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1.
《环境科学学报(英文版)》2023,35(4):517-530
Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis. However, the traditional problems such as high recombination rate of photogenerated carriers limit its application. In this work, we introduce nitrogen deficiency into g-C3N4 to solve this problem a simple and safe in-situ reduction method. g-C3N4/CaCO3 was obtained by a simple and safe one-step calcination method with industrial-grade micron particles CaCO3. Cyano group modification was in-situ reduced during the thermal polymerization process, which would change the internal electronic structure of g-C3N4. The successful combination of g-C3N4 and CaCO3 and the introduction of cyanide have been proved by Fourier transform infrared spectroscopy and X-ray photoelectron spectrometer. The formation of the cyano group, an electron-absorbing group, promotes the effective separation of photogenic electron hole pairs and inhibits the recombination of photogenic carriers. These advantages result in the generation of more •O2− and 1O2 in the catalytic system, which increases the photocatalytic efficiency of nicotine degradation by ten times. Furthermore, the degradation process of nicotine has been studied in this work to provide a basis for the degradation of nicotine organic pollutants in the air. 相似文献
2.
Zhe Feng Lin Zeng Qingle Zhang Shifeng Ge Xinyue Zhao Hongjun Lin Yiming He 《环境科学学报(英文版)》2020,32(1):149-162
A graphite carbon nitride(g-C3N4) modified Bi4O5I2 composite was successfully prepared insitu via the thermal treatment of a g-C3N4/Bi OI precursor at 400°C for 3 hr.The as-prepared g-C3N4/Bi4O5I2 showed high photocatalytic performance in Methyl Orange(MO) degradation under visible light.The best sample presented a degradation rate of 0.164 min-1,which is... 相似文献
3.
《环境科学学报(英文版)》2023,35(3):349-361
At present, the high re-combination rate of photogenerated carriers and the low redox capability of the photocatalyst are two factors that severely limit the improvement of photocatalytic performance. Herein, a dual Z-scheme photocatalyst bismuthzirconate/graphitic carbon nitride/silver phosphate (Bi2Zr2O7/g-C3N4/Ag3PO4 (BCA)) was synthesized using a co-precipitation method, and a dual Z-scheme heterojunction photocatalytic system was established to decrease the high re-combination rate of photogenerated carriers and consequently improve the photocatalytic performance. The re-combination of electron-hole pairs (e− and h+) in the valence band (VB) of g-C3N4 increases the redox potential of e− and h+, leading to significant improvements in the redox capability of the photocatalyst and the efficiency of e−-h+ separation. As a photosensitizer, Ag3PO4 can enhance the visible light absorption capacity of the photocatalyst. The prepared photocatalyst showed strong stability, which was attributed to the efficient suppression of photo-corrosion of Ag3PO4 by transferring the e− to the VB of g-C3N4. Tetracycline was degraded efficiently by BCA-10% (the BCA with 10 wt.% of AgPO4) under visible light, and the degradation efficiency was up to 86.2%. This study experimentally suggested that the BCA photocatalyst has broad application prospects in removing antibiotic pollution. 相似文献
4.
Yixiao Wu Chunlong Chen Shu He Xuesong Zhao Shaobin Huang Gongchang Zeng Yingying You Ying Cao Lishan Niu 《环境科学学报(英文版)》2021,33(1):100-109
In this study, different carbon quantum dots (CQDs)/NaBiO3 hybrid materials were synthesized as photocatalysts to effectively utilize visible light for the photocatalytic degradation of contaminants effectively. These hybrid materials exhibit an enhanced photocatalytic reduction of hexavalent chromium (Cr(VI)) in the aqueous medium. Zero-dimensional nanoparticles of CQDs were embedded within the two-dimensional NaBiO3 nanosheets by the hydrothermal process. Compared with that of the pure NaBiO3 nanosheets, the photocatalytic performance of the hybrid catalysts was significantly high and 6 wt.% CQDs/NaBiO3 catalyst exhibited better photocatalytic performance. We performed the first-principles density functional theory calculations to study the interfacial properties of pure NaBiO3 nanosheets and hybrid photocatalysts, and confirmed the CQDs played an important role in the CQDs/NaBiO3 composites. The experimental results indicated that the enhanced reduction of Cr(VI) was probably due to the high loading of CQDs (electron acceptor) on NaBiO3, which made NaBiO3 nanomaterials to respond in visible light and significantly improved their electron-hole separation efficiency. 相似文献
5.
