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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2012 ·Vol. 20 ·期 1 ·31-38 · IF 2.651

Photooxidation of arsenite by natural goethite in suspended solution

Wang Yajie,Xu Jing,Zhao Yan,Zhang Lin,Xiao Mei,Wu Feng

Iron and arsenic have been found to coexist in a water environment and the fate of arsenite in the aquatic system is influenced by iron. Goethite is a form of iron hydroxide, which is commonly found in sediments. In previous studies, we have used iron complexes to degrade organic pollutants. Results have shown that some organic pollutants could be totally degraded by iron complexes and our work indicated that iron might cause conversion of arsenic when irradiated. This work attempts to investigate the conversion of arsenite [As(III)] using natural goethite, as the iron source, to quantify the effect of various factors on photooxidation. We also consider the possible mechanism for photooxidation of As(III) using a suspension of natural goethite. The As(III) concentration variation under illumination was compared with the one in the dark to quantify the contribution of light to As(III) oxidation to As(V) in goethite suspended solution. The experiments under N 2 and air atmosphere confirmed the participation of dissolved oxygen. The photooxidation efficiency of As(III) under different conditions was compared to determine the effect of different environmental factors such as pH value, goethite concentration, and humic acid concentration on the photooxidation reaction. In the solution containing 100 μg L −1 arsenite and 0.1 g L −1 suspended goethite at pH 3.0, nearly 80 % of As(III) was photooxidized after irradiation by a 250-W metal halogen lamp ( λ  ≥ 313 nm) after 6 h. The effects of initial pH and goethite concentration and humic acid concentration were all examined. The results show that the greatest efficiency of photooxidation of As(III) was at pH 3.0. The extent of photooxidation decreased with increasing goethite concentration and fell sharply in the presence of humic acid under the conditions in this work. Although about 80 % of As(III) was photooxidized after irradiation by a 250-W halogen lamp at pH 3.0 in the presence of goethite suspension, photooxidation was also affected by factors such as pH, concentration of goethite, and presence of humic acid. The scavenger experiments showed that the HO• radical and photogenerated hole are the predominant oxidants in this system responsible for 87.1 % oxidation of As(III), while HO • 2 /O •− 2 is responsible for 12.9 % oxidation of As(III).

CAS / MDL: 149-45-1
研究领域: 环境科学 · 化学
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CHEMOSPHERE · 2019 · IF 5.108

Effects of acetylacetone on the thermal and photochemical conversion of benzoquinone in aqueous solution

Jiyuan Jin,Zhihao Chen,Xiaojie Song,Bingdang Wu,Guoyang Zhang,Shujuan Zhang

Quinones are components of electron transport chains in photosynthesis and respiration. Acetylacetone (AA), structurally similar to benzoquinone (BQ) for the presence of two identical carbonyl groups, has been reported as a quinone-like electron shuttle. Both BQ and AA are important chemicals in the aquatic environment. However, little information is known about their interactions if co-existed. We found here that AA significantly enhanced the conversion of BQ. By analyzing the evolution of chemical concentration, solution pH, dissolved oxygen, and the final products, the interactions between AA and BQ were elucidated. The reactions between BQ and AA generated oxygen but ultimately led to the reduction of solution pH and dissolved oxygen. The reactions proceeded faster under indoor lighting condition than in the dark. The formation of semiquinone radicals is believed as the primary step. The secondary AA-derived radicals might be strongly oxidative or reductive, depending on the concentration of dissolved oxygen. Insoluble humus was generated in the mixture of BQ and AA. These results suggest that the presence of AA might interfere with photosynthesis and respiration through the interactions with quinones.

