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Kilogram Flash Joule Heating Synthesis with

an Arc Welder
Lucas Eddy, Jaeho Shin, Yi Cheng, Chi Hun Choi, Carolyn Teng, Phelecia Scotland, Shichen Xu,
Alexander Lathem, Shihui Chen, Carter Kittrell, Yimo Han, and James M. Tour*
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ABSTRACT: Flash Joule heating has been used as a versatile solid-state synthesis method in the
production of a wide range of products, including organic, inorganic, and ceramic products. Conventional
flash Joule heating systems are large and customized, presenting significant barriers in the cost of
assembly, the expertise needed to operate, and uniformity of results between different systems. Even
laboratory-scale flash Joule heating systems struggle to operate above 10 g capacity, and they suffer from
poor temperature controllability. We present here the use of commercial off-the-shelf arc welders as a
superior alternative to standard flash Joule heating systems due to their low cost ($120), ease of use, compact size, high
temperature controllability, and tunability. We demonstrate the gram-scale synthesis of a variety of organic and ceramic
species using these systems. With the addition of another reactor configuration for only $260, we scale up the synthesis of
these products to record rates for the laboratory scale, achieving a production rate of 3 kg/h for graphene and kilogram-per-
day production rates for SiC, carbon nanotubes, SnSe2, and SnS2.
KEYWORDS: graphene, flash Joule heating, arc welder, carbon nanotubes, p-block metal dichalcogenides, silicon carbide, carbyne,
kilogram scale

1. INTRODUCTION We report here FJH, up to kilogram scales, using commercial

Flash Joule heating (FJH) is a technique by which electric off-the-shelf systems available for as little as $120. We use these
current rapidly travels through a resistive medium, heating the systems as universal reactors to perform flash Joule and arc
sample on the millisecond to second time scale.1 FJH has been heating reactions to synthesize graphene, doped graphene,
used in a wide array of applications including solid-state carbon nanotubes, carbyne, SiC, SnS2, and SnSe2 (Tables S1
synthesis,2,3 especially of graphene,4 ceramics,5 inorganics,2,6 and S2). These commercial systems exhibit superior temper-
high-entropy nanoparticles,7 and their self-encapsulation,8 wet ature controllability relative to those of customized FJH
synthesis,9 waste material upcycling,10−14 and even soil systems and can be adjusted during a reaction (Table S3). We
remediation15 up to kilogram scales.16 Conventional FJH achieve this using multiple models of arc welders, a variable
uses a capacitor bank discharge to rapidly heat feedstocks up to transformer, and two programmable power supply models.
or exceeding 3000 K. FJH systems are typically custom-
designed, laboratory-made, and thus, each system is often Multiple arc welders connected in series can also permit larger-
entirely different.1,16−18 These differences in FJH systems scale reactions. We analyze the input energy use and output
present a barrier to simple reproducibility across laboratories voltage, current, and power signals with microsecond
because even small differences in system power, energy resolution. We also highlight procedures enabling modification
capacity, or time constant can significantly change the reaction of these systems, including making a portable battery-powered
heating profile.19 Furthermore, the assembly of even gram- FJH system that is recharged with portable commercial solar
scale FJH systems often requires tens of thousands of dollars, panels. These inexpensive and commercially available electrical
personnel experienced in the assembly of high-voltage sources are effective FJH systems, particularly in the synthesis
electrical equipment, and months of assembly prior to use.20 of graphene up to kilogram scales, all done in the open air.
Capacitor-based FJH systems feature comparatively low-
temperature controllability,1 are limited to reactions <10 s,4
are difficult to scale cost-effectively, and can suffer damage to Received: August 22, 2024
the system when the resistance of the feedstock is too low.2 Revised: November 12, 2024
Finally, intense optimization work must be performed anew for Accepted: November 21, 2024
every FJH system for every sample type and size to control the Published: December 7, 2024
reaction temperature within ∼100 °C,21,22 so optimization
performed on one system does not easily translate to others.

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This protocol renders Joule heating chemistry at the kilogram

scale readily accessible to most any laboratory.

2. RESULTS AND DISCUSSION

2.1. Synthesis of Flash Graphene with an Arc Welder.
FJH reactions are commonly performed inside a tube reactor,
where the target feedstock is placed inside a fused quartz tube
and between two graphite electrodes, which themselves are
connected to the FJH system. Metallurgical coke (MC) is a
commonly used feedstock in these reactors1,16 for flash
graphene (FG) synthesis due to its high carbon content, low
monetary cost, and resistivity of ∼0.01 Ω·m,23 which translates
to a resistance of ∼1 Ω when packed into a FJH tube,
commonly in 200 mg batches. During the FJH reaction of a
carbon feedstock, all the bonds within the carbon-based
reactants are broken, and the reactants reform into graphene
that is turbostratic in alignment, meaning that the layer
stacking is disordered and thus exhibits a higher interlayer
spacing relative to ordered graphene.1 This mechanism has
been studied and theoretically modeled in detail in our former
studies.11 The previous use of this MC feedstock inspired the
synthesis of metallurgical coke-derived flash graphene
(MCFG) with an arc welder, as illustrated in Figure 1. A Figure 1. Performance of the DEKOPRO arc welder. (a) Photo of
$120 DEKOPRO DKUS-MMA-160A arc welder (Amazon, DEKOPRO DKUS-MMA-160A arc welder. (b) Temperature
Figure 1a) was used to heat 200 mg batches of MC using plotted as a function of the welder current output setting of 200
different arc welder settings. Electrical, thermal, and optical mg of MCFG. The arc welder was plugged into a 120 V outlet.
hazard safety procedures were followed during all reactions MCFG was used for this measurement to avoid any heat
contribution from the thermochemical transition from MC to
(Figures S1 and S2). The temperature of the reaction was
MCFG. The current setting offers tunability at this scale of as little
measured using a Micro-Epsilon CTRM1H1SF100-C3 py- as a 7 °C/setting increment. The red dots illustrate the settings
rometer at 1 ms resolution, with a minimum temperature used in the experiment, and the blue dotted line illustrates the
threshold of 1000 °C. The system current setting, which linear fit of the sample temperature plotted as a function of these
increases the electrical current output but does not correspond settings. Each temperature increment was achieved after ∼10 s of
to the output in a 1:1 ratio, was adjusted in increments of 5 on heating relative to the previous increment. (c) Image of 200 mg of
the arc welder screen, resulting in an average temperature MC in an 8 mm inner diameter quartz tube with graphite
change of 35 °C per the five-increment adjustments (Figure electrodes being heated by the DEKOPRO welder plugged into a
1b). This corresponds to temperature tunability on this system 120 V outlet, which was used for all figures here, at the specified
of 7 °C/increment for this sample, which is very good control current output settings listed below each image. These current
settings were read from the screen of the arc welder and
at these high temperatures. A sample of greater heat capacity
correspond to the output current, but the setting displayed on
would have correspondingly higher temperature tunability. the arc welder is not the current output in amperes; hence, these
Temperature control of this precision can be maintained units are labeled as arbitrary units (a.u.).
during reactions, even minutes in duration (Figure S3),
although temperature-dependent sample resistance changes
may require slight setting adjustments to maintain a constant considered quantitative values, where a lower ID/G indicates
temperature. This arc welder source is only slightly larger than less defective graphene and a higher I2D/G indicates better
a shoebox and weighs only 5.5 kg, underscoring the simplicity graphene conversion.1 Conventionally, an I2D/G of at least 0.3
of arc welders as power sources. Figure 1c shows the changes indicates graphene conversion.22 Figure 2a illustrates the
in sample luminosity as a function of arc welder heating, and effects of different current settings on the FG product using the
additional images are shown in Figure S4. DEKOPRO arc welder. The graphene yield can be monitored
2.2. Characterization of the Arc Welder FG. Consistent by investigating the emergence of a 2D peak. No FG is
with conventional FJH reactors, the quality of the FG observed after reacting with a setting of 10, a low FG yield is
produced corresponds to the input energy and power. This observed with a setting of 50, and a higher FG yield is observed
quality is evaluated in terms of turbostraticity, interlayer with a setting of 90 out of a maximum setting of 160. The long
spacing, crystallinity, and defect density. Raman spectroscopy duration of the reactions in comparison to those with
is one of the primary tools for the bulk analysis of graphene. capacitor-based FJH systems enables FG synthesis to occur
The Raman spectrum of FG exhibits a D peak at ∼1360 cm−1, well under 3000 °C. The turbostratic character of graphene
which arises from defects in the graphene lattice or nonzigzag can be investigated by using a high-duration Raman scan to
edges; a G peak at ∼1600 cm−1, which comes from the examine two small turbostratic (TS) peaks at ∼1880 and
breathing modes of sp2 carbon bonds;22 and a 2D peak at ∼2040 cm−1, which are present in turbostratic graphene and
∼2700 cm−1, which has an intensity proportional to the absent in ordered graphene. These peaks are also present in
crystallinity of graphitic layers and inversely proportional to the FG produced with the arc welder (Figure 2b) at a setting of 90
coupling between layers.1,22,24 The intensities of the D and 2D even though the reaction duration is ∼20 s compared to
peaks are often normalized by the intensity of the G peak, conventional FJH reactions below 5 s. An ordered graphene
leading the peak intensity ratios, denoted ID/G and I2D/G, to be peak, denoted as the M peak, which normally occurs at ∼1740
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begin to form by FJH at as low as ∼800 °C, well beyond the

