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1.
Small ; 20(14): e2306983, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-37988639

RESUMO

Constructing S-scheme heterojunction catalysts is a key challenge in visible-light catalysed degradation of organic pollutants. Most heterojunction materials are reported to face significant obstacles in the separation of photogenerated electron-hole pairs owing to differences in the material size and energy barriers. In this study, sulfur-doped g-C3N4 oxidative-type semiconductor materials are synthesized and then coupled with BiOBr reductive-type semiconductor to form S-g-C3N4/BiOBr S-scheme heterojunction. A strong and efficient internal electric field is established between the two materials, facilitating the separation of photogenerated electron-hole pairs. Notably, in situ XPS proved that after visible light irradiation, Bi3+ is converted into Bi(3+ɑ)+, and a large number of photogenerated holes are produced on the surface of BiOBr, which oxidized and activated H2O into •OH.  â€¢OH cooperated with •O2 - and 1O2 to attack Rhodamine B (RhB) molecules to achieve deep oxidation mineralization. The composite material is designed with a LUMO energy level higher than that of RhB, promoting the sensitization of RhB by injecting photogenerated electrons into the heterojunction, thereby enhancing the photocatalytic performance to 22.44 times that of pure g-C3N4. This study provides a new perspective on the efficient degradation of organic molecules using visible light catalysis.

2.
Small ; : e2400724, 2024 Apr 19.
Artigo em Inglês | MEDLINE | ID: mdl-38639018

RESUMO

The lack of intrinsic active sites for photocatalytic CO2 reduction reaction (CO2RR) and fast recombination rate of charge carriers are the main obstacles to achieving high photocatalytic activity. In this work, a novel phosphorus and boron binary-doped graphitic carbon nitride, highly porous material that exhibits powerful photocatalytic CO2 reduction activity, specifically toward selective CO generation, is disclosed. The coexistence of Lewis-acidic and Lewis-basic sites plays a key role in tuning the electronic structure, promoting charge distribution, extending light-harvesting ability, and promoting dissociation of excitons into active carriers. Porosity and dual dopants create local chemical environments that activate the pyridinic nitrogen atom between the phosphorus and boron atoms on the exposed surface, enabling it to function as an active site for CO2RR. The P-N-B triad is found to lower the activation barrier for reduction of CO2 by stabilizing the COOH reaction intermediate and altering the rate-determining step. As a result, CO yield increased to 22.45 µmol g-1 h-1 under visible light irradiation, which is ≈12 times larger than that of pristine graphitic carbon nitride. This study provides insights into the mechanism of charge carrier dynamics and active site determination, contributing to the understanding of the photocatalytic CO2RR mechanism.

3.
Small ; : e2311841, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38368255

RESUMO

Heterostructures are widely employed in photocatalysis to promote charge separation and photocatalytic activity. However, their benefits are limited by the linkages and contact environment at the interface. Herein, violet phosphorus quantum dots (VPQDs) and graphitic carbon nitride (g-C3 N4 ) are employed as model materials to form VPQDs/g-C3 N4 heterostructures by a simple ultrasonic pulse excitation method. The heterostructure contains strong interfacial P-N bonds that mitigate interfacial charge-separation issues. P-P bond breakage occurs in the distinctive cage-like [P9] VPQD units during longitudinal disruption, thereby exposing numerous active P sites that bond with N atoms in g-C3 N4 under ultrasonic pulse excitation. The atomic-level interfacial P-N bonds of the Z-scheme VPQDs/g-C3 N4 heterostructure serve as photogenerated charge-transfer channels for improved electron-hole separation efficiency. This results in excellent photocatalytic performance with a hydrogen evolution rate of 7.70 mmol g-1  h-1 (over 9.2 and 8.5 times greater than those of pure g-C3 N4 and VPQDs, respectively) and apparent quantum yield of 11.68% at 400 nm. Using atomic-level chemical bonds to promote interfacial charge separation in phosphorene heterostructures is a feasible and effective design strategy for photocatalytic water-splitting materials.

