Catalysis Science & Technology
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2021
·Vol. 11
·期 22
·7316-7325
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IF 6.119
Chao Zhang,Hailian Bao,Xiaodi Chen,Xingliang Liu,Shiai Xu
Three typical arylamine organic dyes were covalently grafted onto g-C3N4 to form the resulting composites g-C3N4/TPA-CNCHO, g-C3N4/EtPTZ-CNCHO and g-C3N4/EtCz-CNCHO. They were synthesized by 1,3-dipolar cycloaddition with (E)-3-(4-(diphenylamino)phenyl)-2-formylacrylonitrile (TPA-CNCHO), (E)-3-(10-ethyl-10H-phenothiazine-3-yl)-2-formylacrylonitrile (EtPTZ-CNCHO), or (E)-3-(9-ethyl-9H-carbazol-3-yl)-2-formylacrylonitrile (EtCz-CNCHO) dyes. The experimental results show that arylamine organic dye moieties were successfully attached to g-C3N4, and this attachment can efficiently extend the light absorption area of pure g-C3N4 from approximately 460 nm to more than 650 nm. The obtained g-C3N4/TPA-CNCHO, g-C3N4/EtPTZ-CNCHO and g-C3N4/EtCz-CNCHO samples showed enhanced H2 evolution activity with photocatalytic H2 production rates that were approximately 105-, 93- and 67-fold that of pure g-C3N4. By combining the comprehensive analysis from experiments and density functional theory (DFT) calculations, a possible mechanism can be drawn: the introduced arylamine organic dye fragments attached to the surface of the g-C3N4 may acquire more light irradiation, and effective photoexcited carrier transfer from the donor dye fragments to the acceptor g-C3N4 could be achieved through the IFCT process. The results confirm that the covalent azomethine ylide bonds formed via 1,3-dipolar cycloaddition between the g-C3N4 and organic dye can truly enhance the photocatalytic H2 evolution rate of the obtained samples. It is believed that this kind of modification can be an effective strategy for achieving other kinds of functional organic dyes grafted onto g-C3N4 with highly efficient photocatalytic H2 activity.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Xinfei Zhang,Xiaobo Jia,Jianhui Zhan,Bin Han,Nan Zhang,Honghao Xie,Feilong Li,Yuan Zhang
The activation of peroxydisulfate (PDS) by g-C 3 N 4 -based catalysts has captured considerable interest; however, the oxidation prowess falls short of expectations, and the inherent processes remain enigmatic. Herein, a novel C C engineered g-C 3 N 4 (CCN) was successfully developed via a one-step thermal polymerization method for the activation of PDS. Our findings revealed that the CCN/PDS system selectively degraded various organic contaminants, operated effectively across a wide pH range (3−9), and maintained high performance in the presence of common water impurities. Experiments and theoretical calculations indicated that the electron transfer process (ETP) was the primary mechanism for phenol degradation. The introduction of C C led to charge redistribution and improved conductivity in g-C 3 N 4 . This enhancement strengthened PDS adsorption at electron-deficient carbon sites and bolstered electron transfer between PDS and organic contaminants. Moreover, a nonradical pathway predicated on ETP emerged when phenol, PDS, and CCN were present, propelled by differences in molecular orbital energies. This study not only deepens our understanding of PDS activation through the ETP but also introduces a novel strategy for the removal of organic contaminants from water.
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Functional Materials Letters
·
2021
·
IF 2.17
Dan Yang,Lei Zhao,Xueting Feng,Lili Ma,Hanming Ding
As a potential nonmetal activator of peroxymonosulfate (PMS), g -C 3 N 4 becomes a hot material owing to its superior chemical and physical properties. Nevertheless, pristine g -C 3 N 4 is unsatisfactory for PMS activation because of its limited photo-generated charge separation and low specific surface area. Herein, a porous sulfur-doped g -C 3 N 4 (S-doped g -C 3 N 4 ) has been prepared through a one-step calcination route without a template. The in - situ doping of sulfur element and the formation of porous morphology have been confirmed via various characterization methods. The catalytic activity of porous S-doped g -C 3 N 4 is approximately 6.2-fold higher than that of the pristine g -C 3 N 4 on rhodamine B (RhB) decomposition in aid of the photo-assisted PMS activation. The superior catalytic activity and high stability of the porous S-doped g -C 3 N 4 catalyst in a wide pH range are attributed to its higher specific surface area, enriched active sites, efficient photo-induced charge separation, and increased visible-light utilization. Meantime, a synergistic effect between the PMS activation process and the photocatalytic process is conducive to produce abundant radicals for the RhB degradation. This study offers new insight into further developing highly efficient nonmetal heterogeneous catalysts for wastewater treatment.
