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Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion

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A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Photocatalysis".

Deadline for manuscript submissions: closed (30 September 2023) | Viewed by 17687

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Dr. Weilong Shi

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School of Material Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China
Interests: photocatalytic water splitting; near-infrared light-driven; g-C₃N₄; ZnIn₂S₄; tetracycline
Special Issues, Collections and Topics in MDPI journals

Dr. Feng Guo

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Guest Editor

School of Energy and Power, Jiangsu University of Science and Technology, Zhenjiang 212003, China
Interests: tetracycline; g-C₃N₄; ZnIn₂S₄; photocatalytic H₂ production; heterojunction
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Xue Lin

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School of Material Science and Engineering, Beihua University, Jilin 132013, China
Interests: photocatalytic H₂ production; heterojunction
Special Issues, Collections and Topics in MDPI journals

Dr. Yuanzhi Hong

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Dear Colleagues,

Energy crisis and environmental pollution have become two serious problems in the further development of human society. The “Honda–Fujishima Effect” was discovered by Prof. Fujishima and Honda in 1967, which opened the way to photocatalysis. Photocatalysis is regarded as a promosing environmentally friendly technology to address the above issues due to its low energy input and carbon footprint. By converting solar energy into other forms of energy, photocatalytic technology provides a green, environmental protective, and highly economic way to solve energy problems. For instance, photocatalytic CO₂ reduction into hydrocarbons and water splitting into H₂ are two representative fields. Moreover, advanced photocatalytic technology also plays a significant role in solving environmental problems such as water pollutant degradation, sterilization, and antiseptics. The core of photocatalysis is the semiconductor photocatalyst. In particular, graphitic carbon nitride (g-C₃N₄) is a typical organic–nonmetallic semiconductor photocatalyst, which has become a research hotspot due to its unique properties, such as being innoxious, low-cost, easy to synthesize, of an appropriate energy band gap (2.7 eV) and with outstanding thermal stability and chemical stability. Nevertheless, some inherent scientific problems, containing small surface area, low utilization of visible light and fast recombination of electrons and holes, which limit its applications in the field of photocatalysis. Among enormous modification methods, the construction of a heterojunction/homojunction between g-C₃N₄ and other semiconductor photocatalysts with interleaved energy band position is an effective channel to improve its photocatalytic activity, which can be attributed to the accelerated photon-generated carrier transfer rate. In particular, in the emerging S-scheme structure, it can simultaneously both accelerated photon-generated carrier transfer rates and higher redox potentials. Although a large number of gratifying results have been achieved in recent years around the world, the economic benefit of photocatalytic technology is not greater than that of the standard of industrialization. Therefore, there is an urgent need to design a neoteric g-C₃N₄-based photocatalytic system that can further promote the development of photocatalysis. This Special Issue aims to collect recent advances in g-C₃N₄-based photocatalysts in energy conversion and environmental protection fields. We welcome original research, review, and perspective within the following scopes:

The photocatalytic pollutant degradation under different water environments;
Photocatalytic water splitting;
Photocatalytic CO₂ reduction;
Photothermal effect-assisted catalytic performance;
g-C₃N₄-based S-scheme heterojunctions;
New fabrication and modification methods of active photocatalysts;
Widening the light response of semiconductors to the solar spectrum;
Enhancing the utilization of photo-generated carriers;
New analytical techniques to probe the reaction intermediates during photocatalysis.

Dr. Weilong Shi
Dr. Feng Guo
Prof. Dr. Xue Lin
Dr. Yuanzhi Hong
Guest Editors

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Keywords

g-C₃N₄
photocatalysts
environmental purification
energy conversion

Published Papers (12 papers)

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Editorial

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3 pages, 152 KiB

Open AccessEditorial

Editorial: Special Issue Entitled “Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion”

by Feng Guo, Xue Lin, Yuanzhi Hong and Weilong Shi

Catalysts 2024, 14(1), 46; https://doi.org/10.3390/catal14010046 - 10 Jan 2024

Cited by 1 | Viewed by 782

Abstract

Solar photocatalysis has evolved rapidly over the past few decades and has received significant attention for its green, safe and renewable energy benefits, particularly in the current era of global crisis, being considered as a potential solution to the major problems we face [...] Read more.

