MICROCHIMICA ACTA
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2020
·Vol. 187
·期 2
·1-10
·
IF 6.232
Zhang Lihui,Liu Candi,Wang Qiwen,Wang Xiaohong,Wang Shengtian
Two-dimensional porous graphitic carbon nitride (g-C 3 N 4 ) nanosheets were synthesized by low-cost and direct thermal oxidation. Porous g-C 3 N 4 assembled with graphene oxide (GO) was immobilized on a glassy carbon electrode. The sensor was applied to simultaneous determination of ascorbic acid (AA), dopamine (DA) and uric acid (UA) with high performance. Cyclic voltammetry and differential pulse voltammetry were used to investigate electrochemical and electrocatalytic properties. The results indicate that the electrochemical sensor possesses high specific surface area, hierarchical pore structure and excellent signal response to AA, DA and UA. The oxidation potentials are well separated at around 0.15, 0.34 and 0.46 V for AA, DA and UA respectively. The determination limits for AA, DA and UA are 3.7 μM, 0.07 μM and 0.43 μM, respectively. The sensor was applied to tracking the three analytes in spiked serum samples with recovery 95.1~105.5% and relation standard deviations of less than 5%.
Schematic representation of porous graphitic carbon nitride nanosheet embedded in graphene oxide for simultaneous determination of ascorbic acid, dopamine and uric acid.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 25
·10141-10150
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IF 3.069
Bin Zhao,Baogang Wang,Hongsheng Lu,Shanshan Dai,Zhiyu Huang
Ionic liquid modified CDs and novel thin nanosheets constructed graphitic carbon nitride (g-C3N4) microspheres were synthesized by the template method and by calcination of a supramolecular precursor, respectively. The CDs were decorated onto the surface of g-C3N4 by solvothermal treatment to tune the visible-light photocatalytic degradation performance of g-C3N4. The CDs could not only form heterojunctions with g-C3N4 by chemical bonding, π–π stacking and electronic attraction interactions, but also change the surface charges of g-C3N4 from negative to positive. The roles played by heterojunctions and surface charges in the photocatalytic performance of CDs (1.6 wt%)/g-C3N4 composites were explored by photocatalytic degradation of anionic (methyl orange, MO), nonionic (p-nitrophenol, p-NP) and cationic (methylene blue/rhodamine B, MB/RhB) pollutants. Compared with g-C3N4, the composite showed obviously higher and lower photocatalytic activity for MO/p-NP and MB/RhB degradation, respectively. These results demonstrated that the surface charges might play a positive or negative but dominant role by enhancing or inhibiting the absorption of pollutant molecules despite the fact that heterojunctions always played a positive role by promoting the light-harvesting ability and separation efficiency of photo-generated electron–hole pairs of g-C3N4.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Suqian Xu,Hanxu Zhu,Wenrui Cao,Zhibin Wen,Jinnan Wang,Corvini Philippe François-Xavier,Thomas Wintgens
Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots were synthesized for the first time to enhance the catalytic activity and utilization of H 2 O 2 . SEM, TEM, XPS, FT-IR, XRD, TPR and solid-state EPR were used to characterize the catalysts. In the Cu-Al 2 O 3 -g-C 3 N 4 system, the electron-rich centre of Cu and electron-deficient site of Al were formed due to the higher electronegativity of Cu. Moreover, Cu ions could coordinate with the hydroxyl on the tri-s-triazine ring of g-C 3 N 4 or the graphene conjugated π-domains of C-dots via the Cu O C linkage so that the orbital interactions involving electron transport from π → Cu also induced the formation of an electron-rich Cu centre and an electron-deficient π-electron conjugated system, resulting in the strengthening of the dual-reaction centres. This mechanism was validated by Roman, EPR and XPS spectra. In addition, EPR experiments demonstrated that two electron-transfer processes formed OH in the presence of H 2 O 2 . The first electron transfer was from the electron-rich Cu centres to H 2 O 2 , and the other was from H 2 O to the electron-deficient site. Thus, more OH were generated and high H 2 O 2 utilization was achieved in the Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots suspension. Furthermore, the turnover frequency (TOF) for the Cu-Al 2 O 3 -C-dots and Cu-Al 2 O 3 -g-C 3 N 4 dispersions were determined and were found to be much higher than those of the classic homogeneous Fenton reaction. Thus, Cu-Al 2 O 3 -g-C 3 N 4 and Cu-Al 2 O 3 -C-dots showed high activity and stability for the catalytic degradation of organic pollutants under mild conditions.
