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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: closed (31 January 2021) | Viewed by 41910

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Prof. Dr. Jana Vejpravová

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Guest Editor

Department of Condensed Matter Physics, Faculty of Mathematics and Physics, Charles University, 121 16 Prague 2, Czech Republic
Interests: low-dimensional magnetism; X-ray and neutron scattering techniques; spin- and chirality-resolved spectroscopies and microscopies; nanocarbons; 2D materials and van der Waals heterostructures

Special Issue Information

Dear Colleagues,

The current requirements of modern society are closely associated with rapidly growing demands for technological advances in many areas, which are directly related to the quality of life, especially human health and environmental sustainability. Rational design and directed modification of matter represent the major challenge in the development of new generation of high-impact functional materials. In this context, the most versatile element is the carbon that forms stable allotrope graphite with sp² hybridization of carbon atoms in a strictly planar configuration of aromatic character, and under normal conditions, a metastable diamond with sp³ tetrahedral environment. Both forms of carbon, however, exhibit extraordinary physical and chemical properties at nanoscale, which have been massively inspiring both basic and applied sciences. The willingness of nanocarbons to undergo a plethora of on-surface chemical reactions and strong noncovalent interactions gives a unique opportunity to establish communication channels between the different carbon allotropes and other active components, giving rise to smart nanocomposite and hybrid materials.

The present Special Issue will focus on the most recent advances in rational design, preparation and advanced characterization of materials based on nanocarbons, including nanocomposites and hybrids for energy storage and biomedicine.

Researchers are warmly invited to submit results of their experimental and theoretical research as original research articles on novel nanomaterials, nanocomposites, and hybrids based on sp² and/or sp³ forms of carbon. I also sincerely invite scholars working in the research area of graphene, carbon nanotubes, and nanodiamonds and their composites and hybrids to contribute review articles to this Special Issue in order to deliver the recent advancements in the field of nanocarbon-based materials to the broad readership of the Nanomaterials journal.

Dr. Jana Vejpravová
Guest Editor

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Keywords

nanocarbons including graphene, carbon nanotubes and nanodiamonds
nanocarbon-based composites
nanocarbon-based hybrids
nanocarbon-based materials for energy storage
nanocarbon-based materials for biomedicine
advanced structural characterization of nanocarbons
magnetism of nanocarbons
advanced spectroscopies of nanocarbon-based materials

Published Papers (11 papers)

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Research

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12 pages, 4379 KiB

Open AccessArticle

Scalable Graphene Defect Prediction Using Transferable Learning

by Bowen Zheng, Zeyu Zheng and Grace X. Gu

Nanomaterials 2021, 11(9), 2341; https://doi.org/10.3390/nano11092341 - 9 Sep 2021

Cited by 3 | Viewed by 2337

Abstract

Notably known for its extraordinary thermal and mechanical properties, graphene is a favorable building block in various cutting-edge technologies such as flexible electronics and supercapacitors. However, the almost inevitable existence of defects severely compromises the properties of graphene, and defect prediction is a difficult, yet important, task. Emerging machine learning approaches offer opportunities to predict target properties such as defect distribution by exploiting readily available data, without incurring much experimental cost. Most previous machine learning techniques require the size of training data and predicted material systems of interest to be identical. This limits their broader application, because in practice a newly encountered material system may have a different size compared with the previously observed ones. In this paper, we develop a transferable learning approach for graphene defect prediction, which can be used on graphene with various sizes or shapes not seen in the training data. The proposed approach employs logistic regression and utilizes data on local vibrational energy distributions of small graphene from molecular dynamics simulations, in the hopes that vibrational energy distributions can reflect local structural anomalies. The results show that our machine learning model, trained only with data on smaller graphene, can achieve up to 80% prediction accuracy of defects in larger graphene under different practical metrics. The present research sheds light on scalable graphene defect prediction and opens doors for data-driven defect detection for a broad range of two-dimensional materials. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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15 pages, 3761 KiB

