CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weirui Chen,Siyou Fu,Xukai Li,Jing Wang,Xunan Ning,Liying Bin,Ping Li,Bing Tang,Laisheng Li
Photocatalytic ozonation (PCO) was a novel water treatment method, but the low photo-generated electron ( e - ) utilization and ambiguous ROS formation mechanism restrained its performance. Herein, C vacancy and F co-decorated g-C 3 N 4 (FCN_Cv) was designed to accelerate the PCO performance with sodium p -perfluorinated nonoxybenzenesulfonate (OBS) acting as model pollutant. Comparative characterizations revealed that FCN_Cv remained the inherent structure of g-C 3 N 4 (BCN), and had an enhanced conduction band potential, narrower band gap and longer e - lifetime. FCN_Cv exhibited the greater activity over BCN, with 99.3 % OBS removal in 30 min but only 78.3 % for BCN during PCO process. •OH was the main ROS for degrading OBS. The greater •OH yield was obtained by FCN_Cv PCO process because of the increase of e - utilization. On one hand, the two electrons reduction of O 2 into H 2 O 2 on FCN_Cv was accelerated, which triggered the peroxone reaction between photogenerated-H 2 O 2 and O 3 . On the other hand, the direct one electron reduction of O 3 by e - also accounted for •OH generation. 17 kinds of intermediates were detected and the OBS degradation routes were inferred, which was involved with hydroxylation, C-O cleavage and aromatic ring opening reactions. Overall, this study demonstrated the feasibility of decorating F element and C vacancy on g-C 3 N 4 in enhancing e - utilization and •OH generation during PCO process as well as deepened the understanding of fate of OBS in PCO process.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Shaoming Yang,Jiayi Chen,Long Yan,Yongxin Liu,Wenlin Zha,Zhili Fang,Jiali Zhang
A molecularly imprinted photoelectrochemical sensor was successfully designed for sensitive detection of norfloxacin (NOR) based on poly ( o -phenylenediamine) (PoPD) sensitized g-C 3 N 4 /Zr-MOFs(Fe) composite. Herein g-C 3 N 4 /Zr-MOFs(Fe) heterojunction composite was explored as photoresponsive oxidase mimic and photoactive material for the purpose of enhancing photoelectrochemical performances. In addition, PoPD molecularly imprinted polymers (MIPs) were introduced not only to act as the recognition element for selective performance, but also to possess photosensitive effect, which enhanced the photocurrent of sensor. SEM, element mapping method, XRD, UV–Vis and electrochemical impedance spectroscopy were employed for the characterization of the structural, chemical composition, optical and electrical properties of g-C 3 N 4 /Zr-MOFs(Fe) composite. Thanks to the photoresponsive oxidase mimic property and the selectivity of MIPs, the as-prepared sensor presented a good linear range of from 1.0 × 10 −8 mol/L to 2.0 × 10 −6 mol/L with NOR and a limit of detection of 5.7 × 10 −9 mol/L. Moreover, the sensor platform has been proved to have excellent selectivity and real sample application.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 47
·21944-21959
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IF 3.3
Xuanlan Luo,Jinhai Yuan,Junhong Liu,Haikun Hu,Ziyi Yang,Xiaopeng Hou,Qi Sun,Di Xu
Ultrasonic assisted hydrothermal and calcination methods were used to prepare type II heterojunction ZnBi2O4/g-C3N4 (ZBN) photocatalysts. The crystal structures, elemental compositions, morphologies and optical properties of the prepared monomer and heterojunction photocatalysts were characterized. The photocatalytic degradation efficiency of acid red B reached 95% in 180 min under UV irradiation, which was 1.82 and 1.44 times higher than that of g-C3N4 and ZnBi2O4, respectively, and the reaction rate constants were increased from 0.004 min−1 and 0.005 min−1 to 0.015 min−1. ZBN exhibited high photocatalytic activity, and the enhancement of activity can be attributed to the construction of the type II heterostructure and reduced carrier recombination. The degradation experiments of carmine, AO7, MO, MB and RhB showed that the composite ZBN had a better degradation effect on different dyes. The results of radical trapping experiments and EPR tests showed that ˙O2− plays a crucial role in the photocatalytic degradation of acid red B. Finally, the mechanism of the photocatalytic degradation of acid red B by ZBN was investigated by combining EPR, VB-XPS and radical trapping experiments.
