Carbon Materials Research Articles

Comparative Remediation of Arsenic and Antimony Co-Contaminated Soil by Iron- and Manganese-Modified Activated Carbon and Biochar.

At present, soil contaminated with arsenic (As) and antimony (Sb) is escalating at an alarming rate, which is harmful to human health. In this study, Fe- and Mn-modified activated carbon (AC) and biochar (BC) were prepared and compared for the remediation of As- and Sb-contaminated soil. The effects on the speciation of As and Sb, soil pH, organic matter (SOM), and enzyme activity with various dosages and remediation times were investigated. The results showed that on the whole, the best stabilization effect of As and Sb was achieved with 3% FeMnBC. Furthermore, with increases in time and dosage, the immobilization effect on As and Sb was more significant. Fe/Mn-modified AC and BC enhanced soil pH, with 3% MnAC being particularly effective; 3% AC and 3% FeMnAC demonstrated the most pronounced enhancement in SOM. The modified carbon materials exhibited a dramatic increase in enzymatic activity. In particular, urease activity showed an increasing trend, and catalase activity first decreased and then increased over 30 days. Among the treatments, 3% MnAC showed the most significant enhancements in catalase and urease activities, whereas 1% FeMnBC had the most pronounced effect on increasing sucrase activity. This study provides theoretical support for the remediation of soil co-contaminated with As and Sb by Fe/Mn-modified AC and BC.

Controlled chemical transformation of lignin by nitric acid treatment and carbonization

This study focuses on understanding the chemical reactions and results of Kraft lignin transformation through nitric acid treatment and subsequent carbonization. With its rich carbon content, lignin stands out as a promising candidate for the manufacturing of high-value carbon materials. The lignin underwent effective nitration, depolymerization, and oxidation under ambient conditions and at 40 °C, while a slight increase in reaction temperature significantly reduced the reaction time. The molecular weight Mw was effectively reduced from 4371 g/mol to 767 g/mol. The acid-treated lignin samples with incorporated nitro groups were further carbonized to create nitrogen-doped carbon structures. The resulting materials show stable nitrogen content (about at 5 wt%) even after carbonization due to the transformation of nitro groups into thermally stable pyridinic moieties, thereby exhibiting enhanced electrocatalytic properties compared to nitrogen-free carbon materials derived from Kraft lignin. The nitric acid-assisted treatment of lignin obviates the need for catalysts, and additional extraction or purification steps for preparing bio-derived carbon precursors, rendering it facile, fast, and cost-efficient.

Recent Progress in Photocatalytic Applications of Electrospun Nanofibers: A Review.

Electrospun fiber-based photocatalysts demonstrate significant potential in addressing global environmental and energy challenges, primarily due to their high specific surface areas and unique properties. This review examines recent advances in the application of these materials in photocatalytic processes, with a particular focus on water splitting and hydrogen production. The principles of the electrospun method are described in detail, along with the operating parameters, material characteristics, and environmental conditions that affect the fiber formation. Additionally, the review discusses the challenges, advantages, and future prospects of photocatalysts incorporating carbon materials, metals, semiconductors, and hybrid structures with improved performance. These materials have the potential to significantly improve the efficiency of hydrogen energy production, water purification, and CO2 recovery, highlighting their importance in engineering sciences.

Efficient solid-phase RNA extraction using carbon nanomaterials

Recent research highlights RNA’s therapeutic potential in nucleic acid-based therapies. However, effective RNA recovery and purification remain challenging due to similar impurities affecting therapeutic outcomes. Traditional RNA isolation methods are often slow, inefficient, and involve toxic reagents. Carbon-based materials offer a promising alternative as adsorbents for nucleic acids due to their excellent mechanical and chemical properties. This study describes an efficient, simple, and cost-effective method for RNA recovery from complex Escherichia coli extracts using carbon materials with different structures and surface modifications. RNA adsorption and desorption screening experiments were performed using different carbon materials. N-doped CNTs (CNT-N-ox) and carbon nanofibers (CNF-ox), both oxidized with HNO3, showed RNA adsorption capacities of 42 % and 55 %, respectively, also allowing effective RNA desorption (81 % and 72 %, respectively). Additionally, the materials demonstrated reusability, maintaining RNA adsorption capacity over four cycles. The selectivity of the materials enabled a simple method to recover RNA free from DNA contamination by performing three consecutive cycles. Moreover, no contaminating protein was found in the recovered sample. The analysis by circular dichroism also revealed that RNA maintained its integrity and stability when recovered from these materials. Overall, the study demonstrates the potential of carbon materials for efficient RNA capture and pre-purification.

