DALTON TRANSACTIONS
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2020
·Vol. 49
·期 16
·5205-5218
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IF 4.174
Xiaoyi Chen,Xiuling Xue,Xiuwen Gong
A number of porous g-C3N4 nanosheet/Ag3PO4/NCDs (PCNNS/AP/NCDs) with little amounts of Ag3PO4 were synthesized via an in situ sedimentation–calcination method. The PCNNS/AP/NCDs photocatalyst exhibited excellent photocatalytic performance for the photocatalytic degradation of tetracycline (TC) under visible light irradiation at a removal rate of 90.5% in 40 min. The study of the reaction kinetics of the as-prepared samples was in accordance with the pseudo-second-order kinetics, with the correlation coefficient (R2) being greater than 0.9776. Meanwhile, the photocatalyst was capable of degrading ciprofloxacin (CIP), and showed good performance even under actual water conditions with natural sunlight irradiation, indicating that the photocatalyst has wide practical applications. In addition, the photocatalytic performance and the XRD and FTIR spectra showed no obvious changes even after four photocatalytic degradation cycles, which revealed the high stability of the PCNNS/AP/NCDs photocatalyst. Furthermore, the possible degradation pathways of TC and the possible Z-scheme mechanism were proposed with ˙O2− and h+ as the main active species contributing to photocatalytic degradation. The results provide a novel insight into the fabrication of Z-scheme PCNNS/AP/NCDs and introduce them as an efficient visible-light-responsive photocatalyst for use in practical applications.
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高影响因子
ADVANCED POWDER TECHNOLOGY
·
2020
·
IF 4.217
Yekun Zhu,Yun Zhang,Lili Cheng,Mohammed Ismael,Zhiyuan Feng,Ying Wu
The g-C 3 N 4 /NaNbO 3 photocatalyst was synthesized by simply calcining the mixture of NaNbO 3 and melamine. The synthesized composite exhibits high photocatalytic performance in the selective oxidation of 5-Hydroxymethylfurfural (HMF) to 5-formyl-2-furancarboxylic acid (FFCA) when using water as solvent. The structure and composition of g-C 3 N 4 /NaNbO 3 photocatalysts were characterized by TG, XRD, SEM, UV–Vis, FT-IR, and XPS methods, and the optical and electrochemical properties were investigated by EIS, PC, and PL techniques. O 2 − was inferred to be the primary active species in this process based on the active species trapping experiment. Heterostructure formation of g-C 3 N 4 /NaNbO 3 composites efficiently promoted the separation of photo-generated electron-hole pairs and accelerated the electron transfer rate, thus reduced the formation of OH, and sequentially improved the selectivity of FFCA. The highest HMF conversion of 35.8% with FFCA selectivity of 87.4% was achieved on C/N-59.6 photocatalyst under the irradiation of visible light. The possible mechanism and reaction route were also proposed.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Lin Gong,Xiaodong Li,Qi Zhang,Bing Huang,Qiang Yang,Guangcheng Yang,Yousong Liu
Transition metal quantum dots (QDs) are ideal electrocatalysts due to their short ion diffusion path, high atom utilization and effective electron transfer properties. However, a lack of facile and large-scale synthesis strategy limits their industrial production and commercial application. In this study, a triaminoguanidine salt-induced one-step deflagration method is first reported for the ultrafast (hundreds of milliseconds) and gram-scale synthesis of Co 3 O 4 QDs-C 3 N 4 /rGO as an efficient oxygen reduction reaction (ORR) catalyst with high durability. The deflagration reaction process is carefully studied and the formation mechanism is proposed to explain the controllable synthesis of Co 3 O 4 QDs. An optimized sample is capable of achieving an excellent ORR performance in terms of an onset potential of 0.97 V (vs. RHE, equivalent to Pt/C) and the limited current density of −5.33 mA·cm −2 at 0.35 V (vs. RHE, ~7% higher than that of Pt/C). It is believed that this simple and effective synthesis strategy will open up an exciting new avenue to the future design and facile synthesis of Co 3 O 4 or other QDs-based functional materials.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zhansheng Wu,Xiufang He,Yongtao Xue,Xia Yang,Yunfeng Li,Qubing Li,Bing Yu
