Catalysts
·
2022
·Vol. 12
·期 3
·247
·
IF 4.501
Ping Ke,Danlin Zeng,Jiawei Cui,Xin Li,Yang Chen
A highly-efficient graphitic carbon nitride (g-C3N4) photocatalyst for visible light photodegradation of rhodamine B (RhB) and methyl orange (MO) simulating dyeing wastewater was synthesized by the thermal polycondensation of melamine. The photocatalysts were characterized by TG-DTG-DSC, XRD, EA, XPS, FT-IR, SEM, TEM, BET, PL and UV-vis DRS. The results showed that the photocatalytic performance of g-C3N4at a higher calcination temperature was significantly enhanced, and its photocatalytic activities for the photodegradation of RhB and MO were remarkably improved by 64.91% and 41.83%, respectively, which was mainly attributed to the satisfactory crystallinity, stable graphene-like structure, large surface area, and excellent optical properties. It was found that •O2−radicals and •OH radicals were the main active species for the photodegradation process by the free radicals trapping experiments and ESR analysis. The photodegradation mechanism of g-C3N4was proposed predicated using the characterization results.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 6
·1609-1618
·
IF 5.721
Chao Zhang,Jiandong Liu,Xingliang Liu,Shiai Xu
Two novel covalent bond photocatalysts, namely, g-C3N4NSs/TC1 and g-C3N4NSs/TC2 were prepared for the first time via the generation of an amide covalent bond between g-C3N4 nanosheets (g-C3N4NSs) and acyl chloride synthesized from triphenylamine-type dyes, 2-cyano-3-(4-(diphenylamino)phenyl)acrylic acid (TC1) or 3,3′-(4,4′-(phenylazanediyl)bis(4,1-phenylene))bis(2-cy-anoacrylic acid) (TC2). The experimental results indicated that triphenylamine D–π–A-type organic dye moieties covalently bonded to g-C3N4 successfully and the spectral response regions of both g-C3N4NSs/TC1 and g-C3N4NSs/TC2 could be extended from ∼460 nm to more than 600 nm. Due to the introduced amide covalent bond, the constructed g-C3N4NSs/TC1 photocatalyst showed remarkably enhanced H2 evolution activity with about 73 555.8 μmol h−1 g−1 and exhibited high apparent quantum yields (AQY) of 35.2%, 27.1%, 16.9% and 5.4% at 420 nm, 500 nm, 520 nm and 600 nm monochromatic light, respectively. Compared with the results for pure g-C3N4 NSs, about 100 times higher H2 production rate and 978 times higher AQY value were obtained for g-C3N4NSs/TC1 with the amide covalent bond under visible light irradiation. Compared to g-C3N4NSs/TC1, g-C3N4NSs/TC2 exhibited slightly lower H2 evolution activity with about 70 986.8 μmol h−1 g−1. Combining the experimental and density functional theory (DFT) calculation results, a possible mechanism can be conjectured that the electronic and geometric structures of g-C3N4NSs/TC1 are more conducive to the charge separation and the unidirectionality of electron transport in the excited state than those of g-C3N4NSs/TC2. The research reveals that this introduction of simple triphenylamine-type dyes into the surface of g-C3N4via covalent links results in a strong covalent interaction between functionalized moieties and g-C3N4 to synergistically improve the electronic and optical properties and photocatalytic performance. The present work highlights the potential use of organic dye covalent-functionalized g-C3N4via post modification as a novel photocatalyst in applications such as H2 production.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Qi Wang,Ningyi Li,Meng Tan,Man Deng,Guoxiang Yang,Qiang Li,Hao Du
Photocatalysis is an emerging technique for the remediation of refractory organic contaminants. Herein, a novel dual Z-scheme Bi/BiOI-Bi 2 O 3 -C 3 N 4 heterojunctions were constructed through a calcining process following with I − etching and UV-reduction processes. Various analytical technologies were adopted to characterize the materials. As a result, the Bi 0 decorated composite presented improved visible-light-response and rapid charge transfer. Due to the synergy of Bi 0 and dual Z-scheme heterostructures, a remarkable photocatalytic performance toward phenol degradation was achieved with the highest degradation efficiency of 93.2% and rate constant of 0.0161 min −1 over the optimal composite within 75 min of visible light irradiation. Interestingly, the concentration of the yielded benzoquinone considerably decreased with the introduction of C 3 N 4 . Trapping experiments and electron spin resonance (ESR) tests indicated that h + , O 2 − , OH and e − contributed to phenol remediation, and h + and O 2 − were the crucial species toward phenol degradation. Furthermore, outstanding stability was obtained only with a decline of 3.8% after 4 cycles. A reasonable charge transfer mechanism was also proposed. This work provides a new route for in situ construction of Bi 0 decorated dual Z-scheme heterojunction for phenolic compounds degradation.
