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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Energy conversion and storage via photoinduced polarization change in non-ferroelectric molecular [CoGa] crystals

To alleviate the energy and environmental crisis, in the last decades, energy harvesting by utilizing optical control has emerged as a promising solution. Here we report a polar crystal that exhibits photoenergy conversion and energy storage upon light irradiation. The polar crystal consists of dinuclear [CoGa] molecules, which are oriented in a uniform direction inside the crystal lattice. Irradiation with green light induces a directional intramolecular electron transfer from the ligand to a low-spin Co III centre, and the resultant light-induced high-spin Co II excited state is trapped at low temperature, realizing energy storage. Additionally, electric current release is observed during relaxation from the trapped light-induced metastable state to the ground state, because the intramolecular electron transfer in the relaxation process is accompanied with macroscopic polarization switching at the single-crystal level. It demonstrates that energy storage and conversion to electrical energy is realized in the [CoGa] crystals, which is different from typical polar pyroelectric compounds that exhibit the conversion of thermal energy into electricity.

25 ENERGY STORAGE↗
DOE OSTI2025

Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation

Abstract The direct utilization of dissolved inorganic carbon in seawater for CO 2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO 2 reduction (CO 2 R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO 2 (aq) (CO 2 dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO 2 (aq) as a reactant generated in situ by acidification of HCO 3 - flows continuously from BiVO 4 photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO 4 PEC CO 2 R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale.

Liu, Bin↗
DOE OSTI2026

Catalytic conversion of cellulose and its derived sugars to 5-Hydroxymethylfurfural, levulinate esters, and sorbitol: a comprehensive review

Cellulose, an abundant, renewable, and sustainable non-edible carbon source from agriculture and forestry, has attracted great attention for producing diverse value-added chemicals and fuels. However, the rigid 3D structure of cellulose, maintained by an extensive hydrogen bonding network, hinders chemical conversion, requiring effective pretreatment to break down the crystalline structure. High-value cellulose-derived compounds such as 5-hydroxymethylfurfural (5-HMF), levulinate esters, and sorbitol, recognized as critical platform chemicals by the U.S. Department of Energy, are particularly attractive for versatile applications. This review provides a comprehensive overview of methodologies for the chemical synthesis of 5-HMF, levulinate esters, and sorbitol, focusing on direct catalytic conversion of cellulose. It delves into recent advancements in reaction systems and catalysts, highlighting catalytic pathways, selectivity, strategies for process optimization, and computational approaches, while discussing the challenges associated with the catalytic conversion of cellulose into these high-value products and offering potential strategies for enhancing future catalytic processes.

Huang, Kaixuan [Yancheng Teachers Univ. (China); N↗
DOE OSTI2022

Enabling technologies for the continuous electrically driven conversion of CO 2 and water to multi-carbon products at high current densities

Here, we demonstrate greatly improved conversion of CO 2 using a gas diffusion electrode (GDE) with flowing electrolyte configuration for CO 2 gas delivery in combination with a high surface area nickel phosphide electrocatalyst. This configuration achieves 40–50% selectivity for total carbon products over H 2 formation (HER) at total current densities ranging from 50 to 300 mA cm -2 . We developed a soft-templating method using CTAB detergent micelles for synthesis of phase-pure Ni 2 P, achieving a 260-fold larger surface area (BET) and porous sponge-like morphology that produces stable currents. This catalyst produces mainly one C-product, methylglyoxal (MG, C 3 H 4 O 2 ) with 38–47% overall selectivity, the highest reported selectivity for a 12-electron reduction product. The versatile soft-templating method for electrocatalyst synthesis uses low-temperature (185 °C) that is permissive for incorporation of co-catalysts that are otherwise destroyed by the high temperatures used in traditional solid-state synthesis (SSS). The non-porous Ni 2 P-SSS catalyst produces mainly H 2 at these current densities. Achieving these high currents and C/H selectivity benefits from use of hydrophobic polymers as co-catalyst binders (cationic = Nafion, anionic = PFAEM and neutral = PTFE) to improve CO 2 conversion. PFAEM is the better ionomer for the CO 2 RR at high current density, postulated as due to suppressing CO 2 conversion to inactive bicarbonate. Precipitation of the carbon products as a polycarbonate polymer occurs at high currents.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Decoupling plasma, catalyst, and gaseous mechanisms for non-oxidative methane conversion