CAS / MDL: 7778-77-0
研究领域: 环境科学 · 生物化学
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY · 2018 · IF 2.891

Dissolved oxygen inhibits the promotion of chlorothalonil photodegradation mediated by humic acid

Huan He,Dan Xiong,Fengxia Han,Zhiang Xu,Bin Huang,Xuejun Pan

Chlorothalonil (CT) is widely used to control fungal diseases, and it is commonly detected in the environment. Phototransformation is an important process which removes CT from aquatic environments. The kinetics and mechanisms of CT photodegradation in solutions with and without humic acid (HA) were investigated, and the influence of dissolved oxygen (DO) on the photodegradation process was also considered. The rate constant observed in pure water was only 0.017 h −1 , but it increased to 0.083 h −1 with 5.0 mgC L −1 of HA present. Reactive species generated by HA were shown to play an important role. Moreover, the degradation of CT was promoted at higher HA concentrations. But higher DO concentrations inhibits CT degradation because of the reaction between DO and excited triplet state CT ( 3 CT*) or HA ( 3 HA*). The contributions of the reactive species tested were in the sequence 3 HA* >  1 O 2  > H 2 O 2 /O 2 −  ≈  OH in a nitrogen-saturated system, but in an oxygen-saturated system the order was OH ≈ 1  O 2  > H 2 O 2 /O 2 −  >  3 HA*. 3 CT* was confirmed as the active form of CT during degradation, with 4-hydroxy-chlorothalonil and 2,4,5-trichloroisophthalonitrile as the main products. Compared to direct photodegradation, CT photodegradation mediated by HA can decrease the toxicity of an aquatic environment as demonstrated through tests with Scenedesmus obliquus.

研究领域: 环境科学 · 水污染控制
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2019 · IF 7.149

Enhanced Photooxidation of Hydroquinone by Acetylacetone, a Novel Photosensitizer and Electron Shuttle

Jiyuan Jin,Shujuan Zhang,Bingdang Wu,Zhihao Chen,Guoyang Zhang,Paul G. Tratnyek

Quinones are important electron shuttles as well as micropollutants in the nature. Acetylacetone (AA) is a newly recognized electron shuttle in aqueous media exposed to UV irradiation. Herein, we studied the interactions between AA and hydroquinone (QH2) under steady-state and transient photochemical conditions to clarify the possible reactions and consequences if QH2 and AA coexist in a solution. Steady-state experimental results demonstrate that the interactions between AA and QH2 were strongly affected by dissolved oxygen. In O2-rich solutions, the phototransformation of QH2 was AA-independent. Both QH2 and AA utilize O2 as the electron acceptor, but in O2-insufficient solutions, AA became an important electron acceptor for the oxidation of QH2. In all cases, the coexistence of AA increased the phototransformation of QH2, whereas the decomposition of AA in O2-saturated and oversaturated solutions was inhibited by the presence of QH2. The underlying mechanisms were investigated by a combination of laser flash photolysis (LFP) and reduction potential analysis. The LFP results show that the excited AA serves as a better electron shuttle than QH2. As a consequence, AA might regulate the redox cycling of quinones, leading to significant effects on many processes, ranging from photosynthesis and respiration to photodegradation.

CAS / MDL: 7778-77-0
研究领域: 环境科学 · 光化学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Oxygen-containing functional groups of biochars enhancing the oxygen release of CaO2 and the generation of free radicals

Qiang Hu,Junheng Zhang,Yadi Pan,Kuan Ding,Chaoyang Xu,Jinyu Hou,Wuxing Liu,Chanchana Thanachayanont,Thipjak Na Lampang,Meiling Chen,Shu Zhang

The low dissolved oxygen (DO) concentration in groundwater is one of the key challenges limiting the efficiency of aerobic microbial remediation, leading to the development of slow-release oxygen agents such as CaO 2 . Our previous studies have demonstrated that the oxygen content in biochars plays a role in the oxygen release reaction of CaO 2 . This study aims to further investigate the relationship between the oxygen-containing functional groups on biochar surface and oxygen release performance of CaO 2 . Surface oxidation and reduction modifications were employed to regulate the oxygen-containing functional groups on bamboo biochars while minimizing alterations to its physical structure. Results showed that the oxidized and reduced biochars were similar in oxygen content (∼20–22 %) and pore structure (with specific surface area of 8–16 m 2 ·g −1 and average pore size of 10–13 nm). On the contrary, the difference in contents between C-O and O C-O functional groups reached ∼10 %, indicating the successful regulation of the oxygen-containing functional groups. The loading capacity of CaO 2 increases with the increase in C-OH groups in biochars, while the O C-O group is identified as the oxygen-containing functional group that contributes most significantly to accelerating the oxygen release of CaO 2 . The dissolution product hydrogen peroxide (H 2 O 2 ) potentially interacted with biochars to activate free radical synthesis. The yield of hydroxyl radicals (•OH) shows a positive correlation with the oxygen content in biochars, while the production of superoxide radicals (•O - 2 ) is most significantly influenced by the presence of O C-O groups. As a result, the yield of •O - 2 was 216–317 times higher than that of •OH.

