JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Xiupei Yang,Maosen Zhang,Jing Yang,Feng Huo,Yingying Li,Lianfang Chen
Bisphenol compounds exist widely in the environment and pose potential hazards to the environment and human health, which has aroused widespread concern. Therefore, there is an urgent need for an efficient and sensitive analytical method to enrich and determine trace bisphenols in environmental samples. In this work, magnetic porous carbon (MPC) was synthesized by one-step pyrolysis combined with a solvothermal method for magnetic solid-phase extraction of bisphenols. The structural properties of MPC were characterized by field emission scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, and saturation magnetization analysis. Its adsorption properties were evaluated by adsorption kinetics and adsorption isotherm studies. By optimizing the magnetic solid-phase extraction and capillary electrophoresis separation conditions, a capillary electrophoresis separation and detection method for four bisphenols was successfully constructed. The results showed that the detection limits of the proposed method for the four bisphenols were 0.71–1.65 ng/mL, the intra-day and inter-day precisions were 2.27–4.03% and 2.93–4.42%, respectively, and the recoveries were 87.68%-108.0%. In addition, the MPC could be easily recycled and utilized, and even if the magnetic solid-phase extraction was repeated 5 times, the extraction efficiency could still be kept above 75%.
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npj Clean Water
·
2023
·Vol. 6
·期 1
·1-10
·
IF 11.4
Li Meng,Song Jiayu,Han Wei,Yeung King Lun,Zhou Shaoqi,Mo Ce-Hui
Although Fenton-like reactions have been extensively used to treat various organic contaminants in wastewaters (oily wastewaters, landfill leachate, denitrification with Fenton oxidized non-degradable large molecular organic pollutants, and removal of phosphorus, etc.), the difficulty in catalyst recovery and the instability of catalytic activity limit their practical application. Herein, iron atoms were inserted in a metal-organic framework (FeNC) with dual reaction sites as highly reactive and stable electro-Fenton-like catalysts for the catalytic oxidation of organic pollutants via the electro-Fenton-like activation reaction of peroxymonosulfate (PMS) with fractional leaching of metal ions. Experiments and density functional theory (DFT) calculations indicate that FeNC with FeN 4 and Fe–Fe active sites can rapidly deliver electrons for PMS dissociation. Further, an electrolysis reactor was constructed for the on-site generation of reactive oxygen species, which can stably and continuously purify various organic wastewaters. The combined use of an electrolysis reactor and magnetic catalyst in the current study provides a direction for the long-term remediation of organic pollutants on an industrial scale.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Liangjie Wang,Chunxiang Geng,Dawei Yu,Daoqing Liu,Hao Sun,Ke Xiao,Huazhang Zhao
High temperatures and high pressures restrict the application of catalytic wet air oxidation (CWAO). Thus, realizing the high performance of CWAO under ambient pressure (AP-CWAO) is attractive. In this study, hydrophobic modification by polytetrafluoroethylene (PTFE) was adopted to enhance the O 2 transfer and salts resistibility of hollow microspheres NiCo 2 O 4 (HM-NiCo 2 O 4 ), for harvesting an efficient catalyst of AP-CWAO to treat high-salt wastewater. Under ambient pressure in 10 g/L NaCl solution, PTFE modified HM-NiCo 2 O 4 (PHM-NiCo 2 O 4 ) can catalyze O 2 to realize about 70 % mineralization of bisphenol A (BPA, 100 mg/L) within 240 min at 80 ℃, while it is only about 50 % for HM-NiCo 2 O 4 . Density functional theory calculations and molecular dynamics simulations show that PTFE indeed can enhance O 2 transfer and salt resistibility of HM-NiCo 2 O 4 . HO•, O 2 •- , and 1 O 2 all contribute to the degradation of BPA in presence of O 2 . These reactive oxygen species generate based on Mars-van Krevelen mechanism.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Tongchen Zhang,Huan Wu,Matin Naghizadeh,Qian Zheng,Sheying Dong
Further improvement on the adsorption performance of microporous organic polymers (MOPs) by delicate design remains a challenge. Herein, a magnetic hydroxyl-functioned microporous organic polymer (Fe3O4/Hy-MOP) was prepared and characterized by a series of techniques, including transmission electron microscopy, vibration sample magnetometry, Fourier transform infrared spectrometry, thermal gravimetric analysis, and zeta potential analysis. As an adsorbent for ultrasound-assisted magnetic solid phase extraction of three personal care products (PCPs, triclosan, triclocarban, and 2-hydroxy-4-methoxybenzophenone), the obtained Fe3O4/Hy-MOP exhibited excellent performance in extracting three PCPs (89–95%) from water samples owing to its hydrophilicity, inherent microporous structure, and easy magnetic separation. Moreover, probing of adsorption behavior by triclosan upon Fe3O4/Hy-MOP surfaces demonstrated that the adsorption process followed the models of Freundlich isotherm, together with pseudo-second-order kinetics. The extraction and adsorption mechanism involved polar force, π–π interaction, and hydrophobic interaction between Fe3O4/Hy-MOP and PCPs. Particularly, the stability and magnetism of Fe3O4/Hy-MOP confer excellent cycling performance, allowing for five recycling iterations without a significant decrease in performance. Such results indicated that magnetic adsorbent Fe3O4/Hy-MOP has potential for application in the extraction and removal of PCPs from actual water samples.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Kaiyuan Luo,Yang Shi,Rongfu Huang,Xipeng Wei,Zelin Wu,Peng Zhou,Heng Zhang,Yin Wang,Zhaokun Xiong,Bo Lai
