CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Min Tang,Wu Liu,Zhiyong Wang,Zhaoduan Hu,Jinquan Wan,Rui Peng
Advanced oxidation processes (AOPs) are highly effective for removing emerging contaminants from water. However, their efficiency is often limited by sluggish catalytic oxidation, excessive input of chemicals and energy for organic mineralization, and undesirable carbon emission. Current improvements mainly focus on enhancing catalyst activation, often neglecting the elimination step of contaminants. This study presents a confined energy-drive strategy to shift the removal pathway of 2,4,6-trichlorophenol (TCP) from degradation mineralization to oxidative coupling polymerization. Nanosphere catalysts (Fe-NC-x, where x = 1, 2, 3, 4) with varying channel diameters were developed by loading iron into nanochannels of different sizes. The confined Fe-NC-1 catalytic system achieved a remarkable 99 % TCP removal within 40 min, in contrast to the 69 % removal observed with the non-confined Fe-NC-0 catalytic system. As the channel confinement decreased, the TCP removal efficiency increased. This enhanced performance is attributed to the in-situ confined energy generated by Fe-NC-1 nanochannels (< 5 nm), which promotes peroxydisulfate pre-adsorption and accelerates electron transfer between peroxydisulfate and the catalyst. Furthermore, the confined energy stabilizes the oxidation transition state of TCP, favoring the low-energy barrier coupling polymerization pathway. This study provides a green and sustainable strategy for AOPs through confined energy-driven, low-carbon methods for water purification and organic carbon recovery.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Jie Yang,Yulin Zhang,Yinan Bu,Baiyang Chen,Juan Li
According to an earlier study, electrodialysis (ED) can efficiently separate most organic halogenated micropollutants from inorganic halogens (i.e., halides and oxyhalides) in water, with only a few micropollutants being poorly-recovered. To optimize the ED process and to gain in-depth knowledge of the mechanisms responsible for their low recoveries, this study designed some experiments to examine the fates and transports of three hard-to-separate organic halogen compounds. Results show that the dominant mechanism responsible for the loss of trichlorophenol (TCP) is migration and retention in the ion exchange membrane (IEM), the dominant mechanism for the loss of trichloroacetic acid (TCAA) is ion exchange with the IEM, and the dominant mechanism for the loss of trichloroacetonitrile (TCAN) is volatilization and chemical decomposition during the ED process. Optimizing specific operating conditions (e.g., sealing, voltage, and membrane type, etc.) can improve recovery of these micropollutants to 70.4–95.8% while maintaining 90.4–99.5% removal of chloride. Even though TCAN underwent hydrolysis, we recovered 82.0% chlorine from TCAN and its hydrolytic products. These results may help not only better understand the fates and transports of organic micropollutants during the ED process, but also help facilitate application of electrodialysis technique for measuring total organic halogen.
研究领域:
环境科学
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水处理技术
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DOI
高影响因子
ACS Omega
·
2020
·
IF 2.87
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.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
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
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Tianming Chen,Chao Zou,Fan Chen,Ye Yuan,Jingjing Pan,Qi Zhao,Mansi Wang,Liang Qiao,Haoyi Cheng,Cheng Ding,Aijie Wang
Biocathode systems could be used for in-situ bioremediation of chlorophenols (CPs) in constructed wetland (CW) sediments. However, little is known regarding whether or how cathode burial depths affect the dechlorination of CPs in sediments. Here, 2,4,6-trichlorophenol (2,4,6-TCP)-dechlorinating biocathode systems were constructed under a cathode potential of − 0.7 V (vs. a saturated calomel electrode, SCE) at three different cathode burial depths (5, 10, and 15 cm). The 2,4,6-TCP removal efficiency and average transformation rate with the biocathode increased by 21.46–36.86% and 14.63–34.88% compared to those in the non-electrode groups. Deeper cathode burial depths enhanced the 2,4,6-TCP dechlorination performance. Furthermore, the oxidation-reduction potential (ORP) of the sediment decreased with sediment depth and the applied potential created a more favorable redox environment for the enrichment of functional bacteria. Deeper cathode burial depths also promoted the selective enrichment of electro-active and dechlorinating bacteria (e.g., Bacillus and Dehalobacter , respectively). The biocathode thus served as the carrier, electron source , and regulator of functional bacteria to accelerate the transformation of 2,4,6-TCP (2,4,6-TCP → 2,4-dichlorophenol → 4-chlorophenol → phenol) in sediments. These results offer insights into the effects of cathode burial depth on 2,4,6-TCP dechlorination in sediments from a redox environment and microbial community structure standpoint.