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

Research

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20 pages, 7311 KiB

Open AccessFeature PaperArticle

A Novel Organic/Inorganic Dual Z-Scheme Photocatalyst with Visible-Light Response for Organic Pollutants Degradation

by Taoming Yu, Doudou Wang, Lili Li, Wenjing Song, Xuan Pang and Ce Liang

Catalysts 2023, 13(11), 1391; https://doi.org/10.3390/catal13111391 - 24 Oct 2023

Cited by 1 | Viewed by 810

Abstract

The design of highly efficient organic/inorganic photocatalysts with visible-light response has attracted great attention for the removal of organic pollutants. In this work, the polyacrylonitrile (PAN) worked as the matrix polymer, while polyaniline (PANI) and Sb₂S₃–ZnO were used as organic/inorganic photocatalysts. The heterojunction PAN/PANI–Sb₂S₃–ZnO photocatalyst was prepared using electrospinning and surface ultrasound. PAN/PANI–Sb₂S₃–ZnO exhibited an excellent visible-light absorption intensity in the wavelength range of 400–700 nm. The maximum removal efficiencies of PAN/PANI–Sb₂S₃–ZnO for four organic dyes were all greater than 99%. The mechanism study showed that a dual Z-scheme could be constructed ingeniously because of the well-matched bandgaps between organic and inorganic components in the photocatalyst, which achieved efficient separation of photogenerated carriers and reserved photogenerated electrons (e⁻) and holes (h⁺) with strong redox ability. The active species •OH and •O₂⁻ played an important role in the photocatalytic process. The composite photocatalyst also had excellent stability and reusability. This work suggested a pathway for designing novel organic/inorganic composite photocatalysts with visible-light response. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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15 pages, 3859 KiB

Open AccessEditor’s ChoiceArticle

Photothermal-Assisted Photocatalytic Degradation of Tetracycline in Seawater Based on the Black g-C₃N₄ Nanosheets with Cyano Group Defects

by Loic Jiresse Nguetsa Kuate, Zhouze Chen, Jialin Lu, Huabing Wen, Feng Guo and Weilong Shi

Catalysts 2023, 13(7), 1147; https://doi.org/10.3390/catal13071147 - 24 Jul 2023

Cited by 27 | Viewed by 1483

Abstract

As a broad-spectrum antibiotic, tetracycline (TC) has been continually detected in soil and seawater environments, which poses a great threat to the ecological environment and human health. Herein, a black graphitic carbon nitride (CN-B) photocatalyst was synthesized by the one-step calcination method of urea and phloxine B for the degradation of tetracycline TC in seawater under visible light irradiation. The experimental results showed that the photocatalytic degradation rate of optimal CN-B-0.1 for TC degradation was 92% at room temperature within 2 h, which was 1.3 times that of pure CN (69%). This excellent photocatalytic degradation performance stems from the following factors: (i) ultrathin nanosheet thickness reduces the charge transfer distance; (ii) the cyanogen defect promotes photogenerated carriers’ separation; (iii) and the photothermal effect of CN-B increases the reaction temperature and enhances the photocatalytic activity. This study provides new insight into the design of photocatalysts for the photothermal-assisted photocatalytic degradation of antibiotic pollutants. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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14 pages, 4271 KiB

Open AccessFeature PaperArticle

Visible-Light-Driven GO/Rh-SrTiO₃ Photocatalyst for Efficient Overall Water Splitting

by Shuai Zhang, Enhui Jiang, Ji Wu, Zhonghuan Liu, Yan Yan, Pengwei Huo and Yongsheng Yan

