CELLULOSE
·
2022
·Vol. 29
·期 6
·3389-3406
·
IF 6.123
Lang Daning,Xu Xia,Wu Ronglan,Wang Wei,Shi Ming,Jia Ke,Chen Shifei,Wang Jide
A cellulosic material has been synthesized that could efficiently and selectively adsorb organic and inorganic contaminants from aqueous solutions without interference from competing adsorption sites. Cellulose-graft-tetraethylenepentamine molecular imprinted polymer (C-TEPA-MIP) was synthesized by using 4-nitrophenol (4-NP) as the template. The C-TEPA-MIP adsorbent could adsorb 4-NP and Cr(VI) simultaneously and selectively, without being affected by the competitive adsorption sites of each of these pollutants. The adsorption of 4-NP was predominantly due to the imprinted sites of 4-NP in C-TEPA-MIP that were located inside of the adsorbent, whereas that of Cr(VI) was primarily due to the amine groups of TEPA found on the surface of the adsorbent. Compared with the non-imprint polymer synthesized without the template, C-TEPA-MIP showed higher selectivity for both 4-NP and Cr(VI) in unitary and binary systems. In addition, C-TEPA-MIP exhibited good stability and recyclability for 4-NP, which makes it a promising candidate material for applications concerning wastewater treatment. Graphical abstract
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ACS Omega
·
2019
·
IF 2.584
Chao Zhang,Jiandong Liu,Xiayun Huang,Daoyong Chen,Shiai Xu
Graphene-like g-C3N4 nanosheets (NSs) have been successfully synthesized with a modified polymerization process of melamine by cocondensation with volatile salts. Volatile ammonium salts such as urea–NH4Cl/(NH4)2SO4/(NH4)3PO4 were added with melamine to modulate the thermodynamic process during polymerization and optimize the structure formation in situ. The surface area, surface structure, and surface charge state of the obtained g-C3N4 NSs could be controlled by simply adjusting the mass ratio of the melamine/volatile ammonium salt. As a consequence, the g-C3N4 NSs exhibited much higher activity than bulk g-C3N4 for the photocatalytic degradation of target pollutants (rhodamine B, methylene blue, and methyl orange), and it also exhibited greater hydrogen evolution under visible light irradiation with an optimal melamine/volatile ammonium salt ratio. The as-prepared g-C3N4 NSs with melamine–urea–NH4Cl showed the highest visible light photocatalytic H2 production activity of 1853.8 μmol·h–1·g–1, which is 9.4 times higher than that of bulk g-C3N4 from melamine. The present study reveals that the synergistic effect of the enhanced surface area, surface structure, and surface charge state is the key for the enhancement of photocatalytic degradation and hydrogen evolution, which could be controlled by the proposed strategy. The result is a good explanation for the hypothesis that adding properly selected monomers can truly regulate the polymerization process of melamine, which is beneficial for obtaining g-C3N4 NSs without molecular self-assembly. Considering the inexpensive feedstocks used, a simple synthetic controlling method provides an opportunity for the rational design and synthesis, making it decidedly appealing for large-scale production of highly photocatalytic, visible-sensitizable, metal-free g-C3N4 photocatalysts.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Mingyuan Guo,Yongning Ma,Zhanqing Liu,Donghua Wang,Yuhao Yang,Xiaolong Li,Enzhou Liu
Halogen doping is an effective approach to regulate the electronic structure and improve photocatalytic properties of g-C 3 N 4 . Here, a salt-assisted approach was employed to prepare layered porous halogen-doped g-C 3 N 4 . The effects of halogen electronegativity and pore morphology were discussed. Highly electronegative F-doped g-C 3 N 4 with smaller pore size and higher surface area displayed the enhanced absorption property on reactants. The H 2 production rate decreased and the RhB degradation significantly increased with increasing the electronegativity of layered porous g-C 3 N 4 , which was significantly different from the conventional halogen-doped g-C 3 N 4 prepared with halogenated acid and monolayer g-C 3 N 4 . The decreased H 2 evolution can be ascribed to the strong adsorption property, and the strong interactions between halide ions and H + were difficult to be disassociated. Additionally, the RhB degradation performance of halogen-doped g-C 3 N 4 significantly increased with increasing the electronegativity. The most active species that dominated the RhB degradation of F-doped g-C 3 N 4 are leaved holes (h + ), which are totally different from that of the pristine g-C 3 N 4 and Cl/Br-doped g-C 3 N 4 (superoxide radicals,·O 2 – ). This work helps us to well understand the role and importance of electronegativity and pore morphology on the H 2 generation and RhB degradation properties of layered porous g-C 3 N 4 .
