JOURNAL OF THE AMERICAN CERAMIC SOCIETY
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2021
·Vol. 104
·期 12
·6319-6334
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IF 3.784
Limin Zhao,Ruifa Jin,Baofeng Zhang
In this paper, a novel Z-scheme photocatalyst Er 3+ :Yb 0.5 Y 2.5 Al 5 N 0.01 F 0.01 O 11.98 /g-C 3 N 4 –Pt–BiPO 4 was synthesized by sol-hydrothermal and calcination methods. The prepared samples were characterized by XRD, SEM, TEM, EDS mappings, XPS, PL, and DRS. In addition, the optimal hydrothermal conditions for the preparation of BiPO 4 were explored with the azofuchsin solution and ciprofloxacin(CIP) solutions as the target pollutants. At the same time, the best calcination temperature and the best calcination time of the Er 3+ :Yb n Y 3−n Al 5 N x F y O 12−x−y and BiPO 4 were investigated. The results showed that the Z-scheme Er 3+ :Yb 0.5 Y 2.5 Al 5 N 0.01 F 0.01 O 11.98 /g-C 3 N 4 –Pt–BiPO 4 photocatalyst has strong redox ability, wide absorption range of visible light, and excellent separation effect of electron–hole pairs, which can efficiently degrade organic pollutants and antibiotic.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Xiao Zhang,Bin Ren,Xi Li,Biming Liu,Shiwen Wang,Peng Yu,Yanhua Xu,Guoqiang Jiang
Carbon-bridge-modified malonamide (MLD)/g-C 3 N 4 (CN) was prepared by copolymerization of MLD with urea and melamine and loaded with Fe 3 O 4 for the high-efficiency removal of tetracycline (TC) in water under photo-Fenton. The prepared catalysts were characterized by SEM, TEM , N 2 adsorption–desorption analysis, XPS, XRD, and FTIR, which proved that the modification method successfully introduced the C bridge into the carbon nitride molecular system and increased the structural defects of the catalyst. The Carbon-bridge-modified MLD/CN/Fe 3 O 4 also had good visible-light response and charge-separation and transport abilities in the photoelectrochemical test. Degradation results showed that the photo-Fenton degradation of TC reached 95.8%, and the mineralization rate was 55.7% within 80 min at 80 mM H 2 O 2 dosage, 0.5 g/L catalyst dosage, and near-neutral pH by 0.8MLD/CN/Fe 3 O 4 . Moreover, the oxidation products and mineralization pathways of TC were explored by LC-MS. Toxicity analysis indicated low environmental threat of the intermediates in TC mineralization. EPR analysis and H 2 O 2 decomposition efficiency analyses showed an improvement in the H 2 O 2 decomposition performance of 0.8MLD/CN/Fe 3 O 4 . This work could provide a valuable insight for the application of heterogeneous photo-Fenton technology in wastewater treatment .
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BIOSENSORS & BIOELECTRONICS
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2021
·
IF 10.618
Fubin Pei,Shasha Feng,Yi Wu,Xuchu Lv,Hualai Wang,Shen-Ming Chen,Qingli Hao,Yang Cao,Wu Lei,Zhaoyang Tong
Aflatoxin B1 (AFB1) is the most toxic mycotoxin , is widely found in foods and animal feeds, and can pose a serious threat to our lives. A label-free photoelectrochemical (PEC) immunosensor was fabricated for the sensitive detection of AFB1. A Z-scheme heterojunction of gold nanoparticles (Au NPs) loaded on graphitic carbon nitride sheet and tungsten trioxide sphere composite (g-C 3 N 4 /Au/WO 3 ) acted as the highly sensitive platform. The g-C 3 N 4 /Au/WO 3 is capable, not only of immobilizing antibodies via Au NPs, but also enhancing the separation of electron-hole pairs due to its good energy band matching efficiency. The mechanism of photo-generated electron/hole transfer on g-C 3 N 4 /Au/WO 3 was explored using scavengers to eliminate active components. On this basis, an electron transfer pathway for the immunosensor was deduced. The PEC immunosensor displayed a linear concentration range from 1.0 pg mL −1 to 100 ng mL −1 and a low detection limit of 0.33 pg mL −1 (S/N = 3) for AFB1. Good reproducibility, stability, and specificity provide a solid foundation for the practical application of this immunosensor.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Zixuan Wang,Han Wang,Ziwei Wang,Danlian Huang,Hong Qin,Yangzhuo He,Ming Chen,Guangming Zeng,Piao Xu