CAS / MDL: 25322-68-3 2564-83-2
研究领域: 环境科学 · 微生物学
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

VS4 Nanodendrites with Narrow Bandgaps in Activating Dissolved Oxygen for Boosted Chemiluminescence and Hemin Detection by Unexpected Quenching

Abubakar Abdussalam,Hongzhan Liu,Islam Mohamed Mostafa,Baohua Lou,Dmytro Viktorovych Snizhko,Yuriy Tymofiiovych Zholudov,Wei Zhang,Guobao Xu

Chemiluminescence (CL)-based analytical methods utilize luminophores that need to be activated with an oxidizing agent to trigger CL emission. Despite its susceptibility to decomposition when exposed to external light or trace metals, hydrogen peroxide (H2O2) has been widely used to develop chemiluminescent methods due to the limited number of suitable alternatives for activating chemiluminescent luminophores. Also, analytical methods based on the well-known luminol/H2O2 CL system have low sensitivity. Dissolved oxygen (DO) is a naturally abundant and environmentally benign alternative oxidant for luminol and other CL luminophores. However, DO alone is inactive and needs an efficient catalyst or a coreaction accelerator for its activation. Because of the narrow bandgap of VS4 (ca. 1.12 eV), it can facilitate fast electron-transfer kinetics with an acceptor molecule such as DO. Here, we introduce vanadium tetrasulfide (VS4) to boost CL for the first time. Under the optimized conditions, VS4 nanodendrite catalyzes the generation of reactive oxygen species by activating DO which subsequently reacts with luminol to generate intense CL. It enhances the CL intensity of luminol/DO by about 10,000 times. Surprisingly, hemin remarkably quenches the generated CL of luminol/DO/VS4 nanodendrites, which is completely opposite to its typical enhancement of luminol CL. Based on the remarkable concentration-dependent quenching of the luminol/DO/VS4 nanodendrite CL by hemin, we have developed a sensitive CL method that can selectively detect hemin in the linear concentration range of 1–250 nM and achieved a limit of detection of 0.11 nM. The practical utility of the developed method was demonstrated by the determination of hemin in a pharmaceutical drug for the treatment of acute intermittent porphyria and in human serum. This study demonstrates that VS4 holds great promise in analytical method development.

CAS / MDL: 70-18-8 62-55-5
研究领域: 分析化学 · 环境科学
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BIOSENSORS & BIOELECTRONICS · 2018 · IF 8.173

A ratiometric electrochemiluminescent biosensor for Con A detecting based on competition of dissolved oxygen

Han Zhang,Cong Zhang,Di Liu,Fumei Zuo,Shihong Chen,Ruo Yuan,Wenju Xu

A novel ratiometric electrochemiluminescent (ECL) biosensor was designed for the detection of concanavalin A (Con A) based on two ECL emitters competing for the dissolved oxygen (O 2 ). In this strategy, CdTe quantum dots (QDs) were used as the cathodic emitter and N-(aminobutyl)-N-(ethylisoluminol) (ABEI) was used as the anodic emitter. With the presence of dissolved O 2 utilized as co-reactant, CdTe QDs showed an ECL emission at − 1.7 V, and ABEI showed an emission at + 0.6 V. Phenoxy-derivatized dextran (Dexp), as a recognition element, was immobilized by graphene oxide functionalized CdTe QDs (G-CdTe QDs) to recognize Con A, and further combine with Dexp, gold and platinum nanoparticles decorated ABEI (Dexp-Au-Pt-ABEI) to form a sandwich structure. With the increasing concentration of analyte Con A, the ECL signal of cathodic CdTe QDs decreased and the anodic response of ABEI increased, thus achieving a ratiometry detection of Con A with a wide linear range from 1.0 × 10 −4 ng/mL to 10 ng/mL. The detection limit was low to 3.0 × 10 −5 ng/mL. This proposed ratiometric ECL biosensor not only conquered the false errors caused by external interferences, but excluded the disability caused by exogenous co-reactant via the application of common dissolved O 2 . It also exhibited an excellent stability, selectivity and reproducibility.

