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1.
ChemSusChem ; : e202401570, 2024 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-39305153

RESUMO

Graphitic carbon nitride (CN) has garnered considerable attention in the field of visible-light CO2 photoreduction, but its efficiency remains limited by the intrinsic π-conjugated skeleton. Here, O and S were co-doped CN (O, S/CN) by a facile "hydrolysis + calcination" approach to modulate the physicochemical and electronic structure.  Distinctive from S doped CN (SCN), O, S/CN owned porous layer structure with several nanosheets and less SO42- groups on the surface. The amount of heteroatom-doping was achieved by changing the hydrothermal temperature. The optimum O, S/CN-80 achieved moderate CO production rate of 1.29 µmol g-1h-1, which was 3.79 times as much as SCN (0.34 µmol g-1h-1). The O and most S atoms were substitutionally doped and the effect of S doped state on the improved efficiency of CO generation in O, S/CN was also explored based on the theoretical calculations. This work provides an inspiration to develop efficient dual-doped CN photocatalysts for photocatalytic CO2 reduction.

2.
Environ Res ; 263(Pt 1): 120043, 2024 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-39307224

RESUMO

The biochar-loaded Fe-Cu layered double hydroxide (FeCu-LDH@BC) catalyst was synthesized via a simple hydrothermal method and used to activate peroxydisulfate (PDS) for penicillin G (PG) degradation under visible light. The physicochemical properties of FeCu-LDH@BC were characterized using SEM, XPS, UV-DRS, SEM-EDS, HRTEM, XRD, BET, PL spectrum, FT-IR, Raman spectrum, TG-DSC, TPD, and EIS, showing that biochar (BC) enhanced the optical properties of FeCu-LDH. Notably, the FeCu-LDH@BC + PDS + Light system achieved a 98.79% degradation efficiency for PG in just 10 min. Furthermore, FeCu-LDH@BC retained excellent activity after four reuse cycles. LSV results indicated enhanced electron transfer in the FeCu-LDH@BC + PDS + Light system, suggesting a synergistic effect between the photocatalytic and PDS activation systems. The interconversion of h+, SO4·â», 1O2, and ·OH species was found to play a key role in PG degradation. Density functional theory was used to identify PG sites susceptible to radical attack, and the possible degradation pathway was proposed based on liquid chromatography-mass spectrometry results. Toxicity evaluation using the TEST software confirmed that the intermediates formed were significantly less toxic than PG. Lastly, the FeCu-LDH@BC + PDS + Light system removed 37.45% of total organic carbon and 63.74% of chemical oxygen demand from real wastewater within 120 min. The type and transformation pathways of organic matter in the wastewater were analyzed using 3D Excitation Emission Matrix spectroscopy to assess the system's application potential.

3.
Molecules ; 29(16)2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39202915

RESUMO

Molecular oxygen activation often suffers from high energy consumption and low efficiency. Developing eco-friendly and effective photocatalysts remains a key challenge for advancing green molecular oxygen activation. Herein, graphitic carbon nitride (g-C3N4) with abundant hydroxyl groups (HCN) was synthesized to investigate the relationship between these polar groups and molecular oxygen activation. The advantage of the hydroxyl group modification of g-C3N4 included narrower interlayer distances, a larger specific surface area and improved hydrophilicity. Various photoelectronic measurements revealed that the introduced hydroxyl groups reduced the charge transfer resistance of HCN, resulting in accelerated charge separation and migration kinetics. Therefore, the optimal HCN-90 showed the highest activity for Rhodamine B photodegradation with a reaction time of 30 min and an apparent rate constant of 0.125 min-1, surpassing most other g-C3N4 composites. This enhanced activity was attributed to the adjusted band structure achieved through polar functional group modification. The modification of polar functional groups could alter the energy band structure of photocatalysts, narrow band gap, enhance visible-light absorption, and improve photogenerated carrier separation efficiency. This work highlights the significant potential of polar functional groups in tuning the structure of g-C3N4 to enhance efficient molecular oxygen activation.