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CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Kangyue Qiao,Songyao Du,Yue Wang,Tongxin Xiao,Guodong Hao,Chao Sui,Yihan Yan
To address the severe Cr(VI) contamination in industrial wastewater, an NH 2 -MIL-101(Fe)/g-C 3 N 4 type-II heterojunction photocatalyst was synthesized via a solvothermal one-pot method. Structural characterization using XRD, SEM, XPS, and BET confirmed successful composite formation with high specific surface area and favorable interfacial contact. Photocatalytic experiments revealed that under conditions of pH = 2, a catalyst dosage of 20 mg, and an initial concentration of 10 mg/L, NM-101(Fe)/0.2CN achieved a 99.5 % reduction efficiency within 80 min. Its reaction rate constant was 3.6 times higher than that of NM-101(Fe) used alone. This study provides new insights for developing highly efficient MOF/polymer composite photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yang Wan,Jiejing Liu,Huijie Wang,Xianghai Song,Weiqiang Zhou,Xin Liu,Jisheng Zhang,Yangyang Yang,Xiaojie Zhang,Binrong Li,Pengwei Huo
The inherent chemical stability of polyethylene terephthalate (PET) poses significant challenges for its natural degradation, leading to severe environmental accumulation. This study presents an innovative Co 1-x S/g-C 3 N 4 S-scheme heterojunction photocatalyst designed to enhance interfacial electron transfer and promote cobalt redox cycling for efficient peroxymonosulfate (PMS) activation, achieving effective PET degradation. Experimental results demonstrated that the optimized photocatalysis/PMS system achieved a 6.3-fold higher PET degradation efficiency compared to the photocatalysis system alone. The optimized system (30 % Co 1-x S/g-C 3 N 4 with 4 mM PMS and 1 mL H 2 O 2 under irradiation) achieved a remarkable PET degradation efficiency of 80.91 ± 1.30 %. Density functional theory (DFT) calculations unveiled the interfacial electronic structure of Co 1-x S/g-C 3 N 4 , demonstrating hole accumulation on g-C 3 N 4 and electron localization on Co 1-x S. Systematic comparative experiments confirmed the cooperative roles of heterojunction architecture, electron transfer dynamics, cobalt active sites, and H 2 O 2 in PMS activation. Degradation intermediates were identified by gas chromatography spectrometry (GC) and liquid chromatography-mass spectrometry (LC-MS), while electron spin resonance (ESR) and radical trapping experiments established SO 4 •− as the predominant reactive species. This study provides a new approach for the construction of S-scheme heterojunction photocatalysts, the activation by PMS, and the treatment of PET plastic in water.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Fan Yang,Jingrui Duan,Yan Chen,Huiying Meng,Wanying Zhang,Ruiting Li,Wen Luo,Yang Wu,Yong Wang,Peng Zhang,Yifan Zhang
In this study, a bimetallic Pt-Ni alloy catalyst, designated PN 0.5 /VCN 1 , was synthesized with the objective of enhancing the photocatalytic hydrogen evolution performance. Photoelectrochemical characterizations confirm that PN 0.5 /VCN 1 significantly improves light absorption, charge transfer efficiency, and proton adsorption/activation capability, leading to enhanced photocatalytic performance. The results demonstrate that under optimized conditions (300 W Xe lamp, lactic acid as the hole scavenger) PN 0.5 /VCN 1 achieves a hydrogen evolution