently bonded networks has been developed from the materials available at the Cambridge Crystallographic Data Centre. Of these 20,000 1D MOFs, more than 12,000 structures have been verified to be solvent-free and in exact agreement with the stoichiometry of the synthesized materials. More than 10% of the complete data set comprise materials including two or more distinct metals. The band gaps of more than 12,000 1D MOFs have been computed at the density functional theory-generalized gradient approximation level, finding more than 2000 materials that have a zero band gap. Molecular simulations of CH4 adsorption in a small number of 1D MOFs indicated that adsorbate-induced deformation plays a significant role in determining adsorption isotherms in these materials. As a result, methods that have been used previously for high-throughput predictions of molecular adsorption in 3D MOFs are not suitable for 1D MOFs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Mechanistic Understanding of Methane Combustion over Ni/CeO 2 : A Combined Experimental and Theoretical Approach

Catalytic oxidation of methane (CH 4 ) over nonprecious Ni/CeO 2 catalysts has received a lot of attention due to the large natural gas reserves found in North America and the prohibitive cost of palladium-based catalysts, commonly used for CH 4 oxidation. However, the catalytic mechanism of CH 4 oxidation over Ni/CeO 2 still remains unclear. Moreover, the parameters affecting the reaction rates, the interaction between nickel and CeO 2 , and the reaction intermediates are still not well understood. In this study, kinetic model fitting, CH 4 temperature-programmed reduction-mass spectroscopy (CH 4 TPR-MS), in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), and density functional theory (DFT) calculations were combined to elucidate the mechanism of complete oxidation of CH 4 over Ni/CeO 2 . CH 4 TPR-MS showed that the complete oxidation of CH 4 over Ni/CeO 2 requires 55–120 °C lower compared to bare CeO 2 or Ni/quartz sand; complete oxidation of CH 4 took place when the surface oxygen species were abundant, while partial oxidation products (CO, H 2 ) were formed when the oxygen species were depleted. In situ DRIFTS showed that CH 3 , CH 2 , CO, and CO 2 were formed after CH 4 activation over Ni/CeO 2 , while CH 3 O species were not observed. Combining those findings with kinetic model fitting, a redox Mars–van Krevelen (MvK) mechanism showed the best description of the experimental observations. The MvK mechanism involves the reaction of dissociated oxygen species with gas-phase CH 4 while water inhibits the reaction rate by adsorbing on the oxidized sites. Moreover, CH 4 activation leads to the reduction of the active sites and oxygen vacancy formation followed by reoxidation of the active sites by gas-phase O 2 . A CH 4 oxidation reaction pathway over Ni/CeO 2 is proposed by DFT calculations. In summary, the findings shown here suggest that CH 4 oxidation over Ni/CeO 2 follows a redox MvK mechanism and provides guidance for the rational design of non-precious-metal catalysts for CH 4 oxidation reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Correlating Experimentally Determined Hydrogen Binding Energy with Hydrogen Evolution Activity over Metal Monolayers on Molybdenum Nitride

It is well established that hydrogen binding energy (HBE) is a key descriptor for hydrogen evolution reaction (HER) activity, and such a relationship is a useful tool for searching efficient and cost-effective HER catalysts. However, in almost all cases, the HBE values are obtained from density functional theory (DFT) calculations. Here in this study, temperature programmed desorption (TPD) was used to experimentally determine the HBE values of metal monolayers supported on molybdenum nitride (Mo 2 N), and electrochemical measurements were performed on the same surfaces. Combined DFT and kinetic Monte Carlo (kMC) simulations were used to validate the trend observed with TPD and the electrochemical HER activity. Depositing one monolayer of Pt on Mo 2 N led to similar HBE values seen for bulk Pt, and electrochemical measurements showed that monolayer Pt on Mo 2 N had similar HER activity to that of bulk Pt. Similar studies were also performed for monolayer Pd on Mo 2 N to confirm the correlation. This work also demonstrates that Mo 2 N is a promising support to reduce precious metal loading in HER catalysts.

