PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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2022
·Vol. 119
·期 30
·e2202682119
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IF 12.779
Mingjie Huang,Yu-Sheng Li,Chuan-Qi Zhang,Chao Cui,Qing-Qing Huang,Mengkai Li,Zhimin Qiang,Tao Zhou,Xiaohui Wu,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS)–based advanced oxidation processes (AOPs) have shown a great potential for pollutant degradation, but their feasibility for large-scale water treatment application has not been demonstrated. Herein, we develop a facile coprecipitation method for the scalable production (∼10 kg) of the Cu-Fe-Mn spinel oxide (CuFeMnO). Such a catalyst has rich oxygen vacancies and symmetry-breaking sites, which endorse it with a superior PMS-catalytic capacity. We find that the working reactive species and their contributions are highly dependent on the properties of target organic pollutants. For the organics with electron-donating group (e.g., -OH), high-valent metal species are mainly responsible for the pollutant degradation, whereas for the organics with electron-withdrawing group (e.g., -COOH and -NO2), hydroxyl radical (•OH) as the secondary oxidant also plays an important role. We demonstrate that the CuFeMnO–PMS system is able to achieve efficient and stable removal of the pollutants in the secondary effluent from a municipal wastewater plant at both bench and pilot scales. Moreover, we explore the application prospect of this PMS-based AOP process for large-scale wastewater treatment. This work describes an opportunity to scalably prepare robust spinel oxide catalysts for water purification and is beneficial to the practical applications of the heterogeneous PMS-AOPs.
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JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 29
·期 5
·1411-1421
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IF 2.523
Wang Yiying,Pang Yuehong,Yang Yan,Shen Xiaofang
Bisphenol A (BPA), as a common endocrine disruptor, is widely present in water environment. It can migrate into food and gradually accumulate in organisms, posing potential health threats to humans. Herein, covalent organic frameworks (COFs) with different pore sizes (15.56 Å for TpPa-2, 21.95 Å for TpBD, and 30.29 Å for TFPB-BD) were synthesized by solvothermal reaction. The corresponding magnetic COFs (MCOFs) were conveniently prepared by co-precipitation method and were used for adsorption of BPA. The adsorption capacity of Fe 3 O 4 /TpPa-2, Fe 3 O 4 /TpBD, Fe 3 O 4 /TFPB-BD reached 44.85, 24.14 and 2.61 mg g −1 respectively, that is Fe 3 O 4 /TpPa-2>Fe 3 O 4 /TpBD>Fe 3 O 4 /TFPB-BD. The adsorption kinetic fitted the pseudo-second-order kinetic model and the adsorption isotherm fitted the Freundlich isothermal model. Both models demonstrated that the adsorption of BPA is based on heterogeneous surface. In addition, recycling experiments indicated that after five cycles of adsorption/desorption, the adsorption capacity can still reach 76.39% of the first use, indicating that recyclable Fe 3 O 4 /TpPa-2 is a potential adsorbent and can be further applied to the adsorption of environmental pollutants.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Ying-Jie Zhang,Jie-Jie Chen,Han-Qing Yu
Persulfate-based heterogeneous catalytic oxidation systems have attracted increasing interests in water pollution control field. Sulfate/hydroxyl radical, singlet oxygen, and catalyst-mediated electron transfer are commonly recognized to be responsible for the organic pollutant removal. However, reliable quantitative methods for detecting reactive oxygen species (ROS) are still lacking to clarify their contribution to the reaction mechanism. In this work, a soluble probe, 9,10-Anthracenediyl-bis (methylene)-dimalonic acid, which is sensitive to both sulfate/hydroxyl radical and singlet oxygen, was developed to semi-quantify the ROS in persulfate-based catalytic oxidation systems. The detection results reveal the predominant catalyst-mediated electron transfer mechanism, rather than the ROS mechanism, and its universality in several representative heterogeneous catalytic systems (i.e., FeMnO, CNT, Mn 3 O 4 , and biochar catalyzing peroxymonosulfate and peroxydisulfate for organic pollutant degradation). Compared with the electron paramagnetic resonance detection with DMPO and TEMP as spin-trapping agents and quenching effects of ROS by alcohol, furfuryl alcohol, and L-histidine, such a semi-quantitative detection method exhibits simplicity and improved reliability in mechanism elucidation. This semi-quantitative method plays a vital role in clarifying the reaction mechanism in persulfate-based heterogeneous catalytic oxidation systems, which might open a door for the optimization and regulation of catalytic oxidation water purification technology.
