CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Chaoting Guan,Jin Jiang,Suyan Pang,Xiao Chen,Richard D. Webster,Teik-Thye Lim
Previous studies have reported that metal-doped graphitic carbon nitride (g-C 3 N 4 ) materials can activate peroxymonosulfate (PMS) to destruct organic pollutants. Herein, we interestingly found that pure g-C 3 N 4 materials synthesized via a facile calcination protocol without any metal doping could serve as the efficient PMS activator for degrading bisphenol A (BPA). The influences of different precursors (i.e., melamine, dicyandiamide, and urea) and annealing ambience (i.e., air or N 2 ) on the catalytic activity were investigated. The resultant g-C 3 N 4 materials exhibited different catalytic activities for PMS activation. The best performance was found in the case of g-C 3 N 4 synthesized from melamine and annealed in N 2 (g-C 3 N 4 -Melamine-N 2 ); 100% BPA (10 μM) removal was achieved by using 0.5 g/L catalyst and 1 mM PMS at pH 7 in 15 min. The difference in catalytic activities of these g-C 3 N 4 materials might be attributed to the fact that different preparation procedures impacted the chemical composition and structure of catalysts and thus changed the type and density of active sites. Important influencing factors such as PMS dosage, temperature, solution pH, and water matrices on degradation kinetics of BPA were evaluated. Results of quenching experiments and electron paramagnetic resonance spectroscopy revealed that sulfate radical and hydroxyl radical were main reactive species for BPA degradation by the g-C 3 N 4 /PMS system, which was also confirmed by the non-selectivity of this system towards various organics. Furthermore, possible transformation pathways of BPA by the g-C 3 N 4 /PMS system were proposed based on the identified oxidation products, primarily involving hydroxylation, bond cleavage, ring opening, as well as radical coupling. This study deepens mechanistic understanding of g-C 3 N 4 materials driven PMS oxidation processes, and also provides a green and efficient strategy for eliminating BPA in water.
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Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Xin Chen,Xiufang He,Xia Yang,Zhansheng Wu,Yunfeng Li
Novel binary coupled 2D/1D g-C 3 N 4 /CaTiO 3 composite photocatalysts with face-to-face contact were synthesized by a solvothermal and calcination method. The properties of g-C 3 N 4 /CaTiO 3 composites were characterized by XRD, SEM, TEM, BET, UV–vis/DRS, etc. The beneficial band position tuning via coupling g-C 3 N 4 with CaTiO 3 , and its 2D/1D face-to-face contacted pattern transfer electrons rapidly and retard photogenerated electrons-holes recombination. The photocatalytic ability was evaluated by using crystal violet (CV) and malachite green (MG). The as-prepared g-C 3 N 4 /2CTO sample shows the highest photocatalytic activity, and the degradation rate of CV and MG can reach up to 99.76% and 95.02% under simulate sunlight owing to the impressive synergic effect between 2D/1D g-C 3 N 4 /CaTiO 3 face-to-face contact pattern. The free radical scavenging experiments demonstrate that the · O 2 − and h + are the main active species. Further, the degradation intermediates of CV and MG detected by GC–MS found both containing phenol , 2,2-Methylenebis(6-Tert-Butyl-4-Methylphenol) (MTBM). Hence, they may have a similar degradation pathway, which provided a significant guideline for the degradation of triphenylmethane dyes. Our prepared novel 2D/1D face-to-face contact pattern nanocomposite is expected to be a fresh scheme for high-efficiency refractory pollutants degradation under sunlight.
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APPLIED SURFACE SCIENCE
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2019
·
IF 5.155
Xinxin Zhang,Kang Hu,Xuliang Zhang,Wajid Ali,Zhijun Li,Yang Qu,Hao Wang,Qingyang Zhang,Liqiang Jing
In this work, an in-situ way has been developed to achieve the co-modification of highly-dispersed Mn and Cu oxides to g-C 3 N 4 nanosheets for efficient CO 2 reduction. The Mn & Cu amount-optimized nanosheets exhibit the improved photocatalytic activity for CO 2 reduction to CO and CH 4 both by 3 times compared with the generally-bulk g-C 3 N 4 , mainly attributed to the nanosheet structure and to the roles of modified Mn and Cu oxides. Based on the transient-state surface photovoltage responses, transient-state photoluminescence spectra, and electrochemical measurements, it is confirmed that the modified Mn and Cu oxides could respectively capture the photogenerated holes and electrons, and provide the catalytic functions for water oxidation and CO 2 reduction. Remarkably, the simultaneous introduction of Mn and Cu oxides shows an obvious synergistic effect on the improvement of photocatalytic activity for CO 2 reduction. This work provides a feasible way to synthesize high-activity g-C 3 N 4 -based photocatalysts for energy production.
