JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Chenjie Ding,Shifei Kang,Wenxin Li,Weikang Gao,Zhihao Zhang,Lulu Zheng,Lifeng Cui
Heterogeneous photo-Fenton catalysts prepared by doping metal ions in g-C 3 N 4 are promising alternatives to traditional homogeneous Fenton catalysts, but are restricted by poor mesoporous structure and agglomerate of metal species. Recently, the highly uniformly dispersed metal-N active sites in various photocatalysts have been proved to be the critical reason for their enhanced catalytic activity. In this study based on reasonable control of mesoporous structure and metal-N active sites, mesoporous Fe-g-C 3 N 4 was synthesized using a simple one-step thermal shrinkage polymerization method using ferrous oxalate as iron source and pore-forming agent. The Fe and N elements in the triazine ring skeleton of Fe-g-C 3 N 4 form a σ-π bond, thus the photogenerated electrons can be quickly transferred to Fe 3+ to form Fe 2+ under the interaction of chemical bonds, accelerating the Fenton reaction rate. Density functional theory calculations results demonstrate that the energy band structure and electron cloud density distribution of Fe-Nx active structure are better than that of routine FeOx crystal structure with metal species agglomeration. In addition, the excellent mesoporous structure of Fe-g-C 3 N 4 creates conditions for the high exposure of Fe-Nx active sites in the photo-Fenton reaction under visible light. The as-developed Fe-g-C 3 N 4 system shows high recyclability and excellent photo-Fenton performance for removal of typical intractable pollutants (The degradation rate of dye and tetracycline reaches 98.2% and 98.7% at 60 and 120 min, respectively). This work provides a facile and sustainable route to develop mesoporous highly-active heterogeneous Fenton-like catalysts and even further general the design of general catalyst with ideal metal-N active sites, thereby promoting a feasible and efficient wastewater remediation solution.
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DOI
PubMed
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Zhenyu Zhao,Xuting Wang,Shifu Wang,Zuoyi Xiao,Shangru Zhai,Jiliang Ma,Xiaoli Dong,Haodong Sun,Qingda An
The development of g-C3N4-based photocatalysts with abundant active sites is of great significance for photocatalytic reactions. Herein, a smart and robust strategy was presented to fabricate three-dimensional (3D) g-C3N4 nanosheet-coated alginate-based hierarchical porous carbon (g-C3N4@HPC), including coating melamine on calcium alginate (CA) hydrogel beads, freeze-drying hydrogel beads as well as pyrolysis at high temperatures. The resulting photocatalyst possessed a significantly high surface area and a large amount of interconnected macropores compared with porous carbon without the melamine coating. The unique structural features could effectively inhibit the curling and agglomeration of g-C3N4 nanosheets, provide abundant photocatalytic active sites, and promote mass diffusion. Therefore, the g-C3N4@HPC composite exhibited remarkable photocatalytic activity and outstanding stability toward the photoreduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) by NaBH4 under natural sunlight and simulated visible-light irradiation (λ > 420 nm) using a 300 W xenon lamp. Moreover, the mechanism toward the photocatalytic reaction was extensively studied by quenching experiments and electron spin resonance (ESR) experiments. The results showed that active hydrogen species were able to be achieved by following a dual-channel pathway in the NaBH4 system, which included photocatalytic reduction of H+ ions and photocatalytic oxidation of BH4– ions. This work not only opens up a new way to design efficient photocatalysts for various reactions but also provides a reference for an in-depth study of the photoreduction mechanism.
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DOI
PubMed
高影响因子
SOLID STATE SCIENCES
·
2019
·
IF 2.155
Hu Jingyu,Yang Ran,Li Zhaohui,Sun Yuanqiang,Qu Lingbo,Alexander Nti Kani
The zinc oxide/graphitic carbon nitride (ZnO/g-C 3 N 4 ) heterostructured nanocomposite was successfully synthesized by a facile two-step process involving thermal condensation of melamine and hydrothermal in situ growth of globular zinc oxide (ZnO) nanoparticles on the surface of graphitic carbon nitride (g-C 3 N 4 ). The morphologies, chemical compositions, and optical properties of the prepared ZnO/g-C 3 N 4 were investigated via a series of characterization techniques. SEM and TEM validate the grafting of ZnO globular with a diameter of 40–50 nm on the surface of g-C 3 N 4 . The visible photodegradation activity of the nanocomposite was assessed via tetracycline and oxytetracycline as target pollutants. Under visible light irradiation, 15 wt% ZnO globular-g-C 3 N 4 exhibits high photocatalytic activity with 78.4% of tetracycline degraded in 50 min and 63.5% of oxytetracycline in 50 min which was much faster photocatalytic degradation efficiency than that of the reported materials. Reactive species scavenging experiments revealed that photogenerated holes are the main reason for the photocatalytic degradation. After six recycles, the ZnO globular-g-C 3 N 4 resulted in 70% degradation efficiency of TC suggesting its high stability and reusability. This work proved a new insight for constructing novel high-performance photocatalysts for TC degradation.