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ANALYTICAL LETTERS
·
2022
·
IF 2.267
Caifen Chen,Dan Li,Baokang Jin
A selective, sensitive electrochemical biosensor is reported to determine bisphenol A (2,2-bis(4-hydroxyphenyl) propane, BPA) based on target-induced chain release. A gold electrode was premodified with dendritic gold nanoparticles (AuNPs) by direct electrochemical deposition to increase the active surface area of the electrode to immobilize hydrosulfonyl group-containing capture DNA (C-DNA). C-DNA was hybridized with a BPA-specific aptamer (T-DNA) to form a double helical structure. After the embedding of methylene blue (MB), this structure emitted measurable electrochemical signals. BPA specifically binds to T-DNA to form a stable BPA G-tetrad structure, thereby inducing the release of the aptamer chain and the embedded MB from the surface into solution, resulting in the reduction of the current signal. The constructed electrochemical biosensor provided a linear response to BPA concentration from 1.0 × 10−9 M to 5.0 × 10−7 M with a detection limit of 9.8 × 10−10 M. This strategy also provided good selectivity for BPA compared to similar interferents.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 17
·4897-4907
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IF 4.478
Yang Zhenglun,Chen Yihui,Jia Jianggang,Hou Chunyan,Xuan Rongrong,Wang Tingting
In the current study, the C18-modified halloysite was fabricated via silylation reaction and subsequently used as sorbent in matrix solid-phase dispersion (MSPD) for the extraction of bisphenol A and diethylstilbestrol from human placenta, followed by high-performance liquid chromatography-tandem mass spectrometry analysis. The as-prepared sorbent was characterized by scanning electron microscopy, energy-dispersive spectrometry, Fourier transform infrared spectroscopy, X-ray diffraction, and thermo-gravimetric analysis. Varied parameters such as methanol concentration in wash solvent, pH and salt concentration in elution solvent, elution volume, and mass ratio of sample to sorbent were optimized. The adsorption capacities of bisphenol A and diethylstilbestrol on the developed C18-modified halloysite were 6.3 and 14.2 mg g −1 , respectively, higher than those on the commercial C18 silica gel. Under the optimal condition, the average recoveries of bisphenol A and diethylstilbestrol by MSPD varied from 91.0 to 106.0%, and the relative standard deviations were less than 10.6% for human placenta samples. The limits of detection in the human placenta were 0.2 μg kg −1 for bisphenol A and diethylstilbestrol. The simple C18-modified halloysite-based MSPD method holds great potential for the determination of trace bisphenol A and diethylstilbestrol in the human placenta and other tissues of pregnant women with high sensitivity, accuracy, and reliability. Graphical abstract
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FOOD CHEMISTRY
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2022
·
IF 9.231
Minglu Wang,Ying Wang,Xiangyang Li,Hongyan Zhang
The continuous intake of diethylstilbestrol (DES) residue seriously threatens the health of consumers, so the rapid and sensitive detection of DES is helpful for timely food safety warning. In this study, a photothermal-sensing microfluidic paper-based analytical chip (PT-Chip) was developed for effectively screening of DES residue in foods. Competitive inhibition immunochromatography was introduced and the composite of black phosphorus nanosheets and gold nanoparticles (BP-Au) was used as signal indicators. Then, the test area was irradiated by an 808 nm laser and the photothermal transduction signal was recorded by a thermal imager to achieve sensitive photothermal detection. The amount of DES was obtained by analyzing the temperature change curve of test area. The PT-Chip can achieve accurate quantification of DES with a detection limit of 0.1 μg/L. And the successful determination of DES in different food samples indicating that the PT-Chip can be used as a promising detection device.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Wenxue Xiong,Feng Hu,Ying Liu,Gang Nie,Ling Xiao
