JOURNAL OF PHYSICS D-APPLIED PHYSICS
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2022
·Vol. 55
·期 44
·444008
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IF 3.409
Jian Cao,Xiaoli Jin,Zhaoyu Ma,Huiqing Wang,Yixue Xu,Yuwei Guo,Haiquan Xie,Junying Zhang
Graphitic carbon nitride (g-C3N4) is gaining more and more attentions as a promising metal-free photocatalyst for H2 production. Nevertheless, from the perspective of practical applications, the photocatalytic performance over g-C3N4 in visible-light region needs a further improvement. In this work, C doping and C quantum dots (QDs) are co-integrated in g-C3N4 by a one-step thermal polymerization method to obtain an advanced C QDs/C doped g-C3N4 photocatalyst. The synergistic effects of C doping and C QDs modification promote the photocatalytic activity of g-C3N4 significantly. The optimal C QDs/C doped g-C3N4 exhibits a significant improvement on visible-light-driven photocatalytic hydrogen production (205 μmol g−1 h−1) with an apparent quantum yield (AQE) at 420 nm reaching 1.24%, which is approximately nine-fold enhancement than that of pristine g-C3N4. The increased photocatalytic activity mainly benefits from the enhanced visible light absorption and carrier separation efficiency. This study may open a new perspective for the design and fabrication of C-modified g-C3N4 for photocatalytic hydrogen production.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Xing Zhang,Suhang Chen,Haidong Luo,Zhenhua Tang,Enzhou Liu,Zhao Qin,Kangzhen Xu
The rapid redox cycle of metal active sites and effective surface reactions are crucial factors to activate peroxymonosulfate (PMS) for environmental remediation. Herein, a novel F-g-C 3 N 4 /Mn x Co 3−x O 4 composite as high-efficient PMS activator was successfully constructed by a one-step hydrothermal method for the degradation of 1,1-diamino-2,2-dinitroethylene (FOX-7). It was discovered that F doping could narrow the band gap, and enhance the light absorption range and the separation of photogenerated electron-hole pairs. Among all samples, the catalytic activity of F-CN/MCO was higher than that of MCO and CN/MCO. This can be attributed to the unique materials morphology and the synergistic effect of photocatalytic and chemical catalytic driven PMS activation. Quenching experiments and electron paramagnetic resonance (EPR) proved that both radical and non-radical pathways are responsible for the degradation of FOX-7, and singlet oxygen ( 1 O 2 ) was identified as the predominant active species. Importantly, the synergy between Co 2+ /Co 3+ and Mn 2+ /Mn 3+ couples enhanced more electron transfer and better redox potential, thus greatly promoting the photocatalytic activation of PMS. This work provides a novel approach for designing efficient catalyst to promote the redox behavior of metal species in sulfate radical-based advanced oxidation processes.
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OPTICAL MATERIALS
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2022
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IF 3.754
Jinfen Niu,Kai Wang,Lan Yang,Jiahui Shi,Yue Zhang,Fan Yang,Xiaojiao Yu,Binghua Yao
Photocatalysis can be a potential technique for decomposing antibiotics contaminants from water. In this study, g-C 3 N 4 modified Bi/BiOBr nanosphere were prepared by a simple microwave solvothermal method, and the structure-properties relationships of the Z-scheme heterojunction were evaluated in degrading organic dyes. Various characterization techniques were then applied to elucidate the structure-performance relationships of the resulting heterojunction photocatalysts in degrading CIP. Compared with pristine g-C 3 N 4 or Bi/BiOBr, the g-C 3 N 4 @Bi/BiOBr nanocomposites showed heightened property in photocatalytic degradation of CIP. The photocatalytic efficiency of CIP decomposition over the Z-scheme of g-C 3 N 4 @Bi/BiOBr heterojunction was about 2.38 and 1.35 times homologous to those of original g-C 3 N 4 and Bi/BiOBr. The enhancement in photocatalytic activity of g-C 3 N 4 @Bi/BiOBr could be described by the Z-scheme pathway and the SPR effect of Bi 0 , which broadened visible light absorption and promoted the separation of photoinduced carriers. In addition, the effect of typical water matrix factors, such as pH, anionic, and cationic on photodegradation rate were evaluated. Furthermore, results of scavenging experiments showed that ·OH, ·O 2 − , and h + all participate in the degradation of CIP. Based on the band structure and scavenging measurements, a possible photocatalytic mechanism for the as-synthesized g-C 3 N 4 @Bi/BiOBr composites was proposed.
