APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Dashi Lei,Juanqin Xue,Xiangyu Peng,Shuhao Li,Qiang Bi,Changbin Tang,Liang Zhang
In this work, direct Z-Scheme photocatalyst (ZnFe 2 O 4 /g-C 3 N 4 ) was employed to purify Cr(VI) and As(III) in wastewater. Results showed that Cr(VI) and As(III) was completely removed in a wide pH range of 3–7 under visible light irradiation. During photo reaction, oxalate enhanced the generation of Fe(II) and CO 2 − , which were beneficial for formation of OH and O 2 − . In photocatalytic system, Fe(II), photogenerated electron, as well as CO 2 − contributed to Cr(VI) reduction, OH and O 2 − were responsible for treatment of As(III). Moreover, ZnFe 2 O 4 /g-C 3 N 4 was easily recycled by magnetic separation, and presented an excellent reuse ability in treatment of Cr(VI) and As(III).
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Peng Du,Jun Tang,Weiping Li,Laihui Luo
To overcome the existence challenge of the luminescent materials in versatile applications, NaLuF 4 : x Eu 3+ nanopariticles and NaLuF 4 :0.15Eu 3+ @ y g-C 3 N 4 composites were designed. Under irradiation of 394 nm, dazzling red emissions with high color purity of 87.6% are observed in the NaLuF 4 : x Eu 3+ nanoparticles and the optimizing content of the dopants is 15 mol%. The electric dipole-dipole interaction leads to the concentration dependent quenching effect. Through assessing the resistance performance of the resultant nanoparticles to the temperature, the studied samples are certified to show high thermal stability. Furthermore, the proper color rendering index (80.2), low correlated color temperature (5014 K) and suitable luminous efficiency (12.1 lm/W) of packaged white light-emitting diode reveal that the NaLuF 4 :0.15Eu 3+ nanoparticles can be employed as the red component for white light-emitting diode. On account of the inconsistent photoluminescence performances of the NaLuF 4 :0.15Eu 3+ nanoparticles and g-C 3 N 4 , the thermometric properties of the NaLuF 4 :0.15Eu 3+ @ y g-C 3 N 4 composites are explored. The maximum absolute and relative sensitivities of the designed composites are 0.0057 K −1 and 0.455% K −1 , respectively, and their values are able to be manipulated via composition regulation. This work proposes a new sight into the exploitation of diverse photoluminescence behaviors of the g-C 3 N 4 and NaLuF 4 : x Eu 3+ nanoparticles to realize versatile applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Fanying Meng,Yingying Qin,Jian Lu,Xinyu Lin,Minjia Meng,Gang Sun,Yongsheng Yan
In the practical process of photocatalytic H 2 evolution, optimizing the ability of light absorption and charge spatial separation is the top priority for improving the photocatalytic performance. In this study, we elaborately engineer neoteric g-C 3 N 4 nanotube@polydopamine(pDA)/NiCo-LDH (LPC) composite photocatalyst by combining hydrothermal and calcination method. In the LPC composite system, the one-dimensional (1D) g-C 3 N 4 nanotubes with larger specific surface area can afford more active sites and conduce to shorten the charge migration distance, as well as the high-speed mass transfer in the nanotube can accelerate the reaction course. The g-C 3 N 4 /NiCo-LDH type-II heterojunction can efficaciously stimulate the spatial separation of photo-produced charge. In addition, pDA as heterojunction metal-free interface mediums can provide multiple action (π-π* electron delocalization effect, adhesive action and photosensitization). The optimized LPC nanocomposite displays about 3.3-fold high photoactivity for H 2 evolution compared with the g-C 3 N 4 nanotube under solar light irradiation. In addition, the cycle experiment result shows that the LPC composite photocatalyst possesses superior stability and recyclability. The resultant g-C 3 N 4 @pDA/NiCo-LDH composite photocatalyst displays the potential practical application in the field of energy conversion.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
·
IF 6.551
Guanlong Wang,Ya Zhao,Huanran Ma,Chenjing Zhang,Xiaoli Dong,Xiufang Zhang
Constructing highly efficient metal-free material towards peroxymonosulfate (PMS) activation under photocatalytic assistance is a promising strategy for water decontamination . Herein, N vacancy modified g-C 3 N 4 nanotube (VCN) was prepared to build a novel photo-assisted PMS activation system (PPAS), in which the unique electronic structure created by N vacancy could favor the PMS activation on VCN under visible-light irradiation. The role of N vacancy in PPAS was firstly studied through tuning its content in VCN. The results showed that the N vacancy greatly improved PMS activation on VCN PPAS towards organic pollutants removal . The VCN PPAS with moderate N vacancy modification performed best, whose kinetic constant for Rhodamine B degradation was 9.6 and 2.6 times higher than that of VCN/PMS system and pristine g-C 3 N 4 PPAS, respectively. Moreover, the VCN PPAS performed well in wide pH range (3−12) and real water background. Selective removal of different organic pollutants was found on VCN PPAS, owing to the different interaction between pollutant and the catalyst surface with surface-bound radicals. The O 2 − and OH were major oxidants for pollutant removal in VCN PPAS, which were produced on dual active sites of VCN via two pathways: The N vacancy enhanced PMS adsorption and trapped photogenerated electrons for PMS reduction into OH, while the electron-deficient C atoms created by N loss promoted the PMS oxidation into O 2 − .
