Environmental Science-Nano
·
2025
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IF 5.1
Qi Xu,Xu Du,Qin Zhou,Lian Yang,Kuixiao Li,Wei Wang,Gang Wang,Guisheng Xu,Feng Xiao
Photocatalytic oxidation technology is recognized as an effective method for removing antibiotics from wastewater. In this work, a novel montmorillonite/graphitic carbon nitride (Mt/g-C3N4) composite was synthesized via a facile thermal polycondensation approach. The optimal 1% Mt/g-C3N4 photocatalyst demonstrated an excellent chlortetracycline (CTC) degradation rate of 0.0353 min-1 under visible light, which is about 42% higher than pristine g-C3N4. Electron spin resonance (ESR) and radical quenching experiments revealed that the •O2- plays the most significant role in the photocatalytic oxidation of CTC, while •OH, 1O2 and h+ also contribute, but not in dominant places. This study elucidates the mechanism by which the photocatalytic activity is enhanced. The improvements are ascribed to the extended absorption of visible light, efficient charge separation, and the inhibition of photo-induced electron-hole pair recombination, following the successful intercalation of g-C3N4 nanosheets into montmorillonite layers. Additionally, HPLC-QTOF-MS was employed to identify the transformation products of CTC, and the primary degradation pathways were elucidated. Furthermore, the ecotoxicity of the transformation products was evaluated using ECOSAR software.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Fei Gao,Weijun Chen,Ye Li,Long Shao,Li He
Organic-inorganic hybrid perovskite films with excellent surface morphology and large grain sizes are crucial for achieving high-performance perovskite solar cells (PSCs). To reduce production costs and meet the growing demand for lightweight thin solar cells, developing ultra-thin absorber layers is an effective approach. However, defects and trap sites are inevitably formed on the surfaces of solution-processed perovskite films. Herein, we present an innovative method that directly incorporates graphite carbon nitride/carbon quantum dots (g-C 3 N 4 /CQDs) into the perovskite precursor solution, using them as structural template to modulate film growth. The g-C 3 N 4 /CQDs delay crystallization through the formation of a MA·g-C 3 N 4 /CQDs intermediate adduct, which reduces light absorption loss by increasing enlarge grain size and minimizing numerous pinhole defects in thin perovskite films. Additionally, the amide bond formed between g-C 3 N 4 and CQDs can accelerate charge transport, as demonstrated by density functional theory calculation. As a result, the PSCs based on high-quality 360 nm MAPbI 3 :g-C 3 N 4 /CQDs films achieved a champion power conversion efficiency of 20.49 %. The devices retained more than 90 % of their initial efficiency for over 500 h in air without encapsulation. This work not only provides valuable insights into the role of 2D/0D carbon-based heterojunctions in PSCs, but also provides a straightforward technique for crystallization regulation to achieve efficient and stable PSCs.
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Journal of Water Process Engineering
·
2024
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IF 6.3
Yali Song,Ziyan Li,Shuaibin Li,Cairong Yang,Long Huang,Xiaojing Zhang,Qiong Wang,Hongzhong Zhang
Holes and O 2 − have been proved the primary species for sulfamethoxazole (SMX) degradation in g-C 3 N 4 photocatalytic system. On the basis, P doped g-C 3 N 4 (PCN) photocatalyst with midgap states was prepared by the polymerization of urea and etidronic acid, in order to enhance the role of main species in SMX removal via tailoring band gap structure. Compared with g-C 3 N 4 , the energy gap, CB position and VB position of PCN change little, however, PCN shows lower recombination efficiency of photogenerated carriers, strong adsorption and harvest of more visible light due to the midgap states induced by P doping, which is favorable to improve the photocatalytic activity. When the additive amount of etidronic acid is 0.03 g for 10 g urea, the obtained PCN-0.03 exhibits excellent visible-driven photocatalytic ability on SMX degradation. The kinetic constant is 2.1 times than that of pure g-C 3 N 4 . Electron spin resonance tests and trapping experiments imply that OH, holes and O 2 − are produced and enhanced by PCN-0.03 under visible light in comparison with g-C 3 N 4 . Holes and O 2 − take the primary role in SMX photodegradation . The detailed and systematical work may provide an effective strategy for water purification , especially containing SMX.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
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IF 5.8
Tian Tian,Dingze Lu,Bang Zhao,Kiran Kumar Kondamareddy,Wenju Gu,Jingxuan Yang,Hongjuan Hao,Huiqing Fan,Wingkei Ho
It is crucial to elucidate the intrinsic relationship between defects in g-C 3 N 4 (pristine graphitic carbon nitride, here onwards bare carbon nitride-BCN) and the enhancement of photogenerated carrier dynamics and photocatalytic performance. Three types of defective g-C 3 N 4 are prepared by defect engineering, called CVCN (carbon vacancies containing carbon nitride), NVCN (nitrogen vacancies containing carbon nitride), and OBCN (oxygen doped bulk carbon nitride). Various characterization techniques are employed to examine the materials' crystalline structure, chemical bonds, surface area, pore properties, light response, carrier recombination, vacancy/doping types, and carrier mobility. Ab initio calculations via VASP further elucidated band structure and charge distribution. Visible light-assisted Rhodamine B (RhB) degradation and hydrogen peroxide production experiments revealed that defect engineering significantly enhanced the photocatalytic degradation capacity of g-C 3 N 4 , with OBCN showing the highest RhB degradation rate which is 6.26 times higher than that of BCN (bulk carbon nitride), but suffering from photo-corrosion and its main reactive substances are h + and ·O 2 - ; while NVCN exhibited the best hydrogen peroxide production capacity which is 1.83 times higher than that of BCN, the main active species is ·O 2 - . Through the Vienna Ab initio Simulation Package software (VASP), the projection enhanced wave method is used to model and analyze the first principles calculation of the band structure of the samples and the change of elemental differential charge. The occurrence of defects slightly modulated the energy band structure of the photocatalyst, significantly inhibited the recombination phenomenon of photogenerated carriers, promoted the separation of photogenerated carriers, and ultimately improved the photocatalytic activity.