Recent Advances in Bonding Regulation of Metalloporphyrin-Modified Carbon-Based Catalysts for Accelerating Energy Electrocatalytic Applications.

Metalloporphyrins modified carbon-based materials, owing to the excellent acid-base resistance, optimal electron transfer rates, and superior catalytic performance, have shown great potential in energy electrocatalysis. Recently, numerous efforts have concentrated on employing carbon-based substrates as platforms to anchor metalloporphyrins, thereby fabricating a diverse array of composite catalysts tailored for assorted electrocatalytic processes. However, the interplay through bonding regulation of metalloporphyrins with carbon materials and the resultant enhancement in catalyst performance remains inadequately elucidated. Gaining an in-depth comprehension of the synergistic interactions between metalloporphyrins and carbon-based materials within the realm of electrocatalysis is imperative for advancing the development of innovative composite catalysts. Herein, the review systematically classifies the binding modes (i.e., covalent grafting and non-covalent interactions) between carbon-based materials and metalloporphyrins, followed by a discussion on the structural characteristics and applications of metalloporphyrins supported on various carbon-based substrates, categorized according to their binding modes. Additionally, this review underscores the principal challenges and emerging opportunities for carbon-supported metalloporphyrin composite catalysts, offering both inspiration and methodological insights for researchers involved in the design and application of these advanced catalytic systems.

Mesoporous carbon spheres modified with atomically dispersed iron sites for efficient electromagnetic wave absorption

Carbon materials have obtained some achievements in electromagnetic wave (EMW) absorption owing to their excellent electrical conductivity and low density. However, poor impedance matching and high electrical conductivity limit their EMW absorption properties. Metal single atoms absorbers have garnered considerable attention in EMW absorption, largely due to the high metal availability and special coordination structure, but the modulation of the EMW absorption properties still needs to be improved. Herein, atomically dispersed Fe sites embedded into the N-doped mesoporous carbon spheres (Fe–SAs/NC) were synthesized through a facile coordination-assisted polymerization assembly strategy without acid leaching treatment. Benefitting from abundant mesoporous structure, the Fe–SAs/NC displays large specific surface area (339 m2 g−1) and optimized impedance matching, which results in an effective reduction of the absorber density. The homogeneously dispersed Fe single atoms (Fe–SAs) on the carbon skeleton lead to the improvement in conduction and dipole polarization losses of Fe–SAs/NC, which endows Fe–SAs/NC with exceptional EMW absorption properties. Experimental results indicate that Fe–SAs/NC displays desirable EMW absorption properties with the minimal reflection loss of −52.5 dB at 2.8 mm and the effective absorption bandwidth of 4.8 GHz. The study provides valuable insights for the development of carbon materials modified with atomically dispersed metal sites to achieve high-efficient EMW absorbers.

Interactive impacts of organic-inorganic modifiers on surface characteristics of Cu+-doped activated carbon for stable CO-adsorptive separation from CO2

Conventional Cu+-doped activated carbon (C) materials are problematic in carbon monoxide (CO)-selective adsorption from carbon dioxide (CO2) due to their CO2-friendly surface basicity and microporosity. In this study, boehmite (AlOOH) film modified-carbon composite (AlC) was hydrothermally synthesized to dope with 30 wt% Cu+ ions by the impregnation-calcination method. The functional hydroxyl groups of Boehmite behaved as metallic anchoring sites for better Cu+ ion dispersion, enhancing the CO adsorption uptake to 38.84 cm3/g at 25 °C and ∼ 100 kPa in isotherm analysis. Additionally, the improved Lewis acidity of AlC surface interface together with pore widening impact reduced the CO2 uptake to 14 cm3/g, around half that of Cu+-doped activated carbon, by undergoing Lewis acid-acid repelling interaction between boehmite film and CO2. However, to address rapid oxidation of Cu+ ions in the hygroscopic AlC structure, iron (II) chloride (FeCl2) surface modification on the Cu+-doped AlC composite created a Fe3+-Cu+ bimetallic interface with high Cu+ immobilization, enriching the CO adsorption stability to 92 % even after 30 day-air exposure. Noticeably, pre-complexation of FeCl2 with thiourea (NH2CSNH2) before its dispersion over the doped Cu+ ions led to distinct Cu+ stabilization mechanisms without bimetallic redox interaction. This involves developing auto-redoxable iron (II) sulfides as barrier coatings for Cu+ species against oxidation and raising the Cu2+ reducibility via cyanide-ligands of thiourea. These combined preservation effects for Cu+ ions ensured CO adsorption stability of 91 %, underlining higher CO adsorption uptake (39.38 cm3/g) and CO/CO2 selectivity (67.49 at 0.2 kPa and 3.09 at ∼ 100 kPa) than modification effects of boehmite and FeCl2.