glass-transition temperature of most commodity polymers
(−100 to 100 °C), and can coexist with FG in reactions that
occur at ∼2000 °C. Temperatures higher than this form a
greater portion of FG with lower portions of the CNT
product.13 Conveniently, the outgassing typical of flash Joule
heating expels most surface contaminants and noncarbon
atoms,1 allowing even mixed and low-purity waste plastics to
be flash Joule heated. Accordingly, we flashed waste plastic
(high-density polyethylene, HDPE) with ferrocene mixed with
20 wt % carbon black as the conductive additive using the
same DEKOPRO commercial arc welder at a 200 mg sample
size of this mixture in a fused quartz tube. The arc welder was
turned to a setting of 70, and the mixture was heated for 10 s
to produce a mixture of CNTs and FG. Figure 3a illustrates the
Raman spectra of the product, which consists of successfully

Figure 2. Characterization of FG synthesized by using the

DEKOPRO arc welder. This FG was synthesized from a 200 mg
batch of MC at a setting of 90 after a ∼20 s flash. (a) Average
Raman map spectra (n = 200, 532 nm excitation) of 200 mg
batches of MC after FJH for ∼10 s at different current output
settings. The standard deviation of each of these graphs is
represented by the shaded area around the line, which is the mean.
(b) High-resolution Raman spectroscopy illustrates the two
turbostratic peaks with the missing M-band, all indicative of
turbostratic FG. The intensity ratio of the G peak to the TS1 peak
is ∼160. (c) TEM image of the FG product. The interlayer spacing
measured between the FG layers is 3.47 Å. Low-resolution TEM
characterization revealed the sheet size to be ∼3 μm2 (Figure S5).
(d) XRD pattern of the FG product.

cm−1, is also absent. A transmission electron microscopy

(TEM) image of this same FG product (Figure 2c) illustrates
graphitic ordering, though with an interlayer spacing of 3.47 Å,
which is characteristic of turbostratic graphene1 and is higher
than the AB-ordered graphene interlayer spacing of ∼3.35 Å.
The X-ray diffraction (XRD) pattern of the product (Figure
2d) illustrates the high crystallinity of the sample by the narrow
(002) peak, and the 3.42 Å interlayer spacing as determined by
the position of the (002) peak is well within the 3.4−3.5 Å
range seen in metallurgical coke (MC) derived FG.16
Combining the information from Figures 1b and 2, we can
conclude that MCFG can be formed from an MC feedstock
with a reaction surface temperature as low as ∼1500 °C (but
Figure 3. Additional FJH synthesis applications of the arc welder
certainly higher than ∼1200 °C) when the sample is heated for systems to form CNTs, heteroatom-substituted graphene, and SiC.
∼20 s. Thus, the use of a continuous and controllable Joule (a) Average Raman spectrum (n = 200, 532 nm excitation) of
heating system, such as an arc welder, can enable future studies CNTs and FG synthesized from ferrocene and plastic waste. (b)
of the flash graphene transition phase space. Additional SEM image of CNTs from this same product. (c) High-resolution
discussion is included in Figure S4. Raman spectra of the RBMs of the innermost tubes of the
2.3. Other Arc Welder Reactions. FJH is also an effective multiwalled CNTs synthesized using two different Raman
tool for the synthesis of carbon nanotubes (CNTs) from excitation wavelengths. CNT index assignment is performed in
amorphous carbon as well as from waste plastics, including Figure S11. (d) XPS spectrum of the products of the PFOS-MCFG
high- and low-density polyethylene, polypropylene, polystyr- FJH reaction. Fluorine substitution into the FG lattice is achieved
ene, and poly(ethylene terephthalate).13 This can be best at ∼9 at. %. (e) Raman spectrum of SiC product resulting from
FJH of a 6 g mixture of GFRP-MC in a 2:1 mass ratio followed by
achieved through a wet mixing method by which plastic waste combustion of the FG. The inset image is a photo of this FJH
is dipped into a water−ethanol solution into which 0.1 wt % reaction. (f) X-ray diffraction pattern of the SiC product of this
ferrocene has been dissolved. This waste plastic product is FJH reaction after a furnace heating step to combust the FG. The
electrically resistive, so it can be mixed with a conductive spectrum is illustrated above the corresponding powder diffraction
additive before it is placed in a quartz tube, such as carbon file of 2H-SiC. Additional characterization and discussion are in
black or MC, to reduce its resistivity and enable FJH. CNTs Figures S12 and S13.

