Electrochemical Formation of a Covalent–Ionic Stage-1 Graphite Intercalation Compound with Trifluoroacetic Acid

Gurzęda, Bartosz; Kim, Tae-In; Arsakay, Madi; Choe, Myeonggi; Lee, Sun Hwa; Lee, Zonghoon; Min, Seung Kyu; Ruoff, Rodney S.

doi:10.1021/acs.chemmater.1c03173

Cited by 7 publications

(3 citation statements)

References 83 publications

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“…Among various top-down approaches, electrochemical synthesis is one of the most promising approaches for the large-scale production of 2D materials with tunable properties. , Generally, it is an intercalation-assisted method for the fabrication of graphene-based layered 2D materials. During this process, guest molecules or ions can be intercalated into the graphite layers under the electric potential, weakening the van der Waals interactions between the interlayers, and facilitating further steps of graphene exfoliation. ,− Depending on the electrochemical conditions, anodic and cathodic exfoliation has been successfully implemented. For anodic intercalation, some commonly used intercalant anions include sulfate (SO 4 2– ), bisulfate (HSO 4 – ), perchlorate (ClO 4 – ), and tetrafluoroborate (BF 4 – ), in either acid or salt form. − Sulfate and bisulfate anions are the most widely used intercalants for scalable graphene exfoliation, particularly in aqueous solution of acidic (H 2 SO 4 ) or neutral inorganic salts (i.e., (NH 4 ) 2 SO 4 ). − Meanwhile, cationic intercalants such as alkylammonium (i.e., tetrabutylammonium, TBA + ) and large metal ions (i.e., Cs + ) in salt form are commonly employed ones for cathodic exfoliation in organic solvents. , More recently, dual-electrode exfoliation via alternating applied potential or simultaneous anodic and cathodic intercalation on both graphite electrodes has been developed to improve the production efficiency. , Besides, the co-intercalation of anionic complexes combining metal cations and chelating anions (i.e., [Mg(TFSI) 3 ] − ) also has shown their potential in anodic intercalation of graphite electrodes .…”

Section: Introductionmentioning

confidence: 99%

“…During this process, guest molecules or ions can be intercalated into the graphite layers under the electric potential, weakening the van der Waals interactions between the interlayers, and facilitating further steps of graphene exfoliation. 6 , 12 − 14 Depending on the electrochemical conditions, anodic and cathodic exfoliation has been successfully implemented. For anodic intercalation, some commonly used intercalant anions include sulfate (SO 4 2– ), bisulfate (HSO 4 – ), perchlorate (ClO 4 – ), and tetrafluoroborate (BF 4 – ), in either acid or salt form.…”

Section: Introductionmentioning

confidence: 99%

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Producing Bilayer Graphene Oxide via Wedge Ion-Assisted Anodic Exfoliation: Implications for Energy and Electronics

Zhang,

Sasidharan,

Shi

et al. 2023

ACS Appl. Nano Mater.

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Electrochemical synthesis has emerged as a promising approach for the large-scale production of graphene-based two-dimensional (2D) materials. Electrochemical intercalation of ions and molecules between graphite layers plays a key role in the synthesis of graphene with controllable thickness. However, there is still a limited understanding regarding the impact of intercalant molecules. Herein, we investigated a series of anionic species (i.e., ClO4 –, PF6 –, BF4 –, HSO4 –, CH3SO3 –, and TsO–) and examined their wedging process between the weakly bonded layered materials driven by electrochemistry. By combining cyclic voltammetry, X-ray diffraction (XRD), and Raman spectroscopy, along with density functional theory (DFT) calculations, we found that stage-2 graphite intercalation compounds (GICs) can be obtained through intercalation of ClO4 –, PF6 –, or BF4 – anions into the adjacent graphene bilayers. The anodic exfoliation step based on ClO4 ––GIC in (NH4)2SO4 (aq.) resulted in the formation of bilayer-rich (>57%) electrochemically exfoliated graphene oxide (EGO), with a high yield (∼85 wt %). Further, the physicochemical properties of these EGO can be readily customized through electrochemical reduction and modification with different surfactants. This versatility allows for precise tailoring of EGO, making it feasible for energy and electronic applications such as electrodes in electrochemical capacitors and functional composites in wearable electronics.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Producing Bilayer Graphene Oxide via Wedge Ion-Assisted Anodic Exfoliation: Implications for Energy and Electronics

Zhang,

Sasidharan,

Shi

et al. 2023

ACS Appl. Nano Mater.

