CHINESE JOURNAL OF CATALYSIS
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2019
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IF 4.914
Lijie Xu,Lanyue Qi,Yang Sun,Han Gong,Yiliang Chen,Chun Pei,Lu Gan
Excitation of metal-free graphitic carbon nitride (g-C 3 N 4 ) under visible light can successfully achieve efficient activation of peroxymonosulfate (PMS). Synergistic effects and involved mechanism were systematically investigated using a light-inert endocrine disrupting compound, dimethyl phthalate (DMP), as the target pollutant. Under visible light irradiation, DMP could not be degraded by direct g-C 3 N 4 -mediated photocatalysis , while in the presence of PMS, the dominant radicals were converted from •O 2 to SO 4 • - and •OH, resulting in effective DMP degradation and mineralization. Results showed that higher dosage of PMS or g-C 3 N 4 could increase the activation amount of PMS and corresponding DMP degradation efficiency, but the latter approach was more productive in terms of making the most of PMS. High DMP concentration hindered effective contact between PMS and g-C 3 N 4 , but could provide efficient use of PMS. Higher DMP degradation efficiency was achieved at pH lower than the point of zero charge (5.4). Based on intermediates identification, the DMP degradation was found mainly through radical attack (•OH and SO 4 • - ) of the benzene ring and oxidation of the aliphatic chains.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Xiuquan Xu,Songmei Wang,Xiaofeng Yu,Jila Dawa,Dongliang Gui,Ronghui Tang
Photocatalytic inactivation has been proved to be an effective strategy for controlling biohazards. Herein, the novel Ag deposited phosphorus and sulfur co-doped g-C 3 N 4 (PSCN) composites with different Ag content were constructed via a facile calcination combining with biogenic-reduction method for inactivating Escherichia coli ( E. coli ). The detailed characterization results indicated that P and S elements were successfully co-doped into g-C 3 N 4 (CN) lattice and Ag nanoparticles (NPs) were evenly deposited on the surface of PSCN with diameter range of 4–20 nm. The Ag/PSCN at depositing amount of 4 wt% (Ag/PSCN-4) achieved the strongest photocatalytic inactivation along with excellent stability, which could completely inactivate 7.0 log cells of E. coli within 60 min of visible light irradiation. This improved bactericidal performance was mainly attributed to the synergistic effects of P-S co-doped together with Ag deposition, which resulted in the increased visible light utilization, the improved separation and transfer efficiency of photo-induced charge carriers. Moreover, active species trapping experiments revealed that the generated superoxide radicals ( O 2 − ) and holes (h + ) played the significant roles in photocatalytic inactivation process. Our present work presented a promising and environmentally friendly strategy to enhance the photocatalytic capacities of CN based composites for pathogens inactivation.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Fang He,Lan Luo,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
Design of highly condensed g-C 3 N 4 is a prospective way to optimize the photoreactivity of g-C 3 N 4 as it possesses condensed structure with decreased interlayer spacing, which benefits both charge transfer and light harvesting. Herein, we report that novel condensed carbonized-tannic acid (C-TA)/g-C 3 N 4 composites have been acquired via a supramolecular self-assembly of TA and melamine into TA/melamine precursors followed by thermal condensation. The acquired condensed C-TA/g-C 3 N 4 composites present superior visible-light photocatalytic activity for H 2 evolution. The 1 wt% C-TA/g-C 3 N 4 composite shows 4.2 times enhancement of photocatalytic activity for H 2 evolution compared to pristine g-C 3 N 4 . The TA with distinct adhesion properties and functional groups of OH, which is firmly linked with melamine, can confine the melamine inside to promote the condensation to gain more condensed g-C 3 N 4 . The condensed C-TA/g-C 3 N 4 composites with decreased interlayer distance effectively promote charge transfer and photocatalytic H 2 evolution.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Mengmeng Dou,Jin Wang,Boru Gao,Ce Xu,Fan Yang