4.
Small ; 20(22): e2308568, 2024 May.
Artigo em Inglês | MEDLINE | ID: mdl-38126907

RESUMO

In this work, cyano contained g-C3N4 comodified by In2S3 and polypyrrole (C≡N─CN/IS/Ppy) materials are synthesized for the photocatalytic production of H2O2 and photocatalysis-self-Fenton reaction for highly efficient degradation of metronidazole. The results from UV-vis spectrophotometry, surface photovoltage, and Kelvin probe measurements reveal the promoted transport and separation efficiency of photoinduced charges after the introduction of In2S3 and Ppy in the heterojunction. The existence of a built-in electric field accelerates the photoinduced charge separation and preserves the stronger oxidation ability of holes at the valence band of C≡N─CN. Linear sweep voltammetry measurements, zeta potential analyzations, nitroblue tetrazolium determination, and other measurements show that Ppy improves the conversion ratio of •O2 - to H2O2 and the utilization ratio of •O2 -, as well as suppresses decomposition of H2O2. Accordingly, the H2O2 evolution rate produced via a two-step single-electron reduction reaction reaches almost 895 µmol L-1 h-1, a value 80% and 7.2-fold higher than those obtained with C≡N─CN/IS and C≡N─CN, respectively. The metronidazole removal rate obtained via photocatalysis-self-Fenton reaction attains 83.7% within 120 minutes, a value much higher than that recorded by the traditional Fenton method. Overall, the proposed synthesis materials and route look promising for the H2O2 production and organic pollutants degradation.

5.
Chemistry ; : e202401675, 2024 Jun 06.
Artigo em Inglês | MEDLINE | ID: mdl-38842477

RESUMO

Single atom catalysts (SACs) exhibit the flexible coordination structure of the active site and high utilization of active atoms, making them promising candidates for nitrogen reduction reaction (NRR) under ambient conditions. By the aid of first-principles calculations based on DFT, we have systematically explored the NRR catalytic behavior of thirteen 4d- and 5d-transition metal atoms anchored on 2D porous graphite carbon nitride C5N2. With high selectivity and outstanding activity, Zr, Nb, Mo, Ta, W and Re-doped C5N2 are identified as potential nominees for NRR. Particularly, Mo@C5N2 possesses an impressive low limiting potential of -0.39 V (corresponding to a very low temperature and atmospheric pressure), featuring the potential determining step involving *N-N transitions to *N-NH via the distal path. The catalytic performance of TM@C5N2 can be well characterized by the adsorption strength of intermediate *N2H. Moreover, there exists a volcanic relationship between the catalytic property UL and the structure descriptor Ψ, which validates the robustness and universality of Ψ, combined with our previous study. This work sheds light on the design of SACs with eminent NRR performance.

6.
Macromol Rapid Commun ; : e2400365, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38849126

RESUMO

Graphitic carbon nitrides (g-C3N4) possess various benefits as heterogeneous photocatalysts, including tunable bandgaps, scalability, and chemical robustness. However, their efficacy and ongoing advancement are hindered by challenges like limited charge-carrier separation rates, insufficient driving force for photocatalysis, small specific surface area, and inadequate absorption of visible light. In this study, boron dopants and nitrogen defects synergy are introduced into bulk g-C3N4 through the calcination of a blend of nitrogen-defective g-C3N4 and NaBH4 under inert conditions, resulting in the formation of BCN nanosheets characterized by abundant porosity and increased specific surface area. These BCN nanosheets promote intermolecular single electron transfer to the radical initiator, maintaining radical intermediates at a low concentration for better control of photoinduced atom transfer radical polymerization (photo-ATRP). Consequently, this method yields polymers with low dispersity and tailorable molecular weights under mild blue light illumination, outperforming previous reports on bulk g-C3N4. The heterogeneity of BCN enables easy separation and efficient reuse in subsequent polymerization processes. This study effectively showcases a simple method to alter the electronic and band structures of g-C3N4 with simultaneously introducing dopants and defects, leading to high-performance photo-ATRP and providing valuable insights for designing efficient photocatalytic systems for solar energy harvesting.

