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介孔g-C3N4
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2024 · IF 3.8

Green One-Pot Synthesis of Mesoporous g-C3N4 for Promoted Organic Dyes Photodegradation in Wastewater Treatment

Dawei Lan,Huiwen Zhu,Jianwen Zhang,Chengrui Xie,Fan Wang,Yueying Zheng,Zeyu Guo,Mengxia Xu,Tao Wu

This work provided a green, one-pot route to synthesize mesoporous g-C3N4. A series of characterizations revealed that the mesoporous sample maintained the typical structure of g-C3N4. The findings displayed that this mesoporous material had enlarged porosity and optical properties. The largest SBET of the mesoporous sample (32.65 m2/g) was 4.36 times larger than that of the bulk sample (7.48 m2/g). The photoactivity of the prepared photocatalysts was measured by the photocatalytic removal of rhodamine B (RhB). In agreement with the characterization analysis, the mesoporous g-C3N4 (99.60%) exhibited a 3.88 times better photocatalytic efficiency than that of bulk g-C3N4 (25.63%) and an 11.19 times faster reaction rate in the same period. In addition, the possible mechanism of this photodecomposition reaction was identified by the electron spin resonance (ESR) and trapping tests. The results demonstrated that •O2– and •OH made contributions, and •O2– played a dominant role in this process. This research offers a promising method for the synthesis of mesoporous g-C3N4 in an environmentally friendly and cost-effective route with remarkably high photoactivity.

研究领域: 环境化学 · 材料科学 · 光催化 · 纳米材料 · 环境功能材料 · 绿色合成
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Photocatalytic degradation of fluoroquinolone antibiotics using ordered mesoporous g-C3N4 under simulated sunlight irradiation: Kinetics, mechanism, and antibacterial activity elimination

Fengliang Wang,Yiping Feng,Ping Chen,Yingfei Wang,Yuehan Su,Qianxin Zhang,Yongqin Zeng,Zhijie Xie,Haijin Liu,Yang Liu,Wenying Lv,Guoguang Liu

The occurrence of fluoroquinolones (FQs) in the ambient environment has raised serious concerns. In this study, the photocatalytic degradation kinetics and mechanism of ciprofloxacin (CIP) was investigated in ordered mesoporous g-C 3 N 4 (ompg-C 3 N 4 ). Under simulated sunlight irradiation, ompg-C 3 N 4 exhibited a 2.9 fold more rapid reaction for CIP degradation than bulk g-C 3 N 4 . This enhancement may be attributed to the large specific surface area and effective charge separation of ompg-C 3 N 4 . The eradication of CIP followed the Langmuir–Hinshelwood (L–H) kinetics model, and surface reactions played a significant role during the photocatalysis process. Further study of reactive species (RSs) by both ESR technology and RSs scavenging experiments revealed that the superoxide anion radical (O 2 − ) and photohole (h + ) were primarily responsible for the degradation of CIP. Based on the identification of intermediates using liquid chromatography with tandem mass spectrometry (HPLC-MS/MS), and the prediction of reactive sites via Frontier Electron Densities (FEDs), the degradation pathways of CIP were proposed. A comparison of the degradation among FQs revealed that the piperazine moiety showed a dramatic effect on the degradation of FQs during the photocatalysis process. A residual antibiotic activity experiment revealed that ompg-C 3 N 4 provided a very desirable performance for the reduction of antibiotic activity. The sufficient photocatalytic degradation of CIP in ambient water revealed that a sunlight-driven ompg-C 3 N 4 photocatalytic process may be efficiently applied for the remediation of CIP contaminated natural waters.

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Inorganic and Organometallic Polymers and Materials · 2022 ·Vol. 32 ·期 5 ·1567-1581 · IF 3.518

Enhanced the Synergistic Effect of Tetracycline Adsorption and Photocatalytic Degradation on a Mesoporous Carbon Nitride

