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Element-Doped Functional Carbon-based Materials

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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Carbon Materials".

Deadline for manuscript submissions: closed (30 June 2019) | Viewed by 48562

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Special Issue Editors

Prof. Dr. Francisco Carrasco-Marín

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Guest Editor

Department of Inorganic Chemistry, University of Granada, Granada, Spain
Interests: carbon materials; energy materials; electro-catalysis; energy storage; supercapacitors; heterogeneous catalysis; green chemistry and environmental chemistry
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Agustín Francisco Pérez-Cadenas

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Guest Editor

Department of Inorganic Chemistry, University of Granada, Granada, Spain
Interests: carbon materials; carbon metal composites; carbon gels; photo-catalysis; electro-catalysis; catalytic combustion; hydrogenation reactions; advanced oxidation processes
Special Issues, Collections and Topics in MDPI journals

Dr. Sergio Morales-Torres

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Guest Editor

Department of Inorganic Chemistry, University of Granada, Granada, Spain
Interests: carbon nanostructures; graphene; nanostructured metal oxide; structured catalysts and membranes; chemical functionalization; advanced oxidation processes; air/water treatment; desalination
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Carbon materials are one of the most fascinating materials because of their unique properties and potential use in several applications. They can be obtained from residues or by using advanced synthesis technologies like chemical vapour deposition. The carbon family is very wide, it includes classical activated carbons to more advanced ones, like carbon nanomaterials. However, these materials possess an easily tuneable porosity or chemical characteristics, which determine their final application. The surface chemistry is one of the most interesting aspects of this broad family of materials which allows the incorporation of different types of chemical functionalities or heteroatoms on the carbon surface such as N, B, S, P modifying, the acid-base character or their electronic properties.

This Special Issue will deal with the recent advances in heteroatom-doped carbon materials. Different synthesis procedures, characterization techniques and applications for these functional materials will be covered, as well as novel insights can be proposed.

It is our pleasure to invite you to submit a manuscript for this Special Issue. Full papers, short communications, and reviews are welcome.

Prof. Dr. Francisco Carrasco-Marín
Prof. Dr. Agustín F. Pérez-Cadenas
Dr. Sergio Morales-Torres
Guest Editors

Manuscript Submission Information

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 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Materials is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

carbon materials
heteroatoms
doping
surface chemistry, adsorption, catalytic applications, environmental applications, electrodes, energy storage

Published Papers (13 papers)

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Editorial

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4 pages, 198 KiB

Open AccessEditorial

Element-Doped Functional Carbon-Based Materials

by Sergio Morales-Torres, Agustín F. Pérez-Cadenas and Francisco Carrasco-Marín

Materials 2020, 13(2), 333; https://doi.org/10.3390/ma13020333 - 11 Jan 2020

Cited by 9 | Viewed by 2182

Abstract

Carbon materials are one of the most fascinating materials because of their unique properties and potential use in several applications. They can be obtained from agricultural waste, organic polymers, or by using advanced synthesizing technologies. The carbon family is very wide, it includes classical activated carbons to more advanced types like carbon gels, graphene, and so on. The surface chemistry of these materials is one of the most interesting aspects to be studied. The incorporation of different types of chemical functionalities and/or heteroatoms such as O, N, B, S, or P on the carbon surface enables the modification of the acidic–basic character, hydrophilicity–hydrophobicity, and the electron properties of these materials, which in turn determines the final application. This book collects original research articles focused on the synthesis, properties, and applications of heteroatom-doped functional carbon materials. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

Research

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16 pages, 2816 KiB

Open AccessFeature PaperArticle

Influence of Surface Chemistry on the Electrochemical Performance of Biomass-Derived Carbon Electrodes for its Use as Supercapacitors

by Abdelhakim Elmouwahidi, Esther Bailón-García, Luis A. Romero-Cano, Ana I. Zárate-Guzmán, Agustín F. Pérez-Cadenas and Francisco Carrasco-Marín

