作者机构:
[Li, Zhi; Zhu, Mingshan; Zhou, Daixi] Jinan Univ, Sch Environm, Guangdong Key Lab Environm Pollut & Hlth, Guangzhou 511443, Peoples R China.;[Hu, Xinjiang] Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410004, Peoples R China.;[Chen, Li] Chinese Peoples Liberat Army Gen Hosp, Med Ctr 1, Dept Gen Practice, Beijing 100853, Peoples R China.
通讯机构:
[Chen, L ] C;[Zhu, MS ] J;Jinan Univ, Sch Environm, Guangdong Key Lab Environm Pollut & Hlth, Guangzhou 511443, Peoples R China.;Chinese Peoples Liberat Army Gen Hosp, Med Ctr 1, Dept Gen Practice, Beijing 100853, Peoples R China.
关键词:
advanced oxidation process;persulfate;reactive oxygen species;single atom catalysts;substance
摘要:
In this review, SACs with different metal species and substrates are summarized to investigate the metal−support interaction effects on the persulfate oxidation reaction for water treatments. Abstract With maximum utilization of active metal sites, more and more researchers have reported using single atom catalysts (SACs) to activate persulfate (PS) for organic pollutants removal. In SACs, single metal atoms (Fe, Co, Cu, Mn, etc.) and different substrates (porous carbon, biochar, graphene oxide, carbon nitride, MOF, MoS2, and others) are the basic structural. Metal single atoms, substances, and connected chemical bonds all have a great influence on the electronic structures that directly affect the activation process of PS and degradation efficiency to organic pollutants. However, there are few relevant reviews about the interaction between metal single atoms and substances during PS activation process. In this review, the SACs with different metal species and substrates are summarized to investigate the metal−support interaction and evaluate their effects on PS oxidation reaction process. Furthermore, how metal atoms and substrates affect the reactive species and degradation pathways are also discussed. Finally, the challenges and prospects of SACs in PS‐AOPs are proposed.
摘要:
Metal-based materials are widely regarded as promising catalysts for activating peroxymonosulfate (PMS) to remove refractory organic contaminants with high efficiency. In our study, Ni-Fe layered double hydroxide (LDH)-biochar (BC) composite-induced PMS-based advanced oxidation process (AOP) was utilized to elucidate the degradation of tetracycline hydrochloride (TCH). In Ni-Fe LDH-BC/PMS system, more than 99% TCH (45 mu M) could be removed effectively at low doses of oxidant (PMS, 0.10 mM) and catalyst (Ni-Fe LDH-BC, 0.10 g/L) addition within 80 min. Besides, the Ni-Fe LDH-BC/PMS system showed high resistance to some inorganic anions, and the Ni-Fe LDH-BC composite possessed excellent reusability in the degradation of TCH (>99% in four cyclic experiments). The reaction mechanisms were investigated via electron paramagnetic resonance detection, chemical quenching tests, probe experiments, and electrochemical measurements. These results indicated that the electron-shuttle mechanism played the dominant role in the removal of TCH. It is worth noting that determination of PMS concentration can reflect the reliability of quenching experiments. In the Ni-Fe LDH-BC composite, BC could not only improve the dispersion of Ni-Fe LDH, but also increase the conductivity of Ni-Fe LDH. Overall, a successful modification strategy was proposed in our study to improve the catalytic property of Ni-Fe LDH, and reaction mechanisms of TCH degradation were discussed deeply and comprehensively.