In this study, the oxidative degradation of tetracycline (TC) by ferrocene-modified graphite phase carbon nitride (Fe/g-C 3 N 4 ) activated persulfate (PS) under light-assisted conditions is examined. The materials are characterized by a series of methods such as SEM, TEM , XRD , FTIR, XPS , etc. This article explores the influence of the amount of sulfate, the initial concentration of pollutants, the amount of catalyst, and the pH value on the reaction system. When the amount of PS added reaches 2.5 mM and the catalyst dosage is 1 g L −1 , the Fe/g-C 3 N 4 /PS/Vis exhibit the best performance for tetracycline removal. In 60 min, the removal of tetracycline reaches 93% under its natural pH. In the reaction system acidic neutral conditions are more conducive to degrade TC. The results show that the doping of ferrocene inhibits the recombination of electron-hole pairs in the g-C 3 N 4 , expands the light response range to speed up the removal rate of tetracycline. At the same time, iron cycle generated by ferrocene modification helps to activate persulfate to produce sulfate radicals with strong oxidizing properties. Sulfate radicals, hydroxyl radicals , superoxide radicals and holes are the main active species proved by ESR test and the quenching experiments. The synergy between photocatalysis and PS activation promotes the production of active species and the tetracycline removal. The results show that the Fe/g-C 3 N 4 composite material activated persulfate under visible light is an effective method to remove tetracycline from water.
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DIAMOND AND RELATED MATERIALS
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2021
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IF 3.315
Yan Hua Gao,Wen Li Zhao,Ying Chen
In this paper, g-C 3 N 4 was modified by the synergistic effect of double salt KCl-(NH 4 ) 2 CO 3 , and porous g-C 3 N 4 with hydroxylated surface was prepared. Combined with a series of characterization (XRD, SEM , BET, FTIR, UV–vis DRS and XPS) and density functional theory (DFT) analysis, it is confirmed that KCl can cooperate with ammonium salt (NH 4 ) 2 CO 3 to produce rich pore structure , and (NH 4 ) 2 CO 3 , as an alkaline slow-release agent, can assist KCl to further enhance hydroxylation . KCl-(NH 4 ) 2 CO 3 not only plays a synergistic role in pore formation, but also introduces hydroxyl and cyano groups, which improves the hydrophilicity of g-C 3 N 4 , promotes the separation efficiency of photo-generated carriers, and is beneficial to enhance the photocatalytic activity . Taking methyl orange (MO) as the model of pollutant degradation, and proposed the possible degradation mechanism . This study provides a simple, efficient and widely applicable method for modifying g-C 3 N 4 to improve its activity.
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NANO
·
2021
·
IF 1.556
Jungang Yi,Kun Wu,Huadong Wu,Jia Guo,Linfeng Zhang,Hao Li,Jianding Li
The presence of the antibiotics in the wastewater has posed a huge risk to aquatic life and human health. It is a great significance to develop an effective technology to treat the antibiotics-containing wastewater. In this study, a series of g-C 3 N 4 /NH 2 -MIL-88B(Fe) composite photocatalysts are synthesized through a simple one-step method. The structure and optical properties of prepared photocatalysts are detected by X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–Vis absorption spectra (UV–Vis DRS), photoluminescence (PL) spectroscopy and transient photocurrent techniques, respectively. FESEM and TEM show that MOF is uniformly dispersed in petaloid g-C 3 N 4 . The uniform dispersion of Fe-MOFs in the heterojunction composites increases the specific surface area ( S BET ) of g-C 3 N 4 , which results in a great adsorption property for the nanocomposite. The capture experiment shows that • O 2 − and h + are the main active substances in ciprofloxacin (CIP) degradation. These prepared composite photocatalysts exhibit excellent CIP photodegradation activity under visibly light irradiation with an apparent rate constant of 0.0127 min − 1 (3.74 times as the rate of single component). The remarkable catalytic performance can be ascribed to the fact that the g-C 3 N 4 /NH 2 -MIL-88B(Fe) heterojunction inhibits the recombination of photoinduced electron–hole pairs and improved the visible light absorption.