4.
Chemosphere ; 364: 143178, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39214404

RESUMO

The synthesis of sulfur-doped exfoliated graphitic carbon nitride (S-gCN) photocatalyst was achieved by the implementation of a two-step calcination technique. The XRD results revealed that all the fabricated photocatalytic materials were crystalline in nature. The inclusion of 5% sulfur in gCN led to a conspicuous escalation in the surface area of photocatalyst, rising from 10.294 to 61.185 m2g⁻1. Morphological scrutiny of the samples using FE-SEM revealed that pristine gCN exhibited tightly stacked small nanosheets, whereas inclusion of sulfur and exfoliation resulted in generation of loosely distributed large nanosheet. Furthermore, the inclusion of sulfur also induced a shift in the energy band gap (Eg) from 2.81 eV to 2.63 eV, making it felicitous for investigation as proficient visible light photocatalyst. Additionally, the photoluminescence photo-induced charge carrier recombination behavior revealed a reduced peak intensity for 5% S-gCN compared to other synthesized compositions. This observation can be directly linked to the minimized electron-hole pairs recombination during photocatalysis, underscoring its superior photocatalytic performance. Our findings revealed that the 5% S-gCN photocatalyst exhibit the most promising attributes, it degraded Tetracycline drug, Chlorpyrifos pesticide and Eriochrome Black T dye under visible light irradiation almost ∼4 times more efficiently than pristine gCN. Additionally, exceptional visible light photocatalytic antibacterial efficacy was also perceived by 5% S-gCN against S. aureus bacteria. Overall, the present research sheds light on how doping and exfoliation interact to modify the structure and catalytic properties of gCN, paving the way for the development of outstanding performance, visible light-responsive efficient photocatalysts for environmental restoration.


Assuntos
Antibacterianos , Grafite , Luz , Enxofre , Enxofre/química , Antibacterianos/química , Antibacterianos/farmacologia , Catálise , Grafite/química , Compostos de Nitrogênio/química , Fotólise , Processos Fotoquímicos , Tetraciclina/química , Tetraciclina/farmacologia , Poluentes Químicos da Água/química , Nitrilas/química , Nitrilas/farmacologia
5.
Small ; : e2404162, 2024 Jul 03.
Artigo em Inglês | MEDLINE | ID: mdl-38958083

RESUMO

The synergistic effect of rare earth single-atoms and transition metal single-atoms may enable us to achieve some unprecedented performance and characteristics. Here, Co-Dy dual-atoms on black phosphorus with a P-Co-Dy charge-transfer bridge are designed and fabricated as the active center for the CO2 photoreduction reaction. The synergistic effect of Co-Dy on the performance of black phosphorus is studied by combining X-ray absorption spectroscopy, ultrafast spectral analysis, and in situ technology with DFT calculations. The results show that the Co and Dy bimetallic active site can promote charge transfer by the charge transfer bridge from P to Dy, and then to Co, thereby improving the photocatalytic activity of black phosphorus. The performance of catalysts excited at different wavelength light indicates that the 4G11/2/2I15/2/4F9/2→6H15/2 and 4F9/2→6H13/2 emissions of Dy can be absorbed by black phosphorus to improve the utilization of sunlight. The in situ DRIFTS and density functional theory (DFT) calculations are used to investigate the CO2 photoreduction pathway. This work provides an depth insight into the mechanism of dual-atom catalysts with enhanced photocatalytic performance, which helps to design novel atomic photocatalysts with excellent activity for CO2 reduction reactions.

6.
Angew Chem Int Ed Engl ; : e202410525, 2024 Jul 23.
Artigo em Inglês | MEDLINE | ID: mdl-39041715

RESUMO

Directional electron flow in the photocatalyst enables efficient charge separation, which is essential for efficient photocatalysis of H2 production. Here, we report a novel class of tetracationic cyclophanes (7) incorporating bipyridine Pt(II) and selenoviologen. X-ray single-crystal structures reveal that 7 not only fixes the distances and spatial positions between its individual units but also exhibits a box-like rigid electron-deficient cavity. Moreover, host-guest recognition phenomena are observed between 7 and ferrocene, forming host-guest complexes with a 1:1 stoichiometry in MeCN. 7 exhibits good redox properties, narrow energy gaps, and strong absorption in the visible range (370-500 nm) due to containing two selenoviologen (SeV2+) units. Meanwhile, the femtosecond transient absorption (fs-TA) reveals that 7 has stabilized dicationic biradical, efficient charge separation, and facilitates directional electron flow to achieve efficient electron transfer due to the formation of rigid cyclophane and electronic architecture. Then, 7 is applied to visible-light-driven hydrogen evolution with high hydrogen production (132 µmol), generation rate (11 µmol/h), turnover number (221), and apparent quantum yield (1.7%), which provides a simplified and efficient photocatalytic strategy for solar energy conversion.