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CHEMOSPHERE
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2022
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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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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jun Luo,Chengcheng Ding,Yonghai Gan,Yang Guo,Yibin Cui,Cheng Sun
A dual-MOFs (Fe and Co)/g-C 3 N 4 heterojunction composite was successful constructed and used to activate peroxymonosulfate (PMS) for degrading sertraline (SER). The composite showed outstanding catalytic activity with 100% of SER removal efficiency in 60 min and the degradation rate 0.057 min −1 . At the same time, the amount of catalyst, concentration of PMS and environmental pH on the degradation for SER were investigated in detail. The main degradation products and pathways of SER were analyzed by Gaussian theory calculation and high-performance liquid chromatography-mass spectrometry (HPLC-MS). Based on the free radical quenching experiments and electron paramagnetic resonance (EPR) characterization analysis, it was confirmed that •OH and SO 4 •- were produced in the catalytic reaction process, and explained catalytic mechanism elaborately. This work demonstrates the connection of MOF-Fe nanoparticles , micropores and heterojunction with the catalytic activity, providing an efficient catalytic system that can promote electron transfer and circulation of high activity center.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2022
·Vol. 23
·期 21
·13221
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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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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yashi Qing,Yanxiang Li,Zhiwei Guo,Yujie Yang,Wangliang Li
17β-estradiol (E2) is one of the endocrine disrupting chemicals (EDCs) ubiquitously with significant impacts on ecosystem and organisms even at extremely low concentrations. Photocatalytic membranes, with the combination of photocatalysis and membrane filtration, have great potential to enhance E2 removal. In this work, a photocatalytic membrane was fabricated from the polyamide (PA) microfiltration membrane and visible light responsive Bi 2 WO 6 /protonated g-C 3 N 4 (BPG) photocatalyst. The BPG photocatalyst was embedded into calcium alginate hydrogel followed by immobilizing onto PA membrane through vacuum filtration and crosslinking. The transparent calcium alginate hydrogel guaranteed 100% light transmittance which contributed to visible light induced photodegradation . Under static and dynamic conditions, the removal efficiency of E2 reached 99.5% and remained 95.1%, which was mainly owing to the synergistic effects of the adsorption of PA and photodegradation of the BPG nanocomposites . The synergistic interaction was fitted by modified Elovich model, and a strong positive correlation (r = 0.834, r s = 0.965) was confirmed by Pearson’s and Spearman’s correlation coefficient , indicating that adsorption could enhance photocatalysis by concentrating contaminants around the photocatalyst and photocatalysis could promote the adsorption by regenerating adsorption sites. The photocatalytic membrane can be reused, and the removal efficiency of E2 was 96.6% after 5 cycles. This work provided not only a facile fabrication of photocatalytic membrane, but also a deep understanding of the synergistic adsorption-photocatalysis for effective removal of E2.
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Journal of Environmental Sciences
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2022
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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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PROGRESS IN ORGANIC COATINGS
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2022
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IF 6.206
Changhua Li,Chen Zhang,Yi He,Hongjie Li,Yang Zhao,Zhijun Li,Dan Sun,Xiangying Yin
Multi-dimensional composite nanocontainers provided an opportunity to prolong the service life of waterborne self-healing coatings through combining intelligent protection with physical barrier. Herein, we constructed a benzotriazole (BTA) corrosion inhibitor loaded nanocontainer with barrier/controlled release/corrosion inhibition properties by assembling graphitic (g)-C 3 N 4 lamella, hollow polyaniline capsule and outer polydopamine wall. Hollow polyaniline and g-C 3 N 4 lamella with adsorption properties provide effective space and sites for loading BTA corrosion inhibitor. Outer polydopamine wall can not only realize the controlled release of corrosion inhibitor, but also ensure the good compatibility between the composite container and the water-based epoxy resin . In addition, polydopamine (PDA) and polyaniline (PANI) as a container frame can also serve as active inhibitors after the release of corrosion inhibitor to enhance the self-healing protection effect of waterborne coatings. In comparative evaluation, the composite coatings containing BTA-loaded nanocontainers (0.5 wt.%) exhibit obviously physical barrier effect after soaking in 3.5 wt.% NaCl solution for 40 days, and maintains good protective performance after immersion for 80 days. Meanwhile, the artificial scratch experiment verified the effective self-repair protection of the composite container to the coating under the condition of damage. To be sure, it will provide an effective improvement idea for the long-term application of waterborne epoxy coating in marine environment.