7.
Environ Res ; 244: 117964, 2024 Mar 01.
Artigo em Inglês | MEDLINE | ID: mdl-38135102

RESUMO

In this study, we evaluate the efficiency of two novel nanostructured adsorbents - chitosan-graphitic carbon nitride@magnetite (CS-g-CN@Fe3O4) and graphitic carbon nitride@copper/zinc nanocomposite (g-CN@Cu/Zn NC) - for the rapid removal of methylparaben (MPB) from water. Our characterization methods, aimed at understanding the adsorbents' structures and surface areas, informed our systematic examination of influential parameters including sonication time, adsorbent dosage, initial MPB concentration, and temperature. We applied advanced modeling techniques, such as response surface methodology (RSM), generalized regression neural network (GRNN), and radial basis function neural network (RBFNN), to evaluate the adsorption process. The adsorbents proved highly effective, achieving maximum adsorption capacities of 255 mg g-1 for CS-g-CN@Fe3O4 and 218 mg g-1 for g-CN@Cu/Zn NC. Through genetic algorithm (GA) optimization, we identified the optimal conditions for the highest MPB removal efficiency: a sonication period of 12.00 min and an adsorbent dose of 0.010 g for CS-g-CN@Fe3O4 NC, with an MPB concentration of 17.20 mg L-1 at 42.85 °C; and a sonication time of 10.25 min and a 0.011 g dose for g-CN@Cu/Zn NC, with an MPB concentration of 13.45 mg L-1 at 36.50 °C. The predictive accuracy of the RBFNN and GRNN models was confirmed to be satisfactory. Our findings demonstrate the significant capabilities of these synthesized adsorbents in effectively removing MPB from water, paving the way for optimized applications in water purification.


Assuntos
Grafite , Compostos de Nitrogênio , Parabenos , Poluentes Químicos da Água , Purificação da Água , Cobre/química , Temperatura , Água/química , Adsorção , Poluentes Químicos da Água/química , Cinética , Concentração de Íons de Hidrogênio , Purificação da Água/métodos
8.
Environ Res ; 257: 119293, 2024 Jun 04.
Artigo em Inglês | MEDLINE | ID: mdl-38838749

RESUMO

Recently, photocatalysis combined peroxydisulfate activation under visible light (PC-PDS/Vis) was developed as a promising technology for removing antibiotics in water. Herein, Mn doped FeOOH (Mn-FeOOH) nanoclusters were grown in-situ on the surface of graphitic carbon nitride nanosheets (CNNS) using a wet chemical method, which served as a visible-light-driven photocatalyst for peroxydisulfate (PDS) activation. Photovoltaic property characterizations revealed that Mn-FeOOH/CNNS owned superior light capture ability and carrier separation efficiency. According to DFT calculations, the synergistic effect between Mn and Fe species was proved to enhance the adsorption and activation of PDS. 99.7% of tetracycline (TC) was rapidly removed in 50 min in the PC-PDS/Vis system. In addition, Mn-FeOOH/CNNS exhibited high recycling stability with low iron leaching, attributed to the interaction between Mn-FeOOH clusters and carbon species. Quenching experiments and electron spin resonance (ESR) tests unveiled that •O2- played a significant role in TC removal, while •OH and SO4•- acted as additional roles contributing to the overall process. These findings given a new strategy for antibiotics degradation by photocatalysis, offering deeper insights for the advancement of sustainable and cutting-edge wastewater treatment technologies.

9.
Environ Res ; 258: 119390, 2024 Jun 13.
Artigo em Inglês | MEDLINE | ID: mdl-38879105

RESUMO

Photocatalysis is recognized to be one of the most promising ways to address energy and environmental issues by utilizing visible light. Graphitic carbon nitride (g-C3N4), with a moderate band gap (∼2.7 eV) has been the flashpoint in environmental photocatalysis as it can work better under visible light, can be synthesized by a facile synthesis process using low-cost materials, thermally and chemically stable. Still the photocatalytic performance of g-C3N4 is not satisfactory because of certain limitations such as insufficient visible light absorption capacity, low electron-hole separation efficiency, high recombination rate, poor surface area. Introduction of doping, band structure engineering, defecting and designing of heterojunction, composites etc. were investigated to amplify its applications. Among all these modifications, elemental doping is a suitable and successful alternative for the enhancement of the photocatalytic activity by changing the optical and electronic properties. This review emphasizes on advancement and trends of elemental doping and its application on photocatalytic organic pollutant remediation in aqueous medium. The fundamental photocatalytic activity of heterogeneous photocatalysis and specifically g-C3N4-based photocatalysis have been discussed. The benfits of non-metal doping, enhanced photocatalytic performance by doping element, mechanism invloved in doping, advantages of co-doping has been explained. Mono, bi, and tri non-metal doped g-C3N4 and their application for the removal of organic pollutants from water medium by visible light photocatalysis has been summerized. Life cycle assessment (LCA) of photocatalytic system has been highlighted. Future research should focus on the large-scale application of the photocatalysis process considering the economic aspects. A rigorous life cycle assessment for deploying the non-metal doped g-C3N4-based photocatalysis technology for successful commercial application is recommended.

