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result(s) for
"Kittrell, Carter"
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Urban mining by flash Joule heating
2021
Precious metal recovery from electronic waste, termed urban mining, is important for a circular economy. Present methods for urban mining, mainly smelting and leaching, suffer from lengthy purification processes and negative environmental impacts. Here, a solvent-free and sustainable process by flash Joule heating is disclosed to recover precious metals and remove hazardous heavy metals in electronic waste within one second. The sample temperature ramps to ~3400 K in milliseconds by the ultrafast electrical thermal process. Such a high temperature enables the evaporative separation of precious metals from the supporting matrices, with the recovery yields >80% for Rh, Pd, Ag, and >60% for Au. The heavy metals in electronic waste, some of which are highly toxic including Cr, As, Cd, Hg, and Pb, are also removed, leaving a final waste with minimal metal content, acceptable even for agriculture soil levels. Urban mining by flash Joule heating would be 80× to 500× less energy consumptive than using traditional smelting furnaces for metal-component recovery and more environmentally friendly.
Precious metals recovery from electronics wastes, termed urban mining, is significant for a circular economy. Here, the authors reported a solvent-free and ultrafast process based on flash Joule heating to recover precious metals and remove toxic heavy metals in electronic wastes.
Journal Article
Gram-scale bottom-up flash graphene synthesis
2020
Most bulk-scale graphene is produced by a top-down approach, exfoliating graphite, which often requires large amounts of solvent with high-energy mixing, shearing, sonication or electrochemical treatment
1
–
3
. Although chemical oxidation of graphite to graphene oxide promotes exfoliation, it requires harsh oxidants and leaves the graphene with a defective perforated structure after the subsequent reduction step
3
,
4
. Bottom-up synthesis of high-quality graphene is often restricted to ultrasmall amounts if performed by chemical vapour deposition or advanced synthetic organic methods, or it provides a defect-ridden structure if carried out in bulk solution
4
–
6
. Here we show that flash Joule heating of inexpensive carbon sources—such as coal, petroleum coke, biochar, carbon black, discarded food, rubber tyres and mixed plastic waste—can afford gram-scale quantities of graphene in less than one second. The product, named flash graphene (FG) after the process used to produce it, shows turbostratic arrangement (that is, little order) between the stacked graphene layers. FG synthesis uses no furnace and no solvents or reactive gases. Yields depend on the carbon content of the source; when using a high-carbon source, such as carbon black, anthracitic coal or calcined coke, yields can range from 80 to 90 per cent with carbon purity greater than 99 per cent. No purification steps are necessary. Raman spectroscopy analysis shows a low-intensity or absent D band for FG, indicating that FG has among the lowest defect concentrations reported so far for graphene, and confirms the turbostratic stacking of FG, which is clearly distinguished from turbostratic graphite. The disordered orientation of FG layers facilitates its rapid exfoliation upon mixing during composite formation. The electric energy cost for FG synthesis is only about 7.2 kilojoules per gram, which could render FG suitable for use in bulk composites of plastic, metals, plywood, concrete and other building materials.
Flash Joule heating of inexpensive carbon sources is used to produce gram-scale quantities of high-quality graphene in under a second, without the need for a furnace, solvents or reactive gases.
Journal Article
High-temperature electrothermal remediation of multi-pollutants in soil
2023
Soil contamination is an environmental issue due to increasing anthropogenic activities. Existing processes for soil remediation suffer from long treatment time and lack generality because of different sources, occurrences, and properties of pollutants. Here, we report a high-temperature electrothermal process for rapid, water-free remediation of multiple pollutants in soil. The temperature of contaminated soil with carbon additives ramps up to 1000 to 3000 °C as needed within seconds via pulsed direct current input, enabling the vaporization of heavy metals like Cd, Hg, Pb, Co, Ni, and Cu, and graphitization of persistent organic pollutants like polycyclic aromatic hydrocarbons. The rapid treatment retains soil mineral constituents while increases infiltration rate and exchangeable nutrient supply, leading to soil fertilization and improved germination rates. We propose strategies for upscaling and field applications. Techno-economic analysis indicates the process holds the potential for being more energy-efficient and cost-effective compared to soil washing or thermal desorption.
