Nanomaterials
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2021
·Vol. 11
·期 8
·2134
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IF 5.076
Fei-Fei Liu,Meng-Ru Li,Su-Chun Wang,Yu-Xue Zhang,Guang-Zhou Liu,Jin-Lin Fan
Graphene oxide (GO) is widely used in various fields and has raised concerns regarding its potential environmental fate and effect. However, there are few studies on its influence on coexisting pollutants. In this study, the phototransformation of GO and coexisting sulfamethazine (SMZ) under UV irradiation was investigated, with a focus on the role of reactive oxygen species. The results demonstrated that GO promoted the degradation of SMZ under UV irradiation. The higher the concentration of GO, the higher the degradation rate of SMZ, and the faster the first-order reaction rate. Two main radicals, ∙OH and1O2, both contributed greatly in terms of regulating the removal of SMZ. Cl−, SO42−, and pH mainly promoted SMZ degradation by increasing the generation of ∙OH, while humic acid inhibited SMZ degradation due to the reduction of ∙OH. Moreover, after UV illumination, the GO suspension changed from light yellow to dark brown with increasing absorbance at a wavelength of 225 nm. Raman spectra revealed that theID/IGratio slightly decreased, indicating that some of the functional groups on the surface of GO were removed under low-intensity UV illumination. This study revealed that GO plays important roles in the photochemical transformation of environmental pollutants, which is helpful for understanding the environmental behaviors and risks of nanoparticles in aquatic environments.Keywords:graphene oxide;sulfamethazine;phototransformation;free radicals
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2017
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IF 5.099
Guoyang Zhang,Bingdang Wu,Shujuan Zhang
Acetylacetone (AcAc) has proven to be a potent photo-activator in the degradation of color compounds. The effects of AcAc on the photochemical conversion of five colorless pharmaceuticals were for the first time investigated in both pure and natural waters with the UV/H 2 O 2 process as a reference. In most cases, AcAc played a similar role to H 2 O 2 . For example, AcAc accelerated the photodecomposition of carbamazepine, oxytetracycline , and tetracycline in pure water. Meanwhile, the toxicity of tetracyclines and carbamazepine were reduced to a similar extent to that in the UV/H 2 O 2 process. However, AcAc worked in a way different from that of H 2 O 2 . Based on the degradation kinetics, solvent kinetic isotope effect , and the inhibiting effect of O 2 , the underlying mechanisms for the degradation of pharmaceuticals in the UV/AcAc process were believed mainly to be direct energy transfer from excited AcAc to pharmaceuticals rather than reactive oxygen species-mediated reactions. In natural waters, dissolved organic matter (DOM) played a crucial role in the photoconversion of pharmaceuticals. The role of H 2 O 2 became negligible due to the scavenging effects of DOM and inorganic ions. Interestingly, in natural waters, AcAc first accelerated the photodecomposition of pharmaceuticals and then led to a dramatic reduction with the depletion of dissolved oxygen. Considering the natural occurrence of diketones, the results here point out a possible pathway in the fate and transport of pharmaceuticals in aquatic ecosystems .
研究领域:
环境科学
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药理学
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PubMed
高影响因子
CHEMOSPHERE
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2018
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IF 4.427
Jing Xu,Heng Zhang,Tao Luo,Zizheng Liu,Jun Xia,Xiang Zhang
The effects of co-existing nitrogen species in surface water on the phototransformation of organoarsenical p -arsanilic acid ( p -ASA) have been investigated using a xenon lamp as a simulated solar light source. Significant enhancements of p -ASA phototransformation efficiency were observed in the presence of nitrate and nitrite, increasing with the concentration of these species and pH, whereas ammonia showed no obvious effect. The products, including inorganic arsenic species and organic derivatives, have been analyzed in order to reveal the phototransformation pathways. In the nitrate and nitrite systems, only small proportions of inorganic arsenic species were generated, with the majority of p -ASA being converted into other organoarsenical derivatives through hydroxylation, nitration, and nitrosation. Phototransformation of p -ASA in collected natural surface water was also observed. This work has implications for the phototransformation of p -ASA in nitrogen-contaminated surface water.
