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Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Energy and Catalysis".

Deadline for manuscript submissions: closed (31 August 2023) | Viewed by 25513

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Prof. Dr. Hermenegildo García

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Departamento de Quimica and Instituto Universitario de Tecnologia Quimica (CSIC-UPV), Universitat Politecnica de Valencia, Av. De los Naranjos s/n, 46022 Valencia, Spain
Interests: heterogeneous catalysis; photocatalysis
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Prof. Dr. Amarajothi Dhakshinamoorthy

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School of Chemistry, Madurai Kamaraj University, Madurai 625 021, India
Interests: heterogeneous catalysis; metal–organic frameworks; solid catalysts; chitosan; carbocatalysis
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

In recent years, the use of carbonaceous solids in photocatalysis and photoelectrocatalysis has attracted many researchers around the world due to their availability, good stability, reliable preparation, and the wide diversity of possible structures. In addition, different types of heterojunctions have also been developed by combining semiconductors with photoresponsive carbons, introducing co-catalysts, and controlling the interfacial contact. One of the fundamental reasons to employ carbon-based solids for photocatalysis is their fast electron mobility, large surface area, high physicochemical stability, and viable synthetic strategies from different precursors. On the other hand, the photocatalytic activity of the carbonaceous solids is very much influenced by doping, the presence of defects, confinement, and morphology. Some of the most widely used carbonaceous materials for the development of photocatalysts/photoelectrocatalysts are activated carbons, carbon dots, carbon nanotubes, nanofibers, graphene-based solids, graphitic carbon nitrides, fullerenes, and three-dimensional structured carbons. This Special Issue aims to show the breadth of the field and the potential for various applications of carbon based materialsincluding photocatalysis for organic compound transformation, special cases of organic pollutant photodegradation, photocatalytic hydrogen generation, oxygen evolution and water splitting, photoreduction of CO₂, photocatalytic, and related solar fuels production.

Prof. Dr. Hermenegildo García
Prof. Dr. Amarajothi Dhakshinamoorthy
Guest Editors

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Keywords

activated carbon
carbon dot
graphene
photocatalysis
photoelectrocatalysis
reduced graphene oxide
solar light conversion
visible light

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Published Papers (10 papers)

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Research

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18 pages, 8211 KiB

Open AccessArticle

Nanometric Cu-ZnO Particles Supported on N-Doped Graphitic Carbon as Catalysts for the Selective CO₂ Hydrogenation to Methanol

by Lu Peng, Bogdan Jurca, Alberto Garcia-Baldovi, Liang Tian, German Sastre, Ana Primo, Vasile Parvulescu, Amarajothi Dhakshinamoorthy and Hermenegildo Garcia

Nanomaterials 2024, 14(5), 476; https://doi.org/10.3390/nano14050476 - 6 Mar 2024

Cited by 2 | Viewed by 1889

Abstract

The quest for efficient catalysts based on abundant elements that can promote the selective CO₂ hydrogenation to green methanol still continues. Most of the reported catalysts are based on Cu/ZnO supported in inorganic oxides, with not much progress with respect to the benchmark Cu/ZnO/Al₂O₃ catalyst. The use of carbon supports for Cu/ZnO particles is much less explored in spite of the favorable strong metal support interaction that these doped carbons can establish. This manuscript reports the preparation of a series of Cu-ZnO@(N)C samples consisting of Cu/ZnO particles embedded within a N-doped graphitic carbon with a wide range of Cu/Zn atomic ratio. The preparation procedure relies on the transformation of chitosan, a biomass waste, into N-doped graphitic carbon by pyrolysis, which establishes a strong interaction with Cu nanoparticles (NPs) formed simultaneously by Cu²⁺ salt reduction during the graphitization. Zn²⁺ ions are subsequently added to the Cu–graphene material by impregnation. All the Cu/ZnO@(N)C samples promote methanol formation in the CO₂ hydrogenation at temperatures from 200 to 300 °C, with the temperature increasing CO₂ conversion and decreasing methanol selectivity. The best performing Cu-ZnO@(N)C sample achieves at 300 °C a CO₂ conversion of 23% and a methanol selectivity of 21% that is among the highest reported, particularly for a carbon-based support. DFT calculations indicate the role of pyridinic N doping atoms stabilizing the Cu/ZnO NPs and supporting the formate pathway as the most likely reaction mechanism. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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17 pages, 4133 KiB

