Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Shuang Liu,Hong Wu,Huaili Zheng,Weizhen Zhang,Wei Ding,Hong Li,Chao Liu
Sulfite (S(IV))-based advanced oxidation process has attracted widespread attention due to the generation of strongly oxidizing sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) for contaminants remediation. However, the contaminant degradation by singlet oxygen ( 1 O 2 ) through a nonradical pathway was still unclear in the S(IV) activation system. Herein, a magnetic Fe 3 O 4 /g-C 3 N 4 (MCN) composite was synthesized for the utilization as a visible-light catalyst to activate S(IV) under visible-LED (Vis-LED) for the organic degradation . The incorporation of Fe 3 O 4 in g-C 3 N 4 up-regulated the photocatalytic performance in the S(IV) activation for X-3B degradation, and > 98% of X-3B (20 mg L −1 ) was degraded with the degradation rate constant ( k obs ) of 0.110 min −1 within 30 min. The SO 4 •− and 1 O 2 produced in the MCN/S(IV)/Vis-LED system were identified as the primary reactive species through the quenching experiments and electron spin resonance. Interestingly, the light-induced generation of superoxide radical (O 2 •− ) played a negligible role in the formation of 1 O 2 , and most of 1 O 2 was corroborated to be originated from SO 4 •− besides SO 5 •− , which was rarely reported in other S(IV) activation processes. The catalysts before and after utilization were characterized to further elucidate the mechanisms for the S(IV) activation. There were two possible pathways for the S(IV) activation: the electron transfer from S(IV) to the photo-generated holes and the ligand-to-metal charge-transfer (LMCT) within the surface Fe(III)−S(IV) complexes. Furthermore, the MCN/S(IV)/Vis-LED system was of high resistance to complex water matrixes (pH, inorganic anions, etc.), demonstrating its application perspective in the purification of wastewater containing organic pollutants .
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 31
·14828-14839
·
IF 3.3
Lin Dong,Yunlan Xu,Dengjie Zhong,Nianbing Zhong,Zhuofan Han,Yi Liu,Haixing Chang
The low electron–hole separation in the photoanode generally restricts the visible light response of photocatalytic fuel cell (PFCs). In this study, 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode was synthesized and assembled with a PFC with Cu cathode to degrade rhodamine B and generate electricity. With visible light irritation, the maximum photocurrent density, maximum power density, and degradation rate of the PFC were 0.59 mA cm−2, 29.88 μW cm−2, and 97.48% (1 h), respectively. The major active species in the PFC were h+, ˙O2−, and ˙OH. The good performance of the PFC was ascribed to the formation of a double Z-type heterojunction in the 5% NH2-MIL-125/g-C3N4/Bi2O3/Ti photoanode so that the photoelectrons of NH2-MIL-125 and Bi2O3 directly combine with the photoholes of g-C3N4, making the photoholes of NH2-MIL-125 and Bi2O3 and the photoelectrons of g-C3N4 directly or indirectly involved in the RhB degradation process and generating electricity. Thus, the separation rate of the e−–h+ pairs in the photoanode and the capability of the PFC are greatly improved.
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MOLECULES
·
2023
·Vol. 28
·期 15
·5815
·
IF 4.6
Dongmei Peng,Zhongfeng Zhang,Jijuan Zhang,Yang Yang
The photocatalytic degradation of formaldehyde by graphite-like C3N4is one of the most attractive and environmentally friendly strategies to address the significant threat to human health posed by indoor air pollutants. Despite its potential, this degradation process still faces issues with suboptimal efficiency, which may be attributed to the rapid recombination of photogenerated excitons and the broad band gap. As a proof of concept, a series of graphite-like C3N4@C60composites combining graphite-like C3N4and C60was developed via an in situ generation strategy. The obtained graphite-like C3N4@C60composites exhibited a remarkable increase in the photocatalytic degradation efficiency of formaldehyde, of up to 99%, under visible light irradiation, outperforming pure graphite-like C3N4and C60. This may be due to the composites’ enhanced built-in electric field. Additionally, the proposed composites maintained a formaldehyde removal efficiency of 84% even after six cycles, highlighting their potential for indoor air purification and paving the way for the development of efficient photocatalysts.Keywords:graphite-like C3N4/C60composite;robust built-in electric field;charge transfer;photocatalysis;formaldehyde degradation
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2023
·Vol. 49
·期 9
·3747-3764
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IF 3.3
Wei Pingping,Gao Juan,Cai Hanyong,Zheng Lingcheng,Wang Yanfen,Li Yang,He Gang
