International Journal of Electrochemical Science
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2023
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IF 1.5
Yucen Yao,Chunxiao Yin,Shiguan Xu,Meng Jiang,Lin Zhu,Ruyi Zou,Wei Sun
In this paper gold nanoparticles (AuNPs) were electrodeposited on the coiled carbon nanotubes (CCNTs) modified carbon ionic liquid electrode (CILE), and horseradish peroxidase (HRP) was fixed on the modified electrode by using Nafion film to get the modified electrode. HRP immobilized with AuNPs-CCNTs composite still retained the biostructure and direct electrochemistry of Nafion/HRP/AuNPs-CCNTs/CILE showed a quasi-reversible electrochemical behavior. Electrocatalysis to KBrO 3 and NaNO 2 were further checked with the apparent heterogeneous electron transfer rate constant ( ks ), the charge transfer coefficient (α) and the Michaelis-Menten constants ( K M a p p ) calculated. The linear detection range for KBrO 3 concentration was from 0.5 to 10.0 mmol·L -1 with a detection limit of 0.16 mmol·L -1 . And for NaNO 2 , the current response showed two linear sections in the concentration range from 0.1 to 0.7 mmol·L -1 and 0.9 to 3.0 mmol·L -1 with low detection limit of 0.03 mmol·L -1 . The sensor was used for the real water samples analysis with high recovery, demonstrating the practical applications.
研究领域:
分析化学
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环境科学
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DOI
高影响因子
Journal of Nanomaterials
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2020
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IF 1.98
Yan Zhang,Jiarong Li,Hongyuan Liu
The batch experiments of photocatalytic oxidation-reduction of bromate and ibuprofen (IBP) by graphene oxide (GO) and TiO2 heterostructure doped with F (FGT) particles were conducted. The performance and mechanism of synergistic removal of bromate and IBP by FGT were discussed. The results show that a demonstrable synergistic effect and excellent removal rate of bromate and IBP by FGT were exhibited. When pH is 5.2 and the dosage of FGT is 0.1 g/L, the reaction rate constants of bromate and IBP increased from 0.0584 min-1 and 0.4188 min-1 to 0.1353 min-1 and 0.4504 min-1, respectively, compared with the degradation of bromate or IBP alone. The reaction of photocatalytic synergistic degradation is appropriately fitted through Langmuir-Hinshelwood first-order kinetics. The mechanism of synergistic removal of bromate and IBP by FGT was discussed. And electrons (e-), hydroxyl radical (⋅OH), and superoxide radical (⋅O2-) are the main active species. The electrons play a main role in the bromate reduction, and bromine is the only reduction product, while the oxidation of IBP is the result of ⋅OH and ⋅O2-, and ⋅OH plays a key role. The recombination of electrons and holes is inhibited by simultaneous consumption of bromate and IBP, which makes full use of the redox properties of FGT and plays a synergistic role in the removal of pollutants. The results indicate that photocatalytic oxidation-reduction by FGT is a promising, efficient, and environmental-friendly method for synchronous removal of combined pollution in water.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Zhihui Hu,Shasha Tang,Yan Jia,Zekun Dong,Yu Tang,Yuan Wu,Yan Zhang
The photocatalytic reduction of bromate (BrO 3 - ) in drinking water shows great promise. However, current photocatalysts mainly depend on UV light for effective bromate transformation. In this study, we introduced a novel visible-light-active catalyst, TBR (a combination of Ti 3 C 2 MXene, Bi, and TiO 2 ), synthesized through a straightforward hydrothermal method. Batch experiments were carried out in the laboratory to evaluate the photocatalytic removal effect of bromate by TBR under visible light. TBR completely eliminated 200 µg/L of bromate within 60 minutes (first-order kinetic constant: 0.0509 min -1 ). By employing photoelectric properties, density functional theory (DFT) and scavenger experiments, an intrinsic mechanism of the photocatalytic breakdown of bromate over the TBR/visible-light system was elucidated. The introduction of Bi induces the surface plasmon resonance (SPR) effect, and reduced the effective mass of electrons, resulting in a narrower band gap (from 2.88 eV to 2.50 eV) of the photocatalyst, and enables it to respond to visible light. Additionally, Ti 3 C 2 acted as an "electron sink," facilitating carrier migration and accumulation on its surface, creating a Schottky barrier that promoted efficient electron transfer and the separation of electron-hole pairs. Generation of ·O 2 - and ·OH radicals fostered mutual conversion of Br - and ·Br, playing a vital role in bromate removal. Moreover, TBR showed excellent stability. This research expands the potential of non-precious-metal photocatalytic co-catalysts for water treatment.