β-Lactam antibiotics are generally used for disease prevention in humans and animals. The antibiotics, which have been excreted into the surrounding environment, have caused serious concerns. In this study, mesoporous carbon nitride (MCN) was synthesized using a template-free method. The photocatalytic degradation of the two typical β-lactam antibiotics, amoxicillin (AMX) and cefotaxime (CFX), was performed using MCN. Considering the complexity of the actual environment, four factors that may influence the photocatalytic degradation of AMX and CFX were studied, containing the initial antibiotics concentration, catalyst dosage, pH and humic acid (HA). The possible mechanism of photocatalysis was presented using ESR spectroscopy and free radical trapping experiments. Furthermore, rational photocatalytic degradation pathways were proposed through the combination of LC-Q-TOF-MS/MS and density functional theory (DFT). Toxicity Estimation Software Tool (TEST) was used to predicate the toxicity of the byproducts. This study identified the catalytic activity difference between AMX and CFX firstly and elucidated their degradation mechanisms. The new findings are very meaningful for optimizing the conditions of photocatalytic degradation of β-lactam antibiotics. In addition, the results of wastewater test and stability experiments indicated that MCN has excellent performance. Therefore, MCN is a promising treatment material for the elimination of the antibiotic activity and mineralization of antibiotics under visible light.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Xianlong Zhang,Dong An,Dexin Feng,Fengbing Liang,Zhen Chen,Weimin Liu,Zhenzhen Yang,Mo Xian
Herein, in situ surfactant-free synthesis of ultrathin BiOCl/g-C 3 N 4 (BOC/CN) nanosheets for enhanced visible-light photodegradation of rhodamine B was described. The formation procedure, microstructural morphology, structure, optical properties , and photocatalytic activity were researched in detail. The results show that ultrathin BOC/CN heterojunctions nanosheets were successfully constructed via one-step surfactant-free solvothermal method by introducing CN into the synthesis system of BOC, and the thickness of BOC/CN nanosheets was ~3.5 nm. The ultrathin 2D/2D BOC/CN heterojunctions significantly enhanced the photodegradation of RhB dye under visible-light irradiation. The best-performing sample BOC/CN-60 had 3.9 and 12.8 times higher photocatalytic efficiency for visible-light RhB removal compared to pure BOC and CN, respectively. The large enhancement in the photodegradation activity should be attributed to the synergistic effect of BOC and CN in BOC/CN nanosheets. The synergism reflects in the widened optical window for effective light absorption , enlarged interfacial area for more efficient electron-hole separation, and a shorter diffusion distance for facilitated charge transfer. A possible visible-light RhB photodegradation mechanism was proposed, based on theoretical analysis and active species trapping experiments.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Weixuan Zeng,Yuan Bian,Sheng Cao,Anquan Zhu,Lulu Qiao,Yongjin Ma,Pengfei Tan,Quanyin Ma,Rui Dong,Jun Pan
Visible light-driven photocatalytic hydrogen production has been deemed a potential means to solve the increasingly serious energy shortage problem. Herein, two dimensional (2D) Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposites that applied in photocatalytic water reduction were fabricated through thermal condensation of thiourea with hydrothermal-prepared Sr 2 Ta 2 O 7 . The resulted Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposite exhibited enhanced hydrogen evolution rate (11.36 μmol g −1 h −1 ) under visible light irradiation, which is about 3.5 times higher than that of pure S-doped g-C 3 N 4 . In light of the UV–vis diffuse reflectance spectroscopy, Mott-Schottky curve and photoluminescence spectra, the enhanced photocatalytic performance could be mainly attributed to the conduction band difference between Sr 2 Ta 2 O 7 and S-doped g-C 3 N 4 . In addition, transient photoluminescence spectra, electrochemical impedance spectra and photocurrent responses proved that the presence of Pt cocatalyst also plays an important role in facilitates the transport of photoexcited electron-hole pairs, subsequently promoting the photocatalytic performance.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Zizheng Ai,Yongliang Shao,Bin Chang,Lei Zhang,Jianxing Shen,Yongzhong Wu,Baibiao Huang,Xiaopeng Hao
As a metal-free polymeric semiconductor, graphitic carbon nitride (g-C 3 N 4 ) is a promising candidate for photocatalytic water splitting but suffers from the insufficient optical absorption and sluggish utilization of photocarriers. Herein, based on the energy band engineering theory, a new design philosophy of tunable p-n homojunction is proposed and realized in a novel P-doped g-C 3 N 4 (PCN) material. Through regulating the tendency of transformation in p-n homojunction, a strong internal electric field is built and integrated with two secondary internal electric fields by further decorating with Ti 3 C 2 , leading to the formation of a triple-internal electric field system. Thus the spatial separation efficiency of photocarriers is improved and their lifetime is prolonged. The specific photocatalyst exhibits excellent overall water splitting performance in pure water with a notable quantum yield. This work presents a peculiar concept of adjustable p-n homojunction and holds great significance for the rational design of advanced photocatalyst in water splitting.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Qiao Wang,Peng Xu,Guangshan Zhang,Limin Hu,Peng Wang