A versatile opened hollow carbon sphere with highly loaded antimony alloy for ultra-stable potassium-ion storage

Carbon materials meet the stringent practical requirements for anodes for potassium-ion batteries (PIBs) due to their abundance and chemical stability. The major issue of carbon-based anodes is the low specific capacity and poor cyclic stability. Equally importantly, scalable synthesis approaches for electrodes are highly desired for the future application in large-scale energy storage systems. Herein, we developed a novel composite of Sb encapsulated in N/P co-doped opened hollow carbon spheres (N/POHCs) with high Sb loading through a simple carbonization and subsequent impregnation process. Beneficial from the virtue of abundant pyridinic-N−P bonding and opened hollow spherical structure advantages, N/POHCs exhibit much lower diffusion barrier than that of pure carbon, prominent Sb carrier capability, as well as the extraordinary resistance to volume expansion. The resulting Sb@N/POHCs composite delivers a high specific capacity of 533.3 mAh g−1 at 0.1 A g−1 with an initial Coulombic efficiency of 83 %, and can maintain a specific capacity of 345 mAh g−1 at 1 A g−1 after 4000 cycles. This work provides rational structure design with universal carrier capability of active materials to achieve high-capacity and long cycle life anode for advanced PIBs accompanied by the potential for large-scale production.

Potential-dependent kinetics of oxygen chemisorption as the crucial step of oxygen reduction reaction: GCDFT study

Nitrogen-doped carbon materials (NCMs) are widely regarded as promising alternatives to expensive platinum-based electrocatalysts for the oxygen reduction reaction (ORR). While NCMs exhibit considerable electrochemical activity in alkaline media, their performance in acidic environments remains a significant challenge. However, acidic conditions are commercially desirable for ORR’s catalysis in proton-exchange membrane fuel cells (PEMFCs). The dramatic pH dependence of NCM effectiveness has sparked ongoing debate, with several factors under consideration, including surface protonation, variations in hydrogen binding energy, differences in proton donors, and interface structure. In this work, we present a grand canonical density functional theory (GCDFT) study of the chemisorption step on pristine and nitrogen-doped graphene. Through nudged elastic band (NEB) calculations at various electrode potentials, we propose a potential-dependent (and thus pH-dependent) mechanism of oxygen chemisorption at graphitic nitrogen (Ngr) defects, offering new insights into the pH dependency of the onset potential in NCM catalysts.

Co-based carbon material as CYP3A4-like nanozyme with both biocatalytic activity and inhibition behaviors

Up to now, the biocatalytic activity of nanozymes has been extensively studied, while little research focus on their inhibitory behaviors. Here, Co-based carbon material (Co-DMOF) containing abundant carboxylic acid groups was prepared, with defects introduced by COx escape during pyrolysis to achieve controllable activity. As a result, Co-DMOF exhibited biocatalytic activity similar to cytochrome P450 3A4 (CYP3A4) in the metabolism of 1,4-Dihydropyridine (1,4-DHP, a calcium channel blocker). Excitingly, studies on IC50 and drug-drug interaction (DDI) suggested that Co-DMOF had similar inhibitory behaviors to CYP3A4. Moreover, Co-DMOF displayed excellent stability even under high temperature (100 °C), organic solvents, and a wide range of pH (4–9). Additionally, it can be reused for at least 7 times with only slight loss of activity. Therefore, Co-DMOF has great potential to become a low-cost alternative to CYP3A4 for drug dosage guideline, drug metabolism and DDI. This work provides more possibilities for expanding the CYP3A4-like nanozyme library.