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converted FG as well as CNTs, as evidenced by the radial S14 and S15). Several alternative systems for FJH were
breathing mode (RBM) Raman peaks at ∼220 and ∼285 cm−1. examined and tested, with prices ranging from $125 to $6,500
The presence of these RBMs confirms the synthesis of CNTs (Table S4 and Figure S16). These systems each exhibit
in the product.10,21 Because these are multiwalled carbon different voltage, current, and thus power ranges, which also
nanotubes, detailed diagnostic information on indices, depend on Ohm’s law on the sample resistance (Figure S17).
diameter, and configuration cannot be easily estab- To explore the effects of these systems on FG conversion, we
lished.22,23,26,27 Scanning electron microscopy characterization synthesized FG, and we recycled electronic waste11 using both
of this same product (SEM, Figure 3b) shows the CNTs, an alternating current (AC) Powerstat variable transformer and
which exhibit a diameter of ∼100 nm, typical of multiwalled a direct current (DC) Zhaoxin programmable power supply
CNTs formed from this method.13 This reaction was (Figure S18). In doing so, we successfully demonstrated FJH
performed at a comparatively low arc welder setting and thus reactions using both AC and DC power sources. Additional
exhibited some regions of amorphous carbon in addition to similar electrical and thermal characterization of the outputs of
FG, demonstrating that CNTs can be made with or without these two systems are included in Figures S19−S24.
FG (Figure S6). The ratio of FG-to-CNTs produced is Although the monetary cost per kilowatt output of
proportional to the reaction temperature and is thus programmable power supplies is in general higher than that
controllable by the arc welder setting.13 Raman spectroscopy of arc welders, they offer higher controllability, typically in
analyses of the RBMs of the CNTs using two different Raman increments of 0.1 A and 0.1 V. In contrast, arc welders do not
excitation wavelengths were performed (Figure 3c). Additional typically feature voltage controllability and exhibit current
SEM and energy-dispersive X-ray analyses are shown in Figure controllability of ∼1 A. The high controllability of the
S7. A simplified mixing technique can also be used with the arc programmable power supply facilitates thermodynamic analysis
welder, whereby the ferrocene is mixed directly into the plastic- of FJH reactions. Though not demonstrated here, program-
carbon black mixture without any wetting or drying steps. This mable power supplies could also be used in feedback mode
method also produced CNTs, though with a yield lower than with a temperature monitor to provide additional sample
that with the wet mixing method (Figures S8 and S9). temperature stability. Figure S19 illustrates the FJH conversion
Additionally, nitrogen-rich polymers, such as polyaniline, can of MC into MCFG at a constant power, except for a brief spike
be used as a feedstock to synthesize nitrogen-doped CNTs.28 at the beginning. The results from this experiment illustrate
The versatility of FJH reactions also enables the synthesis of that even with constant power output, the conversion of MC
heteroatom-doped FG.29 To achieve this, heteroatom-contain- to MCFG experiences two temperature maxima: one from the
ing compounds are mixed with the amorphous carbon reactant. Joule heating and one from the 34 kJ mol−1 exotherm of the
The resulting mixture is then FJH to produce heteroatom- reaction.19
doped FG. A variant of this technique involves flashing the We previously reported that the use of an oscillating current,
heteroatom compound in the presence of FG to achieve a still such as a pulse-width modulated DC current, during FJH
higher doping concentration, termed heteroatom-substituted affords superior FG conversion compared to FG formed from a
reflash graphene. Motivated by these and by the previous work nonoscillating current.16,19 Performing a fast Fourier transform
on destroying harmful per- and polyfluoroalkyl substances on the output current signals of the arc welders (Figures S25−
(PFAS),30,31 we synthesized heteroatom-substituted reflash S29) reveals that the arc welders output with a duty cycle of
graphene using the DEKOPRO arc welder to perform an FJH multiple different frequencies, including one at ∼9.6 kHz. This
reaction on a 200 mg mixture of perfluorooctanesulfonic acid provides the arc welders with an innate advantage in the FJH
(PFOS) and MCFG mixed in a 1:4 weight ratio. The resulting synthesis of FG and other 2D materials compared to
product achieved ∼9% fluorine substitution, as demonstrated conventional flash Joule heaters. Additionally, arc welders
by X-ray photoelectron spectroscopy analysis (XPS, Figure can be arranged in series or parallel to increase power output
3d). Tube FJH reactions with this DEKOPRO arc welder can (Figures S30 and S31). The power source of the arc welder can
be performed in even gram-scale batch sizes, still affording also be tuned. Rather than connecting to a stationary power
successful graphene conversion (Figure S10). This near- outlet, a simple system can be constructed, whereby an arc
constant heating rate also illustrates the thermodynamics of welder can be powered by a portable power system. We thus
the graphene reaction because the first temperature maximum assembled this system, using a car battery, which was charged
at ∼5 s arising from the graphene and MC volatiles exotherm is from solar panels, to enable a portable flash Joule heater that
visible (Figure S10c).19 FJH has also been effectively used in operates entirely on solar power (Figures S32 and S33) and
the upcycling of glass fiber-reinforced plastics (GFRPs) to can be assembled for only $422 (Table S5).
efficiently produce SiC.14 Using a higher-power arc welder, 2.5. Arc Heating. Arc welders are specifically designed to
such as an Amico Electric ARC-200DC, enables upcycling of facilitate arc heating by automatically raising the DC voltage in
GFRP into SiC within the quartz tube even up to a 6 g scale its open circuit state until an arc is formed, at which point the
reaction (Figures 3e,f). GFRP decomposes at ∼1000 °C, but voltage decreases. This same technique has been recently
the best SiC quality is achieved at ∼2000 °C, which can be repeated with a TDK Lambda GENESYS power supply to
reached at this scale by a DEKOPRO arc welder plugged into a perform ultrahigh temperature plasma synthesis by creating an
208 V outlet at maximum setting (160 au). arc across layers of carbon felt.32 This technique is also
2.4. Other Commercial Systems. The DEKOPRO arc possible using arc welders, which are typically 1/30 of the cost
welder offers vastly superior price, temperature controllability, of programmable power supplies of comparable power output,
and ease of use compared with conventional FJH electrical even across carbon paper (Figure S34).
systems. However, other heating systems can offer higher Arc melters have been a widely used tool in inorganic
power output and still higher temperature controllability than synthesis for decades as ultrafast reactors and are thus
even the DEKOPRO system, all while remaining more commonly present in solid-state synthesis laboratories. They
economical and facile than conventional FJH systems (Figures are composed of an arc welder, which provides the heating,
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Figure 4. Kilogram-scale FJH reaction using a $180 Amico Electric arc welder on MC. (a) Schematic image of the clay pot filled with MC. A
cross section has been cut out to show the contents. (b) Photo of the arc welder in use on ∼750 g MC in a clay pot, turning on a rotating
platform at ∼3 rpm, as shown in the Video S1, and reacting for 10 min at 3 kg/h FG production. (c) Power and cumulative energy usage of a
∼70 s MC reaction plotted with respect to time. (d) Average Raman spectra (n = 200, 532 nm excitation) of the FG product synthesized
using both the Amico Electric arc welder and a TDK Lambda GEN 125-80 power supply. The standard deviation of each of these graphs is
represented by the shaded area around the line, which is the mean. (e) Photo of the arc welder in use on a mixture of ∼900 g GFRP and MC
producing SiC at a rate of 430 g/h. (f) XRD pattern of SiC produced from the scaled synthesis method after FG removal by furnace
treatment. The powder diffraction files of both 2H-SiC and 3C-SiC are illustrated below, demonstrating that both phases of SiC were
produced. Additional X-ray photoelectron spectroscopy (XPS), XRD, and thermogravimetric analysis (TGA) characterization is exhibited in
Figures S51 and S52. (g) SEM image of CNTs on MC produced during a 550 g scaled reactor flash at $284/tonne (Table S7) for the starting
material and electrical costs of the flashing step. (h) FG production rate plotted as a function of system price compared using a single Amico
Electric arc welder (1 AW), two Amico Electric welders in series (2 SAW), and the TDK Lambda power supply (PS) with this scaled reactor
compared to commercially available FJH systems from ACS Materials LLC, and a scaled FJH system previously reported by our group.13
The error bars from the commercial FJH systems illustrate the range of production rates quoted by ACS Materials LLC for these FJH
models. The costs of the clay pot, the turning platform, the electrodes, and all arc welder parts are included in these values. The blue dotted
line illustrates the cost and production rate of duplicating each system. For example, having two AWs and two flowerpot reactor systems
running concurrently would cost $520 and produce 6 kg/h MCFG at $200/tonne (Table S8) for starting material and electrical costs of the
flashing step, which is superior cost efficiency relative to using a single reactor system with two SAWs at $530 and 5 kg/h. Also note that, in
the industry, they are unlikely to use arc welders. Much larger systems are likely to be required, while the work here can easily provide
kilograms of material to laboratories.16,20