Z-type 2D/2D C, N, S co-doped TiO 2 /g-C 3 N 4 (DTCN) photocatalysts possessing high catalytic activity were prepared via a simple ultrasonic recombination method. The catalysts’ microscopic morphology, crystal structure, chemical composition, and optical properties were investigated with scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and ultraviolet–visible tests. The photocatalytic activity was also assessed via the degradation of the organic pollutant RhB. The results showed that DTCN could achieve 85.3% degradation of the target pollutant within 60 min, which was 2.47 times (34.5%) and 1.76 times (48.5%) more than TiO 2 and g-C 3 N 4 . The first-order kinetic constants of DTCN reached 0.02838, which was 4.11 and 2.66 times that of TiO 2 and g-C 3 N 4 . Nonmetallic C, N, S (CNS) co-doping effectively improved sunlight utilization of TiO 2 nanosheets through the generation of impurity bands in the forbidden band area. The Z-type heterojunction formed via the coupling of g-C 3 N 4 and CNS–TiO 2 promoted the separation of photoinduced carriers and improved the charge transfer efficiency, boosting the TiO 2 photocatalytic performance. Furthermore, the 2D–2D heterojunction provided a high-speed transport channel for charges. Graphical Abstract Z-type 2D–2D DTCN nanosheet heterojunctions were successfully fabricated. Nonmetallic CNS co-doped effectively improved sunlight utilization of TiO 2 nanosheets through the generating of impurity bands in the forbidden band area. Furthermore, the Z-type heterojunction formed via the coupling of g-C 3 N 4 and CNS–TiO 2 promoted the photoinduced carrier separation and improved the charge transfer efficiency, so boosting the TiO 2 photocatalytic performance.
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CORROSION SCIENCE
·
2023
·
IF 8.3
Jingbao Wang,Jingmao Zhao,Mohammad Tabish,Fan Shi,Baomin Fan,Lijun Peng,Qi Cheng
Filiform corrosion (FFC) challenges the application of Zn-Mg-Al coated steel (ZMA-steel). Herein, a self-healing coating loaded with functionalized mesoporous CeO 2 (mCeO 2 ) was developed to suppress FFC for ZMA-steel in saline media. mCeO 2 of large specific area readily accommodated benzotriazole and immobilized on g-C 3 N 4 generating a nanofiller (BTA@mCeO 2 /g-C 3 N 4 ) for epoxy matrix (EP). Strong barrier of lamellar g-C 3 N 4 , releasing BTA from nanofiller and generating Ce cations accounted for the long-term corrosion-resistance and self-healing effect of BTA@mCeO 2 /g-C 3 N 4 /EP system for ZMA-steel. Through taking full advantages of CeO 2 -based nanofiller, this work may provide an intelligent coating to solve FFC of ZMA-steel.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Juanqin Xue,Long Shi,Peng Wang,Wen Cheng,Mingyang Long,Mengjiao Sheng,Qiang Bi
The coal chemical industry generates large quantities of volatile organic compounds (VOCs) and solid wastes. Within this work, porous semi-coke activated carbon (SAC) was produced from solid waste semi-coke (SC) powder. Through loading high performance photocatalysts onto SAC to efficiently degrade VOCs using synergistic effects of adsorption and photocatalysis, acheiving the resourcefulness of solid waste. The specific surface area of the prepared SAC can reach 619.27 m 2 .g −1 , which was effective against the adsorption of VOCs. An one-step hydrothermal method was used to load a 2D Z-scheme g-C 3 N 4 -Bi 2 WO 6 (NB) photocatalyst on a semi-coke activated carbon. The 50 wt% NB/SAC material degraded formaldehyde, benzene and toluene up to 93.6%, 84.4% and 78.8% in 130 min under visible light irradiation, being 6.09, 4.55 and 4.75 times higher than that of a single photocatalyst, respectively. The capture experiments showed that hydroxyl radicals (⋅OH) and superoxide radicals (⋅O 2 – ) were the active species in the degradation pathway. The material maintained a high degradation performance of 84.8%, 79.6% and 74.0% even after five cycles. In this study, the mechanism of using SAC as a substrate to enhance performance in photocatalytic degradation was described. The results of this study offered new insights into the resourcefulness of solid waste and the effective degradation of VOCs. It also offered a promising theoretical foundation for the exploitation and utilization of high-performance photocatalysts.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2022
·
IF 5.141
Haixian Shi,Dengchong Feng,Hanmei Li,Dingshan Yu,Xudong Chen
Herein, a novel all-organic Z-scheme hydrogen-bonded organic frameworks (HOFs)/g-C 3 N 4 nanosheets (CNNS) heterojunction photocatalyst is synthesized through an in-situ electrostatic method. Characterization and density functional theory studies together verify that the band structures with staggered alignment between HOFs and CNNS can induce a rapid Z-scheme interfacial charge-transfer pathway. Combing the complementary advantages of HOFs and CNNS, the fabricated Z-scheme HOFs/CNNS heterojunction inhibits photoinduced electron-hole recombination and more charge carriers are accumulated to produce highly reactive substances (•O 2 – , •OH and h + ). In addition, the superior hydrophilicity of HOFs can enhance the interaction of HOFs/CNNS heterojunction with water molecules and methyl orange pollutant, which is beneficial to boosting photocatalytic activity . Therefore, in contrast to inactive pure HOFs, the novel Z-scheme HOFs/CNNS heterojunction exhibits a high photocatalytic hydrogen evolution rate of 4450 μmol h -1 g −1 with an apparent quantum efficiency (AQY) of 22 % at 450 nm, which is approximately 11 times higher than that of pure CNNS. Additionally, such heterojunction enables 100 % degradation of methyl orange within 60 min.