View full text Add to dashboard Cite

show abstract

“…In Polymers 2022, 14, 732 2 of 16 addition, the dispersibility of SrGO is further enhanced by the surface modification. Surface modification is typically performed in two ways: via non-covalent interactions, such as physical adsorption [26][27][28], and covalent bonding, such as polymer-grafting [29][30][31][32]. The latter can be more target-selective and elaborately designed based on the synthetic chemistry than the former.…”

Section: Introductionmentioning

confidence: 99%

Surface Modification of Sulfur-Assisted Reduced Graphene Oxide with Poly(phenylene sulfide) for Multifunctional Nanocomposites

Choi

Kim

et al. 2022

Polymers

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The sulfur on the sulfur-assisted reduced graphene oxide (SrGO) surface provides the origin of poly(phenylene sulfide) PPS-grafting via SNAr mechanism. In-situ polymerization from sulfur on SrGO afforded surface modification of SrGO, resulting in enhanced dispersibility in PPS. The tensile strength, electrical and thermal conductivities, and flame retardancy of PPS-coated SrGO were efficiently enhanced using highly concentrated SrGO and masterbatch (MB) for industrial purposes. Three-dimensional X-ray microtomography scanning revealed that diluting MB in the PPS resin afforded finely distributed SrGO across the PPS resin, compared to the aggregated state of graphene oxide. For the samples after dilution, the thermal conductivity and flame retardancy of PPS/SrGO are preserved and typically enhanced by up to 20%. The proposed PPS/SrGO MB shows potential application as an additive for reinforced PPS due to the ease of addition during the extrusion process.

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Preferential Pyrolysis Construction of Carbon Anodes with 8400 h Lifespan for High‐Energy‐Density K‐ion Batteries

et al. 2023

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Carbonaceous materials are promising anodes for practical potassium‐ion batteries, but fail to meet the requirements for durability and high capacities at low potentials. Herein, we constructed a durable carbon anode for high‐energy‐density K‐ion full cells by a preferential pyrolysis strategy. Utilizing S and N volatilization from a π–π stacked supermolecule, the preferential pyrolysis process introduces low‐potential active sites of sp2 hybridized carbon and carbon vacancies, endowing a low‐potential “vacancy‐adsorption/intercalation” mechanism. The as‐prepared carbon anode exhibits a high capacity of 384.2 mAh g−1 (90 % capacity locates below 1 V vs. K/K+), which contributes to a high energy density of 163 Wh kg−1 of K‐ion full battery. Moreover, abundant vacancies of carbon alleviate volume variation, boosting the cycling stability over 14 000 cycles (8400 h). Our work provides a new synthesis approach for durable carbon anodes of K‐ion full cells with high energy densities.

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Electrochemical Formation of a Covalent–Ionic Stage-1 Graphite Intercalation Compound with Trifluoroacetic Acid

Cited by 7 publications

References 83 publications

Producing Bilayer Graphene Oxide via Wedge Ion-Assisted Anodic Exfoliation: Implications for Energy and Electronics

Producing Bilayer Graphene Oxide via Wedge Ion-Assisted Anodic Exfoliation: Implications for Energy and Electronics

Surface Modification of Sulfur-Assisted Reduced Graphene Oxide with Poly(phenylene sulfide) for Multifunctional Nanocomposites

Preferential Pyrolysis Construction of Carbon Anodes with 8400 h Lifespan for High‐Energy‐Density K‐ion Batteries

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