FeMn bimetallic nanoparticles coated with nitrogen-doped graphene shells (FeMn@NG) were prepared by calcination of cellulose supported Prussian blue analogs under N 2 flow, and used as catalysts to activate peroxymonosulfate (PMS) for the degradation of 2,4,6-trichlorophenol (2,4,6-TCP). The addition of cellulose during the formation of Prussian blue analogs reduced the agglomeration of metal particles in the subsequent carbonization process, thus increasing the specific surface area and enhancing the catalytic efficiency of the obtained catalyst. 1 O 2 and the electron transfer pathway were proved to be the main mechanisms by radical quenching experiment, electron paramagnetic resonance and chronoamperometry analysis. The metal leaching of lower than 0.1 mg L −1 and high catalytic stability were attributed to the stable core-shell structure that the metals were encapsulated and protected by graphene shells. The XPS analysis implied that a Fe/Mn redox cycle existed and played a role in balancing electrons during the PMS activation . This study shows that the PMS activator with high catalytic activity can be obtained for the degradation of pollutants by combining Prussian blue analogs with cellulose.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Shan Liang,Xiao-Ling Wu,Jun Xiong,Xin Yuan,Shu-Li Liu,Min-Hua Zong,Wen-Yong Lou
Nanozyme has emerged as promising alternative to natural enzyme during recent years. Currently, laccase nanozyme is mainly limited to Cu-containing materials with catalytic Cu as active site. Noncopper laccase nanozyme, however, has not attracted extensive attention. Herein, inspired by multicopper active site and redox Cu 2+ /Cu + electron transfer pathway of natural laccase, a range of multivalent cerium-based metal–organic frameworks (Ce-MOFs) with considerable laccase-mimicking activity were designed, where the internal cerium redox (Ce 4+ /Ce 3+ ) reactivity could mimic the active center and catalytic function of natural laccase. Compared with natural laccase, Ce-UiO-66 and Ce-MOF-808 exhibited not only better catalytic efficiency (at identical mass concentration) but also superior stability and recyclability toward the oxidation of phenolic compounds. Accordingly, they were applied for detection of mercaptan contaminants and degradation of bisphenol A, showing great potential in environmental catalysis. This work provides new deep insights for rational design of advanced nanozymes and demonstrates the huge potential of applying nanozymes for environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Yue Zhao,Chenghong Feng,Chenhao Tian,Zhenling Li,Yu Yang
Bisphenol analogues (BPs) are widely used as plasticizers and can be released during the aging and degradation of microplastics. Their persistence in water can cause serious harm to the ecosystem and human health. To improve the capture ability of COFs toward these estrogen-like toxins from water, amino group-functionalized COFs (COFs-TpBD(NH 2 ) 2 ) were constructed from nitro group COFs (COFs-TpBD(NO 2 ) 2 ) via the reduction of nitro to amino groups, and the adsorption behaviors for the five BPs (BPA, BPF, BPC, BPS and 4-CP) were compared. The focus was laid on the role of functional-group-tuning in the changes of adsorption capacity, selectivity and mechanisms of the COFs absorbents. The results showed that TpBD(NH 2 ) 2 has a higher adsorption capacity and better adsorption selectivity for most BPs than TpBD(NO 2 ) 2 . COFs with nitro and amino groups show the best adsorption selectivity for BPC (K F = 6.71 min −1 ) and BPF (K F = 9.49 min −1 ), respectively. Chemisorption dominates the adsorption of the two COFs, and internal particle diffusion is the rate-determining step. The adsorption behavior difference between the two COFs was ascribed to the successful conversion of functional groups of the COFs from nitro to amino groups, which was proven by FT-IR, SEM, PXRD, and BET characterization results. Adsorption of BPA, BPC and BPF by TpBD(NO 2 ) 2 is positively related to hydrophobic interactions (represented by log K ow ), but the adsorption mechanism of TpBD(NH 2 ) 2 was mainly attributed to the electrostatic interaction, as evidenced by the zeta potential and pKa. Hydrogen bonds were proven to be a critical factor that affects the adsorption of BPS and 4-CP by COFs. This study on the appropriate selection of COFs functional groups can provide insight into the future design of adsorbents and the prevention of BPs pollution release from microplastics.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhuoyu Bu,Minhui Hou,Zihao Li,Zhujun Dong,Lusha Zeng,Peng Zhang,Guangyu Wu,Xiang Li,Ying Zhang,Yuwei Pan