《环境科学学报(英文版)》2023,35(2):310-318
BiFeO3 (BFO), as a kind of narrow band-gap semiconductor material, has gradually emerged advantages in the application of photocatalysis. In this paper, Ca doped BFO nanoparticles Bi0.9Ca0.1FeO3 (BCFO) were prepared by sol-gel method. And BCFO and CdS nanocomposites with two morphologies were obtained by controlling the time of loading CdS under a low temperature liquid phase process. It is found that the band gap becomes narrower after doping Ca into BFO, which is conducive to the absorption of visible light. Among all the samples, the composite of CdS nanowires and BCFO nanoparticles obtained by reaction time of 10 min has the best photocatalytic performance. The degradation rate of Methyl Orange solution was 94% after 90 min under visible light irradiation, which was much higher than that of pure BCFO and CdS. Furthermore, significant enhancement in the degradation rate (100% degradation in 60 min) can be achieved in poled samples after electric polarization process. The highest degradation rate is due to the promoted separation of photogenerated carriers induced by the internal polarization field and the formation of S-scheme heterostructure between BCFO and CdS. Such BCFO-CdS nanocomposites may bring new insights into designing highly efficient photocatalyst. 相似文献
6.
Renjun Li Yanan Zhou Xueqian Wang Langlang Wang Ping Ning Lei Tao Jun Cai 《环境科学学报(英文版)》2021,33(4):384-397
La2O3/Bi2O3 photocatalysts were prepared by impregnation of Bi2O3 with an aqueous solution of lanthanum precursor followed by calcination at different temperatures. The composite materials were used for the first time for the photocatalytic removal of Hg0 from a simulated flue gas under UV light irradiation. The results showed that the sample containing 6 wt.% La2O3 and calcined at 500°C has the highest dispersion of the active sites, which was promoted by the strong interaction with the support (i.e., the formation of Bi-O-La species). Since they are fully accessible on the surface, the material also exhibits excellent optical properties while the heterojunction formed in La2O3/Bi2O3 promotes the separation and migration of photoelectron-hole pairs and thus Hg0 oxidation efficiency is enhanced. The effects of the various factors (e.g., the reaction temperature and composition of the simulated flue gas (i.e., O2, NO, H2O, and SO2)) on the efficiency of the Hg0 photocatalytic oxidation were investigated. The results demonstrated that O2 and SO2 enhanced the efficiency of the reaction while the reaction temperature, NO, and H2O had an inhibitory effect. 相似文献
7.
Weijia Zhao Hongyun Niu Yongliang Yang Hongzhou Lv Jungang Lv Yaqi Cai 《环境科学学报(英文版)》2022,34(2):244-257
The construction of heterojunction photocatalysts for efficiently utilizing solar energy has attracted considerable attention to solve the energy crisis and reduce environmental pollution. In this study, we use the energy released from an easily-occurred exothermic chemical reaction to serve as the drive force to trigger the formation of Cd S and C3N4 nanocomposites which are successfully fabricated with cadmium nitrate and thiourea without addition of any solvents and prot... 相似文献
8.
《环境科学学报(英文版)》2023,35(2):617-629
In this work, a novel dual Z-scheme Bi2WO6/g-C3N4/black phosphorus quantum dots (Bi2WO6/g-C3N4/BPQDs) composites were fabricated and utilized towards photocatalytic degradation of bisphenol A (BPA) under visible-light irradiation. Optimizing the content of g-C3N4 and BPQDs in Bi2WO6/g-C3N4/BPQDs composites to a suitable mass ratio can enhance the visible-light harvesting capacity and increase the charge separation efficiency and the transfer rate of excited-state electrons and holes, resulting in much higher photocatalytic activity for BPA degradation (95.6%, at 20 mg/L in 120 min) than that of Bi2WO6 (63.7%), g-C3N4 (25.0%), BPQDs (8.5%), and Bi2WO6/g-C3N4 (79.6%), respectively. Radical trapping experiments indicated that photogenerated holes (h+) and superoxide radicals (•O2−) played crucial roles in photocatalytic BPA degradation. Further, the possible degradation pathway and photocatalytic mechanism was proposed by analyzing the BPA intermediates. This work also demonstrated that the Bi2WO6/g-C3N4/BPQDs as effective photocatalysts was stable and have promising potential to remove environmental contaminants from real water samples. 相似文献
9.
