JOURNAL OF MATERIALS SCIENCE
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2020
·Vol. 56
·期 2
·1630-1642
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IF 3.553
Zhou Ling,Sun Menglong,Kou Jiahui,Lu Chunhua,Li Ling,Zhang Fangshu,Xu Zhongzi
Graphitic carbon nitride (g-C 3 N 4 ), as an organic polymer semiconductor, has been the focus of photocatalysts due to its physical and chemical stability, low cost and non-toxicity. However, pristine g-C 3 N 4 also has many drawbacks, such as small specific surface area and easy recombination of photoexcited carriers, which hampered its practical application. In this work, we first propose a design idea of embedding stereo molecular scaffold into g-C 3 N 4 framework with a facile copolymerization method for better exfoliating g-C 3 N 4 to reach a better photocatalytic hydrogen evolution under ordinary pressure. The stereo molecular scaffold looses the interlayer stacking of bulk g-C 3 N 4 , benefitting the exfoliation of g-C 3 N 4 . The hydrogen evolution activity of stereo molecular scaffold doped g-C 3 N 4 (AMCN-3-E) is about 7.54 times higher than that of the pristine MCN, which may due to the activated π → π * and n → π * electron transitions, creating more electron transition paths and accelerating the separation of photoexcited electrons and holes.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Lei Zhao,Dan Yang,Lili Ma,Xueting Feng,Hanming Ding
It is a long-term goal to develop catalysts with high activity and stability in practical applications. Spinel FeCo 2 O 4 has been widely researched in heterogeneous catalysis due to its characteristics of stable structure and environmental friendliness. In this work, the composites of graphitic carbon nitride ( g -C 3 N 4 ) and spinel iron cobaltate (FeCo 2 O 4 ) have been fabricated and used to degrade rhodamine B (RhB) by combining the photocatalytic and Fenton-like reactions. The composite with 3% FeCo 2 O 4 (3%FeCo 2 O 4 /CN) showed the best degradation efficiency, with which about 98% RhB was degraded in 45 min. The catalytic activity of 3%FeCo 2 O 4 /CN was larger than that of FeCo 2 O 4 , g -C 3 N 4 , and their mechanical mixture. The synergetic interaction between photocatalytic and Fenton-like reactions and the effective separation of the photogenerated charges are responsible for the enhanced catalytic activity. The quenching and EPR experiments exhibit that SO 4 − , O 2 − , h + , and ΟΗ, especially SO 4 − , are involved in the removal of RhB. The cycle experiments confirm that the used catalyst can restore its catalytic activity after calcination at 400 °C. The work suggests that the composites show a good ability to degrade organic pollutants in wastewater.
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Journal of Cleaner Production
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2020
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IF 7.246
Qin Huang,Chen Wang,Derek Hao,Wei Wei,Luochun Wang,Bing-Jie Ni
The development of highly efficient and separation-free, low-cost photocatalysts have crucial prospect for sustainable wastewater treatment , because it is able to eliminate the hazards of organic pollutant with facile operation. However, the relatively high cost of previous photocatalysts highly obstructs the application of these materials. Herein, we report a cost-effective and distinct konjac/graphitic carbon nitride (KCN) aerogel , which has superior performance for advanced oxidation water treatment . The abundant porous structure of the ultralight aerogel ensures the rapid adsorption of pollutants, which is much helpful for the further photodegradation process. During the working process, the aerogel is half submerged in pollutant solution and half exposed in air, forming a distinctive gas-solid-liquid triphase system, where oxygen can be rapidly delivered into the solution via the porous channels, boosting the generation of hydroxyl and superoxide radicals. Meanwhile, the aerogel structure can separate the g-C 3 N 4 , obstruct its stacking, as well as improve the light absorption rate. The synthesis, utilization and readily biodegradable treatment of the KCN aerogels are all green and eco-friendly, which is extremely constructive for strategies to develop novel highly efficient photocatalytic materials.
