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ACS Omega · 2020 · IF 2.87

Graphene Oxide–Crospolyvinylpyrrolidone Hybrid Microspheres for the Efficient Adsorption of 2,4,6-Trichlorophenol

Xiaofei Lv,Sifang Li

Microspheres of the graphene oxide and crospolyvinylpyrrolidone composite (GO–PVPP) were prepared via suspension polymerization and investigated for the adsorption of 2,4,6-trichlorophenol (2,4,6-TCP) from wastewater. The microspheres were thoroughly characterized using scanning electron microscopy, infrared spectroscopy, N2 physisorption, elemental analysis, X-ray diffraction, and thermogravimetric analysis. The GO–PVPP microspheres comprised GO sheets on the surface and demonstrated good thermal stability, good swelling rate, and excellent adsorption capacity of 2,4,6-TCP (up to 466.77 mg/g). The adsorptions were determined as a function of pH, temperature, adsorbent loading, adsorption time, and initial content of 2,4,6-TCP in the solutions. The sorption kinetics was satisfactorily modeled using the pseudo-second-order rate equation, and the sorption equilibrium can be described using the Freundlich model. The 2,4,6-TCP adsorption by GO–PVPP was shown to be endothermic and spontaneous. The reusability of GO–PVPP was also demonstrated by the adsorption and desorption cycles.

CAS / MDL: 110-26-9 88-06-2
研究领域: 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Boosting photocatalytic activity of C-F-TiO2 nanosheets derived from in-situ pyrolysis of MXene

Qi Zhao,Ye Yuan,Luyan Zhang,Liang Qiao,Cheng Ding,Kangshun Wang,Hongpeng Li,Jun Ma,Panpan Wang,Tianming Chen,Feihong Wang

Nonmetal doping is widely used in the modification of titanium dioxides (TiO 2 ) for photocatalytic applications. As a typical two-dimensional layered nanomaterial, the excellent physical and chemical properties of MXene materials have been the focus of current research. In this study, carbon and fluorine co-doped MXene derived TiO 2 nanosheets (labelled as C-F-TiO 2 ) were successfully synthesized and used as catalysts for degrading 2,4,6-trichlorophenol (2,4,6-TCP) under UV light irradiation. The C-F-TiO 2 with ultrathin nanosheet structure enhanced light absorption range and decreased the bandgaps. The degradation efficiency of 2,4,6-TCP by C-F-TiO 2 was over 99 % in 90 min, and the degradation rate was more than twice that of commercial TiO 2 . The degradation rate still remained about 90 % in 90 min after five cycles. The results of quenching experiments and electron spin resonance (ESR) illustrated that more reactive oxygen species (ROS) were generated in the C-F-TiO 2 /UV system, which was 1.5 times that of commercial pure TiO 2 , and • O 2 – was the dominant ROS for 2,4,6-TCP degradation. This study provided insight to utilize physicochemical characteristics of MXene to synthesize non-metal co-doped TiO 2 nanosheet as a catalyst, exhibiting excellent reactivity in the potential application for organic pollutant degradation.

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

Crystal defect engineering to construct oxygen vacancies in MXene-derived TiO2 nanocomposites for boosting photocatalytic degradation of 2,4,6-trichlorophenol

Feihong Wang,Qi Zhao,Hongpeng Li,Qiangshun Wu,Luyan Zhang,Yan Li,Liang Qiao,Ye Yuan,Jun Ma,Panpan Wang,Tianming Chen

Chlorophenolic pollutants pose serious threats to the aquatic ecosystem. Photocatalysis technology has broad prospects for decontamination. In this work, MXene-derived TiO 2 nanocomposites with mixed-crystal characteristics and oxygen vacancies (OVs) (E–TiO 2 @rGO) were successfully synthesized by atmosphere modulation. Compared with commercial TiO 2 and N 2 –TiO 2 @rGO (anatase phase), the rate constants of E–TiO 2 @rGO (0.06874 min −1 ) over 2,4,6-trichlorophenol (2,4,6-TCP) degradation increased 4 and 1.3 times, respectively. The enhanced photocatalytic performance was attributed to the co-existence of anatase and rutile phases. On the one hand, the mixed-crystal phase narrowed the band gap, broadening the light absorption range. On the other hand, it induced the generation of OVs, which has been demonstrated by DFT calculation. The presence of OVs improved the adsorption and activation of O 2 and H 2 O molecules, beneficial for the formation of active free radicals. In addition, the incorporation of rGO promoted the separation of electron-hole pairs. The Gibbs free energy of 2,4,6-TCP degradation revealed that the OVs and mixed-crystal could reduce the energy barrier of the rate-determining step, thereby boosting the dichlorination efficiency of 2,4,6-TCP. The superoxide free radical ( O 2 − ) was determined as the dominant active species. Finally, a possible mechanism of 2,4,6-TCP degradation with E–TiO 2 @rGO was clarified clearly. The proposed mixed-crystal defect engineering represents a novel strategy in the design and synthesis of photocatalysts.