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JOURNAL OF MOLECULAR LIQUIDS
·
2020
·
IF 5.065
Sepideh Pourhashem,Jizhou Duan,Fang Guan,Nan Wang,Ying Gao,Baorong Hou
In this research, the effects of visible-light-driven titanium dioxide (TiO 2 ) nanotube/graphitic carbon nitride (g-C 3 N 4 ) hybrids on the corrosion protection performance of epoxy coatings both in the dark and under visible-light irradiation are studied. For this, TiO 2 nanotube/g-C 3 N 4 hybrids and 3-(aminopropyl)triethoxysilane functionalized hybrids were synthesized and characterized by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy , scanning electron microscopy coupled with energy dispersive X-ray spectroscopy mapping, N 2 adsorption/desorption technique, and UV–Vis spectroscopy. TiO 2 nanotubes containing 30 wt% g-C 3 N 4 (H30%) showed the highest photocatalytic performance due to the simultaneous effects of high surface area and band-gap structure; however, the photocatalytic activity decreased after the silane functionalization of H30%. Then, epoxy coatings containing H30% and silane functionalized H30% in different amounts (0.1, 0.3, and 0.5 wt%) were prepared, and their corrosion resistance was investigated by electrochemical impedance spectroscopy in NaCl solution. The results revealed that the epoxy coatings containing 0.3 wt% hybrids have higher corrosion resistance than that of the neat coating, and silane-functionalized nanofillers more effectively enhance the corrosion resistance. However, when these nanocomposite coatings are irradiated with visible light , their corrosion protection performance remarkably reduces owing to the degradation of organic matrix by the oxidizing radicals formed on the photocatalytic hybrid surface.
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Journal of Central South University
·
2022
·Vol. 29
·期 5
·1447-1462
·
IF 2.392
Yang Ting,Hu Xin-yu,Wang Jun-tao,Yang Tian-li,Wang Wen-lei
A series of In x Sb 2− x S 3 nanosheets modified g-C 3 N 4 (In x Sb 2− x S 3 -TCN) heterojunctions with different g-C 3 N 4 contents were fabricated by an in situ deposition method. All the In x Sb 2− x S 3 -TCN composites were applied as photocatalysts in Cr(VI) polluted water treatment and the results displayed that In x Sb 2− x S 3 -TCN could effectively remove Cr(VI) under visible light through synergistic effects of adsorption and photocatalytic reduction. Especially, In x Sb 2− x S 3 -TCN-70 (70 mg g-C 3 N 4 ) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites, which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(VI) aqueous solution, and reduced Cr(VI) to Cr(III) within 10 min under visible light irradiation. DRS and PL results indicated that the interfacial coupling effect between g-C 3 N 4 and In x Sb 2− x S 3 enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination, which improved the photocatalytic activity of composites. Moreover, the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(VI) adsorption-photoreduction.
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MATERIALS CHEMISTRY AND PHYSICS
·
2016
·
IF 2.101
Fang Deng,Lina Zhao,Xule Pei,Xubiao Luo,Shenglian Luo
The g-C 3 N 4 /SnS 2 composites were prepared by in situ hydrothermal method , and the effect of g-C 3 N 4 content on the physical and chemical properties, and photocatalytic performance of g-C 3 N 4 /SnS 2 composites was investigated. The introduction of g-C 3 N 4 enhanced the visible-light absorption of SnS 2 , and reduced the recombination rate of electron-hole pairs. The photocatalytic performance of g-C 3 N 4 /SnS 2 composites was also obviously influenced by g-C 3 N 4 content, and it was found that 15% g-C 3 N 4 /SnS 2 composite exhibited the highest photocatalytic activity and excellent regeneration, which was attributed to the most efficient charge separation, the largest specific surface area and the formation of dominant active species (h + and O 2 − radicals) during the photocatalytic process.