Open AccessArticle

Enhanced Visible Light-Driven Photocatalytic Water-Splitting Reaction of Titanate Nanotubes Sensitised with Ru(II) Bipyridyl Complex

by Mauro Malizia, Stuart A. Scott, Laura Torrente-Murciano, Adam M. Boies, Talal A. Aljohani and Herme G. Baldovi

Nanomaterials 2023, 13(22), 2959; https://doi.org/10.3390/nano13222959 - 16 Nov 2023

Cited by 2 | Viewed by 1382

Abstract

The ion exchange of Na⁺ cations was used to photosensitise titanates nanotubes (Ti-NTs) with tris(2,2’-bipyridine)ruthenium(II) cations (Ru(bpy)₃²⁺); this yielded a light-sensitised Ti-NTs composite denoted as (Ru(bpy)₃)Ti-NTs, exhibiting the characteristic absorption of Ru(bpy)₃²⁺ in visible light. Incident photon-to-current efficiency (IPCE) measurements and the photocatalytic reduction of methyl viologen reaction confirmed that in the photosensitisation of the (Ru(bpy)₃)Ti-NTs composite, charge transfer and charge separation occur upon excitation by ultraviolet and visible light irradiation. The photocatalytic potential of titanate nanotubes was tested in the water-splitting reaction and the H₂ evolution reaction using a sacrificial agent and showed photocatalytic activity under various light sources, including xenon–mercury lamp, simulated sunlight, and visible light. Notably, in the conditions of the H₂ evolution reaction when (Ru(bpy)₃)Ti-NTs were submitted to simulated sunlight, they exceeded the photocatalytic activity of pristine Ti-NTs and TiO₂ by a factor of 3 and 3.5 times, respectively. Also, (Ru(bpy)₃)Ti-NTs achieved the photocatalytic water-splitting reaction under simulated sunlight and visible light, producing, after 4 h, 199 and 282 μmol×H_2×g_cat⁻¹. These results confirm the effective electron transfer of Ru(bpy)₃ to titanate nanotubes. The stability of the photocatalyst was evaluated by a reuse test of four cycles of 24 h reactions without considerable loss of catalytic activity and crystallinity. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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14 pages, 5065 KiB

Open AccessArticle

A Porphyrin-Based Covalent Organic Framework as Metal-Free Visible-LED-Light Photocatalyst for One-Pot Tandem Benzyl Alcohol Oxidation/Knoevenagel Condensation

by Sara Oudi, Ali Reza Oveisi, Saba Daliran, Mostafa Khajeh, Amarajothi Dhakshinamoorthy and Hermenegildo García

Nanomaterials 2023, 13(3), 558; https://doi.org/10.3390/nano13030558 - 30 Jan 2023

Cited by 13 | Viewed by 2995

Abstract

A porphyrin-based covalent organic framework (COF), namely Porph-UOZ-COF (UOZ stands for the University of Zabol), has been designed and prepared via the condensation reaction of 5,10,15,20-tetrakis-(3,4-dihydroxyphenyl)porphyrin (DHPP) with 1,4-benzenediboronic acid (DBBA), under the solvothermal condition. The solid was characterized by spectroscopic, microscopic, and powder X-ray diffraction techniques. The resultant multifunctional COF revealed an outstanding performance in catalyzing a one-pot tandem selective benzylic C-H photooxygenation/Knoevenagel condensation reaction in the absence of additives or metals under visible-LED-light irradiation. Notably, the catalytic activity of the COF was superior to individual organic counterparts and the COF was both stable and reusable for four consecutive runs. The present approach illustrates the potential of COFs as promising metal-free (photo) catalysts for the development of tandem reactions. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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10 pages, 3798 KiB