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LANGMUIR
·
2023
·
IF 3.9
Yanting Dou,Yu Gao,Deng Gu,Jiqi Zheng,Bo Zhang,XiuXin Li,Meijia He,Qinglong Zou,Tiaoli Liao,Fu Ding,Yaguang Sun,Zhenhe Xu
Developing a photocatalyst that can effectively utilize the full solar spectrum remains a high-priority objective in the ongoing pursuit of efficient light-to-chemical energy conversion. Herein, the ternary nanocomposite g-C3N4/RGO/W18O49 (CN/RGO/WO) was constructed and characterized by a variety of techniques. Remarkably, under the excitation of photon energies ranging from the ultraviolet (UV) to the near-infrared (NIR) region, the photocatalytic performance of the CN/RGO/WO nanocomposite exhibited a significant enhancement compared with single component g-C3N4 or W18O49 nanosheets for the degradation of methyl orange (MO). The MO photodegradation rate of the optimal CN/1.0 wt% RGO/45.0 wt% WO catalyst reached 0.816 and 0.027 min–1 under UV and visible light excitation, respectively. Even under low-energy NIR light, which is not sufficient to excite g-C3N4, the MO degradation rate can still reach 0.0367 h–1, exhibiting a significant enhancement than pure W18O49. The outstanding MO removal rate and stability were demonstrated by CN/RGO/WO nanocomposites, which arise from the synergistic effect of localized surface plasmon resonance effect induced by W18O49 under vis–NIR excitation and the Z-scheme nanoheterojunction of W18O49 and g-C3N4. In this work, we have exploited the great potential of integrating nonmetallic plasmonic nanomaterials and good conductor RGO to construct high-performance g-C3N4-based full-solar spectral broadband photocatalysts.
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PubMed
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 23
·7810
·
IF 4.6
Truong Nguyen Xuan,Dien Nguyen Thi,Quang Tran Thuong,Tue Nguyen Ngoc,Khanh Dang Quoc,Zsombor Molnár,Shoaib Mukhtar,Erzsébet Szabó-Bárdos,Ottó Horváth
Graphitic carbon nitride (g-C3N4) has proved to be a promising heterogeneous photocatalyst in the visible range. It can be used, among others, for the oxidative conversion of environmentally harmful nitrophenols occurring in wastewater. However, its photocatalytic activity needs to be enhanced, which can be achieved by modification with various dopants. In our work, copper-modified g-C3N4was prepared by ultrasonic impregnation of the pristine g-C3N4synthesized from thiourea. The morphology, microstructure, and optical properties of the photocatalysts were characterized by XRD, FT-IR, DRS, SEM, XPS, and TEM. DRS analysis indicated a slight change in both the CB and the VB energies of Cu/g-C3N4compared to those of g-C3N4. The efficiency of the photocatalysts prepared was tested by the degradation of nitrophenols. Copper modification caused a sevenfold increase in the rate of 4-nitrophenol degradation in the presence of H2O2at pH = 3. This dramatic enhancement can be attributed to the synergistic effect of copper and H2O2in this photocatalytic system. A minor Fenton reaction role was also detected. The reusability of the Cu/g-C3N4catalyst was demonstrated through five cycles. Copper-modified g-C3N4with H2O2proved to be applicable for efficient visible-light-driven photocatalytic oxidative degradation of nitrophenols.Keywords:graphitic carbon nitride;photocatalysis;copper-modification;oxidation of nitrophenols;visible-light irradiation;pH effect;H2O2effect
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SENSORS AND ACTUATORS A-PHYSICAL
·
2023
·
IF 4.6
Ruizhen Li,Wanzhen Yuan,Yu Hu,Yonggang Zeng