rate of 8.77 mmol·g -1 ·h -1 (4079 times higher than pure CN) with remarkable stability. And stability tests over four cycles (20 h total) indicate no significant activity loss. This enhancement is attributed to the localized surface plasmon resonance (LSPR) effect of the alloy, interfacial electron redistribution, and synergistic metal-defect interactions. The modification strategy proposed in this study offers a rational and cost-effective approach for efficient photogenerated charge separation and accelerated proton reduction kinetics, providing a competitive advantage in the market. This work provides a foundation for designing high-performance photocatalytic systems.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Mengying Xu,Jingyan Zheng,Pier-Luc Tremblay,Xiangyang Jiang,Chun He,Yujie Wang,Muhammad Babur Joya,Tian Zhang
Amid the pursuit of renewable energy, photocatalytic H 2 evolution (PHE) and biosynthetic processes gained attention. Bulk g-C 3 N 4 (CN) was calcined under the atmosphere and various gases (air, CO 2 , N 2 , and Ar) to achieve ultra-thin nanosheets. Using greenhouse gas CO 2 for the calcination (CN–CO 2 ) results in a greater PHE rate than in the atmosphere and air, similar to inert gases N 2 and Ar. Under visible light, CN–CO 2 produced H 2 2.6 times faster than CN. Therefore, CN–CO 2 was chosen to promote polyhydroxybutyrate (PHB) production by Cupriavidus necator H16 in hybrid photosynthetic system. The heterotrophic PHB production was increased to 9.14 g/L, which was 1.9 times higher than without the photocatalyst (4.93 g/L), and 1.1 times more than with CN (8.11 g/L). The autotrophic PHB production was also enhanced by adding CN–CO 2 . In summary, the dual benefits of PHE and biological stimulation were achieved by calcining g-C 3 N 4 in CO 2 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhenhua Niu,Wenjia Luo,Peng Mu,Jian Li
Membrane separation technology has received widespread attention in the field of gas separation because of small footprint, convenient operation and low energy consumption. However, membranes separation are subject to a trade-off between permeance (or permeability) and selectivity. Herein, a novel kind of supported oinic liquid membrane (SILM) was constructed by nanoconfined 1-ethyl-3-methylimidazole acetate ([EMIm][AcO], IL) in the two-dimentional (2D) channels of the g-C 3 N 4 laminated membrane for CO 2 /N 2 and CO 2 /CH 4 separation. Due to the nanoconfinement of ILs in 2D g-C 3 N 4 laminated membrane and the appropriate nanofluidic channels constructed by the g-C 3 N 4 nanosheets, the as-prepared g-C 3 N 4 SILM possesses outstanding permeance and selectivity for CO 2 in separation of CO 2 /N 2 and CO 2 /CH 4 . The experimental result shows that g-C 3 N 4 SILM possesses maximum CO 2 permeance of 992.97 GPU in separation of CO 2 /N 2 and 1160.52 GPU in separation of CO 2 /CH 4 under 1 bar, 25℃. Meanwhile the resultant g-C 3 N 4 SILM shows excellent selectivity for CO 2 /N 2 (52.49) and CO 2 /CH 4 (48.41) respectively. Moreover, the resulted g-C 3 N 4 SILM displays excellent thermal stability and durability. After 60 h test, its separation performance has no obvious change. The findings of our study demonstrate that nanoconfined the IL into the 2D g-C 3 N 4 is a novel strategy for the preparation of high-performance supported liquid membrane for the separation of CO 2 /N 2 and CO 2 /CH 4 .