A series of functional organic-metal AgCl-decorated graphitic carbon nitride(AgCl-CNx)composites were synthesized and applied for the degradation of oxalic acid(OA)under visible light.The highest photocatalytic activity was achieved with AgCl decoration ratio of1.0(denoted as AgCl-CN_(1.0)).The pseudo-first-order constant for OA degradation was 0.0722min-1 with the mineralization efficiency of 90.80%after 60 min reaction in the photocatalytic process with AgCl-CN_(1.0).A variety of characterization techniques including BrunauerEmmett-Teller,X-ray diffraction,scanning electron microscope,transmission electron microscopy,X-ray photoelectron spectroscopy,Fourier transform infrared spectra,ultraviolet-visible diffuse reflectance spectra,photoluminescence,and Mott-Schottky were utilized to elucidate the physicochemical,microstructure,and optical properties contributing to the improvement of the photocatalytic performance.The results showed that AgClCN_(1.0)had an oblate flaky erythrocyte-like structure with a moderate band gap energy of~3.00 eV.In addition,the effects of the key parameters(i.e.,AgCl-CN_(1.0) dosage,initial OA concentration,solution pH,and presence of natural organic matter)on OA degradation were systematically investigated.Radical scavenger experiments indicated that photogenerated holes,electrons,superoxide anion radicals,and hydroxyl radicals were the dominant reactive species.Moreover,AgCl-CN_(1.0) exhibited excellent stability and reusability for OA degradation without detectable Ag~+release in the solution over multiple reaction cycles.The efficient OA mineralization could be mainly ascribed to the moderate specific surface area,increased numbers of active sites,and effective interfacial charge transfer of AgCl-CN_(1.0).Overall,the AgCl-CN_(1.0) composite was demonstrated to be a highly efficient,stable,and recoverable photocatalyst. 相似文献
10.
Here we reported an effective method to solve the rate-limiting steps, such as the reduction of Fe3+ to Fe2+ and an invalid decomposition of H2O2 in a conventional Fenton-like reaction. A magnetic heterogeneous photocatalyst, Fe3O4-schwertmannite(Fe3O4-sch) was successfully developed by adding Fe3O4 in the formation process of schwertmannite. Fe3O4-sch shows excelle... 相似文献
11.
《环境科学学报(英文版)》2023,35(4):249-262
AgCl/ZnO/g-C3N4, a visible light activated ternary composite catalyst, was prepared by combining calcination, hydrothermal reaction and in-situ deposition processes to treat/photocatalyse tetracycline hydrochloride (TC-HCl) from pharmaceutical wastewater under visible light. The morphological, structural, electrical, and optical features of the novel photocatalyst were characterized using scanning electron microscopy (SEM), UV-visible light absorption spectrum (UV–Vis DRS), X-ray diffractometer (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), and transient photocurrent techniques. All analyses confirmed that the formation of heterojunctions between AgCl/ZnO and g-C3N4 significantly increase electron-hole transfer and separation compared to pure ZnO and g-C3N4. Thus, AgCl/ZnO/g-C3N4 could exhibit superior photocatalytic activity during TC-HCl assays (over 90% removal) under visible light irradiation. The composite could maintain its photocatalytic stability even after four consecutive reaction cycles. Hydrogen peroxide (H2O2) and superoxide radical (·O2) contributed more than holes (h+) and hydroxyl radicals (·OH) to the degradation process as showed by trapping experiments. Liquid chromatograph-mass spectrometer (LC-MS) was used for the representation of the TC-HCl potential degradation pathway. The applicability and the treatment potential of AgCl/ZnO/g-C3N4 against actual pharmaceutical wastewater showed that the composite can achieve removal efficiencies of 81.7%, 71.4% and 69.0% for TC-HCl, chemical oxygen demand (COD) and total organic carbon (TOC) respectively. AgCl/ZnO/g-C3N4 can be a prospective key photocatalyst in the field of degradation of persistent, hardly-degradable pollutants, from industrial wastewater and not only. 相似文献
12.
