RSC Advances
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2020
·Vol. 10
·期 33
·19669-19685
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IF 3.119
Shuting Zhang,Guoqiang Li,Liyuan Duan,Hongyu Wang,Yongle Zhao,Yongfa Zhang
Graphitic carbon nitride (g-C3N4) was prepared by a simple thermal polymerization method in this work. The effects of precursor type, thermal polymerization temperature, constant temperature time and atmosphere on the crystal structure, morphology, elemental composition, valence distribution, light absorption properties and photocatalytic activity of the prepared photocatalytic materials were investigated. Taking rhodamine B (RhB) as the target degradant, the blue light catalytic activity of the photocatalytic material was studied in detail. The experimental results showed that the final pyrolysis temperature and constant temperature time are positively related to the adsorption characteristics and photocatalytic ability of the prepared materials. In addition, the adsorption capacity and photocatalytic activity of the products obtained in Ar and H2 atmospheres are better than those produced in CO and CH4, which can be attributed to the combined effect of large specific surface area and structural defects of the materials. The sample's large specific surface area, wide band gap, and excellent photogenerated carrier separation and transfer capabilities make the adsorption performance and photocatalytic performance of the products obtained with ammonium thiocyanate and thiourea as precursors better than those prepared from melamine and dicyandiamide. g-C3N4 prepared by using ammonium thiocyanate as precursor at 550 °C for 5 h under a hydrogen atmosphere showed the best catalytic activity for the degradation of RhB under blue light. It was demonstrated that g-C3N4 prepared exhibited good stability and reusability after four repeat experiments. The active components that play major roles in the degradation of RhB described herein were holes and superoxide radicals, which was inferred by free radical trapping experiments. This work provides a theoretical basis for the idea of converting the mixed salts of desulfurization waste liquid containing ammonium thiocyanate into an excellent photocatalyst g-C3N4 with visible light response.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Ping Sun,Hui Liu,Mingbao Feng,Zhicai Zhai,Yingsen Fang,Xuesheng Zhang,Virender K. Sharma
In this study, two metal-free materials, i.e., N-doped graphene (rGO-N) and g-C 3 N 4 , were strategically combined to prepare a novel g-C 3 N 4 /rGO-N composite for activating peroxymonosulfate (PMS). The g-C 3 N 4 /rGO-N composite showed large specific surface area and high graphite-rich N content, and hence, exhibited excellent catalytic performance because of the synergistic effect of g-C 3 N 4 and rGO-N. The oxidative system could effectively degrade various pollutants (e.g., acid orange 7, orange G, ciprofloxacin, and bisphenol A). The radical quenching experiments and electron paramagnetic resonance spectra analysis revealed that the novel carbonaceous composite could realize PMS-based non-radical oxidative degradation of pollutants unlike the previously reported catalysts, observed the degradation via a radical-dominated pathway. The real-time water treatment experiments demonstrated the potential of the oxidative system to environmental remediation applications. The combination strategy provides an innovative approach to fabricate binary metal-free carbonaceous catalysts for carrying out PMS-based non-radical oxidative degradation of pollutants.