研究领域:
环境科学
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微生物学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 48
·72764-72776
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IF 5.19
Zhong Dan,Feng Weinan,Ma Wencheng,Liu Xinyue,Ma Jun,Zhou Ziyi,Du Xuan,He Fu
Goethite and lepidocrocite, as the main compositions of pipe deposits in the water distribution network, could be used as a catalyst for advanced oxidation processes (AOPs). This research utilizes them to activate PDS/H 2 O 2 and PMS/H 2 O 2 degrading the 2,4,6-trichlorophenol, respectively. To describe the incomplete degradation of pollutants and reflect the induction period, a modified first-order model has been proposed and used to analyze degradation differences under several key affecting factors. The results revealed that the PDS/H 2 O 2 system has a synergy effect in the 2,4,6-trichlorophenol degradation process. The possible degradation pathways and intermediate products were confirmed by gas chromatograph-mass spectrometry (GC–MS). The paper provides a new idea for the effective use of pipe deposits to remove chlorophenols from drinking water, which is of great significance to ensure water quality safety.
研究领域:
环境科学
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水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuedan Cui,Daibing Hou,Yiming Tang,Hantong Qie,Ruiqing Xu,Pengjie Zhao,Aijun Lin,Meng Liu
The current Sulfate Radical Advanced Oxidation Process (SR-AOP) system faces several limitations, such as expensive catalysts, susceptibility to secondary pollutants, limited cycle stability, and suboptimal electron consumption efficiency. Therefore, developing a cost-effective, recyclable, and eco-friendly catalyst holds great promise for improving catalyst performance and electron utilisation efficiency. In this investigation, the effectiveness of natural magnetite treated through ball milling (NMP B ) in activating peroxydisulfate (PDS) to generate sulfate radicals (SO 4 − ) were explored and the combination of NMP B and PDS demonstrated outstanding catalytic efficiency in degrading 2,4,6-trichlorophenol (TCP), achieving a degradation efficiency exceeding 90 % within 6 h. The naturally occurring Fe(II) and graphitised carbon structure within NMP B were crucial in facilitating PDS activation and promoting efficient electron transfer. Subsequently, potential degradation mechanisms for TCP in the NMP B /PDS system was proposed, and the activation mechanism of graphite-carbon enhanced PDS was identified by DFT calculation. Additionally, excellent stability and reusability of NMP B was demonstrated through iron leaching experiment and circulation experiment. Furthermore, TCP degradation intermediates were identified through liquid chromatography combined with mass spectroscopy (LC-MS) and potential TCP degradation pathways were proposed. Importantly, toxicity assessment revealed that the intermediates generated during the TCP degradation process exhibited lower toxicity than TCP. In summary, the NMP B /PDS system demonstrated its effectiveness as an environmentally friendly technology for degrading organic pollutants in contaminated groundwater and surface water environments.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Jinmei Xu,Senqi Xu,Shangqing Tang,Luyao Wang,Kui Wan,Chuqiao Wang
The widespread use and release of 2,4,6-Trichlorophenol (TCP) poses a significant risk to water bodies and ecosystems. Designing efficient and stable catalysts for photocatalytic degradation of TCP remains a great challenge. In this paper, a Z-scheme α-MnO 2 /Bi 2 S 3 (Mn/Bi) composite enriched with oxygen (O Vs ) and sulfur (S Vs ) vacancies is designed for photocatalytic degradation of TCP. 60-Mn/Bi achieved 88 % degradation efficiency for 20 mg/L TCP solution. The reaction rate ( k ) of 60-Mn/Bi is 6.46 and 4.41 times higher than that of α-MnO 2 and Bi 2 S 3 , respectively. The catalyst exhibited high catalytic activity in a wide pH range and high resistance to anion. In addition, the cycling performance of 60-Mn/Bi is relatively stable, and the ion leaching rate is low. The Z-scheme mechanism is confirmed by characterization and DFT, which effectively retained the strong redox capacity. The abundant vacancy structure enhances the adsorption of TCP and promotes the migration of photogenerated carriers. In addition, the rod-shaped Bi 2 S 3 provides a carrier for α-MnO 2 nanoparticles, which effectively alleviates agglomeration and thus exposes more active sites. Three possible degradation pathways were explored by LC-MS and DFT. This study provides a facile method and guidance for the preparation of Z-scheme catalysts to improve photocatalytic degradation performance.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Bingzhi Liu,Tingyu Pan,Jiajun Liu,Li Feng,Yuning Chen,Huaili Zheng
Chlorophenol is a widely used organic compound, and the environmental and health problems caused by it have being worsened in recent years. This study used 2,4,6-trichlorophenol (2,4,6-TCP) as the target pollutant, and employed ultrasound (US) enhanced zero-valent iron (Fe 0 )/EDTA/air system (FEA), namely US/FEA, to remove 2,4,6-TCP. The influence of single factor experimental conditions such as EDTA concentration, Fe 0 dosage, US power, pH and pollutant concentration on the removal efficiency of 2,4,6-TCP was investigated, and the optimal reaction conditions were determined. The mechanism of reactive oxygen species (ROS) produced by US/FEA was explored. The degradation process and removal mechanism of 2,4,6-TCP in the US/FEA were discussed through the determination and analysis of intermediate products. The results showed that US could continuously activate and renew the Fe 0 surface, accelerate its oxidation and corrosion process, and then continuously and stably produce sufficient amounts of Fe 2+ and Fe 3+ . Ultrasonic cavitation effect could reduce the difficulty of O 2 activation reaction, and promote the production of sufficient H 2 O 2 . The addition of EDTA made the system have a wide range of pH applications, and its performance under neutral and alkaline conditions was also superior. The ROS of US/FEA included ·OH, O 2 ·- and Fe(IV), where Fe(IV) was the main contributor to the removal of 2,4,6-TCP. In addition, the degradation of 2,4,6-TCP had two processes including dechlorination and benzene ring opening. First, 2,4,6-TCP was dechlorinated and degraded into phenol. And then, phenol was degraded into small molecular acids by ring-opening, and finally it was mineralized into CO 2 and H 2 O completely. US/FEA is a promising technology for high-efficiency degradation of organic matter and deep environmental purification.
