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CHEMOSPHERE · 2020 · IF 5.778

WS2 as highly active co-catalyst for the regeneration of Fe(II) in the advanced oxidation processes

Haopeng Luo,Xin Zhou,Xiaojie Guo,Zhiyong Fang,Quanyuan Chen,Juan Zhou

The greatest constraint in the advanced oxidation processes involved Fe(II)/PMS was the low utilization of Fe(II) and PMS. In the present study, the co-catalytic effect of WS 2 on the Fe(II)/PMS system for the degradation of organics was investigated. In the presence of WS 2 , Fe(III) was reduced to Fe(II) during the reaction and resulted in improved decomposition of PMS as well as the degradation of 4-chloriphenol (4-CP). The decomposition rate of PMS and degradation efficiency of 4-CP were 10% and 25% in the Fe(II)/PMS process, while the efficiencies respectively increased to 99% and 100% in the WS 2 assisted Fe(II)/PMS system. The degradation of 4-CP was completed via the free radical pathway and SO 4 • - played a more important role than other active species. Low concentration of inorganic ions such as Cl − and HCO 3 − exhibited irrelevant effect while humic acid showed significant suppression on the WS 2 /Fe(II)/PMS system. Additionally, characterization and recycle results implied that WS 2 maintained a good stability during the co-catalytic processes.

研究领域: 环境科学 · 化学工程
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Coatings · 2023 ·Vol. 13 ·期 3 ·655 · IF 3.4

Ti3C2@g-C3N4/TiO2 Ternary Heterogeneous Photocatalyst for Promoted Photocatalytic Degradation Activities

Yuxin Bai,Shasha Xu,Jing Chen,Xun Sun,Shan Zhao,Jingcai Chang,Zuoli He

Ternary heterojunction photocatalysts can improve the transport and separation of photogenerated electrons and holes, which could promote their reduction and oxidation properties for environmental and energy applications. In this research, the ternary photocatalyst Ti3C2@TiO2/g-C3N4was successfully synthesized via direct electrostatic self-assembly during hydrothermal process. Ti3C2MXene was used to optimize the interfacial carrier transport and separation between the interfaces. The obtained ternary heterostructured photocatalyst had a higher photocatalytic degradation performance for removing rhodamine B (RhB) and 4-chlorophenol (4-CP). The synergistic effect of heterojunction between g-C3N4and TiO2and Schottky barrier presented among TiO2and Ti3C2suppressed the recombination of the photogenerated electron–hole pairs. Moreover, the Ti3C2can serve as an active site for the adsorption and activation of organic pollutants resulting from sufficient functional groups (F−here).Keywords:Ti3C2;g-C3N4;heterojunction;photocatalyst;4-chlorophenol

研究领域: 环境科学 · 材料科学 · 化学工程
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Nanomaterials · 2018 ·Vol. 8 ·期 3 ·141 · IF 3.504

Palladium Supported on Titanium Carbide: A Highly Efficient, Durable, and Recyclable Bifunctional Catalyst for the Transformation of 4-Chlorophenol and 4-Nitrophenol

Guangyin Fan,Xiaojing Li,Caili Xu,Weidong Jiang,Yun Zhang,Daojiang Gao,Jian Bi,Yi Wang

Developing highly efficient and recyclable catalysts for the transformation of toxic organic contaminates still remains a challenge. Herein, Titanium Carbide (Ti3C2) MXene modified by alkali treatment process was selected as a support (designated as alk-Ti3C2X2, where X represents the surface terminations) for the synthesis of Pd/alk-Ti3C2X2. Results show that the alkali treatment leads to the increase of surface area and surface oxygen-containing groups of Ti3C2X2, thereby facilitating the dispersion and stabilization of Pd species on the surface of alk-Ti3C2X2. The Pd/alk-Ti3C2X2catalyst shows excellent catalytic activity for the hydrodechlorination of 4-chlorophenol and the hydrogenation of 4-nitrophenol in aqueous solution at 25 °C and hydrogen balloon pressure. High initial reaction rates of 216.6 and 126.3 min−1·gpd−1are observed for the hydrodechlorination of 4-chlorophenol and hydrogenation of 4-nitrophenol, respectively. Most importantly, Pd/alk-Ti3C2X2exhibits excellent stability and recyclability in both reactions without any promoters. The superior property of Pd/alk-Ti3C2X2makes it as a potential material for practical applications.Keywords:palladium;titanium carbide;catalytic transformation;4-chlorophenol;4-nitrophenol