Boron was used as an environmentally friendly and efficient reductant to accelerate the recycle of Fe 2+ enhancing peroxymonosulfate (PMS) activation for sulfamethazine (SMT) degradation. The SMT removal was only 28.1% within 30 min in Fe 2+ /PMS system while SMT removal could reach to 98.9% within only 3 min in Boron/Fe 2+ /PMS (B/Fe 2+ /PMS). Electron paramagnetic resonance spectroscopy (EPR) tests, quantitative detection and radical quenching experiments illustrated that OH and SO 4 − played important role and Fe(IV), 1 O 2 and O 2 − also participated in SMT removal. The addition of boron could enhance the role of OH and SO 4 − in SMT removal in Fe 2+ /PMS system. X-ray photoelectron spectroscopy (XPS), electrochemical tests and density functional theory (DFT) calculation were conducted to confirm the mechanism of boron for accelerating the recycle of Fe 2+ . Possible SMT degradation pathway was proposed. B/Fe 2+ /PMS process could efficiently remove SMT at low Fe 2+ dosage and neutral pH. B/Fe 2+ /PMS system also exhibited a superior resistance to inorganic ions and nature organic matters. Moreover, B/Fe 2+ /PMS system had good applicability to different pollutants, excellent reusability for antibiotics removal, and efficient performance for removing antibiotics in nature fresh water. The results compared with others’ works also demonstrated the present study process was a promising strategy for antibiotics removal.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
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IF 11.357
Honglong Zhang,Zhenyu Shi,Jun Ma,Fuyi Cui,Jing Zhang,Timothy J. Strathmann
In this study, a representative redox mediator, 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO), and its para-substituted derivatives (TEMPOs: 4-hydroxyl-TEMPO, 4-acetylamino-TEMPO, and 4-amino-TEMPO) significantly accelerated the abatement of trace organic contaminants (TrOCs, i.e., bisphenol-A (BPA), phenol, amines, and phenylbutazone) by Mn(VII) over a wide pH range of 4.0–9.0. The addition of substituents at para to the > N–O• moiety significantly influenced the degradation kinetics of TrOCs by changing the reduction potentials of TEMPOs and the corresponding oxoammonium cations (TEMPOs+); a linear relationship was observed between the substituents’ para Hammett sigma constants and the reduction potentials of TEMPOs and TEMPOs+. Pseudo-first-order reaction rate constants (kobs, min–1) of TrOC degradation by Mn(VII)/TEMPOs were also affected by the pKa of the TrOCs. Generally, the highest kobs values for individual TrOCs were observed at pH near the pKa even for TEMPOs+ with relatively pH-invariant reduction potentials. Overall, TrOC abatement kinetics were related to a combination of reactive species (Mn(VII), in situ formed MnO2, and TEMPOs+). For BPA, the relative contributions (R) of reactive species ranked as R(TEMPOs+) > R(Mn(VII)) > R(in situ formed MnO2) at pH 4.0–8.0, whereas R(Mn(VII)) > R(TEMPOs+) at pH 9.0 mainly owing to a change in BPA speciation as the pH approached the pKa1 value for BPA. The results of this study are useful for the development of heterogeneous TEMPO-based redox mediators and future applications of TEMPO-mediated oxidation systems for accelerated abatement of TrOCs in water.
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RESOURCES CONSERVATION AND RECYCLING
·
2022
·
IF 13.716
Di Zhang,Shaowei Hu,Zhiqin Cao,Hongbin Cao,Yuehong Zhao,He Zhao
To address aggravating environmental and energy problems, the harmless treatment and resource utilization of waste has become an inevitable choice. In this study, we report a highly efficient and low-carbon reuse approach of coagulation sludge waste based catalysts for electro-Fenton(EF) process to treat wastewater. The results showed that the relative amount of iron element in flocs increase gradually along with the growth in coagulant dosage, the main composition of floc is iron-HA complex and the interaction force acting between them was weak complexation. According to evaluation by electrochemical characterization, the selectivity of sludge electrodes for hydrogen peroxide in Oxygen Reduction Reaction (ORR) process was more than 40%. Without add additional Fe 2+ , the as-prepared cathode material is able to achieves 98.7% bisphenol A (BPA) pollutant removal from wastewater within 130 min treatment due to its highly active two-electron reduction of oxygen (O 2 ). Based on life cycle assessment (LCA) results, compared to traditional sludge disposal, the raw sludge used for EF could reduce fossil resource consumption by 73.7% and carbon emissions by more than 97.1%. The coagulation sludge applied in the field of EF in this paper proposes a novel and reliable way of collaborative treatment of sludge and sewage pollutants, and has certain guiding significance in environmental treatment and sludge recycling.
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