JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Shuaiyang Zhang,Mengjie Gao,Yunpu Zhai,Jiaqi Wen,Jingkun Yu,Tiwei He,Zhenhui Kang,Siyu Lu
Recently, g-C 3 N 4 (CN) loaded N-doped carbon dots (NCDs) have been widely studied as promising metal-free photocatalysts due to their impressive performance in hydrogen production. However, deep understanding of the effect of nitrogen chemical states on photocatalytic activity is still lacked. In this work, NCDs doped with pyrrole nitrogen, graphite/pyrrole nitrogen, and pyrrole/pyridine nitrogen were prepared and hybridized with g-C 3 N 4 . The characterizations revealed that, incorporation of pyrrole N-doped CDs into g-C 3 N 4 (CN/NCDs-en) effectively enhanced the visible light absorption, facilitated electron-hole separation, and promoted the participation of photoexcited electrons in H 2 evolution reaction. Moreover, theoretical calculation showed that, compared with graphite N and pyridine N, pyrrole N has the most appropriate H adsorption ability, which is conducive to the H 2 formation. Under visible light irradiation, the CN/NCDs-en exhibited the best hydrogen evolution of 3028 μmol h −1 g −1 . These results shed a light on the design and optimization of N-doped metal-free photocatalysts for H 2 evolution reaction.
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Nanomaterials
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2022
·Vol. 12
·期 9
·1416
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IF 5.719
Yining Jia,Rong Huang,Ruijuan Qi
Numerous efforts have been devoted to realizing the high loading and full utilization of single-atom catalysts (SACs). As one of the representative methods, atom migration-trapping (AMT) is a top-down strategy that converts a certain volume of metal nanoparticles (NPs) or metal-based precursors into mobile metal species at high temperature, which can then be trapped by suitable supports. In this study, high-loading iron single atoms anchored onto carbon matrix/g-C3N4hybrid supports were obtained through a single-atom migration-trapping method based on metal–organic framework (MOF) pyrolysis. It is confirmed, by high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS), that the Fe(acac)3precursor is reduced to Fe single atoms (SAs), which are not only anchored onto the original N-doped carbon (NC), but also onto g-C3N4, with an Fe-N coordination bond. Further electrochemical results reveal that Fe-C3N4-0.075 possesses a better half-wave potential of 0.846 V and onset potential of 0.96 V compared to Fe-N-C, the product obtained after pyrolysis of Fe(acac)3@ZIF-8. As opposed to SAs prepared by the pyrolysis process only, SAs prepared by AMT are commonly anchored onto the surface of the supports, which is a simple and effective way to make full use of the source metal and prepare SACs with higher exposing active sites.Keywords:atom migration-trapping;single-atom catalysts;metal–organic frameworks
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Journal of Environmental Sciences
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2022
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IF 6.796
Chenxiao Qi,Haixiang Chen,Xiufang Chen,Chengyu Chu,Xueting Mei,Wangyang Lu,Nan Li
Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis . However, the traditional problems such as high recombination rate of photogenerated carriers limit its application. In this work, we introduce nitrogen deficiency into g-C 3 N 4 to solve this problem a simple and safe in-situ reduction method. g-C 3 N 4 /CaCO 3 was obtained by a simple and safe one-step calcination method with industrial-grade micron particles CaCO 3 . Cyano group modification was in-situ reduced during the thermal polymerization process, which would change the internal electronic structure of g-C 3 N 4 . The successful combination of g-C 3 N 4 and CaCO 3 and the introduction of cyanide have been proved by Fourier transform infrared spectroscopy and X-ray photoelectron spectrometer. The formation of the cyano group, an electron-absorbing group, promotes the effective separation of photogenic electron hole pairs and inhibits the recombination of photogenic carriers. These advantages result in the generation of more •O 2 − and 1 O 2 in the catalytic system, which increases the photocatalytic efficiency of nicotine degradation by ten times. Furthermore, the degradation process of nicotine has been studied in this work to provide a basis for the degradation of nicotine organic pollutants in the air.
