CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Bing Wang,RuiQing Zhang,HuiYong Chen,Zhuo Li,EnZhou Liu,HaiXia Ma,Bo Zhou,Hong Hao,LinYu Jiao
Controllable fine-tuning of heterojunction interfaces at the atomic level represents a promising strategy for enhancing semiconductor photocatalytic performance. Herien, we propose a strategy to introduce hydrogen-bonded electron channels at the heterojunction interface to achieve rapid interfacial electron transfer. This S-scheme hydrogen-bonded supramolecular self-assembled H 12 SubPcB-OPhCH 2 COOH/Ag 3 PO 4 semiconductor heterojunction exhibits efficient and stable photocatalytic degradation of a wide range of pharmaceuticals and personal care products. Experimental results and theoretical simulations demonstrate that the interface O-H⋅⋅⋅O hydrogen bond at the heterojunction generates an internal electric field, which provides the driving force for accelerated S-scheme charge transfer and enhanced redox properties. Furthermore, the combination of TDDFT calculations and synchronous illumination XPS has revealed that hydrogen bonding acts as a suction electron pump in the excited state, transferring electrons from Ag 3 PO 4 to SubPc-2. These findings suggest that hydrogen-bonded supramolecular semiconductor can be used to develop high-performance photocatalytic materials for environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ronghao Wu,Xin Hu,Yihui Li,Yongfu Li,Yanjiang Cai,Peikun Jiang,Bing Yu
Constructing bimetallic nanostructures with specific crystalline phases provides an attractive strategy to develop highly efficient catalysts and explore structure-dependent catalytic properties. Herein, a new iron-based bimetallic catalyst consisting of amorphous MnO 2 and crystalline α-Fe 2 O 3 was synthesized for peroxymonosulfate (PMS) activation, named as a-MnO 2 /α-Fe 2 O 3 . The results show that the removal efficiency of sulfamethoxazole is over 90% within 120 min by the a-MnO 2 /α-Fe 2 O 3 in the presence of PMS at broad pH conditions ranging from 3 to 9. Furthermore, a complete degradation of bisphenol A (BPA) is achieved within 2 min in the a-MnO 2 /α-Fe 2 O 3 /PMS system under optimum conditions, and the BPA degradation rate constant of 1.67 min −1 outperforms most reported Fe- and Mn- based catalysts. The results of electron paramagnetic resonance analysis, quenching tests and Raman spectroscopy analysis show that the mechanism for the a-MnO 2 /α-Fe 2 O 3 -based PMS activation is dominated by the formation of activated surface-PMS complexes. ≡Mn(Ⅳ)–OH and ≡Fe(III)–OH of a-MnO 2 /α-Fe 2 O 3 are active sites for PMS adsorption to form inner-sphere complexes (≡Mn(Ⅳ)-OOSO 3 - ) through the replacement of surface hydroxyl groups. Finally, the a-MnO 2 /α-Fe 2 O 3 exhibits a remarkable removal efficiency of over 99% for BPA in column-bed tests conducted over 600 cycles, demonstrating its immense potential for practical applications.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2023
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IF 11.4
Guiping Liu,Kai Chen,Zhiming Wu,Yanhan Ji,Lianghua Lu,Songmeng Liu,Zhi-Ling Li,Rong Ji,Shuang-Jiang Liu,Jiandong Jiang,Wenjing Qiao
Tetrabromobisphenol A (TBBPA), a widely used brominated flame retardant in electronics manufacturing, has caused global contamination due to improper e-waste disposal. Its persistence, bioaccumulation, and potential carcinogenicity drive studies of its transformation and underlying (a)biotic interactions. This study achieved an anaerobic enrichment culture capable of reductively dehalogenating TBBPA to the more bioavailable bisphenol A. 16S rRNA gene amplicon sequencing and quantitative PCR confirmed that successive dehalogenation of four bromide ions from TBBPA was coupled with the growth of both Dehalobacter sp. and Dehalococcoides sp. with growth yields of 5.0 ± 0.4 × 108 and 8.6 ± 4.6 × 108 cells per μmol Br– released (N = 3), respectively. TBBPA dehalogenation was facilitated by solid humin and reduced humin, which possessed the highest organic radical signal intensity and reducing groups −NH2, and maintained the highest dehalogenation rate and dehalogenator copies. Genome-centric metatranscriptomic analyses revealed upregulated putative TBBPA-dehalogenating rdhA (reductive dehalogenase) genes with humin amendment, cprA-like Dhb_rdhA1 gene in Dehalobacter species, and Dhc_rdhA1/Dhc_rdhA2 genes in Dehalococcoides species. The upregulated genes of lactate fermentation, de novo corrinoid biosynthesis, and extracellular electron transport in the humin amended treatment also stimulated TBBPA dehalogenation. This study provided a comprehensive understanding of humin-facilitated organohalide respiration.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Qiuhui Xu,Wenxiang Zhang,Quan Chi,Yuhang Yang,Xi Tan,Jikai Liu,Huaming Xiao,Xian Wang