Materials 2019, 12(15), 2458; https://doi.org/10.3390/ma12152458 - 02 Aug 2019

Cited by 10 | Viewed by 3108

Abstract

Activated carbons prepared by chemical activation from three different types of waste woods were treated with four agents: melamine, ammonium carbamate, nitric acid, and ammonium persulfate, for the introduction of nitrogen and oxygen groups on the surface of materials. The results indicate that the presence of the heteroatoms enhances the capacitance, energy density, and power density of all samples. The samples treated with ammonium persulfate show the maximum of capacitance of 290 F g⁻¹ while for the melamine, ammonium carbamate, and nitric acid treatments, the samples reached the maximum capacitances values of 283, 280, and 455 F g⁻¹ respectively. This remarkable electro-chemical performance, as the high specific capacitances can be due to several reasons: i) The excellent and adequate textural characteristics makes possible a large adsorption interface for electrolyte to form the electrical double layer, leading to a great electrochemical double layer capacitance. ii) The doping with hetero-atoms enhances the surface interaction of these materials with the aqueous electrolyte, increasing the accessibility of electrolyte ions. iii) The hetero-atoms groups can also provide considerable pseudo-capacitance improving the overall capacitance. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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17 pages, 6285 KiB

Open AccessFeature PaperArticle

Carbon Xerogels Hydrothermally Doped with Bimetal Oxides for Oxygen Reduction Reaction

by Abdalla Abdelwahab, Francisco Carrasco-Marín and Agustín F. Pérez-Cadenas

Materials 2019, 12(15), 2446; https://doi.org/10.3390/ma12152446 - 31 Jul 2019

Cited by 11 | Viewed by 3020

Abstract

A total of two carbon xerogels doped with cobalt and nickel were prepared by the sol–gel method. The obtained carbon xerogels underwent further surface modification with three binary metal oxides namely: nickel cobaltite, nickel ferrite, and cobalt ferrite through the hydrothermal method. The mesopore volumes of these materials ranged between 0.24 and 0.40 cm³/g. Moreover, there was a morphology transformation for the carbon xerogels doped with nickel cobaltite, which is in the form of nano-needles after the hydrothermal process. Whereas the carbon xerogels doped with nickel ferrite and cobalt ferrite maintained the normal carbon xerogel structure after the hydrothermal process. The prepared materials were tested as electrocatalysts for oxygen reduction reaction using 0.1 M KOH. Among the prepared carbon xerogels cobalt-doped carbon xerogel had better electrocatalytic performance than the nickel-doped ones. Moreover, the carbon xerogels doped with nickel cobaltite showed excellent activity for oxygen reduction reaction due to mesoporosity development. NiCo₂O₄/Co-CX showed to be the best electrocatalyst of all the prepared electrocatalysts for oxygen reduction reaction application, exhibiting the highest electrocatalytic activity, lowest onset potential E_onset of −0.06 V, and the lowest equivalent series resistance (ESR) of 2.74 Ω. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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26 pages, 6585 KiB

Open AccessArticle

An Enhanced Carbon Capture and Storage Process (e-CCS) Applied to Shallow Reservoirs Using Nanofluids Based on Nitrogen-Rich Carbon Nanospheres

by Elizabeth Rodriguez Acevedo, Farid B. Cortés, Camilo A. Franco, Francisco Carrasco-Marín, Agustín F. Pérez-Cadenas, Vanessa Fierro, Alain Celzard, Sébastien Schaefer and Agustin Cardona Molina

