APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Liang-pei Hou,Rong-xiang Zhao,Xiu-ping Li,Xiao-han Gao
A series of catalysts of composition X -MoO 2 /g-C 3 N 4 ( X = 0, 0.5, 1, 3, 5 wt.%) were successfully synthesized by calcination of a mixture of (NH 4 ) 6 Mo 7 O 24 ·4H 2 O and g-C 3 N 4 . Oxidative desulfurization experiments were conducted using X -MoO 2 /g-C 3 N 4 as a catalyst, H 2 O 2 as an oxidant, and ionic liquids (ILs) as extraction agents. Catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier-transform infrared (FT-IR), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), and Brunauer-Emmett-Teller analysis (BET). Characterization results suggested that MoO 2 was present in the catalyst and its crystallinity improved with increased Mo-loading. The catalysts had a larger specific surface area due to the presence of MoO 2 dispersed on g-C 3 N 4 . Experimental results showed that 3%-MoO 2 /g-C 3 N 4 had the highest catalytic activity among all the catalysts tested. A desulfurization rate of 96.0% was achieved under optimal conditions. Through gas chromatography-mass spectrometry (GC–MS) analysis, it was shown that dibenzothoiphene sulfone was the sole product of the oxidation desulfurization reaction. An apparent activation energy of 61.1 kJ/mol was estimated based on Arrhenius equation. The activity of 3%-MoO 2 /g-C 3 N 4 slightly decreased after six runs. A possible mechanism for the reaction has been proposed.
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Journal of Water Process Engineering
·
2023
·
IF 7
Guobin Li,Zhenbang Han,Tao Wang,Minghui Zhang,Qiaoqiao Liu,Tong Zhang,Xiaoming Zhao
Fe-doped graphitic carbon nitride (g-C 3 N 4 ) represents an attractive photo-Fenton catalyst for organic contaminants removal, but the practical performances still need to be improved for large-scale application. Herein, we developed a high-efficiency photo-Fenton catalyst by anchoring Fe-g-C 3 N 4 onto an amidoxime-functionalized polyacrylonitrile fiber (AP) substrate through a simple hydrothermal approach. Comprehensive characterizations demonstrate the strong catalyst-support interaction via the axial coordination bonding between -OH groups and Fe 3+ , which could induce electric polarization of Fe-g-C 3 N 4 to promote the H 2 O 2 adsorption and activation. The fibrous support could also accelerate the photoelectrons transfer from g-C 3 N 4 to Fe 3+ by strengthening the d-π conjugated large π bond, as well as alleviate the backflow recombination from Fe 3+ to g-C 3 N 4 through the electron sink effect. These synergistic qualities resulted in superior photo-Fenton performance for organic contaminants removal, which delivered 4.0-fold higher degradation kinetics than that of the Fe doped g-C 3 N 4 powder catalyst and exhibited unexpected high activity at strong basic environment (pH = 12). Our work demonstrates an ingenious and simple way to design exceptional photo-Fenton catalysts for environmental remediation.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 12
·3270-3278
·
IF 5.726
Dan Liu,Chengwei Qiu,Minbo Li,Yanyu Xie,Lu Chen,Huaxiang Lin,Jinlin Long,Zizhong Zhang,Xuxu Wang
Kornblum oxidation (benzyl bromide to benzaldehyde) can be realized efficiently by NaOH-modified graphitic carbon nitride (g-C3N4). Different from the oxidation reaction carried out at high temperature using DMSO as an oxidant, our reaction is eco-friendly because it is carried out at room temperature under LED light irradiation using molecular oxygen as an oxidant, which avoids the problems of toxicity, pollution and purification. Alkali treatment leads to the surface deprotonation of g-C3N4 to form NaOH-modified g-C3N4 (Na/g-C3N4). The modifications of the electronic structure and surface chemical environment of g-C3N4 facilitate light absorption and formation of ˙O2− and therefore make the conversion of benzyl bromide reach up to 99%. This work demonstrates a green and sustainable route for benzaldehyde production and the superiority of g-C3N4 for organic syntheses.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Lei Cui,Siliang Liu,Fangke Wang,Jingyao Li,Yanhua Song,Ye Sheng,Haifeng Zou