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DOI
高影响因子
JOURNAL OF MATERIALS CHEMISTRY
·
2012
·Vol. 22
·期 44
·23428-23438
·
IF 5.968
Liming Sun,Xian Zhao,Chun-Jiang Jia,Yixuan Zhou,Xiufeng Cheng,Pan Li,Li Liu,Weiliu Fan
We present a systematic investigation of the microscopic mechanism of interface interaction, charge transfer and separation, as well as their influence on the photocatalytic activity of heterojunctions by a combination of theoretical calculations and experimental techniques for the g-C3N4–ZnWO4 composite. HRTEM results and DFT calculations mutually validate each other to indicate the reasonable existence of g-C3N4 (001)–ZnWO4 (010) and g-C3N4 (001)–ZnWO4 (011) interfaces. The g-C3N4–ZnWO4 heterojunctions show higher photocatalytic activity for degradation of MB than pure g-C3N4 and ZnWO4 under visible-light irradiation. Moreover, the heterojunctions significantly enhance the oxidation of phenol in contrast to pure g-C3N4, the phenol oxidation capacity of which is weak, clearly demonstrating a synergistic effect between g-C3N4 and ZnWO4. Interestingly, based on the theoretical calculations, we find that electrons in the upper valence band can be directly excited from g-C3N4 to the conduction band, that is, the W 5d orbital of ZnWO4, under visible-light irradiation, which should yield well-separated electron–hole pairs, with high photocatalytic performance in g-C3N4–ZnWO4 heterojunctions as shown by our experiment. The microcosmic mechanisms of interface interaction and charge transfer in this system can be helpful for fabricating other effective hetero-structured photocatalysts.
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DOI
高影响因子
Science of Advanced Materials
·
2019
·Vol. 11
·期 12
·1764-1772
·
IF 1.158
An Ji-Bin,Hu Dai-Peng,Li Yan-Lin,Chen Na-Li
The Magnetic photocatalytic cobalt ferrite/graphitic-carbon nitride (CoFe2O4/g-C3N4) composites with enhanced photocatalytic activity were successfully fabricated through a simple calcination method. Scanning electron microscopy, powder X-ray
diffraction, and infrared spectroscopy were applied to characterize the samples. The photocatalytic behavior of CoFe2O4/g-C3N4 was assessed by degradation of atrazine in photo Fenton-like system under visible light irradiation. The results showed
that CoFe2O4/g-C3N4 with 2.0 gL–1 catalyst loading in the presence of 1 mM peroxymonosulfate (PMS) exhibited the best catalytic performance, and more than 97% of atrazine was destructed in 12 min. This enhancement could be attributed
to the synergistic effect between CoFe2O4 and g-C3N4 promoting longer lifetime of separated electron–hole pairs derived from the formation of the heterojunction between CoFe2O4 and g-C3N4. This could
enhance the composite-mediated activation of PMS for the visible-light driven degradation of atrazine. Moreover, the quenching tests showed that sulfate radicals were responsible for the atrazine degradation. CoFe2O4/g-C3N4 composites have strong
magnetic ability, thus their recovery from water could be readily achieved by applying external magnetic field. This study demonstrates reasonable performance of the PMS/CoFe2O4/g-C3N4 system in water matrix as potentially important candidate for
environmental remediation.