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ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Yue Zhou,Wenhua Lv,Binglong Zhu,Fei Tong,Junli Pan,Jirong Bai,Quanfa Zhou,Hengfei Qin
Graphitic carbon nitride (g-C3N4) has been widely studied as a fascinating visible-light-response two-dimensional semiconductor photocatalyst. Nevertheless, the quantum yield of g-C3N4 is unsatisfactory due to the insufficient surface reactive sites and slow charge migration efficiency caused by grievous agglomeration and large grain size. Herein this obstacle is overcome through a facile eco-friendly strategy based on effects from a bubble template and nonmetal heteroatom doping of g-C3N4. This treatment not only restricts the agglomeration but also creates more surface active sites for reaction and more porous channels for charge carrier transfer. Well-amended g-C3N4 nanosheets with porous network and sulfur-doping were prepared with larger specific surface areas and faster electron–hole migration and separation capacity. The modified g-C3N4 nanosheets possessed a H2 evolution rate 5.3 and 3.8 times enhanced compare with bulk g-C3N4 (BCN) and S-doped g-C3N4 (CNS).
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Wei Li,Xiao Wang,Min Li,Shu-ao He,Qiong Ma,Xuechuan Wang
Hydrogen is known as an alternative new energy for its advantages of non-pollution and high calorific value, and photocatalysis technology is regarded as one of the most effective means to produce hydrogen in recent years. In this topic, aiming at the poor photoresponse, fast combination of photo-induced carriers and unstable structure of traditional photocatalysts, the three-dimensional porous g-C 3 N 4 /graphene oxide framework was constructed by compounding two-dimensional graphene oxide and two-dimensional g-C 3 N 4 via hard template (SiO 2 nanoparticles) method and selective chemical etching. Then, silver bromide nanoparticles , a superior photosensitizer, were immobilized on the three-dimensional porous framework to construct the three-dimensional porous g-C 3 N 4 /graphene oxide-AgBr photocatalyst with Ag plasmas by solvothermal method. Research showed that this novel photocatalyst based on Z-scheme heterostructure (GO-AgBr), p-n heterostructure (g-C 3 N 4 -AgBr) and Ag plasmas presented high-efficient visible-light driven hydrogen evolution (3.69 mmol/g/h) at the absence of Pt co-catalyst, which is higher than the majority of existing catalysts, and it also possessed strong stability on its activity and structure. Accordingly, the enhanced hydrogen evolution and photostability were attributed to the highly ordered structure and fast interfacial electron conduction of three-dimensional porous framework, superior photosensitivity of AgBr and synergistic effect of Ag plasmas. Therefore, this study provided a potential method for exploitation of hydrogen energy.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2018
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IF 4.61
Guanglan Di,Zhiliang Zhu,Qinghui Huang,Hua Zhang,Jianyao Zhu,Yanling Qiu,Daqiang Yin,Jianfu Zhao
Pharmaceuticals have been frequently detected in various water bodies, posing potential threat to human health and ecological environment. In this work, ZnFe-LDH derived mixed metal oxides (ZnO/ZnFe 2 O 4 , ZnFeMMO) were innovatively adopted to modulate the g-C 3 N 4 photocatalytic performance for the enhanced degradation of ibuprofen (IBF) and sulfadiazine (SDZ) as targeted pollutants. Characterization analyses indicated that the g-C 3 N 4 /ZnFeMMO composites were in the feature of rationally-designed microarchitecture, increased specific surface area, improved light absorbance and efficient charge separation, thereby resulting in promoted photocatalytic activities. Furthermore, the ratio of g-C 3 N 4 to ZnFeMMO in the composites was found to exert significant effects on the resulted microstructures and properties. The results showed that the composite with low g-C 3 N 4 content of 1.0 wt% or high g-C 3 N 4 content of 90 wt% exhibited the optimum catalytic activity for the degradation of IBF or SDZ, respectively. Such distinct structure-activities can be attributed to the different dominated reactive species in two cases: h + for IBF degradation but OH for SDZ degradation. A Z-scheme mechanism was proposed for the charge separation, together with ZnFe 2 O 4 as a light sensitizer. Degradation pathways for IBF and SDZ were established by ESI-QToF-MS technology . This work provided a new perspective to develop rationally-architectured g-C 3 N 4 based photocatalysts for the decontamination of water polluted by pharmaceuticals.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Zhiwei Zhao,Junyu Fan,Xiaoyong Deng,Jie Liu