Visible-light responsive g-C 3 N 4 catalysts were successfully prepared by the calcination of urea, i.e., the thermal polycondensation method, and a series of ZnS/g-C 3 N 4 composite photocatalysts were then synthesized using a rapid microwave hydrothermal method . The physicochemical properties of the resulting g-C 3 N 4 and ZnS/g-C 3 N 4 catalysts were characterized via several microscopy and spectroscopy techniques . The reduction of Cr(VI) was used to evaluate the photocatalytic performance of the as-synthesized catalysts under visible light irradiation. The results showed that the calcination temperature substantially affected the crystallinity , specific surface area and photocatalytic performance of g-C 3 N 4 . The optimal temperature for thermal polycondensation in the g-C 3 N 4 synthesis was 600 °C. The bulk g-C 3 N 4 catalyst exhibited no Cr(VI) reduction ability, while a certain amount of ZnS nanoparticles coupling with g-C 3 N 4 significantly improved the Cr(VI) reduction efficiency, creating a synergistic effect between g-C 3 N 4 and ZnS. The simultaneous Cr(VI) reduction and rhodamine B decolorization by the ZnS/g-C 3 N 4 composite catalyst were also accomplished. In addition, a Cr(VI) reduction mechanism under visible light irradiation was proposed.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Huiping Zhao,Guangfang Li,Fan Tian,Qintao Jia,Yunling Liu,Rong Chen
To overcome the issue of UV-light response character of Bi 2 O 2 CO 3 due to its wide band gap, we primarily attempted to understand the possibility of improving the photocatalytic activity of Bi 2 O 2 CO 3 via g-C 3 N 4 surface-decoration by the theoretical calculation. Subsequently, g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 was successfully prepared via a facile hydrothermal method. It was found that the g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 samples exhibited enhanced activities for the photodegradation of tetracycline compared with pure Bi 2 O 2 CO 3 upon simulated solar light irradiation. Among them, the 10 wt% g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 sample showed the highest photocatalytic efficiency. First principle calculation and experimental data confirmed that the charge transfer at the interface between g-C 3 N 4 and Bi 2 O 2 CO 3 could significantly suppress the recombination of photo-generated electron-holes pairs, thus improving the photocatalytic performance. The proposed mechanism for the enhanced photocatalytic activity was also discussed. Moreover, the photodegradation of antibiotics over g-C 3 N 4 surface-decorated Bi 2 O 2 CO 3 was also performed in actual water matrix.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2019
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IF 7.65
Lu-Lu Qu,Zhi-Qin Geng,Wen Wang,Kai-Chun Yang,Wei-Peng Wang,Cai-Qin Han,Guo-Hai Yang,Robert Vajtai,Da-Wei Li,Pulickel M. Ajayan
A three-dimensional (3D) substrate was developed by assembling a monolayer of graphitic carbon nitride (O-g-C 3 N 4 ) on Ag nanorod arrays (Ag NRs) for sensitive and recyclable surface enhanced Raman scattering (SERS) detection. The prepared Ag NRs/O-g-C 3 N 4 substrate not only generated a significant Raman enhancement effect as a result of the strong π-π stacking interaction between O-g-C 3 N 4 and the analytes but also possessed excellent self-cleaning property via visible-light irradiation that was attributed to its outstanding catalytic performance. Highly sensitive SERS detection could be achieved with a LOD of 8.2 × 10 −10 M for R6 G, and the substrate could be used repeatedly for at least four cycles with tolerable intensity attenuation. In addition, the 3D substrate exhibited long-term stability originating from the electron-donor effect of O-g-C 3 N 4 and high reproducibility due to the uniform decoration of O-g-C 3 N 4 on the Ag NRs through the strong interaction. Furthermore, using Ag NRs/O-g-C 3 N 4 , the recyclable detection of antibiotics in a water sample was demonstrated with high sensitivity, which indicates that the 3D Ag NRs/O-g-C 3 N 4 substrate is a promising candidate for eliminating the challenges of single-use SERS substrates and building a portable SERS platform to sense organic molecular species.