10.
Environ Res ; 256: 119202, 2024 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-38782343

RESUMO

A rational design of heterojunctions with high-quality contacts is essential for efficiently separating photogenerated charge carries and boosting the solar-driven harvesting capability. Herein, we fabricated a novel heterojunction of SnO2 quantum dots-anchored CdS-CdCO3 with g-C3N4 nanosheets as a superior photocatalyst. SnO2 quantum dots (SQDs) with positively charged surfaces were tightly anchored on the negatively charged surface of CdS nanosheets (NSs). The resulting CdS@SnO2 was finally decorated with g-C3N4 NSs, and a new crystalline phase of CdS-CdCO3 was formed during the hydrothermal decoration process, g-C3N4 decorated CdS-CdCO3@SnO2 (CdS-CdCO3@SnO2@g-C3N4). The as-synthesized photocatalysts were evaluated for the degradation of methyl orange dye under solar light conditions. The CdS-CdCO3@SnO2@g-C3N4 exhibited 7.7-fold and 2.3-fold enhancements in photocatalytic activities in comparison to those of the bare CdS and CdS@SnO2 NSs, respectively. The optimal performance of CdS-CdCO3@SnO2@g-C3N4 is primarily attributed to the cascade-type conduction band alignments between 2D/0D/2D heterojunctions, which can harvest maximum solar light and effectively separate photoexcited charge carriers. This work provides a new inspiration for the rational design of 2D/0D/2D heterojunction photocatalyst for green energy generation and environmental remediation applications.


Assuntos
Compostos de Cádmio , Nanocompostos , Pontos Quânticos , Compostos de Estanho , Pontos Quânticos/química , Compostos de Cádmio/química , Compostos de Estanho/química , Nanocompostos/química , Catálise , Sulfetos/química , Luz Solar , Processos Fotoquímicos , Grafite/química , Compostos Azo/química , Nitrilas/química , Compostos de Nitrogênio/química
11.
Mikrochim Acta ; 191(4): 182, 2024 03 07.
Artigo em Inglês | MEDLINE | ID: mdl-38451377

RESUMO

The rapid fabrication is described of binary electrocatalyst based on a highly porous metal-organic framework with zirconium metal core (Zr-MOF) decorated over the graphitic carbon nitride (g-C3N4) nanosheets via facile ultrasonication method. It is used for the robust determination of antipsychotic drug chlorpromazine (CLP) from environmental samples. The electrochemical behaviour of 2D Zr-MOF@g-C3N4 was characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) studies. The crystalline and porous nature of the composite was characterized by XRD and SEM analysis. The functional groups and surface characteristics were investigated by FT-IR, Raman and XPS. The major electrochemical properties of the Zr-MOF@g-C3N4 composite towards CLP detection were analyzed by CV, chronocoulometric (CC), chronoamperometric (CA) and differential pulse voltammetry (DPV) techniques. The composite exhibits a low detection limit (LOD) of 2.45 nM with a linear range of 0.02 to 2.99 µM and attractive sensitivity for CLP. The sensor system shows higher selectivity towards the possible interferences of CLP drug and exhibits better repeatability and stability. Finally, the fabricated sensor system shows a high recovery range varying from 96.2 to 98.9% towards the real samples. The proposed electrochemical probe might be a promising alternative to the prevailing diagnostic tools for the detection of CLP.