Endocrine disrupting chemicals (EDCs) are pervasive emerging pollutants found in environmental water, stemming from their widespread use in personal consumer products. This study presents a novel magnetic Porous organic cage (POC) material, Fe 3 O 4 -COOH@CC3R-OH, which has been proven to be highly effective in eco-friendly eliminating EDCs. Featuring a tetrahedral morphology with core–shell structure, the new magnetic adsorbent boasts a substantial Brunauer-Emmett-Teller surface area of 94.02 m 2 /g and a particle pore size of 1.14 nm. Rigorous optimization of adsorption conditions for eight specific EDCs was conducted, complemented by insightful molecular docking simulations shedding light on the adsorption mechanisms. Furthermore, the developed Fe 3 O 4 -COOH@CC3R-OH magnetic solid phase extraction-assisted high performance liquid chromatography-tandem mass spectrometry (MSPE-HPLC-MS/MS) method exhibits good sensitivity and precision in the quantitative detection of EDCs in environmental water samples. This integrated approach provides a robust platform for both efficient removal and accurate detection of EDCs, advancing water quality control and safeguarding human health.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2023
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IF 4.5
Xiaoxian Hu,Jing Qian,Juan Yang,Xiaomin Hu,Yanjiao Zou,Nianjun Yang
Covalent organic frameworks (COFs), a newly emerging kind of porous material, have gained extensive attention due to their fascinating structural features. However, the superiority of COFs as electrochemical sensing materials has not yet been adequately explored. Herein, a new type of core–shell metal–organic framework (MOF)@COF composites are synthesized through in situ growth of TAPB-DMTP-COF on the pre-synthesized Ce-BDC core. The thickness of the COF shell can be controlled to 20–50 nm by adjusting the Ce-MOF mass. It is found that the obtained MOF@COF composite possesses a larger electrochemical active area and faster electron transfer kinetic than its single component. As a case application of this composite, it has been employed as a sensing material for voltammetric detection of metol, where a linear range from 0.1 − 200 μM and a detection limit of 30 nM have been obtained. This study provides a new strategy to synthesize COF-based electrode materials as well as to explore their electrochemical properties and applications.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 7
·1-17
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IF 2.9
Xiao Sihua,Wan Jinquan,Wang Yan,Yan Zhicheng,Ma Yongwen,Sun Jian,Tang Min,Cao Jianye,Chen Jinxin
The large-scale wastewater treatment plants (WWTPs) in developed regions collect volumes of wastewater containing various emerging contaminants (ECs) every day, but without any effective process to eliminate them. Therefore, it is of vital importance to study the occurrence of ECs in the effluents from WWTPs. In this study, the concentration levels and pollution characteristics of typical ECs in effluents were investigated for source identification and risk assessment. In total, 13 of 39 analyzed ECs were detected in the effluents, with the highest detection concentration at 706 µg/L (oxolinic acid). Sulfaphenazole showed the highest detection frequency at 100%, while Liede WWTP (1.2 million m 3 /day), located at Tianhe District, was with the highest detection concentration (899 µg/L) among all sampling sites. Parallel factor analysis was applied to identify the dissolved organic matters (DOMs) of excitation–emission matrix spectroscopy (EEMS) first. Based on previous research data, the connection between DOMs and pollution sources could be built. Then, principal component analysis (PCA) and Pearson’s correlation analysis were used to determine the correlation between ECs and DOMs. Finally, ecological and health risk quotients were calculated for the risk assessment of ECs. The results illustrated that oxolinic acid, sulfaphenazole, sulfaquinoxaline, sulfadimethoxypyrimidine, penicillin V, and flumequine were potentially discharged from human activities and livestock, poultry, and aquaculture industry; the possible sources of sulfadoxine and nafcillin were agricultural activities, food production, and catering industry; sulfapyridine and erythromycin were believed to come from hospital wastewater; and the discharges of lincomycin, sulfameter, and sulfamerazine were related to petrochemical industry or chemical production activities. Except for sulfadoxine, all detected ECs posed a high or median risk on aquatic ecosystem, which is enough to threaten aquatic organisms. Even though only oxolinic acid, sulfaquinoxaline, and sulfadimethoxypyrimidine presented a potential risk on humans’ health, the cumulative effect of ECs in the human body still needs attention. The threats of ECs from large-scale WWTPs in China’s developed regions are pointed out for the first time, which could possibly bring widespread attention on emerging pollution from WWTP effluents, potentially advance the introduction of relevant policies, and provide the direction and target pollutants for follow-up mitigation actions.
