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At least 667 records · Page 37

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DOE OSTI2017

Observed positive vegetation-rainfall feedbacks in the Sahel dominated by a moisture recycling mechanism

Classic, model-based theory of land-atmosphere interactions across the Sahel promote positive vegetation-rainfall feedbacks dominated by surface albedo mechanism. However, neither the proposed positive vegetation-rainfall feedback nor its underlying albedo mechanism has been convincingly demonstrated using observational data. Here, we present observational evidence for the region’s proposed positive vegetation-rainfall feedback on the seasonal to interannual time scale, and find that it is associated with a moisture recycling mechanism, rather than the classic albedo-based mechanism. Positive anomalies of remotely sensed vegetation greenness across the Sahel during the late and post-monsoon periods favor enhanced evapotranspiration, precipitable water, convective activity and rainfall, indicative of amplified moisture recycling. The identified modest low-level cooling and anomalous atmospheric subsidence in response to positive vegetation greenness anomalies are counter to the responses expected through the classic vegetation-albedo feedback mechanism. The observational analysis further reveals enhanced dust emissions in response to diminished Sahel vegetation growth, potentially contributing to the positive vegetation-rainfall feedback.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Selective cobalt and nickel electrodeposition for lithium-ion battery recycling through integrated electrolyte and interface control

Abstract Molecularly-selective metal separations are key to sustainable recycling of Li-ion battery electrodes. However, metals with close reduction potentials present a fundamental challenge for selective electrodeposition, especially for critical elements such as cobalt and nickel. Here, we demonstrate the synergistic combination of electrolyte control and interfacial design to achieve molecular selectivity for cobalt and nickel during potential-dependent electrodeposition. Concentrated chloride allows for the speciation control via distinct formation of anionic cobalt chloride complex (CoCl 4 2- ), while maintaining nickel in the cationic form ([Ni(H 2 O) 5 Cl] + ). Furthermore, functionalizing electrodes with a positively charged polyelectrolyte (i.e., poly(diallyldimethylammonium) chloride) changes the mobility of CoCl 4 2- by electrostatic stabilization, which tunes cobalt selectivity depending on the polyelectrolyte loading. This strategy is applied for the multicomponent metal recovery from commercially-sourced lithium nickel manganese cobalt oxide electrodes. We report a final purity of 96.4 ± 3.1% and 94.1 ± 2.3% for cobalt and nickel, respectively. Based on a technoeconomic analysis, we identify the limiting costs arising from the background electrolyte, and provide a promising outlook of selective electrodeposition as an efficient separation approach for battery recycling.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Ionomer-free and recyclable porous-transport electrode for high-performing proton-exchange-membrane water electrolysis

Abstract Clean hydrogen production requires large-scale deployment of water-electrolysis technologies, particularly proton-exchange-membrane water electrolyzers (PEMWEs). However, as iridium-based electrocatalysts remain the only practical option for PEMWEs, their low abundance will become a bottleneck for a sustainable hydrogen economy. Herein, we propose high-performing and durable ionomer-free porous transport electrodes (PTEs) with facile recycling features enabling Ir thrifting and reclamation. The ionomer-free porous transport electrodes offer a practical pathway to investigate the role of ionomer in the catalyst layer and, from microelectrode measurements, point to an ionomer poisoning effect for the oxygen evolution reaction. The ionomer-free porous transport electrodes demonstrate a voltage reduction of > 600 mV compared to conventional ionomer-coated porous transport electrodes at 1.8 A cm −2 and <0.1 mg Ir cm −2 , and a voltage degradation of 29 mV at average rate of 0.58 mV per 1000-cycles after 50k cycles of accelerated-stress tests at 4 A cm −2 . Moreover, the ionomer-free feature enables facile recycling of multiple components of PEMWEs, which is critical to a circular clean hydrogen economy.