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ANALYTICA CHIMICA ACTA
·
2018
·
IF 5.123
Fenghe Duan,Shuai Zhang,Longyu Yang,Zhihong Zhang,Linghao He,Minghua Wang
A novel nanostructured biosensing platform was designed based on two-dimensional (2D) nanocomposite of graphitic carbon nitride (g-C 3 N 4 ) nanosheets and MoS 2 quantum dots (MoS 2 QDs), followed by decoration with chitosan-stabilized Au nanoparticles (CS-AuNPs) (denoted as MoS 2 [email protected] 3 N 4 @CS-AuNPs), of which CS-AuNPs were prepared by plasma enhanced-chemical vapor deposition. Owning to the good surface plasmon performance of the CS-AuNPs and excellent electrochemical activity of MoS 2 [email protected] 3 N 4 nanosheets, the as-obtained 2D MoS 2 [email protected] 3 N 4 @CS-AuNPs nanocomposite was simultaneously explored to construct both surface plasmon resonance spectroscopy (SPR) sensor and electrochemical aptasensor . The MoS 2 [email protected] 3 N 4 @CS-AuNPs-based aptasensor shows strong bio-binding affinity toward the prostate specific antigen (PSA) targeted aptamer strands as compared to the individual component, including MoS 2 QDs, g-C 3 N 4 , and CS-AuNPs. When detecting PSA, the low limit of detection (LOD) of 0.71 pg mL −1 deduced by electrochemical aptasensor is three orders of magnitude lower than that deduced by SPR sensor (0.77 ng mL −1 ). As expected, both SPR sensor and electrochemical aptasensor demonstrate good selectivity , highly stability, acceptable reproducibility, and well consistent applicability in human serum. The satisfactory results suggest potential application of the MoS 2 [email protected] 3 N 4 @CS-AuNPs in bifunctional biosensing fields and clinical monitoring of cancer markers.
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CHINESE JOURNAL OF CATALYSIS
·
2017
·
IF 2.813
Zhenxing Zeng,Kexin Li,Kai Wei,Yuhua Dai,Liushui Yan,Huiqin Guo,Xubiao Luo
A series of highly dispersed platinum-deposited porous g-C 3 N 4 (Pt/pg-C 3 N 4 ) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g-C 3 N 4 as precursors. Porous g-C 3 N 4 was fabricated by a pretreatment strategy using melamine as a raw material. The morphology, porosity, phase, chemical structure, and optical and electronic properties of as-prepared Pt/pg-C 3 N 4 were characterized. The photocatalytic activity of as-prepared Pt/pg-C 3 N 4 was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as-prepared Pt/pg-C 3 N 4 were further applied to the degradation and mineralization of aqueous 4-fluorophenol. The recyclability of Pt/pg-C 3 N 4 was evaluated under four consecutive photocatalytic runs.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zishui Dong,Sinuo Li,Eldon R. Rene,Yixuan Liu,Weifang Ma
2,4,6-Trichlorophenol (2,4,6-TCP) is commonly used in the production of insecticides and preservatives with the characteristics of accumulation and toxicity due to the complex chemical structure with a halogenated aromatic ring. In order to effectively degrade and mineralize 2,4,6-TCP from water, a stack-coral-like catalyst of magnetic sulfur doping constructed nitrogen vacancies in graphitic carbon nitrides (Fe 3 O 4 /S-g-C 3 N 4 , FSCN-T) was designed and prepared through polymerization combined with precipitation. This visible-light-driven photocatalytic degradation to 5 mg/L 2,4,6-TCP was 95 % within 60 min with 0.1 g/L FSCN-T amendment. The degradation and carbonization rate constant were 0.118 and 0.089 min −1 respectively. This high removal was attributed to nitrogen vacancies, which broaden the visible light absorption range and shorten the electron transfer path with narrow CN bandgap (from 2.94 eV to 2.49 eV). Moreover, the introduction of iron accelerated electron cycling and enhanced magnetic recovery performance with above 95 % recovery and catalytic stability after 5 cycles of use. The degradation contribution from the active species were h + (41 %)> •OH (28.9 %) > •O 2 - (16.1 %)> 1 O 2 (8.7 %). This degradation underwent three pathways of substitution, elimination, and hydroxyl oxidation. Further, the intermediates were oxidized with ring opening and mineralization according to density functional theory (DFT) calculations and LC-Qtof-MS identification. The oxidative degradation process reduced the toxicity of 2,4,6-TCP and its intermediates. This study provided an efficient catalyst and low-energy consumption approach for toxic wastewater treatment.