The hydrophobicity of MoS 2 /g-C 3 N 4 based photocatalysts remains a major hurdle to their successful application for the remediation of water-soluble contaminants such as herbicides and heavy metals. Herein, we develop new photocatalysts based on the graft of three different cyclodextrins (α-CD, β-CD and γ-CD) on MoS 2 /g-C 3 N 4 composites (CDs/MoS 2 /g-C 3 N 4 ) for the removal of glyphosate and Cr (VI) from simulated agricultural runoff. CDs/MoS 2 /g-C 3 N 4 show remarkably enhanced photocatalytic activities for glyphosate degradation and Cr (VI) reduction compared to pristine MoS 2 /g-C 3 N 4 . In addition, γ-CD/MoS 2 /g-C 3 N 4 exhibits the highest hydrophilicity and photocatalytic activity among these three different cyclodextrins grafted MoS 2 /g-C 3 N 4 . The mechanistic investigation indicates that cyclodextrins can not only increase the accumulation of glyphosate and Cr (VI) onto the surface of CDs/MoS 2 /g-C 3 N 4 but also facilitate the fleet separation of photo-induced electron-hole pairs. In summary, these results collectively imply that the graft of cyclodextrins could be an effective strategy to improve the photocatalytic efficiency of MoS 2 /g-C 3 N 4 composites for the removal of glyphosate and Cr (VI) from simulated agricultural runoff.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 44
·期 5
·1795-1805
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IF 3.069
Hao Liu,Xiaodong Zhu,Rui Han,Yuxue Dai,Yuanling Sun,Yanna Lin,Dandan Gao,Xueying Wang,Chuannan Luo
Study of the degradation mechanism of the Cu2O/g-C3N4 p–n heterojunction is very challenging and important for the preparation and practical applications of the g-C3N4 photocatalyst in controlling water pollution. Therefore, the Cu2O/g-C3N4 p–n heterojunction was designed and prepared successfully and the mechanism of enhanced visible-light photocatalytic activity was proposed. The morphology and structure of the synthesized materials were characterized by using SEM, TEM, FT-IR and XPS. And the optical and electrical properties of the materials were studied by measuring DRS, the photocurrent density and the Mott–Schottky curve. The results showed that the g-C3N4 photocatalyst is coated on the surface of Cu2O to form a tight heterojunction, which facilitates the separation and migration of photogenerated carriers, and the quantum yield of the Cu2O/g-C3N4 composite photocatalyst was 3–7 times higher than that of the single component. It has been shown that the built-in electric field formed at the heterojunction interface can effectively separate photogenerated electrons and holes. The photocatalytic performance of the material was evaluated by the photocatalytic degradation of tetracycline (TC) under visible light. The maximum degradation rate of Cu2O/g-C3N4 for TC could reach over 90% in 90 min, and the degradation rate of the single component is more than doubled. Simultaneously, the TOC tests monitored the mineralization of TC up to 83.4%, and the active substances in the reaction process were determined to be ˙O2− and h+ through free radical trap experiments and ESR tests. This work shows that the construction of an internal electric field has greatly improved the photocatalytic performance of g-C3N4. The Cu2O/g-C3N4 p–n heterojunction has good degradation ability toward tetracycline and is a good tetracycline-type wastewater treatment material.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Shu-ao He,Wei Li,Xiao Wang,Qiong Ma,Min Li,Wei Xu,Xue-chuan Wang,Chen-hui Zhao
The two-dimensional (2D) g-C 3 N 4 has a wide application prospect in photocatalysis field due to its larger surface reactions, wider absorption of light and faster charge separation. However, the lack of active site of reduction leads to its poor hydrogen evolution reaction (HER) activity. In this work, the intermediate β-FeOOH was synthesized as a high-efficiency precious metal free co-catalyst in hydrogen production. Then, the g-C 3 N 4 -Fe 3 O 4 /β-FeOOH (CNFF-x,y, x = 1, 2 and 3, y denotes the reaction time (h)) photocatalyst based on p-n and Z-scheme heterojunction was constructed via a subsequent solvothermal process. The chemical composition, microtopography, crystallography, photochemical and electrochemical properties of the CNFF-x,y were analyzed by XRD, FI-IR, TEM, XPS and so on. The visible-light-driven (VLD) catalytic performance of CNFF-x,y heterojunction was evaluated by the hydrogen evolution reaction (HER). Results showed that CNFF-2,10 photocatalyst based on p-n (g-C 3 N 4 -Fe 3 O 4 ) and Z-scheme (Fe 3 O 4 /β-FeOOH) heterojunction presented the highest VLD catalytic HER activity (33.25 μmol g −1 h −1 ) at the absence of Pt co-catalyst after illumination for 6 h. It indicated that the effective introduction of Fe 3 O 4 /β-FeOOH nanoparticles (NPs) into g-C 3 N 4 to construct double-heterojunction (g-C 3 N 4 -Fe 3 O 4 /β-FeOOH) could greatly broaden the light response property and inhibit the recombination of photo-induced carriers, exhibiting enhanced HER activity. Meanwhile, this double-heterojunction photocatalyst presented robust photostability and reproducibility even been used several times. The findings of an intermediate β-FeOOH were put forward in this study will provide some new ideas for the research of HER.
