ENVIRONMENTAL POLLUTION
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2024
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IF 7.6
Fang Yang,Lihe Zhu,Zushen Xu,Yongwei Han,Xue Lin,Junyou Shi,Zhong Sun,Xixin Duan
Sulfamethoxazole (SMX) is one of major antibiotic contaminants in current aqueous environment. In this paper, waste loofah and melamine were co-carbonized to prepare biochar-doped g-C 3 N 4 (CCN) by a one-pot method and then combined with Co 2 PMo 11 VO 40 (CoPMoV) using a binder to obtain the novel polyoxometalates (POMs) photocatalytic composites (CCN/CoPMoV). The incorporation of CoPMoV dramatically reduced the photogenerated carrier recombination and led to a small band gap. Under visible light, the synergetic activation from biochar, g-C 3 N 4 and POMs can remove 98.5% of SMX ( k = 0.215 min −1 ) in the peroxymonosulfate (PMS) system within 20 min and keep its high stability with the degradation of 88.9% after five cycles. Multi-active sites from CCN/CoPMoV are contributed to develop the most active species of SO 4 − ∙ , ·OH, 1 O 2 , and h + . The validity in the degradation of SMX makes CCN/CoPMoV a promising and potential material for the removal of aqueous pollutants in the future.
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高影响因子
CHEMISTRY OF MATERIALS
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2024
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IF 7.2
Shichao Xu,Haifeng Wu,Yuanxi Liu,Zhen-Gang Wang
Recreating the intricate enzymatic sites within in artificial materials poses a significant challenge due to the complex folding characteristics of enzymes. In this study, we designed a supramolecular catalyst by assembling intramolecularly folding G-quadruplex DNA with Fmoc-amino acid aggregates and Cu2+. This supramolecular material possesses active sites and catalytic functions that rely on copper clusters, mirroring the functionality of catechol oxidase. Experimental and theoretical simulations showed that Fmoc-amino acids interact with G-quadruplex DNA through groove binding, facilitating Cu2+ coordination to both components, thereby enhancing the oxidative catalysis of Cu2+ upon assembly. Our catalyst exhibited excellent tolerance to high temperature, varying ionic strength, and extended room-temperature storage in aqueous solutions. Moreover, our supramolecular complex effectively catalyzed the degradation of doxorubicin, a drug with a high affinity for the DNA component, demonstrating its potential for removing pharmacological pollutants. Additionally, by integrating a photoisomerizable azobenzene derivative as a ligand to the G-quadruplex DNA, we can switch the activity of the enzyme-mimetic catalyst between on and off states by adjusting the irradiation wavelength. This multicomponent approach offers a promising avenue for the design and engineering of active, adaptable supramolecular catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jiangli Sun,Huizhong Wu,Chunhong Fu,Chaohui Zhang,Zhongzheng Hu,Minghua Zhou
A novel photoelectrocatalytic (PEC) system consisting of S-scheme MgO/g-C 3 N 4 photoanode and modified carbon felt (MCF) cathode was designed for efficient degradation of tetracycline , in which photoanode had both efficient photocatalytic performance and activation of H 2 O 2 produced by the MCF cathode. After 30 min of LED irradiation, the PEC system could completely remove tetracycline at cathodic bias of −0.5 V (vs. Ag/AgCl), and the degradation rate constants were 5.3 and 1.5 times that of electrocatalysis and photocatalysis . The charge transfer mechanism of S-scheme MgO/g-C 3 N 4 was verified by experimental studies and DFT calculations. Mg-N coordination was the key to activate H 2 O 2 to produce singlet oxygen ( 1 O 2 ) and hydroxyl radicals ( • OH). The PEC system had excellent degradation performance at pH ranges 4–10, which solved the bottleneck that Fenton system is effective at narrow pH range. This study provides new ideas for preparation of bifunctional photoanodes and new insights into the PEC process.