In this study, Co 3 O 4 quantum dots decorated phosphorus-doped g-C 3 N 4 nanosheets was synthesized though one-step thermal polymerization method using vitamin B12 (VB12) as precursor of cobalt and phosphorus mixed with melamine. The prepared photocatalysts were characterized by X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR), BET, transmission electron microscope (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflectance spectroscopy (DRS), photoluminescence (PL) and electrochemical measurements. Appropriate amount of introduced VB12 can improve photocatalytic activities while excess caused inhibition. The sample with the weight ratio of VB12 in precursors at 1% exhibited the optimum photodegradation efficiency for metronidazole (MTZ), about 2 times as higher as the removal rate of pure g-C 3 N 4 . Several effects on the photocatalytic activity was also investigated and the results showed that enough dissolved oxygen and presence of Fe 3+ was found to promote MTZ photodegradation, while NO 3 − , Ca 2+ and HCO 3 − would inhibit it. Superoxide radical O 2 − was identified as the dominate active specie in photodegradation process and possible enhancement mechanism of introduced VB12 for photocatalytic activities was proposed. It was inferred that the synergistic effect of generated Co 3 O 4 quantum dots and P-doped g-C 3 N 4 , including increasing the separation efficiency of photo-inducted electrons and holes, inhibiting the recombination process of them and decreasing the band gap energy, could be the reason for the better photocatalytic activity. At last, MTZ degradation pathway in the photosystem was determined.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2015
·Vol. 17
·期 17
·11577-11585
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IF 4.493
Sugang Meng,Xiaofeng Ning,Tao Zhang,Shi-Fu Chen,Xianliang Fu
The separation mechanisms of photoexcited carriers for composite photocatalysts are a hot point in the photocatalytic field. In this paper, the Ag3PO4/g-C3N4 nanocomposites with different main parts (Ag3PO4 or g-C3N4) were synthesized using a facile in situ precipitation method. The photocatalysts were characterized by X-ray powder diffraction, UV-vis diffuse reflection spectroscopy, transmission electron microscopy and Brunauer–Emmett–Teller methods. The photocatalytic performance was evaluated by the degradation of methylene blue under visible light irradiation. When the main part of the Ag3PO4/g-C3N4 photocatalyst is Ag3PO4, the transfer mechanism of photogenerated electron–hole takes generic band–band transfer, and the photocatalytic activity is decreased. However, when the primary part of the Ag3PO4/g-C3N4 photocatalyst is g-C3N4, the migration of photogenerated electron–hole exhibits a typical Z-scheme mechanism, and the photocatalytic activity is increased greatly. The separation mechanisms of photogenerated carriers were investigated by the electron spin resonance technology, the photoluminescence technique and the determination of reactive species in the photocatalytic reactions. It is hoped that this work could render guided information for design and application of Z-scheme photocatalysts with excellent photocatalytic performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
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IF 8.328
Zhiwang Yang,Xueqing Xu,Xixi Liang,Cheng Lei,Yuhan Cui,Wenhua Wu,Yaoxia Yang,Zhe Zhang,Ziqiang Lei
Photocatalytic synthesis using visible light is a desirable chemical process because of its potential to utilize sunlight. A heterostructured MIL-125/Ag/g-C 3 N 4 nanocomposite was implemented as an efficient bifunctional visible-light response catalyst for the photoreduction of nitrocompounds and the oxidation of alcohols. The photocatalyst was prepared via an accessible method and characterized by XRD, SEM, TEM, XPS, FT-IR, N 2 adsorption–desorption isotherm, UV–vis DRS, PL and EIS. The reactive efficiency of the photocatalyst depends on two primary factors, one is the light adsorption of catalysts, Ag nanoparticles (NPs) were photodeposited on the surface of g-C 3 N 4 and MIL-125 to increase visible-light absorption via the surface plasmon resonance. And the other is the separation efficiency of the photogenerated charge carrier. As an electron-conduction bridge in the interface between MIL-125 and g-C 3 N 4 , Ag NPs could facilitate the direct migration of photoinduced electrons from g-C 3 N 4 to MIL-125 and retard the recombination of electron-holes. Therefore, the MIL-125/Ag/g-C 3 N 4 sample shows highest photocatalytic activity compared with MIL-125, g-C 3 N 4 , MIL-125/Ag and MIL-125/g-C 3 N 4 . A corresponding photocatalytic mechanism of these reactions was discussed in detail. Moreover, the photoreduction of nitrocompounds and oxidation of the alcohols with superior conversions and selectivities were obtained, and the catalyst can be recycled four times. It is concluded that MIL-125/Ag/g-C 3 N 4 would be a promising visible light photocatalyst in the field of selective organic transformations.