摘要:
Developing efficient, stable, and user-friendly methods and technologies for predicting air quality has contributed to environmental research and management. Most traditional machine learning (ML) models often struggle to efficiently process extensive air quality data and grapple with the challenge of imbalanced data distributions. To this end, we introduced a novel multi-strategy collaborative approach that incorporates weighted feature selection, an adaptive enhanced rotation forest algorithm, and Bayesian Optimization for parameter tuning. Moreover, to improve the transparency in black box ML models, the novel Shapley Additive Explanations (SHAP) method was applied to interpret the outputs and analyze the importance of individual variables. Through experiments on real air quality datasets, we have verified the accuracy of our proposed method in classifying air quality levels. Notably, our model demonstrated an average test set accuracy improvement of approximately 10 % in cities like Beijing, Tianjin, Shijiazhuang, and Baoding after hyperparameter optimization using Bayesian methods. Furthermore, compared to alternative algorithms, our model showed an improvement of 1-2 % in evaluation metrics. By introducing novel methodologies and tools, our research contributes significantly to the advancement of air quality classification technology and holds profound implications for informing environmental policy decisions.
关键词:
MOFs;Arsenic;Peroxymonosulfate;Adsorption and catalysis;DFT
摘要:
The removal of arsenic from contaminated water is important for environmental protection and drinking water safety worldwide. In this study, bimetallic metal-organic frameworks (MOFs) with catalytic and adsorptive ef-fects were synthesized and combined with peroxymonosulfate (PMS) for efficient As(III) oxidation and As(III)/As (V) removal. The molar ratio of Fe and Mn precursor was adjusted to balance the adsorption and catalytic processes of As(III) in the system. The results showed that among the Fe/Mn-MOFs and MIL-88(Fe) tested, the Fe/Mn-MOFs with an Fe/Mn molar ratio of 1:1 (Fe0.3Mn0.3-MOFs) could achieve the best catalytic and adsorption performance with 98% removal of As(III). The performance of Fe0.3Mn0.3-MOFs in natural contam-inated water was also verified. Electron spin resonance detection and quenching experiments have revealed that trivalent arsenic oxidation is facilitated primarily by a non-radical process through singlet oxygen. Density-functional theory, XPS and FTIR analyses reveal the structures, corresponding binding energies and binding sites for the adsorption of As(III)/As(V) by Fe0.3Mn0.3-MOFs. The coupling of Fe0.3Mn0.3-MOFs to the PMS system was still able to achieve 78% arsenic removal after five cycles, showing good reliability and effectiveness in arsenic removal. This study provides a new insight into the catalytic and adsorption mechanisms in MOFs/PMS systems and provides a theoretical basis for the application of MOFs in the remediation of arsenic contaminated water.
摘要:
Frequent mining activities have led to an increasing transfer of heavy metals to the soil. Pyrite functionalized Black Soldier Fly feces biochar composite material (BFFS) was synthesized to immobilize Cu and Pb in contaminated mine soil and improve soil quality in our study. Incubation experiments showed that BFFS significantly reduced the leaching rates by 96 % and 90 % for Cu and Pb, respectively, when compared to the control after 220 days. Speciation transformation analysis further revealed that BFFS could significantly reduce easily labile fractions of Cu and Pb, and transformed to recalcitrant fractions. Moreover, BFFS significantly improved the quality of mine soil combined with soil quality index analysis. The potential toxicity and bioavailability of Cu and Pb can still be effectively reduced by BFFS, even during a 90-day field experiment. In addition, the mine soil improved by BFFS further promoted the survival and growth of ramie. Multiple characterization analyses and related experiments indicated that ion exchange, adsorption, complexation, and coprecipitation mainly contribute to the high efficiency immobilization of Cu and Pb by BFFS. These findings could bring some fresh perspectives on the development of immobilization materials and related technologies for the economical, green and sustainable remediation of heavy metals contaminated mine soil.