Periodate (PI) has recently been studied as an excellent oxidant in advanced oxidation processes , and its reported mechanism is mainly the formation of reactive oxygen species (ROS). This work presents an efficient approach using N-doped iron-based porous carbon (Fe@N-C) to activate periodate for the degradation of sulfisoxazole (SIZ). Characterization results indicated the catalyst has high catalytic activity , stable structure, and high electron transfer activity. In terms of degradation mechanism, it is pointed out that the non-radical pathway is the dominant mechanism. In order to prove this mechanism, we have carried out scavenging experiments, electron paramagnetic resonance (EPR) analysis, salt bridge experiments and electrochemical experiments, which demonstrate the occurrence of mediated electron transfer mechanism. Fe@N-C could mediate the electron transfer from organic contaminant molecules to PI, thus improving the efficiency of PI utilization, rather than simply inducing the activation of PI through Fe@N-C. The overall results of this study provided a new understanding into the application of Fe@N-C activated PI in wastewater treatment .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kexin Yin,Lijing Peng,DongDong Chen,Siyi Liu,Yujie Zhang,Baoyu Gao,Kaifang Fu,Yanan Shang,Xing Xu
Developing single-atom catalysts (SACs) with superior Fenton-like performance and low-cost via green synthesis strategy is an urgent problem. It was for the first time to prepare the iron single-atom catalyst (Fe-SAC) with highly atomically-dispersion from natural Fe-rich marine algae ( Enteromorpha ) with iron amount over 1.5 wt%. Iron screening test indicated that the activation performance of Enteromorpha -derived Fe-SACs catalyst was mainly based on Fe-N 4 -C sites, and the roles of radicals accompanying with Fe(IV) and 1 O 2 oxidation showed very small contributions. In contrast, the degradation of organic was dominated by the electron-transfer process (ETP), and the ETP mechanism was greatly enhanced by the iron centers in the Enteromorpha -derived Fe-SACs, which could help extract more electrons from the organics to the Fe-N 4 -C/PMS complex, thus facilitating the ETP in catalytic system. In addition, the commercial ceramic membrane (CM) coated with Enteromorpha -derived Fe-SACs catalyst showed superior catalytic activtiy with a stable water flux.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Huihui Gao,Xiaoyu Han,Rong Wang,Keke Zhu,Runping Han
Phenolic compounds are common industrial pollutants that seriously endangers water ecology and human health. Therefore, the development of efficient and recyclable adsorbents is of importance for wastewater treatment . In this research, HCNTs/Fe 3 O 4 composites were constructed using co-precipitation way by loading magnetic Fe 3 O 4 particles onto hydroxylated multi-walled carbon nanotubes (MWCNTs), showing excellent adsorption capacity for Bisphenol A (BPA) and p -chlorophenol ( p -CP), and excellent catalytic ability of activating potassium persulphate (KPS) for degradation of BPA and p -CP. The adsorption capacity and catalytic degradation potential were evaluated for the removal of BPA and p -CP from solutions. The results showed that the adsorption took only 1 h to reach equilibrium and HCNTs/Fe 3 O 4 had maximum adsorption capacities of 113 mg g −1 for BPA and 41.6 mg g −1 for p -CP at 303 K, respectively. The adsorption of BPA fitted well using the Langmuir, Temkin and Freundlich models while the adsorption of p -CP fitted well using the Freundlich and Temkin models. BPA adsorption on HCNTs/Fe 3 O 4 was dominated by π-π stacking and hydrogen bonding forces. The adsorption included both the mono-molecular layer adsorption on the adsorbent surface and the multi-molecular layer adsorption on the non-uniform surface. The adsorption of p -CP on HCNTs/Fe 3 O 4 was a multi-molecular layer adsorption on a dissimilar surface. The adsorption was controlled by forces such as π-π stacking, hydrogen bonding, partition effect and molecular sieve effect. Moreover, KPS was added to the adsorption system to initiate a heterogeneous Fenton-like catalytic degradation. Over a wide pH range (4–10), 90% of the aqueous BPA solution and 88% of the p -CP solution were degraded in 3 and 2 h, respectively. After three adsorption-regeneration or degradation cycles, the removal of BPA and p -CP remained up to 88% and 66%, indicating that HCNTs/Fe 3 O 4 composite is cost-effective, stable and highly efficient to remove BPA and p -CP from solution.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Lu Zhao,Liang Liu,Xiao-Feng Bai,Ai-Yong Zhang,Shu-Chuan Peng,Chi Zhang,Hai-Hong Niu,Heng Liang
