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At least 541 records · Page 30

Corrosion Engineering of Part‐Per‐Million Single Atom Pt 1 /Ni(OH) 2 Electrocatalyst for PET Upcycling at Ampere‐Level Current Density

The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to plastic down-cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here a corrosion synthesized single atom Pt 1 /Ni(OH) 2 electrocatalyst with part-per-million noble Pt loading for highly efficient and selective upcycling of polyethylene terephthalate (PET) into valuable chemicals (potassium diformate and terephthalic acid) and green hydrogen is reported. Electro-oxidation of PET hydrolysate, ethylene glycol (EG), to formate is processed with high Faraday efficiency (FE) and selectivity (>90%) at the current density close to 1000 mA cm −2 (1.444 V vs RHE). The in situ spectroscopy and density functional theory calculations provide insights into the mechanism and the understanding of the high efficiency. Remarkably, the electro-oxidation of EG at the ampere-level current density is also successfully illustrated by using a membrane-electrode assembly with high FEs to formate integrated with hydrogen production for 500 h of continuous operation. In conclusion, this process allows valuable chemical production at high space-time yield and is highly profitable (588–700 $\$$ ton −1 PET), showing an industrial perspective on single-atom catalysis of electrochemical plastic upcycling.

36 MATERIALS SCIENCE↗

Evidence for Chemical Processing of Precometary Icy Grains In Circumstellar Environments of Pre-Main-Sequence Stars

We report the detection of a broad absorption feature near 2166 cm-1 in the spectrum of the Taurus cloud source Elias 18. This pre-main-sequence source is the second in Taurus, the third in our survey, and the fifth known in the sky to show the broad 2166 cm-1 absorption feature. Of equal importance, this feature is not seen toward several other embedded sources in our survey, nor is it seen toward the source Elias 16, located behind the Taurus cloud. Laboratory experiments with interstellar ice analogs show that such a feature is associated with a complex C=-N containing compound [called X(C=-N)] that results from high-energy processing (ultraviolet irradiation or ion bombardment) of simple ice components into more complex, organic components, We find a nonlinear anticorrelation between the abundance of X(C=-N) and frozen CO in non- polar lattices. We find no correlation between the abundance of X(C=-N) and frozen CO in polar lattices. Because the abundances of frozen CO and H20 are strongly correlated with each other and with visual extinction toward sources embedded in and located behind the Taurus molecular cloud, these ice components usually are associated with intracloud material. Our results indicate that X(C=-N) molecules result from chemical processing of dust grains dominated by nonpolar icy mantles in the local environments of pre-main- sequence stars. Such processing of icy grains in the early solar system may be an important source of organic compounds observed in minor solar system bodies. The delivery of these organic compounds to the surface of the primitive Earth through comet impacts may have provided the raw materials for prebiotic chemistry.

Teglier, Stephen C.↗

Quantum-Dot Laser for Wavelengths of 1.8 to 2.3 micron

The figure depicts a proposed semiconductor laser, based on In(As)Sb quantum dots on a (001) InP substrate, that would operate in the wavelength range between 1.8 and 2.3 m. InSb and InAsSb are the smallest-bandgap conventional III-V semiconductor materials, and the present proposal is an attempt to exploit the small bandgaps by using InSb and InAsSb nanostructures as midinfrared emitters. The most closely related prior III-V semiconductor lasers are based, variously, on strained InGaAs quantum wells and InAs quantum dots on InP substrates. The emission wavelengths of these prior devices are limited to about 2.1 m because of critical quantum-well thickness limitations for these lattice mismatched material systems. The major obstacle to realizing the proposed laser is the difficulty of fabricating InSb quantum dots in sufficient density on an InP substrate. This difficulty arises partly because of the weakness of the bond between In and Sb and partly because of the high temperature needed to crack metalorganic precursor compounds during the vapor-phase epitaxy used to grow quantum dots: The mobility of the weakly bound In at the high growth temperature is so high that In adatoms migrate easily on the growth surface, resulting in the formation of large InSb islands at a density, usually less than 5 x 10(exp 9) cm(exp -2), that is too low for laser operation. The mobility of the In adatoms could be reduced by introducing As atoms to the growth surface because the In-As bond is about 30 percent stronger than is the In-Sb bond. The fabrication of the proposed laser would include a recently demonstrated process that involves the use of alternative supplies of precursors to separate group-III and group-V species to establish local non-equilibrium process conditions, so that In(As)Sb quantum dots assemble themselves on a (001) InP substrate at a density as high as 4 x 10(exp 10) cm(exp -2). Room-temperature photoluminescence spectra of quantum dots formed by this process indicate that they emit at wavelengths from 1.7 to 2.3 microns.