研究领域:
环境科学
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水污染控制
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光化学反应
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PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Zhijie Zhang,Xuesheng Wang,Huiling Tang,Deben Li,Jiayue Xu
Modulating the internal electric field (IEF) represents a potential strategy to stimulate the photocatalytic activity of heterojunctions, especially S-scheme photocatalysts. Herein, a Cs 3 Bi 2 Br 9 @V O -In 2 O 3 (CBB@V O -In 2 O 3 ) S-scheme heterojunction, of which Cs 3 Bi 2 Br 9 perovskite quantum dots (PQDs) are embedded into mesoporous V O -In 2 O 3 hosts, is rationally designed as a cornerstone for further IEF manipulation. Briefly, by introducing oxygen vacancies (V O ) into the composed reduction semiconductor (mesoporous In 2 O 3 ), an enlarged Fermi level ( E F ) gap between CBB and V O -In 2 O 3 is achieved, yielding an intensified IEF over the CBB@V O -In 2 O 3 heterojunction. Such an enhanced IEF affords a much more robust driving force for directional carrier delivery, leading to accelerated carrier transfer of CBB@V O -In 2 O 3 heterojunction. Consequently, the optimized CBB@V O -In 2 O 3 heterojunction features desirable CO 2 -to-CO conversion efficiency, and its CO production rate reaches 130.96 μmol g −1 h −1 . The reaction intermediates and CO 2 photoconversion pathway were unraveled by in-situ diffuse reflectance infrared Fourier transform spectroscopy. Combining with the DFT calculation, it was revealed that oxygen vacancies in V O -In 2 O 3 act as reactive centers, which optimize the coordination modes of the intermediates, thus reducing the activation energy for photocatalytic CO 2 reduction. Our work demonstrates that the IEF modulation of S-scheme-based heterojunction could significantly boost the charge separation and then to drive efficient catalytic reaction , achieving high-efficiency solar fuel production.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2024
·
IF 5.7
Fang Xu,Yukuai Zhang,Longfei Su,Zhenxing Guo,Qiang Cheng,Liqiang Xu,Feng Wang,Guoping Sheng
Understanding the environmental fate of chemical herbicides is crucial to sustainable agriculture. Due to their joint-use with nitrogen fertilizers, their residues often coexist with NO3– in agricultural drainages. In this study, tribenuron-methyl was used as a model to evaluate the role of NO3– in the phototransformation of chemical herbicides, which was characterized by a two-stage process. Initially, a slow hydrolysis occurs (kobs = 2.573 × 10–4 min–1), producing two hydrolysis products: methyl-2-(aminosulfonyl)-benzoate (MSB) and 2-methyl-4-methylamino-6-methoxy-1, 3, 5-triazine (MMT), which can be significantly accelerated by solar irradiation (kobs = 2.152 × 10–2 min–1). Subsequently, MSB undergoes a rapid NO3–-initiated photodegradation process (kobs = 2.251 × 10–2 min–1). MMT was identified as the refractory unit and undergoes a slow NO3–-initiated photodegradation process (kobs = 4.494 × 10–4 min–1). The underlying mechanisms were elucidated through electron paramagnetic resonance spectroscopy and reactive species quenching experiments. This study fills a knowledge gap on the interaction between NO3– and chemical herbicides, highlighting the pivotal role of NO3– in the phototransformation of chemical herbicides.
研究领域:
环境科学
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农业科学
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PubMed
高影响因子
Journal of Environmental Sciences
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2016
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IF 2.208
Suqi Li,Jing Xu,Wei Chen,Yingtan Yu,Zizheng Liu,Jinjun Li,Feng Wu
p -Arsanilic acid ( p -ASA) is widely used in China as livestock and poultry feed additive for promoting animal growth. The use of organoarsenics poses a potential threat to the environment because it is mostly excreted by animals in its original form and can be transformed by UV–Vis light excitation. This work examined the initial rate and efficiency of p -ASA phototransformation under UV-C disinfection lamp. Several factors influencing p -ASA phototransformation, namely, pH, initial concentration, temperature, as well as the presence of NaCl, NH 4 + , and humic acid , were investigated. Quenching experiments and LC–MS were performed to investigate the mechanism of p -ASA phototransformation. Results show that p -ASA was decomposed to inorganic arsenic (including As(III) and As(V)) and aromatic products by UV-C light through direct photolysis and indirect oxidation. The oxidation efficency of p -ASA by direct photosis was about 32%, and those by HO and 1 O 2 were 19% and 49%, respectively. Cleavage of the arsenic–benzene bond through direct photolysis, HO oxidation or 1 O 2 oxidation results in simultaneous formation of inorganic As(III), As(IV), and As(V). Inorganic As(III) is oxidized to As(IV) and then to As(V) by 1 O 2 or HO . As(IV) can undergo dismutation or simply react with oxygen to produce As(V) as well. Reactions of the organic moieties of p -ASA produce aniline, aminophenol and azobenzene derivatives as main products. The photoconvertible property of p -ASA implies that UV disinfection of wastewaters from poultry and swine farms containing p -ASA poses a potential threat to the ecosystem, especially agricultural environments.
