ACS ES&T Engineering
·
2022
·
IF 0
Shuqian Dong,Xu Chen,Linfeng Su,Yingjie Wen,Yuechu Wang,Qihao Yang,Li Yi,Wenwen Xu,Qiu Yang,Peilei He,Yunqing Zhu,Zhiyi Lu
Photo-Fenton degradation as a promising strategy for antibiotic wastewater treatment attracted extensive attention, while the unsatisfactory catalytic performance vitally limits its industrial application. Herein, we demonstrate that confining atomically dispersed Cu into C3N4 (Cu–C3N4) enables fast H2O2 activation and efficient separation of photogenerated electron–hole pairs, resulting in a dramatic improvement of the degradation efficiency of the Photo-Fenton reaction. Photo-Fenton degradation of ciprofloxacin (CIP) was close to 99% within 30 min over optimized Cu–C3N4, corresponding to a pseudo-first-order rate constant of ∼0.0978 min–1, almost 4.5 times higher than pure C3N4 counterpart. The electron paramagnetic resonance, quenching experiments, and X-ray absorption fine structure results reveal that the superior Photo-Fenton catalytic performance is attributed to a nonradical reaction pathway, where the H2O2 is activated by the formation of the O═Cu–N4═O intermediate. The advanced catalyst as well as the refreshing H2O2 activation mechanism are of profound significance for the materials design in the wastewater treatment field.
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ENERGY & FUELS
·
2020
·
IF 3.421
Menglong Sun,Qian Wang,Baiying Dai,Weihua Sun,Yaru Ni,Chunhua Lu,Jiahui Kou
A simple combination of thermal etching and liquid-phase ultrasonic stripping was deployed to prepare high-performance graphite carbon nitride (g-C3N4) nanosheets. Also, graphene oxide with plentiful active groups was used to combine g-C3N4 with a magnetically actuated artificial cilia array (MAACA) to generate a composite cilia array, which can ensure the facile recovery of g-C3N4. This strategy addresses the limitations of an adjustable band gap for easy response to visible light and circumvents the encumbered limitation of recyclability, thus addressing a chronic environmental problem by curbing waste. The underlying functional principle of the array used was analyzed and studied in greater detail. The photocatalytic hydrogen production efficiency of MAACA with 0.4 mg of g-C3N4 at a magnetic field driving frequency of 12.50 Hz was found to be ∼75.0% higher than that at a magnetic field driving frequency of 0 Hz.
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Reaction Kinetics Mechanisms and Catalysis
·
2018
·Vol. 125
·期 2
·1179-1190
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IF 1.515
Mao Yong,Wu Mingzai,Li Guang,Dai Peng,Yu Xinxin,Bai Zhiman,Chen Peng
For highly efficient photodegradation of organic pollutants, the enhancement of photocatalytic activity of metal-free photocatalyst graphitic carbon nitride (g-C 3 N 4 ) under visible light irradiation is meaningful, but still challenging due to the fast recombination of photogenerated electron–hole pairs, low quantum efficiency and specific surface area of pristine g-C 3 N 4 . To address these challenges, boron-doped g-C 3 N 4 together with nitrogen-vacancies (Bd-Nv-C 3 N 4 ) was designed and synthesized through a simple acid-assisted calcination of melamine without any further tedious operations. As expected, based on the synergistic effect of foreign elements doping (boron atoms doping) and intrinsic defects (nitrogen vacancies), the as-prepared novel Bd-Nv-C 3 N 4 photocatalyst shows lower band gap, higher surface area and separation efficiency of photogenerated electron–hole pairs, achieving a nearly tenfold increase of the phtocatalytic constant for methylene blue (MB) degradation compared to that of pristine g-C 3 N 4 without nitrogen-vacancies and boron-doping. This study provides a new train of thought and method for the design and preparation of nonmetal photocatalysts with enhanced visible light irradiation photocatalytic performance.