Adsorption and energy storage characteristics of ionic liquids in porous zeolite-templated carbon materials

The energy storage capacity of supercapacitors is closely related to the capacity of their electrode materials to adsorb electrolytes. Porous zeolite-templated carbon (ZTC) materials are a type of porous carbon material with a well-defined spatial structure and are thus promising electrode materials. This study utilizes molecular dynamics simulations to compare the ion number density and charge density distributions of the [EMI][BF4] ionic liquid for various ZTC materials, while also examining the ion adsorption characteristics for different electrode charges. Parameters such as the degree of confinement (DOC) and the charge compensation per carbon (CCpC) are introduced to represent the ion adsorption and charge storage capacity of the materials, with a higher DOC indicating a greater number of encapsulated ions and a higher CCpC indicating a more efficient charge storage. The findings suggest that materials with a larger pore size tend to exhibit increased ion adsorption. However, many CCpC adsorption sites that can store more charge are then found in positions with a smaller DOC. This work unveils the ion adsorption characteristics of ZTC materials in charged electrode and presents the differential capacitance curves of various materials, thereby providing a theoretical foundation for the utilization of ZTC materials as electrodes in supercapacitors.

Effect of puffing on electrochemical properties of sorghum seed based porous carbon materials in supercapacitors

Biomass-based carbon materials are renewable, affordable and environmentally friendly, possessing great potential in electrochemical energy storage as electrode materials in supercapacitors due to their large specific surface area and self-doped heteroatoms. However, the electrochemical properties of these carbon materials may be influenced to some extent by pretreatment procedures of carbon precursors. For this research, a range of porous carbon materials based on unpuffed and puffed sorghum seeds were synthesized under various pre‑carbonization and activation temperatures. Among them, the puffed sorghum seed-based porous carbon (PH-R6A7), prepared through pre‑carbonization at 600 °C and KOH activation at 700 °C, exhibits a higher graphitization degree, increased N and O content, as well as a greater variety of nitrogen-containing groups and significant increasing graphite nitrogen compared to unpuffed sorghum seed-based porous carbon (PC-R6A7) fabricated under similar conditions. These improvements result in enhanced conductivity and wettability of electrode materials, thereby boosting their electrochemical properties. In a three-electrode setup employing a 6 M solution of KOH, PH-R6A7 demonstrates an exceptional specific capacitance of 523.84 F g−1 at 1 A g−1 compared with PC-R6A7 of 366.00 F g−1; even at a high current density of 20 A g−1 it maintains a high level of capacitance at 387.94 F g−1. When employed in a double-electrode configuration at the same current density (i.e., 1 A g−1), PH-R6A7 also achieves higher specific capacitance of 357.83 F g−1 than PC-R6A7 (286.89 F g−1), accompanied by an increased energy density of 12.35 Wh kg−1 and 8.85 Wh kg−1 at a power density of 249.97 W kg−1 and 4.98 kW kg−1, respectively. Furthermore, after undergoing 10,000 cycles at 2 A g−1, PH-R6A7 demonstrates a superior capacitance retention of 99.68 % and coulomb efficiency of 99.91 %. PH-R6A7 fabricated through the combination method of puffing pretreatment and carbonization activation merits acknowledgment as an electrode material of superior performance and notable practical importance.

Enhanced construction of 3D carbon skeleton through molten salt coupling activation effect for high efficiency capacitive deionization of lead (II) ions removal in wastewater

Efficiently eliminating of highly toxic ultra-dilute lead ions (Pb2+) from wastewater is a challenging task. Capacitive deionization (CDI) technology, based on the electrochemical capacitance mechanism, has emerged as a pivotal approach to address this challenge. In this work, a KNO3-mediated molten salt-coupled activation strategy was proposed to prepare nitrogen-doped hierarchical porous biomass carbon electrode material (3DCF-650-0.2) with a three-dimensional carbon skeleton, which was integrated into a symmetrical CDI device for Pb2+ removal. The 3DCF-650-0.2 electrode exhibited a high specific capacitance of 330.3 F g-1 at a current density of 1 A g-1, with a capacity retention rate of 98.45% after 10,000 cycles at 10 A g-1. Furthermore, the electrochemical adsorption capacity of the CDI device for Pb2+ reached 72.86 mg g-1 (1.2 V, 50 mg L-1), and the CDI device retained a high adsorption capacity of 91.14% after twenty adsorption/desorption cycles. These excellent adsorption properties are attributed to the in-situ activation and gas foaming of KNO3, which favors the production of reasonable pore structure (electric double-layer capacitance) and an appropriate pyrrolic nitrogen doping amount (selective adsorption) in the carbon materials. This work provides insight into the mechanism of the molten salt-coupled activation strategy, offering new ideas for the targeted design of high-performance CDI biomass carbon materials.

Research progress of Mn-based low-temperature SCR denitrification catalysts.

