JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Bing-Xin Gu,Huan-Huan Wu,Dan Sun,Yan-Li Ji,Cong-Jie Gao
Polymer nanofiltration (NF) membranes have been widely applied in the desalination, resource substances purification and separation, and wastewater treatment . Nevertheless, direct construction of subnanometre channel polymer membranes for achieving high-efficient metal ions separation is still challenging because of the complicated membrane preparation and difficultly manipulating the membrane pore-size in sub-nanometer. Herein, we exploited a novel subnanometre channel membrane with zwitterionic β-cyclodextrins (ZCDs) by interfacial polymerization. Wherein ZCDs act as building blocks with hydrophobic inner subnanometre cavities and hydrophilic outer rims, allowing for simultaneously improved water permeability and metal ions selectivity. By modulating the zwitterionic monomer grafting ratio of ZCDs and their loading content in the membrane, the ZCDM membrane exhibits high water permeance (J = 21.7 L m −2 h −1 ∙bar −1 ) and heavy metal ions rejection, e.g., R Cr3+ = 99.8%, R Fe3+ = 98.9%, respectively, these values outperform the state-of-the-art NF membranes. Moreover, the ZCDM membrane has good stability and anti-fouling/-bacterial properties, e.g., the water flux recovery ratio and anti-bacterial ratio is >97% and >99%, in the long-term running process. This work offers a feasible strategy for constructing polymer membranes with uniform subnanometre pore, and demonstrates their potential for the heavy metal separation and wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Hao Ni,Ri-Dong Fan,Krishna R. Reddy,Yan-Jun Du
A novel soil-bentonite backfill is proposed for use in vertical cutoff walls to contain phenol in groundwater at contaminated sites. The backfill consists of sand and bentonite modified with tetramethylammonium and carboxymethylcellulose, labeled as STCMB backfill. Flexible-wall permeability and double-reservoir diffusion tests were conducted to investigate the impact of phenol solution on hydraulic conductivity ( k ), effective diffusion coefficient ( D *) and partition coefficient ( K p ) of the backfill, respectively. The permeability results showed k of the STCMB backfill decreased by 0.91 times when the permeating liquid was changed from tap water to phenol solution. The diffusion testing results showed that D * values for the STCMB and conventional backfill (labeled as SCB backfill) were 4.0 × 10 −10 m 2 /s and 3.0 × 10 −10 m 2 /s, respectively, whereas K p values for the STCMB and SCB backfills were 2.0 mL/g and 0.75 mL/g, respectively. The octanol-water partition coefficient model is suitable for estimating K p for nonpolar organics. Furthermore, a series of solute transport simulations using Pollute V7 program was performed to evaluate the performance of vertical cutoff walls comprising STCMB and SCB backfills in containing phenol in lateral flowing groundwater. Overall, the STCMB backfill has demonstrated superior effectiveness in containing phenol in groundwater.
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MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Xuemei Wang,Yuan Ma,Zheng Zhou,Zhen Zhang,Jie Zhang,Lin Fan,Xinzhen Du,Xiaoquan Lu
Simple and rapid analytical methods for pharmaceuticals and personal care products (PPCPs) are in high demand for environment monitoring. Herein, an in-situ doping strategy was used to ultrarapid synthesize carbon black (CB)-doped Ce (III, IV)-MOF composite with dumbbell-shaped structure at room temperature, which had been used as an electrochemical sensor for the effective and simultaneous detection of typical PPCPs such as dopamine (DA) and acetaminophen (AC) in complex matrices samples using different pulse voltammetry (DPV). Scanning electron microscope (SEM), Nitrogen adsorption-desorption, X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), and X-ray powder diffractometer (XRD) were used to characterize the morphological and electrochemical properties of synthesized a series material. The mixed-valent CB/Ce (III, IV)-MOF with excellent pore structure properties provided more exposed active sites, which were more conducive to adsorption and thus improved sensing performance. The result showed that the proposed method had a wide linear range (for DA: 0.3–252.0 µM, for AC: 0.3–252.0 µM) and low detection limits (for DA: 0.0955 µM, for AC: 0.1170 µM). Based on the synergistic effect of both CB and Ce (III, IV)-MOF, the composites modified electrodes had excellent electroanalytical capability for DA and AC, which could be used for efficient and rapid monitoring of ECs and the construction of new electrochemical sensor based on MOFs.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jianfeng Zhang,Wenrong Bing,Tiancheng Hu,Xu Zhou,Jiejing Zhang,Jing Liang,Yongguang Li
Mixed culture of microorganisms is an effective method to remove high concentration of phenol from wastewater. Currently, the mechanism of how microorganisms collaborate to enhance the biodegradation of phenol is still a challenge. In this study, the isolated Bacillus subtilis ZWB1 and Bacillus velezensis ZWB2 were co-cultured to enhance phenol biodegradation, and the mechanism of microbial collaboration was further explored. The co-culture of strains could significantly increase the rate (16.7 mg/L·h, 1000 mg/L) and concentration of phenol degradation (1500 mg/L), comparing with mono-culture of ZWB1 (4.2 mg/L·h, 150 mg/L) and ZWB2 (6.9 mg/L·h, 1000 mg/L), among which the highest degraded concentration of phenol for ZWB1 and ZWB2 was 150 and 1000 mg/L. Further, the mechanism of microbial collaboration to enhance phenol biodegradation was raised: the decrease of antioxidant enzymes, and increase of degrading enzymes and surfactants on content after co-culture, assisted the microorganisms in withstanding phenol; Bacillus subtilis ZWB1 used the metabolites of Bacillus velezensis ZWB2 to promote its growth, and further to degrade phenol rapidly; Bacillus subtilis ZWB1 alleviated the damage, which resulted from the pH drop (5.8) of the fermentation broth during phenol degradation that inhibited the growth and degraded ability of Bacillus velezensis ZWB2, making the pH of fermentation broth stable at 7. Metabolic analysis showed that co-culture of strains could produce more alkaline and buffering compounds and pairs, to stabilize pH and reduce the toxicity of acidity on ZWB2, thus increasing the degradation rate. This study explains the mechanism of microbial collaboration on phenol biodegradation from multiple perspectives, especially pH stabilization, which provides a theoretical basis for the degradation of pollutants by co-culture microorganisms.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Xiangfen Xue,Mingjie Wei,Jing Yuan,Xinyu Huang,Qinghua Cao,Changkun Xia,Xiangheng Niu,Xiulian Yin