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ADVANCED SYNTHESIS & CATALYSIS
·
2016
·Vol. 358
·期 16
·2631-2641
·
IF 6.453
Lingling Wang,Min Yu,Chaolong Wu,Nan Deng,Chao Wang,Xiaoquan Yao
In this contribution, an Ag/g-C 3 N 4 nanocomposite was synthesized and utilized as highly efficient and green photocatalyst for organic reactions under visible light irradiation. A layered, porous g-C 3 N 4 was synthesized following a modified solvothermal-roasting process by using melamine and cyanuric chloride as precursor. Silver nanoparticles (NPs) were well anchored on g-C 3 N 4 nanosheets, which were prepared by a facile impregnation–roasting method. The inexpensive, stable g-C 3 N 4 coupled with the localized surface plasmon resonance (LSPR) effect of Ag NPs exhibited high photocatalytic activities toward aerobic oxidative amidation of aromatic aldehydes under visible light irradiation. Good to excellent yields were achieved for various substrates under the light of a 25 W compact fluorescent light (CFL) bulb in air. The operationally easy procedure provides an economical, green, and mild alternative for the formation of amide bonds.
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Catalysts
·
2025
·Vol. 15
·期 5
·504
·
IF 4
Xiyuan Gao,Pengnian Shan,Weilong Shi,Feng Guo
The development of photothermal-assisted photocatalytic systems with broad-spectrum solar utilization and high charge separation efficiency remains a critical challenge for antibiotic degradation. Herein, we report novel black g-C3N4(BCN) materials synthesized via a one-step thermal copolymerization strategy using C/N precursors and tetrachlorofluorescein. After the introduction of tetrachlorofluorescein, the color of the sample changes, which gives BCN enhanced light absorption and a significant photothermal effect for poorly heating-assisted photocatalysis. The synergistic coupling of photothermal and photocatalytic processes enabled the optimal BCN-U sample to achieve exceptional degradation efficiency (89% within 120 min) for a typical antibiotic (e.g., tetracycline) under an LED lamp as the visible light source, outperforming conventional yellow g-C3N4(YCN-U) by a factor of 1.37. Mechanistic studies revealed that the photothermal effect facilitates carrier separation via thermal-driven electron excitation while accelerating reactive oxygen species (•OH and •O2−) generation. The synergistic interplay between photocatalysis and photothermal effects, which improved mass transfer, ensures robust stability, which provides new insights into designing dual-functional carbon nitride-based materials for sustainable environmental remediation.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 9
·期 2
·302-309
·
IF 6.569
Jiayu Xin,Fei Li,Zhen Li,Jiaqi Zhao,Yu Wang
Single-atom dispersed carbon nitride photocatalysts have been extensively associated with clean energy conversion, storage and utilization. However, it is still a challenge to elucidate the relationship between the electronic structure of catalysts and their photocatalytic properties. In this work, single atom Ag/C3N4 catalysts have been prepared via pyrolyzing cyanuric acid, AgNO3 and melamine as precursors. We observe that their photocatalytic activity increases on increasing the concentration of Ag from 0.32% to 0.53%, and subsequently decreases on further increasing the concentration of Ag, which indicates that the concentration of Ag atoms can control the performance of single-atom catalysts. Deep investigations suggest that the concentration of Ag atoms can modulate the bottom of the conduction band (CB) and the maximum of the valence band (VB). The higher the bottom of the CB is, the better the performance of catalysts is. In contrast to bulk carbon nitride, the rate constants of the optimized single-atom photocatalyst Ag/C3N4 with 0.53% Ag for rhodamine B (RhB) and tetracycline (TC) degradation are enhanced approximately 165.3 and 24.9 times, respectively. Furthermore, the ESR spectrum shows that the superoxide radical plays a major role in the photocatalytic process. This work provides a new insight into the structure–property relationship and our strategy provides guidance for the synthesis of other single-atom photocatalysts.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Qing Yu,Shiyi Wang,Mengru Wang,Xiaoling Mou,Ronghe Lin,Yunjie Ding