Pollutants removal by Fenton-like catalysis is of considerable interest, and the solid catalyst play governing roles. Two-dimensional MoS 2 can activate peroxymonosulfate (PMS) for radical-mediated catalysis via metallic 1T phase and/or crystal defects (i.e., sulfur vacancy). Herein, we explored the significant synergism between defective sulfur vacancy and metallic 1T rather than semiconducting 2H phase for Fenton-like catalysis on MoS 2 . This synergism was substrate-dependent during MoS 2 preparation. A series of sulfur-defected 1T-MoS 2 were prepared by H 2 O 2 oxidation, drastic structural but no morphological changes were measured. The defect-tailored 1T-MoS 2 exhibited a superior Fenton-like reactivity toward PMS activation and pollutant degradation in various water matrices. A 10.0 mg·L -1 of aqueous phenol was completely degraded in one hour, and the corresponding pseudo-first order reaction constant increased more than 12 times after defect engineering. No synergistic effect was measured between sulfur vacancy and semiconducting 2H phase on defective 2H-MoS 2 . Radical-mediated reaction mechanism was identified by ESR, scavenger inhibiting, spectroscopic analysis and electrochemical measurements. Electron transfer was accelerated within metallic 1T phase to favor PMS activation and pollutant degradation on defective sulfur vacancies serving as surface reactive sites. Our findings provided fundamental insights into PMS activation on sulfur vacancy promoted by 1T-MoS 2 in Fenton-like catalysis for water purification.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Caijuan Zhong,Shengxiao Zhang,Shuangshuang Yang,Baiqing Yuan,Qiang Xu,Zengrun Xie,Chenyu Du
Mo and N co-doped iron biochar material (Fe/Mo x -NC) was prepared through one-pot calcination method with anhydrous iron chloride, ammonium molybdate, and cherry stone powder as precursors. The composite can effectively catalyze activation of peroxymonosulfate (PMS) for organic pollutants degradation, and the removal rate of 20 mg/L bisphenol A (BPA) reaches 99.08% in 30 min in the presence of 0.1 g/L Fe/Mo 0.1 -NC and 1 g/L PMS. Electrochemical analysis indicates that appropriate doped Mo and N can improve the electron transfer performance of the composite, which enhances the PMS activation property for BPA degradation. Quenching experiments and electron paramagnetic resonance analysis both demonstrated that the Fe/Mo 0.1 -NC/PMS system generated SO 4 •− , •OH and 1 O 2 , which involved in BPA degradation. Moreover, a galvanic oxidation process had shown that there existed nonradical pathway which relied on electron transfer. The degradation pathway is proposed by measuring the intermediate products with HPLC-HRMS/MS. Through the exploration of the reaction mechanism, low-valence molybdenum ions can promote the cycle of Fe 2+ /Fe 3+ , and the pyridine-N and graphitic-N contained in Fe/Mo 0.1 -NC can catalyze activation of PMS together with Fe 2+ . The designed membrane filtration device revealed the feasibility of the composite in dynamic process, which was great significant for actual operation of water treatment. Furthermore, the Fe/Mo 0.1 -NC/PMS system could effectively decompose organic pollutants in the effluent from sewage treatment plant, achieving 82.6% of total organic carbon removal rate. This study not only prepared a novel heteroatom doped Fe-biochar material for PMS activation to degrade organic pollutants, but also deepened the reaction mechanism and explored its applicability for advanced treatment of real wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 25
·67758-67770
·
IF 5.8
Wang Ke,Qin Xingzhen,Chai Kungang,Wei Zongwu,Deng Fan,Liao Bingyu,Wu Jinyu,Shen Fang,Zhang Zhi
Endocrine-disrupting compounds (EDCs) are increasingly polluting water, making it of practical value to develop novel desirable adsorbents for removing these pollutants from wastewater. Here, a simple cross-linking strategy combined with gentle chemical activation was demonstrated to prepare starch polyurethane-activated carbon (STPU-AC) for adsorbing BPA in water. The adsorbents were characterized by various techniques such as FTIR, XPS, Raman, BET, SEM, and zeta potential, and their adsorption properties were investigated comprehensively. Results show that STPU-AC possesses a large surface area (1862.55 m 2 ·g −1 ) and an abundance of functional groups, which exhibited superior adsorption capacity for BPA (543.4 mg·g −1 ) and favorable regenerative abilities. The adsorption of BPA by STPU-AC follows a pseudo-second-order kinetic model and a Freundlich isotherm model. The effect of aqueous solution chemistry (pH and ionic strength) and the presence of other contaminants (phenol, heavy metals, and dyes) on BPA adsorption was also analyzed. Moreover, theoretical studies further demonstrate that hydroxyl oxygen and pyrrole nitrogen are the primary adsorption sites. We found that the efficient recovery of BPA was associated with pore filling, hydrogen-bonding interaction, hydrophobic effects, and π-π stacking. These findings demonstrate the promising practical application of STPU-AC and provide a basis for the rational design of starch-derived porous carbon.
