DALTON TRANSACTIONS
·
2024
·
IF 3.5
Xiaoyu Chu,Xinrui Wang,Shuo Tian,Yongkuo Zhao,Shikai Liu,Hong Yan,Yan Shang
Modulating the photogenerated electrons of CeO2 to activate O2 and efficiently photocatalytic degradation of chlorophenols is a highly desired goal. Herein, we have successfully fabricated FePc/CeO2 heterojunction through H-bond induced assembly. The photocatalytic degradation of 2, 4-DCP by the amount-optimized FePc/CeO2 nanocomposite was improved by 3 times compared with pure CeO2. By means of electron paramagnetic resonance (EPR) and single wavelength photocurrent spectroscopy, it is confirmed that the excellent photocatalytic performance is mainly attributed to the formation of Z-scheme heterojunction, which promotes charge separation and transfer, and the introduction of FePc broadens the visible light absorption range of heterojunction. Moreover, O2 temperature-programmed-desorbed curves and electrochemical O2 reduction measurements results demonstrate that the single Fe-N4(II) site in FePc is more conducive to promoting O2 activation than that of other metal phthalocyanines. Based on in situ FT-IR and liquid chromatography-tandem mass spectrometry (LC-MS), a possible reaction pathway of 2, 4-DCP degradation was proposed. This study provides a novel strategy to prepare CeO2 based Z-scheme heterojunctions with abundant monoatomic sites for pollutant degradation.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Xiaoxue Pan,Junyan Wei,Mengting Zou,Jing Chen,Ruijuan Qu,Zunyao Wang
We systemically investigated the transformation behavior of 2,4-dichlorophenol (24-DCP) in seven different reaction systems including KMnO 4 , heat/PS, O 3 , UV, Fenton, NaClO and K 2 FeO 4 treatment. The results revealed that complete removal of 24-DCP could be reached in minutes, especially for Fe(VI), KMnO 4 , NaClO, Fenton and O 3 system. A total of 41 products were identified by LC-MS, and 10 of them were validated using commercial and self-synthesized standards. Hydroxyl substitution and coupling reactions were commonly observed in the studied systems. Meanwhile, extra routes such as sulfate substitution, (de)chlorination and direct oxidation were also involved for certain oxidation methods. Comparisons showed that a high degree of chlorination (>90%) occurred for NaClO system, while coupling products accounted for ~45% of the removed 24-DCP under PS oxidation. Moreover, low mineralization degree together with high aquatic toxicity was attributed to the occurrence of coupling reaction, which was possibly related to the redox potential of the main oxidative species. Considering the low abundance of coupling products and the gentle reaction condition, UV irradiation is a better option for 24-DCP removal in water and wastewaters. These findings can deepen our understanding on the transformation process of 24-DCP and provide some useful information for the environmental elimination of substituted phenols.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
Journal of Environmental Sciences
·
2019
·
IF 3.556
Kaiyuan Zheng,Yuqiao Song,Xu Wang,Xin Li,Xuhui Mao,Dihua Wang
Herein, with the exploitation of iron and nickel electrodes, the 2,4-dichlorophenol (2,4-DCP) dechlorinating processes at the anode and cathode, respectively, were separately studied via various electrochemical techniques (e.g., Tafel polarization, linear polarization , electrochemical impedance spectroscopy). With this in mind, Ni/Fe nanoparticles were prepared by chemical solution deposition, and utilized to test the dechlorination activities of 2,4-DCP over a bimetallic system. For the iron anode, the results showed that higher 2,4-DCP concentration and solution acidity aggravated the corrosion within the electrode. The charge transfer resistance ( R ct ) values of the iron electrode were 703, 473, 444, and 437 Ω ∙ cm 2 for the initial 2,4-DCP concentrations of 0, 20, 50, and 80 mg/L, respectively. When the bulk pH of the 2,4-DCP solution varied from 3.0, 5.0 to 7.0, the corresponding R ct values were 315, 376, and 444 Ω ∙ cm 2 , respectively. For the nickel cathode, the reduction current densities on the electrode at − 0.75 V (vs. saturated calomel electrode) were 80, 106, and 111 μA/cm 2 , for initial 2,4-DCP concentrations of 40, 80, and 125 mg/L. The dechlorination experiments demonstrated that when the initial pH of the solution was 7.0, 5.0, and 3.0, the dechlorination percentage of 2,4-DCP by Ni/Fe nanoparticles was 62%, 69%, and 74%, respectively, which was in line with the electrochemical experiments. 10 wt.% Ni loading into Ni/Fe bimetal was affordable and gave a good dechlorination efficiency of 2,4-DCP, and fortunately the Ni/Fe nanoparticles remained comparatively stable in the dechlorination processes at pH 3.0.