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JOURNAL OF CHROMATOGRAPHY A
·
2018
·
IF 3.716
Ning Zhang,Chuanhui Huang,Ping Tong,Zunmei Feng,Xiaoping Wu,Lan Zhang
Volatile polycyclic aromatic hydrocarbons (PAHs) in water and soil are associated with status in the human body. Development of simple, efficient detection method is challenging due to the coating could be attacked by the abundance of water in the direct-immersion solid-phase microextraction. The stability of coating is essential to the analysis results. In this paper, a stable Ni-Zn MOF/g-C 3 N 4 (MG NFs) nanoflowers with cavity traps structure was firstly reported and acted as solid-phase microextraction (SPME) adsorbent for PAHs. Markedly enhanced moisture and acid stability of the MG NFs was obtained through the doping the hydrophobic graphitic carbon nitride (g-C 3 N 4 ) and metal ions into metal organic frameworks (MOFs). The aperture environment and ambient environment of MG NFs were changed by the doping of the Ni and the g-C 3 N 4, respectively. The moisture and acid stability of MG NFs were prominently increased under the dual protection. Compared to commonly used commercial coatings, the MG NFs own large surface area, unique nanoflowers structure and numerous open metal sites on the nanosheets, which demonstrated significant extraction superiority for PAHs. The MG NFs coated fiber was used for the SPME preconcentration of PAHs and couped with GC–MS for detecting PAHs. It presented low detection limits (0.1–3.0 ng L −1 ), wide linearity (0.3–5000.0 ng L −1 ) and good linearity (the correlation coefficient >0.9951). The inter-day and intra-day relative standard deviation (RSD) (n = 3) for three replicate extractions using one fiber was 3.8%–9.1%, and 3.5%–9.2%, respectively. The fiber-to-fiber reproducibility (n = 3) was 4.2–11.8%. The coupling method was successfully applied in the analysis of real water and soil samples with satisfactory recoveries of 82.9–109.2%, 84.2–106.4%, and the corresponding RSDs were 2.4–11.3%, 3.6–10.8%, respectively. The results indicated the effectiveness of NG NFs coated fiber in further practical application.
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Qiangbin Yang,Jibin An,Zhonghao Xu,Shuting Liang,Honghong Wang
Due to the carcinogenicity of atrazine, the effective removal of atrazine in water and soil has become the focus of attention. In the paper, the advanced oxidation technology based on sulfate radicals ( S O 4 · - ), which the visible light catalysis and nanocatalyst Co 3 O 4 /g-C 3 N 4 synergistically catalyzed to yield S O 4 · - , was constructed to efficiently degrade and remove atrazine. The Co 3 O 4 /g-C 3 N 4 was prepared through a simple solvothermal method, and its microstructure and composition were characterized by SEM and XRD. A series of experiments were carried out to degrade atrazine by Co 3 O 4 /g-C 3 N 4 activation of peroxymonosulfate under visible light, which revealed that the degradation efficiency reached to 78.5 percent in 35 min, CO 3 2− had a significant inhibitory effect on the degradation of atrazine in coexisting ions of NO 3 -, SO 4 2− , Cl- and CO 3 2− , the e -, ⋅OH, and S O 4 · - were mainly active species. Combined with density function theory calculations of Co 3 O 4 /g-C 3 N 4 , the high-efficiency degradation of atrazine was due to the synergetic enhancement between photocatalysis and Co 3 O 4 /g-C 3 N 4 catalyst in the constructed catalytic system.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Chunyan Su,Yazhou Zhou,Lili Zhang,Xiaohui Yu,Shuai Gao,Xiujuan Sun,Chao Cheng,Qinqin Liu,Juan Yang
Graphitic carbon nitride (g-C 3 N 4 ) has been demonstrated to be a rising star among semiconductor materials for photocatalytic hydrogen (H 2 ) production. However, pristine g-C 3 N 4 usually suffers from inferior activity due to the inadequate visible light harvesting capacity and quick charge recombination. Herein, porous P doped g-C 3 N 4 nanosheets (PCNNSs) were fabricated via a simple thermal condensation of adenosine phosphate and urea followed by thermal exfoliation method. The synergetic effect of the porous structure and P dopant can provide abundant active sites for the photocatalytic reaction, which can enhance light absorption range extending from 450 nm to 700 nm attributed to the n→π* electronic transition, and improve hydrophilicity for easier water molecules adsorption via introducing hydroxyl groups. Furthermore, impurity level caused by the P dopant would change the excitation process and accelerate the charge separation efficiency. Therefore, the PCNNSs exhibited significantly elevated photocatalytic H 2 generation performance (9523.7 μmolg -1 h -1 ) under visible-light (λ > 420 nm) irradiation, which was about 20 times that of unmodified g-C 3 N 4 (458 μmol -1 h -1 ).