研究领域:
环境科学
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毒理学
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PubMed
高影响因子
Advanced Composites and Hybrid Materials
·
2024
·Vol. 7
·期 6
·1-9
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IF 23.2
Dai Xiaokang,Wang Longxiang,Fallatah Ahmed M.,Wang Xing,Almalki Abdulraheem S. A.,Qi Yiyu,Jin Xiaoyu,Yang Shengxiang,Yuan Bingnan
Translucent materials are widely used in indoor lighting, electronic display devices, photovoltaic devices, and other aspects of daily life. Developing materials with high transparency that can effectively manage the transmitted light spectrum is of significant practical importance. This study focuses on constructing a flexible composite film matrix using biomass nanocellulose fibrils (CNF) and polyvinyl alcohol (PVA) as raw materials. Based on the down-conversion luminescence principle, we use carbon nitride nanosheets (CNNs) as the core for light management, filtering UV rays from sunlight while converting them into visible light for light compensation. The transparency test results show that the prepared CNNs@CNF/PVA flexible composite film has a total transmittance of about 90% in the visible light range, with a haze greater than 60%. Three-dimensional fluorescence test results indicate that CNNs@CNF/PVA can convert UV light in the range of 250–375 nm into visible light in the range of 420–550 nm. Simulated outdoor lighting results show that the composite film material performs better than ordinary glass and PMMA in light transmission. This biomass-based flexible film material is expected to have broad applications in indoor lighting, flexible photovoltaic devices, and high-quality fruit and vegetable cultivation.
研究领域:
材料科学
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光管理技术
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生物质材料
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DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Yifan Ke,Jingqiu Jiang,Xiqin Mao,Baocheng Qu,Xintong Li,Hongxia Zhao,Jingyao Wang,Zhansheng Li
Glucocorticoids (GCs), as endocrine disruptors , have attracted widespread attention due to their impacts on organisms' growth, development, and reproduction. In the current study, the photodegradation of budesonide (BD) and clobetasol propionate (CP), as targeted GCs, was investigated including the effects of initial concentrations and typical environmental factors (Cl − , NO 2 − , Fe 3+ , and fulvic acid (FA)). The results showed that the degradation rate constants (k) were 0.0060 and 0.0039 min −1 for BD and CP at concentration of 50 μg·L −1 , and increased with the initial concentrations. Under the addition of Cl − , NO 2 − , and Fe 3+ to the GCs/water system, the photodegradation rate was decreased with increasing Cl − , NO 2 − , and Fe 3+ concentrations, which were in contrast to the addition of FA. Electron resonance spectroscopy (EPR) analysis and the radical quenching experiments verified that GCs could transition to the triplet excited states of GCs ( 3 GCs*) for direct photolysis under irradiation to undergo, while NO 2 − , Fe 3+ , and FA could generate ·OH to induce indirect photolysis. According to HPLC-Q-TOF MS analysis, the structures of the three photodegradation products of BD and CP were elucidated, respectively, and the phototransformation pathways were inferred based on the product structures. These findings help to grasp the fate of synthetic GCs in the environment and contribute to the understanding of their ecological risks.
研究领域:
环境科学
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毒理学
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PubMed
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Ruiya Zhou,Juan Liu,Chi Zhou,Xu Zhang
Lignin is a major terrestrial source of chromophoric dissolved organic matter (CDOM), and studying the phototransformation of lignin monomers and their related compounds can enhance our understanding of CDOM intramolecular interactions. Coniferyl aldehyde (Coni) and sinapaldehyde (Sina) form ground-state complexes with CDOM, with equilibrium constants of 7,800 (± 1,800) and 20,000 (± 2,000) M −1 , respectively. In comparison, vanillin (Van) exhibits minimal affinity for CDOM complexation. The bimolecular reaction rate constants between singlet oxygen ( 1 O 2 ) and these phenolic carbonyl compounds ranged from 0.46 (± 0.02) to 1.8 (± 0.1) × 10 7 M −1 s −1 , which is approximately one order of magnitude lower than their reaction rate constants (0.51 (± 0.02)–1.25 (± 0.02) × 10 8 M −1 s −1 ) with the triplet excited state of CDOM ( 3 CDOM*). In acidic CDOM solutions (pH 5.0), 1 O 2 , H 2 O 2 , and organic peroxyl radicals had negligible impact on the transformation. Comparing the initial transformation rate in the presence and in the absence of NaN 3 or furfuryl alcohol led to an overestimation of the contribution of 1 O 2 to the transformation of Van, Coni, or Sina. 3 CDOM* scavengers could not fully inhibit the transformation of Coni or Sina. The remaining transformation is considered to arise from either the unquenched intra-CDOM phase 3 CDOM* or a fraction of Coni⊂CDOM or Sina⊂CDOM complex, which underwent intramolecular photoinduced chemical reactions.