Qiu, Yueming↗

Research and development of an electrochemical biocide reactor

An alternate disinfecting process to chemical agents, heat, or radiation in an aqueous media has been studied. The process is called an electrochemical biocide and employs cyclic, low-level voltages at chemically inert electrodes to pass alternating current through water and, in the process, to destroy microorganisms. The paper describes experimental hardware, methodology, and results with a tracer microorganism (Escherichia coli). The results presented show the effects on microorganism kill of operating parameters, including current density (15 to 55 mA/sq cm (14 to 51 ASF)), waveform of applied electrical signal (square, triangular, sine), frequency of applied electrical signal (0.5 to 1.5 Hz), process water flow rate (100 to 600 cc/min (1.6 to 9.5 gph)), and reactor resident time (0 to 4 min). Comparisons are made between the disinfecting property of the electrochemical biocide and chlorine, bromine, and iodine.

See, G. G.↗

High‐Performance Zinc Tin Oxide TFTs with Active Layers Deposited by Atomic Layer Deposition

Abstract New deposition techniques for amorphous oxide semiconductors compatible with silicon back end of line manufacturing are needed for 3D monolithic integration of thin‐film electronics. Here, three atomic layer deposition (ALD) processes are compared for the fabrication of amorphous zinc tin oxide (ZTO) channels in bottom‐gate, top‐contact n‐channel transistors. As‐deposited ZTO films, made by ALD at 150–200 °C, exhibit semiconducting, enhancement‐mode behavior with electron mobility as high as 13 cm 2 V −1 s −1 , due to a low density of oxygen‐related defects. ZTO deposited at 200 °C using a hybrid thermal‐plasma ALD process with an optimal tin composition of 21%, post‐annealed at 400 °C, shows excellent performance with a record high mobility of 22.1 cm 2 V –1 s –1 and a subthreshold slope of 0.29 V dec –1 . Increasing the deposition temperature and performing post‐deposition anneals at 300–500 °C lead to an increased density of the X‐ray amorphous ZTO film, improving its electrical properties. By optimizing the ZTO active layer thickness and using a high‐ k gate insulator (ALD Al 2 O 3 ), the transistor switching voltage is lowered, enabling electrical compatibility with silicon integrated circuits. This work opens the possibility of monolithic integration of ALD ZTO‐based thin‐film electronics with silicon integrated circuits or onto large‐area flexible substrates.

Allemang, Christopher R.↗

Large-scale Evolution of Seconds-long Relativistic Jets from Black Hole–Neutron Star Mergers

We present the first numerical simulations that track the evolution of a black hole–neutron star (BH–NS) merger from premerger to r ≳ 10 11 cm. The disk that forms after a merger of mass ratio q = 2 ejects massive disk winds (3–5 × 10 –2 M ⊙ ). We introduce various postmerger magnetic configurations and find that initial poloidal fields lead to jet launching shortly after the merger. The jet maintains a constant power due to the constancy of the large-scale BH magnetic flux until the disk becomes magnetically arrested (MAD), where the jet power falls off as L j ~ t –2 . All jets inevitably exhibit either excessive luminosity due to rapid MAD activation when the accretion rate is high or excessive duration due to delayed MAD activation compared to typical short gamma-ray bursts (sGRBs). This provides a natural explanation for long sGRBs such as GRB 211211A but also raises a fundamental challenge to our understanding of jet formation in binary mergers. One possible implication is the necessity of higher binary mass ratios or moderate BH spins to launch typical sGRB jets. For postmerger disks with a toroidal magnetic field, dynamo processes delay jet launching such that the jets break out of the disk winds after several seconds. We show for the first time that sGRB jets with initial magnetization σ0 > 100 retain significant magnetization (σ $\gg$ 1) at r > 10 10 cm, emphasizing the importance of magnetic processes in the prompt emission. The jet–wind interaction leads to a power-law angular energy distribution by inflating an energetic cocoon whose emission is studied in a companion paper.