研究领域: 环境科学 · 材料科学
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WATER AIR AND SOIL POLLUTION · 2020 ·Vol. 231 ·期 8 ·1-14 · IF 1.9

Preparation of TiO2/Sponge Composite for Photocatalytic Degradation of 2,4,6-Trichlorophenol

Zhao Tianyu,Cheng Hao,Liang Yinna,Xiong Jianhua,Zhu Hongxiang,Wang Shuangfei,Liang Jiaxiang,Chen Guoning

Photocatalysis has emerged as a promising approach for treating environmental pollution. In this study, TiO 2 /sponge composites with good photocatalytic activity in visible light were prepared via a simple and efficient low-temperature process and applied to the degradation of 2,4,6-trichlorophenol (2,4,6-TCP) present in papermaking wastewater. The process conditions for preparing TiO 2 /sponge composites were optimized by varying the TiO 2 dosage, cellulose dosage, and surfactant concentration. Scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) results showed that TiO 2 successfully adhered to the sponge surface and that the composites achieved a good recycling effect. Degradation occurred under visible light, and a degradation rate of 81% for 2,4,6-TCP with initial concentration of 20 mg/L was achieved in 4 h. The fragments were analyzed using ultra-performance liquid chromatography tandem mass spectrometry (UPLC-MS), which revealed the formation of 2-hydroxyvaleric acid (2-HVA) as a degradation product; a possible degradation mechanism is proposed to interpret these findings. Visible-light photocatalysis shows high potential for the rapid and environmentally friendly destruction of organic pollutants in papermaking wastewater.

CAS / MDL: 9004-65-3 81-88-9
研究领域: 环境科学 · 材料科学
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Construction of biochar-based organohalide-respiring bacterial agent for remediation of 2,4,6-trichlorophenol contaminated soil

Xueqi Chen,Jiatian Hu,Di Cao,Wenxin Yang,Zimeng Zhang,Yunxia Zu,Fan Chen,Li Zhiling,Wang Aijie

Construction of an efficient bio-reductive dechlorination system remains challenging due to the narrow ecological niche and low-growth rate of organohalide-respiring bacteria during field remediation. In this study, a biochar-based organohalide-respiring bacterial agent was obtained, and its performance and effects on indigenous microbial composition, diversity, and inter-relationship in soil were investigated. A well-performing material, Triton X-100 modified biochar (BC 600-TX100 ), was found to have the superior average pore size, specific surface area and hydrophicity, compared to other materials. Interestingly, Pseudomonas aeruginosa CP-1, which is capable of 2,4,6-TCP dechlorination , showed a 348 times higher colonization cell number on BC 600-TX100 than that of BC600 after 7 d. Meanwhile, the dechlorination rate in soil showed the highest (0.732 d −1 ) in the BC 600-TX100 bacterial agent than in the other agents. The long-term performance of the BC 600-TX100 OHRB agent was also verified, with a stable dechlorination activity over six cycles. Soil microbial community analysis found the addition of the BC 600-TX100 OHRB agent significantly increased the relative abundance of genus Pseudomonas from 1.53 % to 11.2 %, and Pseudomonas formed a close interaction relationship with indigenous microorganisms , creating a micro-ecological environment conducive to reductive dechlorination. This study provides a feasible bacterial agent for the in-situ bioremediation of soil contaminated organohalides. Environmental Implication Halogenated organic compounds are a type of toxic, refractory, and bio-accumulative persistent compounds widely existed in environment, widely detected in the air, water, and soil. In this study, we provide a feasible bacterial agent for the in-situ bioremediation of soil contaminated halogenated organic compounds. The application of biochar provides new insights for “Turning waste into treasure”, which meets with the concept of green chemistry.

研究领域: 环境科学 · 微生物学
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RSC Advances · 2014 ·Vol. 4 ·期 108 ·63494-63501 · IF 3.708

Surface core–shell magnetic polymer modified graphene oxide-based material for 2,4,6-trichlorophenol removal