Open AccessArticle

Waffle-Like Carbons Combined with Enriched Mesopores and Highly Heteroatom-Doped Derived from Sandwiched MOF/LDH/MOF for High-Rate Supercapacitor

by Szu-Chen Wu, Po-Hsueh Chang, Syun-Hong Chou, Chih-Yang Huang, Ta-Chung Liu and Cheng-Hsiung Peng

Nanomaterials 2020, 10(12), 2388; https://doi.org/10.3390/nano10122388 - 30 Nov 2020

Cited by 18 | Viewed by 3412

Abstract

Supercapacitors (SCs) are promising for powering mobile devices, electric vehicles and smart power grids due to their fast charge/discharge rate, high power capability and robust cycle stability. Nitrogen-doped porous carbons are great alternatives because they provide pseudocapacitance without losing their power rate. Nanoporous carbon derived from metal organic frameworks (MOFs) is an ideal precursor for preparing heteroatom-doped carbons due to their abundant nitrogen contents and incredible specific surface areas. However, severe aggregations and the leakage of nitrogen can occur during harsh carbonization. In this study, we used CoAl-LDH (cobalt aluminum layered double hydroxide) as an in-situ growth substrate, allowing Co-based MOF to uniformly grow onto the CoAl-LDH to form a sandwiched MOF/LDH/MOF structure. After acid etching, we obtained waffle-like nanoporous carbons (WNPC). WNPC exhibited high nitrogen and oxygen retention (7.5 wt% and 9.1 wt%) and a broad mesopores distribution with specific surface areas of 594 m²g⁻¹, which promoted a sieving effect. This renders a specific capacitance of 300.7 F·g⁻¹ at 1 A·g⁻¹ and the high retention (72%) of capacitance at 20 A·g⁻¹, ensuring its use at high-rate supercapacitor electrodes. Finally, the WNPC symmetric supercapacitor reaches a superior specific energy of 27 W·h·kg⁻¹ at a power of 500 W·kg⁻¹, and a good cycle stability (85% capacitance retention after 10,000 cycles). Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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13 pages, 1995 KiB

Open AccessArticle

Room-Temperature Reduction of Graphene Oxide in Water by Metal Chloride Hydrates: A Cleaner Approach for the Preparation of Graphene@Metal Hybrids

by Patrick. P. Brisebois, Ricardo Izquierdo and Mohamed Siaj

Nanomaterials 2020, 10(7), 1255; https://doi.org/10.3390/nano10071255 - 28 Jun 2020

Cited by 3 | Viewed by 2236

Abstract

Headed for developing minimalistic strategies to produce graphene@metal hybrids for electronics on a larger scale, we discovered that graphene oxide (GO)-metal oxide (MO) hybrids are formed spontaneously in water at room temperature in the presence of nothing else than graphene oxide itself and metal ions. Our observations show metal oxide nanoparticles decorating the surface of graphene oxide with particle diameter in the range of 10–40 nm after only 1 h of mixing. Their load ranged from 0.2% to 6.3% depending on the nature of the selected metal. To show the generality of the reactivity of GO with different ions in standard conditions, we prepared common hybrids with GO and tin, iron, zinc, aluminum and magnesium. By means of carbon-13 solid-state nuclear magnetic resonance using magic angle spinning, we have found that graphene oxide is also moderately reduced at the same time. Our method is powerful and unique because it avoids the use of chemicals and heat to promote the coprecipitation and the reduction of GO. This advantage allows synthesizing GO@MO hybrids with higher structural integrity and purity with a tunable level of oxidization, in a faster and greener way. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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13 pages, 3078 KiB

Open AccessArticle

Controllable Carbonization of Plastic Waste into Three-Dimensional Porous Carbon Nanosheets by Combined Catalyst for High Performance Capacitor

by Xueying Mu, Yunhui Li, Xiaoguang Liu, Changde Ma, Hanqing Jiang, Jiayi Zhu, Xuecheng Chen, Tao Tang and Ewa Mijowska

Nanomaterials 2020, 10(6), 1097; https://doi.org/10.3390/nano10061097 - 2 Jun 2020

