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The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "2D and Carbon Nanomaterials".

Deadline for manuscript submissions: 25 July 2026 | Viewed by 7563

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Special Issue Editor

Dr. Silvia Villar-Rodil

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Instituto de Ciencia y Tecnología del Carbono (INCAR), Consejo Superior de Investigaciones Científicas (CSIC), C/Francisco Pintado Fe, 26, 33011 Oviedo, Asturias, Spain
Interests: 2D materials; graphene; layered transition metal dichalcogenides (LTMD); molybdenum disulfide (MoS₂); porous carbon materials; materials characterization; XPS spectroscopy; energy storage

Special Issue Information

Dear Colleagues,

The surface chemistry of graphene and graphene oxide (GO) is a fascinating field of research, and one whose development is required to realise the great potential of graphene. Indeed, much effort has been and continues to be devoted to the functionalization of graphene and its derivatives. One of the reasons for this endeavor is that graphene in its pristine form is both inert to reaction and a zero-band gap conductor, which lowers its competitiveness for applications such as sensors and semiconductors. The strategies developed include, amongst others, covalent and non-covalent functionalization with organic and inorganic molecules, as well as band gap opening of graphene by doping, intercalation, and striping. In general, any application of graphene and GO will undoubtedly benefit from the controlled synthesis of defined derivatives. Although, at present, the full potential of graphene derivatives has not yet been exploited, multidisciplinary collaboration of researchers is expected to drive technology forward. Many questions remain in this field of research. For example, while in the chemical synthesis of any new compound, isolation and unambiguous structural characterization are key steps, these are very difficult goals in the case of graphene. This is due to the polydispersity, polyfunctionality and often poor solubility of the derivatives prepared. Indeed, classical methods used by synthetic chemists for decades to isolate and characterize new molecules have a limited applicability in the case of graphene and GO. Therefore, in addition to the development of successful methodologies for the functionalization of graphene and GO, new analytical tools for a satisfactory characterization of structure have to be elaborated and applied to these materials.

It is my pleasure to invite you to submit a manuscript for this Special Issue whose objective is to create a collection of papers addressing critical aspects and the latest developments in the field of graphene and GO chemistry. Full papers, short communications, and reviews are welcome.

Dr. Silvia Villar-Rodil
Guest Editor

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Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 250 words) can be sent to the Editorial Office for assessment.

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Keywords

graphene
graphene oxide
chemistry

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Published Papers (5 papers)

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Research

21 pages, 2810 KB

Open AccessArticle

Graphite Oxide and Reduced Graphite Oxide Models to Reveal the Contribution of Carbon Texture and Surface Chemistry to Hydrogen Storage and Li-Ion Battery Anode Performance

by Anna Bulátkó, Lakshmi Shiva Shankar, Szilvia Klébert, Attila Farkas, Miklós Mohai, György Sáfrán, Róbert Kun and Krisztina László

Nanomaterials 2026, 16(1), 19; https://doi.org/10.3390/nano16010019 - 23 Dec 2025

Viewed by 1018

Abstract

After being an indispensable intermediate in the oxidative exfoliation route towards graphene, graphene oxide has gained its deserved value in materials science for numerous applications, from catalysis, through energy storage and conversion, to sensor use. In this work, three graphene oxides of tuned morphology and chemistry are used as a simplified model for porous carbon materials in hydrogen storage and as a Li-ion battery anode. The BET surface areas were, respectively, 9, 13, and 535 m²/g, while the corresponding O/C values from the X-ray photoelectron spectroscopy were 0.51, 0.17, and 0.12. Additionally, the samples were thoroughly characterized using scanning and transmission electron imaging, powder X-ray diffraction, thermal stability, and Raman and Fourier transform infrared spectroscopic methods. Hydrogen adsorption isotherms (−196 °C) and their comparison with nitrogen uptake revealed that pore accessibility, porous confinement, and surface chemistry, i.e., both morphology and surface chemistry, contribute to efficient adsorption. In the anode application, by contrast, surface chemistry was the single most defining factor for performance. Full article