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Nanomaterials
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2020
·Vol. 10
·期 4
·600
·
IF 4.324
Wan Zhao,Xiuru Yang,Chunxi Liu,Xiaoxiao Qian,Yanru Wen,Qian Yang,Tao Sun,Wenya Chang,Xin Liu,Zhi Chen
The increasing discharge of dyes and antibiotic pollutants in water has brought serious environmental problems. However, it is difficult to remove such pollutants effectively by traditional sewage treatment technologies. Semiconductor photocatalysis is a new environment-friendly technique and is widely used in aqueous pollution control. TiO2is one of the most investigated photocatalysts; however, it still faces the main drawbacks of a poor visible-light response and a low charge-separation efficiency. Moreover, powder photocatalyst is difficult to be recovered, which is another obstacle limiting the practical application. In this article, g-C3N4/TiO2heterojunction is simply immobilized on a glass substrate to form an all-solid-state Z-scheme heterojunction. The obtained thin-film photocatalyst was characterized and applied in the visible-light photodegradation of colored rhodamine B and tetracycline hydrochloride. The photocatalytic performance is related to the deposited layers, and the sample with five layers shows the best photocatalytic efficiency. The thin-film photocatalyst is easy to be recovered with stability. The active component responsible for the photodegradation is identified and a Z-scheme mechanism is proposed.Keywords:thin-film photocatalyst;environmental control;antibiotic residue removal;g-C3N4/TiO2;all-solid-state Z-scheme heterojunction
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CHINESE JOURNAL OF CATALYSIS
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2020
·
IF 6.146
Sufeng An,Guanghui Zhang,Jiaqiang Liu,Keyan Li,Gang Wan,Yan Liang,Donghui Ji,Jeffrey T. Miller,Chunshan Song,Wei Liu,Zhongmin Liu,Xinwen Guo
Heterogeneous catalysts with ultra-small clusters and atomically dispersed (USCAD) active sites have gained increasing attention in recent years. However, developing USCAD catalysts with high-density metal sites anchored in porous nanomaterials is still challenging. Here, through the template-free S-assisted pyrolysis of low-cost Fe-salts with melamine (MA), porous alveolate Fe/g-C 3 N 4 catalysts with high-density (Fe loading up to 17.7 wt%) and increased USCAD Fe sites were synthesized. The presence of a certain amount of S species in the Fe-salts/MA system plays an important role in the formation of USCAD S-Fe-salt/CN catalysts; the S species act as a “sacrificial carrier” to increase the dispersion of Fe species through Fe-S coordination and generate porous alveolate structure by escaping in the form of SO 2 during pyrolysis . The S-Fe-salt/CN catalysts exhibit greatly promoted activity and reusability for degrading various organic pollutants in advanced oxidation processes compared to the corresponding Fe-salt/CN catalysts, due to the promoted accessibility of USCAD Fe sites by the porous alveolate structure. This S-assisted method exhibits good feasibility in a large variety of S species (thiourea, S powder, and NH 4 SCN) and Fe salts, providing a new avenue for the low-cost and large-scale synthesis of high-density USCAD metal/g-C 3 N 4 catalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
·
IF 7.1
Xueming Dang,Zhilian Song,Huimin Zhao
A novel photoelectrochemical (PEC) sensing strategy with an amplified signal was proposed based on polypyrrole/g-C 3 N 4 /WO 3 inverse opal photonic crystals triple heterojunction. The sandwich-type detection model was applied to increase the sensitivity and favor the assembly of heterojunction structure. The heterojunction among PPy, g-C 3 N 4 and WO 3 highly improved the separation of photo-generated charges. Meanwhile, WO 3 IOPCs with good optical performance were employed to enhance the light absorption of PEC detection electrode. With the simultaneous combination of these amplification techniques, the designed PEC sensor achieved high sensitivity with low limit of detection (LOD) as 0.004 nM (≈ 1.99 ng L −1 ) and admirable selectivity in the detection of oxytetracycline under visible light irradiation.
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JOURNAL OF MOLECULAR LIQUIDS
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2021
·
IF 6.165
Shaoxiu Li,Chan Lai,Changhui Li,Jintang Zhong,Zhifeng He,Qiuyi Peng,Xi Liu,Bohan Ke
A new magnetic dual Z-scheme heterostructure photocatalyst, consisting of mesoporous graphitic carbon nitride (mpg-C 3 N 4 ), BiOBr, polythiophene (PTh), and magnetic iron oxide, was developed, and its structural, optical, and electrochemical properties were analyzed. The photocatalyst was employed for the degradation of dimethyl phthalate (DMP) in water under visible light to evaluate its photocatalytic activity. The results revealed that the photocatalytic activity of the new heterostructure photocatalyst was superior to that of its single-component counterparts. The reaction kinetics of photocatalytic DMP degradation followed pseudo first-order kinetics and the reaction rate constant was 3.7- and 4.5-fold higher than those of pristine g-C 3 N 4 and BiOBr, respectively. The enhanced photocatalytic performance was chiefly attributed to the dual Z-scheme heterostructure generated between mpg-C 3 N 4 , PTh, and BiOBr, which effectively hindered the recombination of photogenerated electron and hole pairs in mpg-C 3 N 4 and BiOBr, improving the photogenerated carrier transfer efficiency. Radical trapping test results indicated that the active species, h + , ·O 2 – , and ·OH, coexisted during the photocatalytic reaction process, and that h + played a major role in the destruction of DMP molecules. DMP was degraded into intermediate small-molecule products, such as acids and alcohols, which were ultimately mineralized to CO 2 and H 2 O. The magnetic property of the new heterostructure photocatalyst enabled its straightforward separation from water using magnetic separation technology for further reuse. This study provides a new material and method for the effective removal of DMP from aqueous solution.