connected to an evacuated chamber wherein a user-controlled This technique had previously only been achieved using higher
needle electrode operates as one electrode, and a copper or value, 99.99% graphite rods and had not previously been
brass mortar onto which the reactants are placed operates as reported on a separate feedstock.33,34
the other electrode. Motivated by this, we also tested a Lincoln 2.6. Kilogram-Scale FG Production. Previous attempts at
Electric Precision TIG 275 arc welder connected to an arc scaling up FJH reactions have been made by rapidly
melter chamber using a copper mortar and a 2% lanthanated automating small, gram-scale batches of feedstock to achieve
tungsten electrode to use arc heating to convert MC into cumulative large-scale synthesis over time, even up to
MCFG. The metal presence in the electrodes provided kilogram-scale in hours. These FJH systems tend to involve
sufficient catalyst to form carbyne chains, rapidly identified elaborate automation assemblies.16 Arc welders provide a facile
by a prominent C band, measured by Raman spectroscopy in alternative to scaled and customized FJH systems, can be
different samples from ∼1770 to ∼1840 cm−1 using multiple operated rapidly, require minimal training, and are less than 1%
excitation wavelengths (532, 633, and 785 nm). Though not of the cost of dedicated FJH systems. A kilogram-scale FG
studied here by TEM, these distinct Raman diagnostic signals reaction using an Amico Electric ARC-200DC arc welder is
are definitive fingerprints of their presence. These carbyne shown in Figure 4. The reactor consists of this arc welder
chains are likely bound inside and stabilized by multiwalled connected to two graphite rods placed inside a 13 L, $9.97 clay
CNTs on the surface of the MCFG (Figures S35−S38).33,34 flowerpot (Home Depot) that is filled with 500 g of MC and
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Figure 5. Simultaneous flash-within-flash reactions were performed using the Amico Electric arc welder. (a) Image of the nine tubes filled
with the inorganic reactant feedstock embedded in MC inside the clay flowerpot. Yellow arrows point to the tubes that are visible in the
photo. (b) Zoomed-in image of the tubes inside the flowerpot. The inset photo shows a single tube loaded with 0.4 g of SnCl2·2H2O and 1.0
g of S powder. (c) Raman spectra of SnS2 and SnSe2. (d) XPS spectrum illustrating Sn in the SnSe2 product. (e) XPS spectrum illustrating Sn
in the SnS2 product. (f) XPS spectrum illustrating Se in the SnSe2 product. (g) XPS spectrum illustrating S in the SnS2 product. (h) XRD
pattern of SnSe2. (i) XRD pattern of SnS2. Additional TEM characterization is shown in Figure S54 illustrating a SnS2 crystal sheet size of
∼30 μm2 and a SnSe2 crystal sheet size of ∼0.6 μm2.