Soil contamination is a pressing environmental concern due to increasing anthropogenic activity. Here, the authors developed a rapid and energy-efficient electrothermal process that simultaneously removes heavy metals and organic pollutants in soil.
Journal Article
Nondestructive flash cathode recycling
2024
Effective recycling of end-of-life Li-ion batteries (LIBs) is essential due to continuous accumulation of battery waste and gradual depletion of battery metal resources. The present closed-loop solutions include destructive conversion to metal compounds, by destroying the entire three-dimensional morphology of the cathode through continuous thermal treatment or harsh wet extraction methods, and direct regeneration by lithium replenishment. Here, we report a solvent- and water-free flash Joule heating (FJH) method combined with magnetic separation to restore fresh cathodes from waste cathodes, followed by solid-state relithiation. The entire process is called flash recycling. This FJH method exhibits the merits of milliseconds of duration and high battery metal recovery yields of ~98%. After FJH, the cathodes reveal intact core structures with hierarchical features, implying the feasibility of their reconstituting into new cathodes. Relithiated cathodes are further used in LIBs, and show good electrochemical performance, comparable to new commercial counterparts. Life-cycle-analysis highlights that flash recycling has higher environmental and economic benefits over traditional destructive recycling processes.
Flash recycling method can achieve nondestructive cathode regeneration effectively with higher environmental and economic benefits over traditional destructive recycling processes.
Journal Article
A seamless three-dimensional carbon nanotube graphene hybrid material
by
Hauge, Robert H.
,
Ruan, Gedeng
,
Kittrell, Carter
in
639/301/357/73
,
639/301/357/918
,
639/638/549
2012
Graphene and single-walled carbon nanotubes are carbon materials that exhibit excellent electrical conductivities and large specific surface areas. Theoretical work suggested that a covalently bonded graphene/single-walled carbon nanotube hybrid material would extend those properties to three dimensions, and be useful in energy storage and nanoelectronic technologies. Here we disclose a method to bond graphene and single-walled carbon nanotubes seamlessly during the growth stage. The hybrid material exhibits a surface area >2,000 m
2
g
−1
with ohmic contact from the vertically aligned single-walled carbon nanotubes to the graphene. Using aberration-corrected scanning transmission electron microscopy, we observed the covalent transformation of
sp
2
carbon between the planar graphene and the single-walled carbon nanotubes at the atomic resolution level. These findings provide a new benchmark for understanding the three-dimensional graphene/single-walled carbon nanotube-conjoined materials.
Graphene and single-walled carbon nanotubes have high electrical conductivities and large specific surface areas. Here, these properties are extended into three dimensions by producing a seamless carbon nanotube graphene hybrid material.
Journal Article
High-surface-area corundum nanoparticles by resistive hotspot-induced phase transformation
2022
High-surface-area α-Al
2
O
3
nanoparticles are used in high-strength ceramics and stable catalyst supports. The production of α-Al
2
O
3
by phase transformation from γ-Al
2
O
3
is hampered by a high activation energy barrier, which usually requires extended high-temperature annealing (~1500 K, > 10 h) and suffers from aggregation. Here, we report the synthesis of dehydrated α-Al
2
O
3
nanoparticles (phase purity ~100%, particle size ~23 nm, surface area ~65 m
2
g
−1
) by a pulsed direct current Joule heating of γ-Al
2
O
3
. The phase transformation is completed at a reduced bulk temperature and duration (~573 K, < 1 s) via an intermediate δʹ-Al
2
O
3
phase. Numerical simulations reveal the resistive hotspot-induced local heating in the pulsed current process enables the rapid transformation. Theoretical calculations show the topotactic transition (from γ- to δʹ- to α-Al
2
O
3
) is driven by their surface energy differences. The α-Al
2
O
3
nanoparticles are sintered to nanograined ceramics with hardness superior to commercial alumina and approaching that of sapphire.
High-surface-area corundum are used in ceramics and catalyst supports, yet the synthesis is hampered by high energy barrier and aggregation. Here the authors report the ultrafast synthesis of corundum nanoparticles via the resistive hotspot triggered phase transformation in electric heating process.
