Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 26
·14841-14850
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IF 12.732
Zhujian Huang,Minxian Shen,Junhong Liu,Jiaer Ye,Tewodros Asefa
Advanced oxidation processes (AOPs) aided by catalysts can efficiently degrade organic pollutants and decontaminate wastewater. In this work, a highly active catalyst composed of FeMn-functionalized graphitic carbon nitride (FeMn–C3N4) for AOPs is synthesized via a green synthetic route, involving a small amount of water and no organic solvents. The synthesis also produces only minimal wastewater as a biproduct. The material contains uniformly dispersed Fe and Mn atoms in the framework of g-C3N4. It shows a unique and high catalytic activity for three AOPs, namely a Fenton-like reaction, persulfate activation and visible-light photocatalysis, while also being reusable several times afterwards. Its catalytic activity is 2.6- to 8.0-fold higher than that of g-C3N4 in all three reactions. The optimal reaction conditions for the catalyst are determined, and the mechanisms by which it drives the reactions are proposed. Notably, the Fe and Mn species present in it contribute substantially to its enhanced catalytic activity. Moreover, compared with g-C3N4, FeMn–C3N4 has a narrower band gap and helps generate more ˙OH, SO4˙− and 1O2 species during the reaction. First-principles density functional theory (DFT) calculations reveal that the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) of FeMn–C3N4 are more delocalized than those of g-C3N4. As a result, the former shows enhanced photo-induced charge carrier separation. This highly active catalyst obtained with a facile synthetic route for these three aforementioned AOPs can have great potential for water treatment and environmental remediation applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Marimuthu Karpuraranjith,Yuanfu Chen,Sivamoorthy Rajaboopathi,Manigandan Ramadoss,Katam Srinivas,Dongxu Yang,Bin Wang
Herein, a simple, highly efficient and stable MoS 2 nanobox embedded graphitic-C 3 N 4 @TiO 2 (g-CN@TiO 2 ) nanoarchitecture was synthesized by a facile solvothermal approach. The nano-hybrid photocatalyst was constructed by TiO 2 nanoparticles anchored on the surface of g-CN nanosheets. Then highly crystalline three-dimensional porous MoS 2 nanobox was homogeneously distributed on the g-CN@TiO 2 surface. The g-CN@TiO 2 /MoS 2 hybrid achieved a high photocatalytic degradation efficiency of 97.5% for methylene blue (MB) dye pollutant under visible-light irradiant in an hour which was much better than TiO 2 @MoS 2, g-CN@TiO 2, MoS 2, TiO 2 and g-CN. Furthermore, the reaction rate ( k) value of g-CN@TiO 2 /MoS 2 for MB dye is as high as 3.18 X 10 -2 min −1 , which is ~ 2.65 times better than those of g-CN@TiO 2 and MoS 2 . This work presents a rational structure design, interfacial construction and suitable band gap strategy to synthesize advanced nano-hybrid photocatalyst for degradation of organic pollutant with excellent performance and long-term stability.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Xing Chen,Yao Liu,Xu-Xu Ke,Rohan Weerasooriya,Heng Li,Lian-Chao Wang,Yu-Cheng Wu
Methylated mercury is a bio-magnifier that readily crosses the blood-brain barrier exerting neurotoxic effects. Therefore, the development of a rapid and in situ method of methylmercury (CH 3 Hg + ) detection is research priority. We report a sensitive electrochemical method for the detection of CH 3 Hg + using a modified glassy carbon electrode with Au nanoparticles-graphitic carbon nitride (AuNPs/mpg-C 3 N 4 ). The AuNPs/mpg-C 3 N 4 nanocomposites was synthesized by photochemical method and characterized by X-ray diffraction (XRD), Scanning electron microscope (SEM), Transmission electron microscope (TEM), X-ray photoelectron spectroscopic (XPS), Fourier transform infrared spectrometer (FTIR). The results showed that Au nanoparticles were successfully loaded on the surface of mpg-C 3 N 4 and dispersed uniformly. AuNPs/mpg-C 3 N 4 combined the excellent catalytic properties of AuNPs and unique structure of mpg-C 3 N 4 to improve the electrochemical sensing performance of CH 3 Hg + . The AuNPs/mpg-C 3 N 4 GCE show a high sensitivity for CH 3 Hg + determination using Differential pulse stripping voltammetry (DPSV). The CH 3 Hg + calibration curve is linear within 1 μg/L ∼25 μg/L. The sensitivity and detection limit of CH 3 Hg + is 0.285 μA/μg −1 L and 0.103 μg/L (S/N = 3), respectively. The Hg 2+ shows chemical interference in CH 3 Hg + detection, which is minimized by the addition of SnCl 2 or Diethylene triamine pentaacetic acid (DTPA). We also determined the CH 3 Hg + concentration of natural waters with a ±106% spike recovery. A newly developed AuNPs/mpg-C 3 N 4 modified GCE sensor provides a promising platform for CH 3 Hg + detection in natural water.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 43