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Polymers
·
2024
·Vol. 16
·期 16
·2317
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IF 4.7
Peng Jiang,Kun Wang,Wenrui Liu,Yuhang Song,Runtian Zheng,Lihua Chen,Baolian Su
Converting carbon dioxide (CO2) into high-value-added chemicals using solar energy is a promising approach to reducing carbon dioxide emissions; however, single photocatalysts suffer from quick the recombination of photogenerated electron–hole pairs and poor photoredox ability. Herein, silver (Ag) nanoparticles featuring with localized surface plasmon resonance (LSPR) are combined with g-C3N4to form a Schottky junction for photothermal catalytic CO2reduction. The Ag/g-C3N4exhibits higher photocatalytic CO2reduction activity under UV-vis light; the CH4and CO evolution rates are 10.44 and 88.79 µmol·h−1·g−1, respectively. Enhanced photocatalytic CO2reduction performances are attributed to efficient hot electron transfer in the Ag/g-C3N4Schottky junction. LSPR-induced hot electrons from Ag nanoparticles improve the local reaction temperature and promote the separation and transfer of photogenerated electron–hole pairs. The charge carrier transfer route was investigated by in situ irradiated X-ray photoelectron spectroscopy (XPS). The three-dimensional finite-difference time-domain (3D-FDTD) method verified the strong electromagnetic field at the interface between Ag and g-C3N4. The photothermal catalytic CO2reduction pathway of Ag/g-C3N4was investigated using in situ diffuse reflectance infrared Fourier transform spectra (DRIFTS). This study examines hot electron transfer in the Ag/g-C3N4Schottky junction and provides a feasible way to design a plasmonic metal/polymer semiconductor Schottky junction for photothermal catalytic CO2reduction.
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高影响因子
TALANTA
·
2024
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IF 5.6
Rui Liu,Chaojun Zhang,Tianheng Wu,Rijia Liu,Yuan Sun,Jing Ma
In this work, a novel HKUST-1/CoFe 2 O 4 /g-C 3 N 4 electrode was successfully prepared via the hydrothermal method and the high-temperature calcination method, which can be applied as an electrochemical sensor for the precise detection of ciprofloxacin (CIP) in physiological samples. The novel electrode was characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD) and Fourier-transform infrared spectroscopy (FT-IR), and its electrochemical performance was further evaluated via the cyclic voltammetry (CV) and differential pulse voltammetry (DPV) techniques. The results demonstrated that the HKUST-1/CoFe 2 O 4 /g-C 3 N 4 electrode exhibited an optimal linear range of 0.05–180 μmol L −1 for the CIP detection, which demonstrated a low limit of detection (LOD) of 0.0026 μmol L −1 and a low limit of quantitation (LOQ) of 0.0087 μmol L −1 , respectively. Additionally, the novel semiconductor sensors exhibited exceptional selectivity, stability and repeatability in the determination of CIP. The recovery rate of CIP was found to range from 98.00% to 104.00% in serum, with the relative standard deviations (RSD) below 2.62% (n = 5), while the recovery rate of CIP was found to range from 96.00% to 105.00%, with the RSD less than 3.23% (n = 5) in urine. The current study extends to the application of the semiconductor-based electrochemical sensors and offers a new approach for the clinical pharmaceutical analysis to ensure medication safety, which could provide valuable insights into the potential of semiconductor sensors for future clinical applications.