Direct non-oxidative methane (CH 4 ) conversion to value-added hydrogen (H 2 ) and C 2 products remains hindered by fundamental catalytic scaling constraints and rapid surface deactivation at elevated temperatures. Plasma-enabled catalysis offers a promising route to overcome the thermodynamic and kinetic barriers of direct non-oxidative methane upgrading at mild conditions, yet control over C–C product selectivity and catalyst stability remains elusive. Here, we establish a unified mechanistic framework including Langmuir–Hinshelwood (L–H) and Langmuir–Rideal (L–R) mechanisms that disentangles the roles of plasma excitation (including vibrationally activated species and radicals), surface temperature (T sur ), and catalyst binding energy in steering CH 4 conversion to H 2 and C 2 hydrocarbons. Through a combination of density functional theory (DFT) informed microkinetic modeling, in situ and ex situ surface characterization, and product quantification under dielectric barrier discharge conditions, we show that vibrationally excited CH 4 lowers activation barriers selectively for dissociative chemisorption, enabling surface activation across a wide range of transition metal catalysts at low thermal energy input. We find that once CH 4 is dissociatively chemisorbed, the branching between C 2 H 2 , C 2 H 4 , and C 2 H 6 is governed by surface properties (carbon binding energy, T sur , etc), regardless of plasma excitation. The DFT informed microkinetic model decouples the effects of molecular activation from surface properties and indentifies operating windows that maximize target yields while suppressing carbon accumulation and subsequent catalytic inactivation. Experiments on polycrystalline Cu/Al 2 O 3 , Ni/Al 2 O 3 , and Pt/Al 2 O 3 validate these predictions, revealing catalyst-dependent branching toward ethane or ethylene and distinct deactivation profiles. We unify these trends into a generalized three-dimensional plasma-thermal-catalytic design space, from which reduced descriptors such as T vib /T sur in the limit of vibrationally excited L–H pathways emerge as predictive metrics. These results enable rational tuning of methane conversion pathways and unlock selective C 2 formation using earth-abundant metals under mild plasma conditions.

catalyst inactivation↗
DOE OSTI2021

Axion-photon conversion in strongly magnetised plasmas

Axion dark matter can resonantly convert to photons in the magnetosphere of neutron stars, possibly giving rise to radio signals observable on Earth. This method for the indirect detection of axion dark matter has recently received significant attention in the literature. The calculation of the radio signal is complicated by a number of effects; most importantly, the gravitational infall of the axions onto the neutron star accelerates them to semi-relativistic speed, and the neutron star magnetosphere is highly anisotropic. Both of these factors complicate the calculation of the conversion of axions to photons. In this work, we present the first fully three-dimensional calculation of the axion-photon conversion in highly magnetised anisotropic media. Depending on the axion trajectory, this calculation leads to orders-of-magnitude differences in the conversion compared to the simplified one-dimensional calculation used so far in the literature, altering the directionality of the produced photons. Our results will have important implications for the radio signal one would observe in a telescope.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Next-to-leading order scalar contributions to 𝜇→𝑒 conversion

Within a class of models in which lepton flavor violation is induced dominantly by scalar particle exchanges, we estimate the 𝜇→𝑒 conversion rate in several nuclei. We include next-to-leading order (NLO) terms in the one- and two-nucleon interactions in chiral effective theory, rectifying some incorrect results in the previous literature. We provide an uncertainty budget for the conversion rates and we find that NLO contributions affect the amplitudes at the level of 10%, which could be larger than the uncertainty on the leading order couplings, dominated by the strange and nonstrange nucleon sigma terms. We study the implications of our results for testing Higgs-mediated charged lepton flavor violation (CLFV) in the future by combining results from various experimental searches, such as 𝜇→𝑒 conversion in multiple target nuclei and 𝜇→𝑒⁢𝛾.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Collisions and collective flavor conversion: Integrating out the fast dynamics

In dense astrophysical environments, notably core-collapse supernovae and neutron star mergers, neutrino-neutrino forward scattering can spawn flavor conversion on very short scales. Scattering with the background medium can impact collective flavor conversion in various ways, either damping oscillations or possibly setting off novel collisional flavor instabilities (CFIs). A key feature in this process is the slowness of collisions compared to the much faster dynamics of neutrino-neutrino refraction. Assuming spatial homogeneity, we leverage this hierarchy of scales to simplify the description accounting only for the slow dynamics driven by collisions. We illustrate our new approach both in the case of CFIs and in the case of fast instabilities damped by collisions. In both cases, our strategy provides new equations, the , that simplify the description of flavor conversion and allow us to qualitatively understand the final state of the system after the instability, either collisional or fast, has saturated. Published by the American Physical Society 2024