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Chao Wan,Liu Zhou,Lin Sun,Lixin Xu,Dang-guo Cheng,Fengqiu Chen,Xiaoli Zhan,Yongrong Yang
Two dimensional graphitic carbon nitride nanosheets (2D CNNs), as novel types of emerging materials, have aroused considerable research enthusiasm in recent years. Herein, we describe for the first time a new application of 2D CNNs as an ideal scaffold for synthesizing AgPd/2D CNNs through a facile one-step reduction method and further utilized it as catalysts toward photocatalytic hydrogen generation from FA under visible light (λ > 400 nm). Benefiting from plasmonic and Mott-Schottky, alloying effects, as well as the unique 2D nanosheets structure with a high surface area, the resultant Ag 0.1 Pd 0.9 /2D CNNs affords superior performance under visible light, including 100% H 2 selectivity, 100% conversion, cycle performance, hydrogen evolution rate of 231.6 mmol h −1 and the corresponding TOF value of 2936.8 h −1 , which is 1.87 times and 3.5-fold higher than that of Ag 0.1 Pd 0.9 /2D CNNs under no light (1573.5 h −1 ) and that of Ag 0.1 Pd 0.9 /CN (837.2 h −1 ) under visible light, respectively, even better than most of the noble metal heterogeneous catalysts. This study not only throws light on modulating the structure of g-C 3 N 4 to enhance the photocatalytic activity toward hydrogen evolution reaction but also offers a versatile method for developing high-performance photocatalyst for hydrogen economy and other applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Fang Wang,Yun Liao,Tingting Li,Liangshu Xia
Uranium (VI) removal and recovery from wastewater is crucial for sustainable development of nuclear energy and environmental remediation. Among various techniques, the photocatalytic reducing uranium (VI) to immobile uranium (IV) has been regarded as one of the most effective strategies. As a result, the design and fabrication of photocatalysts have attracted extensive attention. In this study, g-C 3 N 4 decorated dendritic fibrous nano-silica was fabricated first and then coupled with CdS. The fibrous photocatalyst showed high surface area and extended visible light absorption. More importantly, it exhibited a satisfying performance for the photocatalytic reduction of uranium (VI) under air atmosphere with solar irradiation. The SEM images and XPS spectrum confirmed that uranium (VI) was indeed photo-reduced to uranium (IV). Meanwhile, quenching experiments showed that O 2− played a key role in uranium (VI) reduction.
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高影响因子
CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2025
·
IF 10.3
Weixia Wang,Yongji Zhang,Fei Zhao,Libo Wang,Fanpeng Meng,Shuchao Qin,Jinsheng Zhao
Carrier recombination in polymer photocatalysts involves both undissociated exciton decay and charge recombination, which are the main obstacles limiting their photocatalytic activity. Achieving efficient charge generation and separation in a polymer system is a fundamental strategy for the potential success of solar energy conversion to hydrogen, but it remains a huge challenge. In this study, we propose an innovative intermolecular π–π stacking strategy to construct a π-delocalized all-polymer S-scheme heterojunction for photocatalytic hydrogen evolution. Two conjugated porous polymers (CPPs)—PyB, composed of benzo[1,2-b:4,5-b′]dithiophene (BDT) and pyrene units, and PhB, composed of BDT and benzene—were synthesized and integrated with CN nanosheets. The highly planar and π-extended structure of PyB facilitated strong interfacial π–π stacking with CN, forming an extended π-delocalized network that enhanced the internal electric field (IEF), improved charge separation, and boosted visible-light absorption. As a result, the optimized PyB/CN-20 composite achieved a remarkable hydrogen evolution rate (HER) of 23.84 mmol⋅h −1 ⋅g −1 under visible light, approximately 287 times higher than that of pristine CN. This work underscores the critical role of polymer planarity and π-conjugation in heterojunction efficiency, and provides new insights into the rational design of π-delocalized S-scheme systems and establishes a general strategy for developing highly efficient, metal-free photocatalysts by leveraging molecular-level structural control.