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APPLIED SURFACE SCIENCE
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2020
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IF 6.182
Jinge Du,Zhe Xu,Hui Li,Haijun Yang,Shengjun Xu,Jun Wang,Yanan Jia,Shuanglong Ma,Sihui Zhan
A novel Z-scheme Ag 3 PO 4 /g-C 3 N 4 heterostructures was constructed successfully for Escherichia coli inactivation and organic pollutants degradation under visible light irradiation. The Ag 3 PO 4 (8)/g-C 3 N 4 possessed the highest photocatalytic effect with more than 7 log of live Escherichia coli ( E. coli ) totally inactivated within 75 min and complete BPA degradation within 180 min. By mimicking the components of natural water individually, humic acid (HA) and inorganic anion were found to deeply affected the photocatalytic disinfection activity. Moreover, the Ag 3 PO 4 (8)/g-C 3 N 4 revealed significantly boosted visible-light-driven photocatalytic performance for ciprofloxacin and sulfadiazine degradation. The satisfying degradation effects of bisphenol A in nature waters were also obtained. The improved photocatalytic efficiency of Ag 3 PO 4 /g-C 3 N 4 may be attributed to the formation of Z-scheme heterostructure structure and matching valence band and conduction band, resulting in rapid separation of photo-induced carrier, enhanced electronic transport capacity and prolonged carrier lifetime. The possible mechanism was studied using radical quenching tests and electron spin resonance, suggesting that the hole, electron and hydroxyl radical were the paramount active species during Escherichia coli disinfection. This work pioneers a novel strategy for upgrading the photocatalytic disinfection and degradation capacities of g-C 3 N 4 based catalysts.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2020
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IF 4.872
Xiarong Zheng,Yuanqiong Liu,Xiaobin Liu,Qingbiao Li,Yanmei Zheng
A novel composite electrospun fiber with high photocatalytic efficiency, good stability, strong hydrophobicity, good pollution resistance, and easy separation and recovery was synthesized. The TiO 2 @g-C 3 N 4 (TCN) with special core-shell structure (5–10 nm shell) facilitated the separation of photogenerated electron-holes and had high photocatalytic performance. The poly (vinylidene fluoride) (PVDF) electrospun fiber immobilized with TCN was successfully fabricated (PVDF-TCN) with uniform distribution and size of nanofibers by using electrospinning, which was used for degrading tetracycline under visible-light irradiation (> 400 nm). A special rougher surface of electrospun fiber obtained by washing of sacrificial PVP increased the specific surface area, which became more conducive to the adhesion of the catalyst. The water contact angle and FTIR results demonstrated that the electrospun fiber became extremely hydrophilic after adding TCN catalyst, which could effectively mitigate the fiber pollution. The PVDF-TCN-0.2g electrospun fiber exhibited excellent photocatalytic performance and the degradation efficiency of tetracycline was up to 97% in 300 min under visible-light irradiation. The mechanism of PVDF-TCN electrospun fiber degradation of tetracycline in the photocatalytic process was also proposed. In addition, the PVDF-TCN-0.2g exhibited a stable activity after 4 cycles experiments since the degradation efficiency remained about 90%. Therefore, we believed this study provided a new strategy in catalyst immobilization and wastewater treatment.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Xuecheng Liu,Lin Liu,Zurun Yao,Zhehan Yang,Hui Xu
The nitrogen-rich ZnO/g-C 3 N 4 composites were prepared and exhibited excellent photocatalytic performance for hydrogen evolution and NO photo-oxidation under visible-light illumination. The obtained nitrogen-rich ZnO/g-C 3 N 4 composite has efficient visible-light utilization and effective separation of photogenerated electron-hole pairs. Experimental data verifies that the photocatalytic activity of ZnO/g-C 3 N 4 composite could be improved by N dopant. NZnOCN1 composite exhibits the highest photocatalytic activity for H 2 evolution and NO removal. The results show that the possible mechanism of the photocatalytic H 2 evolution reaction is the type II mechanism, while the Z-scheme mechanism of nitrogen-rich ZnO/g-C 3 N 4 composite is conducive to NO photo-oxidation.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Chun Zhang,Yinan Gu,Guixiang Teng,Liping Wang,Xiaodong Jin,Zengwei Qiang,Weigang Ma
