CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yang Li,Qiao Yin,Yingshan Zeng,Zhi Liu
The core of realizing the effective CO 2 conversion by solar energy is to develop a stable photocatalyst with high CO 2 adsorption capacity and high charge separation efficiency. In this work, a hollow spherical Z-scheme SnS 2 /g-C 3 N 4 /C (SCC) photocatalyst is successfully constructed by a morphology-inherited strategy. Biomass mabospores are utilized as both the precursor for formation of hollow spherical structure and carbon source, and the g-C 3 N 4 and SnS 2 nanosheets tightly anchor on the surface of mabospores-derived carbon spheres. The Z-scheme SCC heterostructure exhibits 5.5 times activity enhancement on CO 2 photoreduction to CO with a high evolution rate up to 40.86 μmol∙g −1 ∙h −1 . Examined by various photoelectrochemical analysis, the boosted photocatalytic activity originates mainly from the construction of hollow spherical Z-scheme heterojunction, providing the more preferable basic sites for CO 2 adsorption, promoting the separation efficiency of electron-hole pairs, as well as increasing the reductionability of electrons in conduction band of g-C 3 N 4 . The formed internal electric fields between the g-C 3 N 4 and SnS 2 can also further reinforce the spatial separation of photogenerated charge carriers. Theoretical calculations further verify that the SCC Z-scheme heterostructure can effectively decrease the energy barriers of formed intermediates, especially the crucial COOH*, and thus leading to the facile conversion of CO 2 -to-CO. This work induces a new strategy to construct g-C 3 N 4 -based Z-scheme heterojunction assisted by versatile biomasses with optimized structure and enhanced photoelectrochemical merits for efficient CO 2 conversion into chemical fuels.
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OPTICAL MATERIALS
·
2022
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IF 3.754
Shirong Kang,Hao Zhang,Mingyu Dou,Gaimei Gao,Hongjie Zhu,Hua Yang,Dacheng Li,Jianmin Dou
The heterojunction structure with CdS@g-C 3 N 4 photocatalyst was obtained via a simple microthermal chemical in-situ deposition method. The catalyst CdS@g-C 3 N 4 (weight ratio of 1:3) maintained excellent degradation activity to 10 ppm tetracycline (TC) after four cycles due to Z-scheme electron transport mechanism, which was demonstrated through several methods, and the photo-corrosion of CdS was inhibited successfully own to this electron transfer paths. Microscope images showed CdS nanoparticles were uniformly distributed on g-C 3 N 4 nanosheets , such surface morphology provided numerous active sites and excellent adsorption performance for photodegradation process. Mechanism study demonstrated the high energy active species including h + , •O 2 − and •OH take part in the degradation process. Through the mass spectrometry analysis , intermediate products and degradation pathway were inferred on TC during photodegradation process. In addition, this study proved the extremely low toxicity of TC aqueous solution after degradation, there was special significance for ecological and environmental protection. This work provided a reference for the design of the Z-scheme photocatalyst and synthesis of catalysts at low temperature (80 °C), and it has application potential in the treatment of water pollution.
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CHEMOSPHERE
·
2022
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IF 8.943
Yanlin Zhang,Wei Chu
In this study, a Fe 3+ /g-C 3 N 4 hybrid catalyst system was proposed to activate peroxymonosulfate (PMS) for the metronidazole (MNZ) photocatalytic degradation . The two catalysts, Fe 3+ and g-C 3 N 4 , exhibited an obvious synergistic effect in the photocatalytic degradation process. When 1 mM PMS, 0.04 mM Fe 3+ and 0.05 g L −1 g-C 3 N 4 were applied, the rate constant of the Fe 3+ /g-C 3 N 4 /PMS/LED process at 0.07288 min −1 is around 3.6 to 6.8 times faster than that of Fe 3+ /PMS/LED and g-C 3 N 4 /PMS/LED processes at 0.0198 and 0.01076 min −1 , respectively. Under visible light, electron transfer from photo-activated g-C 3 N 4 to Fe 3+ , resulting in the continuous regeneration of Fe 2+ in the system, which ensures non-stopping production of radicals for MNZ degradation. UV–visible spectra were used to confirm the regeneration of Fe 2+ . In addition, EPR tests were used to identify the reactive oxygen species involved in the reaction system. Typically, the effects of various operation parameters, including the catalyst dosage, PMS dosage, initial concentration of MNZ and initial pH were examined. This work provided a new idea of promoting pollutant degradation by accelerating Fe 3+ /Fe 2+ redox through semiconductor, which could help to use the catalyst more effectively for wastewater treatment and/or chemical industries.