Catalysts 2023, 13(5), 851; https://doi.org/10.3390/catal13050851 - 08 May 2023

Cited by 3 | Viewed by 1345

Abstract

The combining of the heterostructure construction and active sites modification to remodel the traditional wide-band-gap semiconductor SrTiO₃ for improving visible light absorption capacity and enhancing photocatalytic performance is greatly desired. Herein, we research a novel GO/Rh-SrTiO₃ nanocomposite via a facile hydrothermal method. The champion GO/Rh-SrTiO₃ nanocomposite exhibits the superior photocatalytic overall water splitting performance with an H₂ evolution rate of 55.83 μmol∙g⁻¹∙h⁻¹ and O₂ production rate of 23.26 μmol∙g⁻¹∙h⁻¹, realizing a breakthrough from zero with respect to the single-phased STO under visible light (λ ≥ 420 nm). More importantly, a series of characterizations results showed that significantly improving photocatalytic performance originated mainly from the construction of heterostructure and more active sites rooted in Rh metal. In addition, the possible photocatalytic reaction mechanisms and the transport behavior of photogenerated carriers have been revealed in deeper detail. This work provides an effective strategy for heterostructure construction to improve solar utilization through vastly expanding visible light response ranges from traditional UV photocatalysts. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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17 pages, 5760 KiB

Open AccessArticle

Fabrication of FeTCPP@CNNS for Efficient Photocatalytic Performance of p-Nitrophenol under Visible Light

by Shiyun Li, Yuqiong Guo, Lina Liu, Jiangang Wang, Luxi Zhang, Weilong Shi, Malgorzata Aleksandrzak, Xuecheng Chen and Jie Liu

Catalysts 2023, 13(4), 732; https://doi.org/10.3390/catal13040732 - 12 Apr 2023

Cited by 3 | Viewed by 1317

Abstract

A photocatalyst of iron–porphyrin tetra-carboxylate (FeTCPP)-sensitized g-C₃N₄ nanosheet composites (FeTCPP@CNNS) based on g-C₃N₄ nanosheet (CNNS) and FeTCPP have been fabricated by in situ hydrothermal self-assembly. FeTCPP is uniformly introduced to the surface of CNNS. Only a small amount of FeTCPP is introduced, and the stacked lamellar structure is displayed in the composite. As compared with pure CNNS, the FeTCPP@CNNS composites exhibit significantly improved photocatalytic performance by the photodegradation of p-nitrophenol (4-NP). At the optimum content of FeTCPP to CNNS (3 wt%), the photodegradation activity of the FeTCPP@CNNS photocatalyst can reach 92.4% within 1 h. The degradation rate constant for the 3% FeTCPP@CNNS composite is 0.037 min⁻¹ (4-NP), which is five times that of CNNS (0.0064 min⁻¹). The results of recycling experiments show that 3% FeTCPP@CNNS photocatalyst has excellent photocatalytic stability. A possible photocatalytic reaction mechanism of FeTCPP@CNNS composite for photocatalytic degradation of 4-NP has been proposed. It is shown that superoxide radical anions played the major part in the degradation of 4-NP. The appropriate content of FeTCPP can enhance the charge transfer efficiency. The FeTCPP@CNNS composites can provide more active sites and accelerate the transport and separation efficiency of photogenerated carriers, thus further enhancing the photocatalytic performance. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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16 pages, 3993 KiB