Assuntos
Antipsicóticos , Clorpromazina , Espectroscopia de Infravermelho com Transformada de Fourier , Espectroscopia Dielétrica , Eletrodos
12.
Int J Mol Sci ; 25(9)2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38732166

RESUMO

This current study assessed the impacts of morphology adjustment of perovskite BiFeO3 (BFO) on the construction and photocatalytic activity of P-infused g-C3N4/U-BiFeO3 (U-BFO/PCN) heterostructured composite photocatalysts. Favorable formation of U-BFO/PCN composites was attained via urea-aided morphology-controlled hydrothermal synthesis of BFO followed by solvosonication-mediated fusion with already synthesized P-g-C3N4 to form U-BFO/PCN composites. The prepared bare and composite photocatalysts' morphological, textural, structural, optical, and photocatalytic performance were meticulously examined through various analytical characterization techniques and photodegradation of aqueous rhodamine B (RhB). Ellipsoids and flakes morphological structures were obtained for U-BFO and BFO, and their effects on the successful fabrication of the heterojunctions were also established. The U-BFO/PCN composite exhibits 99.2% efficiency within 20 min of visible-light irradiation, surpassing BFO/PCN (88.5%), PCN (66.8%), and U-BFO (26.1%). The pseudo-first-order kinetics of U-BFO/PCN composites is 2.41 × 10-1 min-1, equivalent to 2.2 times, 57 times, and 4.3 times of BFO/PCN (1.08 × 10-1 min-1), U-BFO, (4.20 × 10-3 min-1), and PCN, (5.60 × 10-2 min-1), respectively. The recyclability test demonstrates an outstanding photostability for U-BFO/PCN after four cyclic runs. This improved photocatalytic activity exhibited by the composites can be attributed to enhanced visible-light utilization and additional accessible active sites due to surface and electronic band modification of CN via P-doping and effective charge separation achieved via successful composites formation.


Assuntos
Bismuto , Fotólise , Rodaminas , Catálise , Bismuto/química , Rodaminas/química , Luz , Compostos Férricos/química , Compostos de Nitrogênio/química , Titânio/química , Processos Fotoquímicos , Nitrilas/química , Cinética , Grafite , Óxidos , Compostos de Cálcio
13.
Molecules ; 29(12)2024 Jun 09.
Artigo em Inglês | MEDLINE | ID: mdl-38930812

RESUMO

The utilization of lithium-sulfur battery is hindered by various challenges, including the "shuttle effect", limited sulfur utilization, and the sluggish conversion kinetics of lithium polysulfides (LiPSs). In the present work, a theoretical design for the viability of graphitic carbon nitride (g-C3N4) and phosphorus-doping graphitic carbon nitride substrates (P-g-C3N4) as promising host materials in a Li-S battery was conducted utilizing first-principles calculations. The PDOS shows that when the P atom is introduced, the 2p of the N atom is affected by the 2p orbital of the P atom, which increases the energy band of phosphorus-doping substrates. The energy bands of PC and Pi are 0.12 eV and 0.20 eV, respectively. When the lithium polysulfides are adsorbed on four substrates, the overall adsorption energy of PC is 48-77% higher than that of graphitic carbon nitride, in which the charge transfer of long-chain lithium polysulfides increase by more than 1.5-fold. It is found that there are powerful Li-N bonds between lithium polysulfides and P-g-C3N4 substrates. Compared with the graphitic carbon nitride monolayer, the anchoring effect of the LiPSs@P-g-C3N4 substrate is enhanced, which is beneficial for inhibiting the shuttle of high-order lithium polysulfides. Furthermore, the catalytic performance of the P-g-C3N4 substrate is assessed in terms of the S8 reduction pathway and the decomposition of Li2S; the decomposition energy barrier of the P-g-C3N4 substrate decrease by 10% to 18%. The calculated results show that P-g-C3N4 can promote the reduction of S8 molecules and Li-S bond cleavage within Li2S, thus improving the utilization of sulfur-active substances and the ability of rapid reaction kinetics. Therefore, the P-g-C3N4 substrates are a promising high-performance lithium-sulfur battery anchoring material.

14.
Molecules ; 29(9)2024 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-38731520

RESUMO

Graphitic carbon nitride (g-C3N4), recognized for its considerable potential as a heterogeneous photocatalyst in water splitting, has attracted extensive research interest. By using density functional theory (DFT) calculations, the regulatory role of p-block metal (PM) single atoms on the photocatalytic activity of g-C3N4 in overall water splitting was systematically explored. The incorporation of PM atoms (Ge, Sn and Pb) led to a reduction in the overpotentials required for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). Combined with the electronic structures analysis via hybrid functional, it was found that the introduction of Ge, Sn or Pb optimizes the positions of the valence band maximum (VBM) and the conduction band minimum (CBM), providing a robust driving force for HER and ensuring substantial driving force for OER. Meanwhile, the presence of these three PMs induces the spatial separation of VBM and CBM, inhibiting the recombination of carriers. These findings have significant implications for the design and preparation of efficient photocatalysts.