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高影响因子
DYES AND PIGMENTS
·
2019
·
IF 4.018
Xiuquan Xu,Songmei Wang,Tongjie Hu,Xiaofeng Yu,Jiapeng Wang,Chao Jia
Co-doping has been proven to significantly enhance the photocatalytic performance of g-C 3 N 4 . Herein, Mn and O co-doped g-C 3 N 4 (Mn/O-CN) composites were constructed for the first time by a simple one-pot calcining route. The systematic characterization results of XRD , FT-IR, TEM-EDS, XPS and DRS revealed that the Mn and O elements were co-doped into the CN framework successfully as Mn 3+ / 4+ and n-π* conjugate forms, respectively. The as-prepared Mn/O-CN-2 achieved the highest visible-light-driven degradation rate constant of 0.0290 and 0.0267 min −1 for degradation of Malachite green (MG) and Amido black 10B (AB 10B), which were about 5.09 and 5.45 folds higher than that of pristine CN, respectively. The improved photocatalytic degradation property of Mn/O-CN were mainly benefited from the extended visible light utilization, the enlarged specific surface area, and the accelerated separation and transfer of photo-induced charge carriers, which were all induced by the synergistic effects of Mn and O co-doped. Finally, the active species capturing experiments proved that the superoxide radicals (·O 2 − ) and holes (h + ) acted as the predominant roles in the photocatalytic degradation process .
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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Biao Zhou,Muhammad Waqas,Bo Yang,Ke Xiao,Shengye Wang,Caizhen Zhu,Juying Li,Junmin Zhang
Synthesis of three-dimensional carbon nitride (g-C 3 N 4 ) structures is a promising but challenging task for effectively photocatalytic water splitting to generate H 2 . In this study, thin-shelled honeycomb-like structured g-C 3 N 4 (g-C 3 N 4 -TSH) was successfully synthesized via facile one-step co-pyrolysis of melamine/NH 4 Cl mixture and the morphology evolution mechanism was revealed systematically. By varying the ratios of melamine/NH 4 Cl precursor and thermal preparation temperatures, thin-shelled and thick-shelled honeycomb-like structured g-C 3 N 4 were obtained. Also, the key intermediate phases were identified by their structure characterizations, which revealed low-temperature phase transition of 1-D tube-like melamium/NH 4 Cl adduct, then transforming to 2-D multiple plate-like melamium/melon NH 4 Cl complex by sintering, and finally evolving to g-C 3 N 4 -TSH at high temperature. The final hierarchical structure has several beneficial features as hollow, mesoporous, ultrathin, and honeycomb-like form, which caused its high surface area, excellent mass transfer rate and good light absorption ability. As a result, the g-C 3 N 4 -TSH with Pt as co-catalyst showed remarkable photoactivity for H 2 evolution, with an apparent quantum efficiency of 9.86% at 420 ± 10 nm, which is superior to many reported modified g-C 3 N 4 . This study revealed the evolution mechanism of g-C 3 N 4 -TSH, which is conducive to design various dimension oriented g-C 3 N 4 structures via solid-state chemistry for photocatalytic H 2 evolution.