研究领域: 材料科学 · 环境科学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Important role of carbon doping in photocatalytic peroxymonosulfate activation of carbon nitride for efficient 4-Chlorophenol degradation

Yuan Zhang,Kangping Cui,Xueyan Liu,Minshu Cui,Xing Chen,Yuchao Tang,Haiyang Li,Kun Wang

In order to improve the photocatalytic activity of pristine carbon nitride while maintaining its metal-free property to achieve the activation of peroxymonosulfate (PMS), a series of carbon-doped g-C 3 N 4 (BCN) with different carbon contents were synthesized in this paper by adding benzotriazole to urea. The catalyst obtained by this approach significantly promoted PMS activation and enhanced the degradation efficiency of 4-chlorophenol (4-CP). Experiments and theoretical calculations showed that the introduction of carbon not only narrowed the band gap, but also accelerated the separation of photoinduced electron-hole pairs, which greatly improved the photocatalytic activity of g-C 3 N 4 . In the degradation of pollutants, free radicals and non-free radicals acted simultaneously, with non-free radicals playing a dominant role. This study explained the origin of 1 O 2 by Density functional theory (DFT) calculations, visible light excited photocatalysts to form holes, while carbon introduction decreased the valence-electron density around the area, inducing electron transfer from PMS toward g-C 3 N 4 directed to generate 1 O 2 . The 1 O 2 -dominated degradation process improved the application of the catalysts in complex aqueous matrices. In addition, we proposed 4-CP degradation pathways, and the toxicity of intermediates derived from 4-CP degradation process reduced.

CAS / MDL: 106-48-9 57-13-6
研究领域: 环境科学 · 材料科学
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ENVIRONMENT INTERNATIONAL · 2020 · IF 7.577

A novel stabilized carbon-coated nZVI as heterogeneous persulfate catalyst for enhanced degradation of 4-chlorophenol

Song Li,Jingchun Tang,Qinglong Liu,Xiaomei Liu,Bin Gao

Nano zero-valent iron (nZVI) and its composite materials have been extensively studied in the field of environmental remediation. However, the oxidation and agglomeration of nZVI limits the large-scale application of nZVI in environmental remediation. This study developed a two-step method to prepare stable carbon-coated nZVI (Fe 0 @C) which combined hydrothermal carbonization and carbothermal reduction methods and used glucose and iron oxide (Fe 3 O 4 ) as precursors. When the carbothermal reduction temperature was 700 °C and the elemental molar ratio of carbon to iron was 22:1, stable Fe 0 @C can be generated. The nZVI particles are encapsulated by mesoporous carbon and embedded in the carbon spheres. The unique structure of carbon coating not only inhibits the agglomeration of nZVI, but also makes nZVI stable in air for more than 120 days. Not only that, the as-synthesized Fe 0 @C exhibited high catalytic activity toward the degradation of 4-chlorophenol (4-CP) by activating persulfate. Different from conventional nZVI catalysts in generation of sulfate radicals, Fe 0 @C selectively induced hydroxyl radicals for 4-CP degradation. Moreover, Fe 0 @C has been shown to efficiently degrade 4-CP by using the dissolved oxygen in water to form hydroxyl radicals. This study not only provides a simple, green method for the preparation of stabilized nZVI, but also provides the possibility of large-scale application of nZVI in the field of environmental remediation.