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CHEMICAL ENGINEERING JOURNAL
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2024
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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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Arabian Journal of Chemistry
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2024
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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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VACUUM
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2024
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IF 3.8
Ying Du,Juan Li,Xinqi Ma,Quanhui Guo
With the development of economy, overuse of antibiotics has been seen as a huge threat to human health. Photocatalytic degradation is an effective method for resolving this problem at present. The method of combining plasmon resonance effect and Z-scheme heterojunction can effectively improve the separation efficiency of photogenerated carrier, which is of great significance for the treatment of antibiotic wastewater. Herein, the Ag/Ag 2 CrO 4 /g-C 3 N 4 catalyst was prepared by in-situ loading and photo-reduction method for the degradation of antibiotic wastewater containing tetracycline and quinolone antibiotics . The research results showed that mesoporous graphitized carbon nitride (denoted as g-C 3 N 4 ) provided good support for Ag and Ag 2 CrO 4 nanoparticles , and mesoporous composite Ag/Ag 2 CrO 4 /g-C 3 N 4 (denoted as ACO /CN) provided more reaction sites for organic pollutants degradation. Under visible light irradiation, 5%ACO/CN catalyst showed the best degradation activity and stability for tetracycline (TC), levofloxacin (LVFX), oxytetracycline hydrochloride (OTC) and norfloxacin (NFLX), and their degradation rate constants were respectively 5.66, 8.26, 11.72 and 15.97 times of Ag 2 CrO 4 which indicated it had good potential application value in the treatment of wastewater containing various organic pollutants. This benefits from the plasmon resonance effect of silver effectively improves the utilization efficiency of visible light and the Z-scheme heterojunction between Ag 2 CrO 4 and g-C 3 N 4 promotes the rapid transmission of photogenerated carriers. Based on the experimental results, the possible TC degradation pathway and photocatalytic mechanism were proposed. This study provides a simple way for the successful design and preparation of plasmon resonance effect synergistic Z-scheme heterojunction with promising applications in the treatment of antibiotic wastewater.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Wubin Wang,Jin Wang,Yufei Yan,Kaili Huo,Chao Han,Qingyun Zhang
The positively charged nanofiltration (NF) membrane prepared via interfacial polymerization (IP) of polyethyleneimine (PEI) and trimesoyl chloride (TMC) has drawn considerable attention for lithium-magnesium separation, particularly crucial for lithium recovery from salt lakes with high Mg 2+ /Li + mass ratios. However, NF membranes prepared solely from amine monomers have not achieved efficient Li + and Mg 2+ separation. In this study, PEI-g-C 3 N 5 /TMC composite NF membranes were successfully fabricated by mixing amino-rich graphitic carbon nitride (g-C 3 N 5 ) with PEI, followed by the IP reaction of the mixed solution with TMC. Molecular dynamics (MD) simulation results showed that g-C 3 N 5 had an attractive effect on PEI, which led to a decrease in the diffusion rate of PEI, thereby resulting in a thinner separation layer. Density functional theory (DFT) revealed that g-C 3 N 5 competed with PEI, leading to a reduction in the crosslinking within the polyamide (PA) layer and subsequently causing an increase in the surface pore size of the membrane. Besides, the hydrophilicity and positive charge of the modified membrane were both improved. MD simulations, transition state theory, and DLVO principles indicated that the modification of the PA layer by g-C 3 N 5 enhanced the repulsion of Mg 2+ and the transport of Li + during the NF process. This breakthrough effectively overcame the trade-off effect between membrane separation and permeability, especially at a g-C 3 N 5 content of 0.06 wt%, where the lithium-magnesium selectivity coefficient ( S Li, Mg = 18.18) and pure water flux (Flux = 58.59 L m −2 h −1 ) reached the optimum values. Meanwhile, the PEI-g-C 3 N 5 /TMC membrane demonstrated stable separation performance during prolonged filtration and in solutions with varying Mg 2+ /Li + mass ratios. This study not only provides an effective strategy for the design of NF membranes but also expands the application prospects of nanomaterials in the field of membrane separation.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yan Ding,Chang Bo,Lan Xin Li,Chenyu Gao,Xin Chi Ma,Zhiwei Li,Libin Yang
As a new method to obtain green and renewable energy, photocatalysis , converting from sunlight to chemical energy on the catalysts, shows its superiority since being experimentally found due to easy access and cleanliness. Graphite carbon nitride (g-C 3 N 4 ), as an efficient photocatalyst with a band gap respond to visible light, is prepared in nanotube morphology by template method to provide convenience for the directional transfer of light and separation of carriers to improve photocatalytic activity and quantum efficiency . The thicknesses of g-C 3 N 4 nanotubes (NTs) were controlled by addition amount of the precursor mass in the annealing treatment process. The migration of photogenerated electrons and holes in the wall of g-C 3 N 4 NTs was accelerated in reverse to bypass recombination center in an external magnetic field to improve the photocatalytic activity. The critical thickness of g-C 3 N 4 NTs wall is 72 nm for separating and impelling the photogenerated carrier pairs to the surface in the greatest extent possible and was proved by the experimental results of photoelectrochemical tests and photoluminescence spectra.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Jiaxing Huang,Jiapeng Zhong,Ruipu Yao,Xiaojun Zhong,Qiao Xue,Xiaolong Yu,Qianwei Liang,Ke Zhong,Ningyu Tu,Jianteng Sun