The existence of electrolytes in aquatic environment on the photocatalytic performance and coagulation of nanodispersed TiO2 hydrosol and the corresponding photocatalytic alteration were investigated by studying cations (Na+, K+, Ca 2+, Mg2+, and Al3+). The photocatalysis reactions of nano TiO2 with different dosages of electrolytes were measured by monitoring the degradation of Rhodamine B (RhB) under ultraviolet A (UV-A) irradiation over time. The results showed that the photocatalytic performance of TiO2 was improved by the presence of Al3+, while the performance was impaired by the other tested cations. The negative influences of divalent ions on the photocatalytic performance of TiO2 were more significant than monovalent ions. The TiO2 sol dispersed stable at nano scale at low concentration of electrolyte (< 0.01?mol/L) with slight change of pH, and coagulated into micro sizes at high concentration of electrolytes (> 0.1?mol/L) with larger increase or decrease of pH. The positive effects of Al3+ on the photodegradation rate of RhB might relate to the strong hydrolytic action of Al3+ in aquatic solutions. The photocatalytic processes of TiO2 in the presence of all ions followed the Langmuir-Hinshelwood model, and the reaction kinetic constant was increased with the decrease of pH caused by different cations. These work suggested a new perspective about the relationship between coagulation and photocatalytic performance of TiO2 hydrosols in electrolyte with hydrolysable cations, which demonstrated that TiO2 hydrosols may be suitable as photocatalysts in aquatic environments. 相似文献
13.
Liqin Yang Jun Zhao Caijun Wang Zheng Wang Cuijuan Xing Hao Guo Yuman Wang Zhiju Zhao Zhangji Hu Zhenyu Cai 《环境科学学报(英文版)》2021,33(11):114-122
Streptomycin (STR) plays an essential role in bacterial infection treatments. Selectivity and sensitivity of photoelectrochemical (PEC) sensors are the two most important parameters, which can be measured using the photosensitivity of its active material. We prepared a novel PEC sensor to detect STR using Bi/BiVO4/LDH (layered double hydroxides) heterostructures as an active material, which is photoactive in the visible light wavelength range. The simultaneous presence of LDH and Bi/BiVO4 enhanced the material photocurrent response, which was linear to the STR concentrations in the 0.01–500 nmol/L range. The STR detection limit by this sensor was 0.0042 nmol/L. Our novel PEC-based sensing strategy includes using an ultra-sensitive and highly selective sensor for STR detection. Additionally, the two-pot synthesis of Bi/BiVO4/LDH developed in this work is environmentally friendly. 相似文献
14.
Yupei Long Chenchen Yuan Xiaomin Wang Dongyan Jin Hong Zhou Qiongyin Wang Chenyang Lu Yuqi Chen Yanqing Cong Qi Wang Yi Zhang 《环境科学学报(英文版)》2021,33(6):113-127
Dielectric barrier discharge (DBD) plasma applied as surface treatment technology was employed for the modification of Ag2O and graphitic carbon nitride (g-C3N4) powders. Subsequently, the pretreated powders were sequentially loaded onto TiO2 nanorods (TiO2-NRs) via electro-deposition, followed by calcination at N2 atmosphere. The results indicated that at the optimal plasma discharge time of 5 min for modification of g-C3N4 and Ag2O, photocurrent density of ternary composite was 6 times to bare TiO2-NRs under UV-visible light irradiation. Phenol was degraded by using DBD plasma-modified g-C3N4/Ag2O/TiO2-NRs electrode to analyze the photoelectrocatalytic performance. The removal rate of phenol for g-C3N4-5/Ag2O-5/TiO2-NRs electrode was about 3.07 times to that for TiO2-NRs electrode. During active species scavengers’ analysis, superoxide radicals and hydroxyl radicals were the main oxidation active species for pollutants degradation. A possible electron-hole separation and transfer mechanism of ternary composite with high photoelectrocatalytic performance was proposed. 相似文献
15.