CAS / MDL: 1317-61-9 1310-73-2
研究领域: 环境科学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Experimental and theoretical unraveling of the electrocatalytic hydrodechlorination of chlorinated phenol using Pd promoted by oxygen vacancies in TiO2 array

Zijin Pang,Degang Li,Xinru Wang,Xin Huang,Yu-Shi He,Weimin Zhang,Lipeng Zhang

The electrocatalytic dichlorination (EHDC) shows a promising potential to degrade chlorinated phenols (CPs). It is also a green technology in reducing the corresponding hazardous impact on the environment. In this study, we constructed a catalytic structure which was Pd on a TiO 2 array with oxygen vacancies on carbon fibre paper substrate (Pd/TiO 2 /CFP) by a relatively mild route. Due to the presence of the oxygen vacancies, the resulting strong metal-support interaction (SMSI) effect has been identified which featured a redistribution of spatial charge in Pd/TiO 2 . The electron flow from the oxygen vacancies in the TiO 2 to Pd facilitated the adsorption of Pd with 4-chlorophenol (4-CP) and endowed the Pd metal with an improved chemical reaction kinetics even at a low Pd loading. Experimentally, we studied the dependence of pH, concentration of 4-CP, and working potential on the reaction conditions of EHDC. The results showed that the conversion of 4-CP reached 100 % within 180 min with an apparent rate constant of 2.9 × 10 -2 min −1 and the dominant product was phenol (P). The multi-cycle test illustrated that the Pd/TiO 2 /CFP electrode showed superior stability. The results also revealed that the comprehensive catalytic behavior was much better than those of the Pd/CFP and the TiO 2 /CFP electrodes. The density function theory (DFT) calculations indicated that 4-CP was more preferably absorbed on Pd/TiO 2 /CFP than Pd/CFP due to the SMSI assistance. This study provides a valuable guide in the preparation of precious metal-based electrodes for EHDC with a reduced loading and cost but without performance compromise.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Oxygen-deficient WO3−x nanoplate array film photoanode for efficient photoelectrocatalytic water decontamination

Xuefeng Liu,Hao Zhou,Shuzhao Pei,Shupo Xie,Shijie You

Photoelectrocatalysis (PEC) represents a promising method for water decontamination, but the overall performance is limited by slow interfacial charge transfer. In this study, we address this limitation by creating an efficient PEC system with oxygen-deficient WO 3−x nanoplate array film serving as photoanode through surface reduction method. Oxygen vacancy had a slight impact to catalytic activity of photoanode, but exhibited an enhanced performance when anodic polarization was imposed. Based on a front-side illumination and potential of 1.2 V vs standard hydrogen electrode (SHE), the WO 3−x photoanode produced a photocurrent being 7.3 times as WO 3 photoanode, indicating a substantially enhanced interfacial charge transfer. Both WO 3 and WO 3−x electrodes showed an insignificant removal of 4-chlorophenol (4-CP) and dechlorination under individual photocatalytic condition. When anodic polarization was applied at 1.2 V vs SHE, 85.5% removal of 4-chlorophenol (4-CP) and 48% dechlorination efficiency could be obtained for WO 3−x photoanode, accounting for the values being 32.7% and 25.8% higher than that for WO 3 photoanode. The corresponding first-order kinetic constant for 4-CP removal by WO 3−x ( k  = 0.0157 min −1 ) was approximately 2.53 times as that by WO 3 ( k  = 0.0062 min −1 ). The improved PEC performance of WO 3−x photoanode under low potential bias should result from faster interfacial charge transfer, mitigation of electron-hole recombination, and production of higher amount of hydroxyl radical ( OH). This study not only suggests the important role of oxygen vacancy in PEC system, but also provides a new strategy to develop a full solar-energy-based water purification system.