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APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2022
·Vol. 128
·期 8
·1-11
·
IF 2.983
Chen Zhangxu,Zhu Danchen,Zhang Lidan
To overcome the intrinsic disadvantages of pristine g-C 3 N 4 and make it reusable, improve the activity of g-C 3 N 4 by making use of the near-infrared region, the magnetic Fe 3 O 4 /β-NaYF 4 /g-C 3 N 4 (FO/UC/CN) heterogeneous materials with high and stable NIR enhanced photocatalytic activity were prepared via a new facile one-step solvothermal synthesis method. It can be revealed that FO/UC/CN can activate UV–visible light under excitation of 980 nm. Compared with pure Fe 3 O 4 , g-C 3 N 4 and Fe 3 O 4 /g-C 3 N 4 , the obtained FO/UC/CN15 heterojunction exhibits good photodegradation rates of 65.56, 21.35, 59.22 and 20.49% for MB, MO, RhB and phenol, respectively. In addition, after four cycles of the photocatalytic degradation test, the photodegradation rates remain 62.14, 20.54, 57.64 and 19.36%, respectively. The results illustrate magnetic FO/UC/CN heterojunction exhibits highly NIR-enhanced photocatalytic activity and excellent stability. This study indicates a promising system to synthesize g-C 3 N 4 -based magnetic photocatalysis for effectively utilizing the NIR and treating industrial wastewater, which can be expected to alleviate the energy crisis and enhance the application of solar energy for dealing with environmental remediation in the future.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Pengyao Guo,Xiaomin Hu
To improve the degradation efficiency of g-C 3 N 4 (CN), transition metal elements (Fe and Co) were doped into CN. A novel Co, Fe co-doped CN (Co/Fe-CN) photocatalysts with small size and irregular flake structure were successfully prepared by thermal polymerization of melamine . Co/Fe-CN has a large specific surface area (55.76 m 2 /g), which provides more adsorption sites and reaction sites for the activation of peroxymonosulfate (PMS). Good visible light response performance (474 nm) and suitable band gap (2.83 eV) ensure that it could be excited by visible light. The active species of • O 2 - , 1 O 2 , • OH and SO 4 •- could be stably produced in Co/Fe-CN/Vis/PMS system with appropriate redox potential . Meanwhile, Co and Fe elements doped in CN also could effectively activate PMS and promote the generation of active species. Besides, the continuous generation of photogenerated electrons promoted the cycling of Co 3+ /Co 2+ and Fe 3+ /Fe 2+ , and further enhanced the degradation efficiency of Co/Fe-CN/Vis/PMS towards Levofloxacin (LVFX). LVFX could be rapidly removed, reaching 92.1% within 50 min under visible light illumination, and the kinetic rate constant of LVFX was 0.0638 min -1 . The quenching experiments verified that the 1 O 2 was the main active species in the reaction process. The cycling experiments revealed that the Co/Fe-CN/Vis/PMS system had favorable stability and applicability. This work provides a simple preparation method to fabricate bimetallic co-doped CN for the enhancement of degradation rate in the Photocatalyst/Vis/PMS system.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2022
·Vol. 23
·期 13
·7381
·
IF 6.208
Daqian Wang,Zhihao Zhang,Shuchuan Xu,Ying Guo,Shifei Kang,Xijiang Chang
Defective functional-group-endowed polymer semiconductors, which have unique photoelectric properties and rapid carrier separation properties, are an emerging type of high-performance photocatalyst for various energy and environmental applications. However, traditional oxidation etching chemical methods struggle to introduce defects or produce special functional group structures gently and controllably, which limits the implementation and application of the defective functional group modification strategy. Here, with the surface carboxyl modification of graphitic carbon nitride (g-C3N4) photocatalyst as an example, we show for the first time the feasibility and precise modification potential of the non-thermal plasma method. In this method, the microwave plasma technique is employed to generate highly active plasma in a combined H2+CO2gas environment. The plasma treatment allows for scalable production of high-quality defective carboxyl group-endowed g-C3N4nanosheets with mesopores. The rapid H2+CO2plasma immersion treatment can precisely tune the electronic and band structures of g-C3N4nanosheets within 10 min. This conjoint approach also promotes charge-carrier separation and accelerates the photocatalyst-catalyzed H2evolution rate from 1.68 mmol h−1g−1(raw g-C3N4) to 8.53 mmol h−1g−1(H2+CO2-pCN) under Xenon lamp irradiation. The apparent quantum yield (AQY) of the H2+CO2-pCN with the presence of 5 wt.