Open AccessArticle

Enhanced Photocatalytic Degradation Activity Using the V₂O₅/RGO Composite

by Anuja A. Yadav, Yuvaraj M. Hunge, Seok-Won Kang, Akira Fujishima and Chiaki Terashima

Nanomaterials 2023, 13(2), 338; https://doi.org/10.3390/nano13020338 - 13 Jan 2023

Cited by 63 | Viewed by 4430

Abstract

Semiconductor-based photocatalyst materials played an important role in the degradation of organic compounds in recent years. Photocatalysis is a simple, cost-effective, and environmentally friendly process for degrading organic compounds. In this work, vanadium pentoxide (V₂O₅) and V₂O₅/RGO (reduced graphene oxide) composite were synthesized by a hydrothermal method. The prepared samples were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), Raman spectroscopy, and UV-Vis spectroscopic analysis, etc. Raman analysis shows the occurrence of RGO characteristic peaks in the composite and different vibrational modes of V₂O₅. The band gap of flake-shaped V₂O₅ is reduced and its light absorption capacity is enhanced by making its composite with RGO. The photocatalytic degradation of methylene blue (MB) was studied using both V₂O₅ and V₂O₅/RGO composite photocatalyst materials. The V₂O₅/RGO composite exhibits a superior photocatalytic performance to V₂O₅. Both catalyst and light play an important role in the degradation process. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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17 pages, 4229 KiB

Open AccessEditor’s ChoiceArticle

Photocatalytic Hydrogen Production from Glycerol Aqueous Solutions as Sustainable Feedstocks Using Zr-Based UiO-66 Materials under Simulated Sunlight Irradiation

by Celia M. Rueda-Navarro, Belén Ferrer, Herme G. Baldoví and Sergio Navalón

Nanomaterials 2022, 12(21), 3808; https://doi.org/10.3390/nano12213808 - 28 Oct 2022

Cited by 14 | Viewed by 2742

Abstract

There is an increasing interest in developing cost-effective technologies to produce hydrogen from sustainable resources. Herein we show a comprehensive study on the use of metal–organic frameworks (MOFs) as heterogeneous photocatalysts for H₂ generation from photoreforming of glycerol aqueous solutions under simulated sunlight irradiation. The list of materials employed in this study include some of the benchmark Zr-MOFs such as UiO-66(Zr)-X (X: H, NO₂, NH₂) as well as MIL-125(Ti)-NH₂ as the reference Ti-MOF. Among these solids, UiO-66(Zr)-NH₂ exhibits the highest photocatalytic H₂ production, and this observation is attributed to its adequate energy level. The photocatalytic activity of UiO-66(Zr)-NH₂ can be increased by deposition of small Pt NPs as the reference noble metal co-catalyst within the MOF network. This photocatalyst is effectively used for H₂ generation at least for 70 h without loss of activity. The crystallinity of MOF and Pt particle size were maintained as revealed by powder X-ray diffraction and transmission electron microscopy measurements, respectively. Evidence in support of the occurrence of photoinduced charge separation with Pt@UiO-66(Zr)-NH₂ is provided from transient absorption and photoluminescence spectroscopies together with photocurrent measurements. This study exemplifies the possibility of using MOFs as photocatalysts for the solar-driven H₂ generation using sustainable feedstocks. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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15 pages, 3169 KiB

Open AccessFeature PaperArticle

Phosphorus-Rich Ruthenium Phosphide Embedded on a 3D Porous Dual-Doped Graphitic Carbon for Hydrogen Evolution Reaction

by Aicha Anouar, Antonio Doménech-Carbó and Hermenegildo Garcia

Nanomaterials 2022, 12(20), 3597; https://doi.org/10.3390/nano12203597 - 13 Oct 2022