open to the air (Figures 4a, Figure S39). Unlike large Pyrex in the flowerpot reactor because it was added as a solid) was
beakers that cracked under these thermal stresses, the also mixed with 500 g MC to grow CNTs on the MC (Figure
flowerpots remained uncracked. The arc welder cathode S44). FJH reactions become more efficient at large scales
(negative) clamp is attached to the end of a 0.2 m long, 16 because most of the heat is transferred into the reaction instead
mm diameter graphite rod ($15.99, Amazon), and the anode of out to the environment (Figure S42).19 This production
(positive) clamp is attached to the end of a 0.2 m long, 8 mm method features a higher production rate than other scaled and
diameter graphite rod ($4.80, Amazon). The pot is placed atop automated FJH production methods reported in the literature
a $52.99 JAYEGT Motorized Rotating Display Stand rotating by a factor of up to 22020 and is also more energy efficient,
platform system (22 cm, 250 lb load rating, wired, Amazon). producing graphene with ∼60% less energy per product mass
When the arc welder is turned on, an electric current is (Figure 4e).16,20,35 This improvement in efficiency results in a
permitted to flow across the two graphite electrodes, and proportional reduction in greenhouse gas emissions relative to
rotation of the platform at ∼3 rpm automatically stirs the these other methods (Table S6). Simultaneously, this reaction
reactor and ensures uniform heating (Figure 4b). The FJH system can be constructed at ∼1/160th the cost of even
electrodes are also moved during the reaction to heat a milligram-scale commercially sold FJH systems.36 The
different radius of sample (Figures S40 and S41). The long production rate can be further increased by using multiple
duration of this reaction permits the exertion of enough energy arc welders simultaneously in series to increase maximum
to convert the entire 500 g of MC to MCFG (Figure 4c,d). output voltage or in parallel to increase maximum output
The temperature of the reaction reaches over 3000 °C (Micro- current, which is up to 30 times more cost-effective than
Epsilon CTRM1H1SF100-C3 pyrometer), while the average purchasing larger power supplies (Figure S45). Flashing with
sample resistance decreases during conversion (Figure S42). arc welders in series or using a power supply that outputs a
Batches can be easily loaded and unloaded into the reaction higher voltage is also an effective way to heat a larger volume at
vessel, and thus, two consecutive reactions were performed to a time (Figure S46). Product uniformity could also be
achieve 1 kg of MCFG in total product after 20 min of heating. improved using additional stirring (Figure S47) and electrode
This technique was also used to FJH a 900 g batch of waste configurations (Figure S48). Adding a simple automated
GFRP and MC, mixed in a 1:2 weight ratio, to produce SiC loading and unloading process could enable continuous
(Figure 4e,f and Figure S43); a mixture of 50 g HDPE loaded production of FG from carbon or waste materials (Figure
with 1 wt % ferrocene (we used this higher ferrocene loading S49) while simultaneously ensuring that the highest quality
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product exposed to the highest reaction temperatures at the modulation in the arc systems reduces the energy requirement
center of the reactor is separated from the lower quality to synthesize high-quality FG relative to systems using an
product exposed to lower reaction temperatures at the edges of unmodulated direct current. Pairing these systems with other
the reactor. Further, a pipe-like configuration for continuous reaction geometries and systems also enables facile larger-scale
feed rather than batch feed would be an obvious industrial synthesis by FJH to kilogram scale (Figure S55) even in the
extension. Pairing this technique with an improved character- open air because outgassing prevents oxidative degradation.
ization protocol to verify product uniformity will enable
scaling-up of this technique to a continuous-feed pipe-based 4. EXPERIMENTAL SECTION
system with topological features to ensure mixing as the Materials. Metallurgical coke was obtained from SunCoke in
feedstock passes through the reactor. Finally, flashing MC in chunks ∼10 cm in diameter. These chunks were then ground and
this scaled reactor at a higher energy per mass will convert the sieved. Additional characterization of this raw material has been
initial turbostratic (disordered) MCFG into ordered FG and previously reported.13
graphite19 (Figure S50). GFRP for the scaled reactor was obtained in the form of Garolite
2.7. Inorganic Synthesis Reactor. FJH has also been G-10 sheets purchased from Amazon. These sheets were then cut and
used in the synthesis of 22 inorganic compounds, primarily ground by a hammer mill into a fine powder of 300 g in mass. This
powder was then mixed with small grain (0.05−0.15 mm) MC in a
transition metal dichalcogenides (TMDs) and p-block metal
2:1 ratio to make 900 g of the GFRP-MC mixture.
dichalcogenides (PMDs), through a method called flash- For the scaled flash-within-flash synthesis of p-block metal
within-flash synthesis.2 By this technique, inorganic reactants dichalcogenides, SnCl2·2H2O powder (CAS# 10025-69-1) was
are filled inside an inner quartz tube, which is then surrounded obtained from Alpha Aesar. Sulfur powder (CAS# 7704-34-9) was
by a feedstock, such as MC, before being inserted into another obtained from Millipore Sigma. Se powder (CAS# 7782-49-2) was
quartz outer tube and closed at the end with electrodes, usually obtained from Millipore Sigma.
made of graphite. The outer tube undergoes a conventional For the synthesis of CNTs in the small tube reactions, FeCl3
FJH reaction in which electrical current passes through the (CAS# 7705-08-0) was obtained from Millipore Sigma. Carbon black
MC, heating it. This hot MC then passes heat to the inner tube BP2000 was obtained from Cabot. High-density polyethylene was
obtained from Millipore Sigma. For the scaled reactor, ferrocene
and its inorganic feedstock contents through thermal
(Fe(C5H5)2, CAS# 102-54-5) was obtained from Millipore Sigma.
conduction. Current does not need to flow through the Scaled FG Reaction. A total of 750 g of large MC grains (1.7−3
inorganic feedstock contents of the inner tube in this process, mm) were poured into a terra cotta flowerpot. The pot was obtained
and thus, this inorganic feedstock is not restricted to any from The Home Depot (Store SKU 208337) for $9.97 and had a
electrical resistivity boundaries typical of conventional FJH. height of 21.0 cm, a top diameter of 25 cm, a bottom diameter of 14.6
During the flash-within-flash reaction, the reactant feedstocks cm, a total volume of 13 L, and a mass of 2.2 kg. The arc welder
are decomposed during heating, and the TMD or PMD cathode (negative) clamp was attached to the end of a 0.2 m long, 16
products are formed in kinetically controlled reaction mm diameter graphite rod ($15.99, Amazon), and the anode
conditions at ∼1500−2000 °C.2 Inspired by this technique, (positive) clamp was attached to the end of a 0.2 m long, 8 mm
diameter graphite rod ($4.80, Amazon). Each arc welder clamp was
we performed a flash-within-flash reaction using the scaled
held above the pot by a chemical clamp mounted on a laboratory
reactor technique (Figure 5) and prepared nine quartz tubes: clamp stand. These rods were then embedded ∼3 cm deep into the
five loaded with 0.4 g of SnCl2·2H2O plus 1.0 g of Se powder MC, with the large graphite rod (anode, positive) inserted laterally in
and four loaded with 0.4 g of SnCl2·2H2O and 1.0 g of S the center of the pot and the small graphite rode (cathode, negative)
powder for a total of 12.6 g of feedstock. These tubes were inserted laterally ∼6 cm away from the large rod (Figure S39). These
embedded in the MC until completely covered in a nonagonal arc welder electrodes were plugged in to an Amico Electric ARC-200
pattern around the center electrode (Figure 5a,b). The mixture DC arc welder purchased from Amico Electric for $179.00, which
was then subjected to FJH using a technique analogous to that itself was plugged in to a 208 V, single phase, AC outlet. The clay pot
shown in Figure 4 in which the arc welder electrodes moved in was often mounted onto a wooden block (rectangular prism shape, 3
cm height, 8 cm side length) to add a layer of thermal and electrical
a circular motion around the quartz tubes, flash Joule heating
insulation below the pot and to cover the hole at the bottom of the
the MC and hence transferring this heat through thermal flowerpot. The pot and wood block were then mounted onto a
conduction to the tubes. The result of this 1 min synthesis was JAYEGT Motorized Rotating Display Stand (22 cm, 250 lb load
five tubes each containing ∼0.2 g SnS2 and four tubes each rating, wired) purchased from Amazon for $52.99. The rotating
containing ∼0.15 g SnSe2 products (Figure 5c−i, Figure S53), platform was then turned on and began to spin at ∼3 rpm. Since the
amounting to a PMD production rate of 100 g h−1. The pot was placed on top of the turning stand, but the electrodes were
versatility of this scaled FJH reactor distinguishes it as a viable held independently, the pot and the MC mixture within rotated
inorganic reactor by which several different products can be relative to the electrodes to permit more uniform heating (Figure
simultaneously synthesized. Furthermore, the value of the FG S39). The heating procedure is illustrated in Figure S41. To begin the
FJH reaction, the arc welder dials (arc force and output current dials)
byproduct produced around these tubes offsets the cost of
were then turned to maximum output such that the screen of the arc
these reactions such that the inorganic products are welder displayed an output value of 200. The reaction proceeded
synthesized at a negative net cost. under this orientation for 5 min, during which the lateral center of the
sample, near the surface, was heated and converted to MCFG (Figure
3. CONCLUSIONS S40a). The center electrode (anode) was then moved laterally to the
Commercial power supplies, especially arc welders, provide a outer radius of the pot such that it was still ∼6 cm from the cathode
less expensive, more accessible, standardized, more scalable, but now ∼8 cm from the center of the pot (Figure S40b). This
movement of the electrode was achieved by laterally moving the
and more temperature controllable alternative to conventional laboratory clamp stand holding the electrode. Heating continued in
FJH systems (Table S3). This facilitates FJH synthesis, this orientation for 2.5 min, during which the outer lateral radius of
especially in reactions requiring greater temperature controll- the MC near the surface was heated (Figure S41, step 3). After this, a
ability and those that require sustained heating over longer third electrode orientation was implemented by first moving the outer
durations of seconds or minutes. Innate pulse width electrode to the lateral center of the pot and again moving the