研究领域: 环境科学 · 材料科学
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RSC Advances · 2014 ·Vol. 5 ·期 4 ·2449-2456 · IF 3.708

High-dispersive FeS2 on graphene oxide for effective degradation of 4-chlorophenol

Wanpeng Liu,Lili Xu,Xingfa Li,Chensi Shen,Sadia Rashid,Yuezhong Wen,Weiping Liu,Xiaohua Wu

A high-dispersive FeS2 micro-cube crystal on graphene oxide (FeS2@GO) was fabricated by a one-pot hydrothermal method. The catalytic degradation of 4-chlorophenol (4-CP) and its mechanism in a FeS2@GO-based Fenton system was investigated. Under acidic to slight alkaline conditions, FeS2@GO demonstrated an excellent capacity to remove 4-CP. More than 97% of 4-CP was eliminated within 60 min in pH 7.0 reaction solutions initially containing 0.2 g L−1 FeS2@GO, 128.6 mg L−1 4-CP and 100 mM H2O2 at 25 ± 1 °C, and the removal of 4-CP was further enhanced with increasing FeS2@GO loadings. In the meantime, the FeS2@GO also achieved lower iron leaching and a more complete TOC removal compared with pure synthetic FeS2 without graphene oxide. Furthermore, acetic acid and oxalic acid were identified as the primary products. The remarkable capacity of the FeS2@GO-based Fenton system in removing 4-CP displays its potential application in the treatment of organic compound-contaminated water.

CAS / MDL: 106-48-9
研究领域: 环境科学 · 材料科学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2017 · IF 6.198

Performance and Mechanism of Piezo-Catalytic Degradation of 4-Chlorophenol: Finding of Effective Piezo-Dechlorination

Shenyu Lan,Jinxi Feng,Ya Xiong,Shuanghong Tian,Shengwei Liu,Lingjun Kong

Piezo-catalysis was first used to degrade a nondye pollutant, 4-chlorophenol (4-CP). In this process, hydrothermally synthesized tetragonal BaTiO3 nano/micrometer-sized particles were used as the piezo-catalyst, and the ultrasonic irradiation with low frequency was selected as the vibration energy to cause the deformation of tetragonal BaTiO3. It was found that the piezoelectric potential from the deformation could not only successfully degrade 4-chlorophenol but also effectively dechlorinate it at the same time, and five kinds of dechlorinated intermediates, hydroquinone, benzoquinone, phenol, cyclohexanone, and cyclohexanol, were determined. This is the first sample of piezo-dechlorination. Although various active species, including h+, e–, •H, •OH, •O2–, 1O2, and H2O2, were generated in the piezoelectric process, it was confirmed by ESR, scavenger studies, and LC-MS that the degradation and dechlorination were mainly attributed to •OH radicals. These •OH radicals were chiefly derived from the electron reduction of O2, partly from the hole oxidation of H2O. These results indicated that the piezo-catalysis was an emerging and effective advanced oxidation technology for degradation and dechlorination of organic pollutants.

研究领域: 环境科学 · 材料科学
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Sustainability · 2023 ·Vol. 15 ·期 11 ·9060 · IF 3.9

Ultrasonic–Thermal Regeneration of Spent Powdered Activated Carbon

Tingting Zhang,Yanling Yang,Xing Li,Zhiwei Zhou,Bigui Wei

This study investigated the ultrasonic–thermal regeneration of powdered activated carbon (PAC) spent using 4-chlorophenol (4-CP). Similarly, a thermal regeneration process was also studied and the reaction conditions (i.e., regeneration temperature, heating rate, regeneration time) were tested. Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) analysis were applied to characterize the regenerated PACs under different treatments (thermal, ultrasonic and ultrasonic–thermal) and also compare them with the fresh and exhausted PACs. According to our regeneration observations, the ideal regeneration parameters were determined to be a 40 kHz frequency, 0.18 W/mL sonication power, 0.1 M NaOH and 50% (v/v) ethyl alcohol as the regeneration solution, and 1 g/L of saturated PAC mass with thermal regeneration as the second stage at 500 °C, desorbed for 30 min with a heating rate of 20 °C min−1. Under these conditions, the RE value achieved 90.99% and the η value reached 5.6%. The results of FTIR, XPS and XRD revealed that the oxygen functional group content of ultrasonic–thermal regenerated PAC significantly increased. These oxygenous groups exerted a positive effect on the adsorption process of the regenerated PAC and the subsequent adsorption–regeneration process.Keywords:ultrasonic;thermal;regeneration;powdered activated carbon;characteristic

