The behavior of iodine in stabilized granular activated carbon and silver mordenite in cementitious
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Yamagata, Alessandra Fujii↗
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Gradient synthesis of carbon quantum dots and activated carbon from pulp black liquor for photocatalytic hydrogen evolution and supercapacitor
Black liquor (BL) is a by-product of the chemical pulping industry and is mainly used as a low-value fuel; however, its potential to produce high-value products has not been fully exploited. In this study, a green and simple strategy is reported for the gradient production of Na + -functionalized carbon quantum dots (Na + -CQDs) for the first time, N and S co-doped CQDs (N/S-CQDs), and N and S co-doped KOH-activated carbon (N/S-KAC) from BL by dialysis, hydrothermal carbonization and activation-carbonization, respectively. Due to the good electron trapping ability, photoluminescence and promising up-conversion luminescence of CQDs, the hydrogen evolution efficiency of Na + -CQDs/TiO 2 and N/S-CQDs/TiO 2 photocatalysts was improved by 2.45 and 1.46 times, respectively, compared with pure TiO 2 . N/S-KAC with a high specific surface area of 2294 m 2 g -1 provides an excellent specific capacitance of 253 F g -1 at 0.5 A g -1 and a promising energy density of 26.92 Wh kg -1 under a power density of 566 W kg -1 for the fabricated symmetrical supercapacitor. Moreover, the electrode material has good cycling stability with a capacitance retention of ~ 93.91% after 5000 cycles. In conclusion, this pathway provides a versatile and scalable approach for the construction and co-production of nanostructured materials, photocatalysts and energy storage devices.
36 MATERIALS SCIENCE↗
Performance and Economic Analysis of Organosolv Softwood and Herbaceous Lignins to Activated Carbons as Electrode Materials in Supercapacitors
In this work, yellow pine (YP, softwood) and switchgrass (SG, grass) lignins were extracted as a coproduct of an organosolv γ-valerolactone (GVL) biorefinery that also produces biofuels and furfural. The extracted lignins were converted to carbon precursors for synthesizing porous activated carbon electrodes for high energy-density supercapacitors. This research details the impact of lignin composition on the derived porous structures and electrochemical properties of activated carbons. Lignin precursors with various syringyl (S) to guaiacyl (G) contents were characterized using 31 P nuclear magnetic resonance (NMR) and two-dimensional 1 H‒ 13 C NMR. A two-step activation process, using steam and carbon dioxide as the activating agents, enabled the formation of porous carbons structures with high surface area. The capacitive behavior of supercapacitors was systematically characterized by cyclic voltammetry, charge-discharge cycling, and electrochemical impedance spectroscopy. The specific capacitance of YP and SG capacitors reached 367 and 221 F g −1 , respectively. Both types of capacitors demonstrated remarkably stable capacitance (capacitance retention >90%) along with excellent Coulombic efficiency (>99%) over 10,000 cycles. Compared to SG electrode, the better electrochemical performance achieved with YP electrodes was mainly due to shorter diffusion path, improved ionic mobility, and increased active surface area. The inexpensive lignin-based porous electrodes synthesized in this work can be used for various electrochemical devices for improved performance, decreased cost, and enhanced durability. This work also demonstrates that the selection of feedstock and appropriate processing conditions can tailor the structure of carbon composites for targeted applications. Techno-economic analysis indicates that YP and SG activated carbons can be produced at a minimum selling price of $8,493 and $6,670 per ton, respectively, which is competitive with the commercially available supercapacitor-grade activated carbons.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
An Assessment of the Conversion of Biomass and Industrial Waste Products to Activated Carbon
The production of biochar from biomass and industrial wastes provides both environmental and economic sustainability. An effective way to ensure the sustainability of biochar is to produce high value-added activated carbon. The desirable characteristic of activated carbon is its high surface area for efficient adsorption of contaminants. Feedstocks can include a number of locally available materials with little or negative value, such as orchard slash and crop residue. In this context, it is necessary to determine and know the conversion effects of the feedstocks to be used in the production of activated carbon. In the study conducted for this purpose; several samples (piñon wood, pecan wood, hardwood, dried grass, Wyoming coal dust, Illinois coal dust, Missouri coal dust, and tire residue) of biomass and industrial waste products were investigated for their conversion into activated carbon. Small samples (approximately 0.02 g) of the feedstocks were pyrolyzed under inert or mildly oxidizing conditions in a thermal analyzer to determine their mass loss as a function of temperature and atmosphere. Once suitable conditions were established, larger quantities (up to 0.6 g) were pyrolyzed in a tube furnace and harvested for characterization of their surface area and porosity via gas sorption analysis. Among the samples used, piñon wood gave the best results, and pyrolysis temperatures between 600 and 650 °C gave the highest yield. Slow pyrolysis or hydrothermal carbonization have come to the fore as recommended production methods for the conversion of biochar, which can be produced from biomass and industrial wastes, into activated carbon.