研究领域:
环境科学
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电化学工程
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2015
·
IF 4.529
Yunfang Chen,Jianzhang Fang,Shaoyou Lu,Yan Wu,Dazhi Chen,Liyan Huang,Cong Cheng,Lu Ren,Ximiao Zhu,Zhanqiang Fang
This study aims at photocatalytic degradation of 2,4-DCP with the assistance of H 2 O 2 in aqueous solution by a composite catalyst of Ag-rectorite. The catalysts were prepared via a novel thermal decomposition method followed after the cation-exchange process. The synthesized nano-materials were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Brunauer–Emmett–Teller (BET) surface analyzer, Ultraviolet–visible light (UV–vis) absorption spectra, field-emission scanning electron microscope (FE-SEM) and transmission electron microscope (TEM). The different mechanisms of degradation process with or without visible light irradiation were discussed, respectively. Moreover, the degradation efficiency of 2,4-DCP wastewater under Ag-rectorite/H 2 O 2 /visible light system was investigated by series of experiments, concerning on effects of major operation factors, such as H 2 O 2 dosage and the initial pH value. The highest degradation rate was observed when adding 0.18 mL H 2 O 2 into 50 mL 2,4-DCP solution, and the optimal pH value was 4 for the reaction. Afterwards, total organic carbon (TOC) experiments were carried out to evaluate the mineralization ratio of 2,4-DCP.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
BULLETIN OF MATERIALS SCIENCE
·
2020
·Vol. 43
·期 1
·1-7
·
IF 1.392
Xiao Meng,Peng Yu,Pang Mengting,Hao Baicun,Wang Yujia,Zhang Yulian,Liao Yang,Mao Hui
Heterogeneous Pd catalysts were developed by immobilizing Pd nanoparticles (Pd NPs) onto plant polyphenol (bayberry tannin, BT) decorated γ-Al 2 O 3 . The abundant hydroxyls of plant polyphenols were capable of stabilizing the Pd NPs. Transmission electron microscopy observation confirmed that the Pd NPs with the diameter of 3.75 ± 0.5 nm were highly dispersed in the catalyst. The as-prepared Al 2 O 3 –BT–Pd catalysts were found to be highly active in mild hydrodechlorination (HDC) of 2,4-dichlorophenols (DCPs) using formic acid as a hydrogen source. The 2,4-DCPs were completely dechlorinated in 4 h at 30°C and under atmospheric pressure. During the catalytic HDC, the stabilizing capability of BT successfully prevented the leakage and aggregation of Pd NPs, thus ensuring a high cycling stability with stable and high catalytic activity. The Al 2 O 3 –BT–Pd catalysts were recycled six times, without obvious loss of activity. In the sixth cycle, the catalytic HDC yield still reached 98.29% under the same reaction conditions, superior to the control catalysts, including γ-Al 2 O 3 supported Pd NPs (Al 2 O 3 –Pd) and powdered activated carbon supported Pd NPs (AC–Pd). Furthermore, the Al 2 O 3 –BT–Pd also showed high activity in the mild catalytic HDC of 2,4,6-trichlorophenols and chlorobenzene derivatives. Our results demonstrated efficient catalysts to address the environmental issue of chlorophenol pollution.
研究领域:
环境科学
·
催化化学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Chang Zhou,Qiang Cao,Jia-Liang Wei,Jing-Hui He,Jian-Mei Lu
Soil contaminated by 2,4-dichlorophenol (2,4-DCP) is a substantial environmental concern because it poses severe health hazards. Fenton and Fenton-like oxidation in the removal of 2,4-DCP in soil has attracted considerable attention but suffers from low efficiency due to strong adsorption of pollutants by soil. In this study, the non-toxic catalyst (DFNS-Fe 2 O 3 ) was prepared by loading Fe 2 O 3 on dendritic fibrous nanosilica (DFNS) for degradation of 2,4-DCP in soil. DFNS-Fe 2 O 3 could rapidly remove 2,4-DCP within 120 min (98 %), and the removal rate maintained 70 % after 3 cycles of durability test. In addition, BPA, phenol and 2-CP could be efficiently degraded by DFNS-Fe 2 O 3 . •OH and •O 2 were the main reactive oxygen species (ROS) in the reaction. It is speculated that 2,4-DCP degrades through hydroxylation, substitution process according to the GC-MS results. The toxicity of 2,4-DCP and intermediate products were observed by Ecological Structure Activity Relationships Predictive Model program (ECOSAR). This work paves an avenue for rational design of heterogeneous catalyst on DFNS and their applications in chlorophenol contaminated soil.