《环境科学学报(英文版)》2023,35(3):388-400
Removing large concentrations of organic pollutants from water efficiently and quickly under visible light is essential to developing photocatalytic technology and improving solar energy efficiency. This study used a simple hydrothermal method to prepare a non-metallic, S-doped NaTaO3 (S-NTO) photocatalyst, which was then loaded onto biochar (BC) to form a S-NTO/BC composite photocatalyst. After uniform loading onto BC, the S-NTO particles transformed from cubic to spherical. The photogenerated electron-hole pair recombination probability of the composite photocatalyst was significantly lower than those of the NTO particles. The light absorption range of the catalyst was effectively widened from 310 nm UV region to visible region. In addition, a dual-effect catalytic system was constructed by introducing peroxymonosulfate (PMS) into the environment of the pollution to be degraded. The Rhodamine B, Methyl Orange, Acid Orange 7, tetracycline, and ciprofloxacin degradation efficiency at 40 mg/L reached 99.6%, 99.2%, 84.5%, 67.1%, and 70.7%, respectively, after irradiation by a 40 W lamps for 90 min. The high-efficiency visible-light catalytic activity of the dual-effect catalytic system was attributed to doping with non-metallic sulfur and loading of catalysts onto BC. The development of this dual-effect catalytic system provides new ideas for quickly and efficiently solving the problem of high-concentration organic pollution in aqueous environments, rationally and fully utilizing solar energy, and expanding the application of photocatalytic technology to practice. 相似文献
16.
Yongjin Li Yingying Zhang Jiajing Wang Youzhun Fan Taizhong Xiao Zhaoyi Yin Tianhui Wang Jianbei Qiu Zhiguo Song 《环境科学学报(英文版)》2022,34(5):76-87
For better use of solar energy,the development of efficient broadband photocatalyst has attracted extraordinary attention.In this study,a ternary composite consisting of Sr2 LaF7:Yb3+,Er3+ upconversion(UC) nanocrystals and Bi nanoparticles loaded BiOBr nanosheets with oxygen vacancies(OVs,SLFBB) was designed and synthesized by multistep solvent-thermal method.Mechanisms of in-situ formation of Bi nanoparticles and OVs in BiOBr/Sr2 LaF7<... 相似文献
17.
To utilize visible light more effectively in photocatalytic reactions, a fly ash cenosphere (FAC)-supported CeO2-BiV04 (CeO2-BiVO4/FAC) composite photocatalyst was prepared by modified metalorganic decomposition and impregnation methods. The physical and photophysical properties of the composite have been characterized by X-ray diffraction (XRD), scanning electron microscope (SEM) and energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), and UV-Visible diffuse reflectance spectra. The XRD patterns exhibited characteristic diffraction peaks of both BiVO4 and Ce02 crystalline phases. The XPS results showed that Ce was present as both Ce4+ and Ce3+ oxidation states in Ce02 and dispersed on the surface of BiV04 to constitute a p-n heterojunction composite. The absorption threshold of the CeO2-BiVO4/FAC composite shifted to a longer wavelength in the UV-Vis absorption spectrum compared to the pure Ce02 and pure BiV04. The composites exhibited enhanced photocatalytic activity for Methylene Blue (MB) degradation under visible light irradiation. It was found that the 7.5 wt.% CeO2-BiVO4/FAC composite showed the highest photocatalytic activity for MB dye wastewater treatment. 相似文献
18.