Acetylene coupling with ethylene dichloride, which uses both coal and oil resources, is attractive for sustainable PVC manufacturing. Herein, highly active and stable carbon nitride-based catalysts were developed by a novel pre-oxidation-pyrolysis process, affording unprecedented dehydrochlorination activity with good durability. The best-performing system was further modified with different precious metals (Au, Pt, and Ru) to promote the hydrochlorination chemistry between the in-situ formed hydrogen chloride and acetylene co-feed. The presence of metal centers intensifies the hydrochlorination activity but weakens the dehydrochlorination ability due to competitive adsorption between the two reactants at the metal sites. Superior coupling performance was achieved over C 3 N 4 /AC and single-atom Au/C 3 N 4 /AC catalysts in cascade reactors. Our results strongly suggest that dehydrochlorination is an essential step in the coupling reaction, and the activation of acetylene and ethylene dichloride molecules requires different active sites that should be engineered in future work.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xiuyang Zou,Meisheng Li,Huifang Xiao,Shouyong Zhou,Chenglung Chen,Yijiang Zhao
The complex transport mechanism of water and ions in the membrane hinders the design of free standing membranes. The mechanism of the mass transport characteristics of traditional nanofiltration membranes is no longer applicable to free standing membranes due to the change of the driving force in the membrane. In this study, the vacuum filtration of the g-C 3 N 4 suspension was simulated to form a free standing membrane model for the first time by using the molecular dynamics (MD) simulations. In the nanochannels formed by the g-C 3 N 4 nanosheets , the water molecules rapidly penetrated across the free standing membrane due to ultra-low friction. On the other hand, the hydrated Na + and Mg 2+ ions needed energy to partially dehydrate and penetrate across the free standing membrane. Moreover, the MD simulations indicated that the speed of Mg 2+ ions penetrating across the g-C 3 N 4 nanochannels was lower than that of Na + ions. Combined with the computational works, salt retention experiments were conducted to demonstrate the correctness of the proposed model. Further, the developed membranes exhibited excellent non-swelling stability and antibacterial activity in aqueous solutions. The g-C 3 N 4 free standing membranes prepared in this study can effectively realize the separation of monovalent and divalent ions, accompanied with high permeability.
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CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Bo Yu,Fanming Meng,Muhammad Wasim Khan,Rui Qin,Xingbin Liu
Traditional bulk photocatalysts often experience serious charge recombination and poor visible-light capturing, resulting in inefficient photocatalytic activity. However, proper nanostructure design usually helps to increase the activity of composite photocatalysts. Here, hollow TiO 2 @g-C 3 N 4 /Co 3 O 4 core-shell microspheres are first reported. The hollow structure of the heterostructured will directionally separate the photogenerated carriers, and the photogenerated holes transferred to the surface will be further captured by Co 3 O 4 to achieve an exposed oxidized surface. The novel multi-stage hollow microspheres can simultaneously achieve effective transfer of photogenerated carriers and extended light absorption. Benefiting from these structural and compositional characteristics, the optimized TiO 2 @g-C 3 N 4 /Co 3 O 4 nanospheres have excellent photodegradation activity for tetracycline and MO. Under simulated sunlight, the degradation rates of TC (10 mg/L) and MO (25 mg/L) at 60 min are 91.6% and 97.8%, respectively. At the same time, high activity is maintained after multiple cycles of testing. Possible transfer paths for photogenerated carriers have also been proposed. This work will provide more inspiration for the design of multi-stage hollow photocatalytic systems.