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高影响因子
CARBON
·
2025
·
IF 11.6
Junzhu Yang,Junchen Liu,Yi Zhang,Wei Pei,Qi Xia,Sanyang Han,Yuan Lu
Efficient regeneration of the coenzymes NADH and NADPH is crucial for sustaining biocatalytic processes, particularly in driving the biocatalysis reaction. In this study, the photocatalytic properties of alkali-doped graphitic carbon nitrates were explored to achieve efficient NAD(P)H regeneration. g-C 3 N 4 doped with potassium (KOH), sodium (NaOH), and calcium (Ca(OH) 2 ) was synthesized and characterized, showing significant enhancements in light absorption, charge separation, and photogenerated electron transport. Among the synthesized photocatalysts, KOH-doped g-C 3 N 4 (KCN) exhibited the best photocatalytic performance, regenerating 95 % NADH and 92 % NADPH within 30 min. This result compares favorably with those reported in previous studies. Based on this superior performance, K-0.2 was further applied to the in vitro CO 2 reduction to formate as a proof of concept. To clarify the mechanistic insights of the improved photocatalytic performance of KCN, the chemical model of g-C 3 N 4 and KCN was established, and DFT calculations were performed to reveal the electronic structure modifications responsible for the enhanced photocatalytic activity. Furthermore, to expand the light utilization capability of the system, upconversion nanoparticles (UCNPs) were incorporated into the system to utilize near-infrared light (980 nm), which successfully achieved NADH regeneration under near-infrared excitation and extended the light absorption range of the photocatalytic system. Overall, this study demonstrated that alkali-doped g-C 3 N 4 offered a highly efficient platform for NAD(P)H regeneration, and the integration of UCNPs further enriched the coenzyme regeneration scenario, suggesting a promising strategy for advancing sustainable coenzyme regeneration technologies.
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高影响因子
Journal of Water Process Engineering
·
2025
·
IF 6.7
Yongxiu Song,Shifei Kang,Mingzhu Huang,Youduo Wu,Yuyang Lv,Chuang Xue
The generation of hydroperoxyl radical ( OOH) radicals is an important issue and has significant value in the highly selective removal of pollutants in complex water environment. However, the metal active center catalysts frequently encounter the limited surface site type and energy level mismatch, making it difficult to maintain a stable supply of OOH. Therefore, a novel photocatalytic self-Fenton system based on metal-free g-C 3 N 4 /chitosan (g-C 3 N 4 /CS) catalyst was developed to achieve excellent efficiency in the removal of tetracycline, bisphenol A and 2,4-dichlorophenol across a broad pH range (3.14–9.04), superior the conventional Fenton system which only works at pH 3–5. Chitosan modification enhanced the charge separation and transfer efficiency of the S-scheme charge transfer pathway, optimized the formation of OOH, O 2 − , h + , enhancing the selective generation and stable supply of OOH radical with a high ratio of 33 %, led to the efficiency removal of pollutants. Further mechanistic analysis demonstrated the unique dominance of the desired OOH radicals. g-C 3 N 4 /CS catalyst exhibited excellent stability and reusability by the cycling experiments, suggesting durable OOH supplying. This work offers novel insights into g-C 3 N 4 based metal-free catalyst with special radical features through chitosan modification, demonstrating the potential for industrial applications of OOH dominated g-C 3 N 4 /CS self-Fenton system in wastewater treatment.
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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Tingan Yao,Guohui Dong,Ying Gao,Dongfeng Sun,Hehua Zeng
This study successfully constructed a g-C₃N₄/FeOOH S-scheme heterojunction photocatalyst with lotus-leaf structural effects, addressing the challenges of insufficient oxygen and water adsorption sites and high photocurrent recombination rates in g-C₃N₄ photocatalysts. The optimized photocatalyst exhibits outstanding performance, generating hydroxyl radicals via dual pathways under visible light (generation rate: 2.8 μmol/(L·min)). The lotus-leaf effect in the composite was confirmed through morphology analysis, static water contact angle measurements, and oxygen adsorption/desorption experiments, demonstrating an 18.9-fold enhancement in oxygen capacity. In situ XPS, built-in electric field intensity measurements, and theoretical calculations confirm that the built-in electric field at the interface, directed from g-C₃N₄ toward FeOOH, drives an S-scheme charge transport pathway. This not only achieves efficient spatial separation of photogenerated carriers but also uniquely preserves the system's strongest redox capability, significantly enhancing photocatalytic efficiency. Furthermore, in situ infrared spectroscopy and electron paramagnetic resonance studies confirm the composite material's dual-channel mechanism for hydroxyl radical generation via oxygen reduction and water oxidation. This work provides robust experimental and theoretical foundations for understanding and designing S-scheme heterojunctions for dual-channel hydroxyl radical generation in photocatalysis.
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