7.
Environ Sci Pollut Res Int ; 31(32): 44828-44847, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38955971

RESUMO

In the search of novel photocatalysts to increase the effect of visible light in photocatalysis, g-C3N4 (CN) has become a shining star. Rare earth metals have been used as dopant material to reinforce the photocatalytic activity of CN due to their unique electron configuration recently. In this present study, the pure and different amounts of Ho-doped g-C3N4 (HoCN) photocatalysts were successfully synthesized using urea as a precursor by the one-pot method. Morphological, structural, optical, and vibrational properties of the synthesized photocatalysts were characterized by SEM, EDX, XRD, TGA, XPS, FTIR, PL, TRPL, Raman, DRS, and BET analyses. In addition, theoretical calculations using density functional theory (DFT) were meticulously carried out to delve the changes in the structural and electronic structure of CN with holmium doping. According to calculations, the chemical potential, electrophilicity, and chemical softness are higher for HoCN, while HOMO-LUMO gap, dipole moment, and the chemical hardness are lower for the pure one. Thus, holmium doping becomes desirable with low chemical hardness which indicates more effectivity and smaller HOMO-LUMO gap designate high chemical reactivity. To determine the photocatalytic efficiency of the pure and doped CN photocatalysts, the degradation of methylene blue (MB) was monitored under visible light. The results indicate that holmium doping has improved the photocatalytic activities of CN samples. Most strikingly, this improvement is noticeable for the 0.2 mmol doped CN sample that showed two times better photocatalytic activity than the pure one.


Assuntos
Hólmio , Luz , Catálise , Hólmio/química , Teoria da Densidade Funcional , Processos Fotoquímicos
8.
Heliyon ; 10(11): e31854, 2024 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-38867978

RESUMO

In this study, TiO2 supported over embryonic Beta zeolite (BEA) was prepared for the photocatalytic degradation of Tetracycline (TC) antibiotic under visible light. The immobilization of sol-gel TiO2 over the zeolite increased its surface area from 33 (m2/g) to 226 (m2/g) and enhanced its adsorption efficiency from 8 % to 18 %. In order to expand the photocatalytic activity of TiO2 towards the visible light region (i.e. λ > 380 nm), two different metal sensitization techniques with Iron ions from aqueous solution of FeCl3 were explored. In the ion-exchange method, the substitutional cations within the TiO2/BEA structure were exchanged with Fe3+. Whereas, in the doping technique, solgel TiO2 was doped with Fe3+ during its synthesis and before its immobilization over Zeolite. Four different samples with 20, 40, 60, and 100 % w/w of TiO2/BEA ratio were prepared. After testing the various ion-exchanged photocatalysts under blue and white lights, only Fe-60%TiO2/BEA showed better activity compared to pure TiO2 under white light at TC initial concentration, C o = 20 ppm. For the doped immobilized Titania with 60 wt% TiO2/BEA, three different doped photocatalysts were prepared with 3 %, 7 %, and 10 % per mole Fe/TiO2. All the Fe-doped TiO2/BEA photocatalysts showed better activity compared to pure TiO2 under white light. Under solar irradiations, the 3 % Fe-doped TiO2/BEA was able to degrade all TC within 120 min, while Fe-60%TiO2/BEA needed 200 min, and TiO2 needed more than 300 min. This enhanced performance was a result of both increased surface area due to immobilization over BEA as well as iron doping by Fe3+ that simultaneously increased the visible light absorption of TiO2 and minimized the charge carrier recombination effect.