08 HYDROGEN↗

DOE OSTI2017

High-Performance Flexible Supercapacitors obtained via Recycled Jute: Bio-Waste to Energy Storage Approach

In search of affordable, flexible, lightweight, efficient and stable supercapacitors, metal oxides have been shown to provide high charge storage capacity but with poor cyclic stability due to structural damage occurring during the redox process. Here, we develop an efficient flexible supercapacitor obtained by carbonizing abundantly available and recyclable jute. The active material was synthesized from jute by a facile hydrothermal method and its electrochemical performance was further enhanced by chemical activation. Specific capacitance of 408 F/g at 1 mV/s using CV and 185 F/g at 500 mA/g using charge-discharge measurements with excellent flexibility (~100% retention in charge storage capacity on bending) were observed. The cyclic stability test confirmed no loss in the charge storage capacity of the electrode even after 5,000 charge-discharge measurements. In addition, a supercapacitor device fabricated using this carbonized jute showed promising specific capacitance of about 51 F/g, and improvement of over 60% in the charge storage capacity on increasing temperature from 5 to 75 °C. Based on these results, we propose that recycled jute should be considered for fabrication of high-performance flexible energy storage devices at extremely low cost.

Science & Technology - Other Topics↗

DOE OSTI2023

Depolymerization of polyesters by a binuclear catalyst for plastic recycling

Plastics play an essential role in modern society, however, the relentless growth of their production is threatening both human health and ecosystems. As a result, there are intensive efforts in developing recycling technologies to repurpose waste plastics into the building blocks for valuable materials. Here we show a binuclear complex that can catalyze the degradation of polyethylene terephthalate (PET)-the most widely used polyester globally-and a wide spectrum of other plastics including polylactic acid (PLA), polybutylene adipate terephthalate (PBAT), polycaprolactone (PCL), polyurethane (PU) and Nylon 66. Inspired by hydrolases, the group of enzymes that catalyze bond cleavages with water, the present catalyst design features biomimetic Zn-Zn sites which activate the plastic, stabilize the key intermediate, and enable intramolecular hydrolysis. This synthetic catalyst delivers activities of 36 mg PET d -1 g catal -1 toward PET depolymerization at pH 8 and 40 oC, and of 577 g PET d -1 g catal -1 at pH 13 and 90 oC for scalable PET recycling. We further demonstrate the closed-loop production of a bottle-grade PET. This work presents a practical and viable solution to the sustainable management of plastics waste.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Chemical and Biological Catalysis for Plastics Recycling and Upcycling

Plastics pollution is causing an environmental crisis, prompting the development of new approaches for recycling, and upcycling. Here, we review challenges and opportunities in chemical and biological catalysis for plastics deconstruction, recycling, and upcycling. We stress the need for rigorous characterization and use of widely available substrates, such that catalyst performance can be compared across studies. Where appropriate, we draw parallels between catalysis on biomass and plastics, as both substrates are low-value, solid, recalcitrant polymers. Innovations in catalyst design and reaction engineering are needed to overcome kinetic and thermodynamic limitations of plastics deconstruction. Either chemical and biological catalysts will need to act interfacially, where catalysts function at a solid surface, or polymers will need to be solubilized or processed to smaller intermediates to facilitate improved catalyst–substrate interaction. Overall, developing catalyst-driven technologies for plastics deconstruction and upcycling is critical to incentivize improved plastics reclamation and reduce the severe global burden of plastic waste.

28 EE - Advanced Manufacturing Office (EE-5A)↗

DOE OSTI2016

Light-trapping and recycling for extraordinary power conversion in ultra-thin gallium-arsenide solar cells

Here, we demonstrate nearly 30% power conversion efficiency in ultra-thin (~200 nm) gallium arsenide photonic crystal solar cells by numerical solution of the coupled electromagnetic Maxwell and semiconductor drift-diffusion equations. Our architecture enables wave-interference-induced solar light trapping in the wavelength range from 300-865 nm, leading to absorption of almost 90% of incoming sunlight. Our optimized design for 200 nm equivalent bulk thickness of GaAs, is a square-lattice, slanted conical-pore photonic crystal (lattice constant 550 nm, pore diameter 600 nm, and pore depth 290 nm), passivated with AlGaAs, deposited on a silver back-reflector, with ITO upper contact and encapsulated with SiO 2 . Our model includes both radiative and non-radiative recombination of photo-generated charge carriers. When all light from radiative recombination is assumed to escape the structure, a maximum achievable photocurrent density (MAPD) of 27.6 mA/cm 2 is obtained from normally incident AM 1.5 sunlight. For a surface non-radiative recombination velocity of 10 3 cm/s, this corresponds to a solar power conversion efficiency of 28.3%. When all light from radiative recombination is trapped and reabsorbed (complete photon recycling) the power conversion efficiency increases to 29%. If the surface recombination velocity is reduced to 10 cm/sec, photon recycling is much more effective and the power conversion efficiency reaches 30.6%.