研究领域:
环境科学
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材料科学
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化学工程
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Qian Xiao,Zhe Yang,Wanbin Li,Bo Wei,Hao Guo,Shuili Yu,Qimao Gan,Wenyu Liu,Chuyang Y. Tang
Advanced reduction processes (ARPs) are promising for pollutant removal in drinking water treatment. In this study, we demonstrated highly efficient reduction of bromate, a harmful disinfection byproduct, by coupling ARPs with an iron nanoparticles-intercalated graphene oxide (GO@FeNPs) catalytic membrane. In the presence of 1.0 mM sulfite (S(IV)), the GO@FeNPs membrane/S(IV) system achieved nearly complete removal of 80 μg/L bromate in 3 min. The first-order reaction rate constant for bromate removal in this system was 420 ± 42 min–1, up to 5 orders of magnitude faster than previously reported ARPs. The GO@FeNPs catalytic membrane may offer potential advantages of nanoconfinement and facilitated electron shuttling in addition to the high surface area of the fine FeNPs, leading to the remarkable ARP performance. The GO@FeNPs membrane showed excellent stability, maintaining >97.0% bromate removal over 20 cycles of repeated runs. The membrane can also be applied for fast catalytic reduction of other oxyanions, showing >98.0% removal of nitrate and chlorate. This work may present a viable option for utilizing high-performance reductive catalytic membranes for water decontamination.
研究领域:
环境科学
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材料科学
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水处理技术
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2017
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IF 6.065
Weirui Chen,Xukai Li,Yiming Tang,Jialu Zhou,Dan Wu,Yin Wu,Laisheng Li
A flexible catalyst, Fe-Cu-MCM-41, was employed to enhance diclofenac (DCF) mineralization and inhibit bromate formation in catalytic ozonation process. Greater TOC removal was achieved in Fe-Cu-MCM-41/O 3 process (78%) than those in Fe-MCM-41/O 3 (65%), Cu-MCM-41/O 3 (73%) and sole ozonation (42%). But it was interesting that both Cu-MCM-41/O 3 and Fe-MCM-41/O 3 achieved 93% bromate inhibition efficiency, only 71% inhibition efficiency was observed in Fe-Cu-MCM-41/O 3 . Influence of pH, TBA/NaHSO 3 and detection of by-products were conducted to explore the mechanism. By Pyridine adsorption–IR and XPS, a relationship was found among activity of catalysts, Lewis acid sites and electron transfer effect between Fe (II/III) and Cu (I/II). Fe-Cu-MCM-41 promoted ozone decomposition to generate OH, which accounted for enhanced DCF mineralization. The consumption of aqueous O 3 also suppressed the oxidative of Br − and HBrO/Br − . More HBrO/BrO − accumulated in catalytic ozonation process and less bromate generated. Bromate formation in Fe-Cu-MCM-41/O 3 process was sensitive with pH value, the acidic condition was not favor for bromate formation. Both DCF mineralization and bromate inhibition were influenced by surface reaction. Moreover, Fe-Cu-MCM-41 showed excellent catalytic performance in suppressing the accumulation of carboxylic acid, especially for oxalic acid. Nearly no oxalic acid was detected during Fe-Cu-MCM-41/O 3 process.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
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2016
·Vol. 45
·期 18
·7728-7736
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IF 4.177
Erbin Shi,Xiaoqin Zou,Jia Liu,Huiming Lin,Feng Zhang,Shaoxuan Shi,Fenghua Liu,Guangshan Zhu,Fengyu Qu