79 ASTRONOMY AND ASTROPHYSICS↗

Mechanical and chemical effects of ion-texturing biomedical polymers

To determine whether sputter etching may provide substantial polymer surface texturing with insignificant changes in chemical and mechanical properties, an 8 cm beam diameter, electron bombardment, argon ion source was used to sputter etch (ion-texture process) nine biomedical polymers. The materials included silicone rubber, 32% carbon impregnated polyolefin, polyoxymethylene, polytetrafluoroethylene, ultrahigh molecular weight (UHMW) polyethylene, UHMW polyethylene with carbon fibers (10%), and several polyurethanes (bioelectric, segmented, and cross linked). Ion textured microtensile specimens of each material except UHMW polyethylene and UHMW polyethylene with 10% carbon fibers were used to determine the effect of ion texturing on tensile properties. Scanning electron microscopy was used to determine surface morphology changes, and electron spectroscopy for chemical analysis was used to analyze the near surface chemical changes that result from ion texturing. Ion energies of 500 eV with beam current densities ranging from 0.08 to 0.19 mA/sq cm were used to ion texture the various materials. Standard microtensile specimens of seven polymers were exposed to a saline environment for 24 hours prior to and during the tensile testing. The surface chemical changes resulting from sputter etching are minimal in spite of the often significant changes in the surface morphology.

Weigand, A. J.↗

Manufacturing High-Quality Carbon Nanotubes at Lower Cost

A modified electric-arc welding process has been developed for manufacturing high-quality batches of carbon nanotubes at relatively low cost. Unlike in some other processes for making carbon nanotubes, metal catalysts are not used and, consequently, it is not necessary to perform extensive cleaning and purification. Also, unlike some other processes, this process is carried out at atmospheric pressure under a hood instead of in a closed, pressurized chamber; as a result, the present process can be implemented more easily. Although the present welding-based process includes an electric arc, it differs from a prior electric-arc nanotube-production process. The welding equipment used in this process includes an AC/DC welding power source with an integral helium-gas delivery system and circulating water for cooling an assembly that holds one of the welding electrodes (in this case, the anode). The cathode is a hollow carbon (optionally, graphite) rod having an outside diameter of 2 in. (approximately equal to 5.1 cm) and an inside diameter of 5/8 in. (approximately equal to 1.6 cm). The cathode is partly immersed in a water bath, such that it protrudes about 2 in. (about 5.1 cm) above the surface of the water. The bottom end of the cathode is held underwater by a clamp, to which is connected the grounding cable of the welding power source. The anode is a carbon rod 1/8 in. (approximately equal to 0.3 cm) in diameter. The assembly that holds the anode includes a thumbknob- driven mechanism for controlling the height of the anode. A small hood is placed over the anode to direct a flow of helium downward from the anode to the cathode during the welding process. A bell-shaped exhaust hood collects the helium and other gases from the process. During the process, as the anode is consumed, the height of the anode is adjusted to maintain an anode-to-cathode gap of 1 mm. The arc-welding process is continued until the upper end of the anode has been lowered to a specified height above the surface of the water bath. The process causes carbon nanotubes to form in the lowest 2.5 cm of the anode. It also causes a deposit reminiscent of a sandcastle to form on the cathode. The nanotube-containing material is harvested. The cathode and anode can then be cleaned (or the anode is replaced, if necessary) and the process repeated to produce more nanotubes. Tests have shown that the process results in approximately equal to 50-percent yield of carbon nanotubes (mostly of the single-wall type) of various sizes. Whereas the unit cost of purified single-wall carbon nanotubes produced by other process is about $1,000/g in the year 2000, it has been estimated that for the present process, the corresponding cost would be about $10/g.

Benavides, Jeanette M.↗

Electrochemical chlor-iron process for iron production from iron oxide and salt water

The iron and steel industry accounts for ~8% of global greenhouse gas emissions. Electrochemical reduction of iron ore to metal for electric arc furnaces can enable sustainable steel production, but existing electrochemical processes require expensive capital or electrolytes. Here we report a low-temperature, electrochemical cell that consumes low-cost and abundant iron oxide and aqueous sodium chloride, while co-producing sodium hydroxide and chlorine. Industrially relevant current densities and Faradaic efficiencies for iron production were demonstrated, with 94% selectivity to iron metal at an applied current density of 200 mA cm –2 . Freestanding films of phase-pure iron were formed after 4h of continuous, stable electrolysis. The process can lead to levelized costs of iron that are competitive with iron produced in fossil-fuel-powered blast furnaces, and the co-produced sodium hydroxide can be used for CO 2 capture from the air or ocean, creating a net-negative-emission process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Quinoidal Two‐Dimensional Metal–Organic Framework for High‐Performance Micro‐Supercapacitors and Solid‐State Lithium Batteries