Materials 2019, 12(13), 2088; https://doi.org/10.3390/ma12132088 - 28 Jun 2019

Cited by 11 | Viewed by 3356

Abstract

The implementation of carbon capture and storage process (CCS) has been unsuccessful to date, mainly due to the technical issues and high costs associated with two main stages: (1) CO₂ separation from flue gas and (2) CO₂ injection in deep geological deposits, more than 300 m, where CO₂ is in supercritical conditions. This study proposes, for the first time, an enhanced CCS process (e-CCS), in which the stage of CO₂ separation is removed and the flue gas is injected directly in shallow reservoirs located at less than 300 m, where the adsorptive phenomena control CO₂ storage. Nitrogen-rich carbon nanospheres were used as modifying agents of the reservoir porous texture to improve both the CO₂ adsorption capacity and selectivity. For this purpose, sandstone was impregnated with a nanofluid and CO₂ adsorption was evaluated at different pressures (atmospheric pressure and from 3 × 10⁻³ MPa to 3.0 MPa) and temperatures (0, 25, and 50 °C). As a main result, a mass fraction of only 20% of nanomaterials increased both the surface area and the molecular interactions, so that the increase of adsorption capacity at shallow reservoir conditions (50 °C and 3.0 MPa) was more than 677 times (from 0.00125 to 0.9 mmol g⁻¹). Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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9 pages, 3315 KiB

Open AccessCommunication

Novel Synthesis of Nitrogen-Containing Bio-Phenol Resin and Its Molten Salt Activation of Porous Carbon for Supercapacitor Electrode

by Tao Ai, Zhe Wang, Haoran Zhang, Fenghua Hong, Xin Yan and Xinhua Su

Materials 2019, 12(12), 1986; https://doi.org/10.3390/ma12121986 - 20 Jun 2019

Cited by 14 | Viewed by 2552

Abstract

Nitrogen hybridization is an attractive way to enhance the wettability and electric conductivity of porous carbon, which increases the capacitance of carbon-based supercapacitor, however, there is lack of low-cost methods to prepare the nitrogen-doped porous carbon materials. Herein, a novel facile nitrogen-containing bio-phenolic resin was synthesized by polymerization of the carbamate bio-oil, Phenol and paraformaldehyde. As a precursor of nitrogen-doped porous carbon, the nitrogen-containing bio-phenol resin was activated by the one-step molten-salt method. The resultant nitrogen-doped porous carbon showed a high specific surface area up to 1401 m²·g⁻¹. As a supercapacitor electrode, the nitrogen-doped porous carbons showed specific capacitance of 159 F·g⁻¹ at 0.5 A·g⁻¹. It also exhibited high cyclic stability with 94.8% retention of the initial specific capacitance over 1000 charge-discharge cycles at 1.0 A·g⁻¹. The results suggest that these nitrogen-containing bio-phenol resin provide a new source of nitrogen-doped porous carbon for high-performance supercapacitor electrodes. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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17 pages, 3606 KiB

Open AccessArticle

Enhanced CO₂ Adsorption on Nitrogen-Doped Carbon Materials by Salt and Base Co-Activation Method

by Ruiping Wei, Xingchao Dai and Feng Shi

Materials 2019, 12(8), 1207; https://doi.org/10.3390/ma12081207 - 12 Apr 2019

Cited by 6 | Viewed by 2654

Abstract

Nitrogen-doped carbon materials with enhanced CO₂ adsorption were prepared by the salt and base co-activation method. First, resorcinol-formaldehyde resin was synthesized with a certain salt as an additive and used as a precursor. Next, the resulting precursor was mixed with KOH and subsequently carbonized under ammonia flow to finally obtain the nitrogen-doped carbon materials. A series of samples, with and without the addition of different salts, were prepared, characterized by XRD (X-ray powder diffraction), elemental analysis, BET (N₂-adsorption-desorption analysis), XPS (X-ray photoelectron spectroscopy) and SEM (Scanning electron microscopy) and tested for CO₂ adsorption. The results showed that the salt and base co-activation method has a remarkable enhancing effect on the CO₂ capture capacity. The combination of KCl and KOH was proved to be the best combination, and 167.15 mg CO₂ could be adsorbed with 1 g nitrogen-doped carbon at 30 °C under 1 atm pressure. The materials characterizations revealed that the introduction of the base and salt could greatly increase the content of doped nitrogen, the surface area and the amount of formed micropore, which led to enhanced CO₂ absorption of the carbon materials. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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14 pages, 3320 KiB