08 HYDROGEN↗
DOE OSTI2020

Too Many Materials and Too Many Applications: An Experimental Problem Waiting for a Computational Solution

Finding the best material for a specific application is the ultimate goal of materials discovery. However, there is also the reverse problem: when experimental groups discover a new material, they would like to know all the possible applications this material would be promising for. Computational modeling can aim to fulfill this expectation, thanks to the sustained growth of computing power and the collective engagement of the scientific community in developing more efficient and accurate workflows for predicting materials' performances. We discuss the impact that reproducibility and automation of the modeling protocols have on the field of gas adsorption in nanoporous crystals. We envision a platform that combines these tools and enables effective matching between promising materials and industrial applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Combined First-Principles and Experimental Investigation into the Reactivity of Codeposited Chromium–Carbon under Pressure

High-pressure synthesis in the diamond anvil cell suffers from the lack of a general approach for the control of precursor stoichiometry and homogeneity. Here, we present results from a new method we have developed that uses magnetron cosputtering to prepare stoichiometrically precise and atomically mixed amorphous films of Cr:C. Laser-heated diamond anvil cell experiments carried out on a flake of this sample at pressures between 13.5 and 24.3 GPa lead to the observation of Cr 3 C (Pnma) over the entire pressure range–in good agreement with our in-house theoretical predictions–but also reveal two other metastable phases that were not expected: a novel monoclinic chromium carbide phase and the NaCl-type CrC (Fm3̅m) phase. The unexpected stability of CrC is investigated by using first-principles methods, revealing a large stabilizing effect tied to substoichiometry at the carbon site. These results offer an important case study into the current limitations of crystal structure prediction methods with regard to phase complexity and bolster the growing need for advanced theoretical approaches that can more completely survey experimentally unexplored phase space.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Modeling Structural Colors from Disordered One-Component Colloidal Nanoparticle-Based Supraballs Using Combined Experimental and Simulation Techniques

Bright, saturated structural colors in birds have inspired synthesis of self-assembled, disordered arrays of assembled nanoparticles with varied particle spacings and refractive indices. However, predicting colors of assembled nanoparticles, and thereby guiding their synthesis, remains challenging due to the effects of multiple scattering and strong absorption. In this work, we use a computational approach to first reconstruct the nanoparticles’ assembled structures from small-angle scattering measurements and then input the reconstructed structures to a finite-difference time-domain method to predict their color and reflectance. This computational approach is successfully validated by comparing its predictions against experimentally measured reflectance and provides a pathway for reverse engineering colloidal assemblies with desired optical and photothermal properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Experimental Measurement of Particle-to-Particle Heat Transfer in Nanoparticle Solids

Thermal conductivity in nanoparticle solids has been previously reported in the range of 0.1-1 W m -1 K -1 , which is a much smaller variation than the orders of magnitude differences achievable in electrical conductivity of similar systems. Both the low absolute magnitude of thermal conductivity and the relative insensitivity compared to electrical conductivity may be largely attributed to the poor interfacial thermal conductance of the many interfaces of the nanocrystal solid, but a direct experimental study of these interfaces is challenging. Here, in this work, we overcome this challenge via direct spectroscopic observation of heat flow within the components of a nanocrystal solid. These thermal transfers are studied by mixing two distinct types of particles: one that serves as a selectively excited antenna to inject heat and the other as the thermal acceptor to report the time-dependent change in temperature. Using transient spectroscopy, the equilibration between the heat donor and heat acceptor is observed to require similar to ~300 ps at room temperature, speeds up at reduced temperature, and has only weak sensitivity to the relative stoichiometry of the components or the intervening ligands. These results contrast strongly with the 10-20 ps time-scale of through-bond heat transfer at the ligand-particle surface and highlight the substantially lower interfacial thermal conductance of particle-to-particle transport without covalent bonding. It is also found, serendipitously, that the mixed composite films show an unexpected, substantially enhanced nonlinear absorption at the resonant wavelength of the plasmonic particles, which is tentatively attributed to a local field enhancement.

heat transfer↗
DOE OSTI2026

Solvent-Mediated Control of Nanocellulose Dispersion: An Integrated Computational and Experimental Investigation