14 SOLAR ENERGY↗

DOE OSTI2021

Intelligence-assisted predesign for the sustainable recycling of lithium-ion batteries and beyond

The unprecedented consumption of lithium-ion batteries (LIBs) is occurring to meet the needs of modern transportation electrification. Recycling-friendly designs intrinsically facilitate the long-term sustainable utilization of natural resources, reducing the detrimental impacts of spent LIBs on the environment, and improving the economic viability of recycling. For this, we propose the incorporation of an intelligence-assisted predesign strategy into the battery-management system and battery chemistry, including ameliorating the traceability of battery structure and operation status, promoting cost-effective material sorting and separation, and adopting sustainable battery materials. The purposeful predesign of intelligent “Reuse–Refurbish–Recover” (3R) LIBs could be realized in an economically and environmentally sustainable (EES) manner. We report the intelligence-assisted predesign strategy will promote multi-disciplinary cooperation in a systematic and synergetic way; in addition, it will empower governments to establish and implement a series of regulations and standards for addressing the environmental pollution issues from spent batteries, thus avoiding the ever-increasing consumption of natural resources.

25 ENERGY STORAGE↗

DOE OSTI2013

Effect of compatibilizer on impact and morphological analysis of recycled HDPE/PET blends

Blends based on recycled high density polyethylene (rHDPE) and recycled polyethylene terephthalate (rPET) were prepared using a corotating twin screw extruder. PET and HDPE are incompatible polymers and their blends showed poor properties. Compatibilization is a step to obtain blends with good mechanical properties and in this work, ethylene glycidyl methacrylate copolymer (E-GMA) was used as a compatibilizing agent. The effect of blends based on rHDPE and rPET with and without a compatibilizer, E-GMA were examined. From the studies clearly showed that the addition of 5% E-GMA increased the impact strength. SEM analysis of rHDPE/rPET blends confirmed the morphological interaction and improved interfacial bonding between two phases.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Study on the recycling of waste PVC compounds from electrical wires

The good mechanical, thermal and electrical properties of poly (vinyl chloride) (PVC) make it a polymer used in many applications, among which is the coating of wires and cables. The processing of PVC for this application is made using the extrusion process. The PVC waste resulting from extrusion can be recycled or placed on landfills. The objective of this work is to develop recycling methods to decrease the amount of PVC stored in landfills. This work evaluated the influence of successive processing of PVC on the final properties of the obtained compound, which will be used in the process of coating wire and cable by extrusion. The mechanical properties of the electrical wires were assessed according to the Brazilian Association of Technical Standards (ABNT NBR 6251). Tests of tensile strength, elongation at break, before and after thermal aging in an oven with air circulation for a period of 168 hours at 100 °C were performed. The degradation of the PVC compound was carried out through Fourier transform infrared spectroscopy (FTIR) and mechanical properties evaluation. The results showed that the compound can be reprocessed five times keeping the minimum requirements of the ABNT NBR 6251 Standard. Reprocessing was stopped upon color changing (yellowing) of the compound. Yellowing is a characteristic degradation behavior by dehydrochlorination of PVC. FTIR analysis showed changes at 1600 cm{sup −1}, 1430 cm{sup −1}, 685 cm{sup −1} and 614 cm{sup −1} bands. The performance of the PVC compound for coating electrical wire and cable was fair, meeting the requirements of the ABNT NBR 6251 Standard even after five reprocessing cycles.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Ideal solar cell equation in the presence of photon recycling

Previous derivations of the ideal solar cell equation based on Shockley's p-n junction diode theory implicitly assume negligible effects of photon recycling. This paper derives the equation in the presence of photon recycling that modifies the values of dark saturation and light-generated currents, using an approach applicable to arbitrary three-dimensional geometries with arbitrary doping profile and variable band gap. The work also corrects an error in previous work and proves the validity of the reciprocity theorem for charge collection in such a more general case with the previously neglected junction depletion region included.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2012