Mei-Lan Chen,Jian-Qing Min,Sheng-Dong Pan,Mi-Cong Jin

A novel well-designed graphene oxide-based magnetic polymer (GO-Fe3O4@P) has been successfully synthesized via distillation–precipitation polymerization, ring-opening and amidation reactions. The as-prepared GO-Fe3O4@P was further characterized by transmission electron microscopy (TEM), vibrating sample magnetometer (VSM), BET analysis, zeta potential analysis, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR) and the characterization results revealed that core–shell structural Fe3O4@P microspheres were covalently bonded onto the GO sheet. The adsorption characteristics of the GO-Fe3O4@P intended for removal of 2,4,6-trichlorophenol (2,4,6-TCP) were investigated. Batch adsorption studies were carried out to optimize adsorption conditions. The effect of solution pH, adsorption isotherm, kinetics, and thermodynamics was deeply investigated. The results indicated that the adsorption property of GO-Fe3O4@P was highly pH dependent and the adsorption mechanism referred to hydrogen bond and π–π stacking interactions. The adsorption data for 2,4,6-TCP onto GO-Fe3O4@P was well fitted to a Langmuir isotherm. The maximum adsorption capacity (qm) of GO-Fe3O4@P to 2,4,6-TCP was found to be 232.6 mg g−1. Kinetic results showed that the adsorption reached equilibrium within 4 min, 10 min, and 60 min for initial 2,4,6-TCP concentrations of 10 mg L−1, 100 mg L−1, and 500 mg L−1, respectively. The data of adsorption kinetics obeyed the pseudo-second-order rate model well. Thermodynamic parameters such as ΔHθ, ΔSθ, and ΔGθ for the 2,4,6-TCP adsorption onto GO-Fe3O4@P have been estimated, suggesting the adsorption process was endothermic and entropy favored in nature.

研究领域: 环境科学 · 材料科学
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Environmental Technology & Innovation · 2022 · IF 7.758

Enhanced 2,4,6-trichlorophenol removal from soil by electrokinetic remediation coupled with biochar in a permeable reactive barrier

Qiang Liu,Yuyu Jiang,Yangyang Liu,Xiaolei Zhang,Yunfeng Xu,Huihui Chen,Weimin Cao

Coconut shell biochars prepared from the oxygen free pyrolysis under 300–700 °C were incorporated in the permeable reactive barrier (PRB) for electrokinetic remediation (EK) to remove 2,4,6-trichlorophenol (2,4,6-TCP) from soil. The result indicated the removal of 2,4,6-TCP from the soil under EK was increased by about 2 folds using biochar in PRB than those without biochar PRB. The orthogonal test suggested that the voltage input rather than the pyrolysis temperature of biochar was the major factor governing the removal of TCP during the EK-PRB process. The optimum TCP removal reached over 55% under 2 V cm −1 of voltage, 700 °C pyrolysis temperature and 40 mg L −1 of initial TCP concentration. The roles of biochar during EK remediation were identified as three aspects: accelerating the migration of TCP in soil by enlarging the electroosmotic flow (EOF), enhancing the direct removal of TCP by adsorption, and promoting the electrochemical degradation of TCP. The biochar from high pyrolysis temperature was preferred to be coupled with EK for the removal of organic contaminants owing to its great ability of enhancing EOF as well as pollutant adsorption.

CAS / MDL: 88-06-2
研究领域: 环境科学 · 土壤修复
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Electronic structure modulation on PdCo bimetal for enhanced atomic hydrogen mediated electro-dehalogention of 2,4,6-trichlorophenol

Chuyan Deng,Yujun Zhou,Xin Cai,Jiamin Gao,Junwen Qi,Zhigao Zhu,Yue Yang,Jiansheng Li

Atomic hydrogen (H*)-mediated indirect electrochemical reduction has regarded as a highly effective strategy for halogenated organic pollutants (HOPs) removal in wastewater. The efficient generation and prompt utilization of H* are critical factors which directly determine the degradation performance. This study presented a new strategy for the electro-reduction of a typical HOP—2,4,6-trichlorophenol (2,4,6-TCP), achieved by modulating the electronic structure of a PdCo bimetal electrode (Pd 1 Co 1 /CP). Through characterizations and density functional theory (DFT) analysis, ZIF-67 as the Co source could effectively improve the uniform distribution of Pd and Co, which exposed more active sites for H* on-demand generation. Meanwhile, the introduction of Co atoms and the optimum of Pd/Co ratios modulated the electronic structure of Pd sites. In 120 min, 92 % 2,4,6-TCP (initial concentration 10 mg/L) was degradated with a reaction rate constant (k obs ) of 0.103 min −1 , which was 2.1 times higher than that of Pd/CP electrode. Lower Gibbs free energy for hydrogen adsorption (−0.477 eV) was found in Pd 1 Co 1 /CP which benefited the surface-adsorbed H* stability for enhanced utilization. The degradation pathway of 2,4,6-TCP was further studied. These findings highlight the critical role of modulating the electronic structure of the electrode to optimize the utilization of surface-adsorbed active intermediates, presenting a novel and promising approach for advancing wastewater treatment technologies.

