Chemosensors
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2022
·Vol. 10
·期 7
·286
·
IF 4.229
Yonghuan Su,Lixia Su,Bingqian Liu,Youxiu Lin,Dianping Tang
A highly sensitive self-powered photoelectrochemical (spPEC) sensing platform was constructed for Hg2+determination based on the g-C3N4-CdS-CuO co-sensitized photoelectrode and a visible light-induced redox cycle for signal amplification. Through successively coating the single-layer g-C3N4, CdS, and CuO onto the surface of an electrode, the modified electrode exhibited significantly enhanced PEC activity. The microstructure of the material was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR). However, the boost in photocurrent could be noticeably suppressed due to the consumption of hole-scavenging agents (reduced glutathione) by the added Hg2+. Under optimal conditions, we discovered that the photocurrent was linearly related to the Hg2+concentration in the range of 5 pM–100 nM. The detection limit for Hg2+was 0.84 pM. Moreover, the spPEC sensor demonstrated good performance for the detection of mercury ions in human urine and artificial saliva.Keywords:g-C3N4-CdS-CuO composites;self-powered photoelectrochemical assay;Hg2+detection;redox cycle signal amplification
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 29
·13931-13939
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IF 3.925
Nan Sun,Yuhan Jing,Yong Zhang,Xinru Li,Yaoning Bai,Yuwei Yan,Taoyuan Ouyang,Honglin Tan,Xiaoming Cai,Jinming Cai
Copper-based photocatalysts have attracted much attention because of their great prospects in photochemical conversion. However, the preparation of highly stable copper-based photocatalysts is a challenge. In this study, copper nanoparticles (Cu NPs) wrapped in graphitized polyacrylonitrile (g-PAN) were prepared by a two-step sintering method. Even if Cu@g-PAN is placed in the air for one month, the Cu NPs were still not oxidized. Furthermore, we succeeded in further introducing graphitized carbon nitride (g-C3N4) into the g-PAN shell structure, which was confirmed using a Scanning Transmission Electron Microscope (STEM), FT-IR, and UV-Vis absorption spectra. Cu@g-PAN/g-C3N4 can degrade 88.61% of methylene blue (MB) in one hour, showing a higher catalytic activity than Ag@g-PAN/g-C3N4 (55.18%). XPS and Auger electron spectroscopy tests of catalyzed Cu@g-PAN/g-C3N4 show that Cu is not oxidized. We have proposed a possible mechanism for charge separation and transformation in the Cu@g-PAN/g-C3N4 composites to explain the enhanced photocatalytic performance. This work provides a new method to protect Cu NPs and demonstrates the prospect of rational design of copper-based photocatalysts with high stability and efficiency.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
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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JOURNAL OF LUMINESCENCE
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2022
·
IF 4.171
Xin Bao,Enshan Liu,Xi Yuan,Hui Wang,Haibo Li,Songnan Qu
The development of anti-water phosphorescent carbon dots (CDs) based materials is of great practical interest. Herein, we report a rational design of CDs based composite with anti-water phosphorescence by controlling a one-step microwave assisted heating of green fluorescent CDs and urea. Upon increasing the microwave-heating temperature, urea was gradually converted to C 3 N 4 , in which the CDs were uniformly embedded in the C 3 N 4 matrix. The fluorescence/phosphorescence intensity of these CDs based composites are determined by the morphologies of the C 3 N 4 , which can be adjusted by controlling the microwave heating time. More importantly, the combining CDs in C 3 N 4 not only promote the phosphorescence emission but also prevent the phosphorescence quenching by water, leading to stable phosphorescence emission in aqueous environment. Based on the anti-water phosphorescence properties of these CDs based composites, a concept of multiple data encryption was demonstrated.
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Nanomaterials
·
2022
·Vol. 12
·期 9
·1416
·
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
·
2022
·
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
·
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
·
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
·
2022
·
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
·
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
·
2022
·
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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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 2
·1-9
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IF 6.408
Ma Xiangyu,Ma Yuheng,Ejeromedoghene Onome,Kandawa-Schulz Martha,Song Wei,Wang Yihong
An ultrasensitive photochemical biosensor based on the target miRNA-triggered catalytic hairpin assembly (CHA) reaction between Au nanoparticles (AuNPs)/C 3 N 4 nanosheets and CdS quantum dots (QDs) was developed for the determination of miRNAs. Firstly, AuNPs/C 3 N 4 nanosheets were immobilized onto a working glassy carbon electrode. Then, the hairpin probe 1 (H1) was loaded through Au–S bonding. Afterward, the unbound sites were blocked with 6-mercaptohexanol to avoid nonspecific adsorption. In the presence of the target miRNA, the CHA reaction between the H1 and hairpin probe 2-CdS QDs (H2-CdS QDs) could be triggered. As a result, the AuNPs/C 3 N 4 nanosheet and CdS QDs were linked by the double helix structure H1-H2. Unlike the other CHA reactions, H2 used in this work is longer than H1 so that the AuNPs/C 3 N 4 nanosheets could touch the CdS QDs. Given the matched energy band positions between the C 3 N 4 nanosheet and CdS QDs, a strong photocurrent could be obtained after the CHA reaction was triggered by the target miRNA. In addition, p-type C 3 N 4 nanosheets and n-type CdS QDs presented reduction photocurrents and oxidation photocurrents, respectively. Therefore, the photocurrents were vectors in this design that can eliminate the interference of nonspecific adsorption and avoid the generation of false-positive signals. Under the optimal conditions, the limit of detection was 92 aM. The constructed photoelectrochemical biosensor showed good reproducibility and selectivity in the analysis of serum samples, which indicates its great prospects in disease diagnostics and bioanalysis. Graphical abstract
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