An efficient photocatalyst was constructed via a simple single-stage thermal condensation reaction and applied to photoinduced peroxymonosulfate (PMS) activation for naproxen (NPX) degradation. Batch experiments demonstrated that phosphorus (P)–iron (Fe)-codoped g-C 3 N 4 (PFeCN) exhibited superior catalytic performance compared to previously reported catalysts, achieving 97 % NPX degradation within 20 min and a reaction rate constant approximately tenfold higher than that of pristine g-C 3 N 4 . P Fe codoping increased active site exposure, improved charge carrier separation efficiency, and enhanced light absorption capacity. Specifically, P N sites served as adsorption and activation centers for PMS, while Fe doping alleviated the reduction in specific surface area caused by P doping and further enhanced photoelectrochemical properties. Radical species analysis confirmed superoxide radicals as the dominant reactive species. The degradation pathways and toxicity evolution of NPX were also investigated, providing critical insights for environmental risk assessment. Furthermore, PFeCN maintained robust catalytic performance under various environmental conditions and after multiple cycles, indicating strong application prospects. This study offers key perspectives on the rational design of heteroatom-doped photocatalysts through atomic-level engineering for efficient photoinduced PMS activation.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2025
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IF 5.4
Xiaohua Zheng,Zhongchen Chen,Chenbin Cai,Huilin Han,Ruomeng Zhang,Jingting Yang
In recent years, ternary heterojunction catalysts have emerged owing to their exceptional properties for integrating the advantages of various materials, enabling the efficient separation of photoinduced charges and enhanced redox performance. In this study, a novel dual Z -scheme g-C 3 N 4 /Ag 6 Si 2 O 7 /AgBr (CNASAB) photocatalyst was prepared using a one-step coprecipitation method. Its catalytic performance was assessed through the photodegradation of tetracycline hydrochloride (TC) and Rhodamine B (RhB). The results showed that among various CNASAB compositions, CNASAB6 exhibited the highest catalytic activity. The catalyst achieved complete degradation of RhB within 6 min under visible light irradiation, with catalytic rates 73.7, 53.0, and 6.8 times higher than those of the individual components, g-C 3 N 4 , Ag 6 Si 2 O 7 , and AgBr, respectively. Additionally, the catalyst exhibited significant degradation of TC with an efficiency of 63.38 % within 2 min, indicating a broadened degradation ability. Ultraviolet-visible diffuse reflectance spectroscopy, photoluminescence spectroscopy and electrochemical impedance spectroscopy analyses confirmed that the ternary heterojunction broadened the spectral response range, reduced electrochemical impedance, and improved the separation of photoinduced electron-hole pairs. The successful construction of this ternary heterojunction not only provides a promising strategy for the photocatalytic degradation of organic pollutants but also has substantial potential for environmental purification applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jie Mao,Jihui Wang,Jun Zhang,Sha Shi,Yizhen Zhang,Yaohui Bai,Jiuhui Qu
The persistence of pharmaceuticals and personal care products (PPCPs) in aquatic ecosystems poses severe environmental risks, primarily owing to their incomplete removal by conventional treatment methods and potential for inducing bacterial resistance. While CdS/g-C 3 N 4 heterojunctions exhibit promise for photocatalytic degradation, the role of nitrogen-defect engineering in steering interfacial charge behavior to synergize photocatalysis with persulfate (PS)-based advanced oxidation remains unexplored. Herein, a nitrogen-deficient Z-scheme CdS/g-C 3 N 4 (CdS/N-CN) heterojunction was designed via hydrothermal synthesis to enable solar-driven cooperative photocatalysis and PS activation for PPCPs degradation. The optimized system achieved complete degradation of 10 mg/L sulfamethoxazole (SMX) within 60 min under visible light, achieving a rate constant (0.157 min −1 ) 29 times higher than pristine g-C 3 N 4 . Mechanistic investigations demonstrated dual-pathway operation: a built-in electric field drove Z-scheme charge transfer, migrating electrons from N-CN to CdS while holes in N-CN served as primary oxidants. Meanwhile, electrons from CdS activated PS to generate sulfate and hydroxyl radicals, with the latter transforming into singlet oxygen for supplementary oxidation. This synergistic photocatalysis-PS activation system maintained efficient redox activity while enhancing charge separation, ultimately enabling effective PPCPs decontamination. This research presents a novel strategy for leveraging solar-driven heterojunctions and persulfate chemistry for sustainable water remediation.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Ying Zhang,Chao Qu,Decai Yang,Lanyang Wang,Youguo Luo,Qing Ye
Graphitic carbon nitride-based (g-C 3 N 4 ) catalysts that respond to visible light have exhibited substantial potential for application in water splitting for hydrogen production. However, the material faces challenges such as low quantum efficiency and restricted utilization of visible light. In this study, we developed a Z-scheme heterojunction photocatalyst comprising ultrathin g-C 3 N 4 (ExCN) and CuZnInS (CZIS), which significantly enhances the photocatalytic hydrogen production performance. Notably, the hydrogen production rate reached up to 185.23 μmol g −1 h −1 without platinum co-catalysts. Comprehensive characterization and mechanism analysis revealed that the ultrathin, porous structure and oxygen-doped characteristics of ExCN markedly increased the number of active sites and extend the visible light response range. Moreover, ExCN serves as an effective carrier for CZIS particles. The coupling of CZIS with ExCN to form a Z-scheme heterojunction effectively promoted the spatial separation of photogenerated charge carriers. The narrow bandgap of CZIS broadens the light response range, while metal sites function as electron traps, suppressing electron-hole recombination and further enhancing catalytic efficiency. This study offers new insights into the rational design of visible-light-responsive hydrogen production catalysts based on graphitic carbon nitride.
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