9.
Int J Mol Sci ; 25(12)2024 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-38928465

RESUMO

In environmental chemistry, photocatalysts for eliminating organic contaminants in water have gained significant interest. Our study introduces a unique heterostructure combining MIL-101(Cr) and bismuth oxyiodide (Bi5O7I). We evaluated this nanostructure's efficiency in adsorbing and degrading tetracycline (TC) under visible light. The Bi5O7I@MIL-101(Cr) composite, with a surface area of 637 m2/g, prevents self-aggregation seen in its components, enhancing visible light absorption. Its photocatalytic efficiency surpassed Bi5O7I and MIL-101(Cr) by 33.4 and 9.2 times, respectively. Comprehensive analyses, including scanning electron microscopy (SEM) and transmission electron microscopy (TEM), confirmed the successful formation of the heterostructure with defined morphological characteristics. BET analysis demonstrated its high surface area, while X-ray diffraction (XRD) confirmed its crystallinity. Electron spin resonance (ESR) tests showed significant generation of reactive oxygen species (ROS) like h+ and·â€¢O2- under light, crucial for TC degradation. The material maintained exceptional durability over five cycles. Density functional theory (DFT) simulations and empirical investigations revealed a type I heterojunction between Bi5O7I and MIL-101(Cr), facilitating efficient electron-hole pair separation. This study underscores the superior photocatalytic activity and stability of Bi5O7I@MIL-101(Cr), offering insights into designing innovative photocatalysts for water purification.


Assuntos
Bismuto , Estruturas Metalorgânicas , Tetraciclina , Estruturas Metalorgânicas/química , Bismuto/química , Catálise , Tetraciclina/química , Luz , Poluentes Químicos da Água/química , Purificação da Água/métodos , Espécies Reativas de Oxigênio/química , Adsorção , Processos Fotoquímicos
10.
J Hazard Mater ; 474: 134703, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-38805817

RESUMO

Graphitic carbon nitride has gained considerable attention as a visible-light photocatalyst. However, its photocatalytic efficiency is restricted by its limited capacity for absorbing visible light and swift recombination of charge carriers. To overcome this bottleneck, we fabricated an atomic Fe-dispersed ultrathin carbon nitride (Fe-UTCN) photocatalyst via one-step thermal polymerization. Fe-UTCN showed high efficiency in the photodegradation of acetaminophen (APAP), achieving > 90 % elimination within 60-min visible light irradiation. The anchoring of Fe atoms improved the photocatalytic activity of UTCN by narrowing the bandgap from 2.50 eV to 2.33 eV and suppressing radiative recombination. Calculations by density functional theory revealed that the Fe-N4 sites (adsorption energy of - 3.10 eV) were preferred over the UTCN sites (adsorption energy of - 0.18 eV) for the adsorption of oxygen and the subsequent formation of O2•-, the dominant reactive species in the degradation of APAP. Notably, the Fe-UTCN catalyst exhibited good stability after five successive runs and was applicable to complex water matrices. Therefore, Fe-UTCN, a noble-metal-free photocatalyst, is a promising candidate for visible light-driven water decontamination.

11.
Anal Chim Acta ; 1309: 342668, 2024 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-38772655

RESUMO

BACKGROUND: Surface-enhanced Raman scattering (SERS) has gained widespread use in molecule-level detection benefiting from its high sensitivity, nondestructive data acquisition, and capacity for providing molecular fingerprint information. However, the strong adhesion of target molecules to the substrate (known as the "memory effect") inherently hinders the reusability of SERS substrates. Research has shown that self-cleaning SERS substrates based on versatile semiconductor materials with SERS enhancement capabilities and solar photocatalytic properties offer an effective platform for the sensitive detection and degradation of harmful molecules. RESULTS: In this research, a resuable SERS-active substrate was facilely fabricated by anchoring silver nanoparticles (AgNPs) to the edges of MoS2 nanosheet decorated on ZnO nanorod arrays (NRAs). This innovative design exhibited a remarkable SERS enhancement factor (EF) of 4.6 × 107 and demonstrated significant solar photocatalytic efficiency. Such superior characteristics of ternary plasma heterojunction were ascribable to the synergistic effect of the "Schottky barrier" and "hot spots" between MoS2 and AgNPs, the inherent chemical enhancement proficiency of the MoS2/ZnO NRAs heterojunction, as well as the ultrafast electron transfer within the ternary heterojunction. SIGNIFICANCE: The developed ternary heterojunction substrate enabled highly sensitive SERS detection of trace amounts of organic molecules. Moreover, this SERS substrate exhibited self-cleaning and recyclability via solar-light-driven photocatalysis. This bifunctional recyclable SERS substrate proved capable of meeting various requirements for routine monitoring of environmental organic pollutants and provided a robust avenue for advancing energy utilization materials that serve as high-performance SERS sensors and catalysts.