A facile electrochemical plating strategy has been employed to prepare the electroactive metal–organic framework film (NENU-3) onto a copper electrode in the acid electrolyte containing 1,3,5-benzenetricarboxylic acid (H3BTC) and phosphotungstic acid (PTA). The as-made NENU-3 films have been characterized using powder X-ray diffraction (PXRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR) spectroscopy and thermogravimetric analyses (TGA). These analyses indicate that NENU-3 films have high phase purity and high stability. Further, different electrochemical techniques are utilized for measuring the electrochemical behaviors of the NENU-3 film electrodes. Accordingly, the kinetic parameters of a NENU-3 film electrode towards the electrocatalytic reduction of bromate are obtained, including the electron transfer coefficient (α), the catalytic rate constant (ks), and the diffusion coefficient (D). The film electrodes present excellent electrocatalytic ability for the bromate reduction, and can be used successfully for the amperometric detection of bromate. Under the optimized conditions, the proposed sensor exhibits a wide linear range (0.05–72.74 mM) and a lower detection limit (12 μM) measured by chronoamperometry (CA). Moreover, the films possess high electrochemical stability and strong anti-interference capability in the bromate detection process. It has been demonstrated that the electrochemical plating method reported here offers a reliable and efficient way to fabricate MOF films on conductive substrates for bromate detection.
研究领域:
分析化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Ziying Wang,Na An,Yisheng Shao,Naiyun Gao,Erdeng Du,Bin Xu
Bromide (Br − ), which is omnipresent in water bodies, can not only affect the degradation kinetics of target pollutants but may also form undesired byproducts (such as bromate ( BrO 3 - ) and brominated disinfection byproducts (Br-DBPs)) through sulfate radical ( SO 4 ∙ - )-based advanced oxidation processes (AOPs). This study found that Br − significantly suppressed the degradation of diethyl phthalate (DEP) based on the ultraviolet (UV)/persulfate (PS) treatment and was efficiently converted into reactive species (radicals and free bromine) by the SO 4 ∙ - or hydroxyl radical (HO ) generated in the UV/PS system. These reactive bromine species could, in turn, brominate the phenolic degradation intermediates of DEP as well as natural organic matter (NOM), yielding Br-DBPs, including tribromomethane (TBM), which was observed when Br − , DEP and/or NOM coexisted in this UV/PS system. However, the Br-DBPs were a short-lived form of bromine during the transformation of Br – and were degraded by the excessive oxidants (e.g., S O 4 ∙ - and HO ). Instead, Br − was eventually transformed into BrO 3 - , with free bromine acting as the requisite intermediate. The BrO 3 - formation initially showed a delay before increasing monotonically. In general, raising the PS dosage and the initial Br − concentrations enhanced both the maximum concentration of TBM and the formation of BrO 3 - , while increasing the amounts of DEP and NOM facilitated the former and inhibited the latter. The maximum concentration of TBM increased while the formation of BrO 3 - was suppressed with increasing pH from 5.0 to 8.0. In addition, through simulating the steady-state concentration of radicals, it was found that the contribution of bromine atom radical (Br ) towards oxidizing free bromine to BrO 3 - was far greater than those of S O 4 ∙ - and HO . The findings demonstrate the potential negative effects of Br − on SO 4 ∙ - -based AOPs, which need to be considered when this technology is applied in practice.