Open AccessArticle

Electroanalytical Performance of Nitrogen-Doped Graphene Films Processed in One Step by Pulsed Laser Deposition Directly Coupled with Thermal Annealing

by Florent Bourquard, Yannick Bleu, Anne-Sophie Loir, Borja Caja-Munoz, José Avila, Maria-Carmen Asensio, Gaëtan Raimondi, Maryam Shokouhi, Ilhem Rassas, Carole Farre, Carole Chaix, Vincent Barnier, Nicole Jaffrezic-Renault, Florence Garrelie and Christophe Donnet

Materials 2019, 12(4), 666; https://doi.org/10.3390/ma12040666 - 23 Feb 2019

Cited by 13 | Viewed by 4819

Abstract

Graphene-based materials are widely studied to enable significant improvements in electroanalytical devices requiring new generations of robust, sensitive and low-cost electrodes. In this paper, we present a direct one-step route to synthetize a functional nitrogen-doped graphene film onto a Ni-covered silicon electrode substrate heated at high temperature, by pulsed laser deposition of carbon in the presence of a surrounding nitrogen atmosphere, with no post-deposition transfer of the film. With the ferrocene methanol system, the functionalized electrode exhibits excellent reversibility, close to the theoretical value of 59 mV, and very high sensitivity to hydrogen peroxide oxidation. Our electroanalytical results were correlated with the composition and nanoarchitecture of the N-doped graphene film containing 1.75 at % of nitrogen and identified as a few-layer defected and textured graphene film containing a balanced mixture of graphitic-N and pyrrolic-N chemical functions. The absence of nitrogen dopant in the graphene film considerably degraded some electroanalytical performances. Heat treatment extended beyond the high temperature graphene synthesis did not significantly improve any of the performances. This work contributes to a better understanding of the electrochemical mechanisms of doped graphene-based electrodes obtained by a direct and controlled synthesis process. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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11 pages, 2191 KiB

Open AccessArticle

On the Interactions and Synergism between Phases of Carbon–Phosphorus–Titanium Composites Synthetized from Cellulose for the Removal of the Orange-G Dye

by Hesham Hamad, Jesica Castelo-Quibén, Sergio Morales-Torres, Francisco Carrasco-Marín, Agustín F. Pérez-Cadenas and Francisco J. Maldonado-Hódar

Materials 2018, 11(9), 1766; https://doi.org/10.3390/ma11091766 - 18 Sep 2018

Cited by 27 | Viewed by 3777

Abstract

Carbon–phosphorus–titanium composites (CPT) were synthesized by Ti-impregnation and carbonization of cellulose. Microcrystalline cellulose used as carbon precursor was initially dissolved by phosphoric acid (H₃PO₄) to favor the Ti-dispersion and the simultaneous functionalization of the cellulose chains with phosphorus-containing groups, namely phosphates and polyphosphates. These groups interacted with the Ti-precursor during impregnation and determined the interface transformations during carbonization as a function of the Ti-content and carbonization temperature. Amorphous composites with high surface area and mesoporosity were obtained at low Ti-content (Ti:cellulose ratio = 1) and carbonization temperature (500 °C), while in composites with Ti:cellulose ratio = 12 and 800 °C, Ti-particles reacted with the cellulose groups leading to different Ti-crystalline polyphosphates and a marked loss of the porosity. The efficiency of composites in the removal of the Orange G dye in solution by adsorption and photocatalysis was discussed based on their physicochemical properties. These materials were more active than the benchmark TiO₂ material (Degussa P25), showing a clear synergism between phases. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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12 pages, 2604 KiB