Open AccessFeature PaperArticle

Hollow g-C₃N₄@Cu_0.5In_0.5S Core-Shell S-Scheme Heterojunction Photothermal Nanoreactors with Broad-Spectrum Response and Enhanced Photocatalytic Performance

by Yawei Xiao, Zhezhe Wang, Bo Yao, Yunhua Chen, Ting Chen and Yude Wang

Catalysts 2023, 13(4), 723; https://doi.org/10.3390/catal13040723 - 11 Apr 2023

Cited by 2 | Viewed by 1281

Abstract

Improving spectral utilization and carrier separation efficiency is a key point in photocatalysis research. Herein, we prepare hollow g-C₃N₄ nanospheres by the template method and synthesize a g-C₃N₄@Cu_0.5In_0.5S core-shell S-scheme photothermal nanoreactor by a simple chemical deposition method. The unique hollow core-shell structure of g-C₃N₄@Cu_0.5In_0.5S is beneficial to expand the spectral absorption range and improving photon utilization. At the same time, the photogenerated carriers can be separated, driven by the internal electric field. In addition, g-C₃N₄@Cu_0.5In_0.5S also has a significantly enhanced photothermal effect, which promotes the photocatalytic reaction by increasing the temperature of the reactor. The benefit from the synergistic effect of light and heat, the H₂ evolution rate of g-C₃N₄@Cu_0.5In_0.5S is as high as 2325.68 μmol h⁻¹ g⁻¹, and the degradation efficiency of oxytetracycline under visible light is 95.7%. The strategy of combining S-scheme heterojunction with photothermal effects provides a promising insight for the development of an efficient photocatalytic reaction. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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13 pages, 8823 KiB

Open AccessArticle

Facile Construction of Intramolecular g-CN-PTCDA Donor-Acceptor System for Efficient CO₂ Photoreduction

by Jiajia Wei, Xing Chen, Xitong Ren, Shufang Tian and Feng Bai

Catalysts 2023, 13(3), 600; https://doi.org/10.3390/catal13030600 - 16 Mar 2023

Cited by 3 | Viewed by 1540

Abstract

Due to the different electron affinity, the construction of a donor-acceptor (DA) system in the graphitic carbon nitride (g-CN) matrix is an attractive tactic to accelerate photo-induced electron-holes separation, and then further elevate its photocatalytic performance. In this work, perylene tetracarboxylic dianhydride (PTCDA) with magnificent electron affinity and excellent thermal stability was chosen to copolymerize with urea via facile one-pot thermal copolymerization to fabricate g-CN-PTCDA equipped with DA structures. The specific surface area of g-CN-PTCDA would be enlarged and the visible light absorption range would be broadened simultaneously when adopting this copolymerization strategy. A series of characterizations such as electron paramagnetic resonance (EPR), steady and transient photoluminescence spectra (PL), electrochemical impedance spectroscopy (EIS), and photocurrent tests combined with computational simulation confirmed the charge separation and transfer efficiency dramatically improved due to the DA structures construction. When 0.25% wt PTCDA was introduced, the CO evolution rate was nearly 23 times than that of pristine g-CN. The CO evolution rate could reach up to 87.2 μmol g⁻¹ h⁻¹ when certain Co²⁺ was added as co-catalytic centers. Meanwhile, g-CN-1 mg PTCDA-Co exhibited excellent long-term stability and recyclability as a heterogeneous photocatalyst. This research may shed light on designing more effective DA structures for solar-to-energy conversion by CO₂ reduction. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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15 pages, 6710 KiB

Open AccessArticle

Surface Plasmon Resonance Induced Photocatalysis in 2D/2D Graphene/g-C₃N₄ Heterostructure for Enhanced Degradation of Amine-Based Pharmaceuticals under Solar Light Illumination