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ACS ES&T Engineering
·
2023
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IF 7.1
Kui Yang,Daoyuan Zu,Zhong Zhang,Jinxing Ma,Zhifeng Yang
A reactive electrochemical membrane (REM) has been identified as an excellent platform in micropolluted water purification due to its rapid mass transfer capability. Unlike traditional flow-by systems, the convection-enhanced REM systems activate the REM’s inner reaction sites, potentially imparting a spatially variable reactivity. Therefore, we explored the spatial scale of micropollutant oxidation in REM. Theoretical and experimental evidence demonstrated that an REM might feature nonuniform oxidation activity along its reaction depth (about hundreds of micrometers). That is, the zone generating •OH was located within a few micrometers beneath the REM surface, i.e., less than 1% of its reaction depth due to the rapid overpotential/potential drop in the REM. The nonuniform reactive character might render the REM of a strong direct electron transfer ability, enabling rapid removal of electron-rich micropollutants even at low potentials. However, unsatisfactory removal of electron-poor micropollutants has been observed, and a higher potential was required to prompt the generation of •OH. These results provide in-depth insight into the spatial scale of nonuniform oxidation of micropollutants in REM, contributing to the analysis of micropollutant oxidation mechanisms and the optimization of the design and operation of REM modules for cost-effective water purification.
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BIOSENSORS & BIOELECTRONICS
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2023
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IF 12.6
Yu-Huan Liu,Chang Liu,Xin-Hui Wang,Tong Li,Xing Zhang
Bisphenol A (BPA) is an endocrine disrupting chemical and broadly used in plastics. The leakage of BPA in food and water cycles poses a significant risk to the environment and human health. Thus, monitoring the concentration of BPA to avoid its potential risk is highly important. In this work, a simple and efficient oxygen deficient molecularly imprinted TiO 2 electrochemical sensor was proposed for the detection of BPA. The introduction both oxygen vacancies and molecular imprinting evidently enhanced the electrochemical oxidation signal of BPA. The sensor had a good linear response ranging from 0.01 μM to 20 μM with a limit of detection of 3.6 nM. Additionally, the sensor showed remarkable stability, reproducibility and interference resistant ability. It also exhibits excellent recovery during the detection of real water. These findings suggested that the sensor has the potential to be developed as a simple, efficient and low-cost monitoring system for the monitoring of BPA in water.
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CHEMOSPHERE
·
2023
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IF 8.8
Hao Li,Canyuan Lin,Ruhui Ma,Yuancai Chen
In this study, the selective adsorption of aromatic compounds on mesoporous MIL-53(Al) was investigated, and followed the order: Biphenyl (Biph) > Triclosan (TCS) > Bisphenol A (BPA) > Pyrogallol (Pyro) > Catechol (Cate) > Phenol (Phen), and exhibited high selectivity toward TCS in binary compounds. In addition to hydrophobicity and hydrogen bonding, π–π interaction/stacking predominated, and more evidently with double benzene rings. TCS-containing halogens could increase π interaction on the benzene rings via forming Cl–π stacking with MIL-53(Al). Moreover, site energy distribution confirmed that complementary adsorption mainly occurred in the Phen/TCS system, as evidenced by Δ Q pri (the decreased solid-phase TCS concentration of the primary adsorbate) < Q sec (the solid-phase concentrations of the competitor (Phen)) . In contrast , competitive sorption occurred in the BPA/TCS and Biph/TCS systems within 30 min due to Δ Q pri = Q sec , followed by substitution adsorption in the BPA/TCS system, but not for the Biph/TCS system, likely attributed to the magnitude of energy gaps (E g ) and bond energy of TCS (1.80 eV, 362 kJ/mol) fallen between BPA (1.74 eV, 332 kJ/mol) and Biph (1.99 eV, 518 kJ/mol) according to the density-functional theory of Gaussian models. Biph with a more stable electronic homeostasis than TCS lead to the occurrence of substitution adsorption in the TCS/BPA system, but not in the TCS/Biph system. This study provides insight into the mechanisms of different aromatic compounds on MIL-53(Al).
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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
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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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