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Arabian Journal of Chemistry
·
2024
·
IF 5.3
Azim Khan,Ruhumuriza Jonathan,Shafiq Ur Rehman,Muhammad Shoaib,Feng Cao,Sajjad Ali,Mohamed Bououdina,Pir Muhammad Ismail,Junwei Wang,Hazem Abu-Farsakh,Yifan Liu,Xian Jian
Enhancement in the visible light absorption and efficient interfacial charge transfer is crucial for optimizing photocatalytic efficiency in the degradation of pollutants such as methyl orange (MO) and formaldehyde. This study focuses on the properties of a TiO 2 /C/g-C 3 N 4 hybrid efficient photocatalyst, which is developed using an air calcination method to deposit graphitic nitride (g-C 3 N 4 ) onto a carbon-modified TiO 2 surface. The characterization techniques, including high-resolution transmission electron Microscopy (HRTEM), X-ray diffraction (XRD), Raman spectroscopy, thermogravimetric analysis (TGA), Fourier-transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS), were used to provide a comprehensive understanding of the material’s structural, morphological, thermal, and chemical properties. This hybrid catalyst is specifically engineered for the efficient decomposition of methyl orange (MO) and formaldehyde, demonstrating a significant increase in photocatalytic activity. The TiO 2 /C/g-C 3 N 4 photocatalyst also exhibits an enhanced specific surface area of 181.2 m 2 /g, which facilitates increased physical adsorption and photo-catalytic active sites. Experimental results confirm that this catalyst effectively adsorbs MO physically even in the dark without degradation. Combining physical and photo-catalytic functions, this catalyst degrades 94 % of MO within 180 min with the initial concentration 0.2 mol/L of MO, and achieves almost 100 % decolorization of MO under visible light irradiation. Notably, the catalyst retains its high activity after 4 cycles of MO degradation, underscoring its durability and consistent performance. Additionally, the hybrid catalyst features a staggered type-II energy level configuration, which effectively enhances charge separation and boosts photocatalytic efficacy. The incorporation of an ultrafine carbon layer further augments electron mobility towards the surface, crucial for effective catalytic reactions. This study paves the way for future development of highly efficient photocatalytic materials for environmental purification.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ke Xiang,Shaoyi Wu,Tiefeng Xu,Wangyang Lu
The photocatalysis-assisted peroxymonosulfate (PMS) activation process has shown great potential for organic wastewater treatment. Herein, the composite photocatalyst (FeTAPc/PDI/CN) was obtained by grafting graphitic carbon nitride (CN) and amino iron phthalocyanine (FeTAPc) onto both ends of perylene tetracarboxylic anhydride (PTCDA) through an imidization process. Under simulated solar irradiation, the catalyst exhibited a remarkable degradation performance toward the target pollutant by activated PMS over a wide pH range from 3 to 11. The degradation efficiency of SMX reached 100 % in 7 min with the reaction kinetic constant of 0.845 min −1 , which was 13 times higher than that of pure CN. In addition, the removal rate of FeTAPc/PDI/CN-4 for SMX was more than 80 % after 9 cycles. The introduction of phthalocyanine and PDI improved the separation efficiency of photogenerated electron-hole pairs. Furthermore, the active species involved in the SMX degradation were identified as •OH, SO 4 • - , •O 2 – and 1 O 2 . The possible degradation pathways were proposed based on the identified intermediates, in which the oxidation of the amino group on the benzene ring was the main degradation pathway. This study is anticipated to result in a favorable method for designing CN-based photocatalysts with high stability and excellent catalytic activity for environmental remediation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Feng He,Qianxiang Xiao,Yin Chen,Hongqing Wang,Xiangke Wang
In the photoreduction of U(VI), protective gases and additional sacrificial agents are still the major obstacles. Herein, we developed an oxygen-deficient WO x /g-C 3 N 4 catalyst for the simultaneous reduction of U(VI) and preparation of benzaldehyde by selective oxidation of benzyl alcohol without protective gases and sacrificial agents. The removal of U(VI) by WO x /g-C 3 N 4 could reach 98.5% and the conversion of benzyl alcohol was nearly 32% with a selectivity close to 100%. Compared with single g-C 3 N 4 and defect-free WO 3 , the photoreduction activity of WO x /g-C 3 N 4 was 10.4 and 7 times higher, respectively. Besides, the role of oxygen and oxygen defects was explored. Owing to oxygen defects in the catalyst, oxygen was adsorbed on the oxidation end (WO x ) of the catalyst and activated without entering the reduction end to interfere with the photoreduction of U(VI), while favoring the generation of •O 2 - to improve the selectivity of benzaldehyde. Finally, a new mechanism was proposed.
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