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 26
·13299-13310
·
IF 11.301
Cheng-Qun Xu,Wei-De Zhang,Kenzo Deguchi,Shinobu Ohki,Tadashi Shimizu,Renzhi Ma,Takayoshi Sasaki
A facile “one-pot” method to improve the utilization of visible light using organic chemistry protocols is reported. The incorporation of acetylacetone (acac) into the conjugated polymer matrix g-C3N4 derived from urea (UCN) can tune the electronic structure effectively. As a result, the modified g-C3N4 showed a narrowed band gap and enhanced charge carrier migration and separation. Meanwhile, the high utilization ratio of visible light leads to efficient photocatalytic hydrogen evolution, and an apparent quantum efficiency (AQE) as high as 18.8% at 450 nm is achieved, exceeding that of most of the previously reported doped g-C3N4 photocatalysts. Furthermore, density functional theory (DFT) calculations certify the proposed structure of g-C3N4 by incorporation of acetylacetone and explain the enhanced ability to harvest photons due to the introduction of an electron push–pull system into the CN network. In addition, the incorporation of acac into g-C3N4 is also found to be applicable to other precursors (dicyandiamide and thiourea) through similar synthetic routes. Optical absorption under visible light is extended similarly, highlighting the universality of the current strategy. The work provides a route of organic chemistry to design and synthesize functional g-C3N4 with high photocatalytic performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Yingying Wang,Hanlin Huang,Zhenzhen Zhang,Cong Wang,Yuying Yang,Qi Li,Dongsheng Xu
Solar-energy-driven CO 2 conversion into value-added chemical fuels holds great potential renewable energy generation. However, most of the photocatalysts facilitate a two-electron reduction process producing CO, hard for the eight-electron CH 4 production pathways which can stockpile more solar energy for further utilization. Herein, we developed an in situ assembly strategy to fabricate the lead-free perovskite Cs 2 AgBiBr 6 @g-C 3 N 4 Z-scheme system in toluene and the Cs 2 AgBiBr 6 @g-C 3 N 4 type-II heterojunction structure in CH 2 Cl 2 . By combining the reducing ability of the conduction band of g-C 3 N 4 and the oxidizing ability of the valence band of Cs 2 AgBiBr 6 perovskite, this Z-scheme system exhibits superior CH 4 production in photocatalytic CO 2 reduction, in contrast to the high CO selectivity for the heterojunction photocatalysts, which is 10-fold and 16-fold higher than that of pure g-C 3 N 4 and pure CABB, respectively. The stability (four consecutive photocatalytic cycles in solvent methanol as sacrificial reagent without obvious decrease of efficiency) and the mechanism (the prominent activity and the high CH 4 production selectivity boosted by Z-scheme system) were demonstrated. In this work, the first report for constructing lead-free halide perovskite Z-scheme and type-II photocatalytic systems for the regulation products selectivity of CO 2 reduction reaction provides a promising strategy for the fabrication other types of inorganic/organic heterojunction systems.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Hongmei Chen,Yanyun Fan,Hongyan Xu,Danfeng Cui,Chenyang Xue,Wendong Zhang
Herein, a microwave hydrothermal method was developed for constructing g-C 3 N 4 nanosheets. The specific surface area of the photocatalyst using this method was larger than the bulk carbon nitride . In addition, this method yields g-C 3 N 4 with a lower electron-hole recombination rate and faster interface charge transport. Particularly, the conduction band shifts to a more negative position, leading to better reducibility. As expected, the g-C 3 N 4 nanosheets had excellent activity in hydrogen evolution (over 10 times that of the bulk carbon nitride). Additionally, the photocatalyst prepared using this method had good stability in the hydrogen evolution reaction. This work proposes a new, universal, facile and green technique route for preparing g-C 3 N 4 nanosheets.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Fei Guo,Dongsheng Li,Rui Ding,Jiaming Gao,Xuehua Ruan,Xiaobin Jiang,Gaohong He,Wu Xiao
Two-dimensional nanomaterials have the characteristics of high aspect ratio and high space utilization, which has huge potential advantages in gas separation. In this work, g-C 3 N 4 two-dimensional nanosheets with sieving pore structure were selected as templates and combined with ZIF-90 to construct a 0-dimensional/2-dimensional composite material ZIF-90@C 3 N 4 (ZCN). The complete two-dimensional g-C 3 N 4 nanosheets were stripped under acid etching conditions at 25 °C. ZIF-90 was distributed in an orderly manner on the two-dimensional nanosheets, and the nanosheets were spread out due to the growth of ZIF-90 to provide more free volume. The gas permeation experiment proved that the ZCN has a better CO 2 /N 2 separation performance. The ZCN/Pebax mixed matrix membrane (MMM) with the optimized 8.0 wt% ZCN loading showed an improved CO 2 permeability of 110.5 Barrer and a CO 2 /N 2 selectivity of 84.4, surpassing the Robeson upper bound (2008). The results demonstrated that the designed composite filler with 2D nanosheets is an effective strategy to enhance gas separation performance of MMMs and verified the application potential in gas purification industry.
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