A POPULATION OF NON-RECYCLED PULSARS ORIGINATING IN GLOBULAR CLUSTERS

We explore the enigmatic population of long-period, apparently non-recycled pulsars in globular clusters, building on recent work by Boyles et al. This population is difficult to explain if it formed through typical core-collapse supernovae, leading many authors to invoke electron capture supernovae. While Boyles et al. dealt only with non-recycled pulsars in clusters, we focus on the pulsars that originated in clusters but then escaped into the field of the Galaxy due to the kicks they receive at birth. The magnitude of the kick induced by electron capture supernovae is not well known, so we explore various models for the kick velocity distribution and size of the population. The most realistic models are those where the kick velocity is {approx}< 10 km s{sup -1} and where the number of pulsars scales with the luminosity of the cluster (as a proxy for cluster mass). This is in good agreement with other estimates of the electron capture supernovae kick velocity. We simulate a number of large-area pulsar surveys to determine if a population of pulsars originating in clusters could be identified as being separate from normal disk pulsars. We find that the spatial and kinematical properties of the population could be used, but only if large numbers of pulsars are detected. In fact, even the most optimistic surveys carried out with the future Square Kilometer Array are likely to detect <10% of the total population, so the prospects for identifying these as a separate group of pulsars are presently poor.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Recycled dark matter

Here, we outline a new production mechanism for dark matter that we dub “recycling”: dark sector particles are kinematically trapped in the false vacuum during a dark phase transition; the false pockets collapse into primordial black holes (PBHs), which ultimately evaporate before Big Bang Nucleosynthesis (BBN) to reproduce the dark sector particles. The requirement that all PBHs evaporate prior to BBN necessitates high scale phase transitions and hence high scale masses for the dark sector particles in the true vacuum. Our mechanism is therefore particularly suited for the production of ultra heavy dark matter (UHDM) with masses above ~10 12 GeV. The correct relic density of UHDM is obtained because of the exponential suppression of the false pocket number density. Recycled UHDM has several novel features: the dark sector today consists of multiple decoupled species that were once in thermal equilibrium and the PBH formation stage has extended mass functions whose shape can be controlled by IR operators coupling the dark and visible sectors.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2017

Establishment of a low recycling state with full density control by active pumping of the closed helical divertor at LHD

We report superior control of particle recycling and hence full governance of plasma density has been established in the Large Helical Device (LHD) using largely enhanced active pumping of the closed helical divertor (CHD). In-vessel cryo-sorption pumping systems inside the CHD in five out of ten inner toroidal divertor sections have been developed and installed step by step in the LHD. The total effective pumping speed obtained was 67 ± 5 m3 s -1 in hydrogen, which is approximately seven times larger than previously obtained. As a result, a low recycling state was observed with CHD pumping for the first time in LHD featuring excellent density control even under intense pellet fueling conditions. A global particle confinement time ($τ^*_p$) is used for comparison of operation with and without the CHD pumping. The $τ^*_p$ was evaluated from the density decay after the fueling of hydrogen pellet injection or gas puffing in NBI plasmas. A reliably low base density before the fueling and short $τ^*_p$ after the fueling were obtained during the CHD pumping, demonstrating for the first time full control of the particle balance with active pumping in the CHD.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Extending the low-recycling, flat temperature profile regime in the lithium tokamak experiment-β (LTX-β) with ohmic and neutral beam heating

Abstract Recent experiments in the lithium tokamak experiment- β (LTX- β ) have extended the duration, performance, operating conditions, and diagnosis of the flat-temperature profile, low-recycling regime first observed in LTX. As expected, Li retains hydrogen and suppresses edge neutral cooling, allowing increased edge electron temperature, roughly equal to the core T e . Flat temperature profiles had been obtained transiently in LTX, as the plasma density decayed following the cessation of edge gas puffing. Careful control over the fueling in LTX- β has now been shown to sustain the flat T e profile and hot edge unique to the low-recycling regime for multiple confinement times in high performance discharges with decaying or steady density. With low density, the flat T e profile is also seen to extend into the scrape-off layer. Neutral beam heating is observed in target discharges with relatively flat electron temperature profiles ( T edge ∼ T core /2), though beam heating is stronger in discharges with higher fueling, higher density, and depressed edge T e . Beam heating produces additional peaking of the T e profile, without degradation of the energy confinement time. Neutral beam heating of target discharges with relatively flat electron temperature profiles similarly results in broad beam heated temperature profiles. Energy confinement in LTX- β generally compares favorably to ohmic and H-mode scalings, frequently exceeding them by factors of 2–4. New and improved diagnostics in LTX- β enable better characterization of this unique regime, including measurements of ion temperature and high field side Thomson scattering profiles. As an initial step toward characterizing turbulence with no T e gradient and roughly equal density and pressure gradient, core fluctuation spectra have been measured in peaked T e discharges using far-forward scattering and fluctuation reflectometry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Rerouting of the lignin biosynthetic pathway by inhibition of cytosolic shikimate recycling in transgenic hybrid aspen

