Catalysis Science & Technology
·
2018
·Vol. 9
·期 1
·75-85
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IF 5.365
Ruyi Zhong,Zisheng Zhang,Shuqi Luo,Z. Conrad Zhang,Limin Huang,Meng Gu
Knowledge of the interfacial structure of nanocomposite materials is a prerequisite for rational design of nanostructured photocatalysts. Herein, TiO2 and g-C3N4 2D/2D nanocomposites were fabricated from three distinct synthetic protocols (i.e., co-calcination, solvothermal treatment and charge-induced aggregation), showing different degrees of enhancement (1.4–6.1 fold) in the visible-light induced photocatalytic hydrogen evolution reaction compared to the simple physical mixture. We propose that the interfacial Ti–O–N covalent bonding promotes the charge carrier transfer and separation more effectively than the electrostatic interaction, thus accelerating the photocatalytic H2 production. Meanwhile, the exposed surface area of TiO2 in the composite needs to be enlarged for deposition of the co-catalyst. This research sheds light on the rational design of hybrid nanocomposites based on earth-abundant elements for photocatalysis.
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NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 21
·17644-17651
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IF 3.201
Shaobo Li,Tao Zhu,Lichun Dong,Mingdong Dong
Heteroatom doping has been demonstrated to be an effective way to tune the properties of nanomaterials including chemical reactivity and electronic and optical performance. In this study, rGO/g-C3N4 and boron doped rGO/g-C3N4 (B-rGO/g-C3N4) nanocomposites were fabricated via a rapid plasma treatment method, and their photocatalytic performance under visible light radiation was examined. The results showed that the photocatalytic efficiency of B-rGO/g-C3N4 for rhodamine B degradation can be 50% higher than that of rGO/g-C3N4 at an optimum rGO loading of 5 wt%. XPS and FTIR analyses indicated the enhanced C–O–C covalent bonding between rGO and g-C3N4 in B-rGO/g-C3N4, and the optical characterization demonstrated that it could further improve the separation of the photo-generated chargers and narrow the bandgap of the nanocomposite. This work provides an idea that boron doping could be an effective way to promote the chemical interaction between different components in composite materials, which is important in designing and developing new functional nanomaterials.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
·
2019
·
IF 3.261
Asif Hayat,Fazal Raziq,Muhammad Khan,Ikram Ullah,Mati Ur Rahman,Wasim Ullah Khan,Javid Khan,Akhlaq Ahmad
In this work, we report the fabrication of polypyrrole/g-C 3 N 4 (PPy/g-C 3 N 4 ) nanocomposites via simple wet-chemical method. The photocatalytic activities of the composites are evaluated for water splitting to evolve H 2 , Rhodamine B dye (RhB) and 2,4-dichlorophenol (2,4-DCP) degradation under visible-light. The results reveal that the photocatalytic performance of g-C 3 N 4 for H 2 evolution, RhB dye and 2, 4-DCP degradation are significantly improved after coupling polypyrrole (PPy). Worth noting, the amount optimized (1 wt%PPy/g-C 3 N 4 ) photocatalyst showed highest photoactivity compared to the other photocatalysts. Further, it is confirmed by means of radical trapping experiments that superoxide radical (O 2 − ) is the dominant specie involved in the degradation of pollutants over PPy/g-C 3 N 4 nano-composites. Moreover, clear photocatalytic reactions for H 2 evolution and pollutants degradation are proposed. This work would help us to deeply understand the reaction mechanism and will provide feasible routes to fabricate g-C 3 N 4 based highly efficient photocatalysts for energy and environmental applications.