(This article belongs to the Special Issue The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide)

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16 pages, 2528 KB

Open AccessArticle

Magnetic Properties of Nitrogen-Doped Graphene Induced by Dopant Configurations

by Madhuparna Chakraborty, Gregory Jensen, David C. Ingram, Eric Stinaff and Wojciech M. Jadwisienczak

Nanomaterials 2025, 15(22), 1694; https://doi.org/10.3390/nano15221694 - 9 Nov 2025

Cited by 1 | Viewed by 1501

Abstract

In this study, we experimentally demonstrate that the magnetic properties of nitrogen-doped graphene (NG) are influenced by the configuration of nitrogen dopants, namely graphitic, pyridinic, and pyrrolic, along with the overall nitrogen concentration. The NG materials were prepared via a two-step thermal treatment process. The first step involved heating in ammonia at 400 °C, followed by a second post-annealing step at 600 °C. Scanning Electron Microscopy–Energy Dispersive X-ray Spectroscopy (SEM–EDS) analysis performed at 25 μm resolution confirmed uniform elemental distribution across the samples. X-ray photoelectron spectroscopy (XPS) revealed that while the total nitrogen content decreased from 11.9 at.% in NG to 5.5 at.% in the post-annealed sample, the ratio of graphitic to pyrrolic nitrogen increased from 0.4% to 3.8% and the ratio of graphitic to pyridinic nitrogen increased from 0.8% to 2.5%. Raman spectroscopy confirmed the presence of prominent D and G bands at ~1352 cm⁻¹ and ~1589 cm⁻¹, respectively, along with a 2D band at ~2692 cm⁻¹, indicating the presence of few-layered graphene and defect-related features. The

\frac{I_{D}}{I_{G}}

ratio increased from 1.12 to 1.27 in the post-annealed sample, indicating increased disorder after annealing. Magnetic characterization showed a marked enhancement in the magnetic properties with increased graphitic nitrogen content. The saturation magnetization (M_s) reached 0.13 emu g⁻¹, ~42% higher than that of the material heated in ammonia, with the coercivity increasing from 40 Oe to 750 Oe. These results emphasize the pivotal role of nitrogen configuration in the graphene host, specifically the promotion of graphitic nitrogen species, in tailoring the ferromagnetic response of NG. Full article

(This article belongs to the Special Issue The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide)

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11 pages, 659 KB

Open AccessArticle

Spectrum Analysis of Thermally Driven Curvature Inversion in Strained Graphene Ripples for Energy Conversion Applications via Molecular Dynamics

by James M. Mangum, Md R. Kabir, Tamzeed B. Amin, Syed M. Rahman, Ashaduzzaman and Paul M. Thibado

Nanomaterials 2025, 15(17), 1332; https://doi.org/10.3390/nano15171332 - 29 Aug 2025

Cited by 2 | Viewed by 1338

Abstract

The extraordinary mechanical flexibility, high electrical conductivity, and nanoscale instability of freestanding graphene make it an excellent candidate for vibration energy harvesting. When freestanding graphene is stretched taut and subject to external forces, it will vibrate like a drum head. Its vibrations occur at a fundamental frequency along with higher-order harmonics. Alternatively, when freestanding graphene is compressed, it will arch slightly out of the plane or buckle under the load. Remaining flat under compression would be energetically too costly compared to simple bond rotations. Buckling up or down, also known as ripple formation, naturally creates a bistable situation. When the compressed system vibrates between its two low-energy states, it must pass through the high-energy middle. The greater the compression, the higher the energy barrier. The system can still oscillate but the frequency will drop far below the fundamental drum-head frequency. The low frequencies combined with the large-scale movement and the large number of atoms coherently moving are key factors addressed in this study. Ten ripples with increasing compressive strain were built, and each was studied at five different temperatures. Increasing the temperature has a similar effect as increasing the compressive strain. Analysis of the average time between curvature inversion events allowed us to quantify the energy barrier height. When the low-frequency bistable data were time-averaged, the authors found that the velocity distribution shifts from the expected Gaussian to a heavy-tailed Cauchy (Lorentzian) distribution, which is important for energy harvesting applications. Full article