09 BIOMASS FUELS↗
From cellulose to 1,2,4-benzenetriol via catalytic degradation over a wood-based activated carbon catalyst
In this study, spherical P-doped activated carbon (CSP) was obtained from poplar bark by microwave carbonization with phosphoric acid as the dopant and activating agent. Phosphorus bonded with four oxygen atoms to form a phosphate-like structure rather than directly bonding with C atoms in CSP; such groups can provide Lewis acid active sites with moderately strong acidity. The Lewis acid and total acid content increased with increasing phosphoric acid doping ratio. The use of phosphoric acid as an activating agent promotes the formation of a developed porous structure. CSP 1 (mass ratio of raw material to acid = 1 : 1) had a specific surface area of 1115 m 2 g –1 with developed micro–mesoporous structures, mainly micropores. Investigation of the activity of CSP in catalytic cellulose hydrolysis during hydrothermal degradation showed that Brønsted acid sites promote hydrolysis and dehydration of cellulose, Lewis acid sites promote subsequent reactions such as isomerization, rearrangement, and oligomerization, and the developed pores can provide reaction sites and facilitate reactant transportation. The optimal reaction conditions, i.e. , 1 h at 230 °C and 1 MPa with CSP 1 (0.4 g) as the catalyst, gave a cellulose conversion of >99.9%, with 42.30% selectivity for 1,2,4-benzenetriol. This study provides an effective method for preparing 1,2,4-benzenetriol from cellulose with biomass-based activated carbon as the catalyst, which enables green synthesis of 1,2,4-benzenetriol and promotes the use of biomass waste resources.
1,2,4-benzenetriol↗
Emerging Modification Technologies of Lignin-based Activated Carbon toward Advanced Applications
Lignin-based activated carbon (LAC) is a promising high-quality functional material due to high surface area, abundant porous structure, and various functional groups. Modification is the most important step to functionalize LAC by altering its porous and chemical properties. Here, this Review summarizes the state-of-the-art modification technologies of LAC toward advanced applications. Promising modification approaches are reviewed to display their effects on the preparation of LAC. The multiscale changes in the porosity and the surface chemistry of LAC are fully discussed. Advanced applications are then introduced to show the potential of LAC for supercapacitor electrode, catalyst support, hydrogen storage, and carbon dioxide capture. Finally, the mechanistic structure-function relationships of LAC are elaborated. These results highlight that modification technologies play a special role in altering the properties and defining the functionalities of LAC, which could be a promising porous carbon material toward industrial applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Removal of radionuclides from acidic solution by activated carbon impregnated with methyl- and carboxy-benzotriazoles
The removal efficiencies of metals commonly used to model the fate and transport of aqueous uranium and radioactive its daughter products, were observed on activated carbons impregnated with different benzotriazole derivatives. Acidic solutions containing U(VI), Sr(II), Eu(III), and Ce(III) were used to determine the immobilization potential of carboxybenzotriazole (CBT) and methylbenzotriazole (MeBT), where these derivatives were sorbed to different types of granular activated carbon (GAC). This sorption behavior can be predicted by Redlich–Peterson model. Flow-through column tests showed that the immobilization of uranium and some of its daughter products, significantly improves in response to oxidized GACs saturated with carboxybenzotrzole (CBT), which reached a maximum elimination for U(VI) at 260 BV, Eu(III) at 114 BV, Ce(III) at 126 BV, and Sr(II) at 100. MeBT significantly desorbed from GAC under acidic conditions. Trace amounts of CBT were observed in some column effluents, but this did not appear to alter the effectiveness of metal removal, regardless of the model radionuclide studied. These results suggest that enhanced immobilization of selected metals on GAC, can be achieved by impregnating oxidized activated carbon with carboxylated benzotriazoles, and that metal removal efficiency on this media, is related to their valence and ionic radius in acidic environments.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Lignin-Derived Magnetic Activated Carbons for Effective Methylene Blue Removal