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Jiangping Jing,Zhuoyuan Chen,Chang Feng
Graphitic carbon nitride (g-C 3 N 4 ) usually shows amphoteric property in a neutral solution. In this work, a K&I co-doped g-C 3 N 4 is prepared by simply sintering the mixture of dicyandiamine, KI and I 2 . The K&I co-doping modulates the band structure of g-C 3 N 4 with pulling the Fermi level toward its conduction band minimum. The obtained K&I co-doped g-C 3 N 4 (K&I-C 3 N 4 ) generates positive photocurrents over the whole investigated potential range, exhibiting a typical n-type semiconductor characteristic. Therefore, the K&I co-doping transforms the g-C 3 N 4 from amphoteric to n-type semiconductor. Also, the prepared K&I-C 3 N 4 shows widened light absorption range and enhanced separation efficiency of the photogenerated charge carriers, which results in the dramatically enhanced photoelectrochemical performance.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Jinhong Fan,Hehe Qin,Simin Jiang
Peroxymonosulfate (PMS) is an alternative to hydrogen peroxide in advanced oxidation processes. Herein, we present a simple one-pot synthetic approach for the Mn-doped graphite phase carbon nitride (g-C 3 N 4 ) materials and make it as a catalyst to activate PMS for acetaminophen (ACT) degradation. Fabricated Mn-g-C 3 N 4 composites (MnCN) were characterized by SEM, EDS, XRD, XPS, and FTIR. Results showed that Mn was uniformly dispersed in the structure of g-C 3 N 4 mostly in the form of Mn-N coordination. The effects of pH, contents of doped Mn, catalyst dosage, and reusability of catalyst and corresponding kinetic study were conducted to determine the catalytic performance of MnCN. High reaction efficiency was obtained in a wide pH range of 3.2–9. 100% removal of ACT in 15 min under optimized conditions with initial pH 6.5, 0.8 g/L of PMS and 200 mg/L of catalyst of 0.5-MnCN. Additionally, the reaction mechanism of the PMS/MnCN system was investigated using the electron spin resonance technique, quenching studies as well as different organics with electron-donating or electron-withdrawing groups. No PMS decomposition was detected without substrates. No inhibition effect by ethanol or tert -Butyl alcohol and complete inhibition effect by benzoquinone and partly by furfuryl alcohol, as well as ESR spectrum of TEMP- 1 O 2 were observed, suggesting that the activation of PMS proceeded in a new way, which is different from traditional sulfate radical-based advanced oxidation processes. A possible mechanism was proposed for ACT removal. PMS was first bounded to Mn-N sites to generate the superoxide anion. Then singlet oxygen produced by superoxide anion would react with ACT by replacing the electron-donating group of acylamino.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Ruobai Li,Meixuan Cai,Zhijie Xie,Qianxin Zhang,Yongqin Zeng,Haijin Liu,Guoguang Liu,Wenying Lv
A copper ferrite modified graphitic carbon nitride (CuFe 2 O 4 /g-C 3 N 4 ) nanocomposite was successfully synthesized for the utilization as a visible-light responsive photocatalyst. The as-synthesized catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflectance spectra (UV–vis/DRS), photoluminescence (PL) analysis, and an electrochemical workstation. Compared to g-C 3 N 4 and CuFe 2 O 4 , the CuFe 2 O 4 /g-C 3 N 4 composites possessed excellent photocatalytic performance for the destruction of propranolol (PRO). A removal efficiency of 82.2% was achieved with 1 g/L catalyst and 1 mM peroxydisulfate (PDS) under visible light irradiation (λ < 420 nm) within 120 min. The g-C 3 N 4 coupled with CuFe 2 O 4 improved the capacity for visible light capture, whereas the presence of PDS enhanced the transfer of photogenerated electron. Quenching experiments and electron spin resonance (ESR) suggested that the reactive oxygen species (ROS) were superoxide radicals (O 2 − ), h + , hydroxyl radicals ( OH), and sulfate radicals (SO 4 − ). Moreover, the byproducts of PRO were investigated by HPLC-MS/MS, and the transformation pathways under the Vis/g-C 3 N 4 /CuFe 2 O 4 /PDS process were tentatively proposed based on the intermediates. The research provided a potential approach of CuFe 2 O 4 modified g-C 3 N 4 as a photocatalyst combined with PDS for the treatment of contaminated water.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2018
·Vol. 29
·期 24
·20580-20587
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IF 2.324
Fang Lu,Xue Yan,Hu Xing-Ming,Xie Dong,Li Wen-Jun
Electrochemiluminescence (ECL) is a very sensitive method for trace analysis because of its background interference and high signal-to-noise ratio. In the past decade, the determination of Cu 2+ in environment has attracted considerable attention since it plays an essential role in many physiological processes. Herein, a novel ECL sensor based on C,N quantum dots embedded g-C 3 N 4 nanosheets (C,N-QDs@NSs) was constructed for the detection of Cu 2+ . The nanocomposite was rapidly obtained via the oxidation of normal g-C 3 N 4 in H 2 O 2 solution using sonochemical synthesizing method. Due to the abundant surface defects on C,N-QDs@NSs, the ECL intensity was magnified 2.5 times for using a C,N-QDs@NSs electrode in comparision to a g-C 3 N 4 modified electrode. Besides, C,N-QDs@NSs could accelerate the rate of electron transfer in ECL reaction and thus resulted in the lower cathodic peak potential. Significantly, Cu 2+ could effectively quench the ECL of C,N-QD@NSs, which endowed C,N-QD@NSs with a great advantage in the ECL detection of Cu 2+ . under optimum conditions, C,N-QDs@NSs modified electrode exhibited a linear detection range from 5 × 10 −4 to 10 µM with a detection limit of 2 × 10 −4 µM (S/N = 3) for Cu 2+ , and was finally applied to detect Cu 2+ in real samples with satisfactory results.