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Axionlike-particle contributions to the μ → e conversion

We study the μ → e conversion process in nuclear targets arising in models of axionlike particles (ALPs) with hadronic and charged lepton flavor violating (CLFV) interactions. Contributions to this process generally fall into two categories: spin-independent (SI) and spin-dependent (SD). While the SI contribution can be generated by a dipole operator through purely leptonic ALP interactions, the SD contribution can also be present through ALP-quark interactions at tree-level. It is naively anticipated that the SI contribution would be dominant due to its coherent enhancement. In this paper, we show that is not generically the case; in particular, for naturally sized ALP couplings to quarks of order ∼ m q / f a , the SD interaction induced by ALP- π 0 mixing turns out to be the leading contribution to μ → e conversion. Intuitively, this stems from the suppressed dipole contribution by the QED one-loop factor which counters the effect of SI coherent enhancement. Our study highlights the importance of μ → e conversion searches in exploring the parameter space of generic ALP models, and demonstrates the competitiveness of these searches in probing the CLFV ALP parameter space in the heavy mass range of m a ≳ m μ . Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Axion magnetic resonance: A novel enhancement in axion-photon conversion

We identify a new resonance, axion magnetic resonance, that can greatly enhance the conversion rate between axions and photons. A series of axion search experiments rely on converting them into photons inside a constant magnetic field background. A common bottleneck of such experiments is the conversion amplitude being suppressed by the axion mass when m a ≳ 10 − 4 eV . We point out that a spatial or temporal variation in the magnetic field can cancel the difference between the photon dispersion relation and that of the axion, hence greatly enhancing the conversion probability. We demonstrate that the enhancement can be achieved by both a helical magnetic field profile and a harmonic oscillation of the magnitude. Our approach can extend the projected ALPS II reach in the axion-photon coupling ( g a γ ) by two orders of magnitude at m a = 10 − 3 eV with moderate assumptions (see .) Published by the American Physical Society 2024

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Quasisteady evolution of fast neutrino-flavor conversions

In astrophysical environments such as core-collapse supernovae (CCSNe) and binary neutron star mergers (BNSMs), neutrinos potentially experience substantial flavor mixing due to the refractive effects of neutrino self-interactions. Determining the survival probability of neutrinos in asymptotic states is paramount to incorporating flavor conversions’ effects in the theoretical modeling of CCSN and BNSM. Some phenomenological schemes have shown good performance in approximating asymptotic states of fast neutrino-flavor conversions (FFCs), known as one of the collective neutrino oscillation modes induced by neutrino self-interactions. However, a recent study showed that they would yield qualitatively different asymptotic states of FFC if the neutrino number is forced to evolve. It is not yet fully understood why the canonical phenomenological models fail to predict asymptotic states. In this paper, we perform detailed investigations through numerical simulations and then provide an intuitive explanation with a quasihomogeneous analysis. Based on the analysis, we propose a new phenomenological model, in which the quasisteady evolution of FFCs is analytically determined. The model also allows us to express the convolution term of spatial wave number as a concise form, which corresponds to useful information on analyses for the nonlinear feedback from small-scale flavor conversions to large-scale ones. Furthermore, our model yields excellent agreement with numerical simulations, which lends support to our interpretation.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Nuclear-Level Effective Theory of 𝜇 → 𝑒 Conversion

The Mu2e and COMET 𝜇 → 𝑒 conversion experiments are expected to significantly advance limits on new sources of charged lepton flavor violation. Almost all theoretical work in the field has focused on just two operators. However, general symmetry arguments lead to a 𝜇 → 𝑒 conversion rate with six response functions, each of which, in principle, is observable by varying nuclear properties of targets. We construct a nucleon-level nonrelativistic effective theory (NRET) to clarify the microscopic origin of these response functions and to relate rate measurements in different targets. This exercise identifies three operators and their small parameters that control the NRET operator expansion. We note inconsistencies in past treatments of these parameters. The NRET is technically challenging, involving 16 operators, several distorted electron partial waves, bound muon upper and lower components, and an exclusive nuclear matrix element. We introduce a trick for treating the electron Coulomb effects accurately, which enables us to include all of these effects while producing transition densities whose one-body matrix elements can be evaluated analytically, greatly simplifying the nuclear physics. We derive bounds on operator coefficients from existing and anticipated 𝜇 → 𝑒 conversion experiments. We discuss how similar NRET formulations have impacted dark matter phenomenology, noting that the tools this community has developed could be adapted for charged lepton flavor violation studies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Linear-frequency conversion with time-varying metasurfaces