研究领域: 生物传感器技术 · 分析化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2017 · IF 5.401

Highly enhanced sensitivity of optical oxygen sensors using microstructured PtTFPP/PDMS-pillar arrays sensing layer

Yongyun Mao,Yibo Gao,Shanshan Wu,Siying Wu,Jiayan Shi,Bingpu Zhou,Yanqing Tian

In this work, we presented a facile and cost-effective approach to fabricate novel PtTFPP/PDMS micro-pillar array (MPA) sensor film with I 0 /I 100 for gaseous oxygen and dissolved oxygen are 288 and 84, respectively. The sensitivity of the sensor film exhibited over ∼30-fold increment when compared with contemporary PtTFPP/PDMS-based oxygen sensors. The detection limit was as low as 0.10   μmol/L, which means that the ultrasensitive sensor films enable reliable monitoring of dissolved oxygen (DO) within nanomolar concentration ranges that are particularly difficult to achieve in previous works. Furthermore, the remarkably light intensity-changing characteristic of the sensing film under lower O 2 partial pressures facilitates convenient identification of O 2 concentrations even with the naked eye. We believe that the proposed device could be a promising candidate in various oxygen sensing fields such as nearly anoxic systems, unsteady pressure measurement and unsteady flow visualization, etc.

CAS / MDL: 9001-37-0
研究领域: 材料科学 · 传感技术 · 生物医学工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Faceted TiO2 photocatalytic degradation of anthraquinone in aquatic solution under solar irradiation

Tingming Ye,Weixiao Qi,Xiaoqiang An,Huijuan Liu,Jiuhui Qu

Anthraquinone (AQ), a common oxygenated polycyclic aromatic hydrocarbon (PAH) in the water environment, often occurs with higher concentrations than its parent anthracene as it is the dominant intermediate from anthracene during both wastewater treatment and transformation in natural waters. During the elimination of PAHs and their intermediates, the water matrix often induces positive or negative effects. In this paper, photocatalytic degradation of AQ in the presence of inorganic ions (NO 3 − , HCO 3 − , Fe 3+ ) and organic matter (humic acid) was studied with {101} and {010}-TiO 2 as sunlight-driven photocatalysts. Meanwhile, the effect of dissolved oxygen (DO) on photocatalytic degradation of AQ was evaluated. The results showed that NO 3 − had a slight suppressing effect, while HCO 3 – and Fe 3+ promoted the photocatalytic activity due to formation of new oxidizers (CO 3 − and H 2 O 2 ). Interestingly, HA could envelope {101}-TiO 2 to inhibit photodegradation ; however, it had almost no effect on {010}-TiO 2 due to the different surface structures and properties. High dissolved oxygen content in water could markedly promote the photodegradation of AQ. This was consistent with the results of scavenging experiments, which demonstrated that O 2 – and h + played more important roles than OH did. A small amount of benzene was detected as an intermediate product of AQ by LC-QTOF-MS analysis. Hopefully, this work can contribute to the understanding of the potential of water remediation by faceted photocatalysts.

CAS / MDL: 75-65-0
研究领域: 环境科学 · 化学
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Water Science and Engineering · 2024 · IF 3.7

Enhanced total nitrogen removal and membrane fouling control by increasing biomass in MBR equipped with ceramic membrane