In this work, uniform g-C 3 N 4 shells have grown on the surface of electrospinning TiO 2 nanofibers to form one dimensional core/shell structured TiO 2 /g-C 3 N 4 nanofibers by a facial melamine-involved vapor deposition approach. During the heat treatment process in a simple setup, the TiO 2 nanofibers served as supports to prevent the collapses and aggregations of g-C 3 N 4 while forming heterojunctions with g-C 3 N 4 at the interface. The as prepared heterogeneous TiO 2 /g-C 3 N 4 photocatalyst exhibited remarkably enhanced visible light photocatalytic activity for RhB degradation by maxing heterojunctions at the core/shell interface. The photodegradation reaction rate constant of the obtained heterojunction is 0.064 min −1 , which is 4.0 times that of pure g-C 3 N 4 (0.016 min −1 ). To reach higher RhB degradation efficiency (>90%), TiO 2 /g-C 3 N 4 shortened the irradiation time by 60 min compared with individual components (pure g-C 3 N 4 or TiO 2 nanofibers). The remarkably high photocatalytic performances are mainly ascribed to the synergetic effect of efficient photogenerated charge separation properties and decreased electron transfer resistance of the heterojunctions formed between g-C 3 N 4 and TiO 2 . We believe the proposed simple method and setup is an attractive strategy for constructing one dimensional g–C 3 N 4 –based nano-heterojunctions with excellent photocatalytic properties.
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Catalysts
·
2022
·Vol. 12
·期 9
·998
·
IF 4.501
Mengfan Niu,Liyun Cao,Qianqian Liu,Xiaoyi Li,Qian Chen,Dinghan Liu,Wenbin Li,Jianfeng Huang,Liangliang Feng
Exploring low-cost and highly active, cost-effective cocatalysts is of great significance to improve the hydrogen evolution performance of semiconductor photocatalysts. Herein, a novel ultrasmall V-doped NiP2nanoparticle, as an efficient cocatalyst, is reported to largely upgrade the photocatalytic hydrogen evolution reaction (HER) of g-C3N4nanosheets under visible-light irradiation. Experimental results demonstrate that V-NiP2cocatalyst can enhance the visible-light absorption ability, facilitate the separation of photo-generated electron-hole pairs and boost the transfer ability of electrons of g-C3N4. Moreover, the V-NiP2/g-C3N4hybrid exhibits prominent photocatalytic HER activity 17 times higher than the pristine g-C3N4counterpart, even outperforming the 1 wt.% platinum-loaded g-C3N4. This work displays that noble-metal-free V-NiP2cocatalyst can serve as a promising and efficient alternative to Pt for high-efficiency photocatalytic H2evolution.Keywords:g-C3N4;cocatalyst;V-NiP2;photocatalyst;hydrogen evolution reaction
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Zhikun Huang,Haojie Yu,Li Wang,Xiaowei Liu,Shuning Ren,Jinyi Liu
Designing graphitic carbon nitride (CN) based heterostructured photocatalysts with high catalytic activity is highly desired for peroxymonosulfate (PMS) activation to degrade organic pollutants from water. Herein, a novel heterostructured composite (U-F@CN) consisting of ferrocene-modified Uio-66-NH 2 (U-F) and CN was synthesized. The U-F@CN exhibited superior photocatalytic performance to degrade bisphenol A (BPA) in the presence of PMS under visible light. The experimental results indicated that BPA could be removed entirely by U-F@CN within 60 min under visible light irradiation. In addition, the outstanding photocatalytic activity could be maintained at high level in a wide pH range, appropriate temperature region and natural water condition. Benefiting from the good chemical stability, outstanding optical property and in-situ generation of interfacial heterojunction of U-F@CN, the interfacial transport of photogenerated charges could follow the Z-scheme mechanism, which can accelerate the charge separation and transport to yield abundant reactive active species (ROS) to efficiently active PMS and under visible light. This work provides a novel approach to design CN-based heterostructured photocatalysts with high stability and superior photocatalytic activity for environmental remediation.
