JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Ping Tan,Zhen Mao,Yuhan Li,Jiayuan Yu,Liangjun Long
The construction of CN/UiO-67 (CNU) S-scheme heterojunction composites through in situ formation of UiO-67 on carbon nitride (C 3 N 4 ) helps to address the limitations of carbon nitride (CN) in photocatalytic NO elimination. The optimized CNU 3 demonstrates superior photocatalytic efficiency, which is attributed to electronic channels constructed by Zr-N bonds and S-scheme electron transport mechanism, effectively promoting the efficient separation of photogenerated charge carriers with high redox potentials. Density Functional Theory (DFT) calculations reveal redistributed electronic orbitals in CNU 3 , with progressive and continuous energy levels near the Fermi level, which bolsters electronic conduction. Comprehensive quenching experiments, Electron Paramagnetic Resonance (EPR), and in situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analyses highlight a synergistic interplay of electrons, holes, and superoxide radicals in CNU 3 , inhibiting the generation of toxic nitrogen oxide intermediates and culminating in highly efficient photocatalytic NO oxidation. This study not only elucidates the mechanisms underpinning the enhanced performance of CNU 3 heterojunctions but also offers new perspectives on the preparation and interfacial charge separation of heterojunction photocatalysts.
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BIOELECTROCHEMISTRY
·
2024
·
IF 4.8
Pengfei Yu,Jiaqi Cui,Jun Yang,Mati Ullah Khan,Lina Yang,Shanshan Li,Meixin Li,Shuang Liu,Ling Kong,Zhiwei Chen
Zearalenone (ZEN), a secondary metabolite mycotoxin primarily synthesized by Fusarium species and prevalent in cereal grains, exerts estrogenic effects that could induce reproductive toxicity and teratogenic outcomes. To enhance the precision of ZEN detection, we have developed an innovative photoelectrochemical (PEC) aptamer-based sensor employing in situ growth silver sulfide (Ag 2 S) quantum dots-sensitized graphitic carbon nitride/bismuth oxybromide (g-C 3 N 4 /BiOBr) heterojunction. The g-C 3 N 4 /BiOBr composite exhibits robust structural stability and straightforward synthesis. In situ growth Ag 2 S quantum dots could significantly amplify the signal, thereby elevating the sensor’s sensitivity. The sensor utilizes ZEN-specific aptamers for target-specific binding, ensuring high selectivity. Within the concentration range of 0.001 to 100 ng·mL −1 , the photocurrent response demonstrated a significant linear correlation with the logarithmic scale of ZEN concentration, with a detection limit reaching 0.122 pg·mL −1 . This PEC aptamer sensor exhibits excellent stability, reproducibility, and selectivity, which is expected to be used as an effective analytical tool for ZEN detection in practical applications.
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MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Wenrong Cai,Yanjing Shi,Datong Wu,Junyao Li,Laidi Xu,Yong Kong
This work proposes a novel dual-signal electrochemiluminescence ( ECL) immunosensor based on energy resonance transfer (RET) for the detection of β2-Microglobulin (β2-MG). Introducing carbon vacancy into g-C 3 N 4 (V C -g-C 3 N 4 ) can lead to the narrowing of the band gap and the reduction of LUMO, thereby significantly enhancing the ECL efficiency of the material. Meanwhile, Zr-MOF can effectively load Ru(bpy) 3 2+ (Ru-Zr-MOF), enabling its stable existence on the electrode. The ECL emission spectrum of V C -g-C 3 N 4 overlaps well with the fluorescence excitation spectrum of Ru-Zr-MOF, indicating an effective ECL-RET effect between them. As the concentration of β2-MG increases, the intensity of anodic ECL signal gradually increases, while the intensity of cathodic ECL signal gradually decreases. The difference between the cathodic and anodic ECL signals has a good linear relationship within the concentration range from 0.2 pg/mL to 200 ng/mL, with a detection limit of 27.73 fg/mL. The constructed immunosensor can be used for practical analysis in human serum. The proposed sensor has great potential in clinical detection of β2-MG, providing new insights for biomolecular detection and disease diagnosis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Hao-Yu Zhou,Bai-Yu Feng,Zhen-bin Pang,Guo-Zhi Han