Shan-Shan Gao,Xing Yin,Rui Huang,Jia-Yu Tian

Simultaneous nitrification and denitrification (SND) is an efficient method to remove nitrogen in municipal wastewater treatment. However, low dissolved oxygen (DO) concentrations are generally required, leading to serious membrane fouling in membrane bioreactors (MBRs). This study aimed to clarify the synergistic effect of biomass and DO on nitrogen removal and membrane fouling. To achieve this goal, four submerged MBRs equipped with ceramic membranes were operated with different biomass (mixed liquor suspended solids (MLSS)) concentrations (3 000 mg/L, 5 000 mg/L, 7 500 mg/L, and 12 000 mg/L) under various DO concentrations (2.0 mg/L, 1.0 mg/L, and 0.5 mg/L). As a result, increasing biomass in the MBRs enhanced total nitrogen (TN) removal via SND, and excellent TN removal efficiencies of 60.7% and 75.8% were obtained using the MBR with an MLSS concentration of 12 000 mg/L and DO concentrations of 2.0 mg/L and 1.0 mg/L. However, a further decrease in DO deteriorated TN removal due to the inhibition of nitrification. Moreover, high MLSS concentrations were beneficial to membrane fouling control for ceramic membranes in MBRs. The lowest transmembrane pressure development rate was observed for the MBR with an MLSS concentration of 12 000 mg/L. High biomass offset the adverse effect of DO decrease on membrane fouling to some extent, and improved the stability of the reactor. Therefore, biomass might be an important parameter for membrane fouling reduction in ceramic MBRs. Overall, optimal biomass and DO concentrations for TN removal were identified, providing useful information for the successful operation of MBRs with efficient TN removal and membrane fouling control.

研究领域: 环境工程 · 污水处理 · 微生物学
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ACS Applied Energy Materials · 2024 · IF 5.4

Fish-Gill-Inspired Underwater Self-Breathing Zinc–Air Batteries

Fancheng Meng,Peng Chen,Shulin Li,Na Cao,Sheng Cheng,Xiangfeng Wei,Jiangtao Di,Jiehua Liu

Compared with the rapidly developing lithium- and sodium-ion batteries, zinc-air batteries (ZABs) offer the advantages of safety and high energy density. Nevertheless, their applications in underwater conditions are currently limited due to the low oxygen levels in such environments. Drawing inspiration from fish gills, we have successfully constructed a self-breathing zinc-air battery (ZAB) that can extract dissolved oxygen from water and convert it to electrical energy. By utilizing a Co2Fe-NC catalyst and a large-window cathode, the ZAB demonstrates a continuous discharge duration of 68.6 h in the underwater condition, thanks to its well-engineered architecture, optimized catalyst, and gas diffusion layer. Meanwhile, the underwater ZAB outperforms fish gills as it also operates efficiently in air, exhibiting a high capacity of 740 mA h g–1 and a high power density of 320 mW cm–2. Additionally, prolonged cycling tests indicate the ZAB’s capability for stable charging and discharging with minimal potential variation. This study introduces an innovative approach to the development of breathable underwater metal–air batteries.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 能源技术 · 仿生学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Hexavalent chromium removal by green synthesized nano-size iron particles combined with iron sulfides: Effects of dissolved oxygen and phosphate

Weidong Gao,Haijun Chen,Xinyue Ma,Nan Xu,Fang Feng,Shan Zhang

The removal of hexavalent chromium (Cr(VI)) from wastewater using the green synthesized nano-zero-valent-iron (GnZVI) has attracted great attention. However, the Cr(VI) removal capacity of GnZVI remains limited by dissolved oxygen (DO) or phosphate in wastewater. Therefore, Cr(VI) removal by GnZVI combined with iron sulfides (i.e., FeS or FeS 2 ) impacting by DO and phosphate was investigated at pH 2.0 and 6.0. Experimental results showed that DO inhibited the Cr(VI) removal by GnZVI with FeS at pH 2.0, because high DO saturation was beneficial to Fe(II) oxidization into Fe(III). Nevertheless, DO promoted the corrosion and dissolution of FeS 2 but GnZVI for Cr(VI) reduction at pH 2.0. Especially, phosphate inhibited the Cr(VI) reduction by the combination of GnZVI and iron sulfides at pH 2.0, likely because phosphate inhibited Fe(II) release from GnZVI hybrid materials during the reduction process from Cr(VI) to Cr (III). Differently, at pH 6.0, phosphate mainly promoted Cr(VI) removal by FeS compared with GnZVI via the formation of phosphate complexation, while it inhibited Cr(VI) removal using GnZVI combined with FeS 2 through the competitive adsorption. This study reveals the potential inherent mechanisms and emphasizes a sustainable strategy for the effective removal of Cr(VI) using a hybrid technique that combines GnZVI and iron sulfides under complex wastewater conditions.

研究领域: 环境科学 · 材料科学
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