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
Journal of Water Process Engineering
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2025
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IF 6.7
Ying Xu,Shuili Yu,Zhiqiang Fan,Xingli Ji,Cong Huang,Zheng Xu,Rui Liu,Chao Jiang
Bromate (BrO 3 − ), a carcinogenic and regulated disinfection by-product, poses a persistent challenge to drinking water safety due to its high solubility and chemical stability. In this work, a noble-metal-free Fe 3 O 4 /TiO 2 /Bi photocatalyst was successfully prepared and subsequently applied for BrO 3 − reduction under ultraviolet light. The ternary composite design enables cooperative functionality among the components, where Fe 3 O 4 facilitates charge transfer and magnetic separability, Bi 0 acts as a hole scavenger, and TiO 2 serves as the primary photoactive material. Characterization results confirmed the successful formation of the heterostructure with enhanced charge separation properties. The composite containing 5 wt% Bi exhibited the highest activity, achieving 99 % BrO 3 − removal within 25 min at pH 7.0, with a pseudo-first-order rate constant of 0.185 min −1 , which is 11.8 times that of pure TiO 2 . The enhanced photocatalytic performance is ascribed to the synergistic effect between Bi, Fe 3 O 4 and TiO 2 . Bi 0 nanoparticles functioned as hole acceptors to suppress recombination, while Fe 3 O 4 facilitated electron transport and provided magnetic separability. The photocatalyst retained high activity over five consecutive cycles with negligible metal leaching and performance loss. In addition, its effectiveness was verified in tap water containing typical inorganic ions and dissolved organic matter, demonstrating moderate inhibition but maintaining BrO 3 − reduction capability. This study provides a cost-effective, magnetically recoverable, and noble-metal-free photocatalyst with improved charge separation efficiency and recovery feasibility, offering practical potential for BrO 3 − mitigation in drinking water treatment.
研究领域:
环境科学
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材料科学
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水处理技术
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光催化
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2017
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IF 6.942
Guangsen Xia,Yujue Wang,Bin Wang,Jun Huang,Shubo Deng,Gang Yu
Previous studies indicate that effective generation of hydrogen peroxide (H 2 O 2 ) from cathodic oxygen (O 2 ) reduction is critical for the improved water treatment performance (e.g., enhanced pollutant degradation and reduced bromate formation) during the electro-peroxone (E-peroxone) process (a combined process of electrolysis and ozonation). However, undesired reactions (e.g., O 3 , H 2 O 2 , and H 2 O reductions) may occur in competition with O 2 reduction at the cathode. To get a better understanding of how these side reactions would affect the process, this study investigated the cathodic reaction mechanisms during electrolysis with O 2 /O 3 gas mixture sparging using various electrochemical techniques (e.g., linear sweep voltammetry and stepped-current chronopotentiometry). Results show that when a carbon brush cathode was used during electrolysis with O 2 /O 3 sparging, H 2 O and H 2 O 2 reductions were usually negligible cathodic reactions. However, O 3 can be preferentially reduced at much more positive potentials (ca. 0.9 V vs. SCE) than O 2 (ca. −0.1 V vs. SCE) at the carbon cathode. Therefore, cathodic O 2 reduction was inhibited when the process was operated under current limited conditions for cathodic O 3 reduction. The inhibition of O 2 reduction prevented the desired E-peroxone process (cathodic O 2 reduction to H 2 O 2 and ensuing reaction of H 2 O 2 with O 3 to OH) from occurring. In contrast, when cathodic O 3 reduction was limited by O 3 mass transfer to the cathode, cathodic O 2 reduction to H 2 O 2 could occur, thus enabling the E-peroxone process to enhance pollutant degradation and mineralization. Many process and water parameters (applied current, ozone dose, and reactivity of water constituents with O 3 ) can cause fundamental changes in the cathodic reaction mechanisms, thus profoundly influencing water treatment performance during the E-peroxone process. To exploit the benefits of H 2 O 2 in water treatment, reaction conditions should be carefully controlled to promote cathodic O 2 reduction during the E-peroxone process.