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TALANTA
·
2024
·
IF 5.6
Xue Zhang,Yunsheng Shang,Qi Xie,Xingzhe Hu,Ke Wu,Lu-Lu Qu,Yingqiu Gu
Developing a Surface-enhanced Raman spectroscopy (SERS) method with excellent detecting ability, good recyclability and analyzing multiple pollutants rapidly are critical for evaluation of water quality in emergency pollution affairs. While constructing a multifunctional substrate with these characteristics to realize the application of SERS in water quality monitoring remains a challenge. In this work, a reusable Au@R–Fe 3 O 4 /g-C 3 N 4 SERS substrate is prepared by loading Au nanoparticles (Au NPs) on Fe 3 O 4 nanorings (R–Fe 3 O 4 ) and the formed Au@R–Fe 3 O 4 is further combined with g-C 3 N 4 nanosheets through a simple electrostatic assembly method. The Au@R–Fe 3 O 4 /g-C 3 N 4 nanocomposite presents multifunction of magnetic enrichment, SERS signal enhancement, multiple pollutants analyzing, and photocatalytic activity , which achieves quantitative detection of rhodamine B (RhB), tetracycline hydrochloride (TC), and 4-chlorophenol (4-CP), with detection limits of 5.30 × 10 −9 , 7.50 × 10 −8 , 7.69 × 10 −8 mol/L, respectively. Furthermore, the recyclable detection capability of Au@R–Fe 3 O 4 /g-C 3 N 4 for multi components is demonstrated by the strong SERS signal after 9 cycles of “detection-degradation” processes. Combined with good uniformity and stability, this SERS method based on Au@R–Fe 3 O 4 /g-C 3 N 4 substrate provides a new strategy for the multi-pollutants detection and degradation in water environment.
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高影响因子
Chemistry-An Asian Journal
·
2024
·
IF 3.5
Chunxia Yang,Hailong Cao,Fengyun Su,Mengzhen Tian,Haiquan Xie,Yezhen Zhang,Xiaoli Jin,Xin Li,Zhengdao Li
Photocatalytic H 2 evolution by water splitting is a promising approach to address the challenges of environmental pollution and energy scarcity. Graphitic carbon nitride (g-C 3 N 4 ) has emerged as a star photocatalyst because of its numerous advantages. To address the limitations of traditional g-C 3 N 4 , namely its inadequate visible light response and rapid recombination of photogenerated carriers, we employed a schiff base reaction to synthesize −C=N− doped g-C 3 N 4 . The introduction of −C=N− groups at the bridging nitrogen sites induced structural distortion in g-C 3 N 4 , facilitating n-π* electronic transitions from the lone pair electrons of nitrogen atom and extending light absorption up to 600 nm. Moreover, the presence of heterogeneous π-conjugated electron distribution effectively traps photogenerated electrons and enhances charge carrier separation. Benefiting from its expanded spectral response range, unique electronic properties, increased specific surface area, the doped g-C 3 N 4 exhibited outstanding photocatalytic H 2 evolution performance of 1050.13 μmol/g/h. The value was 5.9 times greater than the pristine g-C 3 N 4 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Guanhan Chen,Wenhui Ding,Wenyi Dong,Hongjie Wang,Shuting Zhu,Tianzhe Liang,Cheng Luo,Yuxiong Huang
The wide occurrence of pharmaceutically active contaminants (PhACs) in aquatic environments has received more and more concern owing to the associated high risks to ecosystems. Even worse, conventional wastewater treatment techniques fail to provide effective decontamination for these emerging contaminants . Herein, we designed and constructed mAg 3 PO 4 @g-C 3 N 4 heterojunction for a persulfate-assisted photocatalytic system (mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis) for the rapid and effective degradation of PhACs. Superior mineralization of CBZ (87.15 %) was achieved within 30-minute treatment with mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis, exhibiting 11-fold enhancement compared to mAg 3 PO 4 /Vis system. Integrating experimental investigations with theoretical calculations, singlet oxygen ( 1 O 2 ) was identified as the key reactive species, while the 1 O 2 -dominated ring-opening pathway contributed significantly to the high mineralization of CBZ. Moreover, mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis showed robust degradation performance of multiple PhACs across various water matrices. Multiple PhACs could be simultaneously degraded with high mineralization efficiency in the wastewater effluent, demonstrating the promising application of mAg 3 PO 4 @g-C 3 N 4 /PDS/Vis for decontaminating emerging contaminants in wastewater treatment .