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RSC Advances
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2020
·Vol. 10
·期 54
·32652-32661
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IF 3.119
Yu Gao,Kun Qian,Baotong Xu,Fu Ding,Valerian Dragutan,Ileana Dragutan,Yaguang Sun,Zhenhe Xu
The generation of hydrogen-based energy and environmental remediation using sunlight is an emerging topic of great significance for meeting the ever-growing global need. However, the actual photocatalytic performance is still far below expectations because of the relatively slack charge-carrier separation and migration as well as insufficient spectral absorption in semiconductors. Therefore, the rational construction of heterojunctions is considered as an effective approach to solving the above issues. In this context, we have, for the first time, designed and synthesized a two-dimensional 2D-on-2D heterostructure, based on 2D Ag-doped ZnIn2S4 nanoplates deposited on 2D g-C3N4 nanosheets (denoted as g-C3N4/Ag:ZnIn2S4). This construct benefits from improved visible-light absorption by unveiling a greater number of catalytically active sites, effectively enhancing charge-carrier separation and relocation. Detailed analysis has proved that under visible-light irradiation, the optimized g-C3N4/20 wt% Ag:ZnIn2S4 nanocomposite has substantially upgraded photocatalytic activity in hydrogen formation by water splitting (hydrogen evolution rate of up to 597.47 μmol h−1 g−1) and in residual dyestuff degradation (methyl orange, MO; degradation rate constant of 0.1406 min−1). Noteworthily, these two exceptionally high values respectively represent 30.73 and 5.42 times enhancements vs. results obtained with bare g-C3N4. Another strong point of our g-C3N4/Ag:ZnIn2S4 is its impressive recyclability for 20 runs, with no relevant metal release in the aqueous solution following photocatalysis. This work introduces new, superior access to highly efficient photocatalysts founded on 2D/2D nanocomposites serving both the production of hydrogen as an energy carrier and environmental remediation.
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ANALYTICA CHIMICA ACTA
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2020
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IF 5.977
Jun-Tao Cao,Yu-Xiang Dong,Yan Ma,Bing Wang,Shu-Hui Ma,Yan-Ming Liu
Photoactive materials with high photo-electron transfer efficiency and stable signal output hold a key role in constructing the photoelectrochemical (PEC) biosensing systems. In this study, the ternary [email protected] 3 N 4 heterojunction was first prepared and characterized, and its application in PEC bioanalysis was explored. The gold nanoparticles sandwiched between CdS and g-C 3 N 4 , acting as both plasmonic photosensitizer and electron relay, significantly boosted the light absorption and accelerated the charge transfer from g-C 3 N 4 to CdS, both of which contributed to the enhancement of photoelectric conversion efficiency. Signal quenching with graphene oxide-CuS efficiently weakened the photocurrent from [email protected] 3 N 4 . The combination of the excellent PEC properties of [email protected] 3 N 4 and the remarkable quenching effects of graphene oxide-CuS enabled construction of a sandwich-type PEC immunosensor for prostate specific antigen (PSA) detection. This immunosensor achieved sensitive PSA analysis by multiple signal amplification mechanisms, with a detection limit of 0.6 pg mL −1 and a wide linear range from 1.0 pg mL −1 to 10 ng mL −1 . This work not only demonstrates the great potential of noble metal sandwiched ternary heterojunctions in the PEC field, but also lays a foundation for developing the general PEC immunoassays .