研究领域:
环境科学
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电化学工程
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DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
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IF 1.5
Siyue Zhang,Hui Cheng,Baoli Wang,Fan Shi,Lijun Yan,Lina Zeng,Lin Li,Shuhai He,Wei Sun
Petal-shaped FeS@MoS 2 -C nanocomposite was synthesized using carbon fiber as the basic carrier by hydrothermal method. The uniformly dispersed nanocomposite, hemoglobin (Hb) and Nafion mixture were drip-coated on the newly prepared carbon ionic liquid electrode (CILE) to build a modified electrode named as Nafion/Hb/FeS@MoS 2 -C/CILE. The morphology and valence state of FeS@MoS 2 -C nanocomposite was investigated by SEM, TEM, XPS etc. and the biological structure of Hb was not changed based on UV-VIS and FT-IR spectroscopic analysis. Electrochemistry of Nafion/Hb/FeS@MoS 2 -C/CILE was recorded by cyclic voltammetry with voltammetric behaviors investigated. Also, the modified electrode has excellent catalytic performance for nitrite, hydrogen peroxide, bromate with the detection range as 0.10~5.00 mmol L -1 , 0.10~14.00 mmol L -1 , 0.05~25.00 mmol L -1 , respectively. The pickle juice sample was analyzed by this method satisfactory, further proving the practical application.
研究领域:
生物化学
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分析化学
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DOI
高影响因子
CHEMOSPHERE
·
2019
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IF 5.108
Qi Han,Wenyi Dong,Hongjie Wang,Hang Ma,Peng Liu,Yurong Gu,Hongkai Fan,Xin Song
This study systematically investigated the performance of ozonation on tetrabromobisphenol A (TBBPA) degradation under different ozone dosages (5.21–83.33 μmoL/L), initial solution pH (3.0–11.0) and temperatures (10–50 °C). At the same time, the generations of inorganic products (bromide ion and bromate) under different experimental conditions were evaluated and the organic products were also identified. Then, the possible mechanism was proposed and verified by the quantum chemical calculation. In addition, variations and controlling of the toxicity were also analyzed, including acute toxicity, chronic toxicity and genotoxicity. Ozonation was proved to be an efficient and promising technology for removing TBBPA from water. TBBPA of 1.84 μmoL/L could be completely degraded within 5 min under the ozone dosage of 41.67 μmoL/L in wide ranges of pH (3.0–11.0) and temperature (10–40 °C). During the degradation of TBBPA, over 65% of the average bromine ion was detected and nine products were identified. The proposed degradation pathways verified that TBBPA might undergo addition and stepwise oxidative debromination, the hydrogen extraction, and the deprotonation. The results of toxicity testing showed that ozonation could effectively control the acute and chronic toxicity of the water samples, although the toxicity increased in the initial reaction stage due to the accumulation of more toxic intermediates.
研究领域:
环境科学
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化学工程
·
毒理学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2019
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IF 7.149
Zhihao Chen,Xuchun Li,Shujuan Zhang,Jiyuan Jin,Xiaojie Song,Xiaomeng Wang,Paul G. Tratnyek
Research efforts on advanced oxidation processes (AOPs) have long been focused on the fundamental chemistry of activation processes and free radical reactions. Little attention has been paid to the chemistry of the precursor oxidants. Herein, we found that the precursor oxidants could lead to quite different outcomes. A counterintuitive result was observed in the photoreduction of bromate/iodate: the combination of H2O2 and UV enhanced the reduction of bromate/iodate, whereas the addition of persulfate to the UV system led to an inhibitory effect. Thermodynamic and kinetic evidence suggests that the reduction of bromate in UV/H2O2 was attributable to the direct reaction between HOBr and H2O2. Both experimental determination and kinetic simulation demonstrate that the reaction between HOBr and H2O2 dominated over the •OH-mediated reactions. These results suggest that H2O2 possesses some particular redox properties that distinguish it from other peroxides. The prototypical UV/H2O2 process is not always an AOP: it can also be an enhanced reduction process for chemicals with intermediates that are reducible by H2O2. Considering the increasing interest in persulfate-based AOPs, the results of this study identify some novel advantages of the classical H2O2-based AOPs.
研究领域:
环境化学
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水处理
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化学工程
✓ 已验证
DOI
PubMed
高影响因子