Open AccessArticle

Effect of Reaction Temperature on Structure, Appearance and Bonding Type of Functionalized Graphene Oxide Modified P-Phenylene Diamine

by Hong-Juan Sun, Bo Liu, Tong-Jiang Peng and Xiao-Long Zhao

Materials 2018, 11(4), 647; https://doi.org/10.3390/ma11040647 - 23 Apr 2018

Cited by 5 | Viewed by 4253

Abstract

In this study, graphene oxides with different functionalization degrees were prepared by a facile one-step hydrothermal reflux method at various reaction temperatures using graphene oxide (GO) as starting material and p-phenylenediamine (PPD) as the modifier. The effects of reaction temperature on structure, appearance and bonding type of the obtained materials were investigated by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). The results showed that when the reaction temperature was 10–70 °C, the GO reacted with PPD through non-covalent ionic bonds (–COO⁻H₃⁺N–R) and hydrogen bonds (C–OH…H₂N–X). When the reaction temperature reached 90 °C, the GO was functionalized with PPD through covalent bonds of C–N. The crystal structure of products became more ordered and regular, and the interlayer spacing (d value) and surface roughness increased as the temperature increased. Furthermore, the results suggested that PPD was grafted on the surface of GO through covalent bonding by first attacking the carboxyl groups and then the epoxy groups of GO. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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9 pages, 2631 KiB

Open AccessArticle

Universal Effectiveness of Inducing Magnetic Moments in Graphene by Amino-Type sp³-Defects

by Tao Tang, Liting Wu, Shengqing Gao, Fang He, Ming Li, Jianfeng Wen, Xinyu Li and Fuchi Liu

Materials 2018, 11(4), 616; https://doi.org/10.3390/ma11040616 - 17 Apr 2018

Cited by 4 | Viewed by 3225

Abstract

Inducing magnetic moments in graphene is very important for its potential application in spintronics. Introducing sp³-defects on the graphene basal plane is deemed as the most promising approach to produce magnetic graphene. However, its universal validity has not been very well verified experimentally. By functionalization of approximately pure amino groups on graphene basal plane, a spin-generalization efficiency of ~1 μ_B/100 NH₂ was obtained for the first time, thus providing substantial evidence for the validity of inducing magnetic moments by sp³-defects. As well, amino groups provide another potential sp³-type candidate to prepare magnetic graphene. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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14 pages, 14273 KiB

Open AccessArticle

Enhanced CO₂ Adsorption by Nitrogen-Doped Graphene Oxide Sheets (N-GOs) Prepared by Employing Polymeric Precursors

by Abdulaziz Ali Alghamdi, Abdullah Fhead Alshahrani, Nezar H. Khdary, Fahad A. Alharthi, Hussain Ali Alattas and Syed Farooq Adil

Materials 2018, 11(4), 578; https://doi.org/10.3390/ma11040578 - 10 Apr 2018

Cited by 40 | Viewed by 4847

Abstract

Nitrogen-doped graphene oxide sheets (N-GOs) are prepared by employing N-containing polymers such as polypyrrole, polyaniline, and copolymer (polypyrrole-polyaniline) doped with acids such as HCl, H₂SO₄, and C₆H₅-SO₃-K, which are activated using different concentrations of KOH and carbonized at 650 °C; characterized using SEM, TEM, BET, TGA-DSC, XRD, and XPS; and employed for the removal of environmental pollutant CO₂. The porosity of the N-GOs obtained were found to be in the range 1–3.5 nm when the KOH employed was in the ratio of 1:4, and the XRD confirmed the formation of the layered like structure. However, when the KOH employed was in the ratio of 1:2, the pore diameter was found to be in the range of 50–200 nm. The SEM and TEM analysis reveal the porosity and sheet-like structure of the products obtained. The nitrogen-doped graphene oxide sheets (N-GOs) prepared by employing polypyrrole doped with C₆H₅-SO₃-K were found to possess a high surface area of 2870 m²/g. The N-GOs displayed excellent CO₂ capture property with the N-GOs; PPy/Ar-1 displayed ~1.36 mmol/g. The precursor employed, the dopant used, and the activation process were found to affect the adsorption property of the N-GOs obtained. The preparation procedure is simple and favourable for the synthesis of N-GOs for their application as adsorbents in greenhouse gas removal and capture. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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12 pages, 2634 KiB