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laboratory clamp stand. Then, both electrodes were pushed deeper outlet. The use of two arc welders in series rather than only one arc
into the pot to a depth of ∼6 cm into the MC (Figure S41, step 4). welder increases the production rate and the voltage of the arc welder
The reaction was then continued for another 2.5 min. Of the 750 g of series system, allowing this higher resistance GFRP-MC sample to be
MC in the pot, the top-center 500 g of MC was removed, and the heated more easily, as described in Figure S46. The clay pot was
bottom 250 g of MC was left behind (Figure S41, step 5). Only this mounted onto a wooden block (rectangular prism shape, 3 cm height,
top 500 g was characterized (Figure 5d) and counted toward the 8 cm side length) to add a layer of thermal and electrical insulation
MCFG production rate. 250 g of MC was left behind since this MC below the pot. The pot and wood block were then mounted onto a
has low (∼10%) conversion to MCFG, and this remaining MC adds a JAYEGT Motorized Rotating Display Stand. The rotating platform
layer of thermal protection to the flowerpot, allowing the flowerpot to was then turned on and began spinning at ∼3 rpm. The heating
survive multiple FJH cycles. After the 500 g of MCFG are removed, procedure is illustrated in Figure S41. To begin the FJH reaction, the
an additional 500 g of MC are added to the flowerpot, bringing the arc force dials on both systems were turned to their maximum setting,
total again to 750 g in preparation for another reaction. This FJH and the current dial output on both systems were adjusted so that a
procedure was then repeated once more to recover an additional 500 value of 40 was displayed on the screens of each arc welder. The
g of MCFG product to accumulate a total of 1 kg MCFG. This single reaction proceeded with these settings for 1 min to pretreat the
arc welder method thus uses three separate heating steps: the first GFRP-MC feedstock, making it more conductive (Figure S41, step
heating step with a 5 min duration, the second heating step with a 2.5 1). For the second step, the current output dials of both arc welders
min duration, and the third heating step with a 2.5 min duration, for a were then each increased so that a value of 80 was displayed on the
total heating duration of 10 min for 500 g of MCFG production. screens of each arc welder. Simultaneously, the rotating platform was
Thus, a 500 g/10 min (3 kg/h) production rate is counted. turned on and began spinning at ∼3 rpm. The reaction proceeded
This MCFG production procedure was also analogously performed under this configuration for 5 min, during which the lateral center of
with two Amico Electric ARC200-DC arc welders in series (Figures the sample, near the surface, was heated and converted to SiC (Figure
S30a and S31a), assisted using two power diodes, instead of only one S40a). The reaction was paused for ∼30 s by turning off the arc
arc welder to increase the production rate. When two arc welders in welders and the turning platform, and the electrodes were manually
series are used, then the process proceeds identically, except that the operated to push some of the GFRP-MC powder mixture back to the
interelectrode distance is ∼8 cm, instead of the 6 cm used for a single radial center of the reactor. The center electrode (anode) was then
arc welder, and the first heating step had a 3 min duration, the second moved laterally to the outer radius of the pot such that it was still ∼6
a 1.5 min duration, and the third a 1.5 min duration, for a total cm from the cathode, but now ∼8 cm from the center of the pot
heating duration of 6 min for 500 g of MCFG production. Thus, a (Figure S40b). This movement of the electrode was achieved by
500 g/6 min (5 kg/h) production rate is counted. The two arc laterally moving the laboratory clamp stand holding the electrode.
welders were also only turned onto a screen-displayed current setting Heating continued in this orientation for 5 min at the previous arc
of 150 for FJH when connected in series instead of the maximum welder current output settings (80 au) and turning platform rotation
(200) setting when a single arc welder was used. rate (∼3 rpm), during which the outer lateral radius of GFRP-MC
This procedure was also analogously performed by using the 10 kW near the surface was heated (Figure S41, step 3). The reaction was
TDK Lambda GENESYS GEN 125−80−3P208 programmable power paused again for ∼30 s by turning off the arc welders and the rotating
supply. The MCFG production procedure for FJH with the power platform, and the graphite electrodes were again manually used to stir
supply is identical to that for a single arc welder, except that the the unreacted portion of the GFRP-MC powder mixture to the radial
interelectrode interelectrode distance is ∼8 cm, instead of the 6 cm center of the reactor. The initial electrode configuration was restored
used for a single arc welder, and the first heating step had a 3 min (Figure S41, step 2), the arc welders were turned back on to their
duration, the second a 1.7 min duration, and the third a 2 min previous current output setting (80 au), and the turning platform was
duration. This total heating duration (6.7 min) is considered for 500 g turned on again. Heating resumed for another 3 min. Finally, the arc
of MCFG production for a production rate of 500 g/6.7 min (4.5 kg/ welders and the rotating platform were turned off. Thus, this single
h). The power supply was turned to its maximum setting (125 V and arc welder method thus uses four separate heating steps and two
80 A) during this FJH reaction. pauses during which manual mixing is performed: the first preheating
Scaled SiC Reaction. A schematic illustration of the SiC reactor is step with a 1 min duration, the second heating step with a 5 min
shown in Figure S43. Prior to flashing in the scaled reactor, the 300 g duration, the first pause with a ∼ 40 s duration, the third heating step
of GFRP powder was hand-mixed with 600 g of MC powder (0.05− with a 5 min duration, the second pause with a ∼ 40 s duration, and
0.15 mm) to make a 1:2 GFRP-MC mixture (further described in the fourth heating step with a 3 min duration, for a total process
materials section). 500 g of large MC grains (1.7−3 mm) were used duration of 15.3 min. After this process, the centermost ∼110 g of
to fill the bottom of the 13 L terra cotta flowerpot to act as thermal product is removed for characterization and was identified as SiC. The
insulation. A square Garolite G-10 GFRP plate was purchased from rest of the feedstock was less well-reacted and was thus left behind.
Amazon for $14.95 (257.5 mm side length, 2.0 mm thickness, Thus, a 110 g/15.3 min SiC production rate (0.43 kg/h) is counted.
702401461076) and was cut with a bandsaw to a circular shape (∼18 Quartz Tube Synthesis of CNTs. For the high-yield method, a
cm diameter) to fit inside the pot. This GFRP was then placed and surface-wetting method was used to load metal catalyst onto HDPE.10
rested upon this large grain MC layer to prevent fine grains of GFRP- HDPE was purchased from Polywize and ground using a 1400 rpm,
MC mixture from falling to the bottom of the pot. 300 g of large MC 110 V micro plant grinder. A solution of 80%/20% v/v mixture of
grains (1.7−3 mm) were then used to fill the volume in the pot above water and ethanol was prepared, and FeCl3 at a concentration of 0.1 g
the plate. The 900 g of 1:2 GFRP-MC powder mixture was then mL−1 was dissolved in the solution. Five g of <0.1 mm grain size
poured above the large grain MC layer. The arc welder cathode HDPE was submerged in 15 mL solution and sonicated for 15 min.
(negative) clamp was attached to a 0.2 m long, 16 mm diameter Solvent was evaporated for 30 min with a rotary evaporator and then
graphite rod, and the anode (positive) clamp was attached to a 0.2 m placed under a vacuum for 3 h. Afterward, the sample was dried at
long, 8 mm diameter graphite rod. Each arc welder clamp was itself room temperature for 18 h. 80 wt % catalyst-loaded HDPE was
held above the pot by a chemical clamp mounted on a laboratory ground with 20 wt % amorphous carbon black (Cabot) using a mortar
clamp stand. These rods were then embedded ∼3 cm deep into the and pestle. 0.20 g of the HDPE and carbon black homogeneous
GFRP-MC mixture, with the large graphite rod (anode, positive) mixture was loaded into a quartz tube with an internal diameter of 8
inserted laterally in the center of the pot and the small graphite rode mm. A copper wool plug and a graphite electrode were used to
(cathode, negative) inserted laterally ∼6 cm away from the large rod compress the sample.
(Figure S39). These arc welder electrodes were plugged into two Scaled CNT-MCFG Reactor. A schematic illustration of the scaled
Amico Electric ARC-200 DC arc welders connected in a series CNT-MCFG reactor is shown in Figure S44. 50 g of HDPE was
configuration as illustrated in Figures S30a, S31a. Each of these arc mixed with 0.5 wt % ferrocene and compressed into pellets ∼1 cm in
welders were themselves plugged into a 208 V, single phase, AC diameter. These pellets were then mixed with 500 g of large grain MC