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
CHEMOSPHERE
·
2023
·
IF 8.8
Ying Wang,Wei Jiang,Yanqiang Tang,Zheming Liu,Qingdong Qin,Yan Xu
Nanoscale zero–valent iron (NZVI) has been widely used in rapid remediation of contaminants. However, several obstacles such as aggregation and surface passivation hampered NZVI from further application. In this study, sulfurized nanoscale–zero valent iron supported by biochar (BC–SNZVI) was successfully synthesized and utilized for highly efficient 2,4,6–trichlorophenol (2,4,6–TCP) dechlorination in aqueous solution. SEM-EDS analysis revealed the even distribution of SNZVI on the surface of BC. FTIR, XRD, XPS and N 2 Brunauer–Emmett–Teller (BET) adsorption analyses were carried out to characterize the materials. Results showed that BC–SNZVI with S/Fe molar ratio of 0.088, Na 2 S 2 O 3 as sulfurization agent, and pre–sulfurization as the sulfurization strategy exhibited the superior performance for 2,4,6–TCP removal. The overall removal of 2,4,6–TCP was well described with the pseudo–first–order kinetics (R 2 > 0.9), and the observed kinetics constant K obs was 0.083 min −1 with BC–SNZVI, which was one order of magnitude higher than that of BC–NZVI (0.0092 min −1 ) and SNZVI (0.0042 min −1 ), and two orders of magnitude higher than that of NZVI (0.00092 min −1 ). Moreover, the removal efficiency of 2,4,6–TCP reached 99.5% by BC–SNZVI with dosage of 0.5 g L −1 , initial 2,4,6–TCP concentration of 30 mg L −1 and initial solution pH of 3.0 within 180 min. The removal of 2,4,6–TCP by BC–SNZVI was acid–promoted and the removal efficiencies of 2,4,6–TCP decreased with the increase of initial 2,4,6–TCP concentrations. Furthermore, more extensive dechlorination of 2,4,6–TCP was achieved with BC–SNZVI and complete dechlorination product phenol became predominant. The facilitation of sulfur for Fe 0 utilization and electron distribution in the presence of biochar remarkably enhanced the dechlorination performance of BC–SNZVI for 2,4,6–TCP. These findings provide insights into BC–SNZVI as an alternative engineering carbon based NZVI material for treating chlorinated phenols.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Ying Wang,Yanqiang Tang,Wei Jiang,Qingdong Qin,Rongsheng Lu,Yan Xu
Sulfurized nanoscale zero-valent iron supported on biochar (BC-SNZVI) has been successfully synthesized for 2,4,6-trichlorophenol (2,4,6-TCP) removal, while was only effectively under acidic conditions. To obtain highly efficient removal of 2,4,6-TCP within a broader pH range, weak static magnetic fields (WMF) was applied in BC-SNZVI/2,4,6-TCP aqueous systems. Results showed 30 mT WMF supported the most extensive 2,4,6-TCP removal, and 87.4% of 2,4,6-TCP (initial concentration of 30 mg/L) was removed by 0.5 g/L BC-SNZVI at neutral pH (pH = 6.8) within 180 min, which was increased by 54.4% compared to that without WMF. The observed rate constant ( K obs ) under 30 mT WMF was 2.1-fold greater than that without WMF. Although three typical anions (NO 3 − (0.5–10.0 mM), H 2 PO 4 − (0.05–0.5 mM), and HCO 3 − (0.5–5.0 mM)) still inhibited 2,4,6-TCP removal, WMF could efficiently alleviate the inhibitory effects. Moreover, 73.1% of 2,4,6-TCP was successfully removed by BC-SNZVI under WMF in natural water. WMF remarkably boosted the dechlorination of 2,4,6-TCP, increasing the 2,4,6-TCP dechlorination efficiency from 45.2% (in the absence of WMF) to 83.8% (in the presence of WMF) by the end of 300 min. And the complete dechlorination product phenol appeared within 10 min. Force analysis confirmed the magnetic field gradient force ( F B ) moved paramagnetic Fe 2+ at the SNZVI surface along the direction perpendicular to the external applied field, promoting the mass-transfer controlled SNZVI corrosion. Corrosion resistance analysis revealed WMF promoted the electron-transfer controlled SNZVI corrosion by decreasing its self-corrosion potential ( E corr ). With the introduction of sulfur, the magnitude of F B doubled and the E corr decreased comparing with NZVI. Our findings provide a facile and viable strategy for treating chlorinated phenols at neutral pH.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
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
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）