12.
Small ; 20(35): e2400618, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38644234

RESUMO

There are few reports on lanthanide single atom modified catalysts, as the role of the 4f levels in photocatalysis is difficult to explain clearly. Here, the synergistic effect of 4f levels of Nd and heterostructures is studied by combining steady-state, transient, and ultrafast spectral analysis techniques with DFT theoretical calculations based on the construction of Nd single atom modified black phosphorus/g-C3N4 (BP/CN) heterojunctions. As expected, the generation rates of CO and CH4 of the optimized heterostructure are 7.44 and 6.85 times higher than those of CN, and 8.43 and 9.65 times higher than those of BP, respectively. The Nd single atoms can not only cause surface reconstruction and regulate the active sites of BP, but also accelerate charge separation and transfer, further suppressing the recombination of electron-hole pairs. The electrons can transfer from g-C3N4:Nd to BP:Nd, with a transfer time of ≈11.4 ps, while the radiation recombination time of electron-hole pairs of g-C3N4 is ≈26.13 µs, indicating that the construction of heterojunctions promotes charge transfer. The 2P1/2/2G9/2/4G7/2/2H11/2/4F7/2→4I9/2 emissions from Nd3+ can also be absorbed by heterostructures, which improves the utilization of light. The energy change of the key rate measurement step CO2 *→COOH* decreases through Nd single atom modification.

13.
Environ Sci Pollut Res Int ; 31(17): 25373-25387, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38472583

RESUMO

Mn3O4/ZnO-Al2O3-CeO2 catalyst was synthesized through a solid-state process from a 3% Mn-doped Zn-(Al/Ce) layered double hydroxide structure. Detailed structural and optical characterization using XRD, FTIR, UV-visible DRS, and TEM was conducted. By investigating clofibric acid (CA) degradation in aqueous solution, Mn3O4/ZnO-Al2O3-CeO2 photocatalytic activity was evaluated. The results show that the heterostructure mixed oxide catalyst has excellent CA photodegradation performance. Further, the characterization reveals that such photocatalytic efficiency can be attributed to two facts that are summarized in the optical properties and the synergic effect between Mn and Ce elements. The sample demonstrated a narrow band gap of 2.34 eV based on DRS. According to the experimental results of the photodegradation, after 120 min of irradiation, the photocatalyst exhibited the highest photocatalytic activity, with a degradation efficiency of 93.6%. Optimization outcomes indicated that maximum degradation efficiency was attained under the following optimum conditions: catalyst dose of 0.3 g/L, initial dye concentration of 20 mg/L, pH 3.86, and 120 min of reaction time. The quenching test demonstrates that photogenerated electrons and superoxide radicals are the most powerful reactive species. The catalyst could be useful in decreasing the photogenerated charges recombination, which offers more redox cycles simultaneously during the catalytic process. The strong Ce-Mn interaction and the formation of their different oxidation states offer a high degradation efficiency by facilitating electron-hole transfer. The introduction of Mn3O4 in the catalyst can effectively improve the visible absorption properties, which are beneficial in the photocatalytic process by reaching a high catalytic efficiency at a low cost.


Assuntos
Óxidos , Óxido de Zinco , Óxidos/química , Água , Óxido de Zinco/química , Fotólise , Luz , Zinco
14.
Chemosphere ; 355: 141801, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38552804

RESUMO

Three-dimensional donor-acceptor (D-A) type conjugated porous polymers (CPPs) was designed and synthesized via imine condensation of copper tetraaminoporphyrin (CuTAPP) as donor and 1,3,5-tris-(4-formyl phenyl) triazine (TFPT) as acceptor, named as CuPT-CPP. The CuPT-CPP possesses a high specific surface area (73.7 m2/g) and excellent photophysical properties. The simultaneous introduction of the organometallic molecules and D-A structures in CuPT-CPP could be broadened the visible-light response range (400-800 nm) and facilitated efficient photogenerated carrier separation and transportation. As heterogeneous photocatalysts, CuPT-CPP has excellent photocatalytic performances under visible light irradiation, leading to excellent model pollutant rhodamine B degradation efficiency up to about 100% in 3 h, it has superb stability and reusability during the photocatalytic processes, and CuPT-CPP also exhibited broad substrate adaptability, which could photocatalytic degradation of methylene blue (MB), methyl orange (MO), and tetracycline hydrochloride (TC). This work indicates that three-dimensional D-A type porphyrin- and triazine-based CuPT-CPP has great potential in the practical application of photocatalysis.