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Y.Q. He,Fangling Zhang,Bei Ma,Na Xu,Lucas Binnah Junior,Binghua Yao,Qian Yang,Dongjie Liu,Zhanying Ma
In this study, a highly efficient ternary 6.7%Au/Ni 2 P/g-C 3 N 4 nanocomposite is rationally fabricated through a two-step hydrothermal followed by green photoreduction strategy. The XPS analysis, SEM and HRTEM images reveal that Ni 2 P and good nanoparticles (AuNPs) are successfully loaded onto the surface of g-C 3 N 4 and heterojunction formed among them. The optimized 6.7%Au/0.5%Ni 2 P/g-C 3 N 4 demonstrates the highest photocatalytic efficiency towards decomposition of levofloxacin hydrochloride with 88.23% removal rate and hydrogen generation rate of 78.65 μmol·g −1 ·h −1 , in comparison with the binary 0.5%Ni 2 P/g-C 3 N 4 (76.86%, 47.06 μmol·g −1 ·h −1 ) and pristine g-C 3 N 4 (61.26%, 45.61 μmol·g −1 ·h −1 ). Notably, this is the first time using Ni 2 P and AuNPs co-modified g-C 3 N 4 -based nanocomposites to evaluate the photocatalytic degradation performance of levofloxacin hydrochloride. The study of the corresponding enhanced mechanism indicates that the dramatically improved photocatalytic performance is originated from the synergistic effects: including (1) the strong optical absorption property of Ni 2 P and the SPR effect of AuNPs endows the remarkably improved visible-light harvesting for increasing charge carrier production; (2) the co-catalysts of Ni 2 P and AuNPs play key roles as interfacial electron sinkers and facilitate photogenerated electron-hole pairs separation and migration; (3) the co-integration improves the specific surface area of final product which can provide more active sites for the improvement of photocatalytic performance. Moreover, a plausible degradation pathway for levofloxacin hydrochloride is proposed based on the UPLC-MS analysis. Our work highlights a good example for designing and constructing other highly-efficient g-C 3 N 4 -based multicomponent photocatalysts for both solar energy conversion and environmental remediation.
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MATERIALS RESEARCH BULLETIN
·
2020
·
IF 4.019
Xinyue Gu,Jie Mei,Jiahao Lai,Siying Lv,Jing Yang,Shihai Cui,Sen Chen
In view of the deterioration of the environment and the shortage of resources, it is necessary to develop efficient photocatalysts for the degradation of organic pollutants. Herein, a novel and environmentally friendly ZnNb 2 O 6 /g-C 3 N 4 heterojunction nanocomposite was synthesized by calcination-hydrothermal method successfully. The chemical and physical capabilities of the material were characterized by various kinds of analytical instruments. Compared with ZnNb 2 O 6 and g-C 3 N 4 , ZnNb 2 O 6 /g-C 3 N 4 showed the strongest photocatalytic activity. The nanomaterial was used in the removal of the pollutant 2,4-DCP. The effects of degradation conditions were discussed including component ratio, material dosage, initial analyte concentration, pH and salinity. After 180 min’ simulated sunlight illumination, the removal efficiency of 2,4-DCP (10 mg/L) reached 95.7% under the optimum condition. Furthermore, the possible photocatalytic mechanisms were discussed according to four aspects: (i) The conformation of the active species; (ii) The calculation of valence and conduction band; (iii) The analysis Z-scheme heterojunction mechanism; (iv) The speculation of feasible photocatalytic paths. In conclusion, the ZnNb 2 O 6 /g-C 3 N 4 (ZC-7) nanocomposite has the least recombination rate of electron-hole pairs and the highest photocatalytic efficiency.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Xin Wang,Wangyang Lu,Zhiguo Zhao,Huitian Zhong,Zhexin Zhu,Wenxing Chen
Peroxymonosulfate (PMS) activation with the generation of strongly oxidizing hydroxyl radicals (•OH) and sulfate radicals (SO 4 • − ) has attracted widespread attention for the elimination of organic contaminants. However, the design of an eco-friendly catalytic system with high mineralization rate and high stability remains a challenge. Here, an iron-based photocatalyst (β-FeOOH@g-C 3 N 4 ) for the activation of PMS was prepared by a cyclic microwave-assisted reaction, whereby Fe 3+ was introduced at the nitrogen sites of g-C 3 N 4 , resulting in in situ growth and a uniform distribution of nano-β-FeOOH thereon. β-FeOOH@g-C 3 N 4 maintained high catalytic activity after acid treatment or repeated tests, demonstrating excellent stability and reusability. Moreover, compared with the catalytic systems with β-FeOOH or g-C 3 N 4 alone, the catalytic activity of β-FeOOH@g-C 3 N 4 was increased 5–10 times for the catalytic oxidation of carbamazepine (CBZ) and other emerging contaminants under solar irradiation. Importantly, the CBZ mineralization rate with the β-FeOOH@g-C 3 N 4 /PMS system under solar irradiation was as high as 92%. From the results of electron paramagnetic resonance spectroscopy and radical trapping experiments, large amounts of O 2 • − , 1 O 2 , and Fe V = O are present at the beginning of the reaction, which contribute to the rapid oxidative removal of CBZ, while SO 4 • − and •OH contribute to the deep oxidation, leading to a significantly enhanced total organic carbon (TOC) removal efficiency. This work provides an alternative method for the design of a highly efficient and stable catalyst for PMS activation to eliminate emerging contaminants.