Frequency conversion is a hallmark of nonlinearity. The spectral manifestations, emergent within a system, can typically be attributed to a marked nonlinearity within the material properties, complex geometric configurations, and/or the unique functional form of interactions taking place in the constitutive subsystems. These phenomena, irrespective of their origins, have been harnessed and exploited in applications ranging from the generation of entangled photons, a cornerstone in quantum technologies, to nanomechanical frequency mixing, advancing subsurface scanning probe microscopy. Here, we propose a frequency conversion mechanism based on time-varying metasurfaces, an emerging frontier in metamaterial research. We show how temporal properties of metasurfaces can effectively emulate a nonlinear medium, thereby facilitating frequency conversion. The proposed material configuration has the potential not only to advance integrated photonics and quantum optics, but also to create opportunities in quantum sensing, quantum materials, and crucially quantum communications. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Efficient Hydraulic-to-electric Energy Conversion for PCM-based Ocean Thermal Gradient Energy System to Power Uncrewed Underwater Vehicles

Since the 2000, there have been numerous investigations into electrical energy storage types that use ocean thermal-to-electricity conversion techniques. Field tests have demonstrated that this technology is feasible for UUVs with long-term missions of over 3,000 km per deployment. Nonetheless, the energy generated by this method is not sufficient to meet the energy requirements of Unscrewed Underwater Vehicles (UUVs). The objective of this study is to design a highly effective ocean thermal gradient energy system to support long-term missions of a UUV. To enhance the performance of the thermal gradient energy system, we have developed a hybrid type (buoyancy regulation and electrical storage). Phase Change Material (PCM)-based energy harvesting system to facilitate efficient UUV operations. A prototype of the hydraulic-to-electric conversion system was implemented, and experimental findings indicate that the hybrid system successfully delivers hydraulic energy for buoyancy change and improved efficiency of hydraulic-to-electric energy conversion, demonstrating its potential as a promising technology for supporting long-term UUV missions.

Deng, Zhiqun↗
DOE OSTI2021

World Record Demonstration of > 30% Thermophotovoltaic Conversion Efficiency

Thermophotovoltaic (TPV) devices are solid-state heat engines that convert thermal radiation into electricity using semiconductor diodes, and have applications in energy storage, primary power conversion, and waste heat recovery. Higher temperature emitters and wider band gap photovoltaics (PVs) generally afford higher TPV efficiencies. High temperature emitters are accessible in thermal energy storage applications. We have demonstrated a world record 31% +/- 2% TPV conversion efficiency with a 0.9 cm2 GaAs-based PV device under a 2430 °C thermal emitter, producing an electrical output power of 2.23 W. Critical to the result was the cell’s high reflectance of photon energies below the device band gap. Unlike solar PV, for which sub-band gap (SBG) light is lost, a TPV cell can reflect and recycle SBG light to the thermal emitter. The demonstration was made on a custom-built measurement platform in which a ~100 cm2 graphite thermal emitter was heated under vacuum up to 2430 °C. The TPV efficiency was evaluated by comparing the measured electrical output power of the TPV with the calorimetrically measured total net power incident on the cell. The measured TPV efficiency as a function of thermal emitter temperature was corroborated by our full system modeling predictions. As far as the authors are aware, this is the highest TPV conversion efficiency ever measured, and device improvements should yield > 40% efficiency in the near future.

27 ARPA - Advanced Research Projects Agency-Energy↗
DOE OSTI2023

Two-step conversion of polyethylene into recombinant proteins using a microbial platform