Selective catalytic reduction (SCR) is a efficiently nitrogen oxides removal technology from stationary source flue gases. Catalysts are key component in the technology, but currently face problems including poor low-temperature activity, narrow temperature windows, low selectivity, and susceptibility to water passivation and sulphur dioxide poisoning. To develop high-efficiency low-temperature denitrification activity catalyst, manganese-based catalysts have become a focal point of research globally for low-temperature SCR denitrification catalysts. This article investigates the denitrification efficiency of unsupported manganese-based catalysts, exploring the influence of oxidation valence, preparation method, crystallinity, crystal form, and morphology structure. It examines the catalytic performance of binary and multicomponent unsupported manganese-based catalysts, focusing on the use of transition metals and rare earth metals to modify manganese oxide. Furthermore, the synergistic effect of supported manganese-based catalysts is studied, considering metal oxides, molecular sieves, carbon materials, and other materials (composite carriers and inorganic non-metallic minerals) as supports. The reaction mechanism of low-temperature denitrification by manganese-based catalysts and the mechanism of sulphur dioxide/water poisoning are analysed in detail, and the development of practical and efficient manganese-based catalysts is considered.

An Oriented Diffusion Strategy to Configure All-Region Ultrahigh-Density Metal Single Atoms for High-Capacity Sodium Storage.

Single-atom metals (SAMs), despite being promising for high-utilization catalysis, biomedicine, and energy storage, usually suffer from limited catalytic performance caused by low metal loading. Herein, via an oriented diffusion strategy, all-region ultrahigh-loading (18.9wt.%) Sn-SAMs over carbon nanorings matrix (Sn-SAMs@CNR) are initially achieved based on the transformation of a g-C3N4@SnO2@polydopamine ring-like nested structure. The formation process of Sn-SAMs involves a critical conversion from oxygen-coordination (SnO2) to nitrogen-coordination (Sn-N4) and simultaneous anti-Osterwalder ripening promoted under spatial confinement. Notably, the g-C3N4-derived N-containing gaseous intermediates dynamically drive the oriented diffusion (inside-out diffusion) of Sn-SAMs across the carbon nanorings, realizing an all-region ultrahigh loading of SAMs throughout the carbon matrix. This strategy is also applied to other metal materials (Fe, Co, Ni, Cu, and Sb), and features excellent universality. When applied as the anode for sodium-ion batteries, experimental analyses and theoretical calculations demonstrate that high-loading Sn-N4 active sites significantly optimize electron density distribution and improve reaction kinetics. Consequently, Sn-SAMs@CNR exhibits outstanding durability of 364mAhg-1 even after 5000 cycles with an impressively low (0.00068%) capacity decay per cycle. This work opens up a universally new avenue for all-region ultrahigh loading of SAMs to carbon matrix for high-performance energy storage.

Modulating electronic by construction WS2/WN heterostructure coupled with N-doped carbon to boost alkaline seawater hydrogen production

The development of an efficient and durable non-precious electrocatalyst for alkaline seawater electrolysis is of great significance. Herein, two-dimensional (2D) lamellar heterostructure WS2/WN was dispersed on the carbon matrix (marked as WS2/WN@CM). The obtained WS2/WN@CM catalysts demonstrate exceptional performance in the hydrogen evolution reaction (HER) in alkaline freshwater (1.0 M KOH), alkaline simulated seawater (1.0 M KOH + 0.5 M NaCl) and alkaline natural seawater (1.0 M KOH + seawater), respectively, which achieved a low overpotential (92 mV, 95 mV and 113 mV) at 10 mA cm−2 and outstanding long-term durability at 200 mA cm−2 for 100 h. The catalyst benefits from the 3D carbon skeleton, which not only effectively prevents stacking of the 2D lamellar WS2/WN to fully utilize the active material, but also provides rapid electron transport. Moreover, stress effects at WS2/WN interfaces lead to distortions of torsion angles in the WS2 lattice, thereby increasing crystal surface defects accompanied by an enhancement of electrical conductivity. Density functional theory (DFT) calculations combined with XPS evidence confirm the electronic structure reorganization of WS2/WN at interfaces, which optimizes the adsorption energy of specific intermediates. Additionally, WN captures many electrons from WS2, so the WN region favors the reduction reaction and thus enhances the HER process.