by Faisal Al Marzouqi and Rengaraj Selvaraj

Catalysts 2023, 13(3), 560; https://doi.org/10.3390/catal13030560 - 10 Mar 2023

Cited by 1 | Viewed by 1044

Abstract

Pharmaceuticals, especially amine-based pharmaceuticals, such as nizatidine and ranitidine, contaminate water and resist water treatment. Here, different amounts of graphene sheets are coupled with g-C₃N₄ nanosheets (wt% ratio of 0.5, 1, 3 and 5 wt% of graphene) to verify the effect of surface plasmon resonance introduced to the g-C₃N₄ material. The synthesized materials were systematically examined by advanced analytical techniques. The prepared photocatalysts were used for the degradation of amine-based pharmaceuticals (nizatidine and ranitidine). The results show that by introducing only 3 wt% graphene to g-C₃N₄, the absorption ability in the visible and near-infrared regions dramatically enhanced. The absorption in the visible range was 50 times higher when compared to the pure sample. These absorption features suggest that the surfaces of the carbon nitride sheet are covered by the graphene nanosheet, which would effectively apply the LSPR properties for catalytic determinations. The enhancement in visible light absorption in the composite was confirmed by PL analysis, which showed greater inhibition of the electron-hole recombination process. The XRD showed a decrease in the (002) plan due to the presence of graphene, which prevents further stacking of carbon nitride layers. Accordingly, the Gr/g-C₃N₄ composite samples exhibited an enhancement in the photocatalytic performance, specifically for the 5% Gr/g-C₃N₄ sample, and close to 85% degradation was achieved within 20 min under solar irradiation. Therefore, applying the Gr/g-C₃N₄ for the degradation of a pharmaceutical can be taken into consideration as an alternative method for the removal of such pollutants during the water treatment process. This enhancement can be attributed to surface plasmon resonance-induced photocatalysis in a 2D/2D graphene/g-C₃N₄ heterostructure. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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Review

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20 pages, 2715 KiB

Open AccessReview

Recent Innovative Progress of Metal Oxide Quantum-Dot-Integrated g-C₃N₄ (0D-2D) Synergistic Nanocomposites for Photocatalytic Applications

by Tejaswi Tanaji Salunkhe, Thirumala Rao Gurugubelli, Bathula Babu and Kisoo Yoo

Catalysts 2023, 13(11), 1414; https://doi.org/10.3390/catal13111414 - 03 Nov 2023

Cited by 2 | Viewed by 1734

Abstract

Modern industrialization has unleashed unprecedented environmental challenges, primarily in the form of pollution. In response to these pressing issues, the quest for innovative and sustainable solutions has intensified. Photocatalysis, with its unique capabilities, has emerged as a potent technology to combat the adverse effects of industrialization on the environment. This review highlights recent advances in harnessing photocatalysis to address environmental pollution. Photocatalysis offers a multifaceted approach, utilizing solar energy for catalytic reactions and enabling efficient pollutant removal. Quantum dots and graphitic carbon nitride (g-C₃N₄) are essential elements in this science. In contrast to quantum dots, which have enormous potential due to their size-dependent bandgap tunability and effective charge carrier production, g-C₃N₄ has properties like chemical stability and a configurable bandgap that make it a versatile material for photocatalysis. In this review, we explore recent achievements in integrating metal oxide quantum dots with g-C₃N₄, forming nanocomposites with superior photocatalytic activity. These nanocomposites exhibit extended light absorption ranges and enhanced charge separation efficiency, positioning them at the forefront of diverse photocatalytic applications. In conclusion, this comprehensive review underscores the critical role of photocatalysis as a potent tool to counteract the adverse environmental effects of modern industrialization. By emphasizing recent advancements in g-C₃N₄ and quantum dots and highlighting the advantages of metal oxide quantum dots decorated/integrated with g-C₃N₄ nanocomposites, this work contributes to the evolving landscape of sustainable solutions for environmental remediation and pollution control. These innovations hold promise for a cleaner and more sustainable future. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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18 pages, 3138 KiB

Open AccessFeature PaperReview

Recent Advances in g-C₃N₄ Photocatalysts: A Review of Reaction Parameters, Structure Design and Exfoliation Methods

by Junxiang Pei, Haofeng Li, Songlin Zhuang, Dawei Zhang and Dechao Yu

Catalysts 2023, 13(11), 1402; https://doi.org/10.3390/catal13111402 - 28 Oct 2023