Fibrillated cellulose derived from forestry feedstocks represents a renewable and high-strength materials platform for circular bioeconomies. However, its practical implementation is hindered by the irreversible aggregation of nanocellulose architectures, including cellulose nanofibers (CNFs). Solvent-based dispersion offers a simple and practical route to prevent CNF aggregation. Here, in this work, we integrate classical and enhanced sampling molecular dynamics (MD) simulations with experimental suspension rheology and atomic force microscopy (AFM) to elucidate how solvent environments tune CNF–CNF interactions and dispersion stability. CNF–CNF contact free energies computed from MD simulations reveal reduced aggregation in acetone/water, γ-valerolactone (GVL)/water, and tetrahydrofuran (THF)/water and pure acetone compared with pure water, reflecting stronger CNF-solvent relative to inter-CNF interactions. Correspondingly, CNF-solvent suspensions in these solvent systems exhibit stronger inter-fibril network structures and enhanced recovery compared to water, indicating improved CNF-solvent affinity. Liquid cell AFM imaging in acetone–water mixtures and in pure acetone further confirm the presence of well-dispersed CNFs. By combining multiscale computation with targeted experiments, this study establishes a rational framework for solvent design to achieve stable nanocellulose dispersions for high-strength biobased materials and efficient bioenergy conversion.

cellulose↗
DOE OSTI2025

Understanding (La,Sr)(Co,Fe)O$_{3-δ}$ Phase Instability within SOECs Using a Combined Experimental and Atomistic Modeling Approach

Understanding the onset of degradation in the air electrode within solid oxide electrolysis cells (SOECs), and the subsequent impact on cell performance, is a critical step in mitigating the performance losses and stability issues of SOECs. In an effort to identify early onset degradation phenomena, SOECs were characterized as fabricated and after testing potentiostatically at 1.3 V for 1000 h at 750 °C. SOEC air electrodes composed of a 1:1 composite of La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3–δ (6428-LSCF) and Gd 0.1 Ce 0.9 O 1.95 (GDC) were studied using synchrotron X-ray diffraction (XRD), scanning transmission electron microscopy coupled with energy dispersive X-ray spectroscopy (STEM-EDS), and X-ray absorption near-edge spectroscopy (XANES) to evaluate the changes in the air electrode structurally and chemically. These techniques show the migration of Sr species from the air electrode through pores in the GDC barrier layer, progressing to the electrolyte boundary, where it accumulates and reacts with (Zr 0.84 Y 0.16 )O 2–δ (YSZ) to form SrZrO 3 . Microscopy results are paired with atomistic simulations to better understand the relationship between the thermodynamic instability of 6428-LSCF and cell fabrication/testing conditions. First-principles calculations reveal that LSCF-6428 is not stable during cell manufacturing and testing conditions, which supports the experimental identification of secondary phases in both as-fabricated and tested cells. Together, these results demonstrate that the challenging environments encountered by SOECs during cell manufacturing and operation lead to instabilities of the target 6428-LSCF anode material and underscore the need for more durable, high-performing SOEC components.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Sustainable Aviation Fuel from High-Strength Wastewater via Membrane-Assisted Volatile Fatty Acid Production: Experimental Evaluation, Techno-economic, and Life-Cycle Analyses

To reduce emissions from combustion of fossil fuels, sustainable aviation fuels (SAFs) have the potential to decarbonize the aviation sector. Redirecting wastes from conventional waste management practices and using them as cost-effective feedstocks for low-carbon fuels can reduce emissions from both waste disposal and fuel combustion. One approach is to upgrade wet wastes to SAF precursors, such as volatile fatty acids (VFAs). Here, in this study, novel membrane-assisted arrested methanogenesis was developed to convert high-strength wastewater to VFAs. Based on experimental results of VFA production, techno-economic and life-cycle analyses were conducted to estimate the potential economic and environmental benefits of SAF production from high-strength wastewater via VFAs. By evaluating three proposed scenarios for VFA production, a minimum production cost of VFA is achieved at $\$$0.60/kg VFA at a wastewater flow rate of 1100 MT/d. For the corresponding VFA-derived SAF, the estimated minimum fuel selling price is $\$$4.64/gasoline gallon equivalent. The life-cycle analysis shows that up to a 71% reduction in greenhouse gas emissions can be achieved relative to its fossil-counterpart along with lower water and fossil-fuel consumption.