In-situ nitrogen-doped porous carbon derived from penicillin mycelial residue for CO2 adsorption and adsorption mechanism investigation

The in-situ nitrogen-doped porous carbon materials was synthesized using penicillin mycelial residue (PMR) as the sole endogenous nitrogen-rich precursor through a two-step process applied for CO2 adsorption. Precise control over the structural properties and CO2 adsorption performance of the porous carbon was achieved by varying the KOH dosage and activation temperature. The porous carbon prepared under mild activation conditions (600 ℃, KOH/BC = 1) exhibited high nitrogen content and abundant ultramicroporous structures (pore size ≤ 0.7 nm), and demonstrated outstanding adsorption performance. The CO2 adsorption capacities reached 6.55 mmol/g at 0 ℃ and 3.48 mmol/g at 25 ℃, showing promising CO2/N2 selectivity and robust cyclic adsorption stability. Quantitative structure–activity relationship analysis displayed a strong correlation between adsorption density, CO2/N2 selectivity, and nitrogen content. Density functional theory calculations further confirmed that nitrogen-doping, especially pyrrolic-N, serves as favorable structural sites for CO2 adsorption. Additionally, Grand Canonical Monte Carlo simulations verified that the ultramicroporous structures significantly enhances CO2 adsorption due to their strong affinity for CO2. This study provides an economic strategy for the preparation of in-situ nitrogen-doped porous carbon with enriched micropore using PMR, highlighting their promising performances in CO2 adsorption, synchronously extending the harmless treatment and resource utilization of PMR to demonstrate a sustainable approach for environmental remediation.

Modified Biochar Materials From Eucalyptus globulus Wood as Efficient CO2 Adsorbents and Recyclable Catalysts

AbstractHighly porous carbon materials derived from renewable resources constitute a promising and sustainable strategy regarding the enhancement of CO2 capture technologies. In this work, the valorization of Eucalyptus globulus wood, a forest invasive species present in European forests, is performed through its transformation in biochar. The deposition of nitrogen and different metals (aluminum, copper and chromium) onto biochar is performed, using the magnetron sputtering as a pioneering technique, to produce coated biochar nanoparticles with improved properties. The resultant modified biochar particles maintain a highly porous structure and present a remarkable CO2 adsorption capacity (up to 4.80 mmol g−1 for N@BC), which is attributed to the synergy of their large total surface area (527 m2 g−1) and microporosity (pore diameter = 21 Å), with a high content of nitrogen and oxygen heteroatom moieties (40.4% N, 11.4% O). Their application as heterogeneous bifunctional catalysts in CO2 cycloaddition to epichlorohydrin is performed, in the absence of any solvent or co‐catalyst, under moderate conditions (20 bar CO2, 120 °C), leading to good conversions (up to 58% conversion) and excellent selectivity for cyclic carbonates. Cu‐coated biochar is shown to be more stable than non‐modified material, being recycled and reused along 4 consecutive runs without loss of catalytic activity or selectivity.

Cauliflower-like Ni/NiCoP@Boron-doped diamond composite electrodes for high-performance symmetric supercapacitors

Due to the lack of electrocatalytic active sites, the supercapacitors (SCs) even based on the most stable sp3 carbon material (Boron-doped diamond) suffer from poor capacitance and low energy density. Herein, a cauliflower-like biphasic Ni/NiCoP layer has been successfully deposited on the BDD film and further applied as binder-/current collector-free SC electrodes. In a redox-active aqueous electrolyte (0.05 M Fe(CN)63−/4− + 1.0 M KOH), the Ni/NiCoP@BDD electrode with exceptional cyclic stability (∼89.0 % after 10,000 cycles) delivers a specific capacitance of 256.1 mF cm−2 at a current density of 30 mA cm−2, about 2 times higher than that in inert electrolyte. Furthermore, such a symmetric PC device provides a desired energy density of 70.0 Wh kg−1 at a high power density of 3601 W kg−1.

Assessment of Edge Modification of Nanographene.

Carboxy groups on the edges of nanographene (NG) enable functionalization for realizing NG-organic hybrid materials. Therefore, assessment of the edge-functionalization of the electronic structures of NGs is valuable for the rational design of functional carbon materials. In this study, the structures of model NGs comprising 174 carbon atoms with armchair edges and various functional groups at the edges were computed. To achieve the greatest possible similarity between the computed structure and the real one, the carbon framework was designed based on experimental observations. The functional groups can be accessed via suitable chemical reactions. The computations predicted that although the conversion of carboxyl groups with electron-withdrawing/donating groups influences the orbital energies, the HOMO-LUMO (H-L) gap is not significantly affected, except in a few cases. Among the evaluated examples, π-extension had the greatest influence on the H-L gap. Interestingly, for the Pd2+-coordinated NG, the participation of the low-lying LUMO localized on Pd2+ in the surface-to-metal transitions seemingly narrowed the H-L gap, and a surface-to-ligand transition was observed.