研究领域:
环境科学
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2015
·
IF 3.34
Qiong Tan,Guiqiu Chen,Guangming Zeng,Anwei Chen,Song Guan,Zhongwu Li,Yanan Zuo,Zhenzhen Huang,Zhi Guo
Immobilized Phanerochaete chrysosporium loaded with TiO 2 nanoparticles (PTNs) are novel high-value bioremediation materials for adsorbing cadmium and for degrading 2,4-dichlorophenol (2,4-DCP). The real-time changes in H + and O 2 fluxes were measured using the noninvasive microtest technique (NMT). The H + influx increased after the addition of 2,4-DCP, and shifted to efflux following the addition of Cd 2+ . The O 2 flux decreased after the addition of both 2,4-DCP and Cd 2+ . A larger Cd 2+ flux was immediately observed after exposure to 0.5 mM Cd 2+ (−351.25 pmol cm −2 s −1 ) than to 0.1 mM Cd 2+ (−107.47 pmol cm −2 s −1 ). The removal of Cd 2+ by the PTNs increased more after treatment with the 0.5 mM exposure solution (27.6 mg g −1 ) than with the 0.1 mM exposure solution (3.49 mg g −1 ). The enzyme activities were analyzed to review the antioxidative defense system of PTNs in a solution containing various concentrations of Cd 2+ . The activities of the coenzyme nicotinamide adenine dinucleotide (NADH) oxidase as well as the enzyme catalase (CAT) plateaued at 6.5 U g −1 FW and 9.7 U g −1 FW, respectively, after exposure to 0.25 mM Cd 2+ . The activity of superoxide dismutase (SOD) increased gradually in solutions containing 0.1–0.6 mM Cd 2+ , and eventually reached a maximum (68.86 U g −1 FW). These results illustrate how the antioxidative defense system and the physiological fluxes of PTNs respond to the stress caused by toxic pollutants .
研究领域:
环境生物学
·
微生物学
✓ 已验证
DOI
PubMed
高影响因子
LUMINESCENCE
·
2025
·Vol. 40
·期 4
·e70164
·
IF 3
Lin Zhou,Xuan Chen,Zhanghong Guo,Haining Cui,Jinxin Ma,Qijun Song
Metal nanoclusters (MNCs) have attracted widespread attention due to their unique subnanometer size, tunable fluorescence emission, and excellent biocompatibility. However, the enzyme-like activity and the optical properties of MNCs are rarely exploited simultaneously. Here, iridium nanoclusters (Py-IrNCs) with excellent fluorescence properties and the laccase-like activity were synthesized by the reduction of IrCl 3 with NaBH 4 in the presence of pyrogallol. The laccase activity of Py-IrNCs exhibited in the catalytic transformation of 2,4-dichlorophenol (2, 4-DP) is substantially superior to that of natural laccase, which is manifested by the fact that the amount of Py-IrNCs was only 2.5% of natural laccase to achieve the same catalytic performance. In the coexisting of 4-aminoantipyrine (4-AP), a distinct color change and quench of fluorescence were observed; thus, a sensitive colorimetric and fluorescence dual-mode determination of 2,4-DP was achieved with a linear range of 0–40 μM and a limit of detection of 0.5 μM. The dual-mode detections can be mutually verified, which effectively improved the reliability of the analysis, demonstrating a promising application potential of Py-IrNCs in pollutant determination.
研究领域:
分析化学
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环境科学
·
纳米技术
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产品关联
DOI
PubMed
高影响因子
ULTRASONICS SONOCHEMISTRY
·
2012
·
IF 3.567
Deming Zhao,Min Li,Dexing Zhang,Shams Ali Baig,Xinhua Xu
Palladium/Iron (Pd/Fe) nanoparticles were prepared by using ultrasound strengthened liquid phase reductive method to enhance dispersion and avoid agglomeration. The dechlorination of 2,4-dichlorophenol (2,4-DCP) by Pd/Fe nanoparticles was investigated to understand its feasibility for an in situ remediation of contaminated groundwater. Results showed that 2,4-DCP was first adsorbed by Pd/Fe nanoparticles, then quickly reduced to o-chlorophenol (o-CP), p-chlorophenol (p-CP), and finally to phenol (P). The induction of ultrasound during the preparation of Pd/Fe nanoparticles further enhanced the removal efficiency of 2,4-DCP, as a result, the phenol production rates increased from 65% (in the absence of ultrasonic irradiation) to 91% (in the presence of ultrasonic irradiation) within 2 h. Our data suggested that the dechlorination rate was dependent on various factors including Pd loading percentage over Fe 0 , Pd/Fe nanoparticles availability, temperature, mechanical stirring speed, and initial pH values. Up to 99.2% of 2,4-DCP was removed after 300 min reaction with these conditions: Pd loading percentage over Fe 0 0.3 wt.%, initial 2,4-DCP concentration 20 mg L −1 , Pd/Fe dosage 3 g L −1 , initial pH value 3.0, and reaction temperature 25 °C. The degradation of 2,4-DCP followed pseudo-first-order kinetics reaction and the apparent pseudo-first-order kinetics constant was 0.0468 min −1 .