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DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 9
·998
·
IF 4.501
Mengfan Niu,Liyun Cao,Qianqian Liu,Xiaoyi Li,Qian Chen,Dinghan Liu,Wenbin Li,Jianfeng Huang,Liangliang Feng
Exploring low-cost and highly active, cost-effective cocatalysts is of great significance to improve the hydrogen evolution performance of semiconductor photocatalysts. Herein, a novel ultrasmall V-doped NiP2nanoparticle, as an efficient cocatalyst, is reported to largely upgrade the photocatalytic hydrogen evolution reaction (HER) of g-C3N4nanosheets under visible-light irradiation. Experimental results demonstrate that V-NiP2cocatalyst can enhance the visible-light absorption ability, facilitate the separation of photo-generated electron-hole pairs and boost the transfer ability of electrons of g-C3N4. Moreover, the V-NiP2/g-C3N4hybrid exhibits prominent photocatalytic HER activity 17 times higher than the pristine g-C3N4counterpart, even outperforming the 1 wt.% platinum-loaded g-C3N4. This work displays that noble-metal-free V-NiP2cocatalyst can serve as a promising and efficient alternative to Pt for high-efficiency photocatalytic H2evolution.Keywords:g-C3N4;cocatalyst;V-NiP2;photocatalyst;hydrogen evolution reaction
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Jiangping Jing,Zhuoyuan Chen,Chang Feng,Mengmeng Sun,Jian Hou
Photoelectrochemical cathodic protection is emerging as a green and environmental method to protect metals against corrosion. Graphitic carbon nitride (g-C 3 N 4 ) shows great application potential in this area because of its high efficiency, high stability and low cost. However, the pristine g-C 3 N 4 shows amphoteric properties, resulting in its failure in providing photoelectrochemical cathodic protection for the coupled metal in NaCl solution. In this work, a K&I co-doping technique was performed to modulate the band structure of g-C 3 N 4 , and an n-type g-C 3 N 4 (n-C 3 N 4 ) was obtained. The changes in the molecular structure were studied by SEM, HRTEM , XRD , EDS, XPS and FT-IR technologies. The n-type semiconductor characteristics were verified by the photoinduced i-V curves, SKP potential distributions and pH drift techniques. The n-C 3 N 4 can generate positive photocurrent in the whole investigated potential range, making it able to provide photoelectrochemical cathodic protection for the coupled 316L stainless steel in NaCl solution. This work is very helpful for promoting the application of g-C 3 N 4 in the fields of the photoelectric conversion and the photoelectrochemical cathodic protection.
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Jianhua Ge,Yujie Liu,Daochuan Jiang,Lei Zhang,Pingwu Du
Photocatalytic H 2 production via water splitting in a noble-metal-free photocatalytic system has attracted much attention in recent years. In this study, noble-metal-free Ni 3 N was used as an active cocatalyst to enhance the activity of g-C 3 N 4 for photocatalytic H 2 production under visible-light irradiation ( λ > 420 nm). The characterization results indicated that Ni 3 N nanoparticles were successfully loaded onto the g-C 3 N 4 , which accelerated the separation and transfer of photogenerated electrons and resulted in enhanced photocatalytic H 2 evolution under visible-light irradiation. The hydrogen evolution rate reached ∼305.4 μmol h −1 g −1 , which is about three times higher than that of pristine g-C 3 N 4 , and the apparent quantum yield (AQY) was ∼0.45% at λ = 420. Furthermore, the Ni 3 N/g-C 3 N 4 photocatalyst showed no obvious decrease in the hydrogen production rate, even after five cycles under visible-light irradiation. Finally, a possible photocatalytic hydrogen evolution mechanism for the Ni 3 N/g-C 3 N 4 system is proposed.
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DOI
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2022
·Vol. 22
·期 7
·2009-2021
·
IF 3.536
Liu Quanfeng,Yu Jiang,Jiang Yinying,Zhong Chengwei,Ding Senxu,Zhou Peng,Jin Yuanxiao
Purpose Soil organic matter pollution is a serious threat to the human living environment. The purpose of this paper is to investigate the effect of MIL-101(Fe)/g-C 3 N 4 catalyzed peroxynitrite degradation of 2-chlorophenol in soil and to analyze the reaction mechanism and further to explore the optimal parameters of this reaction system with utilizing the mathematical model. Methods MIL-101(Fe)/g-C 3 N 4 was successfully obtained by hydrothermal synthesis method by growing MIL-101(Fe) on the surface of g-C 3 N 4 to catalyze the degradation of 2-CP (2-chlorophenol) in soil by sodium persulfate. The influence factors on the removal rate of 2-CP were analyzed by the response surface methodology (RSM) and combined with theoretical calculations. RSM can be used to model continuous variable surfaces with less data and determine the optimal level range. Results MIL-101(Fe)/g-C 3 N 4 had a good catalytic performance due to its good catalytic properties and the adsorption of g-C 3 N 4 on 2-CP in the system and made the best removal rate of 2-CP increase to 91.2%. The correlation of model fitting results was significant, and the verification of its optimal parameters yielded results with an error of only 4.1%. Conclusion Further studies revealed that SO 4 •− and • OH were the reactive radicals, and SO 4 •− was the dominant, which impelled Fe 2+ and Fe 3+ to interconvert in the complex system. Possible degradation pathways were derived by analyzing the intermediates. Generally, this experiment provides some ideas for future research of MOFs in soil organic pollutant removal systems. Graphical abstract