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ANALYTICA CHIMICA ACTA
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2016
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IF 4.712
Ning Zhang,Jia Gao,Chuanhui Huang,Wei Liu,Ping Tong,Lan Zhang
In this paper, Zinc oxide (ZnO) hybridized with graphite-like C 3 N 4 (ZnO/g-C 3 N 4 ) nanoflowers based solid phase microextraction (SPME) coating was prepared on fiber using in situ hydrothermal growth method for gas chromatographic -mass spectrum (GC- MS) separation and analysis target analytes in complex matrixes for the first time. The proposed hybrid ZnO/g-C 3 N 4 fiber exhibited wide linearity for the pesticide residues in range of 0.003–5.0 ng mL −1 . The limits of detection (LOD) were 0.001–0.0025 ng mL −1 . The relative standard deviation (RSD) for three replicate extractions using one fiber was ranged from 2.3% to 7.6%. The fiber to fiber RSD was 5.3–11.3% (n = 3). This method was successfully used for simultaneous determination of nine pesticide residues in cucumber, pear, Green tea and Minjiang water with satisfactory recoveries of 79.1–103.5%. These results indicated that the ZnO/g-C 3 N 4 composite provided a promising alternative in sample pretreatment and analysis.
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MICROCHEMICAL JOURNAL
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2017
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IF 3.034
Jingrong Zhou,Yunfei Tian,Xi Wu,Xiandeng Hou
Photochemical vapor generation (PCVG) is a green and effective sampling technology for analytical atomic spectrometry , and in recent years it has been received continuous attention. In this work, visible light photochemical vapor generation was achieved with metal-free g-C 3 N 4 /CQDs (carbon nitride/carbon quantum dots) composites as a photocatalyst, and used for selective and ultrasensitive detection of total mercury by inductively coupled plasma mass spectrometry (ICP-MS). The limit of detection can be as low as 8 ng L − 1 , making it one of the most sensitive methods for mercury determination . The visible light photochemical vapor generation can also be coupled to other analytical atomic spectrometric techniques.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ying Du,Linfei Li,Yanting Tang,Juan Li,Quanhui Guo,Guikuan Yue
With the production and application of antibiotics, the generated substandard antibiotic wastewater has brought unprecedented damage to the environment and finally the health of human beings. To alleviate this problem, photocatalytic degradation was proposed, and various catalysts have been developed with high efficiency and low cost. Herein, a novel 0D/3D/2D dual Z-heterojunction photocatalyst CdS QDs/Bi 2 WO 6 /g-C 3 N 4 was constructed by in-situ growth method in order to efficiently degrade multiple antibiotic pollutants. The combination of multi-dimensional materials is more conducive to the close contact between materials and the effective transport of photogenerated carriers. Results reveal that the sample of 75 %CdS QDs/Bi 2 WO 6 /g-C 3 N 4 (denoted as 0.75CSBC) showed the best degradation activity and stability for tetracycline (TC), and the degradation rate could reach 80.83 % within 12 min under visible light irradiation. Based on the detailed analysis of the results from free radical trapping experiment, Mott-Schottky test and liquid chromatography-mass spectrometry (LC-MS) test, the photocatalytic degradation mechanism and pathway were proposed. Besides, 0.75CSBC showed excellent degradation activity for levofloxacin (LVFX), oxytetracycline hydrochloride (OTC) and norfloxacin (NFLX), confirming its good universality. The multi-dimensional dual Z-heterojunction photocatalyst not only provides more active sites but also promotes the efficient migration of photogenerated charge, together with an excellent stability, indicating its wide practical application in the field of photocatalytic wastewater treatment. This work also provides an interesting method for the preparation of multi-dimensional heterogeneous catalysts.
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