In this paper, using PVP-modified polystyrene microspheres as template, tetrabutyl titanate (TEOT), tetraethyl orthosilicate (TEOS) and melamine as precursor, we developed a facile one-pot two-step method to preparing a novel kind of mesoporous hollow SiO 2 @TiO 2 @g-C 3 N 4 ternary composite microspheres with plush surface, in which highly active black titanium dioxide (TiO 2 ) was formed by simple calcination without further chemical reduction treatment. The structure and morphology of the composite microspheres were detailed characterized for understanding the formation mechanism. Research results indicated that the hollow SiO 2 microspheres can promote the formation of oxygen vacancies in TiO 2 , and the ternary combination narrowed the bandgap width of the black hollow composite microspheres to 1.43 eV, thus endowing it with excellent broad-spectrum catalytic performance for rapid photo-degradation of persistent organic pollutants (POPs) such as dyes and antibiotics in water under sunlight. The removal rates of dyes reached more than 70 %, as well as that of antibiotics more than 50 % within one hour. Finally, a plausible catalytic degradation mechanism was discussed.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Qian Liu,Kangping Cui,Minshu Cui,Shijie Sun,Haiyang Li
As a green photocatalyst with simple synthesis method, excellent electronic structure, and metal-free properties, the deficiencies of pristine graphitic carbon nitride, such as high electron transfer resistance and narrow energy band gap, inhibit its photocatalytic activity to some extent. In this paper, we synthesized a sulfur and chlorine co-doped g-C 3 N 4 (SCl-CN) capable of efficient photocatalytic activation of peroxymonosulfate (PMS) by calcining a mixture of ammonium chloride and thiourea. By means of DFT calculation, the contribution of sulfur and chlorine to photogenic electron hole separation was discussed. The electrostatic potential of SCl-CN and the adsorption model between SCl-CN and PMS were deduced, and the activation mechanism of PMS was further analyzed. According to the calculated results, the incorporation of sulfur and chlorine tuned the electronic configuration of the material and intensified the interactions between SCl-CN and PMS. It is shown that free and non-free radicals act simultaneously in the SCl-CN/PMS/Vis system. This study provides a new idea for the study of photocatalytic activation of PMS by non-metallic co-doped carbon nitride.
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ADSORPTION-JOURNAL OF THE INTERNATIONAL ADSORPTION SOCIETY
·
2024
·Vol. 31
·期 1
·1-13
·
IF 3
Wu Jinze,Yao Jiale,Zhu Xiping,Zuo Danying,Zhang Hongwei,Jiang Shuai,Li Hongjun
Most hydrogels for dye treatment only have the adsorption ability for anionic or cationic dyes, while a few zwitterionic hydrogels that can adsorb both anionic and cationic dyes need a complicated regeneration process when they are reused. To prepare reusable zwitterionic adsorbent hydrogels, in this paper, a zwitterionic composite hydrogel with Ag@g-C 3 N 4 was prepared, which not only can adsorb both anionic and cationic dyes but also has photocatalytic degradation ability. The scanning electron microscopy images show that the optimum hydrogel has a large number of micro pores for dye adsorption. The adsorption capacity of the hydrogel achieves the highest in mixed dye concentration of 50 mg·L -1 with pH value of 7–9. Benefiting from the synergistic effect of adsorption and photocatalytic degradation, the removal efficiency of methyl orange and methylene blue in mixed dyes was up to 93.86% and 91.80%, respectively. The photocatalytic activity trapping experiments showed that superoxide radicals as well as hydroxyl radicals played a major role in photocatalytic degradation. After 5 consecutive photocatalytic degradations, the removal ratio of the hydrogel for dyes was still above 80%, indicating good photocatalytic degradation and reusability properties. This research suggested the zwitterionic composite hydrogel has a promising prospect in removing dyes from wastewater treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Chuangbin Hong,Wenguang Wang,Liangpeng Wu,Jiehang Zhou,Shimin Long,Wentao Zhou,Yuxi Guo