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Surfaces and Interfaces
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2021
·
IF 4.837
Chunli Wang,Yunxiang Dai,Xiaoheng Fu,Hongbo Lu,Jing Zhang
In this work, a novel 2-dimentional (2D)-2D bentonite/g-C 3 N 4 composite (B/g-C 3 N 4 ), with a layer-layer cross structure and large surface area, was synthesized by a self-assembly process, with the aim for the photocatalytic oxidation of arsenic (As(III)) in wastewater. The structure and properties of the mineral-based composite were characterized by X-ray diffraction (XRD), infrared spectroscopy (IR), scanning electron microscopy (SEM), and photocurrent measurements. The photocatalytic activity of 2D-2D B/g-C3N4 for As(III) removal was further investigated under visible light . The results reveal that the As(III) oxidation rate by 2D-2D B/g-C3N4 composite was three times higher than that by pure g-C3N4, owing to the enlarged specific surface area and the suppressed electron–hole recombination by the incorporated bentonite. Moreover, the composite exhibited a high photocatalytic oxidation efficiency in a wide pH adaptability from 3 to 8.5. Through electron spin resonance (ESR) technique and radical quenching experiments, the photocatalytic mechanism of As(III) oxidation was proposed, where superoxide radicals played a critical role in the photo-oxidation of As(III) in both acid and basic conditions. This work paved a new way to design the mineral-based photocatalyst for treatment of pollutants in a wide pH range.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Tongtong Zhang,Yuqi Wang,Xin Xie,Yanning Shao,Yuhao Zeng,Siyu Zhang,Qishe Yan,Zhongjun Li
A dual Z-scheme carbon-bridged g-C 3 N 4 /BiOI-Bi 2 O 3 photocatalyst were synthesized by simple solvothermal and calcination methods. The physical and chemical properties of prepared samples were explored via a series of characterization and Density Functional Theory (DFT) calculations. The formation mechanism of the composite photocatalyst was systematically studied and the formation process was simulated. Under the irradiation of visible light, 10% carbon-bridged g-C 3 N 4 /BiOI-Bi 2 O 3 exhibited the best photocatalytic performance. And the kinetics reaction model was followed pseudo-first-order kinetics. Moreover, the possible TC degradation pathways were established based on LC-MS. The enhanced photocatalytic activity was mainly attributed to the dual Z-scheme heterojunction formed by carbon-bridged g-C 3 N 4 deposition on the surface of Bi 2 O 3 and BiOI and a higher charge transfer rate of carbon-bridged g-C 3 N 4 , which effectively promoted the separation and transfer of electron-hole pairs. The trapping experiments were carried out to further explore its photocatalytic mechanism. This work provided an in-depth understanding of g-C 3 N 4 and bismuth-based catalysts.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Yangqing He,Zhengrui Huang,Zhanying Ma,Binghua Yao,Haiyang Liu,Linlin Hu,Qing Zhao,Qian Yang,Dongjie Liu,Deguo Du
In this study, zinc (II) 1, 8(11),15(18),22(25) - tetrakis (4-carboxylphenoxy) phthalocyanine (α-ZnTcPc) was synthesized as sensitizer to construct a novel photocatalyst α-ZnTcPc/g-C 3 N 4 by a polycondensation strategy. The FT-IR and XPS spectra demonstrated that the α-ZnTcPc molecules were covalently coupled on g-C 3 N 4 . The 10%α-ZnTcPc/g-C 3 N 4 composites exhibit excellent extended spectral response with intense broad near-infrared absorption at 695 nm and with significantly fascinated charge carrier separation. As expected, the 10%α-ZnTcPc/g-C 3 N 4 displayed a remarkable improved photocatalytic performance in decomposition of methylene blue (MB) and antibiotic tetracycline with degradation rates of 94.49% and 91.43% under visible light irradiation, respectively. The hydroxyl radicals (·OH) were observed as the main reactive oxidizing species in tetracycline decomposition. Moreover, the possible mechanism for enhanced visible light photocatalytic capability might be ascribed to the synergetic effect between α-ZnTcPc and g-C 3 N 4 , which creates large surface areas, decreases the recombination rate of photogenerated charge carries, as well as improves the visible light harvesting significantly. This work not only presents a practical method to conquer the drawback of pure g-C 3 N 4 , but also provides useful insights to construct other g-C 3 N 4 -based composites to take full advantage of solar light towards practical applications for eliminating recalcitrant organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Ruiyang Zhang,Tao Ran,Yuehan Cao,Liqun Ye,Fan Dong,Qian Zhang,Lizhi Yuan,Ying Zhou