Journal Article
Structure-Assigned Optical Spectra of Single-Walled Carbon Nanotubes
by
Hauge, Robert H.
,
Bachilo, Sergei M.
,
Strano, Michael S.
in
Carbon
,
Carbon nanotubes
,
Condensed matter: electronic structure, electrical, magnetic, and optical properties
2002
Spectrofluorimetric measurements on single-walled carbon nanotubes (SWNTs) isolated in aqueous surfactant suspensions have revealed distinct electronic absorption and emission transitions for more than 30 different semiconducting nanotube species. By combining these fluorimetric results with resonance Raman data, each optical transition has been mapped to a specific (n,m) nanotube structure. Optical spectroscopy can thereby be used to rapidly determine the detailed composition of bulk SWNT samples, providing distributions in both tube diameter and chiral angle. The measured transition frequencies differ substantially from simple theoretical predictions. These deviations may reflect combinations of trigonal warping and excitonic effects.
Journal Article
Electronic Structure Control of Single-Walled Carbon Nanotube Functionalization
by
Usrey, Monica L.
,
Hauge, Robert H.
,
Dyke, Christopher A.
in
Carbon
,
Carbon nanotubes
,
Chemical bonds
2003
Diazonium reagents functionalize single-walled carbon nanotubes suspended in aqueous solution with high selectivity and enable manipulation according to electronic structure. For example, metallic species are shown to react to the near exclusion of semiconducting nanotubes under controlled conditions. Selectivity is dictated by the availability of electrons near the Fermi level to stabilize a charge-transfer transition state preceding bond formation. The chemistry can be reversed by using a thermal treatment that restores the pristine electronic structure of the nanotube.
Journal Article
Increased CO2 selectivity of asphalt-derived porous carbon through introduction of water into pore space
by
Jalilov, Almaz S.
,
Tour, James M.
,
Li, Yilun
in
639/301/299/1013
,
639/4077/4057
,
639/4077/4082/4090
2017
The development of inexpensive porous solid sorbents, such as porous carbons, that can selectively capture carbon dioxide (CO
2
) from natural gas wells is essential to reduce emission of CO
2
to the atmosphere. However, at higher pressures, the selectivity for CO
2
over that for methane (CH
4
) remains poor. Here we show that H
2
O can be imbibed within asphalt-derived porous carbon, with a surface area of 4,200 m
2
g
−1
, to generate a hydrated powder material. While maintaining a high CO
2
uptake capacity of 48 mmol g
−1
(211 wt%), the molar selectivity for CO
2
over CH
4
increases to >200:1 and the H
2
O remains within the pores on repeated cycling. To mimic realistic natural gas wells, we used a 90% CH
4
and 10% CO
2
gas mixture and showed selective CO
2
separation at 20 bar. Furthermore, in situ vibrational spectroscopy reveals the formation of an ordered matrix within the pores consisting of gas hydrates.
CO
2
is often found alongside CH
4
in natural gas wells; therefore, separation of the gases is an important industrial process. Jalilov et al. demonstrate that the adsorption selectivity for CO
2
over CH
4
can be significantly enhanced through introduction of water into the pores of a high-surface-area carbon.
Journal Article
Band Gap Fluorescence from Individual Single-Walled Carbon Nanotubes
by
O'Connell, Michael J.
,
Hauge, Robert H.
,
Huffman, Chad B.
in
Absorption spectra
,
Algorithms
,
Carbon
2002
Fluorescence has been observed directly across the band gap of semiconducting carbon nanotubes. We obtained individual nanotubes, each encased in a cylindrical micelle, by ultrasonically agitating an aqueous dispersion of raw single-walled carbon nanotubes in sodium dodecyl sulfate and then centrifuging to remove tube bundles, ropes, and residual catalyst. Aggregation of nanotubes into bundles otherwise quenches the fluorescence through interactions with metallic tubes and substantially broadens the absorption spectra. At pH less than 5, the absorption and emission spectra of individual nanotubes show evidence of band gap-selective protonation of the side walls of the tube. This protonation is readily reversed by treatment with base or ultraviolet light.
Journal Article