Propranolol , a widely used β-adrenergic receptor antagonist drug with potential toxic effects to organisms and human beings, was not completely removed from environment through traditional wastewater treatments . It is necessary to sensitively and selectively monitor the trace content propranolol in various samples. In this work, a novel photoelectrochemical (PEC) aptasensor based on Au nanoparticles (NPs) modified g-C 3 N 4 /BiPO 4 heterojunction was successfully fabricated for detecting (S)-propranolol (S-Pro), an important racemic enantiomer of propranolol. Herein, g-C 3 N 4 was employed as visible light-active semiconductor. The photocatalytic activity of g-C 3 N 4 was enhanced via forming heterojunction with BiPO 4 to facilitate the separation and migration of photogenerated carriers . In addition, Au NPs with perfect conductivity and surface plasmon resonance (SPR) effect are not only beneficial to the electron transfer and visible light harvest of g-C 3 N 4 /BiPO 4 heterojunction, but also the crucial factor on assembling S-Pro-binding DNA aptamer via Au-S bonding. At the same time, as a π-π conjugated material, g-C 3 N 4 with large surface area also provides an excellent platform for loading Au NPs. Under the visible light illumination, the PEC aptasensor displayed high PEC performance. On such a sensor, specific captured S-Pro by the aptamer was quickly oxidized by the photogenerated holes to inhibit the recombination of the photogenerated carriers, enhanced the PEC response, and realized the detection of S-Pro. Under optimal conditions, the designed PEC aptasensor exhibited a wide linear range of 10 nM to 1000 nM with a low detection limit (defined as S/N = 3) of 2.55 nM. Moreover, the proposed sensor displayed high selectivity , good reproducibility, and general long-term stability. And the S-Pro in real sample was accurately detected using this proposed sensor.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 10
·1-14
·
IF 2.9
Jiang Huize,Yang Jinge,Wang Xinxin,Wang Aihong,li Yuzhi,Wang Jinyu
The massive use of acetaminophen (APAP) poses a potential crisis for humans and the environment. In this paper, the degradation of APAP in aqueous solution was carried out using photocatalytic synergistic persulfate oxidation. To enhance the photocatalytic activity of g-C 3 N 4 and thus activate the persulfate (K 2 S 2 O 8 , PS) more effectively, the heterojunction photocatalyst TiO 2 /g-C 3 N 4 (TCN) was prepared by a hydrothermal method. The TCN-PS catalytic system showed a high efficiency for APAP degradation. When the amount of TCN and PS added was 0.6 g/L, the degradation rate of APAP at 10 mg/L was 78.3% after 60 min of illumination. Moreover, the TCN-PS catalytic system was effective in removing organic pollutants in acidic, neutral, and weakly alkaline environments. The radical quenching experiment results indicate that both sulfate radicals (SO 4 − •) and hydroxyl radicals (•OH) are involved in the degradation reaction. After five cycles, the TCN-PS catalytic system still has stable catalytic activity.
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Nano Research
·
2023
·
IF 9.9
Yu Fan,Luo Chunjia,Niu Xiaohan,Chao Min,Zhang Pengfei,Yan Luke
Graphitic carbon nitride (g-C 3 N 4 ) nanosheets have attracted widespread interest in the construction of advanced separation membranes. However, dense stacking and a single functionality have limited the membrane development. Here, an advanced two-/three-dimensional (2D/3D) g-C 3 N 4 /TiO 2 @MnO 2 membrane is constructed by intercalating 3D TiO 2 @MnO 2 nanostructures into g-C 3 N 4 nanosheets. The 3D flower-like nanostructures broaden the transport channels of the composite membrane. The membrane can effectively separate five oil-in-water (O/W) emulsions, with a maximum flux of 3265.67 ± 15.01 L·m −2 ·h −1 ·bar −1 and a maximum efficiency of 99.69% ± 0.45% for toluene-in-water emulsion (T/W). Meanwhile, the TiO 2 @MnO 2 acts as an excellent electron acceptor and provides positive spatial separation of electrons–holes (e − –h + ). The formation of 2D/3D heterojunctions allows the material with wider light absorption and smaller bandgap (2.10 eV). These photoelectric properties give the membrane good degradation of three different pollutants, with about 100% degradation for methylene blue (MB) and malachite green (MG). The photocatalytic antibacterial efficiency of the membrane is also about 100%. After cyclic experiment, the membrane maintains its original separation and photocatalytic capabilities. The remarkable multifunctional and self-cleaning properties of the g-C 3 N 4 based membrane represent its potential value for complex wastewater treatment.