% Pt cocatalyst is 4.14% at 450 nm. Combined with density functional theory calculations, we illustrate that the synergistic N vacancy generation and carboxyl species grafting modifies raw g-C3N4materials by introducing ideal defective carboxyl groups into the framework of heptazine ring g-C3N4, leading to significantly optimized electronic structure and active sites for efficient photocatalytic H2evolution. The 5.08-times enhancement in the photocatalytic H2evolution over the as-developed catalysts reveal the potential and maneuverability of the non-thermal plasma method in positioning carboxyl defects and mesoporous morphology. This work presents new understanding about the defect engineering mechanism in g-C3N4semiconductors, and thus paves the way for rational design of effective polymeric photocatalysts through advanced defective functional group engineering techniques evolving CO2as the industrial carrier gas.Keywords:g-C3N4;carboxyl group;defect engineering;non-thermal plasma method;CO2utilization
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lijun Luo,Demei Meng,Lijin He,Xiaoxia Wang,Lihong Xia,Xuejun Pan,Fengzhi Jiang,Hongbin Wang,Jianhui Dai
A new porous C 3 N 4 /reduced graphene oxide/TiO 2 nanobelt catalyst (CRT) was assembled and used to remove 17α-ethinylestradiol (EE2) in the presence of peroxydisulfate (PS) and visible light. The characterization results showed that larger porous graphite carbon nitrides (pg-C 3 N 4 ) covered onto the surface of TiO 2 /reduced graphene oxide (RGO), in which layered RGO was wrapped onto the surface of anatase TiO 2 nanobelt uniformly. The layered RGO in CRT played significant role in separation of electron-hole pairs and nonradical activation. The electron paramagnetic resonance and quenching experiment revealed that h + , 1 O 2 and •O 2 – and direct electron transfer route contributed to complete removal of 6 mg/L EE2 within 6 min only with 0.5 g/L dosage and 1 mM PS. The degradation rate of EE2 in CRT/PS/Vis was 207.51 times than that in photocatalysis. The degradation products were identified by a solid phase extraction pretreatment method combined with ultra-high-performance liquid chromatography-mass spectrometry, and possible degradation pathways were proposed. Moreover, the estrogenic activities can be rapidly eliminated in CRT/PS/Vis process.
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RSC Advances
·
2022
·Vol. 12
·期 24
·15354-15360
·
IF 4.036
Jinghua Liu,Xiong He,Fei Guo,Baosheng Liu,Zijun Sun,Li Zhang,Haixin Chang
Owing to the wide negative potential window (∼1.2 V) along with high specific capacitance (1340 F g−1) in alkaline electrolyte, vanadium nitride (VN) has been served as promising negative supercapacitor electrode material. However, VN is easy to dissolve during cycling process and shows low capacitance retainability. Herein, a hybrid electrode (marked as VN/NCNT/NCN), featuring VN nanoparticles and N-doped carbon nanotube inserted in N-doped carbon nanosheets, has been fabricated with a facile C3N4 self-sacrificing method. The porous structure and high conductive carbon skeleton, as well as the uniform distribution of VN nanoparticles give VN/NCNT/NCN a great amount of active site and fulfill excellent electrochemical performance for VN/NCNT/NCN-based electrode. The as-fabricated hybrid electrode exhibits a maximum specific capacitance of 232.9 F g−1 at 1 A g−1. Moreover, the cycling performance has been greatly improved and the specific capacitance remains 91% after 5000 cycles.
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