09 BIOMASS FUELS↗
DOE OSTI2022

Developing an Undergraduate Research Laboratory for Experimental Physical Chemistry [Book Chapter]

Embarking on a faculty career in physical chemistry at a primarily undergraduate institution (PUI) is exciting, but also overwhelming. Becoming both an effective teacher and a productive researcher requires a good plan, hard work and support from others who understand what it takes to be successful. The phrase, “building a laboratory,” calls to mind the physical construction of a research instrument, but beginning a career at a PUI involves much more than assembling equipment. Funding for the lab must be secured, students must be recruited and mentored, and the lab must be overseen to keep things running on a daily basis. While many of these tasks would also be part of starting a career at a doctoral level institution, there are many special considerations that must be taken into account when working with undergraduate students because their laboratory experience and chemical knowledge are still within those beautiful but nascent stages. Here, this unique aspect makes building a research program challenging, but also very rewarding. Exposing young minds to the wonders of physical chemistry and building personal relationships through the mentoring process can be immensely gratifying. This chapter is a compilation of holistic advice for building an experimental physical chemistry research laboratory for undergraduates, reflecting a typical experience found in the United States.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Experimental Evidence and Mechanistic Description of the Phenolic H-Transfer to the Cu 2 O 2 Active Site of oxy-Tyrosinase

Tyrosinase is a ubiquitous coupled binuclear copper enzyme that activates O 2 towards the regioselective monooxygenation of monophenols to catechols via a mechanism that remains only partially defined. Here, we present new mechanistic insights into the initial steps of this monooxygenation reaction by employing a pre-steady state stopped-flow kinetics approach that allows direct measurement of the monooxygenation rates for a series of para-substituted monophenols by oxy-tyrosinase. The biphasic Hammett plot and the associated solvent kinetic isotope effect values provide direct evidence for an initial H-transfer from the protonated phenolic substrate to the Cu 2 O 2 core of oxy-tyrosinase. The correlation of these experimental results to quantum-mechanics/ molecular-mechanics calculations provides a detailed mechanistic description of this H-transfer step. Furthermore, these new mechanistic insights revise and expand our fundamental understanding Cu 2 O 2 active sites in biology.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

High-Performance Iridium–Molybdenum Oxide Electrocatalysts for Water Oxidation in Acid: Bayesian Optimization Discovery and Experimental Testing

Ir oxides are costly and scarce catalysts for oxygen evolution reaction (OER) in acid. There has been extensive interest in developing alternatives that are either Ir-free or require smaller amounts of Ir to drive the reactions at acceptable rates. One design strategy is to identify Ir-based mixed oxides that achieve similar performance while requiring smaller amounts of Ir. The obstacle to this strategy has been a very large phase space of the Ir-based mixed metal oxides, in terms of the metals combined with Ir and the different crystallographic structures of the mixed oxides, which prevents a thorough exploration of possible materials. In this work, we developed a workflow that uses machine-learning-aided Bayesian optimization in combination with density functional theory to make the exploration of this phase space plausible. This screening identified Mo as a promising dopant for forming acid-tolerant Ir-based oxides for the OER. We synthesized and characterized the Ir–Mo mixed oxides in the form of thin-film electrocatalysts with a known surface area. We show that these mixed oxides exhibited overpotentials ~30 mV lower than a pure Ir control while maintaining 24% lower Ir dissolution rates than the Ir control. Furthermore, these findings suggest that Mo is a promising dopant and highlight the promise of machine learning to guide the experimental exploration and optimization of catalytic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Experimental Definition of the S = 1 π vs S = 2 σ Reactivity and S = 2 Character in the Ground State of an S = 1 Fe IV O Complex