研究领域:
环境科学
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生物化学
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PubMed
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Qiang Liu,Xiaojun Niu,Dongqing Zhang,Xingyao Ye,Peibing Tan,Ting Shu,Zhang Lin
Phosphite, an essential component in the biogeochemical phosphorus cycle, may make significant contributions to the bioavailable phosphorus pool as well as water eutrophication. However, to date, the potential impacts of coexisting photochemically active substances on the environmental fate and transformation of phosphite in aquatic environments have been sparsely elucidated. In the present study, the effect of zinc oxide nanoparticles (ZnO NPs), a widely distributed photocatalyst in aquatic environments, on phosphite phototransformation under simulated solar irradiation was systematically investigated. The physicochemical characteristics of the pristine and reacted ZnO NPs were thoroughly characterized. The results showed that the presence of ZnO NPs induced the indirect phototransformation of phosphite to phosphate, and the reaction rate increased with increasing ZnO NPs concentration. Through experiments with quenching and trapping free radicals, it was proved that photogenerated reactive oxygen species (ROS), such as hydroxyl radical (•OH), superoxide anion (O 2 •− ), and singlet oxygen ( 1 O 2 ), made substantial contributions to phosphite phototransformation. In addition, the influencing factors such as initial phosphite concentration, pH, water matrixes (Cl − , F − , Br − , SO 4 2− , NO 3 − , NO 2 − , HCO 3 − , humic acid (HA) and citric acid (CA)) were investigated. The component of generated precipitates after the phosphite phototransformation induced by ZnO NPs was still dominated by ZnO NPs, while the presence of amorphous Zn 3 (PO 4 ) 2 was identified. This work explored ZnO NPs-mediated phosphite phototransformation processes, indicating that nanophotocatalysts released into aquatic environments such as ZnO NPs may function as photosensitizers to play a beneficial role in the transformation of phosphite to phosphate, thereby potentially mitigating the toxicity of phosphite to aquatic organisms while exacerbating eutrophication. The findings of this study provide a novel insight into the comprehensive assessment of the environmental fate, potential ecological risk, and biogeochemical behaviors of phosphite in natural aquatic environments under the condition of combined pollution.
研究领域:
环境科学
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生态学
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水生生物学
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PubMed
高影响因子
JOURNAL OF PHYSICAL ORGANIC CHEMISTRY
·
2015
·Vol. 28
·期 6
·428-430
·
IF 1.38
Qiuxia Wu,Xuming Zheng,Kemei Pei
Phototransformation mechanism of monuron induced by the triplet benzophenone in aqueous solution was investigated by laser flash photolysis technique, while quenching of the triplet benzophenone by monuron was studied by nanosecond transient absorption spectroscopy. The transient species in the transient absorption spectra have been identified by quantum chemistry calculations. The results show that under 355-nm irradiation proton transfer between the triplet benzophenone and monuron happens, and monuron radical is formed and followed by dechlorination degradation reactions. This work indicated that in aqueous solution some dissolved natural organic matters are helpful to degradation of the organic pollutants under the sunlight. Copyright © 2015 John Wiley & Sons, Ltd.
研究领域:
环境科学
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光化学
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DOI
高影响因子
CRYSTAL GROWTH & DESIGN
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2022
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IF 4.01
Jiemin Qiu,Weihao Ye,Xiaokai Xu,Baoyan Guo,Ruizhe Wang,Chaofan Hu,Jianle Zhuang,Hanwu Dong,Guangqi Hu,Yingliang Liu
Ultraviolet (UV) absorbers are of vital importance in reducing the damage of UV irradiation to materials, incredibly effective in delaying the life of polymers. However, commercial inorganic UV absorbers tend to generate free radicals that accelerate the decomposition of materials. The carbon dots (CDs) that mineralize CaCO3 to different degrees to prepare excellent UV absorbers with UV absorption properties were proposed in this work. CDs with a negative charge of −3.77 mV and a surface rich in functional groups such as −COOH, −OH, −NH2, and −C═O were synthesized by a one-step method to induce the typical rhombic CaCO3 to form other irregular morphologies, including polycrystalline rhombic, flower-like, flower-like with more petals, and smooth spherical shapes. The UV absorption properties of CDs endow CaCO3 with a strong UV absorption capacity at 200–400 nm and the stability of spherical CDs@CaCO3 is higher than that of pure CDs. It shows that spherical CDs@CaCO3 have superior dispersibility, optical stability, high-temperature resistance, and anti-photoaging performance. Finally, to reflect the practical application of CDs@CaCO3, it was compounded with polyurethane (PU). It increases the UV resistance and mechanical properties of PU film, and the application of light conversion film has great potential in agriculture. The development of a new inorganic UV absorber has excellent prospects for application in the field of UV resistance.
研究领域:
材料科学
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化学工程
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高影响因子
危险品化学品经营许可证（带存储）