Large-scale environmental remediation of polluted water requires an effective and recyclable adsorbent produced from an abundant, low-cost, and renewable feedstock via a simple processing procedure. In this work, we demonstrate that lignin-derived magnetic activated carbons (mACs) uniquely satisfy these five criteria for (i) high-performance adsorption, (ii) high regeneration efficiency, (iii) feedstock economic and environmental viability, (iv) single-step processing and (v) large-scale production. The mACs are synthesized via an efficient co-carbonization and activation with simultaneous impregnation of ferric sulfate. Here, the Langmuir model closely fits the adsorption of methylene blue (MB) by mACs within the temperature range of 298–323 K, where the adsorption capacity increases as temperature increases. This capacity increased from 55.0 mg g -1 to 220.2 mg g -1 with the presence of magnetic nanoparticles. In addition, the magnetite nanoparticles on the ACs surface significantly improve its recycling ability with the removal percentage above 95% after four cycles for 5:1 mAC.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
In Operando Calorimetric Measurements for Activated Carbon Electrodes in Ionic Liquid Electrolytes under Large Potential Windows
This study aims to investigate the effect of the potential window on heat generation in carbon-based electrical double layer capacitors (EDLCs) with ionic-liquid (IL)-based electrolytes using in operando calorimetry. The EDLCs consisted of two identical activated-carbon electrodes with either neat 1-butyl-1-methylpyrrolidinium bis(trifluoromethane-sulfonyl)imide ([Pyr 14 ][TFSI]) electrolyte or 1.0 m [Pyr 14 ][TFSI] in propylene carbonate (PC) as electrolyte. The instantaneous heat generation rate at each electrode was measured under galvanostatic cycling for different potential windows ranging from 1 to 4 V. First, the heat generation rates at the positive and negative electrodes differed significantly in neat IL owing to the differences in the ion sizes and diffusion coefficients. However, these differences were minimized when the IL was diluted in PC. Second, for EDLC in neat [Pyr 14 ][TFSI] at high potential window (4 V), a pronounced endothermic peak was observed at the beginning of the charging step at the positive electrode owing to TFSI - intercalation in the activated carbon. On the other hand, for EDLC in 1.0 m [Pyr 14 ][TFSI] in PC at potential window above 3 V, an endothermic peak was observed only at the negative electrode owing to the decomposition of PC. Third, for both neat and diluted [Pyr 14 ][TFSI] electrolytes, the irreversible heat generation rate increased with increasing potential window and exceeded Joule heating. This was attributed to the effect of potential-dependent charge redistribution resistance. Additionally, a further increase in the irreversible heat generation rate was observed for the largest potential windows owing to the degradation of the PC solvent. Finally, for both types of electrolyte, the reversible heat generation rate increased with increasing potential window because of the increase in the amount of ion adsorbed/desorbed at the electrode/electrolyte interface.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Machine-learning-assisted material discovery of oxygen-rich highly porous carbon active materials for aqueous supercapacitors
Abstract Porous carbons are the active materials of choice for supercapacitor applications because of their power capability, long-term cycle stability, and wide operating temperatures. However, the development of carbon active materials with improved physicochemical and electrochemical properties is generally carried out via time-consuming and cost-ineffective experimental processes. In this regard, machine-learning technology provides a data-driven approach to examine previously reported research works to find the critical features for developing ideal carbon materials for supercapacitors. Here, we report the design of a machine-learning-derived activation strategy that uses sodium amide and cross-linked polymer precursors to synthesize highly porous carbons (i.e., with specific surface areas > 4000 m 2 /g). Tuning the pore size and oxygen content of the carbonaceous materials, we report a highly porous carbon-base electrode with 0.7 mg/cm 2 of electrode mass loading that exhibits a high specific capacitance of 610 F/g in 1 M H 2 SO 4 . This result approaches the specific capacitance of a porous carbon electrode predicted by the machine learning approach. We also investigate the charge storage mechanism and electrolyte transport properties via step potential electrochemical spectroscopy and quasielastic neutron scattering measurements.