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高影响因子
ECOTOXICOLOGY
·
2022
·Vol. 31
·期 3
·503-515
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IF 2.935
Hu Xuemei,Peng Kuan,Chen Yijun,Chen Xiaoyong,Liu Shuguang,Zhao Yunlin,Wu Yaohui,Xu Zhenggang
Photocatalysts have been widely prepared and used in wastewater treatment. Although the influence of photocatalyst application on survival and activity of organisms has been examined, its impact on composition and diversity of microbial community is not fully understood. In this study, the impact of photocatalyst g-C 3 N 4 (Graphitic carbon nitride) on microbial communities in riverbed sediments polluted by antibiotic tetracycline (TC) was investigated. The sediment samples collected from the Xiangjiang River of China were exposed to different concentrations of TC, g-C 3 N 4 and TC/g-C 3 N 4 and the bacterial community were analyzed by Illumina sequencing. The results showed that the dominant bacterial phyla were Acidobacteriota, Proteobacteria, Actinobacteriota , and Chloroflexi in the study site. When compared to the control treatments, the application of TC, g-C 3 N 4 and TC/g-C 3 N 4 exhibited distinguishable effects on bacterial community structure in sediments. The presence of TC had greater influence on bacterial composition, while g-C 3 N 4 and TC/g-C 3 N 4 had less influence on bacteria. The diversity and richness of microorganisms in sediment increased under g-C 3 N 4 application and reached the highest values when g-C 3 N 4 was 75 mg/kg. The photocatalyst g-C 3 N 4 restored bacterial community diversity affected by TC, reduced the TC residues in aquatic environment, and eliminated the side effects of TC application in sediments. Our study indicated that g-C 3 N 4 was an environmentally friendly photocatalyst with lightly negative effects on microbial community in riverbed sediments, and could be used for effective remediation of TC-contaminated environments.
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高影响因子
Reaction Kinetics Mechanisms and Catalysis
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2022
·Vol. 135
·期 1
·219-231
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IF 1.843
Li Jianyu,Zhang Jiaojing,Wang Yuanyuan,Wang Huan,Song Hua
The high efficiency amphiphilic CTAB-PW( x )/g-C 3 N 4 catalysts with different quaternary ammonium phosphotungstate (CTAB-PW) loadings ( x , wt%) were designed and successfully synthesized. The catalysts were characterized by XRD, SEM, FTIR, XPS and BET. The effects of CTAB-PW loading, oxidative desulfurization (ODS) conditions and different sulfides on the performance of ODS were investigated using green oxidant H 2 O 2 as oxidant in solvent-free reaction system. The results show the crystalline structure of CTAB-PW and g-C 3 N 4 were retained in CTAB-PW( x )/g-C 3 N 4 hybrid materials. And the use of cetyltrimethylammonium bromide (CTAB) can save cost and prevent the application of harmful solvents. The CTAB-PW( x )/g-C 3 N 4 with CTAB-PW loading of 50% exhibited the best ODS performance. The benzothiophene, dibenzothiophene removal rate of 99.9% and 4,6-dimethyl-dibenzothiophene removal rate of 98.9% were achieved under the conditions of catalyst dosage of 0.04 g, O/S molar ratio of 8, reaction temperature of 60 °C for 2 h. Moreover, the removal rate of benzothiophene still maintained at 94.3% after the catalyst was recovered for 5 times, which was mainly due to the presence of amino group in g-C 3 N 4 , which can inhibit the leaching of active phosphotungstate (HPW). Graphical abstract
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 11
·5176-5187
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IF 3.925
Yuzhen Li,Shaojie Wang,Yunsheng Xia,Lizhen Gao
A series of Z-scheme CuSnO3/g-C3N4 heterojunctions were synthesized by a precipitation–calcination method. Morphological features, chemical composition, optical properties and crystallographic information of the prepared materials were obtained using scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), UV–Vis diffuse reflection spectroscopy (UV-Vis DRS), and photoluminescence spectroscopy (PL). The as-fabricated catalysts assisted by H2O2 showed remarkably enhanced photocatalytic performance for the degradation of tetracycline (TC) under visible light irradiation. The 20 wt% CuSnO3/g-C3N4 composite exhibited the highest photocatalytic degradation activity, which could be up to 93.6% at 60 min for the degradation of TC under visible light irradiation. Reactive species scavenging experiments revealed that superoxide radicals were the main active species during the photocatalytic process. This work will be useful for the design of other direct Z-scheme photocatalytic systems for applications in energy conversion and environmental remediation.