Cited by 34 | Viewed by 4018

Abstract

Polyethylene terephthalate (PET) plastic has been extensively used in our social life, but its poor biodegradability has led to serious environmental pollution and aroused worldwide concern. Up to now, various strategies have been proposed to address the issue, yet such strategies remain seriously impeded by many obstacles. Herein, waste PET plastic was selectively carbonized into three-dimensional (3D) porous carbon nanosheets (PCS) with high yield of 36.4 wt%, to be further hybridized with MnO₂ nanoflakes to form PCS-MnO₂ composites. Due to the introduction of an appropriate amount of MnO₂ nanoflakes, the resulting PCS-MnO₂ composite exhibited a specific capacitance of 210.5 F g⁻¹ as well as a high areal capacitance of 0.33 F m⁻². Furthermore, the PCS-MnO₂ composite also showed excellent cycle stability (90.1% capacitance retention over 5000 cycles under a current density of 10 A g⁻¹). The present study paved an avenue for the highly efficient recycling of PET waste into high value-added products (PCSs) for electrochemical energy storage. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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15 pages, 4164 KiB

Open AccessArticle

Tuning Properties of Partially Reduced Graphene Oxide Fibers upon Calcium Doping

by Krzysztof Tadyszak, Jacek K. Wychowaniec, Karol Załęski, Emerson Coy, Łukasz Majchrzycki and Raanan Carmieli

Nanomaterials 2020, 10(5), 957; https://doi.org/10.3390/nano10050957 - 18 May 2020

Cited by 4 | Viewed by 3763

Abstract

The arrangement of two-dimensional graphene oxide sheets has been shown to influence physico-chemical properties of the final bulk structures. In particular, various graphene oxide microfibers remain of high interest in electronic applications due to their wire-like thin shapes and the ease of hydrothermal fabrication. In this research, we induced the internal ordering of graphene oxide flakes during typical hydrothermal fabrication via doping with Calcium ions (~6 wt.%) from the capillaries. The Ca²⁺ ions allowed for better graphene oxide flake connections formation during the hydrogelation and further modified the magnetic and electric properties of structures compared to previously studied aerogels. Moreover, we observed the unique pseudo-porous fiber structure and flakes connections perpendicular to the long fiber axis. Pulsed electron paramagnetic resonance (EPR) and conductivity measurements confirmed the denser flake ordering compared to previously studied aerogels. These studies ultimately suggest that doping graphene oxide with Ca²⁺ (or other) ions during hydrothermal methods could be used to better control the internal architecture and thus tune the properties of the formed structures. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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13 pages, 3579 KiB

Open AccessArticle

Unraveling Origins of EPR Spectrum in Graphene Oxide Quantum Dots

by Krzysztof Tadyszak, Andrzej Musiał, Adam Ostrowski and Jacek K. Wychowaniec

Nanomaterials 2020, 10(4), 798; https://doi.org/10.3390/nano10040798 - 21 Apr 2020

Cited by 12 | Viewed by 4202

Abstract

Carbon nanostructures are utilized in a plethora of applications ranging from biomedicine to electronics. Particularly interesting are carbon nanostructured quantum dots that can be simultaneously used for bimodal therapies with both targeting and imaging capabilities. Here, magnetic and optical properties of graphene oxide quantum dots (GOQDs) prepared by the top-down technique from graphene oxide and obtained using the Hummers’ method were studied. Graphene oxide was ultra-sonicated, boiled in HNO₃, ultra-centrifuged, and finally filtrated, reaching a mean flake size of ~30 nm with quantum dot properties. Flake size distributions were obtained from scanning electron microscopy (SEM) images after consecutive preparation steps. Energy-dispersive X-ray (EDX) confirmed that GOQDs were still oxidized after the fabrication procedure. Magnetic and photoluminescence measurements performed on the obtained GOQDs revealed their paramagnetic behavior and broad range optical photoluminescence around 500 nm, with magnetic moments of 2.41 µ_B. Finally, electron paramagnetic resonance (EPR) was used to separate the unforeseen contributions and typically not taken into account metal contaminations, and radicals from carbon defects. This study contributes to a better understanding of magnetic properties of carbon nanostructures, which could in the future be used for the design of multimodal imaging agents. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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10 pages, 1910 KiB