Cited by 2 | Viewed by 1936

Abstract

Metal phosphides have recently emerged as promising electrocatalysts for hydrogen evolution reaction (HER). Herein, we report the synthesis of ruthenium diphosphide embedded on a dual-doped graphitic carbon by pyrolyzing chitosan beads impregnated with ruthenium chloride and phosphorus pentoxide. The as-synthesized RuP₂@N-P-C displays a good electrocatalytic activity in acidic, neutral and alkaline media. We show that the HER activity of the electrocatalyst can be tuned by varying the concentration of Li⁺ cations. Co-diffusion effects on H⁺ exerted by Li⁺ on HER in the porous carbon matrix have been observed. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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13 pages, 2957 KiB

Open AccessArticle

Promotional Effects on the Catalytic Activity of Co-Fe Alloy Supported on Graphitic Carbon for CO₂ Hydrogenation

by Bogdan Jurca, Lu Peng, Ana Primo, Alvaro Gordillo, Amarajothi Dhakshinamoorthy, Vasile I. Parvulescu and Hermenegildo García

Nanomaterials 2022, 12(18), 3220; https://doi.org/10.3390/nano12183220 - 16 Sep 2022

Cited by 5 | Viewed by 1925

Abstract

Starting from the reported activity of Co-Fe nanoparticles wrapped onto graphitic carbon (Co-Fe@C) as CO₂ hydrogenation catalysts, the present article studies the influence of a series of metallic (Pd, Ce, Ca, Ca, and Ce) and non-metallic (S in various percentages and S and alkali metals) elements as Co-Fe@C promoters. Pd at 0.5 wt % somewhat enhances CO₂ conversion and CH₄ selectivity, probably due to H₂ activation and spillover on Co-Fe. At similar concentrations, Ce does not influence CO₂ conversion but does diminish CO selectivity. A 25 wt % Fe excess increases the Fe-Co particle size and has a detrimental effect due to this large particle size. The presence of 25 wt % of Ca increases the CO₂ conversion and CH₄ selectivity remarkably, the effect being attributable to the CO₂ adsorption capacity and basicity of Ca. Sulfur at a concentration of 2.1% or higher acts as a strong poison, decreasing CO₂ conversion and shifting selectivity to CO. The combination of S and alkali metals as promoters maintain the CO selectivity of S but notably increase the CO₂ conversion. Overall, this study shows how promoters and poisons can alter the catalytic activity of Co/Fe@C catalysts, changing from CH₄ to CO. It is expected that further modulation of the activity of Co/Fe@C catalysts can serve to drive the activity and selectivity of these materials to any CO₂ hydrogenation products that are wanted. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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19 pages, 4904 KiB

Open AccessArticle

Photocatalytic Water Splitting Promoted by 2D and 3D Porphyrin Covalent Organic Polymers Synthesized by Suzuki-Miyaura Carbon-Carbon Coupling

by Maria Novoa-Cid, Arianna Melillo, Belén Ferrer, Mercedes Alvaro and Herme G. Baldovi

Nanomaterials 2022, 12(18), 3197; https://doi.org/10.3390/nano12183197 - 14 Sep 2022

Cited by 8 | Viewed by 2492

Abstract

This work deals with the synthesis of metal-free and porphyrin-based covalent organic polymers (COPs) by the Suzuki–Miyaura coupling carbon-carbon bond forming reaction to study the photocatalytic overall water splitting performance. Apart from using 5,10,15,20-Tetrakis-(4-bromophenyl)porphyrin, we have chosen different cross-linker monomers to induce 2-dimensional (2D) or 3-dimensional (3D) and different rigidity in their resulting polymeric molecular structure. The synthesised COPs were extensively characterised to reveal that the dimensionality and flexibility of the molecular structure play an intense role in the physical, photochemical, and electronic properties of the polymers. Photoinduced excited state of the COPs was evaluated by nanosecond time-resolved laser transient absorption spectroscopy (TAS) by analysing excited state kinetics and quenching experiments, photocurrent density measurements and photocatalytic deposition of Ru³⁺ to RuO_2, and photocatalysis. In summary, TAS experiments demonstrated that the transient excited state of these polymers has two decay kinetics and exhibit strong interaction with water molecules. Moreover, photocurrent and photocatalytic deposition experiments proved that charges are photoinduced and are found across the COP molecular network, but more important charges can migrate from the surface of the COP to the medium. Among the various COPs tested, COP–3 that has a flexible and 3D molecular structure reached the best photocatalytic performances, achieving a photocatalytic yield of 0.4 mmol H₂ × g_COP–3⁻¹ after 3 h irradiation. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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15 pages, 3812 KiB