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RSC Advances
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2023
·Vol. 13
·期 22
·15302-15310
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IF 3.9
Deng Gu,Yuanjin Wang,Zhiman Liang,Yanting Dou,Zhenhe Xu,Jiqi Zheng,Yaguang Sun,Fu Ding,Yu Gao
The construction of a heterojunction and the introduction of a cocatalyst can both promote the transfer of photogenerated electrons, which are effective strategies to enhance photocatalytic efficiency. In this paper, a ternary RGO/g-C3N4/LaCO3OH composite was synthesized by constructing a g-C3N4/LaCO3OH heterojunction and introducing a non-noble metal cocatalyst RGO through hydrothermal reactions. TEM, XRD, XPS, UV-vis diffuse reflectance spectroscopy, photo-electrochemistry and PL tests were carried out to characterize the structures, morphologies and carrier separation efficiencies of products. Benefiting from the boosted visible light absorption capability, reduced charge transfer resistance and facilitated photogenerated carrier separation, the visible light photocatalytic activity of the ternary RGO/g-C3N4/LaCO3OH composite was effectively improved, resulting in a much increased MO (methyl orange) degradation rate of 0.0326 min−1 compared with LaCO3OH (0.0003 min−1) and g-C3N4 (0.0083 min−1). Moreover, by combining the results of the active species trapping experiment with the bandgap structure of each component, the mechanism of the MO photodegradation process was proposed.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 46
·期 4
·1960-1971
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IF 3.591
Wen He,Yongbo Xie,Qiang Yin,Zixuan Zhao,Lang Shi,Hongqing Wang
Scientists are still working on developing a “turn-on” fluorescence sensor for Co2+, especially in acidic solutions. A novel “on–off–on” fluorescence sensor based on g-C3N4 nanosheets was designed and prepared in this paper. It was able to detect (2-(5-bromo-2-pyridylazo)-5(diethylamino)phenol (abbreviated to 5-Br-PADAP) and Co2+ quantitatively by quenching and restoring the fluorescence of the g-C3N4 nanosheet system, respectively. Also discussed are the effects of solvent, pH, order of addition, and interaction time of 5-Br-PADAP and Co2+, as well as the concentration range of the object on measurement. Furthermore, in acidic conditions, the sensor demonstrated good selectivity and sensitivity. In the solvent system EtOH : H2O (v/v = 1 : 9, pH = 3), the fluorescence intensity had a good linear relationship with 5-Br-PADAP and Co2+ concentrations in the ranges of 0–15 μM and 0–10 μM, with low detection limits of 64 nM and 44 nM, respectively. Experiments and theoretical calculations were used to describe the interaction characteristics and sensing mechanism. It was eventually successful in detecting Co2+ in environmental samples.