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Catalysis Science & Technology
·
2024
·
IF 4.4
Qianqian Shang,Hongbing Wang,Changjie Kan,Rui Ding,Yankai Li,Shiva Pandeya,Ziliang Li,Mahesh Kumar Joshi
Exfoliation and hetero-element doping are common procedures for band gap engineering and enhancing the photocatalytic properties of g-C3N4. A novel and facile strategy for simultaneous exfoliation and hetero-element doping is still in high demand. Herein, we prepared hydroxide and fluoride doped ultrathin g-C3N4 nanosheets through the single-step solvothermal exfoliation of bulk g-C3N4 (BCN) using varying concentrations of ethanol and hydrofluoric acid (HF). The microscopic and spectroscopic analysis confirmed the doping of hydroxide groups and fluoride groups (HO−/F− groups) into g-C3N4 nanosheets (HF-CNS). The HO− groups are primarily located at the terminal amino groups of the heptazine rings in HF-CNS, while the F− groups are likely incorporated into the g-C3N4 lattice by forming C–F bonds. The UV-vis absorption spectra and DFT calculations showed that the electronic band structure, and hence charge carrier recombination, can be tuned by varying the HF amount during the exfoliation process. BET-specific surface area was increased from 18.65 m2 g−1 for BCN to 159.87 m2 g−1 for HF-CNS. The transient photocurrent increased from 5 μA to 20 μA. HF-CNS significantly improved the photocatalytic degradation of tetracycline, achieving 99% removal in 50 minutes, compared to 20% for BCN. Tetracycline degradation followed pseudo-first-order kinetics, with apparent rate constants (K) increasing from 0.0028 min−1 for BCN to 0.0793 min−1 for HF-CNS, a 30-fold enhancement. The photocatalytic hydrogen evolution for HF-CNS was 11 times higher than that of BCN. The HF-CNS exhibited remarkable stability and reusability, indicating its potential as a promising photocatalyst for green hydrogen production and degradation of organic pollutants.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yujiao Zhang,Yan Wang,Zhao Hu,Jinshu Huang,Song Yang,Hu Li
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 Ti 3+ was precisely regulated at the interface of g-C 3 N 4 /TiO 2 Z-scheme heterojunction (g-C 3 N 4 /Ov-Ti 3+ -TiO 2 ) by optimizing the opening degree of the calcination system, showing excellent production rate of CO and CH 4 from CO 2 photoreduction under visible light. This photocatalytic system also exhibited prominent stability. Combining theoretical calculation and characterization, the introduction of Ov and isolated Ti 3+ on the interface could construct a charge transfer channel to break the forbidden transition of n → π*, improving the separation process of photoexcited electron-hole pairs. The photoexcited electrons weakened the covalent interaction of C O bonds to promote the activation of adsorbed inert CO 2 molecules, significantly reducing the energy barrier of the rate-limiting step during CO 2 reduction. This work demonstrates the great application potential of reasonably regulating heterojunction interface for efficient photocatalytic CO 2 reduction.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Mshari A. Alotaibi,Abdulrahman I. Alharthi,Adeel Ahmed,Awais Khalid
The disastrous pollution resulting from antibiotics may traverse extensive distances through water, presenting a serious threat to aquatic ecosystems and human well-being. The catalyst-assisted heterogeneous activation of peroxymonosulfate (PMS) has emerged as an intriguing technology for purifying such wastewater. Herein, we have designed cobalt tetroxide anchored over graphitic carbon nitride (Co 3 O 4 -g-C 3 N 4 ) catalysts through an impregnation and high-temperature calcination technique for the effective degradation of moxifloxacin (MOX) antibiotics from wastewater. The experiments revealed that the MOX degraded completely in 21 min in the Co 3 O 4 -g-C 3 N 4 /PMS system with a degradation kinetics constant of 0.1858 min −1 , faster than the Co 3 O 4 /PMS under optimal conditions ([Co 3 O 4 -g-C 3 N 4 ] = 0.5 g/L, [PMS] = 0.5 mM, [MOX] = 20 mg/L, pH = 6.3). Specifically, the higher degradation of MOX in the Co 3 O 4 -g-C 3 N 4 /PMS system can be credited to the larger surface area (97.22 m 2 /g) of the Co 3 O 4 -g-C 3 N 4 catalyst in comparison to the Co 3 O 4 (69.08 m 2 /g), which enhanced the accessibility of catalytic active sites and improved the PMS activating process. Further, the impression of varied operating factors and intervening anions on MOX abatement was also scrutinized. The production of reactive oxygen species was verified using quenching experiments and further validated by electron paramagnetic resonance analysis. The mechanistic degradation pathways of MOX were anticipated through the acquisition of degradation by-products. The mechanistic insight revealed that the PMS activation was caused by the transitions of Co 3+ /Co 2+ pairs in the reaction system. Overall, this study sheds new insights for subsequent research into the catalytic mechanism of heterogeneous catalysts utilizing PMS activation to degrade organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhiwei Zhao,Yu Li,Fei Wang,Zhitao Xu,Sai Zhang,Li Li,Junyu Fan,Jie Liu