Assuntos
Poluentes Ambientais , Porfirinas , Água , Fotólise , Porosidade , Metais , Polímeros
15.
J Colloid Interface Sci ; 663: 891-901, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38447403

RESUMO

Exploring the real force that drives the separation of Coulomb-bound electron-hole pairs in the interface of heterojunction photocatalysts can establish a clear mechanism for efficient solar energy conversion efficiency. Herein, the formation of oxygen vacancy (Ov) and isolated Ti3+ was precisely regulated at the interface of g-C3N4/TiO2 Z-scheme heterojunction (g-C3N4/Ov-Ti3+-TiO2) by optimizing the opening degree of the calcination system, showing excellent production rate of CO and CH4 from CO2 photoreduction under visible light. This photocatalytic system also exhibited prominent stability. Combining theoretical calculation and characterization, the introduction of Ov and isolated Ti3+ on the interface could construct a charge transfer channel to break the forbidden transition of n â†’ π*, improving the separation process of photoexcited electron-hole pairs. The photoexcited electrons weakened the covalent interaction of CO bonds to promote the activation of adsorbed inert CO2 molecules, significantly reducing the energy barrier of the rate-limiting step during CO2 reduction. This work demonstrates the great application potential of reasonably regulating heterojunction interface for efficient photocatalytic CO2 reduction.

16.
Small ; 20(31): e2310894, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-38431943

RESUMO

A visible-light-driven CO2 reduction optical fiber is fabricated using graphene-like nitrogen-doped composites and hollow quartz optical fibers to achieve enhanced activity, selectivity, and light utilization for CO2 photoreduction. The composites are synthesized from a lead-based metal-organic framework (TMOF-10-NH2) and g-C3N4 nanosheet (CNNS) via electrostatic self-assembly. The TMOF-10-NH2/g-C3N4 (TMOF/CNNS) photocatalyst with an S-type heterojunction is coated on optical fiber. The TMOF/CNNS coating, which has a bandgap energy of 2.15 eV, has good photoinduced capability at the coating interfaces, high photogenerated electron-hole pair yield, and high charge transfer rate. The conduction band potential of the TMOF/CNNS coating is more negative than that for CO2 reduction. Moreover, TMOF facilitates the CO desorption on its surface, thereby improving the selectivity for CO production. High CO2 photoreduction and selectivity for CO production is demonstrated by the TMOF/CNNS-coated optical fiber with the cladding/core diameter of 2000/1000 µm, 10 wt% TMOF in CNNS, coating thickness of 25 µm, initial CO2 concentration of 90 vol%, and relative humidity of 88% RH under the excitation wavelength of 380-780 nm. Overall, the photocatalytic hollow optical fiber developed herein provides an effective and efficient approach for the enhancement of light utilization efficiency of photocatalysts and selective CO2 reduction.

17.
J Environ Manage ; 354: 120353, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38377756

RESUMO

Waste beverages are utilized as resources in various valuable, albeit energy-consuming, waste-to-energy processes. There is a growing need for alternative cost-effective methods to harness their potential. This study explored the feasibility of employing waste beverages as feedstock for the counterpart component of a TiO2-based composite photocatalyst. Several commonly available carbonated soft drinks from the Japanese market have been investigated to achieve this goal. The investigation revealed that a mild hydrothermal treatment condition could transform all examined beverages into carbonaceous materials suitable for fabricating a core-shell structure with TiO2, resulting in a remarkably efficient visible light active photocatalyst. Notably, a pH-adjusted photocatalyst derived from Coca Cola® exhibited superior visible light photodegradability toward dye molecules and enhanced bactericidal efficacy compared to the counterpart derived from pure sucrose. The heightened visible light photocatalytic activity can be attributed to the distinctive carboxy-rich surface functional groups, based on the findings of experimental analyses and density functional theory calculations. The bidentate-type bonding of these groups with TiO2 induces a modified interfacial bond structure that facilitates the efficient transfer of photoexcited carriers. This study presents a novel avenue for the effective utilization and recycling of waste beverages, and adds value under environmentally benign conditions.