15.
Molecules ; 29(12)2024 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-38930926

RESUMO

The effective treatment and recovery of fracturing wastewater has always been one of the difficult problems to be solved in oilfield wastewater treatment. Accordingly, in this paper, photocatalytic-coupled low-temperature plasma technology was used to degrade the simulated wastewater containing hydroxypropyl guar, the main component of fracturing fluid. Results indicated that hydroxypropyl-guar wastewater could be degraded to a certain extent by either photocatalytic technology or plasma technology; the chemical oxygen demand and viscosity of the treated wastewater under two single-technique optimal conditions were 781 mg·L-1, 0.79 mPa·s-1 and 1296 mg·L-1, 1.01 mPa·s-1, respectively. Furthermore, the effective coupling of AgIn5S8/gC3N4 photocatalysis and dielectric-barrier discharge-low-temperature plasma not only enhanced the degradation degree of hydroxypropyl guar but also improved its degradation efficiency. Under the optimal conditions of coupling treatment, the hydroxypropyl-guar wastewater achieved the effect of a single treatment within 6 min, and the chemical oxygen demand and viscosity of the treated wastewater reduced to below 490 mg·L-1 and 0.65 mPa·s-1, respectively. In the process of coupled treatment, the AgIn5S8/gC3N4 could directly absorb the light and strong electric field generated by the system discharge and play an important role in the photocatalytic degradation, thus effectively improving the energy utilization rate of the discharge system and enhancing the degradation efficiency of hydroxypropyl guar.

16.
Molecules ; 29(9)2024 Apr 24.
Artigo em Inglês | MEDLINE | ID: mdl-38731422

RESUMO

In this study, S-doped graphitic carbon nitride (S-C3N4) was prepared using the high-temperature polymerization method, and then S-C3N4/AgCdS heterojunction photocatalyst was obtained using the chemical deposition method through loading Ag-doped CdS nanoparticles (AgCdS NPs) on the surface of S-C3N4. Experimental results show that the AgCdS NPs were evenly dispersed on the surface of S-C3N4, indicating that a good heterojunction structure was formed. Compared to S-C3N4, CdS, AgCdS and S-C3N4/CdS, the photocatalytic performance of S-C3N4/AgCdS has been significantly improved, and exhibits excellent photocatalytic degradation performance of Rhodamine B and methyl orange. The doping of Ag in collaboration with the construction of a Z-scheme heterojunction system promoted the effective separation and transport of the photogenerated carriers in S-C3N4/AgCdS, significantly accelerated its photocatalytic reaction process, and thus improved its photocatalytic performance.

17.
Environ Geochem Health ; 46(3): 76, 2024 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-38367100

RESUMO

The escalating global industrial expansion has led to the extensive release of organic compounds into water bodies, resulting in substantial pollution and posing severe threats to both human health and the ecosystem. Among common micropollutants, bisphenol A (MP-BA) has emerged as a significant endocrine-disrupting chemical with potential adverse effects on human health and the environment. This study aims to develop an efficient photocatalyst, specifically by incorporating palladium-doped graphitic carbon nitride (Pd@GCN), to eliminate MP-BA pollutants present in industrial wastewater. The examination of optical properties and photoluminescence indicates that incorporating Pd into GCN enhances the visible light absorption spectra, which extends beyond 570 nm, and accelerates the separation rate of electron-hole pairs. The photocatalytic degradation efficiency of MP-BA increases from 81.7 to 98.8% as the solution pH rises from 5.0 to 9.0. Moreover, Pd@GCN significantly improves the removal rate of MP-BA in wastewater samples, reaching an impressive 92.8% after 60 min of exposure to solar light. Furthermore, the Pd@GCN photocatalyst exhibits notable reusability over six cycles of MP-BA degradation, indicating its promising potential for the treatment of organic pollutants in wastewater under solar light conditions.