Open AccessArticle

Enhanced Visible Light-Driven Photoelectrocatalytic Degradation of Paracetamol at a Ternary z-Scheme Heterojunction of Bi₂WO₆ with Carbon Nanoparticles and TiO₂ Nanotube Arrays Electrode

by Nondumiso Mahhumane, Leskey M. Cele, Charles Muzenda, Oluchi V. Nkwachukwu, Babatunde A. Koiki and Omotayo A. Arotiba

Nanomaterials 2022, 12(14), 2467; https://doi.org/10.3390/nano12142467 - 19 Jul 2022

Cited by 6 | Viewed by 2487

Abstract

In this study, a ternary z-scheme heterojunction of Bi₂WO₆ with carbon nanoparticles and TiO₂ nanotube arrays was used to remove paracetamol from water by photoelectrocatalysis. The materials and z-scheme electrode were characterised using X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDS), EDS mapping, ultraviolet diffuse reflection spectroscopy (UV-DRS), photocurrent measurement, electrochemical impedance spectroscopy (EIS), uv-vis spectroscopy and total organic carbon measurement (TOC). The effect of parameters such as current density and pH were studied. At optimal conditions, the electrode was applied for photoelectrocatalytic degradation of paracetamol, which gave a degradation efficiency of 84% within 180 min. The total organic carbon removal percentage obtained when using this electrode was 72%. Scavenger studies revealed that the holes played a crucial role during the photoelectrocatalytic degradation of paracetamol. The electrode showed high stability and reusability therefore suggesting that the z-scheme Bi₂WO₆-CNP-TiO₂ nanotube arrays electrode is an efficient photoanode for the degradation of pharmaceuticals in wastewater. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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Review

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15 pages, 6795 KiB

Open AccessReview

Graphitic Carbon Nitride as Visible-Light Photocatalyst Boosting Ozonation in Wastewater Treatment

by Amarajothi Dhakshinamoorthy, Antón López-Francés, Sergio Navalon and Hermenegildo Garcia

Nanomaterials 2022, 12(19), 3494; https://doi.org/10.3390/nano12193494 - 6 Oct 2022

Cited by 2 | Viewed by 1971

Abstract

Light can boost ozone efficiency in advanced oxidation processes (AOPs), either by direct ozone photolysis with UV light or by using a photocatalyst that can be excited with UV-Vis or solar light. The present review summarizes literature data on the combination of ozone and the g-C₃N₄ photocatalyst for the degradation of probe molecules in water, including oxalic, p-hydroxybenzoic and oxamic acids as well as ciprofloxacin and parabens. g-C₃N₄ is a metal-free visible-light photocatalyst based on abundant elements that establishes a synergistic effect with ozone, the efficiency of the combination of the photocatalysis and ozonation being higher than the sum of the two treatments independently. Available data indicate that this synergy derives from the higher efficiency in the generation of hydroxyl radicals due to the efficient electron quenching by O₃ of photogenerated conduction band electrons in the g-C₃N₄ photocatalyst. Given the wide use of ozonizers in water treatment, it is proposed that their implementation with g-C₃N₄ photocatalysis could also boost ozone efficiency in the AOPs of real waste waters. Full article

(This article belongs to the Special Issue Carbon-Based Nanomaterials for Visible-Light Photocatalysis and Photoelectrocatalysis)

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