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Nano Energy
·
2015
·
IF 10.325
Guisheng Li,Zichao Lian,Wenchao Wang,Dieqing Zhang,Hexing Li
Size-controllable g-C 3 N 4 quantum dots (QDs) were in-situ synthesized and grafted onto single-crystalline TiO 2 nanotube arrays (TiO 2 -NTAs) based on nanotube-confinement effect. This photoelectrocatalyst exhibited high activity in synergetic H 2 evolution and organic pollutant degradation. The g-C 3 N 4 QDs, together with TiO 2 -NTAs due to multiple light reflections, promoted light harvesting owing to the narrow energy band gap and upconversion from quantum size effect of g-C 3 N 4 QDs. Meanwhile, the single-crystal TiO 2 in-situ formed during the g-C 3 N 4 synthesis process favored the photoelectron transfer, and the g-C 3 N 4 /TiO 2 heterojunctions further promoted separation of photoelectrons from holes. Moreover, the strong g-C 3 N 4 –TiO 2 interaction and the confinement effect of TiO 2 nanotubes efficiently inhibited self-gathering and leaching of g-C 3 N 4 QDs, leading to excellent stability in photoelectrocatalysis .
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RSC Advances
·
2015
·Vol. 5
·期 107
·88249-88257
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IF 3.84
Jinjuan Xue,Shuaishuai Ma,Yuming Zhou,Qianli Wang
A novel ternary plasmonic photocatalyst, Au-loaded porous graphitic C3N4/graphene layered composite (Au/pg-C3N4/GR), was fabricated by a facile sonication-photodeposition technique. In this hybrid structure, a polymeric semiconductor pg-C3N4 was immobilized on the surfaces of graphene sheets to form a layered composite with Au nanoparticles of sizes 10–15 nm uniformly deposited on it. The photocatalytic performance of the as-prepared Au/pg-C3N4/GR composite was evaluated by degradation of methylene blue (MB) and ciprofloxacin (CIP) as representative dye pollutant and antibiotic pollutant under visible light irradiation, respectively. The degradation rates of MB and CIP over the Au/pg-C3N4/GR photocatalyst were 4.34 and 3.05 times higher that of porous g-C3N4 (pg-C3N4), respectively, and even 7.42 and 6.09 times higher than that of pure g-C3N4, respectively. The results indicated that an improved photocatalytic efficiency was obtained when Au nanoparticles and graphene sheets co-incorporated in porous g-C3N4. The porous structure within the samples is advantageous to the adsorption capacity. The surface plasmon resonance (SPR) effect of Au and electron-acceptor role of graphene, which would improve the visible light harvesting ability, facilitate photogenerated charge carrier separation, as well as create more active reaction sites, and synergistically contribute to the enhancement of photocatalytic activity. Moreover, a possible photocatalytic mechanism was also tentatively proposed.
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JOURNAL OF HAZARDOUS MATERIALS
·
2014
·
IF 4.331
Jinfeng Zhang,Yingfei Hu,Xiaoliang Jiang,Shifu Chen,Sugang Meng,Xianliang Fu
A direct Z-scheme photocatalyst Bi 2 O 3 /g-C 3 N 4 was prepared by ball milling and heat treatment methods. The photocatalyst was characterized by X-ray powder diffraction (XRD), UV–vis diffuse reflection spectroscopy (DRS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Brunauer–Emmett–Teller (BET) surface areas, photoluminescence technique (PL), and electron spin resonance (ESR) technology. The photocatalytic activity was evaluated by degradation of methylene blue (MB) and rhodamine B (RhB). The results showed that Bi 2 O 3 /g-C 3 N 4 exhibited a much higher photocatalytic activity than pure g-C 3 N 4 under visible light illumination. The rate constants of MB and RhB degradation for Bi 2 O 3 (1.0 wt.%)/g-C 3 N 4 are about 3.4 and 5 times that of pure g-C 3 N 4 , respectively. The migration of photogenerated carriers adopts a Z-scheme mechanism. The photoexcited electrons in the CB of Bi 2 O 3 and photogenerated holes in the VB of g-C 3 N 4 are quickly combined, so the photoexcited electrons in the CB of g-C 3 N 4 and holes in the VB of Bi 2 O 3 participate in reduction and oxidation reactions, respectively. O 2 − , OH and h + are the major reactive species for the Bi 2 O 3 /g-C 3 N 4 photocatalytic system.