Assuntos
Poluentes Ambientais , Grafite , Compostos de Nitrogênio , Fenóis , Águas Residuárias , Humanos , Paládio , Ecossistema , Compostos Benzidrílicos
18.
Environ Geochem Health ; 46(7): 219, 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38849667

RESUMO

This study investigates the removal of amoxicillin micropollutants (AM) from hospital wastewater using CoMoO4-modified graphitic carbon nitride (CMO/gCN). Consequently, CMO/gCN exhibits notable improvements in visible light absorption and electron-hole separation rates compared to unmodified gCN. Besides, CMO/gCN significantly enhances the removal efficiency of AM, attaining an impressive 96.5%, far surpassing the performance of gCN at 48.6%. Moreover, CMO/gCN showcases outstanding reusability, with AM degradation performance exceeding 70% even after undergoing six cycles of reuse. The removal mechanism of AM employing CMO/gCN involves various photoreactions of radicals (•OH, •O2-) and amoxicillin molecules under light assistance. Furthermore, CMO/gCN demonstrates a noteworthy photodegradation efficiency of AM from hospital wastewater, reaching 92.8%, with a near-complete reduction in total organic carbon levels. Detailed discussions on the practical applications of the CMO/gCN photocatalyst for removal of micropollutants from hospital wastewater are provided. These findings underline the considerable potential of CMO/gCN for effectively removing various pollutants in environmental remediation strategies.


Assuntos
Amoxicilina , Grafite , Oxirredução , Águas Residuárias , Poluentes Químicos da Água , Amoxicilina/química , Águas Residuárias/química , Grafite/química , Poluentes Químicos da Água/química , Fotólise , Hospitais , Compostos de Nitrogênio/química , Catálise , Purificação da Água/métodos
19.
J Environ Sci (China) ; 141: 287-303, 2024 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-38408829

RESUMO

Graphitic carbon nitride with nanorod structure (Nr-GCN) was synthesized using melamine as a precursor without any other reagents by hydrothermal pretreatment method. XRD, FTIR, SEM, N2 adsorption-desorption from BET, UV-Vis DRS spectroscopy, and photoluminescence were used to characterize the prepared samples. Also, the photoelectrochemical behavior of nanoparticles was studied by photocurrent transient response and cyclic voltammetry analysis. Polystyrene (PS) fibrous mat was fabricated by electrospinning technique and used as a support for the stabilization of the nanoparticles. The performance of the synthesized nanoparticles and photocatalytic fibers (PS/Nr-GCN) was evaluated in oilfield-produced water treatment under visible light irradiation. During this process, oil contaminants were adsorbed by hydrophobic polystyrene fibers and simultaneously degraded by Nr-GCN. The removal efficiency of chemical oxygen demand (COD) has been obtained 96.6% and 98.4% by Nr-GCN and PS/Nr-GCN, respectively, at the optimum conditions of pH 4, photocatalyst dosage 0.5 g/L, COD initial concentration 550 mg/L, and illumination time 150 min. The gas chromatography-mass spectroscopy analysis results showed 99.3% removal of total petroleum hydrocarbons using photocatalytic fibers of PS/Nr-GCN. The results demonstrated that the GCN has outstanding features like controllable morphology, visible-light-driven, and showing high potential in oily wastewater remediation. Moreover, the synergistic effect of adsorption and photocatalytic degradation is an effective technique in oilfield-produced water treatment.


Assuntos
Grafite , Nanotubos , Compostos de Nitrogênio , Poliestirenos , Adsorção , Campos de Petróleo e Gás
20.
Angew Chem Int Ed Engl ; : e202405902, 2024 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-38807439

RESUMO

The development of robust and reliable methods for the construction of C(sp2)-C(sp3) bonds is vital for accessing an increased array of structurally diverse scaffolds in drug discovery and development campaigns. While significant advances towards this goal have been achieved using metallaphotoredox chemistry, many of these methods utilise photocatalysts based on precious-metals due to their efficient redox processes and tuneable properties. However, due to the cost, scarcity, and toxicity of these metals, the search for suitable replacements should be a priority. Here, we show the use of commercially available heterogeneous semiconductor graphitic carbon nitride (gCN) as a photocatalyst, combined with nickel catalysis, for the cross-coupling between aryl halide and carboxylic acid coupling partners. gCN has been shown to engage in single-electron-transfer (SET) and energy-transfer (EnT) processes for the formation of C-X bonds, and in this manuscript we overcome previous limitations to furnish C-C over C-O bonds using carboxylic acids. A broad scope of both aryl halides and carboxylic acids is presented, and recycling of the photocatalyst demonstrated. The mechanism of the reaction is also investigated.

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