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CRYSTENGCOMM
·
2023
·
IF 3.1
Yujie Jia,Shuhan Jiang,Qianchen Ou,Yanan Liu,Jian Zhang,Yangjie Zhou,Yuan Lian,Hongmei Wang
NiFe-LDH/g-C3N4 (LDH/CN) heterostructures with different amounts of NiFe-LDH (LDH) were prepared by a hydrothermal method and characterized using different experimental techniques. Their photocatalytic properties were investigated using the degradation of tetracycline hydrochloride (TC) and the production of hydrogen from water splitting. Experimental results showed that the hydrogen production rate (780.5 μmol g−1 h−1) was 2.29 times that of pristine CN, and the TC removal rate (76.3%) of 1.8LDH/CN was 3.71 times that of CN. According to the detailed study of the structural, optical, and photoelectrochemical properties, a type II charge transfer mechanism was proposed to explain the improved photocatalytic performance of LDH/CN.
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LANGMUIR
·
2022
·
IF 4.331
Zhenyu Zhao,Xuting Wang,Shifu Wang,Zuoyi Xiao,Shangru Zhai,Jiliang Ma,Xiaoli Dong,Haodong Sun,Qingda An
The development of g-C3N4-based photocatalysts with abundant active sites is of great significance for photocatalytic reactions. Herein, a smart and robust strategy was presented to fabricate three-dimensional (3D) g-C3N4 nanosheet-coated alginate-based hierarchical porous carbon (g-C3N4@HPC), including coating melamine on calcium alginate (CA) hydrogel beads, freeze-drying hydrogel beads as well as pyrolysis at high temperatures. The resulting photocatalyst possessed a significantly high surface area and a large amount of interconnected macropores compared with porous carbon without the melamine coating. The unique structural features could effectively inhibit the curling and agglomeration of g-C3N4 nanosheets, provide abundant photocatalytic active sites, and promote mass diffusion. Therefore, the g-C3N4@HPC composite exhibited remarkable photocatalytic activity and outstanding stability toward the photoreduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) by NaBH4 under natural sunlight and simulated visible-light irradiation (λ > 420 nm) using a 300 W xenon lamp. Moreover, the mechanism toward the photocatalytic reaction was extensively studied by quenching experiments and electron spin resonance (ESR) experiments. The results showed that active hydrogen species were able to be achieved by following a dual-channel pathway in the NaBH4 system, which included photocatalytic reduction of H+ ions and photocatalytic oxidation of BH4– ions. This work not only opens up a new way to design efficient photocatalysts for various reactions but also provides a reference for an in-depth study of the photoreduction mechanism.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chenjie Ding,Shifei Kang,Wenxin Li,Weikang Gao,Zhihao Zhang,Lulu Zheng,Lifeng Cui
Heterogeneous photo-Fenton catalysts prepared by doping metal ions in g-C 3 N 4 are promising alternatives to traditional homogeneous Fenton catalysts, but are restricted by poor mesoporous structure and agglomerate of metal species. Recently, the highly uniformly dispersed metal-N active sites in various photocatalysts have been proved to be the critical reason for their enhanced catalytic activity. In this study based on reasonable control of mesoporous structure and metal-N active sites, mesoporous Fe-g-C 3 N 4 was synthesized using a simple one-step thermal shrinkage polymerization method using ferrous oxalate as iron source and pore-forming agent. The Fe and N elements in the triazine ring skeleton of Fe-g-C 3 N 4 form a σ-π bond, thus the photogenerated electrons can be quickly transferred to Fe 3+ to form Fe 2+ under the interaction of chemical bonds, accelerating the Fenton reaction rate. Density functional theory calculations results demonstrate that the energy band structure and electron cloud density distribution of Fe-Nx active structure are better than that of routine FeOx crystal structure with metal species agglomeration. In addition, the excellent mesoporous structure of Fe-g-C 3 N 4 creates conditions for the high exposure of Fe-Nx active sites in the photo-Fenton reaction under visible light. The as-developed Fe-g-C 3 N 4 system shows high recyclability and excellent photo-Fenton performance for removal of typical intractable pollutants (The degradation rate of dye and tetracycline reaches 98.2% and 98.7% at 60 and 120 min, respectively). This work provides a facile and sustainable route to develop mesoporous highly-active heterogeneous Fenton-like catalysts and even further general the design of general catalyst with ideal metal-N active sites, thereby promoting a feasible and efficient wastewater remediation solution.