Two-dimensional (2D) metal-organic frameworks (MOFs) integrating redox-active linkers enable dense charge sites and open ion pathways for microscale energy storage. We report a quinoidal dicarboxylate ligand, AQM-H2L, derived from p-azaquinodimethane, forming crystalline frameworks with Cu2+ and Zn2+ nodes. The Cu-based MOF (AQM-AQM-H2L-Cu) exhibits layered sheets (>14 Å spacing) constructed from dinuclear Cu-carboxylate units and conjugated AQM linkers, which narrow the bandgap and introduce Cu2+/Cu+ pseudocapacitance. Exfoliated nanosheets (∼5 nm) retain crystallinity and excellent processability. Integrated into graphene films, they deliver areal and volumetric capacitances of 29.6 mF cm-2 and 18.1 F cm-3, achieving 2.6 mWh cm-3 energy density at 160 mW cm-3. As ionic fillers (1 wt%) in PEO solid polymer electrolytes, the nanosheets markedly enhance LiFePO4 cell performance, affording 169.8 mAh g-1 at 0.2 C and 93% retention after 400 cycles. This work establishes quinoidal linkers as a compact and robust design motif for ionically active 2D frameworks toward high-performance miniature and solid-state energy devices.

Chen, Ziman↗

Development of AlGaN‐Based Deep‐Ultraviolet Avalanche Photodetectors—Toward Their Intrinsic Characteristics

Al 0.6 Ga 0.4 N deep‐UV p–i–n avalanche photodiodes (APDs) are demonstrated grown by metalorganic chemical vapor deposition (MOCVD) on a (0001) c‐plane aluminum nitride (AlN) bulk substrate and fabricated both with and without an ion implantation process for mesa‐edge electric‐field termination. Three design considerations are taken into account: the optical absorption of the AlN bulk substrate, the photosensitivity of the APD, and the breakdown electric field. The MOCVD growth conditions of the AlGaN APD layers are optimized. Then, a detailed description of the seven device fabrication steps of the APDs is provided, which includes nitrogen ion implantation. The APDs fabricated by the ion implant process exhibit a dark‐current density under low reverse bias ≈1 × 10 −9 A cm −2 . This is one order of magnitude lower than the APD fabricated without ion implantation from the same wafer. The breakdown voltage of the APD is ≈−140 V. The calculated optical gain of the ion‐implanted APD beyond avalanche breakdown is ≈5.2 × 10 5 (current limited) and the device has an average zero‐bias photoresponse of ≈68 mA W −1 at a wavelength of 250 nm.

Jeong, Hoon [Department of Electronic Engineering ↗

Reducing Zinc Redistribution and Extending Cycle Life Via Electrochemical Synthesis of Zinc/Zinc Oxide Anodes in Rechargeable Alkaline Batteries

Redistribution of zinc over the electrode surface, also known as shape change, is a major problem and a cause of failure in alkaline zinc anode batteries. To mitigate this phenomenon, we propose a scalable approach based on an in situ formed, highly porous electrochemically synthesized ZnO matrix with uniformly electrodeposited zinc particles. This results in ∼70% improvement in cycle life performance at a rate of 10 mA cm −2 compared to control Zn anodes, which have not gone through the formation process. A quantitative electrolyte analysis revealed under-saturated zincate ion concentration in the electrochemically synthesized ZnO/Zn cells indicating reduced zincate movement. Post mortem analysis of the anodes indicated higher retention of both Zn and ZnO on the electrochemically synthesized ZnO anodes signifying reduced redistribution of active material. Image analysis of the cycled anodes revealed a narrower Zn particle size distribution (62−79 μ m) in contrast to a wider particle size distribution of 51–96 μ m observed in the control anodes. The formation approach results in electrochemically synthesized ZnO/Zn anodes providing a stable ZnO matrix in which Zn particles retain their localized distribution on cycling better than control electrodes conventionally made by pasting zinc particles together with a binder.