《环境科学学报(英文版)》2023,35(2):414-428
MXenes, a new family of two-dimensional transition metal carbides or nitrides, have attracted tremendous attention for various applications due to their unique properties such as good electrical conductivity, hydrophilicity, and ion intercalability. In this work, Ti3C2 MXene, or MX, is converted to MX-TiO2 composites using a simple and rapid microwave hydrothermal treatment in HCl/NaCl mixture solution that induces formation of fine TiO2 particles on the MX parent structure and imparts photocatalytic activity to the resulting MX-TiO2 composites. The composites were used for enrofloxacin (ENR), a frequently found contaminating antibiotic, removal from water. The relative amount of the MX and TiO2 can be controlled by controlling the hydrothermal temperature resulting in composites with tunable adsorption/photocatalytic properties. NaCl addition was found to play important role as composites synthesized without NaCl could not adsorb enrofloxacin well. Adding NaCl into the hydrothermal treatment causes sodium ions to be simultaneously intercalated into the composite structure, improving ENR adsorption greatly from 1 to 6 mg ENR/g composite. It also slows down the MX to TiO2 conversion leading to a smaller and more uniform distribution of TiO2 particles on the structure. MX-TiO2/NaCl composites, which have sodium intercalated in their structures, showed both higher ENR adsorption and photocatalytic activity than composites without NaCl despite the latter having higher TiO2 content. Adsorbed ENR on the composites can be efficiently degraded by free radicals generated from the photoexcited TiO2 particles, leading to high photocatalytic degradation efficiency. This demonstrates the synergetic effect between adsorption and photocatalytic degradation of the synthesized compounds. 相似文献
19.
《环境科学学报(英文版)》2023,35(3):47-60
Photocatalytic degradation was considered as a best strategy for the removal of antibiotic drug pollutants from wastewater. The photocatalyst of ABC (Ag2CO3/BiOBr/CdS) composite synthesized by hydrothermal and precipitation method. The ABC composite used to investigate the degradation activity of tetracycline (TC) under visible light irradiation. The physicochemical characterization methods (e.g. scanning electron microscopy (SEM), transmission electron microscopy (TEM), high resolution-transmission electron microscopy (HR-TEM), ultraviolet visible spectroscopy (UV), photoluminescence (PL) and time resolved photoluminescence (TRPL) clearly indicate that the composite has been construct successfully that enhances the widened visible light absorption, induces charge transfer and separation efficiency of electron – hole pairs. The photocatalytic activity of all samples was examined through photodegradation of tetracycline in aqueous medium. The photocatalytic degradation rate of ABC catalyst could eliminate 98.79% of TC in 70 min, which is about 1.5 times that of Ag2CO3, 1.28 times that of BiOBr and 1.1 times that of BC catalyst, respectively. The role of operation parameters like, TC concentration, catalyst dosage and initial pH on TC degradation activity were studied. Quenching experiment was demonstrated that ·OH and O2·− were played a key role during the photocatalysis process that was evidently proved in electron paramagnetic resonance (EPR) experiment. In addition, the catalyst showed good activity perceived in reusability and stability test due to the synergistic effect between its components. The mechanism of degradation of TC in ABC composite was proposed based on the detailed analysis. The current study will give an efficient and recyclable photocatalyst for antibiotic aqueous pollutant removal. 相似文献
20.
Yao Xiao Honghong Lyu Chengliang Yang Beibei Zhao Lan Wang Jingchun Tang 《环境科学学报(英文版)》2021,33(5):93-107
In order to enhance the removal performance of graphitic carbon nitride (g-C3N4) on organic pollutant, a simultaneous process of adsorption and photocatalysis was achieved via the compounding of biochar and g-C3N4. In this study, g-C3N4 was obtained by a condensation reaction of melamine at 550°C. Then the g-C3N4/biochar composites were synthesized by ball milling biochar and g-C3N4 together, which was considered as a simple, economical, and green strategy. The characterization of resulting g-C3N4/biochar suggested that biochar and g-C3N4 achieved effective linkage. The adsorption and photocatalytic performance of the composites were evaluated with enrofloxacin (EFA) as a model pollutant. The result showed that all the g-C3N4/biochar composites displayed higher adsorption and photocatalytic performance to EFA than that of pure g-C3N4. The 50% g-C3N4/biochar performed best and removed 45.2% and 81.1% of EFA (10 mg/L) under darkness and light with a dosage of 1 mg/mL, while g-C3N4 were 19.0% and 27.3%, respectively. Besides, 50% g-C3N4/biochar showed the highest total organic carbon (TOC) removal efficiency (65.9%). Radical trapping experiments suggested that superoxide radical (?O2?) and hole (h+) were the main active species in the photocatalytic process. After 4 cycles, the composite still exhibited activity for catalytic removal of EFA. 相似文献