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 13
·10633-10640
·
IF 3.289
Chao Sun,Rui Zhou,Jianan E,Jiaqiang Sun,Yu Su,Hejun Ren
Magnetic nanoscaled ascorbic acid/magnetite (H2A/Fe3O4) composite was prepared by oxidative polymerization and proposed as a novel heterogeneous catalyst of persulfate (PS) for improved degradation of 2,4-dichlorophenol (2,4-DCP). The composite was fully characterized and evaluated in terms of catalytic activity, effect of reaction parameters, iron ion leaching, and identification of primary reaction oxidants, as well as the possible role of H2A. The degradation efficiency of 2,4-DCP reached 98.5% within 150 min using the H2A/Fe3O4 nanocomposite compared with only 35.1% under the same conditions for pure nano Fe3O4. This result indicated an enhancement in the performance of activated PS. The findings of this study provide some new insights into the potential of using H2A to enhance the performance of Fe3O4 nanoparticles in the activation of PS for improving the degradation of organic pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
WATER AIR AND SOIL POLLUTION
·
2017
·Vol. 228
·期 9
·1-11
·
IF 1.702
Feng Weihua,Zhang Lanxin,Fang Jianzhang,Lu Shaoyou,Wu Shuxing,Chen Yi,Fang Zhanqiang
Graphitic carbon nitride (g-C 3 N 4 ) is a photocatalyst with wide application in removal of organic pollutants. In this study, we designed a porous g-C 3 N 4 (p-g-C 3 N 4 )/8-quinolinolato iron(III) (Q 3 Fe)/H 2 O 2 system to enhance the organic pollutant removal efficiency by combining photocatalysis and Fenton interaction under neutral condition. The p-g-C 3 N 4 was prepared through a two-step thermal oxidation reaction. Afterwards, Q 3 Fe-coupled p-g-C 3 N 4 was prepared by an impregnating method. The 2,4-dichlorophenol (2,4-DCP) photodegradation ratio and decomposition rate of the p-g-C 3 N 4 /Q 3 Fe/H 2 O 2 system are approximately 5 and 18 times as high as those of individual p-g-C 3 N 4 system, respectively. Besides, its degradation rate is 4.3 times as high as that in the p-g-C 3 N 4 /H 2 O 2 system. Meanwhile, Q 3 Fe/g-C 3 N 4 also exhibits higher activity than individual p-g-C 3 N 4 in 2,4-DCP photo-decomposing. On the basis of the results of the radical trapping experiments and the Fe(II) concentration in different systems, the synergistic effect between photocatalysis and Fenton reaction is vital for the efficient pollutant degradation. The coupled system combining p-g-C 3 N 4 with Q 3 Fe and H 2 O 2 shows potential for efficient treatment of recalcitrant organic pollutants. The combined system in this work indicated a new idea for the decomposition of organic pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2024
·
IF 5.8
Zhoujie Pi,Puyu Zhou,Kun Luo,Li He,Shengjie Chen,Zhu Wang,Shanshan Zhang,Xiaoming Li,Qi Yang
Chlorophenols (CPs) have strong toxicity because of the presence of chlorine atoms. Although dechlorination can eliminate their toxicity, their by-products may cause secondary pollution. In this study, a two-step process of pre-reduction dechlorination and oxidation, reductive dechlorination by sulfidated nanoscale zero-valent iron (S-nZVI) and advanced oxidation by S-nZVI-activated peroxydisulfate (PDS), was innovatively adopted to achieve efficient and complete mineralization of 2,4-dichlorophenol (2,4-DCP). The pre-reduction of S-nZVI achieved 80% dechlorination of 2,4-DCP. With the subsequent addition of PDS, 2,4-DCP and its dechlorination by-products in the solution were almost completely removed, and the mineralization rate reached 91.5% under the optimal conditions of unadjusted initial pH (5.4), S-nZVI dosage 2.5 g L−1, and PDS concentration of 1.8 mM. The electron spin resonance (ESR) and radical quenching experiments demonstrated that both ·OH and SO4− were involved in the degradation of 2,4-DCP, while SO4− played a more predominant role. Based on the transformation products of 2,4-DCP identified by GC-MS, the degradation mechanism of 2,4-DCP in this system included two steps, namely, reductive dechlorination induced by electron transformation and oxidation degradation involving single electron transfer, radical adduct formation, and hydrogen atom abstraction. This study demonstrated that the novel S-nZVI pre-reduction and sequential S-nZVI/PDS process is a very promising and efficient approach for the complete removal of CPs in water.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）