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RENEWABLE ENERGY
·
2021
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IF 8.001
Yanan Wei,Xin Li,Yunlei Zhang,Yongsheng Yan,Pengwei Huo,Huiqin Wang
Wide-light absorption performance and efficient carrier separation ability are the necessary conditions for excellent photocatalytic materials. In this research, g-C 3 N 4 QDs (CN QDs) and Au nano-particles (NPs) co-modified CeO 2 /Fe 3 O 4 micro-flowers (MFs) photocatalyst (CACeF) has been prepared. CO 2 photoreduction experiments showed that the composite had obviously enhanced photoreduction activity and photocatalytic stability. The yields of CO and CH 4 over it as catalyst in 4 h is about 5 and 8 times greater than that of pure CeO 2 . Photoelectrochemical tests showed that the heterojunction between CN QDs and Au NPs can greatly improve the carrier separation ability and the light-utilization efficiency of photocatalysts. Besides, the excellent electronic transmission performance of Au NPs provided a specific channel for the electron transmission, and the strong local surface plasmon resonance (LSPR) of Au NPs resulted in a lot of hot-electrons can directly take part in the CO 2 photoreduction. The synergistic effect between CN QDs and Au NPs can further enhance the photocatalytic activity of the photocatalyst. Fe 3 O 4 QDs can ensure the effective recovery and reuse of the composite without affecting the photocatalytic performance of composite. Finally, a potential photoreduction mechanism of CN QDs and Au NPs co-modified CeO 2 /Fe 3 O 4 MFs photocatalyst were discussed in total.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Zanling Huang,Xia Zhao,Hong Xia,Fushen Lu,Liangsheng Hu,Paul K. Chu
Photocatalysis has attracted worldwide attention in the fields of energy storage and environmental remediation. However, the solar-to-energy conversion efficiency is still low due to fast charge carrier recombination in the bulk phase of conventional photocatalysts. Herein, a series of photocatalysts including g-C 3 N 4 (GCN), non-polar MgO(110)/GCN composite, MgO(110)+GCN mixture, polar MgO(111)/GCN composite, and MgO(111)+GCN mixture are prepared and their photocatalytic activities are investigated systematically. The polar and non-polar MgO improve the photocatalytic properties of GCN in the following order: MgO(111)+GCN>MgO(110)/GCN>MgO(111)/GCN>MgO(110)+GCN>GCN. Benefiting from charge carrier separation rendered by the local electric field (LEF) induced by MgO(111) polarization, MgO(111) improves the performance of GCN significantly when it is mixed with GCN. However, the enhancement effects are reduced when it is combined with or integrated into GCN as in the MgO(111)/GCN composite, where the traditional heterojunction effect constitutes the main enhancement mechanism. Our study reveals that the photocatalytic enhancement by the LEF effect is superior to that by the traditional heterojunction effect based on polar supporting materials. Our results offer insights into the enhancement mechanism of photocatalysts with polar supporting materials and reveal a simple strategy to optimize photocatalytic processes to exploit solar energy efficiently.
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MICROCHEMICAL JOURNAL
·
2020
·
IF 3.594
Yao Chen,Yanyan Zhu,Yuhui Zhao,Jing Wang,Meng Li
The complexation of metals and metal compounds with organic skeletons into nanohybrid composites attracts attention in electrochemical applications due to the improved charge transfer pathways, which enhance the electrocatalytic activity. In this study, CuO, Cu 2 O, and CuS were anchored on g-C 3 N 4 sheets to construct electrochemical sensors for the detection of acetaminophen (AP). The CuX/g-C 3 N 4 nanohybrid composites were analyzed via transmission electron microscopy, infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. Among the CuX/g-C 3 N 4 nanocomposites, CuS/g-C 3 N 4 displays a higher electrochemical activity. The electrochemical CuS/g-C 3 N 4 , CuO/g-C 3 N 4 , and Cu 2 O/g-C 3 N 4 sensors have wide linear ranges of 5 to 500 µM with a low detection limit (LOD) of 0.26 µM, 5 to 300 µM with a LOD of 0.32 µM, and 5 to 250 µM with a LOD of 0.47 µM, respectively. The better performance of the CuS/g-C 3 N 4 sensor is probably because of its significantly higher catalytic rate constant with respect to the oxidation of AP in electrochemical kinetics compared with those of the two other sensors, which leads to the enhanced electrocatalytic oxidation of AP. The CuX/g-C 3 N 4 -based electrochemical sensors display an excellent selectivity, repeatability, reproducibility, and stability. These features suggest that CuX/g-C 3 N 4 based electrochemical sensors can be sensitively detected of AP.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 56