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Sustainability
·
2023
·Vol. 15
·期 17
·13279
·
IF 3.9
Ke Li,Miaomiao Chen,Lei Chen,Songying Zhao,Wencong Xue,Yanchao Han
In this study, a novel Fe3O4/Ag3PO4/g-C3N4magnetic composite photocatalyst was successfully synthesized, tailored specifically for the visible light-driven photocatalytic degradation of sulfonamide antibiotics, more precisely, sulfamethazine (SMZ). To analyze the fabricated samples, characterization techniques such as X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), photoluminescence spectroscopy (PL), and UV-vis diffuse reflectance spectra (UV-vis) were systematically employed. The composite showcased efficient visible-light absorption and charge separation, with its peak photocatalytic performance recorded at a solution pH value of 6.0. Significantly, the Fe3O4/Ag3PO4/g-C3N4magnetic composite photocatalyst displayed excellent stability and recyclability, consistently maintaining a high degradation efficiency of over 97% even after five consecutive cycles. Further experimentation with radical scavengers confirmed a significant decrease in photocatalytic activity, establishing that superoxide radicals (•O2−) and photo-generated holes (h+) are the primary active species during the degradation of SMZ. Overall, it provides a crucial understanding regarding the photocatalytic decomposition of sulfonamide antibiotics using magnetic composite photocatalysts. It also emphasizes the promising potential of the Fe3O4/Ag3PO4/g-C3N4composite for tangible applications in environmental remediation.Keywords:visible light;photocatalysis;Fe3O4/Ag3PO4/g-C3N4;sulfonamide
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Songyu Yang,Kailin Wang,Qiao Chen,Yan Wu
S-scheme heterostructure photocatalysts can achieve highly efficient solar energy utilization. Here, single-atom Ni species were deposited onto TiO 2 /g-C 3 N 4 (TCN) composite photocatalyst with an S-scheme heterojunction for highly efficient photocatalytic water splitting to produce hydrogen. Under solar irradiation, it realized the hydrogen production activity of 134 µmol g –1 h –1 , about 5 times higher than the TCN without atomic Ni. In-situ Kelvin probe force microscopy characterization and the density functional calculation certify that by forming the S-scheme heterojunction, the photo-excited electrons from the TiO 2 combine with the photogenerated holes at the coupled g-C 3 N 4 driven by a built-in electric field. More importantly, the single-atom Ni species stabilized the photogenerated electrons from the g-C 3 N 4 could effectively enhance the charge separation between the holes on the valence band of TiO 2 and electrons at the conduction band of g-C 3 N 4 . Meanwhile, the Ni atoms act as the surface catalytic centers for the water reduction reaction, which greatly improves the reactivity of the photocatalyst. The present work provides a new approach for developing noble metal-free heterojunctions for high-efficiency photocatalysis.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Ya Lu,Zhuanfang Bi,Guangyi Shang
Fluorene, as one of the important organic compounds widely used in the field of medicine and photoelectric materials, could damage human health even if it is extremely low in the environment. The development of ultrasensitive and easy-recyclable surface-enhanced Raman scattering (SERS) detection of trace fluorene is highly desired. In this work, a nanocomposite of Ag nanoparticles (Ag NPs) and porous g-C3N4 is synthesized by a facile method. The advantageous features of the as-prepared nanocomposite include a high SERS sensitivity due to the plasmonic effect of the Ag NPs, excellent recyclability due to the self-cleaning ability originating from the photocatalytic degradation of porous g-C3N4 under visible light irradiation, and good adsorption due to the large specific surface area of porous g-C3N4. The experimental results show that an ultralow detection limit of 1.35 × 10–13 M for R6G can be achieved. Especially, the nanocomposite exhibits excellent performance for the detection of fluorene with the detection limit of 3.11 × 10–11 M and multidetection of at least 13 cycles. The present research provides a nanocomposite with excellent synergistic activity of plasmonic enhancement and photocatalytic degradation for the recyclable SERS detection of trace fluorene.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Tao Yu,Tao Xie,Wei Zhou,Yizhong Zhang,Yiliang Chen,Boyu Shao,Wan-Qian Guo,Xin Tan
Tuning the structural defects of graphite carbon nitride (g-C3N4) is an effective strategy to modify its band structure and promote charge separation, but it is still limited by complex and harsh preparation processes. Herein, g-C3N4 with nitrogen defects were fabricated by one-pot thermal polymerization of urea and fumaric acid. The N–(C)3 site, being the active site for photocatalytic hydrogen evolution, reached at a rate of 94.1 μmol·h–1, which was approximately 2.64 times that of the original g-C3N4. Nitrogen defective g-C3N4 had more electrons and stronger H2O molecule adsorption capacity, identified by systematic experiments and DFT calculations. The carboxyl group of fumaric acid reacted with amino group of urea to prevent self-polymerization process of urea and induce nitrogen defects. The changed band structures promoted the absorption of visible light, effective separation of charge, and increased hydrogen evolution driving force. This work will provide a simple and green approach to prepare nitrogen defective g-C3N4 with tunable band structures.
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