Monitoring and regulating the formation of toxic byproducts in advanced oxidation processes (AOPs) is of great significance for their practical application in water treatment. In this work, we found that dichloroacetonitrile (DCAN), a common N-containing byproduct in chloramination disinfection, can be formed with the co-presence of g-C 3 N 4 and chloride in a peroxymonosulfate (PMS) system. The measured value was 12.01 μM within 12 h under the given conditions. Structure analysis of raw and used g-C 3 N 4 demonstrated that g-C 3 N 4 decomposition indeed occurred, and C = N bonds acted as primary active sites, releasing N resources for subsequent DCAN formation. Additionally, multiple parameters, including the reactant (i.e., g-C 3 N 4 , PMS, Cl - , phenol) dose and solution pH, were observed to remarkably affect the yield of DCAN. Phenol was identified as the organic precursor of DCAN and may cooperate with inorganic chloramine to promote DCAN formation via the decarboxylation pathway. This study highlights the generation of DCAN in N-involved catalyst-based AOPs and improves understanding of the DCAN formation mechanism.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yunfei Sun,Yaping Wang,Yun Chen,Junchao Qian,Feng Chen,Zelong Zhou,Chaoya Han,Yu Shi,Xiaowang Lu,Chaoying Ni
Bisphenol A (BPA), a prevalent organic pollutant found in wastewater environment, is notorious for its resistance to natural degradation, raising significant ecological and human health concerns. In this study, a “signal-on” photoelectrochemical aptasensing system was designed for detecting BPA in real water samples with high specificity and sensitivity. One-dimensional (1D) β-FeOOH nanobelts were synthesized on a two-dimensional (2D) porous carbon nitride (g-C 3 N 4 ) through an in-situ growth procedure. The β-FeOOH/g-C 3 N 4 nanocomposites demonstrated superior photoelectric conversion efficiency due to several factors: (i) The 1D nanobelt-like structure of β-FeOOH shortens the charge transfer path within the nanocomposite, enabling directional and rapid migration of photoinduced charges from the interior to the surface. (ii) β-FeOOH possesses strong visible absorption capabilities, enhancing the utilization of g-C 3 N 4 under photoexcitation, resulting in the generation of numerous photo-induced carriers. (iii) The in-situ formation of the β-FeOOH/g-C 3 N 4 heterojunction establishes an intimate interfacial contact, facilitating the rapid separation and transfer of charges between β-FeOOH and g-C 3 N 4 . A photoelectrochemical aptasensing platform based on the photoactive material of β-FeOOH/g-C 3 N 4 detects BPA with reduced photocurrent owing to the presence of BPA-aptamer macromolecules on the electrode surface. This BPA detection system exhibits excellent linearity over a wide concentration range from 10 pM to 10 nM, with high sensitivity (a detection limit of 3.5 pM), stability, specificity, and repeatability. Furthermore, this research offers a straightforward and rapid sensing platform for monitoring BPA enriched water environments.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Kexin Li,Bin He,Ruirui Wang,Ruiyi Yan,Ruirui Zhang,Ruixia Liu
The selective oxidation reaction of cyclohexane is one of the typical activated sp 3 C-H reactions, and its product adipic acid (AA) is the indispensable raw material used to produce nylon. However, subjecting to the inertness of C-H bond and the great reactivity of AA, the targeted transformation of cyclohexane remains a challenge. Here, the interfacial hydrogen bond (IHD) was developed by anchoring CeO 2 on graphite carbon nitride (g-C 3 N 4 ) surface, which could boost targeted acquisition adipic acid from aerobic oxidation of cyclohexane. The results indicated that the IHD effect can be flexibly regulated by changing the ratio of Ce 3+ /Ce 4+ , further optimizing the properties of surface OH species and Lewis acid sites. Under the synergistic effect of Ce 3+ /Ce 4+ and Lewis acid sites on reaction interface, the glorious performance (32.2% conversion of cyclohexane with 66.4% selectivity) was obtained over the as-prepared CeO 2 /g-C 3 N 4 IHD system. In addition, the interfacial adsorption properties of cyclohexane were explored by the virtue of in situ infrared spectroscopy, revealing the IHD effect could tune the adsorption behavior of cyclohexanone and further improve the selectivity of AA. This work disclosed that engineering the interface hydrogen bond effect between CeO 2 and g-C 3 N 4 provided feasible strategies to obtain excellent catalyst for cyclohexane oxidation.
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