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Catalysts
·
2019
·Vol. 10
·期 1
·6
·
IF 3.444
Jia Huang,Gang Nie,Yaobin Ding
To develop highly efficient heterogeneous photocatalysts for the activation of dissolved oxygen is very interesting in the field of green degradation of organic pollutants. In the paper, oxygen atom doped g-C3N4(O-g-C3N4) was prepared via a facile chemical oxidation of g-C3N4by peroxymonosulfate. X-ray photoelectron spectroscopy analysis suggests the oxidative treatment of g-C3N4by peroxymonosulfate evidently increased atomic percentage of oxygen on O-g-C3N4surface to 6.9% as compared with 1.8% for g-C3N4. Meanwhile, the doped oxygen atom mainly existed as carbonyl and carboxyl groups. Optical characterization indicates the introduction of oxygen improved the response of O-g-C3N4to visible light, and more obviously, separation of photo-generated h+-e−. 4-chloro-7-nitrobenzo-2-oxa-1,3-diazole (NBD-Cl) probe measurement indicates the formation of O2•−was dramatically enhanced through activation of dioxygen by photo-generated electrons in the O-g-C3N4photocatalytic system. Through high performance liquid chromatography (HPLC) and Liquid chromatography–mass spectrometry (LC-MS) analysis, it was found rhodamine B (RhB) photocatalytic degradation by O-g-C3N4followed step by step N-deethylation reaction pathways induced by the formed O2•−, rather than the non-selective decomposition of the chromophore in RhB by other radicals, such as hydroxyl radicals. This study provides a facile method to develop oxygen atom doped g-C3N4photocatalyst, and also clarifies its photocatalytic activation mechanism of molecular oxygen for N-deethylation reaction of RhB.Keywords:photocatalysis;oxygen doped g-C3N4;activation of dioxygen;superoxide radicals;selective N-deethylation of rhodamine B
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JOURNAL OF HAZARDOUS MATERIALS
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2019
·
IF 7.65
Jiaxing Huang,Daguang Li,Ruobai Li,Ping Chen,Qianxin Zhang,Haijin Liu,Wenying Lv,Guoguang Liu,Yiping Feng
Anatase TiO 2 nanoparticles coated with P and O co-doped g-C 3 N 4 were prepared via a single-step procedure. The resulting POCN/anatase TiO 2 demonstrated remarkable performance in the degradation of enrofloxacin (ENFX). The photocatalytic activity of this heterojunction was 28.9 and 3.71 times better than that of the CN and anatase TiO 2 , respectively. The microtopography of the POCN/anatase TiO 2 was revealed in this study. Co-doping with P and O increased the visible light adsorption capacity of the g-C 3 N 4 , whereas the anatase TiO 2 nanoparticles enhanced the adsorption properties of the ENFX and the separation of the photoinduced carriers of the POCN/anatase TiO 2 . The O 2 ·− and h + were the main reactive oxidative species in the photocatalytic degradation of ENFX. The results of the detection of H 2 O 2 and ESR confirmed that POCN/anatase TiO 2 was a type Z-scheme photocatalyst. Finally, the ENFX degradation pathways were estimated through the detection of by-products.
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MATERIALS RESEARCH BULLETIN
·
2019
·
IF 3.355
Xiaofeng Hu,Jisong Hu,Qingqi Peng,Xinguo Ma,Shijie Dong,Huihu Wang
In this work, a special hybrid structure with 2D configuration comprising of g-C 3 N 4 , reduced graphene oxide (RGO), and BiOI (g-C 3 N 4 /BiOI/RGO) was rationally constructed and immobilized on Ni foam with RGO functioned as electron transfer mediator and binder. The immobilized 2D g-C 3 N 4 /BiOI/RGO hybrid structure exhibited the enhanced photocatalytic CO 2 reduction to CO and the methyl orange (MO) degradation efficiency under visible light irradiation. Particularly, the hybrid heterojunction with a mass ratio 6% of BiOI to g-C 3 N 4 displayed the highest CO yield and degradation rate constant for MO, which was 1.6 times and 3 times of g-C 3 N 4 /RGO binary heterojunction immobilized on Ni foam. The enhanced photocatalytic activity was ascribed to the rapid charge separation. More importantly, combined with the theoretical calculations on the work functions of g-C 3 N 4 , rGO and BiOI, the experimental results clarified the charges transfer route of g-C 3 N 4 /BiOI/RGO heterojunction conforming to the Z-scheme mechanism.
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