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Biochar
·
2023
·Vol. 5
·期 1
·1-18
·
IF 12.7
Wang Shulian,Huang Yan,Ma Shuanglong,Zhan Sihui,Wang Jingzhen,Gao Boqiang,Tang Xiaodan,Zhu Qiuhui,Xu Shengjun,Zhuang Xuliang
Metal-free porous biochars are popularly utilized as catalysts for peroxydisulfate (PDS) activation. The enhancement effect of PDS activation of porous biochars fabricated by employing both hard template and alkali metal activating agent has not been explored completely. In addition, the role of the inherent carbon defect in PDS activation has not been clearly elucidated. Hence, a series of carbonaceous catalysts were fabricated using a sole template (KCl), a sole activating agent (Na 2 S 2 O 3 ) or a combination of template and activating agent (KCl/Na 2 S 2 O 3 , KCl/KHCO 3 , KCl/NaHCO 3 , and KCl/Na 2 C 2 O 4 ), to systematically investigate the effect of specific surface area (SSA) and intrinsic defect of porous biochar on its PDS activation ability. The biochar synthesized by KCl and Na 2 S 2 O 3 (SK-C) exhibited the optimum degradation performance. The SK-C was found to possess an interconnected hollow cage with three-dimensional mesh structure showing the largest surface area, pore volume and C- sp 3 edge defect content among all the catalysts, which explained its paramount catalytic ability. The SSA and C- sp 3 content together can determine the catalytic performance in a quantitative relationship. The single electron transfer pathway from SDZ to inner-sphere bound SK-C/PDS* was the protagonist of pollutant oxidation. The degradation intermediates were detected and recognized and their toxicities were evaluated. This study for the first time comprehensively identified the synergistic effect between the SSA and inherent defects on improving the catalytic performance of biochar for PDS activation to removal contaminants. Graphical Abstract
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Zhefei Hu,Yanhao Jiang,Panpan Cao,Yanjuan Liu,Yuefei Zhang,Wei Chen,Sheng Tang
In this work, 2-undecylimidazole (UI) and propyl methacrylate (PMA) dual-functionalized silica gel was prepared and applied as a mixed-mode chromatographic stationary phase. Successful preparation of this stationary phase (SiO 2 -UI-PMA) was proved through a range of characterization techniques. The chromatographic performance of the obtained SiO 2 -UI-PMA was investigated for the separation of environmental endocrine disruptors (phthalates, steroid hormones, bisphenols and alkylphenols), sulfonamides and food-borne stimulants in reversed-phase chromatography, as well as for the separation of inorganic anions in anion-exchange chromatography. The effect of column temperature, acetonitrile content, salt concentration and mobile phase pH on retention was studied to explore the separation mechanism, and the results indicated that this stationary phase provided multiple interactions with analytes. Compared with the commercial C18 column, the SiO 2 -UI-PMA demonstrated more preferable separation ability under the mobile phase conditions with a low content of acetonitrile, thereby acting as a good alternative candidate for the conventional reversed-phase stationary phase in chromatographic analysis. Furthermore, the SiO 2 -UI-PMA stationary phase exhibited high column efficiency (45 860 plates m −1 for progesterone) even though it was prepared from the non-serviceable silica based chromatographic packing materials.
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危险品化学品经营许可证（带存储）