The construction of semiconductor heterojunction is an effective way for charge separation in photocatalytic degradation of pollutants. In this study, a novel MoS 2 @MoO 3 /(Cu + /g-C 3 N 4 ) ternary composites (MMCCN) was prepared via a simple calcination method. The as-prepared composites exhibited exceptional performance in activating peroxymonosulfate (PMS) for the degradation of rhodamine B (RhB). The activity testing results indicated that 99.41 % of RhB (10 mg·L −1 , 10 mL) was effectively removed by the synergistic effect of composites photocatalyst (0.1 g·L −1 ) and PMS (0.1 g·L −1 ) under visible light irradiation for 40 min. Its reaction rate constant exceeded that of Cu + /g-C 3 N 4 , MoO 3 and MoS 2 by a factor of 3.56, 17.30 and 11.73 times, respectively. The crystal structure, band gap and density of states (DOS) of the semiconductors were calculated according to the density functional theory (DFT). Free radical trapping tests and electron spin resonance spectroscopy validated that 1 O 2 , O 2 − and h + are primary reactive species participating in the decomposition of RhB. The ternary composites demonstrated good stability and maintained excellent degradation efficiency even across four reaction cycles. Furthermore, the activation mechanism and the intermediates produced during the decomposition course of RhB by MMCCN/PMS/vis system were analyzed and elucidated. A double S-scheme heterojunctions was responsible for efficient separation of photo-induced electron-hole pairs. This work presents a novel method in the construction of double S-scheme heterojunctions for PMS activation which is expected to find wide applications in wastewater treatment and environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Kailin Wang,Yang Yang,Shumail Farhan,Yan Wu,Wen-Feng Lin
Probing the spatial separation and transport process of photogenerated charges at nanoscale interfaces is essential for understanding catalytic reaction mechanisms on heterostructure photocatalysts. Here, we developed a p-n junction Na 0.6 CoO 2 /g-C 3 N 4 S-scheme photocatalyst via electrostatic self-assembly technology. A significant hydrogen production rate of ∼ 0.294 mmol g − 1 h −1 was achieved on the optimal Na 0.6 CoO 2 /g-C 3 N 4 , which was ten times higher than that of pure g -C 3 N 4 . In-situ XPS shows that the electrons in Na 0.6 CoO 2 / g -C 3 N 4 had different flow directions without and with illumination, demonstrating a built-in electric field being formed through Na 0.6 CoO 2 and g -C 3 N 4 interaction. DFT calculations and ultraviolet photoelectron spectroscopy verified that g -C 3 N 4 and Na 0.6 CoO 2 possess the energy band structures conforming to the heterostructure of S-scheme. In-situ Kelvin probe microscope studies show that Na 0.6 CoO 2 and g -C 3 N 4 both have a self-induced electric field effect, and their combination significantly strengthens the built-in electric field and improves the space separation of photogenerated electrons. Compared with the change of the surface photovoltage of g -C 3 N 4 (60 mV) and Na 0.6 CoO 2 (−30 mV), the average surface contact potential difference of Na 0.6 CoO 2 / g -C 3 N 4 reached 320 mV, yielding a higher efficiency of photogenerated electron separation. This work also provides direct evidence on the existence of a built-in electric field and an electron flow direction for heterostructure photocatalyst materials.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Chen Hu,Chao Yang,Bo Li,Bangzhu Peng
Consumption of contaminated wines is a significant source of ochratoxin A (OTA) intake in humans, yet existing techniques for OTA removal are inadequate. This study constructs a TiO 2 /SiO 2 /g-C 3 N 4 catalyst (TiSiMs-TCN) with a tubular structure, capable of efficiently removing OTA from both simulated and real wines under visible light irradiation. The results of experiments, characterizations, and theoretical calculations demonstrate that the incorporation of silica enhances the adsorption capacity for OTA, and the tubular structure improves the catalyst's photoelectric properties. The internal electric field between TiSiMs and TCN facilitates electron transfer and the generation of active species, rapidly degrading the adsorbed OTA and promoting the regeneration of active sites, thus maintaining continuous adsorption-photocatalysis synergy. The OTA degradation pathway was analyzed using the Fukui index, electrostatic potential distribution, and intermediate product identification. Toxicological experiments confirm that TiSiMs-TCN is a safe and stable material capable of effectively detoxifying OTA contamination.