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JOURNAL OF RARE EARTHS
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2022
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IF 4.632
Deyang Ning,Junqi Li,Yuanpei Lan,Hong Yong Sohn,Jian Yang,Chaoyi Chen,Zhiyao Chu,Xisong Mao
In this work, we firstly synthesized a CeO 2 /C 3 N 4 photocatalyst with Z-scheme heterojunction by a facile LiCl–KCl molten salt method. The synthesized catalyst has an excellent quality for removing organic pollution of dyes and antibiotics in wastewater. As an example, the CeCN–1:5 prepared with a mass ratio of Ce 2 (CO 3 ) 3 · x H 2 O:C 3 H 3 N 6 = 1:5 exhibits a methylene blue (MB) removal capacity of 100% within 90 min and tetracycline (TC) removal capacity of 94.6%. After 4 cycles, the CeCN–1:5 keeps a removal efficiency of nearly 100% in 150 min for MB and 85.7% for TC. The kinetics study reveals that the MB removal process with the CeCN–1:5 fits the modified Elovich model with strong adsorption while TC removal fits the first-order model. The large surface area (238 m 2 /g) and negative zeta potential (−39.3 mV) of CeCN–1:5 contribute to superior adsorption capacity to MB. However, the adsorption of TC is restricted due to the positive surface/pore potential in acidic solution. CeCN–1:5 has combined Z-scheme heterojunction and exhibits a low recombination rate of electrons (e – )/holes (h + ) and the photo-generated active radicals of · OH/ · O 2 – that promotes the photocatalytic performance. This novel CeO 2 /C 3 N 4 photocatalyst with an excellent photocatalysis removal activity has an enormous potential for photocatalytic applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Tianjun Ni,Hui Zhang,Zhibin Yang,Liping Zhou,Likun Pan,Chunling Li,Zhijun Yang,Dong Liu
In this work, Co 3 O 4 /g-C 3 N 4 catalyst with highly efficient adsorption and degradation of antibiotics was developed based on the combination of three-dimensional (3D) porous morphological controls of g-C 3 N 4 and the loading of Co 3 O 4 quantum dots (Co 3 O 4 QDs). It was discovered that the catalyst can effectively activate peroxymonosulfate (PMS) through a non-photochemical path, and a high tetracycline elimination rate of 99.7% can be achieved within 18 min. The characterization and density functional theory calculation results demonstrated that the porous 3D structure can not only promote the substrate adsorption reaction but also provide large surface area and countless exposed active sites for catalytic reaction . The introduction of Co 3 O 4 QDs lowered activation energy barrier and lead to high energy of PMS adsorption. More efficient charge migration between the catalyst and PMS further accelerated PMS activation. Thus, leading to the excellent catalytic performance. In addition, non-free radical mediated degradation mechanism of catalytic activity was also proposed. This work provides a scheme for designing novel and efficient PMS activators for the removal of abusive antibiotics from aqueous environments.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Sixing Dai,Lei Xiao,Qinliu Li,Gazi Hao,Yubing Hu,Wei Jiang
Graphitic carbon nitride (g-C 3 N 4 ) is a promising candidate for photocatalytic degradation of emerging environmental contaminants, pharmaceuticals and personal care products (PPCPs). To improve the photodegradation performance of pure g-C 3 N 4 , the construction of different heterostructures , surface modification and morphology engineering could be considered. However, the surface of g-C 3 N 4 is usually difficult to modify due to fewer functional groups on its surface. In this work, surface hydroxylated g-C 3 N 4 nanofibers were prepared by NaOH treatment (NTCN), and then went through an in-situ growth method to obtain 0D/1D Co 3 O 4 -NTCN nanocomposites . Hydrolysis can effectively modify the surface of g-C 3 N 4 to make it rich in hydroxyl and reduce the number of amino groups, which is conducive to photocatalytic activity. Surface hydroxylation of NTCN was confirmed by FTIR and XPS. Structurally, Co 3 O 4 -NTCN has a unique 0D / 1D structure, which has not been reported much on photocatalysts based on carbon nitride , providing a large surface area and short diffusion distances and resulting in more exposure to the light and the effective transfer of interfacial photogenerated charge from the interior to the surface. The photodegradation ratio of TC, DCF and MT can reach 97.3% TC, 88.9% and 63.2% within 60 min respectively. DFT calculation is used to illustrate the band structure and separation and migration of photoinduced charges of Co 3 O 4 -NTCN composites. Radicals trapping test demonstrate O 2 ⋅− and ⋅OH are the major radicals, and a possible Z-scheme mechanism is proposed.
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