Photocatalytic NO x removal is regarded as a promising technique for air purification in recent years. However, NO x removal process usually accompanies with toxic NO 2 generation, leading to serious secondary pollutant and limiting its practical application. Herein, a noble-metal-free g-C 3 N 4 /α-Ni(OH) 2 photocatalyst was fabricated through hydrothermal method. The introduction of α-Ni(OH) 2 microspheres combines with g-C 3 N 4 , resulting in an enlarged surface area from 35 to 95 m 2 /g, while the unique structure of α-Ni(OH) 2 broadens visible-light response range and accelerates photogenerated charge carriers transfer. More importantly, the H atoms of α-Ni(OH) 2 improve the adsorption and activation of O 2 and oxygen atoms to promote NO and NO 2 oxidized to nitrate. Consequently, g-C 3 N 4 /α-Ni(OH) 2 shows enhanced NO removal ratio of 51.3% without any toxic NO 2 generation, indicating its great potential for air purification. Our results provide fresh insight into the design of highly efficient and safe photocatalyst for toxic byproduct control in the application of environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Wen Cao,Yuhang Yuan,Cao Yang,Shichuan Wu,Jianhua Cheng
For the first time, visible-light-driven g-C 3 N 4 /MIL-68(In)-NH 2 heterojunction composites with high photocatalytic activity were prepared for the degradation of ibuprofen (IBP) using an in-situ solvothermal synthesis method assisted with ultrasonication. The composites achieved intensive visible-light absorption, enhanced separation efficiency of photogenerated carriers, and high adsorption capacity, thus achieving excellent photocatalytic degradation for IBP. Among all the composites, 10 wt% g-C 3 N 4 /MIL-68(In)-NH 2 exhibited the maximum photocatalytic rate (0.01739 min −1 ), 19.28 and 2.00 times higher than those of g-C 3 N 4 and MIL-68(In)-NH 2 , respectively. Moreover, the pH, ibuprofen concentration, and catalyst dosages played important roles both in photodegradation and adsorption. In addition, the photocatalytic mechanism was also elucidated, demonstrating that h + was the main reactive species, followed by OH and O 2 − radicals, responsible for the degradation of IBP. Finally, seven aromatic intermediates of IBP were identified, and five possible degradation pathways were proposed, mainly involving hydroxylation, aldehyde oxidation, decarboxylation, and dehydrogenization reactions.
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Journal of the Taiwan Institute of Chemical Engineers
·
2019
·
IF 3.834
Kané Rabé,Lifen Liu,Noor Ahmed Nahyoon,Yizhen Zhang,Ahmed Mahmoud Idris,Jiaqi Sun,Lixin Yuan
We have prepared and studied a novel low cost catalyst of g-C 3 N 4 /Fe 0 (1%)/TiO 2, using a simple process involving the formation of zero valence iron by chemical reduction . This ternary catalyst g-C 3 N 4 /Fe 0 (1%)/TiO 2 was characterized using XRD (X-Ray diffraction), UV–vis spectrum, EDS (Energy Dispersive spectrum) and TEM (transmission electron microscopy), it demonstrated high-visible-light activity in a wide range of pH condition, it can photo-catalytically degraded Rhodamine B (RhB), Tetracycline (TC), and Berberine hydrogen chloride (BH) (∼98% in 90 min) under visible light. The high activity arises from the increased harvest of more visible light and the improved separation of photo-excited electrons and holes via Z-scheme and heterojunctions mechanism. Also, the time required to remove 100% RhB, TC, and 96% BH can be shortened from 90 min to 60 min by introducing 3.18 mM Na 2 SO 3 to this photocatalysis system that assisted the generation of reactive oxidizing species and pollutant degradation. The results showed promising application prospect for this developed catalyst and the tested photocatalysis pollutant degradation system.
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