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FUEL
·
2024
·
IF 6.7
Wenting Chen,Xinwei Zhao,Qi Zeng,Lili Liu,Pengju Yang,Shupeng Guo,Juzhi Leng,Min Zhong,Wei Hong,Lin Zhang
Combining the advantages of multiple strategies including morphology control, atom doping, and defect construction, the photocatalytic hydrogen evolution reaction (HER) performance of graphitic carbon nitride (g-C 3 N 4 ) may be boosted significantly. Herein, holey ultra-thin g-C 3 N 4 nanosheets (CNS-x, x = H, O, N) modified with structural vacancies and sulfur (S) dopant are synthesized through a straightforward method involving the pyrolysis of thiocyanuric acid under various gas atmospheres. The textural properties, type and concentration of structural defect, and S doping level are significantly influenced by the gas atmosphere. Remarkably, CNS-H with C, N dual defects and S-dopant exhibits the HER rate of 46.59 mmol·g −1 ·h −1 , which is 16.68 times higher than that of bulk g-C 3 N 4 . The corresponding apparent quantum yields are 17.24 % at 420 nm and 1.90 % at 520 nm. The enhanced HER performance of CNS-H can be attributed to the combined effect of improved charge separation, extended photoabsorption, and optimized properties of the platinum cocatalyst.
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Catalysts
·
2025
·Vol. 15
·期 9
·808
·
IF 4
Shuai Liu,Yipei Chen,Honglei Zhang,Yang Meng,Tao Wu,Guangsuo Yu
Constructing heterojunction photocatalysts with efficient interfacial charge transfer is critical for solar-driven hydrogen evolution. In this study, a highly dispersed MoS2/g-C3N4composite was successfully synthesized via a stirring-assisted hydrothermal in situ growth strategy. The introduction of stirring during synthesis significantly enhanced the uniform dispersion of MoS2nanosheets and exposed abundant edge sites, leading to well-integrated heterojunctions with enhanced interfacial contact. Comprehensive structural and photoelectronic characterizations (XRD, SEM, TEM, EDS mapping, UV–Vis, TRPL, EIS, EPR) confirmed that the composite exhibited improved visible-light absorption, accelerated charge separation, and suppressed recombination. Under simulated solar irradiation with triethanolamine (TEOA) as a sacrificial agent, the optimized 24% MoS2/g-C3N4-S catalyst achieved a high hydrogen evolution rate of 14.33 mmol·g−1·h−1at a catalyst loading of 3.2 mg, significantly outperforming the unstirred and pristine components, and demonstrating excellent cycling stability. Mechanistic studies revealed that the performance enhancement is attributed to the synergistic effects of Type-II heterojunction formation and edge-site-rich MoS2co-catalysis. This work provides a scalable approach for non-noble metal interface engineering and offers insight into the design of efficient and durable photocatalysts for solar hydrogen production.
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LANGMUIR
·
2025
·
IF 3.9
Xiao Zhang,Menglin Zhang,Zhiren Guo,Xiang Li,Ting Liu,Jinying Li,Dongxiang Zhang,Xiyan Xu
The persistent contamination of aquatic environments by tetracycline (TC) necessitates advanced remediation strategies. Herein, a ternary Fe–O–P-co-modified graphitic carbon nitride (FOPCNx) was synthesized via structural integration of Fe–N2 configurations with O/P dual doping for efficient TC degradation in a solar-driven photo-Fenton system. This study pioneers the synergistic coupling of Fe–N2 coordination and heteroatomic O/P substitution to optimize charge dynamics. Comprehensive characterization confirmed the formation of Fe–N2 active sites and aromatic structures incorporated with the aromatic group, which collectively enhanced visible-light absorption, suppressed electron–hole recombination, and facilitated charge carrier redistribution. The optimized FOPCN2 demonstrated exceptional photoelectric efficiency (3.7-fold higher photocurrent density than pristine g-C3N4) and achieved 98.9% TC removal within 40 min of irradiation with a kinetic constant of 0.113 min–1, outperforming conventional systems. Mechanistic studies revealed dual enhancement pathways: Fe–N2 sites promoted electron transfer and Fe(III)/Fe(II) cycling, while the O/P dual doping enabled electron delocalization for improved charge mobility. The system exhibited remarkable pH adaptability (3–7), robust resistance to inorganic anions, and universal degradation capability for mixed organic pollutants. Three TC degradation pathways were identified through intermediate analysis, with radical trapping and EPR verification confirming the dominant roles of •OH, e–, and O2•–. This work provides critical insights into structure–activity relationships for carbon nitride modification, establishing a paradigm for designing multifunctional photocatalysts for antibiotic-contaminated wastewater remediation.
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