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(1.7−3 mm). 500 g of large MC grains (1.7−3 mm) were used to fill attached to the end of a 0.2 m long, 8 mm diameter graphite rod. Each
the bottom of the 13 L terra cotta flowerpot to act as thermal arc welder clamp was itself held above the pot by a chemical clamp
insulation. 500 g mixture of MC and ferrocene-loaded HDPE was mounted on a laboratory clamp stand. These rods were then
mixed and filled the top of the container, resting upon the 500 g large embedded ∼3 cm deep into the MC, with the large graphite rod
MC grains. The arc welder cathode (negative) clamp was attached to (anode, positive) inserted laterally in the center of the pot and the
a 0.2 m long, 16 mm diameter graphite rod and the anode (positive) small graphite rode (cathode, negative) inserted laterally ∼6 cm away
clamp was attached to a 0.2 m long, 8 mm diameter graphite rod. from the large rod (Figure S39). These arc welder electrodes were
These rods were then embedded ∼3 cm deep into the HDPE-MC plugged into an Amico Electric ARC-200 DC arc welder, which itself
mixture and ∼4 cm apart. Each arc welder clamp was itself held above was plugged into a 208 V, single-phase AC outlet. The clay pot was
the pot by a chemical clamp mounted on a laboratory clamp stand. mounted onto a wooden block (rectangular prism shape, 3 cm height,
These rods were then embedded ∼3 cm deep into the HDPE-MC 8 cm side length) to add a layer of thermal and electrical insulation
mixture, with the large graphite rod (anode, positive) inserted laterally below the pot. The pot and wood block were then mounted onto a
in the center of the pot and the small graphite rode (cathode, JAYEGT Motorized Rotating Display Stand. Nine fused quartz tubes
negative) inserted laterally ∼4 cm away from the large rod (Figure (4 cm length, 8 mm inner diameter, 12 mm outer diameter) were
S39). These arc welder electrodes were plugged into two Amico prepared with the PMD feedstock in the following way: four were
Electric ARC-200 DC arc welders connected in a series configuration each filled with a mixture of 0.4 g SnCl2·2H2O powder and 1.0 g S
as illustrated in Figure S30a, S31a. Each of these arc welders were powder, and five were filled each with a mixture 0.4 g SnCl2·2H2O
themselves plugged into a 208 V, single phase, AC outlet. The use of powder and 1.0 g Se powder. Each tube was then capped on each end
two arc welders in series rather than only one arc welder increases the with a tight-fitting graphite cap (cylinder shape, 8 mm diameter, and
production rate and the voltage of the arc welder series system, ∼6 mm length). These nine quartz tubes were placed evenly spaced in
allowing this higher resistance HDPE-MC sample to be heated more a nonagonal pattern around the center electrode, ∼3 cm from the
easily, as described in Figure S46. The clay pot was mounted onto a center electrode. Each tube was oriented vertically and embedded 5
wooden block (rectangular prism shape, 3 cm height, 8 cm side cm into the MC so that the tubes were completely covered by the
length) to add a layer of thermal and electrical insulation below the MC. The rotating platform was then turned on and began spinning at
pot. The pot and wood block were then mounted onto a JAYEGT ∼3 rpm. Because the pot was placed on top of the turning stand but
Motorized Rotating Display Stand. The rotating platform was then the electrodes were held independently, the pot and the MC mixture
turned on and began spinning at ∼3 rpm. Since the pot was placed on within rotated relative to the electrodes to permit more uniform
top of the turning stand but the electrodes were held independently, heating (Figure S39). To begin the FJH reaction, the arc welder dials
the pot and the feedstock mixture within rotated relative to the (arc force and output current dials) were then turned to the maximum
electrodes to permit more uniform heating (Figure S39). The heating output such that the screen of the arc welder displayed an output
procedure is illustrated in Figure S41. To begin the FJH reaction, the value of 200. The reaction proceeded for 1 min before the arc welder
arc force dials on both systems were turned to their maximum setting,
and rotating platform were turned off. The nine quartz tubes were
and the current dials output on both systems were adjusted so that a
recovered, and an average of 0.2 g of SnS2 was recovered from the five
current output value of 60 was displayed on the screens of each arc
tubes with Se, and 0.15 g SnSe2 was recovered from the four tubes
welder. This configuration and system setting was maintained during
with S, for a total yield of 1.6 g PMD product. The production rate of
2.5 min of pretreatment flashing, as illustrated in step 1 of Figure S41.
1.6 g/1 min (0.1 kg/h) was thus counted.
This pretreatment step made the feedstock more conductive to allow
Arc Melter. The arc melting process occurs within a custom-
a higher current to flow through the sample in subsequent heating
designed arc melter comprising a vacuum chamber surrounded by a
steps. For the second heating step, the current output of both arc
welders was then adjusted so that a current output of 120 au was cylindrical glass shield, a water-cooled copper crucible featuring
achieved, as read from the screens of the arc welders, and the rotating grooves for sample placement, and a tungsten electrode tip (2%
platform was turned on at ∼3 rpm. This second heating configuration lanthanated). To initiate an arc, a potential difference is established
was maintained for 2.5 min. For the third heating step, the center between the tungsten tip and the samples on the crucible by applying
electrode (anode) was then moved laterally to the outer radius of the an adjustable DC current (60−75 A). Simultaneously, a piece of Zr
pot such that it was still ∼4 cm from the cathode, but now ∼6 cm with a high oxygen affinity is introduced into the chamber to capture
from the center of the pot (Figure S40b). This movement of the any trace oxygen present. The chamber is evacuated to a base pressure
electrode was achieved by laterally moving the laboratory clamp stand of 30 mTorr to remove air, after which it is filled with argon gas to
holding the electrode. The reaction was allowed to proceed for facilitate arc formation. The tungsten electrode is then brought closer
another 2.5 min in this configuration. during which the outer lateral to the Zr piece to melt it and absorb any residual oxygen. The samples
radius of HDPE-MC near the surface was heated (Figure S41, step 3). are positioned in separate grooves and are heated by bringing the
After this, a third electrode orientation was implemented for a fourth tungsten tip into contact with them and applying DC current.
heating step by first moving the anode to the lateral center of the pot Analysis. Raman Spectroscopy Analysis. Raman spectra were
and again moving the laboratory clamp stand. The reaction was then collected using a Renishaw inVia microscope outfitted with a 50 mW,
continued for another 2.5 min. Thus, the reaction consisted of four 532 nm laser and a 50× objective lens. Except where explicitly stated,
heating steps: one pretreatment heating step for 1 min, a second all Raman spectra were collected as follows and as previously
heating step for 2.5 min, a third heating step for 2.5 min, and a fourth reported:16,22 two Raman spectra were measured on each of 100
heating step for 2.5 min for a total reaction time of 9.5 min. 400 g of points across a square 1 mm2 grid on the sample using a map scan
the top-center-most feedstock was now obtained as the CNT-MCFG with LiveTrack focusing software enabled. The average Raman spectra
product, leaving behind 150 g of poorly reacted HDPE-MC feedstock shown for each sample are the average of these 200 spectra. The I2D/G
at the bottom and sides of the container and the initial layer of 500 g and ID/G ratios and their standard deviations are calculated from these
of MC. Only this 400 g of CNT-MCFG product was considered in 200 spectra per sample as well using a custom Python program as
the production rate calculation. Hence, a CNT-MCFG production previously described. Graphene yield is a metric that describes the
rate of 400 g/9.5 min (2.5 kg/h) was achieved. amount of product that has been converted to graphene as a portion
Scaled PMD Synthesis. The synthesis of the PMD SnS2 and of the total product. For the 200 spectra of each sample, a custom
SnSe2 was achieved by combining the previously reported flash- Python program first determines the number of spectra that have a
within-flash synthesis technique2 with the scaled reactor, as illustrated discernible G peak. Among these spectra, the program counts the
in Figure 5a. To achieve this synthesis, 500 g large MC grains (1.7−3 portion of which that has an I2D/G peak ratio of at least 0.3. This
mm) were poured into the 13 L terra cotta flowerpot. The arc welder portion is equal to the graphene yield. A spectrum without a
cathode (negative) clamp was attached to the end of a 0.2 m long, 16 discernible G peak in a carbon sample most often results from the
mm diameter graphite rod, and the anode (positive) clamp was Raman laser being insufficiently focused.