Development of highly efficient photocatalysts is a primary goal in the photocatalysis domain among which reusable composites with a synergistic photocatalytic effect have attracted extensive interest. The ability of catalysts to capture light determines their photocatalytic effect, and porous or hollow photocatalysts are more conducive to the entry and reflection of light. The goal of this research is to develop a type of visible-light-driven, double-shell photocatalyst with high antibacterial activity and excellent cycling stability. Photocatalysts were fabricated using hollow graphitized ZnFe2O4 nanospheres (G-ZnFe2O4) as the carrier. After G-ZnFe2O4 was functionalized with a polydopamine (PDA) template layer, Ag nanoparticles (NPs) and cubic AgCl NPs were in situ generated on the surface of the PDA/G-ZnFe2O4 nanospheres successively. Then, the PDA template was removed using KOH solution, and double-shell Ag/AgCl/G-ZnFe2O4 nanocubes (referred to as DAGZNs) with excellent photocatalytic antibacterial activity were constructed. The DAGZNs showed excellent antibacterial properties against Staphylococcus aureus and Escherichia coli. The efficient synergistic photocatalytic antibacterial activity coupled with magnetic separability and recyclability of DAGZNs make them potential for practical application in water purification and environmental protection. The method of designing and synthesizing double-shell structures to enhance photocatalysis may also be extended to synthesis of other photocatalytic and optical materials.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Haiping Liu,Jing Liang,Shuai Fu,Li Li,Jiehu Cui,Penghui Gao,Fengying Zhao,Jianguo Zhou
Exploiting metal-free cocatalysts is of huge interest for photocatalytic technology in environmental wastewater remediation and water splitting fields. The N doped carbon quantum dots (NCDs) modified defect-rich g-C 3 N 4 (DCN) was prepared through impregnation method. The structural, optical and electronic properties of NCDs/DCN were systematically investigated. The NCDs/DCN with outstanding visible light absorption, narrowed gap and electron transfer ability were conducive to combined pollutions photocatalytic removal and simultaneous H 2 production and rhodamine B (RhB) degradation. The resulting NCDs/DCN performed much higher removal efficiency in different combined pollutions systems containing OFL/Cr (VI), BPA/Cr (VI) and CIP/Cr (VI) than in single system owing to the synergistic effect between organic pollution oxidation and Cr (VI) reduction. The free-radical quenching experiments, spectral technology and electron spin resonance (ESR) confirmed that Cr(VI) can be reduced by the conduction band (CB) electrons, and the h + and O 2 − radicals dominated OFL degradation. The optimized NCDs/DCN displayed excellent simultaneously photocatalytic H 2 production activity and RhB degradation with the H 2 evolution rate of 3.68 μmol‧h −1 ‧g −1 and 100% RhB removal efficiency. The photocatalytic activity of simultaneous combined pollutions removal and synergistic H 2 generation and RHB degradation provides a promising strategy for real wastewater remediation applications and energy utilization.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Zhiwei Zhao,Wei Zhang,Wen Liu,Yunyi Li,Jiangyu Ye,Jialiang Liang,Meiping Tong
In this work, a novel strategy for building single-atom silver-induced amorphous graphitic carbon nitride (g-C 3 N 4 ) with a hollow tubular morphology is developed. By forming a tubular supramolecular gel, silver is successfully isolated by the nitrogen atoms in both melamine and nitrate anions, impeding agglomeration in the subsequent thermal polymerization. The high density of single-atom-dispersed silver (atomic ratio up to 11.6%) selectively breaks the hydrogen bonds in layered g-C 3 N 4 , leading to a fully amorphous structure. Silver-induced full amorphization not only enhances the visible light absorption of g-C 3 N 4 but also accelerates charge transfer, endowing the as-prepared photocatalyst having the optimal silver content with 52 times higher surface area specific naproxen (NPX) removal activity than pure g-C 3 N 4 . Both density functional theory (DFT) calculations and steric effects are applied to explain the degradation pathway of NPX. The toxicity of NPX is reduced by sufficient irradiation. This work provides useful insights into the design and morphology control of single metal ion-dispersed g-C 3 N 4 for environmental applications.