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ChemSusChem
·
2024
·
IF 7.5
Dong Li,Kaixuan Wang,Ying Chen,Renyi Li,Jiahong Tang,Yizhou Zhao,Wei Guo,Qi Chen,Yujing Li
Graphical A 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is synthesized by immobilizing CsPbBr 3 (CPB) quantum dots on one-dimensional porous tubular g-C 3 N 4 (TCN). The strong Pb−N chemical bonding between CPB quantum dots and TCN provides a fast charge transfer channel for the CPB@TCN, which promotes the efficient separation and transfer of photogenerated carriers, resulting in excellent photocatalytic activity. Halide perovskite CsPbBr 3 (CPB) quantum dots (QDs) are considered as a promising candidate for solar-driven CO 2 conversion for their unique optoelectronic properties and suitable band structures. However, the CO 2 conversion efficiency of pristine CsPbBr 3 quantum dots is severely limited due to their rapid electron-hole pair recombination and insufficient active sites. In this study, by immobilizing CPB QDs onto one-dimensional (1D) porous tubular g-C 3 N 4 (TCN), an effective 0D/1D CPB@TCN heterojunction photocatalyst for CO 2 reduction is fabricated. Density functional theory (DFT) calculations combined with experimental studies demonstrate that CPB QDs are uniformly anchored on the surface of TCN through Pb−N chemical bonding, resulting in efficient separation and transfer of photogenerated carriers in CPB@TCN photocatalysts. The resultant CPB@TCN photocatalysts exhibit significantly enhanced photocatalytic activity for CO 2 reduction with the highest conversion rate of 22.62 μmol g −1 h −1 , which is 5.33-times higher than that of pristine CPB QDs. This work unveils the interfacial bonding mechanism of CPB@TCN heterojunction through Pb−N chemical bond, which provides new insights for the development perovskite-based heterojunction photocatalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Na Wang,Yibo Zhang,Zelin Meng,Mingyang Song,Heming Zhao,Yang Wang,Shuai Bai,Jianglei Hu,Fengwei Shi,Xia Yang
Addressing the low surface area and high charge recombination of graphitic carbon nitride (g-C 3 N 4 ), this study employs a synergistic carboxylation and MOF-loading strategy. Copper-based MOF (Cu-MOF) was uniformly loaded onto carboxylated spherical g-C 3 N 4 (C 3 N 4 –C) via a solvothermal method, creating a visible-light-responsive C 3 N 4 –C-MOF photocatalyst. Material characterization results indicate that the characteristic peak at 1632 cm −1 in the Fourier Transform Infrared Spectroscopy confirms the successful grafting of 4-carboxybenzoic acid (4-CBA). Carboxylation enhanced hydrophilicity and optimized surface charge, improving reactant adsorption. Photoelectrochemical tests showed significantly boosted visible light absorption, increased photocurrent density, and reduced EIS arc radius, confirming efficient interfacial charge separation. Photocatalytic hydrogen production experiments revealed that under simulated solar irradiation, the hydrogen production rate of C 3 N 4 –C-MOF2.0 reached up to 12.68 mmol g −1 h −1 , representing an approximately 1.68-fold increase compared to the unmodified C 3 N 4 -MOF. This work provides a novel approach for designing MOF/functionalized g-C 3 N 4 composites, advancing solar-driven hydrogen production.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2014
·
IF 2.235
Fa-tang Li,Ya-bin Xue,Bo Li,Ying-juan Hao,Xiao-jing Wang,Rui-hong Liu,Jun Zhao
Mesoporous γ-Al2O3 with high surface area (159 m2/g) is prepared via a precipitation method. The as-synthesized Al2O3 exhibits optical absorption ability in the ultraviolet region and is used as the active component to be combined with g-C3N4 to form effective heterostructured photocatalysts. This heterojunction structure is confirmed by X-ray diffraction, scanning electron microscopy, element map, transmission electron microscopy, high-resolution transmission electron microscopy, Fourier transform infrared, and X-ray photoelectron spectroscopy measurements. The photocatalytic performances of the composites are evaluated by the degradation of rhodamine B (RhB) and methyl orange (MO). Among the prepared photocatalysts, 2g-C3N4:1Al2O3 (weight ratio) exhibits the highest photocatalytic activity, the reaction rate constant of which is 2.5 and 3.7 times that of pure g-C3N4 in degradation of RhB and MO, respectively. The enhancement in activity of heterojunctions is ascribed to their high specific surface areas, excellent adsorption abilities for dyes, and efficient transfer of photogenerated electrons from the lowest unoccupied molecular orbital of g-C3N4 to the defect sites of γ-Al2O3.
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