Open AccessArticle

Adsorption Behavior of Selective Recognition Functionalized Biochar to Cd(II) in Wastewater

by Shiqiu Zhang, Xue Yang, Le Liu, Meiting Ju and Kui Zheng

Materials 2018, 11(2), 299; https://doi.org/10.3390/ma11020299 - 14 Feb 2018

Cited by 59 | Viewed by 4842

Abstract

Biochar is an excellent absorbent for most heavy metal ions and organic pollutants with high specific surface area, strong aperture structure, high stability, higher cation exchange capacity and rich surface functional groups. To improve the selective adsorption capacity of biochar to designated heavy metal ions, biochar prepared by agricultural waste is modified via Ionic-Imprinted Technique. Fourier transform infrared (FT-IR) spectra analysis and X-ray photoelectron spectroscopy (XPS) analysis of imprinted biochar (IB) indicate that 3-Mercaptopropyltrimethoxysilane is grafted on biochar surface through Si–O–Si bonds. The results of adsorption experiments indicate that the suitable pH range is about 3.0–8.0, the dosage is 2.0 g·L⁻¹, and the adsorption equilibrium is reached within 960 min. In addition, the data match pseudo-second-order kinetic model and Langmuir model well. The computation results of adsorption thermodynamics and stoichiometric displacement theory of adsorption (SDT-A) prove that the adsorption process is spontaneous and endothermic. Finally, IB possesses a higher selectivity adsorption to Cd(II) and a better reuse capacity. The functionalized biochar could solidify designated ions stably. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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16 pages, 2659 KiB

Open AccessArticle

Green Synthesis of Three-Dimensional Hybrid N-Doped ORR Electro-Catalysts Derived from Apricot Sap

by Ramesh Karunagaran, Campbell Coghlan, Cameron Shearer, Diana Tran, Karan Gulati, Tran Thanh Tung, Christian Doonan and Dusan Losic

Materials 2018, 11(2), 205; https://doi.org/10.3390/ma11020205 - 28 Jan 2018

Cited by 9 | Viewed by 4929

Abstract

Rapid depletion of fossil fuel and increased energy demand has initiated a need for an alternative energy source to cater for the growing energy demand. Fuel cells are an enabling technology for the conversion of sustainable energy carriers (e.g., renewable hydrogen or bio-gas) into electrical power and heat. However, the hazardous raw materials and complicated experimental procedures used to produce electro-catalysts for the oxygen reduction reaction (ORR) in fuel cells has been a concern for the effective implementation of these catalysts. Therefore, environmentally friendly and low-cost oxygen reduction electro-catalysts synthesised from natural products are considered as an attractive alternative to currently used synthetic materials involving hazardous chemicals and waste. Herein, we describe a unique integrated oxygen reduction three-dimensional composite catalyst containing both nitrogen-doped carbon fibers (N-CF) and carbon microspheres (N-CMS) synthesised from apricot sap from an apricot tree. The synthesis was carried out via three-step process, including apricot sap resin preparation, hydrothermal treatment, and pyrolysis with a nitrogen precursor. The nitrogen-doped electro-catalysts synthesised were characterised by SEM, TEM, XRD, Raman, and BET techniques followed by electro-chemical testing for ORR catalysis activity. The obtained catalyst material shows high catalytic activity for ORR in the basic medium by facilitating the reaction via a four-electron transfer mechanism. Full article

(This article belongs to the Special Issue Element-Doped Functional Carbon-based Materials)

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