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FOOD CHEMISTRY
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2022
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IF 9.231
Dezhuang Gong,Xiquan Li,Xiuling Zhang,Wentao Zhang,Tianhao Chen,Xinhua Zhang
In this research, novel citrus-pectin-based [email protected] /graphite carbon nitride nanocomposites (CACNs) were formed by assembling citrus-pectin-based [email protected] ( [email protected] ) prepared by daylight-driven reduction onto a graphite carbon nitride (g-C 3 N 4 ) surface. The as-prepared samples were characterized by various techniques to study their morphology, structure, optical and electrochemical properties. The CACNs were found to have enhanced photoelectrochemical properties, which provided excellent photocatalytic activity to degrade the food colorant new coccine (NC) under visible light. For the NC degradation, the recommended photocatalyst offered approximately 95.7% of the degradation efficiency under visible-light irradiation for 60 min, which has superior photostability and reusability. Its degradation rate constant was approximately 5.16 and 37.6 times those of pure g-C 3 N 4 and [email protected] , respectively. The NC degradation conformed to pseudo-first-order kinetics. Thus, the developed nanocomposites provide a useful reference for the removal of hazardous food colorants and resource utilization of peel waste.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2022
·
IF 3.428
Rui Zhang,Jiacheng Jiang,Kunlin Zeng
Photocatalysts usually exist in powder form, which limits their practical application in photocatalytic degradation of antibiotics in wastewater. To solve this problem. Here, we report the construction of Z-scheme Bi 2 WO 6 /g-C 3 N 4 on activated carbon fiber membrane (ACF) as a thin-film photocatalyst. The catalyst was characterized by XRD , SEM, XPS and other means. Chlortetracycline was used as a model pollutant to study the photocatalytic activity of the sample. According to the results of XPS and XRD, the composite material was successfully prepared. Ultraviolet diffuse reflectance characterization showed that the edge and intensity of the absorption band of the composite material were enhanced. The photodegradation experiment of chlortetracycline shows that 10% Bi 2 WO 6 /g-C 3 N 4 /ACF (area: 4 × 4 cm 2 ) has the best photocatalytic activity. Cycling experiments have proved that the 10% Bi 2 WO 6 /g-C 3 N 4 /ACF composite material has a stable degradation ability during the photodegradation process. Therefore, Bi 2 WO 6 /g-C 3 N 4 /ACF can be used as a recyclable, large surface area photocatalyst to eliminate water Antibiotics in the environment.
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FOOD CHEMISTRY
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2022
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IF 9.231
Jiaodi Li,Chenxi Wang,Xiaoling Chen,Minghui Huang,Qian Fu,Rongjie Li,Yilin Wang,Chunyan Li,Pengcheng Zhao,Yixi Xie,Junjie Fei
Gallic acid (GA) is found in a wide range of natural plants and is relevant to the health of human beings. Here, a photoelectrochemical sensing platform based on g-C 3 N 4 @CNT heterojunction has been prepared for the highly sensitive and selective detection of GA. Under the light of xenon lamp, the photocurrent of g-C 3 N 4 @CNT is 7 times higher than that of g-C 3 N 4 . And the sensor generates 4 times more photocurrent in the presence of GA than without GA. This sensor has a wide linear range from 10 nM to 10 μM with a limit of detection as low as 2 nM. Also, the abundant amino groups of g-C 3 N 4 provide excellent selectivity for the sensor. Furthermore, the sensor can be used for the analysis of GA in black tea samples, which provides a novel and rapid method for the detection of GA in food samples.
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Materials Today Chemistry
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2022
·
IF 7.613
Hui Liu,Wangchen Huo,Tian C. Zhang,Like Ouyang,Shaojun Yuan
Antibiotics, once being released into the environment, become recalcitrant organic pollutants, which pose a potential risk to ecological balance and human health. In this study, a Z-scheme heterojunction of bismuth oxyiodide (BiOI)/exfoliated g-C 3 N 4 (BiOI/ECN hereafter) was synthesized by the combination of thermal exfoliation of g-C 3 N 4 and chemical precipitation of BiOI for efficient photocatalytic degradation of tetracycline in aqueous solutions under visible light irradiation. The optimized BiOI/ECN delivered an outstanding degradation rate at circa 0.0705 min −1 , which was 10 times higher than that of the bulk g-C 3 N 4 . The photocatalytic degradation efficiency of tetracycline remained almost unchanged in a pH range of 3–11, and the BiOI/ECN displayed an excellent photostability upon recycled usage. The photocatalytic mechanism of tetracycline was ascribed to the main reactive oxidation species of photogenerated holes and superoxide radicals. In addition, the possible degradation pathways of tetracycline were investigated by HPLC-MS to identify intermediates. The toxicity of photocatalytic-generated intermediates of tetracycline was found significantly alleviated according to the calculation of quantitative structure–activity relationship prediction. This work not only provides an attractive photocatalyst for the removal of tetracycline but also opens a new avenue for rational design of Z-scheme heterojunction composites for tetracycline degradation.