研究领域: 环境科学 · 材料科学
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY · 2025 · IF 4.7

Recognition-enrichment-in-situ degradation of p-chlorophenol by Fe-IL@UIO-66

Yanhao Xu,Ziyi Zhong,Pinle Zhang,Huancheng Huang,Kuan Cai,Xinliang Liu

Persistent organic pollutants (POPs) represent a significant environmental and health risk due to their high toxicity, persistence, strong accumulation potential, and adverse effects on human health. 4-Chlorophenol (4-CP), a type of POP, has low catalytic efficiency at low concentrations and is easily interfered with by other pollutants, making its degradation challenging. A new “recognition-enrichment-in-situ degradation” strategy is introduced to selectively remove chlorophenols from contaminated aqueous environments. In this study, ionic liquids were incorporated into the UIO-66 framework as active sites for selective adsorption. 4-CP contains phenolic hydroxyl groups and exhibits high polarity. The dispersive interactions between 4-CP and ionic liquids, along with hydrogen-bonding interactions between the Tf 2 N anion and the hydroxyl groups of 4-CP, enhance the selective enrichment of 4-CP within the nanocavities of the metal–organic frameworks (MOFs). Fe 3+ was then introduced, enabling in-situ degradation of 4-CP through photo-induced generation of free radicals and cavities from H 2 O 2 catalyzed by Fe-IL@UIO-66. The results indicated that the adsorption capacity of IL@UIO-66 for 4-CP reached 53 %, significantly higher than that for five other organic pollutants. The adsorption capacity of IL@UIO-66 for 4-CP reached 509.5 mg g −1 , 49.9 % greater than that of the original UIO-66. The degradation efficiency of 4-CP by Fe-IL@UIO-66 increased from 61 % to 81 %, and after four cycles, the material retained a catalytic activity with a degradation efficiency of 64.2 %. This study provides valuable insights into the recognition-enrichment-in-situ catalytic strategy for treating low-concentration, highly toxic wastewater.

研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Removal of 4-chlorophenol, bisphenol A and nonylphenol mixtures by aqueous chlorination and formation of coupling products

Wenrui Xiang,Ruijuan Qu,Xinghao Wang,Zunyao Wang,May Bin-Jumah,Ahmed A. Allam,Feng Zhu,Zongli Huo

Phenolic endocrine disrupting chemicals (EDCs) such as bisphenol A (BPA), 4-chlorophenol (4-CP) and nonylphenol (NP) are the most commonly detected pollutants in natural environments. The transformation of mixtures of the three phenolic pollutants during chlorination process was studied for the first time in this work. Single phenol can be effectively removed by free chlorine via electrophilic substitution and electron transfer reactions, with the generation of chlorinated phenols and self-coupling products. In mixture solution, the apparent second-order rate constants ( k app ) of 4-CP, BPA and NP at pH 8.0 was increased by 8.6%, 25% and 16%, respectively, as compared to the degradation of single-compound. According to the products identification and density functional theory calculations, the cross-coupling process can occur more easily than the self-coupling reaction, which might accelerate the removal of phenolic mixtures. In addition, humic acid (HA) exerts some inhibitory effect on the degradation of phenolic compounds, due to the competition for chlorine consumption and the reduction of phenoxy radicals to parent phenols. These findings shed light on the environmental fate of phenolic mixtures during aqueous chlorination process, which provide new information for the application of chlorination in water and wastewater treatment.

CAS / MDL: 1415-93-6 7772-98-7
研究领域: 环境科学 · 水处理工程 · 化学动力学
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