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Regulating the properties of activated carbon for supercapacitors: impact of particle size and degree of aromatization of hydrochar
Hydrochar (HC), obtained by the hydrothermal carbonization (HTC) of biomass, is an excellent precursor for preparing activated carbon (AC). However, the effects of the intrinsic properties of HC on the microstructure and electrochemical properties of AC are largely unknown. Here, this study investigates the impact of particle size and the degree of aromatization of in-situ HC on the microstructure and electrochemical properties of AC. Our results show that a large particle size and a high degree of aromatization help protect the HC from overactivation by ZnCl 2 , resulting in an large specific surface area (SSA > 2000 m 2 /g) and high mesopore to micropore volume ratio value ( V mes /V mic > 0.3) of the AC. Electrochemical performance measurements show a maximum specific capacitance of 218 F/g at 0.5 A/g was achieved in all samples where the AC (AC180-10 h) was prepared by activating HC180-10 h with a large size, a high degree of aromatization, and abundant surface oxygen-containing functional groups. After AC180-10 h was assembled into a supercapacitor, the specific capacitance of AC180-10 h still reached 158 F/g at 0.5 A/g, and it showed excellent cycling stability. This study advances the understanding of the impact of HC particle size and degree of aromatization on AC properties, providing new insights into tailoring HC qualities so that improving improve the properties of AC.
36 MATERIALS SCIENCE↗
Static iodine loading comparisons between activated carbon, zeolite, alumina, aerogel, and xerogel sorbents
Different sorbents, including activated carbons, an aerogel, xerogels, an alumina, a zeolite, and a carbon foam were investigated for static I 2(g) loading at 71 °C for 56 d followed by 4.7 d of desorption.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
The Role of Lignin Molecular Weight on Activated Carbon Pore Structure
Over the past decade, the production of biofuels from lignocellulosic biomass has steadily increased to offset the use of fuels from petroleum. To make biofuels cost-competitive, however, it is necessary to add value to the “ligno-” components (up to 30% by mass) of the biomass. The properties of lignin, in terms of molecular weight (MW), chemical functionality, and mineral impurities often vary from biomass source and biorefinery process, resulting in a challenging precursor for product development. Activated carbon (AC) is a feasible target for the lignin-rich byproduct streams because it can be made from nearly any biomass, and it has a market capacity large enough to use much of the lignin generated from the biorefineries. However, it is not known how the variability in the lignin affects the key properties of AC, because, until now, they could not be well controlled. In this work, various fractions of ultraclean (<0.6% ash) lignin are created with refined MW distributions using Aqueous Lignin Purification using Hot Agents (ALPHA) and used as precursors for AC. AC is synthesized via zinc chloride activation and characterized for pore structure and adsorption capacity. We show that AC surface area and the adsorption capacity increase when using lignin with increasing MW, and, furthermore, that reducing the mineral content of lignin can significantly enhance the AC properties. The surface area of the AC from the highest MW lignin can reach ~1830 m2/g (absorption capacity). Furthermore, single step activation carbonization using zinc chloride allows for minimal carbon burn off (<30%), capturing most of the lignin carbon compared to traditional burn off methods in biorefineries for heat generation.