Lignin is a phenolic polymer deposited in the plant cell wall and is mainly polymerized from three canonical monomers (monolignols), i.e., p-coumaryl, coniferyl, and sinapyl alcohols. After polymerization, these alcohols form different lignin substructures. In dicotyledons, monolignols are biosynthesized from phenylalanine, an aromatic amino acid. Shikimate acts at two positions in the route to the lignin building blocks. It is part of the shikimate pathway which provides the precursor for the biosynthesis of phenylalanine, and is involved in the transesterification of pcoumaroyl- CoA to p-coumaroyl shikimate, one of key steps in the biosynthesis of coniferyl and sinapyl alcohols. The shikimate residue in p-coumaroyl shikimate is released in later steps, and the resulting shikimate becomes available again for the biosynthesis of new p-coumaroyl shikimate molecules. In this study, we inhibited cytosolic shikimate recycling in transgenic hybrid aspen by accelerated phosphorylation of shikimate in the cytosol through expression of a bacterial shikimate kinase. Here, this expression elicited an increase in p-hydroxyphenyl units of lignin and, by contrast, a decrease in guaiacyl and syringyl units. Transgenic plants with high shikimate kinase activity produced a lignin content comparable to that in wild-type plants and had an increased processability via enzymatic saccharification. Although expression of many genes was altered in the transgenic plants, elevated shikimate kinase activity did not exert a significant effect on the expression of the majority of genes responsible for lignin biosynthesis. The present results indicate that cytosolic shikimate recycling is crucial to the monomeric composition of lignin rather than for lignin content.

shikimate pathway↗

DOE OSTI2017

Rapid and near-complete dissolution of wood lignin at ≤80°C by a recyclable acid hydrotrope

We report the discovery of the hydrotropic properties of a recyclable aromatic acid, p-toluenesulfonic acid (p-TsOH), for potentially low-cost and efficient fractionation of wood through rapid and near-complete dissolution of lignin. Approximately 90% of poplar wood (NE222) lignin can be dissolved at 80°C in 20 min. Equivalent delignification using known hydrotropes, such as aromatic salts, can be achieved only at 150°C or higher for more than 10 hours or at 150°C for 2 hours with alkaline pulping. p-TsOH fractionated wood into two fractions: (i) a primarily celluloserich water-insoluble solid fraction that can be used for the production of high-value building blocks, such as dissolving pulp fibers, lignocellulosic nanomaterials, and/or sugars through subsequent enzymatic hydrolysis; and (ii) a spent acid liquor stream containing mainly dissolved lignin that can be easily precipitated as lignin nanoparticles by diluting the spent acid liquor to below the minimal hydrotrope concentration. Our nuclear magnetic resonance analyses of the dissolved lignin revealed that p-TsOH can depolymerize lignin via ether bond cleavage and can separate carbohydrate-free lignin from the wood. p-TsOH has a relatively low water solubility, which can facilitate efficient recovery using commercially proven crystallization technology by cooling the concentrated spent acid solution to ambient temperatures to achieve environmental sustainability through recycling of p-TsOH.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Recycling of multilayer plastic packaging materials by solvent-targeted recovery and precipitation

Many plastic packaging materials manufactured today are composites made of distinct polymer layers (i.e., multilayer films). Billions of pounds of these multilayer films are produced annually, but manufacturing inefficiencies result in large, corresponding postindustrial waste streams. Although relatively clean (as opposed to municipal wastes) and of near-constant composition, no commercially practiced technologies exist to fully deconstruct postindustrial multilayer film wastes into pure, recyclable polymers. Here, we demonstrate a unique strategy we call solvent-targeted recovery and precipitation (STRAP) to deconstruct multilayer films into their constituent resins using a series of solvent washes that are guided by thermodynamic calculations of polymer solubility. We show that the STRAP process is able to separate three representative polymers (polyethylene, ethylene vinyl alcohol, and polyethylene terephthalate) from a commercially available multilayer film with nearly 100% material efficiency, affording recyclable resins that are cost-competitive with the corresponding virgin materials.

36 MATERIALS SCIENCE↗