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JOURNAL OF MOLECULAR LIQUIDS
·
2024
·
IF 5.3
Tianqi Liu,Hailian Huang,Yunzong Liu,Konstantinos Papadikis,Beata Layla Mehdi,Pow-Seng Yap,Graham Dawson
A novel magnetic quinary nanocomposite, protonated g-C 3 N 4 /Fe 3 O 4 /AgBr/AgCl/AgI, was synthesized using a wet chemical method. The multi-heterojunction photocatalyst with multi carrier source and multi-channel carrier transport is constructed to enhance the photocatalytic degradation performance of pure g-C 3 N 4 . The design of the quinary nanocomposite is also an effective approach solving the chemical stability problem of silver halides. The photocatalytic degradation efficiency under visible light irradiation was analyzed for methylene blue (MB) as the target organic pollutant. The quinary nanocomposite with 10 % g-C 3 N 4 displayed high photocatalytic performance, with 83 % of MB degraded under 6 h LED white light irradiation. The effective quinary nanocomposite has good magnetic properties and can be magnetically separated to prevent secondary pollution of the photocatalyst in water. The band gap of protonated g-C 3 N 4 /Fe 3 O 4 /AgBr/AgCl/AgI was found to be lower than pure g-C 3 N 4 . Parameters such as initial concentration of pollutant, initial solution pH, and light source were studied. Zeta potential results showed that the quinary nanocomposite could disperse homogenously to decrease aggregation in the solution. The photocatalytic mechanism was investigated, and the mineralization results were analyzed based on liquid chromatography-mass spectroscopy (LC-MS) and total organic carbon (TOC). It was found that the hydroxyl and superoxide radicals were major reactive species by scavenging experiments. Additionally, protonated g-C 3 N 4 /Fe 3 O 4 /AgBr/AgCl/AgI nanocomposite showed excellent reusability after magnetic separation and regeneration, thus suggesting it to be a promising photocatalyst for treating wastewater containing organic contaminants.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yaxin Li,Wei Qin,Xinyang Li,Qi Zhu,Fu-quan Bai,Tao Tian
It is highly desirable to enhance the charge separation and introduce catalytic functions for efficient water splitting into hydrogen on g-C 3 N 4 . Herein, heterojunctions of PCN-222(M)/g-C 3 N 4 -AA were successfully synthesized through the in-situ hydrothermal method, where metallic ions (M) were strategically incorporated into porphyrinic metal-organic framework (MOF) ligands. This heterojunction design strategy is considered to establish directional charge transfer channels for photogenerated electron-hole (e − -h + ) pairs and thereby enhance its separation efficiency. Remarkably, the 1 % PCN-222(Pd)/g-C 3 N 4 -AA composite demonstrated superior photocatalytic hydrogen evolution performance, achieving a rate of 2338.17 μmol·g −1 ·h −1 . This rate was 3.23 times higher than that of pure g-C 3 N 4 and 2.79 times higher than that of g-C 3 N 4 -AA. The composite morphology was characterized by a series of physicochemical properties. Bandgap analysis via Tauc plot revealed that metal ion doping in the porphyrin center effectively modulates the HOMO-LUMO levels at the composite interface. First-principles calculations coupled with hydrogen adsorption free energy analysis elucidated how interfacial engineering between PCN-222(M) and g-C 3 N 4 -AA governs heterostructure formation and charge transfer pathways. This work systematically deciphers the synergistic effects of bimetallic MOF integration and provides insights into the underlying photocatalytic reaction mechanism.