Biochemistry & Molecular Biology↗
Activated carbon supported Ni, Fe, and bimetallic NiFe catalysts for CO x -free H 2 production by microwave methane pyrolysis
The goal of this study was to test the effect of metal-impregnated carbon-based catalysts on the conversion of methane to hydrogen gas and solid carbon using microwave reactor technology. Monometallic and bimetallic catalysts on activated carbon supports (Ni/AC, Fe/AC, Ni-Fe/AC) are compared during methane pyrolysis testing. Catalytic methane pyrolysis was carried out in a microwave reactor at reaction temperatures of 600 °C and 800 °C. For comparison, one of the catalysts (Ni-Fe/AC) was tested in a conventionally heated reactor at 800 °C. The prepared catalysts were characterized by X-ray diffraction (XRD), while post-reaction catalysts were characterized by XRD and SEM. During reaction testing, the monometallic Ni/AC catalyst exhibited the best catalytic activity (CH 4 conversion: 46.0 and H 2 yield: 46.9%) when reacted in the microwave reactor, however, it suffered from rapid deactivation from carbon deposition (carbon yield: 0.39 gC/g catalyst). The bimetallic Ni-Fe/AC catalyst was slightly less active (CH 4 conversion: 36.9 and H 2 yield: 40.5%) but it was more resistant to carbon formation (carbon yield: 0.27 gC/g catalyst) suggesting it may have greater long-term stability. The Ni-Fe/AC catalyst was also the most energy efficient as it required the least microwave power to maintain the 800 °C reaction temperature compared to the other catalysts tested. Methane conversion of the bimetallic Ni-Fe/AC at 800 °C under microwave irradiation was three times the conversion under conventional heating at the same reaction temperature. Finally, this work demonstrates the use of microwave-specific catalysts for catalytic methane pyrolysis in a microwave reactor, and can be used as a foundation for further methane pyrolysis process and catalyst optimization for CO x -free H 2 production.
08 HYDROGEN↗
A comprehensive study on two types of supercapacitor composite electrodes comprising MnO 2 and activated carbon nanofibers: Self-supporting membrane and ground powder
Manganese dioxide (MnO 2 )@carbon composites have been attractively considered as electrode materials for supercapacitors (SCs) due to synergistic effects. This work systematically investigated the structure of MnO 2 @carbon nanofiber (CNF) composite electrodes with the different forms of CNFs and the corresponding electrochemical performance of SCs. In brief, novel activated carbon nanofibers were first fabricated by electrospinning the hydroxyl-containing poly(amic acid) solution, and then the preferred CNF material was decorated by MnO 2 crystals in the form of self-supporting membrane and ground powders, respectively. Additionally, the synthesis parameters were investigated and optimized based on the electrochemical performance of SCs. The results reveal that the powdered composite electrode exhibits a higher specific surface area of 501 m 2 g –1 compared to the self-supporting membrane composite electrode under the same conditions, resulting in a promising specific capacity of 214.1 mAh g –1 (770.8 Fg –1 ) in 6M KOH solution at 0.5 A g –1 . In addition, the capacitance of the symmetrical SC device assembled by G-HMC-1:3–80 reaches 179.8 Fg –1 , coupled with an energy density of 24.86 Whkg –1 at 230 Wkg –1 power density. This work provides valuable hints for designing SC composite electrode materials with outstanding performance.
25 ENERGY STORAGE↗
Model-based economic analysis under uncertainty for PFAS treatment by granular activated carbon and ion exchange technologies
Recent drinking water regulations have imposed the need for per- and polyfluoroalkyl substances (PFAS) remediation. In response, treatment facilities may be required to retrofit existing treatment schemes to treat PFAS below maximum contaminant levels (MCLs). Adsorption technologies such as granular activated carbon (GAC) and ion exchange (IX) have been demonstrated to be effective; however, there are limited techno-economic metrics available which provide guidance on technology selection and design for diverse PFAS-containing source water conditions. Process systems engineering (PSE) tools which can traditionally perform these analyses are hindered by the data availability, model validity, and understanding of treatment phenomena for emerging contaminants. This work employs published data regressions, statistical models, process models, techno-economic analyses, and other process systems tools in a model-based uncertainty framework to consider the limitations of emerging contaminant research. Through this analysis framework, economic results are provided as probabilistic distributions based on the uncertainty of the models and diverse conditions that treatment facilities experience.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Decoupling the role of lignin, cellulose/hemi-cellulose, and ash on ZnCl 2 -activated carbon pore structure
Controlling biomass sugar and lignin composition enables the development of a clear correlation between composition and activate carbon pore structure.
Wu, Chengjun [Department of Chemical and Biomolecu↗