·期 2
·1630-1642
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IF 3.553
Zhou Ling,Sun Menglong,Kou Jiahui,Lu Chunhua,Li Ling,Zhang Fangshu,Xu Zhongzi
Graphitic carbon nitride (g-C 3 N 4 ), as an organic polymer semiconductor, has been the focus of photocatalysts due to its physical and chemical stability, low cost and non-toxicity. However, pristine g-C 3 N 4 also has many drawbacks, such as small specific surface area and easy recombination of photoexcited carriers, which hampered its practical application. In this work, we first propose a design idea of embedding stereo molecular scaffold into g-C 3 N 4 framework with a facile copolymerization method for better exfoliating g-C 3 N 4 to reach a better photocatalytic hydrogen evolution under ordinary pressure. The stereo molecular scaffold looses the interlayer stacking of bulk g-C 3 N 4 , benefitting the exfoliation of g-C 3 N 4 . The hydrogen evolution activity of stereo molecular scaffold doped g-C 3 N 4 (AMCN-3-E) is about 7.54 times higher than that of the pristine MCN, which may due to the activated π → π * and n → π * electron transitions, creating more electron transition paths and accelerating the separation of photoexcited electrons and holes.
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Journal of Cleaner Production
·
2020
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IF 7.246
Qin Huang,Chen Wang,Derek Hao,Wei Wei,Luochun Wang,Bing-Jie Ni
The development of highly efficient and separation-free, low-cost photocatalysts have crucial prospect for sustainable wastewater treatment , because it is able to eliminate the hazards of organic pollutant with facile operation. However, the relatively high cost of previous photocatalysts highly obstructs the application of these materials. Herein, we report a cost-effective and distinct konjac/graphitic carbon nitride (KCN) aerogel , which has superior performance for advanced oxidation water treatment . The abundant porous structure of the ultralight aerogel ensures the rapid adsorption of pollutants, which is much helpful for the further photodegradation process. During the working process, the aerogel is half submerged in pollutant solution and half exposed in air, forming a distinctive gas-solid-liquid triphase system, where oxygen can be rapidly delivered into the solution via the porous channels, boosting the generation of hydroxyl and superoxide radicals. Meanwhile, the aerogel structure can separate the g-C 3 N 4 , obstruct its stacking, as well as improve the light absorption rate. The synthesis, utilization and readily biodegradable treatment of the KCN aerogels are all green and eco-friendly, which is extremely constructive for strategies to develop novel highly efficient photocatalytic materials.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2020
·
IF 4.872
Xiarong Zheng,Yuanqiong Liu,Xiaobin Liu,Qingbiao Li,Yanmei Zheng
A novel composite electrospun fiber with high photocatalytic efficiency, good stability, strong hydrophobicity, good pollution resistance, and easy separation and recovery was synthesized. The TiO 2 @g-C 3 N 4 (TCN) with special core-shell structure (5–10 nm shell) facilitated the separation of photogenerated electron-holes and had high photocatalytic performance. The poly (vinylidene fluoride) (PVDF) electrospun fiber immobilized with TCN was successfully fabricated (PVDF-TCN) with uniform distribution and size of nanofibers by using electrospinning, which was used for degrading tetracycline under visible-light irradiation (> 400 nm). A special rougher surface of electrospun fiber obtained by washing of sacrificial PVP increased the specific surface area, which became more conducive to the adhesion of the catalyst. The water contact angle and FTIR results demonstrated that the electrospun fiber became extremely hydrophilic after adding TCN catalyst, which could effectively mitigate the fiber pollution. The PVDF-TCN-0.2g electrospun fiber exhibited excellent photocatalytic performance and the degradation efficiency of tetracycline was up to 97% in 300 min under visible-light irradiation. The mechanism of PVDF-TCN electrospun fiber degradation of tetracycline in the photocatalytic process was also proposed. In addition, the PVDF-TCN-0.2g exhibited a stable activity after 4 cycles experiments since the degradation efficiency remained about 90%. Therefore, we believed this study provided a new strategy in catalyst immobilization and wastewater treatment.
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