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Carbon nanotube RBMs were scanned using 10% laser power for Carolyn Teng − Department of Chemistry, Rice University,
100 accumulations at 100 s per accumulation. These data were then Houston, Texas 77005, United States
smoothened with the OriginLab graphing software using the Phelecia Scotland − Department of Materials Science and
Savitzky−Golay method with a second-order polynomial. These NanoEngineering, Rice University, Houston, Texas 77005,
RBM peak positions identified correspond to the RBMs of the
innermost CNTs in the multiwalled CNTs synthesized. Relative to
United States
the Raman peak positions of the RBMs of single-walled CNTs, the Shichen Xu − Department of Chemistry, Rice University,
innermost CNTs of multiwalled CNTs exhibit a blueshift in the Houston, Texas 77005, United States
Raman signal that is dependent on the innermost CNT diameter,25 by Alexander Lathem − Applied Physics Graduate Program and
up to 7% for 1.7 nm diameter tubes.26 Thus, this blueshift was Smalley-Curl Institute and Department of Chemistry, Rice
considered in the assignment by Raman spectroscopy analysis of University, Houston, Texas 77005, United States
RBMs to their respective CNT indices. This assignment was then Shihui Chen − Department of Chemistry, Rice University,
performed by comparing our measured Raman excitation energy and Houston, Texas 77005, United States
RBM wavenumber values to previously reported values.27,37 RBMs Carter Kittrell − Department of Chemistry, Rice University,
can still be excited by a Raman laser off resonance by as much as 0.2
eV.38
Houston, Texas 77005, United States; orcid.org/0000-
Transmission Electron Microscopy Analysis. Transmission elec- 0002-8449-4292
tron microscopy (TEM) images were collected using an FEI Titan Yimo Han − Applied Physics Graduate Program and Smalley-
Themis operating at 300 keV with a convergence angle of 25 mrad. Curl Institute and Department of Materials Science and
An aliquot of the sample (5 mg of sample/1 mL of ethanol) was NanoEngineering, Rice University, Houston, Texas 77005,
prepared and was sonicated for 1 h to ensure homogeneous United States; orcid.org/0000-0003-0563-4611
dispersion. The resultant aliquot was drop cast on a Cu/lacey carbon
TEM grid (Ted Pella). The resultant grid was dried at 80 °C with Complete contact information is available at:
overnight vacuum drying. https://pubs.acs.org/10.1021/acsnano.4c11628
Scanning Electron Microscopy Analysis. Scanning electron
microscope images of the arc melter products were taken by using Notes
an FEI Helios SEM system. All other SEM images were obtained by The authors declare the following competing financial
using an FEI Quanta 400 ESEM FEG. interest(s): A company has licensed the FJH approach for
X-ray Diffraction Analysis. X-ray diffractometry scans were
performed using a Rigaku Smartlab II instrument using zero
graphene synthesis from Rice University. J.M.T. is a stock-
background sample holders, 40 kV, a 30 mA X-ray source, and a holder in that company, but not an employee, officer, or
Cu K-β filter. director. Potential conflicts of interest are mitigated through
X-ray Photoelectron Spectroscopy Analysis. XPS analysis was regular disclosures to and compliance with Rice University's
performed using PHI Quantera XPS. Office of Sponsored Programs and Research Compliance. The
other authors declare no conflicts.
ASSOCIATED CONTENT A version of this work was previously published on a preprint
*
sı Supporting Information server: Eddy, L.; Shin, J.; Cheng, Y.; Choi, C. H.; Teng, C.;
The Supporting Information is available free of charge at Scotland, P.; Xu, S.; Lathem, A.; Chen, S.; Kittrell, C. Han, Y.;
https://pubs.acs.org/doi/10.1021/acsnano.4c11628. Tour, J. M. Kilogram Flash Joule Heating Synthesis with an
Additional safety instructions, graphs, photographs, Arc Welder. 2024. ChemRxiv. 10.26434/chemrxiv-2024-nfnc9
tables, and data (PDF) (accessed November 1, 2024.)
A video of the scaled flowerpot reactor being used to
convert MC to MCFG (MP4) ACKNOWLEDGMENTS
The funding of the research was provided by the Air Force
AUTHOR INFORMATION Office of Scientific Research (FA9550-22-1-0526, J.M.T.), the
Corresponding Author U.S. Army Corps of Engineers, ERDC (W912HZ-21-2-0050
James M. Tour − Applied Physics Graduate Program and and W912HZ-24-2-0027, J.M.T.), the Welch Foundation (C-
Smalley-Curl Institute, Department of Chemistry, and 2065-20210327, Y.H.), and a Rice Academy Fellowship (Y.C.).
Department of Materials Science and NanoEngineering, Rice The characterization equipment used in this project is partly
University, Houston, Texas 77005, United States; The from the Shared Equipment Authority (SEA) at Rice
NanoCarbon Center and The Rice Advanced Materials University. We also thank Onur Tosun and Emilia Morosan
Institute and Department of Computer Science, Rice for their help accessing and using the arc melter system, as well
University, Houston, Texas 77005, United States; as Juan Fernando Harmjanz for his help with Fourier analysis.
orcid.org/0000-0002-8479-9328; Email: [email protected]
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