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PubMed
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Journal of Environmental Chemical Engineering
·
2014
·
IF 0
Wei Chen,Zhouli Chen,Tianyu Liu,Zhimin Jia,Xiaoheng Liu
Novel hybridization of g-C 3 N 4 /Zn 0.28 Cd 0.72 S heterjunctions photocatalysts was successfully synthesized via the combination of chemisorptions and thermal post-treatment, wherein the g-C 3 N 4 serves as substrates to provide sites to anchor the Zn 0.28 Cd 0.72 S nanorods . These nanostructured g-C 3 N 4 /Zn 0.28 Cd 0.72 S composites were extensively characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), ultraviolet–visible diffuse reflection spectroscopy (UV–vis-DRS) and X-ray photoelectron spectrometer (XPS). The UV–vis-DRS results revealed that absorption spectral range of hybrid composites is a monotonous enhancement with the increasing Zn 0.28 Cd 0.72 S concentration in the visible light region. Interestingly, the catalytic performance of the g-C 3 N 4 /Zn 0.28 Cd 0.72 S is strongly dependent on the loading of Zn 0.28 Cd 0.72 S. The photocatalytic results demonstrate that 70 wt% g-C 3 N 4 /Zn 0.28 Cd 0.72 S hybrid photocatalyst exhibits the highest efficiency for the degradation of RhB and 4-ABA pollutants under visible light irradiation. And cycling photocatalytic tests for photocatalytic decomposition of RhB also indicate this photocatalyst is stable enough. The Fermi level ( E F ) and band position calculations reveal that g-C 3 N 4 and Zn 0.28 Cd 0.72 S are well-matched overlapping band structure, which may be in favour of enhanced separation rate of holes and electrons for reason of the development of heterogeneous interface. The interfacial charge transfer process was further verified in the photoreaction system of g-C 3 N 4 /Zn 0.28 Cd 0.72 S on the basis of VB-XPS and photoluminescence spectra (PL) analysis.
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APPLIED CATALYSIS A-GENERAL
·
2015
·
IF 3.942
Hong Liu,Zhengzheng Xu,Zhe Zhang,Dan Ao
A series of novel visible light-responsive Mn 0.8 Cd 0.2 S/g-C 3 N 4 hybrid materials with different g-C 3 N 4 contents were synthesized via a facile hydrothermal method. The obtained Mn 0.8 Cd 0.2 S/g-C 3 N 4 composites displayed highly efficient photocatalytic activities for H 2 evolution from aqueous solutions containing sacrificial reagents (Na 2 S and Na 2 SO 3 ) under visible light ( λ > 420 nm) even without noble metal co-catalysts. The highest H 2 evolution rate of 4.0 mmol h −1 g −1 (with an apparent quantum efficiency of 4.1% at 420 nm) was achieved on the Mn 0.8 Cd 0.2 S/g-C 3 N 4 (10 wt%) sample, which was about 3.40 times higher than that of pure Mn 0.8 Cd 0.2 S. The enhanced photocatalytic activity of Mn 0.8 Cd 0.2 S/g-C 3 N 4 composites should be attributed to the well-matched band structure and intimate contact interfaces between Mn 0.8 Cd 0.2 S and g-C 3 N 4 , which led to the effective transfer and separation of the photogenerated charge carriers. In addition, the Mn 0.8 Cd 0.2 S/g-C 3 N 4 photocatalysts showed good stability during the photocatalytic water splitting to hydrogen under visible light. A possible mechanism of the enhanced photocatalytic activity of Mn 0.8 Cd 0.2 S/g-C 3 N 4 was also proposed.
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