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CERAMICS INTERNATIONAL
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2022
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IF 5.532
Zhiyao Chu,Junqi Li,Yuan-Pei Lan,Chaoyi Chen,Jian Yang,Deyang Ning,Xuewen Xia,Xisong Mao
A ternary photocatalyst of LaOCl/CeO 2 -g-C 3 N 4 was designed and firstly synthesized by a facile KCl–LiCl molten salt method. The 60 %LaOCl/40 %CeO 2 -g-C 3 N 4 with a 6: 4 weight ratio of LaOCl to CeO 2 has an optimal degradation ratio (nearly 100%) for methylene blue (MB) with an impressive cyclic stability. Both of adsorption and photodegradation contribute to the high MB removal ratio, and kinetic study results show that the rate constant of photocatalytic degradation route is 0.0174 min −1 , which is less than that of adsorption process (2.4406 min −1 ). The excellent adsorption performance of 60 %LaOCl/40 %CeO 2 -g-C 3 N 4 is attributed to its negative zeta potential (−35.40 mV) and larger average pore size. The photochemical characterizations suggest that the 60 %LaOCl/40 %CeO 2 -g-C 3 N 4 form a dual Z-scheme heterojunction , which enhances its separation efficiency of photogenerated e - / h + with an outstanding redox ability, and further promotes the photocatalytic activity.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zengyue Chen,Yunfeng Li,Fei Tian,Xin Chen,Zhansheng Wu
In this work, a green reaction route for the preparation of BiVO 4 /g-C 3 N 4 composite is constructed using the acetic acid and reusable ethylene glycol system combined with the microwave method. The rice grain-like BiVO 4 is successfully deposited on the surface of hollow tubular g-C 3 N 4 to form a S-scheme heterojunction within 25 min. The performance of the prepared photocatalysts is evaluated by removing glyphosate, methyl orange and tetracycline hydrochloride from simulated agricultural and urban runoff. The degradation evaluation results show that acetic acid in this route could play a better induction role compared to the conventional inducer nitric acid, while the ethylene glycol in this route can be recycled. The recovery of ethylene glycol could reach more than 85%, and the performance of the produced photocatalyst will not be decreased after the recovery of ethylene glycol reaches 20 times. The BV/CN 60 -R 20 sample has the highest photocatalytic activity for glyphosate removal under simulated sunlight irradiation, which is 14.5 times and 9.7 times higher than that of pure BiVO 4 and g-C 3 N 4 , respectively. In summary, the establishment of the ethylene glycol and acetic acid system not only provides a new perspective for the replacement of strong acids in the preparation of BiVO 4 -based photocatalyst but also provides a reference for the construction of other harmless and recyclable systems.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wen-Chen Zhou,Wei-De Zhang
The development of stable and efficient non-noble metal-based photocatalysts for water splitting is currently a key but challenging process for effective conversion and storage of sustainable energy. Here, we designed a new non-noble metal composite photocatalyst by covalently connecting nickel molecular ligand (NiL) to the graphitized carbon nitride (CN) framework for photocatalytic hydrogen evolution under visible light irradiation. Compared to CN , NiL-modified CN (NiL/CN) shows excellent photogenerated carrier migration rate. Without Pt as a co-catalyst, NiL/CN exhibits high photocatalytic activity (23.4 μmol h −1 ) with high stability. Experiments and theoretical calculations disclose that ligand–metal charge transfer (LMCT) mechanism plays a key role on the enhancement of photocatalytic activity. This work provides a promising method for future designing low-cost, high-performance photocatalysts for hydrogen production under solar light.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
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IF 5.816
Jiawei Zhang,Yuying Dang,Wei Wang,Haijuan Zhan,Xudong Song,Baojun Ma
g-C 3 N 4 has great potential as metal-free and low-cost photocatalyst . However, its efficiency of photo-excited carriers separation is very low, it needs large amount of Pt (such as 3.0%) to resolve this problem. Here, we designed composite co-catalyst (Pt/MoP) and prepared (Pt/MoP)/g-C 3 N 4 . The optimal activity of (Pt/MoP)/g-C 3 N 4 reaches 531.75 μmol/h/g with 1.0% Pt. Compared with 3.0%Pt/g-C 3 N 4 , the activity of (Pt/MoP)/g-C 3 N 4 increased 2 times, whereas the amount of Pt is reduced 3 times. Photoelectrochemistry , surface photovoltage (SPV) and transient photovoltage (TPV) spectra prove (Pt/MoP) can effectively separate photo-excited carriers, thereby improve photocatalyst activity of g-C 3 N 4 . Here, MoP acts as electron storage due to the large capacitance, and Pt acts as proton reduction sites. This article gives a method to effectively reduce the amount of noble metal in photocatalysts.
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APPLIED CLAY SCIENCE
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2021
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IF 5.467
Yunhui Chen,Liping Wen,Jinxin Chen,He'an Luo,Jikai Liu
The clay mineral/g-C 3 N 4 composites were prepared through a simple one-pot synthesis with acid-treated clay minerals and melamine as precursors. Three typical clay minerals, e.g., kaolinite , sepiolite , and talc, were adopted as photocatalyst carriers. Notably, the acid-treated clay minerals coupled with g-C 3 N 4 in three different ways. The kaolinite/g-C 3 N 4 composite, in particular, proceeded with an intercalation reaction due to the in situ growth of g-C 3 N 4 within the layers of acid-treated kaolinite, leading to the expansion of kaolinite layers and a prominently large specific surface area of 61.9 m 2 g −1 . The resultant composites were used in photocatalytic H 2 generation by water splitting and CO 2 reduction, exhibiting superior photocatalytic performance to the g-C 3 N 4 . Among the obtained composites, the optimized kaolinite/g-C 3 N 4 showed the best photocatalytic activities , e.g. 3.03 μmol g −1 h −1 of CO evolution and 385 μmol g −1 h −1 of H 2 evolution, compared with merely 0.91 μmol g −1 h −1 of CO evolution and 96.4 μmol g −1 h −1 of H 2 evolution for bare g-C 3 N 4 . The superior performance of kaolinite/g-C 3 N 4 can be ascribed to the large specific surface area and better distribution of g-C 3 N 4 , which can enhance the light absorption , increase the number of active sites and favor the charge separation.
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