Open AccessArticle

Transferless Inverted Graphene/Silicon Heterostructures Prepared by Plasma-Enhanced Chemical Vapor Deposition of Amorphous Silicon on CVD Graphene

by Martin Müller, Milan Bouša, Zdeňka Hájková, Martin Ledinský, Antonín Fejfar, Karolina Drogowska-Horná, Martin Kalbáč and Otakar Frank

Nanomaterials 2020, 10(3), 589; https://doi.org/10.3390/nano10030589 - 24 Mar 2020

Cited by 3 | Viewed by 2728

Abstract

The heterostructures of two-dimensional (2D) and three-dimensional (3D) materials represent one of the focal points of current nanotechnology research and development. From an application perspective, the possibility of a direct integration of active 2D layers with exceptional optoelectronic and mechanical properties into the existing semiconductor manufacturing processes is extremely appealing. However, for this purpose, 2D materials should ideally be grown directly on 3D substrates to avoid the transferring step, which induces damage and contamination of the 2D layer. Alternatively, when such an approach is difficult—as is the case of graphene on noncatalytic substrates such as Si—inverted structures can be created, where the 3D material is deposited onto the 2D substrate. In the present work, we investigated the possibility of using plasma-enhanced chemical vapor deposition (PECVD) to deposit amorphous hydrogenated Si (a-Si:H) onto graphene resting on a catalytic copper foil. The resulting stacks created at different Si deposition temperatures were investigated by the combination of Raman spectroscopy (to quantify the damage and to estimate the change in resistivity of graphene), temperature-dependent dark conductivity, and constant photocurrent measurements (to monitor the changes in the electronic properties of a-Si:H). The results indicate that the optimum is 100 °C deposition temperature, where the graphene still retains most of its properties and the a-Si:H layer presents high-quality, device-ready characteristics. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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18 pages, 5083 KiB

Open AccessArticle

Comparative Study of Synthesis Methods to Prepare New Functionalized Adsorbent Materials Based on MNPs–GO Coupling

by Pablo Montoro-Leal, Juan Carlos García-Mesa, María del Mar López Guerrero and Elisa Vereda Alonso

Nanomaterials 2020, 10(2), 304; https://doi.org/10.3390/nano10020304 - 11 Feb 2020

Cited by 6 | Viewed by 2351

Abstract

In this work, the synthesis of new adsorbent nanomaterials based on the coupling of magnetic nanoparticles and graphene oxide (MNPs–GO) was addressed. Separately, MNPs and GO have adsorbent properties of great interest, but their use involves certain difficulties. The coupling seeks compensation for their disadvantages, while maintaining their excellent properties. Three different routes to synthesize coupled MNPs–GO were studied and are compared in this work. The three synthesized materials were functionalized with chelating groups: [1,5-bis (di-2-pyridyl) methylene] thiocarbonohydrazide (DPTH) and [1,5-bis(2-pyridyl)3-sulfophenylmethylene] thiocarbonohydrazide (PSTH). The new adsorbent nanomaterials were characterized adequately. Moreover, their capacities of adsorption toward heavy and noble metals were determined, in order to apply them as extractants in magnetic solid-phase extraction to preconcentrate metals in environmental samples. The results showed that one of the routes provided nanomaterials with better adsorbent characteristics and higher yields of functionalization. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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8 pages, 2811 KiB

Open AccessArticle

A Novel Route to High-Quality Graphene Quantum Dots by Hydrogen-Assisted Pyrolysis of Silicon Carbide

by Na Eun Lee, Sang Yoon Lee, Hyung San Lim, Sung Ho Yoo and Sung Oh Cho

Nanomaterials 2020, 10(2), 277; https://doi.org/10.3390/nano10020277 - 6 Feb 2020