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
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2021
·
IF 2.262
Tian Ma,Yunhai Wu,Ningning Liu,Xiaoming Tao,Yunying Wu
In this work, iron-doped graphite carbon nitride (Fe-g-C3N4) was integrated with CoMoO4 through a simple hydrothermal route and high temperature calcination to synthesize distinctive composites, aiming to create a promising heterogeneous catalyst to active peroxymonosulfate (PMS) for the degradation of methylene blue (MB), a widely used organic dye. The characterization results, including SEM, EDX, FTIR, XRD and XPS, indicated that the crystal structure and physicochemical properties of CoMoO4-Fe-g-C3N4 have changed after modification, with rougher surface and efficient catalytic activity. The effects of several operational factors (catalyst dosage, oxidant dosage, reaction temperature and initial pH) were also extensively evaluated. Under the condition of CoMoO4-Fe-g-C3N4=0.1 g L−1, oxidant = 2.0 mM, dye = 100 mg/L, T = 25 °C, the MB in the CoMoO4-Fe-g-C3N4/PMS catalytic system can reach almost complete degradation in 90 minutes without pH adjustment. Further, stability experiment showed that the CoMoO4-Fe-g-C3N4 catalysts exhibited high stability and superior reusability, with 80% removal rate even after five concessive cycles of use. Additionally, through radical quenching experiments, it proved that SO4•− radicals were dominant and HO• radicals also worked in the MB degradation process. An underlying mechanism was proposed based on the detection of XPS results that both radical and non-radical degradation pathways existed during MB degradation process. The electron transfer from high-valence iron species (FeIV=O) to MB resulting in the degradation of MB through a non-radical mechanism. From the investigation, the CoMoO4-Fe-g-C3N4 composite was proved to have potential superiority as a promising catalyst for the degradation of refractory organic contaminant removal from water.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wenxiu Li,Wei Li,Zanwu Guo,Yi Song,Shaoru Tang,Yanan Ma,Xueqing Xing,Qian Wang
The atomically thin nanosheets of graphitic carbon nitride (g-C3N4) with mesopores have been successfully exfoliated with supercritical CO2 (scCO2). The thickness of the as-synthesized samples could be directly tailored by simply regulating the scCO2 pressure. The obtained bilayer mesoporous g-C3N4 nanosheets doped with monatomic Co through a microwave-assisted approach havve been employed as single-atom catalysts to enhance the photocatalytic hydrogen evolution performance. The as-prepared Co/P/CN-sc sample exhibited a boosted H2 production performance due to its unique structural advantages by exposing more active sites and facilitating the separation of charge carriers. Based on X-ray photoelectron spectroscopy, steady-state and time-resolved photoluminescence spectroscopy, X-ray absorption fine structure measurement, and density functional theory (DFT) calculations, a possible mechanism has been proposed. The work shows a new perspective for designing an inexpensive photocatalyst with a unique structure through a facile and green approach for photocatalytic hydrogen evolution.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·
IF 3.3
Weilong Zhang,Xian Li,Huan Cheng,Jie Yang,Jumei Li
Herein, hollow hZrO2/g-C3N4 composite photocatalysts were successfully fabricated using polymethylacrylic acid (PMAA) nanospheres as sacrificial templates via reflux-precipitation polymerization and subsequent ZrO2 layer coating by sol–gel method over PMAA nanospheres, calcining process, and forming composites with g-C3N4 in sequence. The formation mechanism of the unique composites was proved by FESEM, TEM, XPS, XRD, and EDX mapping characterizations. The photodegradation tests of methylene blue (MB) and ciprofloxacin (CIP) were used to investigate the photocatalytic activity. The results revealed that hZrO2/g-C3N4 exhibited significantly boosted photocatalytic activity for degrading 99.7% methylene blue and 81.5% ciprofloxacin in 120 min under simulated sunlight irradiation (Xe lamp, 500 W), which was much better than that of hZrO2 (42.1% for MB and 19.1% for CIP). The enhanced performance is presumably attributed to the synergetic interaction of the two components and the efficient separation of the photoproduced electron–hole pairs between ZrO2 and g-C3N4, which was verified using photocurrent and EIS characterizations. On the basis of the scavenging studies of free radicals (e−, h+, ˙O2−, and ˙OH), the mechanism of the boosted photocatalytic activity was proposed. More significantly, the composites presented excellent reusability confirmed by cyclic photocatalytic degradation experiments, which is crucial for the sustainable and green applications of photocatalysts.
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PROGRESS IN ORGANIC COATINGS
·
2023
·
IF 6.6
Qiang Liu,Hao Li,Ling Kong,Yiming Du,Yunsheng Da,Zhouping Sun,Yong Dong,Yanyan Liu,Hua Wang
Due to the low volatile organic compound (VOC) emissions, waterborne coatings are gaining much attention. However, the weak barrier properties prevent them from being practical. In this study, a novel well-dispersed low-defective the g-C 3 N 4 nanosheets are successfully prepared using urea and polydopamine, followed by the preparation of an extensible bio-inspired coating. The bio-inspired coating comprises of PDA@g-C 3 N 4 nanosheets that are oriented and possess zigzag channels, rendering them impervious to corrosion factors. Electrochemical tests have demonstrated that the bio-inspired coating displays a substantially improved resistance of 1.18 × 10 10 Ω cm 2 , surpassing the pure epoxy coating (6.77 × 10 7 Ω cm 2 ) by three orders of magnitude. Moreover, the excellent corrosion resistance of the bio-inspired coating has been substantiated through salt spray tests. The development of bio-inspired composite coatings presents a novel avenue for investigating the synthesis of waterborne epoxy coatings with exceptional performance.
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