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Boru Gao,Mengmeng Dou,Jin Wang,Shuming Li,Dongying Wang,Lin Ci,Yao Fu
Contaminants such as antibiotics and the resulting antibiotic-resistant bacteria (ARB) and antibiotic-resistant genes (ARGs) have become a hot topic in the field of wastewater purification. In this study, a method was proposed to simultaneously remove antibiotics and reduce ARB and ARGs with C–(N) 3 defect carbon nitride-coupled persulfates (CN-C V2 /PS). The location of the C–(N) 3 defects was determined by a combination of spectroscopic techniques and electron spin resonance tests. Based on photoluminescence and electrochemical tests, and deformation charge density calculations, electron traps were generated at defect sites resulting in enhanced electron–hole separation. The mineralization rates of CN-C V2 /PS for six typical antibiotics were 11–17% and 21–28% higher than those of CN-C V2 and conventional CN , respectively. Over the same reaction time, the inactivation rates of CN-C V2 /PS for E. coli and E. faecalis screened from wastewater treatment plants were 3.6 and 2.7 log higher than that of CN-C V2 . In addition, CN-C V2 /PS showed a reduction rate of more than 2.5 log for tet A and intI 1. DFT calculation showed that due to the formation of defects, the adsorption energy between the PS and catalysts increased from –8.924 eV (CN) to –18.340 eV (CN-C V2 ). At the same time, the effective stretch of peroxide bond of PS changed from 1.505 Å to 1.519 Å. Both results indicated that the activation of PS was significantly enhanced in the presence of the modified CN-C V2 . The synergetic effect of CN-C V2 /PS is expected to remove the antibiotics, resistant bacteria and genes efficiently in future wastewater advanced treatment.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jianfei Li,Bin Zhang,Junyan Lu,Zihao Guo,Mingxia Zhang,Degang Li,Zengdian Zhao,Shasha Song,Yan Liu,Luchang Qin
The path and mechanism of charge transfers in composite catalyst are important for degrading organic pollutants effectively. A quasi-ternary Z-scheme heterojunction photocatalyst with carbon quantum dots (CQD), CdS, and graphitic carbon nitride (g-C 3 N 4 ) (CQD/CdS/g-C 3 N 4 ) has been successfully constructed in this work, and its electron transfer path is elucidated by contrast CdS/CQD/g-C 3 N 4 photocatalyst. The built-in electric field at the interface between CdS and g-C 3 N 4 induces exciton separations. The energy barrier between CQD and CdS accelerated charge transfers and further prevents exciton annihilation. As a result, CQD/CdS/g-C 3 N 4 exhibits the greatest photocatalytic degradation, and the removal rates of Rhodamine B and sulfadiazine are 94.7 % and 76.0 %, which are 2.46 times and 1.47 times of CdS/CQD/g-C 3 N 4 , 7.02 times and 7.92 times of g-C 3 N 4 , respectively. It is further proved that CQD as the active site can promote the generation of H 2 O 2 and effectively inhibit the formation of •O 2 – in the photocatalytic reaction. In addition, the degradation pathway and products of sulfadiazine are explored by means of HPLC-MS and calculation of Gaussian software. This work demonstrates the relationship between photocatalytic activity and electron transfer path, meanwhile, provides a reference for the design of efficient heterogeneous photocatalysts for environmental remediation.
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高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Jin Chen,Ke Li,Jie Yan,Suqing Qin,Yuzhao Ma,Xiaofeng Yang,Yanjun Li
Designing heterojunction photocatalysts with staggered band structures and optimal interfacial interactions constitutes a feasible strategy to achieve superior photocatalytic performance. Herein, we synthesized a Pt@BiOBr/g-C 3 N 4 S-scheme heterojunction via in-situ construction and photochemical deposition. Notably, Platinum nanoparticles (NPs), precisely deposited via photochemical reduction, extend light absorption into the visible-NIR spectrum through localized surface plasmon resonance (SPR) while acting as electron mediators to suppress recombination. Under simulated solar irradiation, the optimized Pt@BiOBr/g-C 3 N 4 S-scheme heterojunction demonstrates complete degradation of tetracycline hydrochloride (TC-HCl) within 10 min. Additionally, the photocatalyst showed exceptional degradation efficiency for organic dyes including methyl orange (MO) and rhodamine B (RhB). More importantly, the synergistic interplay between internal electric field (IEF) and the SPR of Pt nanoparticles collectively facilitates rapid charge separation while suppressing electron-hole recombination. This study offers a path toward highly effective photocatalysts engineered for practical applications and elucidates the activity enhancement mechanism through Pt incorporation in ternary heterojunction systems.
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