Cited by 1 | Viewed by 1832

Abstract

Graphitized carbon nitride (g-C₃N₄), as a metal-free, visible-light-responsive photocatalyst, has a very broad application prospect in the fields of solar energy conversion and environmental remediation. The g-C₃N₄ photocatalyst owns a series of conspicuous characteristics, such as very suitable band structure, strong physicochemical stability, abundant reserves, low cost, etc. Research on the g-C₃N₄ or g-C₃N₄-based photocatalysts for real applications has become a competitive hot topic and a frontier area with thousands of publications over the past 17 years. In this paper, we carefully reviewed the recent advances in the synthesis and structural design of g-C₃N₄ materials for efficient photocatalysts. First, the crucial synthesis parameters of g-C₃N₄ were fully discussed, including the categories of g-C₃N₄ precursors, reaction temperature, reaction atmosphere and reaction duration. Second, the construction approaches of various nanostructures were surveyed in detail, such as hard and soft template, supramolecular preorganization and template-free approaches. Third, the characteristics of different exfoliation methods were compared and summarized. At the end, the problems of g-C₃N₄ materials in photocatalysis and the prospect of further development were disclosed and proposed to provide some key guidance for designing more efficient and applicable g-C₃N₄ or g-C₃N₄-based photocatalysts. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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18 pages, 9751 KiB

Open AccessFeature PaperReview

S-Scheme Heterojunction Photocatalyst for Photocatalytic H₂O₂ Production: A Review

by Weili Fang and Liang Wang

Catalysts 2023, 13(10), 1325; https://doi.org/10.3390/catal13101325 - 27 Sep 2023

Cited by 2 | Viewed by 2232

Abstract

Hydrogen peroxide (H₂O₂) is a clean and mild oxidant that is receiving increasing attention. The photocatalytic H₂O₂ production process utilizes solar energy as an energy source and H₂O and O₂ as material sources, making it a safe and sustainable process. However, the high recombination rate of photogenerated carriers and the low utilization of visible light limit the photocatalytic production of H₂O₂. S-scheme heterojunctions can significantly reduce the recombination rate of photogenerated electron–hole pairs and retain a high reduction and oxidation capacity due to the presence of an internal electric field. Therefore, it is necessary to develop S-scheme heterojunction photocatalysts with simple preparation methods and high performance. After a brief introduction of the basic principles and advantages of photocatalytic H₂O₂ production and S-scheme heterojunctions, this review focuses on the design and application of S-scheme heterojunction photocatalysts in photocatalytic H₂O₂ production. This paper concludes with a challenge and prospect of the application of S-scheme heterojunction photocatalysts in photocatalytic H₂O₂ production. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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32 pages, 3747 KiB

Open AccessReview

A Brief Review on the Latest Developments on Pharmaceutical Compound Degradation Using g-C₃N₄-Based Composite Catalysts

by Subhadeep Biswas and Anjali Pal

Catalysts 2023, 13(6), 925; https://doi.org/10.3390/catal13060925 - 24 May 2023

Cited by 4 | Viewed by 1464

Abstract

Pharmaceutical compounds (PCs) are one of the most notable water pollutants of the current age with severe impacts on the ecosystem. Hence, scientists and engineers are continuously working on developing different materials and technologies to eradicate PCs from aqueous media. Among various new-age materials, graphitic carbon nitride (g-C₃N₄) is one of the wonder substances with excellent catalytic property. The current review article describes the latest trend in the application of g-C₃N₄-based catalyst materials towards the degradation of various kinds of drugs and pharmaceutical products present in wastewater. The synthesis procedure of different g-C₃N₄-based catalysts is covered in brief, and this is followed by different PCs degraded as described by different workers. The applicability of these novel catalysts in the real field has been highlighted along with different optimization techniques in practice. Different techniques often explored to characterize the g-C₃N₄-based materials are also described. Finally, existing challenges in this field along with future perspectives are presented before concluding the article. Full article

(This article belongs to the Special Issue Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion)

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Development of g-C₃N₄-Based Photocatalysts: Environmental Purification and Energy Conversion