·22720-22727
·
IF 11.301
Xueming Dang,Ruying Yang,Zhe Wang,Siyi Wu,Huimin Zhao
Graphitic carbon nitride (g-C3N4) possesses unique electronic and optical properties in the visible-light-driven production of H2O2. However, bulk g-C3N4 suffers from inefficient sunlight absorption and low carrier mobility. Herein, P doped g-C3N4 with a hollow sphere architecture was synthesized. The hollow sphere structure provides a large accessible surface area for charge transfer and enhances photo-absorption properties. Particularly, the doped P can regulate the energy band structure with stronger reducibility for O2 activation and accelerate photo-generated carrier separation. Meanwhile, the P heteroatom is beneficial to produce 1,4-endoperoxide species more easily and enhance selectivity for H2O2 synthesis through a two-electron O2 reduction process. The resultant catalyst exhibits a high H2O2 production rate of 174 μmol h−1 g−1 in pure water and 1684 μmol h−1 g−1 with isopropanol as a hole scavenger, which are 7.5 and 11.2 times those of bulk g-C3N4. This work provides a new avenue for the design and modification of other photocatalysts for H2O2 production.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
·
IF 4.939
Puhui Deng,Weisong Hong,Zhiwei Cheng,Linping Zhang,Yu Hou
Ni/porous g-C 3 N 4 was prepared by high temperature thermal polymerization process using carbon dots as soft template and photodeposition. With nickel nanoparticles supported as co-catalyst, the hydrogen evolution reaction (HER) activity of the photocatalyst has been significantly enhanced under visible light, which is up to 1273.58 μmol g −1 h −1 , superior to pristine g-C 3 N 4 (4.12 μmol g −1 h −1 ). This is attributed to the inhibited recombination of photogenerated electron-hole pairs and the much better electron transport efficiency. The formed porous structure of carbon nitride could facilitate light utilization and together with nickel nanoparticles, better charge separation can be realized which are proved by the photoluminescence , time-resolved photoluminescence spectra , transient photocurrent measurements and electrochemical impendence spectroscopy. This work provides a useful route to obtain less expensive and efficient photocatalyst containing no noble metals for hydrogen production .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Wenliang Liu,Su Chang,Dong Liu,Fushan Wen
Three-dimensional ordered macroporous (3DOM) materials have been widely concerned due to the unique structure. Herein, pure TiO 2 , pristine g-C 3 N 4 , 3D-Ti (TiO 2 with 3DOM structure) and 3D-xCN/Ti (x = 25 and 35 wt %) (3DOM materials with a certain ratio of TiO 2 and g-C 3 N 4 as the pore walls) were prepared. The morphologies of the samples were characterized by SEM, TEM and HRTEM, and the physical and chemical properties of the samples were explored by FT-IR, XPS, BET and UV–vis DRS. The 3D-25CN/Ti, with the structure of 3DOM and the couple of g-C 3 N 4 and TiO 2 , extended the light spectral responsive range, and exhibited an excellent hydrogen evolution rate (14.1 mmol g −1 h -1 ) , which was 28 times that of pure TiO 2 (0.55 mmol g −1 h -1 ) under simulated sunlight. The high hydrogen evolution rate is attributed to the synergistic effect of the great separation and transfer capability of charge carriers and the larger specific area, which originate from the g-C 3 N 4 /TiO 2 heterojunction and the 3DOM structure, respectively. The effective separation of the carriers was further confirmed through the photoluminescent spectroscopies and a series of photoelectrochemical experiments: Tafel, transient photocurrent response, electrochemical impedance. Finally, the mechanism of the photocatalytic hydrogen evolution was briefly discussed. These investigations reveal an important new strategy for improving the efficiency of photocatalytic hydrogen evolution.