Liu Zheng,Ding Hekun,He Xiao,Wang Dongbo,Ma Dachao,Feng Qingge

A mesoporous g-C 3 N 4 with guanidine hydrochloride as precursor was prepared by molten salt assisted hard template of silica (SiO 2 ) aerogel for photocatalytic degradation of tetracycline (TC). The study shows that the successfully synthesized mesoporous g-C 3 N 4 presented a coral-like rod shaped and heptazine ring structure. When the amount of SiO 2 aerogel template was 1.4 g, the lower band gap (2.31 eV) of the sample (GM-1.4) with the lower interfacial resistance was displayed. The photocatalytic degradation rate of GM-1.4 for TC reached to 100% under visible illumination for 210 min, and the degradation efficiency of TC was enhanced with the synergistic effect of adsorption. Furthermore, the rich porous structure provided more active sites, boosted the separation and transfer of photoexcited charge carriers, and then enhanced the production of main active species · O 2 − and h + , resulting in the efficient destruction of the intrinsic structure and functional groups of TC molecules.

CAS / MDL: 75-77-4
研究领域: 环境科学 · 材料科学 · 化学 · 纳米技术
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Origins of selective differential oxidation of β-lactam antibiotics with different structure in an efficient visible-light driving mesoporous g-C3N4 activated persulfate synergistic mechanism

Mengmeng Dou,Jin Wang,Zhaokun Ma,Boru Gao,Xue Huang

In the study, an efficient ‘1 + 1 > 2′ synergistic coupling system driven by visible light consisting of mesoporous g-C 3 N 4 (MCN) and persulfate (PS)was constructed. The free radical transformation, electron transfer and non-covalent interaction between the MCN layer and PS in the system were explored via experiments and DFT calculations. The similarity for the fate of the seven β-lactam antibiotics with typical structures in the oxidation system was studied systematically in depth. First, the consistencies and differences of the seven antibiotics were summarized from three aspects: three-dimensional structures, electron cloud distributions, and the vulnerable sites. Notably, the selective differential degradation of β-lactam antibiotics in the MCN/PS system was speculated to be related with the molecular ionization potential (MIP), as a key index to describe the difficulty of oxidation. The distribution relationship between MIP and the oxidation kinetic constant ( K ) was explored and showed the following trend: a higher MIP indicates a weaker ability to provide electrons, and this leads to a greater resistance to oxidative degradation. In total, four main oxidation pathways of β-lactam antibiotics were systematically summarized combining HPLC-QTOF-MS and the simplified Fukui function calculation. The toxicity assessment of intermediate products provided by the T.E.S.T software of USEPA also shows a decreasing trend in the oxidation process. In the end, the superior practicability and stability of the MCN/PS system was verified by complex environment simulation and cyclic test. This research clarified the selective differential degradation mechanism of β-lactam antibiotics and provided a possible idea for the effective removal of refractory organic pollutants in water.

研究领域: 环境科学 · 化学工程 · 分析化学 · 药学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Photocatalytic difference of amoxicillin and cefotaxime under visible light by mesoporous g-C3N4: Mechanism, degradation pathway and DFT calculation

Mengmeng Dou,Jin Wang,Boru Gao,Ce Xu,Fan Yang

β-Lactam antibiotics are generally used for disease prevention in humans and animals. The antibiotics, which have been excreted into the surrounding environment, have caused serious concerns. In this study, mesoporous carbon nitride (MCN) was synthesized using a template-free method. The photocatalytic degradation of the two typical β-lactam antibiotics, amoxicillin (AMX) and cefotaxime (CFX), was performed using MCN. Considering the complexity of the actual environment, four factors that may influence the photocatalytic degradation of AMX and CFX were studied, containing the initial antibiotics concentration, catalyst dosage, pH and humic acid (HA). The possible mechanism of photocatalysis was presented using ESR spectroscopy and free radical trapping experiments. Furthermore, rational photocatalytic degradation pathways were proposed through the combination of LC-Q-TOF-MS/MS and density functional theory (DFT). Toxicity Estimation Software Tool (TEST) was used to predicate the toxicity of the byproducts. This study identified the catalytic activity difference between AMX and CFX firstly and elucidated their degradation mechanisms. The new findings are very meaningful for optimizing the conditions of photocatalytic degradation of β-lactam antibiotics. In addition, the results of wastewater test and stability experiments indicated that MCN has excellent performance. Therefore, MCN is a promising treatment material for the elimination of the antibiotic activity and mineralization of antibiotics under visible light.

研究领域: 环境科学 · 材料科学 · 化学工程 · 分析化学 · 毒理学
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