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ACS Applied Optical Materials
·
2023
·
IF 0
Xiaoya Bu,Yan-gai Liu,Ci’an Xie,Baochen Wang
The long-afterglow luminescent material Sr2MgSi2O7:(Eu, Dy) was combined with the photocatalytic material g-C3N4 to construct a type of Sr2MgSi2O7:(Eu, Dy)/g-C3N4 self-luminous photocatalytic composite. This overcomes the limitation that photocatalytic experiments can only be carried out under an external light source, and it provides a more flexible way to use photocatalytic technology in environmental purification. The morphology, structure, luminescence, and photocatalytic properties of the samples were investigated using a variety of advanced characterization techniques. The results show that the significant improvement in the photocatalytic performance is attributed to the formation of a Z-scheme heterojunction between the luminescent and photocatalytic materials and the promotion of the photocatalytic reaction by the properties of the long-afterglow luminescent material itself. A possible mechanism for the photocatalytic process of the composite is proposed, and it is speculated that the reason for the increased photocatalytic activity is internal electron transfer and electron–hole pair separation based on tests such as X-ray photoelectron spectroscopy and density functional theory calculations. This study provides a strategy for enhancing the photocatalytic activity of photocatalysts and achieving round-the-clock degradation of pollutants.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Shihui Zhang,Xu Zhang,Wanting Shi,Weiyan He,Caihong Li,Xiaojing Wang
Slow charge transfer and a weak built-in electric field (BIEF) at the heterojunction interface critically hinder the construction of efficient S-scheme heterojunctions. Secondary calcination and ultrasonic treatment of g-C 3 N 4 enhance interfacial contact with MIL-101, shortening carrier migration paths. P and Mn doping increases the Fermi-level difference between g-C 3 N 4(C,S) and MIL-101, strengthening the BIEF to drive directional carrier migration. This facilitates the recombination of carriers with low-redox-potential at the heterojunction interface while spatially separating carriers with high-redox-potential, successfully constructing an S-scheme P-Mn-MCN (C,S) heterojunction. The optimized system delivers remarkable photocatalytic performance, achieving 98 % tetracycline hydrochloride degradation under visible light within 60 min.
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RSC Advances
·
2020
·Vol. 10
·期 33
·19169-19177
·
IF 3.119
Biao Zhou,Bo Yang,Muhammad Waqas,Ke Xiao,Caizhen Zhu,Ling Wu
Constructing a 0D/3D p–n heterojunction is a feasible strategy for accelerating photo-induced charge separation and promoting photocatalytic H2 production. In this study, a 0D/3D MoS2/g-C3N4 (0D/3D-MCN) photocatalyst with a p–n heterojunction was prepared via a facile light-assisted deposition procedure, and the 3D spongy-like g-C3N4 (3D-CN) was synthesized through simple thermolysis of NH4Cl and melamine mixture. For comparison, 2D-MoS2 nanosheets were also embedded in 3D-CN by a solution impregnation method to synthesize a 2D/3D-MCN photocatalyst. As a result, the as-prepared 0D/3D-MCN-3.5% composite containing 3.5 wt% 0D-MoS2 QDs exhibited the highest photocatalytic H2 evolution rate of 817.1 μmol h−1 g−1, which was 1.9 and 19.4 times higher than that of 2D/3D-MCN-5% (containing 5 wt% 2D-MoS2 nanosheets) and 3D-CN, respectively. The results of XPS and electrochemical tests confirmed that a p–n heterojunction was formed in the 0D/3D-MCN-3.5% composite, which could accelerate the electron and hole movement in the opposite direction and retard their recombination; however, it was not found in 2D/3D-MCN-5%. This study revealed the relationship among the morphologies of MoS2 using g-C3N4 as a substrate, the formation of a p–n heterojunction, and the H2 evolution activity; and provided further insights into fabricating a 3D g-C3N4-based photocatalyst with a p–n heterojunction for photocatalytic H2 evolution.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2025
·
IF 5.4
Xiangta Xie,Yuyan Feng,Dongbo Wang
A novel in-situ grown α-Bi 2 O 3 /Bi 2 O 2 CO 3 /g-C 3 N 4 heterojunction (BBCx) was successfully fabricated via a two-step in-situ growth by a simple solvothermal calcination method. In this process, g-C 3 N 4 served as the substrate for the growth of Bi 2 O 2 CO 3 nanoplates, while Bi 2 O 2 CO 3 acted as the substrate for the subsequent growth of α-Bi 2 O 3 nanoplates. By characterizing the nanocomposite using different techniques, it was confirmed that the components of this ternary material are tightly bonded through heterojunction formation. Photocatalytic tests demonstrated that the composite exhibited higher activity than pure α-Bi 2 O 3 , Bi 2 O 2 CO 3 and g-C 3 N 4 . Among the composite materials, BBC400—obtained by solvothermal treatment followed by calcination at 400 °C for 2 h—exhibited the highest degradation efficiency toward tetracycline hydrochloride (TC-HCl), with a removal rate of 70% of TC-HCl within 120 min and a rate constant of 0.0081 min −1 . This rate constant was approximately 16.2 times (0.0005 min −1 ), 1.92 times (0.0042 min −1 ) and 1.35 times (0.006 min −1 ) higher than those of pure Bi 2 O 2 CO 3 , g-C 3 N 4 and α-Bi 2 O 3 , respectively. This synthesis approach offers a new strategy for the in-situ construction of heterojunction nanocomposites.
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