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CHEMOSPHERE
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2020
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IF 5.778
Ren He,Kehui Xue,Jing Wang,Ying Yan,Yi Peng,Tianli Yang,Yunchu Hu,Wenlei Wang
The direct shedding of piperazine rings is critical for the degradation of antibiotic persistent organic pollutants. In this work, nitrogen-deficient g-C 3 N 4 loaded with polyoxometalates porous photocatalysts with P–N heterojunctions were carried out through the formation of chemical bonds between the nitrogen-deficient C + in g-C 3 N x and the bridging oxygen in polyoxometalates (POMs), including phosphomolybdic acid (PMA), phosphotungstic acid (PTA) and silicotungstic acid (STA). The adsorption and photocatalysis experiments confirm the ability of the g-C 3 N x /POMs nanosheets to efficiently remove ciprofloxacin via the synergistic effects of adsorption and photo-catalysis. Approximately, g-C 3 N x /POMs-30 exhibits the optimal degradation ability, and the degradation rates of g-C 3 N x /PMA-30, g-C 3 N x /PTA-30 and g-C 3 N x /STA-30 could respectively reach 93.1%, 97.4% and 95.6% within only 5 min under visible light. The free radical scavenging experiment and ESR free radical capture experiments confirm that ·OH and ·O 2 − are free radicals that effectively degrade CIP. According to the results of the LC-MS analysis, the intermediates produced after CIP degradation and the efficient degradation pathway are proposed. The direct shedding of piperazine rings in the decarboxylation and defluorination process leads to the most efficient degradation of CIP into the small molecules.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Lei Chen,Jin-Tao Ren,Zhong-Yong Yuan
The modification of electronic structure in heterogeneous catalysts has been particularly proven as one of efficient approaches for enhancing the catalytic performances in redox. Herein, phosphorus-doped g-C 3 N 4 nanosheets with atomically dispersed V-based nanocomposites (V/P-CN) were fabricated through a facile organophosphonic acid-modified co-condensation route. The use of organophosphonic acid not only achieves the in-situ P-doping but also tailors the texture of the synthesized V/P-CN, leading to narrow band gap, electron-enriched structure, nanosheet morphology, abundant mesh-like pores and enlarged surface area. Series of physicochemical and electrochemical characterizations indicate the enhanced electron transfer from the P-doped g-C 3 N 4 to V-based nanocomposites. The heterojunction-induced electron–enriched structure of V-based nanocomposites in V/P-CN endows with the impressive intrinsic oxidative desulfurization activities. Radical scavenger experiment further suggests the significant electron interaction in the heterojunction catalysts favors the enriched electron dispersion around V-based active species and employs as rate-determining step for oxidative desulfurization. This work offers a facile but economic and powerful method to modulate the structure of the heterojunction catalysts for green catalysis, especially redox reactions.
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NANO
·
2021
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IF 1.556
Zongli Ren,Zhongwei Zhao,Zhao Yang,Bin Cheng,Xuan Yang
Constructing heterojunction photocatalyst is an effective method to enhance the separation of photogenerated electron and hole, which significantly improves ability of visible light response. In this study, calcination methods have been proposed to prepare highly efficient magnetic ternary photocatalyst g-C 3 N 4 /TiO 2 -MnFe 2 O 4 halloysite. It showed an enhanced photocatalytic degradation for dyes (crystal violet) and nonsteroidal anti-inflammatory drugs (acetaminophen) under vision light irradiation. Compared to pure g-C 3 N 4 , TiO 2 , MnFe 2 O 4 halloysite and binary g-C 3 N 4 -MnFe 2 O 4 halloysite, the optimized ternary g-C 3 N 4 /TiO 2 -MnFe 2 O 4 halloysite displayed enhanced photodegradation efficiency with 91.1% removal of crystal violet (10 ppm) in 90 min under visible light irradiation, the optimized ternary g-C 3 N 4 /TiO 2 -MnFe 2 O 4 halloysite composite showed significantly enhanced photocatalytic activity with more than 79.1% removal of acetaminophen (10 ppm) within 90 min under visible light. The photocatalytic mechanism was identified through the free radical quenching experiment. The heterojunction photocatalyst could be easily recovered by an extra magnetic field and reused several times without any obvious deterioration in catalytic activity. Besides, the ternary heterojunction also exhibited antibacterial ability against Escherichia coli . The superior photocatalytic performance of composite should be mainly attributed to both the improvement of light harvesting as well as the enhanced separation and transfer efficiency. It is expected that this novel ternary visible-light responding composite would be a promising candidate material for organic pollutants degradation and bacteria inactivation.
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