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Inorganic Chemistry Frontiers
·
2020
·Vol. 8
·期 5
·1154-1165
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IF 5.958
Kunqiao Li,Wanbao Wu,Yanqiu Jiang,Zhe Wang,Xing Liu,Junzhuo Li,Debin Xia,Xianzhu Xu,Jizhuang Fan,Kaifeng Lin
The Z-scheme photocatalytic system has great potential in solar energy conservation with simultaneous wide light-absorption range, efficient electron–hole pair separation and strong redox ability. Herein, a direct Z-scheme g-C3N4/MoO3 photocatalytic composite with oxygen vacancies is successfully fabricated via a facile in situ method of a one-pot pyrolysis strategy. The as-prepared g-C3N4/MoO3 possesses a porous architecture with increased specific surface area. The existence of an oxygen vacancy in MoO3 is verified by XPS, UV-DRS analysis and electrochemical measurements. The g-C3N4/MoO3 exhibits superior visible-light photocatalytic performance for water splitting, as evidenced by an about 17-fold (20.52 μmol h−1) increase in the rate of H2 evolution relative to pristine C3N4 (1.23 μmol h−1). According to the characterization results and boosted photocatalytic performance, the migration and separation of photoinduced charge carriers in g-C3N4/MoO3 follows a possible mechanism based on a Z-scheme photocatalytic system constructed by the oxygen vacancies. The O-vacancy functions as the recombination and storage center for fast charge transfer through two components. The combined effect of defective MoO3 and a Z-scheme interfacial heterojunction has achieved greatly enhanced photocatalytic performance. This work demonstrates the facilitation effect of an effective Z-scheme system involving oxygen vacancies on the charge transfer to enhance the photocatalytic activity for water splitting.
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
·
2020
·Vol. 38
·期 2
·2000272
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IF 3.099
Gongduan Fan,Jiuhong Lin,Mingqian Xia,Jing Luo,Banghao Du,Heliang Pang,Zhongsen Yan
Photocatalysis has attracted much attention as an emerging algae removal technology, but the inactivation performance is inevitably affected by the extracellular polymeric substance (EPS) produced by algae. In this study, a photocatalyst (Ag 2 O/g-C 3 N 4 ) with efficient algae inactivation is adopted to investigate the interactions with EPS, and the impact of EPS on photocatalytic algae removal is studied. The results show that EPS can adhere to the surface of Ag 2 O/g-C 3 N 4 by electrostatic force. The interaction with EPS decreases the surface zeta potential of the Ag 2 O/g-C 3 N 4 from 7.71 to −22.3 mV with the increase in EPS concentration, and the maximum ratio of particle size increases from 825 to 1281 nm. In addition, the interaction with EPS inhibits the release of Ag + in Ag 2 O/g-C 3 N 4 by half, thus, the toxicity of metal ions will be alleviated. Meanwhile, EPS can also be degraded by Ag 2 O/g-C 3 N 4 , indicating that EPS can work as a radical scavenger to protect the algae cells. Without the protection of EPS, 97.8% of algae cells are inactivated after 5 h photocatalysis. Therefore, more attention should be given to the interaction between EPS and photocatalyst to promote the design and application of the photocatalytic.
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CARBON
·
2020
·
IF 8.821
Jinqiao Li,Xiaoteng Liu,Huinan Che,Chunbo Liu,Chunxiang Li
Realizing the efficient utilization of photogenerated carriers is a pivotal process to access the efficient transformation of light energy . Herein, we firstly practice a facile template method to synthesize O-doped crystalline/none-crystalline g-C 3 N 4 embedded nano-homojunction photocatalysts (CMCCN-x). This nano-homojunction makes the crystalline phase sufficiently contact with amorphous phase and further facilitates the photoinduced electron transformation. Therefore, the best performance catalyst CMCCN-5 well integrates the advantages of crystal g-C 3 N 4 and amorphous g-C 3 N 4 , which exhibits an excellent photogenerated carrier separation ability and abundant photocatalytic hydrogen evolution reaction activity sites. Excellent performance in the separation and use of photogenic carriers endows CMCCN-5 with efficient utilization of photogenerated carriers. Although there is a limited light absorption range (<460 nm), the photocatalytic hydrogen evolution rate of CMCCN-5 is up to 203.66 μmol h −1 under the visible light irradiation, about 86 times higher than pristine g-C 3 N 4 . The AQY numbers of CMCCN-5 at 420 nm and 450 nm are up to 26.9% and 14.0%, respectively. Thus, the significant effectiveness is forcefully proved for the facile construction of O-doped g-C 3 N 4 crystalline/none-crystalline nano-homojunction.