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PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Lingli Wang,Yu Zhu,Dan Yang,Lei Zhao,Hanming Ding,Zhaohui Wang
Effective photogenerated charge separation and rapid Cu(II)/Cu(I) redox cycling is still challenging for photocatalytic reactions and copper-based Fenton-like process, respectively. Herein, a novel heterogeneous Fenton-like catalyst of copper incorporated carbon ring- g -C 3 N 4 (Cu-C-CN) was prepared through a facile calcination method. The carbon ring could be intimately connected with g -C 3 N 4 via sp 2 -hybridized C N bonds to form an in-plane π-conjugated structure. The carbon ring spliced g -C 3 N 4 (C-CN) can serve as an effective electron-hole separator owing to the varied electron affinity of two domains (e.g. carbon-ring and g -C 3 N 4 ). The copper species were further introduced to the framework of g -C 3 N 4 via the Cu N bonds to act as acceptors of conduction-electrons from g -C 3 N 4 and H 2 O 2 activators. Taking the photodegradation of methylene blue (MB) as a model reaction, the decomposition efficiency over Cu-C-CN is 5.5 times higher than that of pristine g -C 3 N 4 , and would nearly linearly increase with pH. The notable enhancement in photodegradation efficiency could be ascribed to the synergetic collaboration between photocatalysis process and Fenton-like process to generate abundant OH and e − . The Cu-C-CN catalyst shows high recycling stability with negligible Cu leaching due to the strong affinity of Cu 2+ to g -C 3 N 4 framework. The strategy of coupling Fenton-like catalysts, electron-deficient domains (e.g. carbon-ring) into semiconductor-based photocatalysis provides a facile and promising solution to the remediation of water pollution with solar energy.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Peng Lv,Chongyang Zhao,Woo Jae Lee,Siping Huo,Se-Hun Kwon,Jun Fang,Yang Yang
Zero-dimensional/two-dimensional (0D/2D) TiO 2 /g-C 3 N 4 heterostructural photocatalysts were fabricated via ALD technique. TiO 2 nanoparticles were “site-selectively grown” on g-C 3 N 4 nanosheets and the surface modification induced band engineering of the composite photocatalysts. Thus, the redox properties of the photocatalysts were fine tuned. Under visible light , since only g-C 3 N 4 was excited, TiO 2 was acting as the electron transport channel in the optimized interfacial structures . They effectively suppressed the recombination and facilitated the transfer of photogenerated charges, improving the photocatalytic activity. When both the components were excited under UV–vis light, the dynamic equilibrium of the conduction band positions on these n–n type semiconductor heterojunctions led to the increased recombination rate of charges, decreasing the reactivity for H 2 evolution. However, the photocatalytic degradation of organic pollutants by these composite photocatalysts exhibited enhanced activities, resulting from the photogenerated holes on VB of TiO 2 which could promote oxidation of organic pollutants with strong oxidation potentials. Furthermore, TiO 2 /g-C 3 N 4 photocatalysts with limited numbers of deposition cycles exhibited optimal photocatalytic activity under visible light. In contrast, excessive deposition cycles on g-C 3 N 4 for TiO 2 /g-C 3 N 4 led to continuous film and increased thickness of TiO 2 , resulting in the attenuation of the reactivity. We verified this TiO 2 /g-C 3 N 4 photocatalysts with less mass-loading, but more enhanced photocatalytic activity.
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高影响因子
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