Assuntos
Carbono , Nanoestruturas , Luz , Nanoestruturas/química , Antibacterianos , Bebidas
18.
Environ Res ; 249: 118361, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38325776

RESUMO

Bismuth-iron semiconductor materials have been widely studied in the photocatalytic field due to their excellent light responsiveness. Among them, the potential and mechanism regarding photocatalytic degradation of organic pollutants by Bi2Fe4O9 are seriously ignored. In this research, Bi2Fe4O9/reduced graphene oxide (BFO/rGO) was successfully synthesized for tetracycline (TC) removal. Under visible light irradiation, the TC degradation efficiency reached 83.73% within 60 min, which was much higher than that of pure BFO or rGO. The impacts of crucial factors (TC initial concentration, humic acid concentration, pH value and inorganic anions) were systematically analyzed. The photoelectric performance experiments indicated that the addition of rGO decreased the electron-hole pair recombination efficiency and improved the charge transfer efficiency, thus significantly enhancing the photocatalytic performance. According to quenching experiments and EPR (Electron Paramagnetic Resonance) analysis, superoxide radical (•O2-) and hole (h+) were determined as the main active species during degradation reactions. Eventually, the possible degradation routes of TC were presented by identifying intermediates.


Assuntos
Bismuto , Grafite , Luz , Nanocompostos , Tetraciclina , Tetraciclina/química , Grafite/química , Bismuto/química , Nanocompostos/química , Catálise , Poluentes Químicos da Água/química
19.
Environ Sci Pollut Res Int ; 31(11): 16453-16472, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38321273

RESUMO

The synthesis and characterization of a hydrochar/CeO2 composite along with its evaluation in methylene blue degradation under visible light are presented. The methodology consisted of a single-pass hydrothermal method, having as synthesis conditions 9 h of reaction time, 210 °C, autogenous pressure, and a biomass/CeO2 ratio of 100:1. The composite characterization revealed good dispersion of CeO2 in the carbonaceous matrix and significant synergy in the composite activation using visible irradiation. The photodegradation experiments showed an efficiency of 98% for white LED light, 91% for UV light, 96% for solar irradiation, and 85% for blue LED light using as conditions pH 7.0, 50 mg of composite, 50 mL of solution, 10 mg/L of dye initial concentration, and 120 min of contact time. Meanwhile, the reusability experiments evidenced a reuse capacity of up to five times with a constant photodegradation efficiency (99%); moreover, it was determined that the presence of electrolytes at pH below 7.0 during degradation negatively affected methylene blue degradation. Finally, the results of this work demonstrate that the hydrochar/CeO2 composite can be synthesized by a green method and used for the efficient treatment of water contaminated with methylene blue.


Assuntos
Luz , Azul de Metileno , Azul de Metileno/química , Raios Ultravioleta , Fotólise , Luz Azul
20.
Polymers (Basel) ; 16(2)2024 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-38256985

RESUMO

The utilization of titanium dioxide (TiO2) as a photocatalyst for the treatment of wastewater has attracted significant attention in the environmental field. Herein, we prepared an NH2-MIL-125-derived N-doped TiO2@C Visible Light Catalyst through an in situ calcination method. The nitrogen element in the organic connector was released through calcination, simultaneously doping into the sample, thereby enhancing its spectral response to cover the visible region. The as-prepared N-doped TiO2@C catalyst exhibited a preserved cage structure even after calcination, thereby alleviating the optical shielding effect and further augmenting its photocatalytic performance by increasing the reaction sites between the catalyst and pollutants. The calcination time of the N-doped TiO2@C-450 °C catalyst was optimized to achieve a balance between the TiO2 content and nitrogen doping level, ensuring efficient degradation rates for basic fuchsin (99.7%), Rhodamine B (89.9%) and tetracycline hydrochloride (93%) within 90 min. Thus, this study presents a feasible strategy for the efficient degradation of pollutants under visible light.

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