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Environmental Science-Nano
·
2021
·Vol. 8
·期 3
·773-783
·
IF 8.131
Haixia Wang,Dong Liang,Yan Xu,Xiang Liang,Xiaoqing Qiu,Zhang Lin
The development of an effective and stable photochemical sensor is urgently needed to solve the growing environmental pollution problem caused by immoderate usage of the organic phosphorus pesticide, chlorpyrifos. Under the circumstances, 2D/2D Z-scheme β-Bi2O3/g-C3N4 heterojunctions have been attempted to fabricate a photoelectrochemical sensor, which can detect chlorpyrifos selectively and sensitively. The 2D/2D intimate contact interfaces could facilitate the separation and migration of electron–hole pairs. Consequently, β-Bi2O3/g-C3N4 composites possess higher photocurrent response than single β-Bi2O3 and g-C3N4. After incubation with chlorpyrifos, in situ formed Bi–chlorpyrifos complex blocks the transformation of photogenerated charges, and thus contributes to a dramatic decline in photocurrent signal intensity and selective determination of chlorpyrifos. The novel photoelectrochemical sensor with strong stability presents a perfect linear relationship between photocurrent intensity and logarithm of chlorpyrifos concentration ranging from 0.01 to 80 ng mL−1, and displays excellent properties over a wide linear range with an ideal detection limit of 0.03 ng mL−1 (S/N = 3). To some extent, the Z-scheme β-Bi2O3/g-C3N4 sensor is promising for the detection of chlorpyrifos pesticides in practical environmental pollution treatment applications.
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CHEMICAL PHYSICS LETTERS
·
2020
·
IF 2.029
Hao Zhang,Yunqing Tang,Zhixiang Liu,Zhi Zhu,Xu Tang,Yemei Wang
Alkali metal (Li, Na, K and Rb) doped g-C 3 N 4 were prepared by water bath heating and high temperature calcination method. Photoelectric properties were studied by first-principles calculations and experiments. Computational results show that absorption spectra of Rb doped g-C 3 N 4 increases significantly in the wavelength range of 500–1100 nm, which is consistent with the UV–vis spectrum. Rb doped g-C 3 N 4 showed the best photo-reduction CO 2 performance, with a CO productivity more than three times higher compared with bulk g-C 3 N 4 . This work provides a guiding significance for construction of doped g-C 3 N 4 materials applied in fields of environmental remediation, energy conversion and medical imaging.
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RSC Advances
·
2020
·Vol. 10
·期 2
·1181-1190
·
IF 3.119
Weidong Peng,Chun Yang,Jiang Yu
A facile and feasible method was successfully utilized to incorporate Bi2O3 and g-C3N4 quantum dots on TiO2 surface to synthesize a novel composite g-C3N4/TiO2/Bi2O3. The photocatalytic activity of the composite g-C3N4/TiO2/Bi2O3 for degradation of dyes under sunlight and UV light irradiation was evaluated. It possessed the higher photocatalytic performance than that of pristine TiO2 or g-C3N4 under the same conditions. Under sunlight irradiation, the reaction rate constants of the g-C3N4/TiO2/Bi2O3 was about 4.2 times and 3.3 times higher than that of TiO2 and g-C3N4, respectively. The promising photocatalytic performance was attributed to the broader light absorption range and efficient separation of photoinduced carriers. Moreover, based on the TEM, XPS, XRD, UV-vis spectrum, radicals scavenging test and Mott–Schottky analysis systematic mechanism for photodegradation process was proposed. This work provides a promising strategy for the modification of TiO2-based semiconductors by incorporating different quantum dots and promoting the efficiency of the photocatalysts in practical application.
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