通讯机构:
[Xinjiang Hu] C;[Mingshan Zhu] G;College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha 410004, PR China<&wdkj&>Guangdong Key Laboratory of Environmental Pollution and Health, School of Environment, Jinan University, Guangzhou 511443, PR China
关键词:
17beta-estradiol;Al(2)O(3) nanoparticles;Graphene-like magnetic biochar;Mircoplastics;Potassium ferrate
摘要:
A graphene-like magnetic biochar (GLMB) was synthesized using lotus seedpod and potassium ferrate with simple step and applied for E2 adsorption. GLMB was characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM), atomic force microscope (AFM), X-ray photoelectron spectroscopy (XPS), Raman, X-ray diffraction (XRD), vibrating sample magnetometer (VSM) and BET surface area. Several common (solution pH, ionic strength, humic acid and foreign ions) and new (Al2O3 nanoparticles and microplastics (MPs)) water experiment conditions were investigated. Characterization results demonstrated that the sample was fabricated successfully and it possessed some graphene-like properties and a large surface area (828.37 m(2)/g). Adsorption results revealed that the pseudo-second-order kinetics and Langmuir isotherm models could provide a better description for E2 uptake behavior. The E2 adsorption capacity could be influenced by solution pH, ionic strength and SO42- ions, and the effect of humic acid and background electrolyte (Na+, K+, Ca2+, Mg2+, Cl-, NO3-, PO43-) could be neglected. The presences of Al2O3/MPs significantly decreased the time to reach adsorption equilibrium for E2 adsorption on GLMB, but had no obvious improvement or inhibiting effects on E2 removal when the adsorption reached equilibrium. The adsorption mechanism for E2 adsorption on GLMB was multiple, which involving n-n interactions, micropore filling effects, electrostatic interaction. The regeneration experiments showed that GLMB possessed a good regeneration performance. Based on the experimental results and comparative analysis with other adsorbents, GLMB was an economical, high-efficiency, green and recyclable adsorbent for E2 removal from aqueous solution. (C) 2020 Published by Elsevier B.
摘要:
A novel graphite-phase carbon nitride (g-C3N4)/bismuth ferrite (BiFeO3)/carbon nanotubes (CNTs) ternary magnetic composite (CNBT) was prepared by a hydrothermal synthesis. Using this material, Cr(VI) and methylene blue (MB) were removed from wastewater through synergistic adsorption and photocatalysis. The effects of pH, time, and pollutant concentration on the photocatalytic performance of CNBT, as well as possible interactions between Cr(VI) and MB species were analyzed. The obtained results showed that CNTs could effectively reduce the recombination rate of electron-hole pairs during the photocatalytic reaction of the g-C3N4/BiFeO3 composite, thereby improving its photocatalytic performance, while the presence of MB increased the reduction rate of Cr(VI). After 5 h of the simultaneous adsorption and photocatalysis by CNBT, the removal rates of Cr(VI) and MB were 93% and 98%, respectively. This study provides a new theoretical basis and technical guidance for the combined application of photocatalysis and adsorption in the treatment of wastewaters containing mixed pollutants.
通讯机构:
[Wang, Hui; Zhao, Yunlin] C;Cent South Univ Forestry & Technol, Coll Environm Sci & Engn, Changsha 410004, Hunan, Peoples R China.;Cent South Univ Forestry & Technol, Fac Life Sci & Technol, Changsha 410004, Hunan, Peoples R China.
关键词:
g-C3N4 nanosheets;BiFeO3;Cr(VI) photoreduction;Heterojunction;Electrolyte ion
摘要:
A novel ternary composite of graphitic carbon nitride (g-C3N4)/graphene oxide (GO) sheets/BiFeO3 (CNGB) with highly enhanced visible-light photocatalytic activity toward Cr(Vl) photoreduction is prepared and characterized. The characterization and photocatalysis experiments corroborate its reasonable band gap, efficient charge separation and transfer, widened visible-light adsorption, easy solid-liquid separation, good stability and superior catalytic activity of CNGB. Three CNGB samples with different ratios of g-C3N4 and BiFeO3 (CNGB-1, -2, -3 with 2:4, 3:3, and 4:2, respectively), though possessing different adsorption ability, eventually remove all Cr(Vl) ions via photocatalysis within 90 min. The catalytic efficiency of the composite is the highest at pH 2; increases in pH decrease the catalytic ability. The inorganic anions such as SO4-, Cl-, and NO3- only slightly affects the photocatalytic process. The matching of the band structure between BiFeO3 and g-C3N4 generates efficient photogenerated electron migration from the conduction band of g-C3N4 to that of BiFeO3, which is also facilitated by the electron bridging and collecting effects of GO, and holes transfer from the valence band of BiFeO3 to that of g-C3N4, yielding the efficient separation of photogenerated electron-hole pairs and the subsequent enhancement of photocatalytic activity. The research provides a theoretical basis and technical support for the development of photocatalytic technologies for effective application in wastewater treatment and Cr-contaminated water restoration. (C) 2018 Elsevier Ltd. All rights reserved.