Cited by 16 | Viewed by 3151

Abstract

Graphene quantum dots (GQDs) can be highly beneficial in various fields due to their unique properties, such as having an effective charge transfer and quantum confinement. However, defects on GQDs hinder these properties, and only a few studies have reported fabricating high-quality GQDs with high crystallinity and few impurities. In this study, we present a novel yet simple approach to synthesizing high-quality GQDs that involves annealing silicon carbide (SiC) under low vacuum while introducing hydrogen (H) etching gas; no harmful chemicals are required in the process. The fabricated GQDs are composed of a few graphene layers and possess high crystallinity, few defects and high purity, while being free from oxygen functional groups. The edges of the GQDs are hydrogen-terminated. High-quality GQDs form on the etched SiC when the etching rates of Si and C atoms are monitored. The size of the fabricated GQDs and the surface morphology of SiC can be altered by changing the operating conditions. Collectively, a novel route to high-quality GQDs will be highly applicable in fields involving sensors and detectors. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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Review

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14 pages, 4400 KiB

Open AccessReview

Fabrication Techniques for Graphene Oxide-Based Molecular Separation Membranes: Towards Industrial Application

by Ohchan Kwon, Yunkyu Choi, Eunji Choi, Minsu Kim, Yun Chul Woo and Dae Woo Kim

Nanomaterials 2021, 11(3), 757; https://doi.org/10.3390/nano11030757 - 17 Mar 2021

Cited by 50 | Viewed by 6624

Abstract

Graphene oxide (GO) has been a prized material for fabricating separation membranes due to its immense potential and unique chemistry. Despite the academic focus on GO, the adoption of GO membranes in industry remains elusive. One of the challenges at hand for commercializing GO membranes lies with large-scale production techniques. Fortunately, emerging studies have acknowledged this issue, where many have aimed to deliver insights into scalable approaches showing potential to be employed in the commercial domain. The current review highlights eight physical methods for GO membrane fabrication. Based on batch-unit or continuous fabrication, we have further classified the techniques into five small-scale (vacuum filtration, pressure-assisted filtration, spin coating, dip coating, drop-casting) and three large-scale (spray coating, bar/doctor blade coating, slot die coating) approaches. The continuous nature of the large-scale approach implies that the GO membranes prepared by this method are less restricted by the equipment’s dimensions but rather the availability of the material, whereas membranes yielded by small-scale methods are predominately limited by the size of the fabrication device. The current review aims to serve as an initial reference to provide a technical overview of preparing GO membranes. We further aim to shift the focus of the audience towards scalable processes and their prospect, which will facilitate the commercialization of GO membranes. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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36 pages, 7522 KiB

Open AccessReview

A Review of Strategies for the Synthesis of N-Doped Graphene-Like Materials

by Alenka Vesel, Rok Zaplotnik, Gregor Primc and Miran Mozetič

Nanomaterials 2020, 10(11), 2286; https://doi.org/10.3390/nano10112286 - 18 Nov 2020

Cited by 42 | Viewed by 6106

Abstract

Methods for synthesizing nitrogen-doped graphene-like materials have attracted significant attention among the scientific community because of the possible applications of such materials in electrochemical devices such as fuel cells, supercapacitors and batteries, as well as nanoelectronics and sensors. The aim of this paper is to review recent advances in this scientific niche. The most common synthesis technique is nitridization of as-deposited graphene or graphene-containing carbon mesh using a non-equilibrium gaseous plasma containing nitrogen or ammonia. A variety of chemical bonds have been observed, however, it is still a challenge how to ensure preferential formation of graphitic nitrogen, which is supposed to be the most favorable. The nitrogen concentration depends on the processing conditions and is typically few at.%; however, values below 1 and up to 20 at.% have been reported. Often, huge amounts of oxygen are found as well, however, its synergistic influence on N-doped graphene is not reported. The typical plasma treatment time is several minutes. The results reported by different authors are discussed, and future needs in this scientific field are summarized. Some aspects of the characterization of graphene samples with X-ray photoelectron spectroscopy and Raman spectroscopy are presented as well. Full article

(This article belongs to the Special Issue Nanocarbon Based Materials)

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