(This article belongs to the Special Issue The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide)

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17 pages, 3417 KB

Open AccessEditor’s ChoiceArticle

Graphene/Zirconia Composites for Components in Solid Oxide Fuel Cells: Microstructure and Electrical Conductivity

by Francisco J. Coto-Ruiz, Ana de la Cruz-Blanco, Rocío Moriche, Ana Morales-Rodríguez and Rosalía Poyato

Nanomaterials 2025, 15(17), 1314; https://doi.org/10.3390/nano15171314 - 26 Aug 2025

Cited by 1 | Viewed by 1509

Abstract

In this paper, 8 mol% yttria cubic stabilized zirconia (8YCSZ) composites with reduced graphene oxide (rGO) contents up to 10 vol% were consolidated by spark plasma sintering (SPS) at two different temperatures with the aim of evaluating the relationship of their electrical properties with the graphene content, the rGO crystallinity, and the microstructural features. Successful in situ reduction of GO was accomplished during SPS, and highly densified composites with homogeneous rGO distribution, even at the highest contents, were obtained. The electrical properties were analyzed using impedance spectroscopy. Measurements were taken up to 700 °C, revealing an inductive response for the composites with 5 and 10 vol% rGO and a capacitive response for the composites with 1 and 2.5 vol% rGO. The results indicate that, along with the ionic conduction typical of zirconia, there are additional polarization mechanisms associated with the presence of graphene at ceramic grain boundaries that substantially modify the impedance response. A minor electronic conductivity contribution was identified in the composites below the percolation threshold. These characteristics make the 8YCSZ composites promising candidates for application as SOFC components, as ceramic interconnects when the graphene content is above the percolation threshold, or as electrolytes when the graphene content is below this limit. Full article

(This article belongs to the Special Issue The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide)

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18 pages, 7323 KB

Open AccessArticle

Graphene Oxide-Doped CNT Membrane for Dye Adsorption

by Mariafrancesca Baratta, Fiore Pasquale Nicoletta and Giovanni De Filpo

Nanomaterials 2025, 15(11), 782; https://doi.org/10.3390/nano15110782 - 22 May 2025

Cited by 7 | Viewed by 1451

Abstract

Recently, graphene oxide (GO) has been largely investigated as a potential adsorbent towards dyes. However, the major obstacle to its full employment is linked to its natural powder consistence, which greatly complexifies the operations of recovery and reuse. With the aim to overcome this issue, the present work reports on the design of GO-modified carbon nanotubes buckypapers (BPs), in which the main component, GO, is entirely entrapped in the BP grid generated by CNTs for the double purpose of (a) increasing adsorption performance of GO-BPs and (b) ensure a fast process of regeneration and reuse. Adsorption experiments were performed towards several dyes: Acid Blue 29 (AB29), Crystal Violet (CV), Eosyn Y (EY), Malachite Green (MG), and Rhodamine B (RB) (C_i = 50 ppm, pH = 6). Results demonstrated that adsorption is strictly dependent on the charge occurring both on GO-BP and dye surfaces, observing great adsorption capacities towards MG (493.44 mg g⁻¹), RB (467.35 mg g⁻¹), and CV (374.53 mg g⁻¹), due to the best coupling of dye cationic form with negative GO-BP surface. Adsorption isotherms revealed that dyes capture onto GO-BPs is thermodynamically favored (ΔG < 0), becoming more negative at 313 K. Kinetic studies evidenced that the process can be described through a pseudo-first-order model, with MG, RB, and CV exhibiting the highest values of k₁. In view of these results, the following trend in GO-BP adsorption performance has been derived: MG ≈ RB > CV > AB29 > EY. Full article

(This article belongs to the Special Issue The 15th Anniversary of Nanomaterials–Surface Chemistry of Graphene and Graphene Oxide)

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