期刊:
Journal of the Taiwan Institute of Chemical Engineers,2019年102:330-339 ISSN:1876-1070
通讯作者:
Li, Meifang;Liu, Yunguo
作者机构:
[Liu, Shaobo] Cent S Univ, Sch Architecture & Art, Lushan South Rd, Changsha 410083, Hunan, Peoples R China.;[Liu, Shaobo] Cent S Univ, Sch Met & Environm, Lushan South Rd, Changsha 410083, Hunan, Peoples R China.;[Yin, Zhihong; Liu, Yunguo; Tan, Xiaofei; Li, Meifang; Liu, Ni] Hunan Univ, Coll Environm Sci & Engn, Lushan South Rd, Changsha 410082, Hunan, Peoples R China.;[Yin, Zhihong; Liu, Yunguo; Tan, Xiaofei; Li, Meifang; Liu, Ni] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Lushan South Rd, Changsha 410082, Hunan, Peoples R China.;[Jiang, Luhua] Cent S Univ, Sch Minerals Proc & Bioengn, Lushan South Rd, Changsha 410083, Hunan, Peoples R China.
通讯机构:
[Li, MF; Liu, YG] H;Hunan Univ, Coll Environm Sci & Engn, Lushan South Rd, Changsha 410082, Hunan, Peoples R China.;Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Lushan South Rd, Changsha 410082, Hunan, Peoples R China.
关键词:
Bond strength (chemical);Carbonization;Chemical activation;Graphene;Graphene oxide;Hydrogen bonds;Ionic strength;Magnetite;Magnetite nanoparticles;Mechanisms;Nanomagnetics;Organic acids;Thermoanalysis;Water pollution;Adsorption capacities;Bio chars;Carbonization methods;Initial concentration;Oxygen-containing functional groups;Pseudo second order kinetics;Thermo dynamic analysis;Zeta potential measurements;Adsorption
摘要:
A novel graphene oxide supported activated magnetic biochar (GO-AMBC) is fabricated for 17 beta-estradiol (E2) removal from aqueous solution by grafting graphene oxide (GO) and magnetite nanoparticles onto the activated biochar surface with a one-step activation, magnetization, and carbonization method. GO-AMBC is characterized using SEM, TEM, FTIR, VSM, XRD, XPS, BET surface area and zeta potential measurements. The characterization results show that GO-AMBC possesses a larger surface area and more oxygen-containing functional groups than the unmodified biochar. When the E2 initial concentration is 6 mg/L, its adsorption capacity by GO-AMBC (46.22 mg/g) is more than two times higher than that of pristine biochar (23.09 mg/g) at 298 K and pH = 7.0. Adsorption results show that E2 uptake follows by pseudo-second-order kinetic and Freundlich isothermal models. Thermodynamic analysis indicates that the adsorption process is spontaneous and exothermic. E2 removal by GO-AMBC is significantly affected by the actual water conditions, including solution pH, ionic strength, and organic acids. Among them, organic acids have obvious inhibition effect on E2 removal, and the inhibition effect by oxalate is stronger than that of benzoate. The adsorption mechanism of E2 on GO-AMBC is mainly controlled by hydrogen bonds, electrostatic and pi-pi interactions. The experimental results of this study and comparative analysis with other adsorbents suggest that GO-AMBC is an economical, efficient and recyclable adsorbent and has great potential for E2 removal from contaminated water. (C) 2019 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.