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Journal of Environmental Sciences
·
2022
·
IF 6.796
Wenxia Wang,Zhen Li,Kailin Wu,Guodong Dai,Qingping Chen,Lihua Zhou,Junxia Zheng,Liang Ma,Guiying Li,Wanjun Wang,Taicheng An
Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical. Herein, aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity, rapid combination of photo-generated carriers and unstable structure, a novel Ag-bridged dual Z-scheme g-C 3 N 4 /BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method. Results showed that Ag-AgI nanoparticles and three-dimensional (3D) BiOI microspheres were decorated highly uniformly on the 3D porous g-C 3 N 4 nanosheet, resulting in a higher specific surface area and abundant active sites. The optimized 3D porous dual Z-scheme g-C 3 N 4 /BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline (TC) in water with approximately 91.8% degradation efficiency within 165 min, outperforming majority of the reported g-C 3 N 4 -based photocatalysts. Moreover, g-C 3 N 4 /BiOI/Ag-AgI exhibited good stability in terms of activity and structure. In-depth radical scavenging and electron paramagnetic resonance (EPR) analyses confirmed the relative contributions of various scavengers. Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework, fast electron transfer of dual Z-scheme heterojunction, desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas. Therefore, the 3D porous Z-scheme g-C 3 N 4 /BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation. The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
·
IF 3.656
Zhenyu Shen,Zhexin Zhu,Gangqiang Wang,Zhendong Wang,Wenxing Chen,Wangyang Lu
It is of great significance for improving the electron transmission performance of graphite phase carbon nitride (g-C 3 N 4 ) by an economical method. Herein, urea was mixed with tourmaline (TM) and calcined to obtain g-C 3 N 4 /TM composite photocatalyst . Under solar light, g-C 3 N 4 /TM activated peroxymonosulfate (PMS) to degrade carbamazepine (CBZ) entirely within 25 min. g-C 3 N 4 /TM had a superior photocatalytic oxidation performance under solar light than g-C 3 N 4 . Photogenerated electron-hole pairs of g-C 3 N 4 were efficaciously suppressed, originating from the more excellent electronic transfer to TM. Four active species, including SO 4 • - , •OH, 1 O 2 , and O 2 • - , were identified for the degradation of CBZ. Ten intermediates of CBZ and six intermediates of sulfaquinoxaline sodium (SQXNa) were determined by using ultra-performance liquid chromatography coupled with a high definition mass spectrometer (UPLC-HDMS), and a degradation pathway was proposed. As the reaction progressed, all aromatic nuclear intermediates were mineralized. The degradation of other organic pollutants by the g-C 3 N 4 /TM/PMS system validated the universal adaptability in practical applications. This research provided an effective way to improve the g-C 3 N 4 photocatalytic activity in wastewater treatment.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 21
·13221
·
IF 6.208
Haohao Huo,Yuzhen Li,Shaojie Wang,Siyang Tan,Xin Li,Siyuan Yi,Lizhen Gao
Herein, Zn3In2S6photocatalyst with (110) exposed facet was prepared by low temperature solvothermal method. On this basis, a highly efficient binary Zn3In2S6/g-C3N4was obtained by low temperature solvothermal method and applied to the degradation of tetracycline (TC). The samples of the preparation were characterized by X-ray diffraction, scanning electron microscope, transmission electron microscope, UV–vis diffuse reflection spectroscopy, and photoluminescence spectroscopy. Furthermore, the degradation performance of photocatalysts on TC was investigated under different experimental conditions. Finally, the mechanism of Zn3In2S6/g-C3N4composite material degrading TC is discussed. The results show that Zn3In2S6and Zn3In2S6/g-C3N4photocatalysts with excellent performance could be successfully prepared at lower temperature. The Zn3In2S6/g-C3N4heterojunction photocatalyst could significantly improve the photocatalytic activity compared with g-C3N4. After 150 min of illumination, the efficiency of 80%Zn3In2S6/g-C3N4to degrade TC was 1.35 times that of g-C3N4. The improvement of photocatalytic activity was due to the formation of Zn3In2S6/g-C3N4heterojunction, which promoted the transfer of photogenerated electron–holes. The cycle experiment test confirmed that Zn3In2S6/g-C3N4composite material had excellent stability. The free radical capture experiment showed that ·O2−was the primary active material. This study provides a new strategy for the preparation of photocatalysts with excellent performance at low temperature.Keywords:Zn3In2S6/g-C3N4;tetracycline;low temperature;photocatalytic
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高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Lidong Kou,Qingfeng Fan,Yuhong Yang,Xianying Duan,Kai Jiang,Jing Wang
N -doped carbons have attracted extensive attention as catalysts for peroxymonosulfate (PMS) activation towards environmental remediation. However, synthesis of N -rich carbocatalysts is challenging and PMS activation mechanism is still unclear. Herein, novel N -rich porous carbocatalysts ( C -P x CN-T) were synthesized by carbonization of polyaniline nanorods coated g-C 3 N 4 . C –P 50 CN-900 (polyaniline content 50%) calcined at 900 °C had high surface area (358 m 2 /g), product yield (27.1%) and N content (12.27 at%). It showed superior performance in activating PMS to degrade and mineralize various phenolic pollutants in a wide pH range (2–11) and with the co-existence of water constituents. A positive correlation was observed between phenol oxidation rates and contents of C O, C –C/C C and graphitic N, which served as active sites to facilitate adsorption of pollutants and PMS on C –P 50 CN-900 and subsequent electron-transfer from pollutants to PMS. Overall, this study provides new insights into rational design of N -doped carbocatalysts and elucidation of electron transfer pathway in PMS activation.
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