Background: The increasing prevalence of plastic waste combined with the inefficiencies of mechanical recycling has inspired interest in processes that can convert these waste streams into value-added biomaterials. To date, the microbial conversion of plastic substrates into biomaterials has been predominantly limited to polyhydroxyalkanoates production. Expanding the capabilities of these microbial conversion platforms to include a greater diversity of products generated from plastic waste streams can serve to promote the adoption of these technologies at a larger scale and encourage a more sustainable materials economy. Results: Herein, we report the development of a new strain of Pseudomonas bacteria capable of converting depolymerized polyethylene into high value bespoke recombinant protein products. Using hexadecane, a proxy for depolymerized polyethylene, as a sole carbon nutrient source, we optimized media compositions that facilitate robust biomass growth above 1 × 10 9 cfu/ml, with results suggesting the benefits of lower hydrocarbon concentrations and the use of NH 4 Cl as a nitrogen source. We genomically integrated recombinant genes for green fluorescent protein and spider dragline-inspired silk protein, and we showed their expression in Pseudomonas aeruginosa, reaching titers of approximately 10 mg/L when hexadecane was used as the sole carbon source. Lastly, we demonstrated that chemically depolymerized polyethylene, comprised of a mixture of branched and unbranched alkanes, could be converted into silk protein by Pseudomonas aeruginosa at titers of 11.3 ± 1.1 mg/L. Conclusion: This work demonstrates a microbial platform for the conversion of a both alkanes and plastic-derived substrates to recombinant, protein-based materials. The findings in this work can serve as a basis for future endeavors seeking to upcycle recalcitrant plastic wastes into value-added recombinant proteins.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Use of the lignocellulose-degrading bacterium Caldicellulosiruptor bescii to assess recalcitrance and conversion of wild-type and transgenic poplar

Abstract Background Biological conversion of lignocellulosic biomass is significantly hindered by feedstock recalcitrance, which is typically assessed through an enzymatic digestion assay, often preceded by a thermal and/or chemical pretreatment. Here, we assay 17 lines of unpretreated transgenic black cottonwood ( Populus trichocarpa ) utilizing a lignocellulose-degrading, metabolically engineered bacterium, Caldicellulosiruptor bescii . The poplar lines were assessed by incubation with an engineered C. bescii strain that solubilized and converted the hexose and pentose carbohydrates to ethanol and acetate. The resulting fermentation titer and biomass solubilization were then utilized as a measure of biomass recalcitrance and compared to data previously reported on the transgenic poplar samples. Results Of the 17 transgenic poplar lines examined with C. bescii , a wide variation in solubilization and fermentation titer was observed. While the wild type poplar control demonstrated relatively high recalcitrance with a total solubilization of only 20% and a fermentation titer of 7.3 mM, the transgenic lines resulted in solubilization ranging from 15 to 79% and fermentation titers from 6.8 to 29.6 mM. Additionally, a strong inverse correlation ( R 2 = 0.8) between conversion efficiency and lignin content was observed with lower lignin samples more easily converted and solubilized by C. bescii . Conclusions Feedstock recalcitrance can be significantly reduced with transgenic plants, but finding the correct modification may require a large sample set to identify the most advantageous genetic modifications for the feedstock. Utilizing C. bescii as a screening assay for recalcitrance, poplar lines with down-regulation of coumarate 3-hydroxylase 3 (C3H3) resulted in the highest degrees of solubilization and conversion by C. bescii . One such line, with a growth phenotype similar to the wild-type, generated more than three times the fermentation products of the wild-type poplar control, suggesting that excellent digestibility can be achieved without compromising fitness of the tree.

09 BIOMASS FUELS↗
DOE OSTI2024

A miniaturized feedstocks-to-fuels pipeline for screening the efficiency of deconstruction and microbial conversion of lignocellulosic biomass

Sustainably grown biomass is a promising alternative to produce fuels and chemicals and reduce the dependency on fossil energy sources. However, the efficient conversion of lignocellulosic biomass into biofuels and bioproducts often requires extensive testing of components and reaction conditions used in the pretreatment, saccharification, and bioconversion steps. This restriction can result in a significant and unwieldy number of combinations of biomass types, solvents, microbial strains, and operational parameters that need to be characterized, turning these efforts into a daunting and time-consuming task. Here we developed a high-throughput feedstocks-to-fuels screening platform to address these challenges. The result is a miniaturized semi-automated platform that leverages the capabilities of a solid handling robot, a liquid handling robot, analytical instruments, and a centralized data repository, adapted to operate as an ionic-liquid-based biomass conversion pipeline. The pipeline was tested by using sorghum as feedstock, the biocompatible ionic liquid cholinium phosphate as pretreatment solvent, a “one-pot” process configuration that does not require ionic liquid removal after pretreatment, and an engineered strain of the yeast Rhodosporidium toruloides that produces the jet-fuel precursor bisabolene as a conversion microbe. By the simultaneous processing of 48 samples, we show that this configuration and reaction conditions result in sugar yields (~70%) and bisabolene titers (~1500 mg/L) that are comparable to the efficiencies observed at larger scales but require only a fraction of the time. We expect that this Feedstocks-to-Fuels pipeline will become an effective tool to screen thousands of bioenergy crop and feedstock samples and assist process optimization efforts and the development of predictive deconstruction approaches.

09 BIOMASS FUELS↗