Iron(IV)-oxo intermediates found in iron enzymes and artificial catalysts are competent for H atom abstraction in catalytic cycles. For S = 2 intermediates, both axial and equatorial approaches are well-established. The mechanism for S = 1 sites is not as well understood: an equatorial approach is more energetically favorable, and an axial approach requires crossing from the S = 1 to the S = 2 surface. Here, in this study, we use 1s2p resonant inelastic X-ray scattering (RIXS) and Fe L-edge X-ray absorption spectroscopy on the S = 1 [Fe IV O(TMC)(CH3CN)] 2+ and observe both S = 2 and S = 1 final states, which enables the experimental evaluation of the energetics of the axial and equatorial reactivity of an S = 1 Fe IV O center on its S = 2 vs S = 1 surface. The observation of S = 2 final states in the RIXS spectrum demonstrates significant S = 2 character spin–orbit mixed into the S = 1 ground state.

energy↗
DOE OSTI2025

High-Pressure Effects on an Octa-Hydrated Curium Complex: An Experimental and Theoretical Investigation

An octa-hydrated curium compound [Cm(H 2 O) 8 ](Hdtp)(dtp)·H 2 O (Cm1,H 2 dtp = 2,3-di(tetrazol-5-yl)pyrazine) along with its lanthanide analogues [Ln(H 2 O) 8 ](Hdtp)-(dtp)·H 2 O (Ln1, Ln 3+ = La 3+ –Nd 3+ , Sm 3+ –Lu 3+ ) were synthesized and characterized using single crystal X-ray diffraction and spectroscopic methods. Bond length analysis of VIII Cm(III)–OH 2 (where VIII refers to the coordination number) was compared to VIII Ln(III)–OH 2 (Ln 3+ = Nd 3+ and Sm 3+ ), indicating similar VIII M(III)–OH 2 bond lengths owing to the similar eight-coordinate ionic radii of these VIII M(III) cations. Owing to the reduced coordination number, the VIII Cm(III)–OH 2 bond lengths were shorter than previously reported IX Cm(III)–OH 2 bonds in [Cm(H 2 O) 9 ](CF 3 SO 3 ) 3 . The octa-aquo complexes were also characterized by solid-state UV–vis–NIR spectroscopy in addition to variable-temperature and variable-pressure photoluminescence. Variable-pressure absorption spectra of Cm1 were compared with Ln1 and show that the Cm(III) f → f transitions have a stronger dependence on pressure than that observed in Ln1 (Ln 3+ = Nd 3+ and Sm 3+ ). The experimental and computational analyses reveal that the monotonic decrease in the computed energy difference between the ground state and the first excited state corresponds to the observed red shift of the photoluminescence peak. This is accompanied by a gradual reduction in the average Cm(III)–OH 2 bond length and a delocalization of spin densities, alongside an intensified interaction involving the 5f orbitals under increasing pressure. Furthermore, these changes accommodate the new geometry and collectively modify the energy landscape, resulting in peak broadening and quenching.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Experimental Investigation of Hydraulic Fracturing and Stress Sensitivity of Fracture Permeability Under Changing Polyaxial Stress Conditions

Understanding and predicting fracture propagation and subsequent fluid flow characteristics is critical to geoenergy technologies that engineer and/or utilize favorable geological conditions to store or extract fluids from the subsurface. Fracture permeability decreases nonlinearly with increasing normal stress, but the relationship between shear displacement and fracture permeability is less well understood. We utilize the new Geo–Reservoir Experimental Analogue Technology (GREAT cell), which can apply polyaxial stress states and realistic reservoir temperatures and pressures to cylindrical samples and has the unique capability to alter both the magnitude and orientation of the radial stress field by increments of 11.25° during an experiment. We load synthetic analogue materials and real rock samples to stress conditions representative of 500–1,000 m depth, investigate the hydraulic stimulation process, and then conduct flow experiments while changing the fluid pressure and the orientation of the intermediate and minimum principal stresses. High–resolution circumferential strain measurements combined with fluid pressure data indicate fracture propagation can be both stable (no fluid pressure drop) and unstable (fluid pressure drop). The induced fractures exhibit both opening and shear displacements during their creation and/or during fluid flow with changing radial stress states. Flow tests during radial stress field rotation reveal that fracture normal effective stress has first–order control on fracture permeability but increasing fracture offset can lead to elevated permeabilities at maximum shear stress. Here, the results have implications for our conceptual understanding of fracture propagation as well as fluid flow and deformation around fractures.

58 GEOSCIENCES↗