研究领域: 环境科学 · 材料科学 · 理论化学
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BIOINORGANIC CHEMISTRY AND APPLICATIONS · 2015 · IF 2.081

Application of Novel Amino-Functionalized NZVI@SiO2 Nanoparticles to Enhance Anaerobic Granular Sludge Removal of 2,4,6-Trichlorophenol

Zeyu Guan,Jinquan Wan,Yongwen Ma,Yan Wang,Yajie Shu

A novel amino-functionalized silica-coated nanoscale zerovalent iron (NZVI@SiO2-NH2) was successfully synthesized by using one-step liquid-phase method with the surface functionalization of nanoscale zerovalent iron (NZVI) to enhance degradation of chlorinated organic contaminants from anaerobic microbial system. NZVI@SiO2-NH2 nanoparticles were synthesized under optimal conditions with the uniform core-shell structure (80–100 nm), high loading of amino functionality (~0.9 wt%), and relatively large specific surface area (126.3 m2/g). The result demonstrated that well-dispersed NZVI@SiO2-NH2 nanoparticle with nFe0-core and amino-functional silicon shell can effectively remove 2,4,6-trichlorophenol (2,4,6-TCP) in the neutral condition, much higher than that of NZVI. Besides, the surface-modified nanoparticles (NZVI@SiO2-NH2) in anaerobic granule sludge system also showed a positive effect to promote anaerobic biodechlorination system. More than 94.6% of 2,4,6-TCP was removed from the combined NZVI@SiO2-NH2-anaerobic granular sludge system during the anaerobic dechlorination processes. Moreover, adding the appropriate concentration of NZVI@SiO2-NH2 in anaerobic granular sludge treatment system can decrease the toxicity of 2,4,6-TCP to anaerobic microorganisms and improved the cumulative amount of methane production and electron transport system activity. The results from this study clearly demonstrated that the NZVI@SiO2-NH2/anaerobic granular sludge system could become an effective and promising technology for the removal of chlorophenols in industrial wastewater.

研究领域: 环境科学 · 微生物学
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Desalination and Water Treatment · 2015 · IF 1.173

Synthesis of poly (styrene-divinyl benzene) magnetic porous adsorbents prepared by sulfonation for the adsorption of 2,4-dichlorophenol and 2,4,6-trichlorophenol from aqueous solutions

Ping Yu,Qilong Sun,Jianfeng Li,Jianming Pan,Zhenjiang Tan,Yongsheng Yan

Poly(styrene-divinyl benzene) (St-DVB) magnetic porous microspheres were prepared by sulfonation for the adsorption of 2,4-dichlorophenol(2,4-DCP) and 2,4,6-trichlorophenol (2,4,6-TCP) from aqueous solution. The as-prepared microspheres were characterized by FT-IR, XRD, SEM, TGA, VSM, and N2 adsorption–desorption techniques, showing that the as-prepared microspheres were porous and had good magnetism (Ms = 40 emu g−1). The adsorption performance of St-DVB magnetic porous microspheres were investigated by batch mode adsorption experiments with respect to pH, temperature, initial concentration, and contact time. The St-DVB magnetic porous microspheres were sensitive to pH. The equilibrium data was better fitted to the Langmuir isotherm model than the Freundlich model. The kinetics experimental data was well fitted to the pseudo-second-order model. The thermodynamic parameters were calculated by the Gibbs free energy function, revealing that the adsorption process was spontaneous and endothermic. Furthermore, the St-DVB magnetic porous microspheres had good recycling performance.

研究领域: 环境科学 · 材料科学
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ANALYTICAL LETTERS · 2018 · IF 1.206

Sensitive and Selective Determination of 2,4,6-Trichlorophenol Using a Molecularly Imprinted Polymer Based on Zinc Oxide Quantum Dots

Xinyu Lin,Yilin Wu,Yue Hao,Qian Sun,Yongsheng Yan,Chunxiang Li

Novel core-shell molecularly imprinted polymers were prepared based on zinc oxide quantum dots for the determination of 2,4,6-trichlorophenol by fluorescence. Principally, ZnO quantum dots and 2,4,6-trichlorophenol were chosen as the core substrate and the template molecule, respectively. The specific recognition sites for 2,4,6-trichlorophenol were obtained during the polymerization process in presence of 3-aminopropyltriethoxysilane and tetraethylorthosilicate. Molecularly imprinted ZnO quantum dots were characterized by transmission electron microscopy and Fourier transform infrared spectroscopy and the optical properties were evaluated by spectrofluorometry. Under the optimal conditions, molecularly imprinted ZnO quantum dots were successfully applied to the sensitive determination and selective recognition of 2,4,6-trichlorophenol in water. A linear relationship was obtained to cover the concentration range of 0–160 µmol L−1 with a correlation coefficient of 0.9931 calculated by the Stern–Volmer equation. The products were used for the determination of 2,4,6-trichlorophenol in the water from local rural areas and the results strongly supported that the molecularly imprinted ZnO quantum dots were suitable for the determination of 2,4,6-trichlorophenol in real examples.

研究领域: 分析化学 · 环境科学
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