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PubMed
高影响因子
Current Analytical Chemistry
·
2024
·Vol. 20
·期 3
·183-190
·
IF 1.7
Ma Yue,Liu Xuqiao,Yan Kai,Zhang Jingdong
Background: 17β-estradiol (E2) is a steroid hormone that has the potential to disrupt the endocrine system, leading to adverse effects on both humans and ecosystems, even when present in low concentrations. The quantitative determination of E2 is of great practical significance.
Hypothesis: Electrochemical methods offer several advantages, including low cost, ease of operation, and potential for miniaturization, which makes them suitable for on-field detection applications. Methods: This research developed a miniaturized electrochemical sensor utilizing
graphitic carbon nitride (g-C3N4) assembled on an AuNPs/ITO film electrode for sensitive voltammetric detection of a steroid hormone, E2. Results: Compared with AuNPs/ITO electrodes, the g-C3N4/AuNPs/ITO exhibits higher sensitivity for voltammetric
detection of E2. Under optimal conditions, the differential pulse voltammetric response on the g-C3N4/AuNPs/ITO electrode was proportional to E2 concentration in the 25 ~ 600 μmol/L range, with a detection limit of 6.5 μmol/L. Conclusion: The proposed g-C3N4/AuNPs/ITO
electrode exhibited a wide linear range, good selectivity, and practical applicability for determining E2 in environmental water samples with acceptable recovery.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Wenjie Tian,Xiongxiong Zeng,Wencong Liu,Lei Mao,Fen Guo,Yang Gui,Lan Yuan
Constructing a dual-functional photoredox system coupling fine-chemical synthesis with hydrogen peroxide (H 2 O 2 ) production provides an intriguing and eco-friendly protocol for advancing sustainable practical applications. Herein, we present a facile one-pot strategy for fabricating a porous N-rich g-C 3 N 4 /g-C 3 N 5 heterojunction (denoted as pN-N 4 -N 5 ) using mixed melamine and 3-amino-1,2,4-triazine as the precursors with NH 4 Cl as a penetrant for in-situ structure engineering. The resultant metal-free pN-N 4 -N 5 exhibited a remarkable performance of H 2 O 2 generation rate of 2.71 mmol g −1 h −1 with simultaneous production of industrially important 2-phenylbenzimidazole (2-BZ) under visible light and open air, along with a yield of 97 % and selectivity of > 99 %, outperforming most of the reported carbon nitride-based reaction systems for single-functional H 2 O 2 or 2-BZ synthesis. Extensive characterizations and density functional theory (DFT) studies revealed that such a heterojunction with well-matched band structure, enlarged interlayer space and enriched amino groups on the catalyst surface enables the facilitated spatially oriented charge flow, efficient mass transfer and reactants activation, thus offering an efficient and sustainable platform to furnishing the three-in-one photoredox systems to produce bidirectional valuable products.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chuanxin Teng,Qingli Xie,Rongping Yang,Shiji Deng,Kaiwei Li,Hanli Qiao,Xuehao Hu,Libo Yuan,Xiaogang Xue
Tetracycline (TC) detection is crucial for food safety, ecological balance, and human health. This study proposes an evanescent wave enhanced micro-structure polymer optical fiber (POF) sensor for highly sensitive detection of TC by employing the C 3 N 4 -MIL-53 heterostructure. The micro-structure composed of a side-polish region and micro-grooves, which can effectively enhance the intensity of POF's evanescent wave. The C 3 N 4 -MIL-53 heterostructure was fabricated and modified on the side-polish region as the sensitive film for selective adsorption and enrichment of TC molecules. This molecular adsorption process induced localized refractive index increases in the film, which subsequently led to an attenuation of the transmitted light. A theoretical model was established to illustrate the enhanced sensing principle of the micro-structure on POF and the structural parameters of the sensors are experimentally optimized. The sensor demonstrates the rapid detection capability of TC, and the sensitivity of the sensor reaches to −0.00155 ppm −1 with range of 5–20 ppm, and the LOD is 0.005 ppm. The proposed micro-structure POF sensor features easy fabrication and low-cost, which provides a new approach for TC detection.
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