Kolhekar, Snehal (ORCID:0000000210321153)↗

Soil Water Content (m3 m-3) located in the Dominican Republic , February 2013 - December 2016

Daily data that has been processed to monthly. Data represents near-surface soil moisture (depth of 0-10 cm) at a latitude of 17.90 N, and longitude -71.67 E. Data was downloaded from the PBO soil moisture data network and is publicly available. Data from this site is referenced as Dominican Republic (2) in Table 1 and Figure 4 of Solander et al., 2020, The pan-tropical soil moisture response to El Nino, Hydrol. Earth Syst. Sci., in press.

54 ENVIRONMENTAL SCIENCES↗

Soil Water Content (m3 m-3) from the Dominican Republic, February 2013 - August 2017.

Daily data that has been processed to monthly. Data represents near-surface soil moisture (depth of 0-10 cm) at a latitude of 19.76 N, and longitude -70.57 E. Data was downloaded from the PBO soil moisture data network and is publicly available. Data from this site is referenced as Dominican Republic (1) in Table 1 and Figure 4 of Solander et al., 2020, The pan-tropical soil moisture response to El Nino, Hydrol. Earth Syst. Sci., in press.

54 ENVIRONMENTAL SCIENCES↗

Soil Water Content (m3 m-3) from Australia, May 2014 - March 2017

Hourly data processed to monthly. Data collected from Cosmic Neutron Probes at variable depth averaging 28 cm that was interpolated to near-surface (0-10 cm). Site located at latitude -17.12 deg N, longitude 145.63 deg E. Data was downloaded from COSMOS data portal and is publicly available. Data from this site is referenced as Australia (1) in Table 1 and Figure 4 of Solander et al., 2020, The pan-tropical soil moisture response to El Nino, Hydrol. Earth Syst. Sci., in press.

54 ENVIRONMENTAL SCIENCES↗

Soil Water Content (m3 m-3) from Australia, June 2011 - December 2016

Hourly data processed to monthly. Data collected from Cosmic Neutron Probes at variable depth averaging 38 cm that was interpolated to near-surface (0-10 cm). Site located at latitude -14.16 deg N, longitude 131.39 deg E. Data was downloaded from the The COsmic-ray Soil Moisture Observing System (COSMOS) soil moisture data network and is publicly available. Data from this site located at, referenced as Australia (2) in Table 1 and Figure 4 of Solander et al., 2020, The pan-tropical soil moisture response to El Nino, Hydrol. Earth Syst. Sci., in press.

54 ENVIRONMENTAL SCIENCES↗

Soil Water Content (m3 m-3), October 2011 - May 2017

Hourly data processed to monthly. Data collected from Cosmic Neutron Probes at variable depth averaging 15 cm that was interpolated to near-surface (0-10 cm). Site located at latitude 0.28 deg N, longitude 36.87 deg E. Data was downloaded from the The COsmic-ray Soil Moisture Observing System (COSMOS) soil moisture data network and is publicly available. Data was made available by the COsmic-ray Soil Moisture Observing SysteM (COSMOS). Data from this site is referenced as Kenya in Table 1 and Figure 4 of Solander et al., 2020, The pan-tropical soil moisture response to El Nino, Hydrol. Earth Syst. Sci., in press.

54 ENVIRONMENTAL SCIENCES↗

Development of a process for producing ribbon shaped boron filaments

A ribbon-shaped boron filament with a tensile strength of 138 KN/sq cm (200 ksi) was investigated. The investigation was carried out using both carbon and tungsten as substrate materials. No satisfactory results were obtained utilizing uncoated, copper-plated or silicon carbide coated tungsten ribbon substrates. Carbon ribbon substrates were prepared by pyrolysis of stretched polyimide tape. A severe deposition gradient occurred in all dc reactor experiments due to convective cooling at the edge of the substrate that resulted in a weak, nonuniform filament. RF heating, however, completely eliminated this gradient problem and a 90 cm (35.5 in.) long boron ribbon was produced at .85 cm/sec (100 ft/hr) using a frequency of 40.68 megahertz. This boron ribbon, however, exhibited a light-bulb effect during deposition to 59 KN/sq cm (85.7 ksi) were obtained from this ribbon. Several silicon carbide ribbon shaped filaments were also produced during this investigation by decomposition of CH3SiHCl2 onto carbon substrates. Contrary to the boron work, silicon carbide ribbon was readily prepared in dc static reactors. A very uniform and smooth deposition was obtained with strengths up to 71.1 KN/sq cm (103.5 ksi).

Basche, M.↗