A convenient, fast, low-cost detection and discrimination method is demanded for environmental monitoring but still it remains more technological challenges. Herein, we demonstrate that the inner filter effect (IFE), in combination with three-dimensional fluorescence spectroscopy, can offer a virtual sensor array (VSA) as a proper solution. And with the aid of pattern recognition techniques, it is feasible to recognize compounds with structural similarities economically and effectively. In this study, with the help of visual clustering plots of principal component analysis (PCA), a prediction model based on hierarchical strategy was made using support vector machine (SVM) method for the qualitative profiling of aromatic pollutants. The VSA was constructed by a single metal–organic framework (MOF) recognition unit (MOF-74 (Zn)) with the excitation wavelength as external regulatory factors. Pattern characteristics of four aromatics with very similar structures (phenylamine, chlorobenzene, nitrobenzene, and phenol), both single analyte and binary mixtures, were acquired. The primary constituents of multi-dimensional spectral signals were subsequently extracted and fed into a vector machine to construct a prediction model through 10-fold cross-validation optimization, resulting in a classification accuracy of 100% for single analytes and 96% for mixtures. Quantitative research has shown that, except for chlorobenzene, all three other analytes can be predicted in concentration within an acceptable error range, and the mixture can be predicted proportionally. Moreover, the VSA can be used to distinguish these pollutants in tap and river water also. We propose for the first time a new tack for the construction of VSA in a general manner, namely using three-dimensional full range fluorescence scanning for IFE based sensing to get multiple times of information resulting from different weak interaction between analyte and sensor for decision-making.
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Separations
·
2023
·Vol. 10
·期 10
·523
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IF 2.6
Xiangfen Cui,Jingmei Liao,Huaying Liu,Wei Tang,Cheng Tie,Senlin Tian,Yingjie Li
The presence of organic pollutants in wastewater remains a prominent environmental concern due to the related ecological and health hazards. In response, this study employs an adsorptive methodology to address the removal of phenol and catechol, utilizing an organo-bentonite material modified with a pH-responsive switchable surfactant, dodecyldimethylamine oxide (C12DAO). The synthesized organo-bentonite (C12DAO-Bt) manifests commendable thermostability resulting from thermogravimetric analyses. The adsorption capacities of C12DAO-Bt concerning phenol and catechol intensify with the augmentation of the C12DAO/bentonite mass ratio. The utmost adsorption capacities of 150C12DAO-Bt, deduced through a pseudo-second-order kinetic model, stand at 5.72 mg·g−1for phenol and 5.55 mg·g−1for catechol, respectively. Subject to modification by a pH-responsive surfactant, conditions leaning towards weakly acidic and neutral conditions (pH = 6~7) are conducive to the adsorption of phenolic compounds. Conversely, alkaline conditions (pH = 8~9) facilitate the dissociation of adsorbates from adsorbents. The augmentation of cationic strength within the examined scope incites the adsorption procedure while impeding the desorption efficacy. In the case of cationic species with comparable ionic strengths, Na+exhibited a superior effect on the adsorption–desorption dynamics of phenol, while Ca2+exerts a more pronounced effect on those of catechol. Moreover, even following five consecutive acid–base regulation cycles, C12DAO-Bt retains a relatively high adsorption capacity and desorption efficacy, which underscores its exceptional regenerative capacity for removing phenolic compounds from wastewater.Keywords:pH-responsive surfactants;organic bentonite;reversible adsorption;phenolic pollutants;wastewater
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CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Tianbo Zhou,Xueshuai Wang,Yi Liu,Liuchun Zheng
The conventional direct esterification and polycondensation is difficult to obtain kilogram scale of poly(butylene succinate) (PBS) ionomers with both high molecular weight and high ionic group content. Therefore, the investigation of relationship between the content of ion group and performance (such as mechanical properties) is impossible. In this work, the preparation of PBS ionomers with high molecular weight and high ion group content was achieved by transesterification method using sodium dimethyl isophthalate-5-sulfonate (SIPM) as the ionic monomer, and the polycondensation time decreased significantly with the increase of SIPM content. The mechanism of reducing the polycondensation time of PBS prepared by transesterification is proposed. The tensile strength, flexural strength and impact strength of PBS ionomers increased significantly with increasing SIPM content. At high ion group content, the formed multiplets-clusters among ion groups, which act as reversible physical crosslinking points and nano-fillers, substantially improved the mechanical properties. The tensile strength, flexural strength and impact strength improved and reached to 50.1 MPa, 40.9 MPa and 13.1 kJ/m 2 at high ion group content from 34.2 MPa, 24.1 MPa and 5.8 kJ/m 2 for PBS, respectively. It showed a totally opposite trend from the previous research. In addition, the hydrophilicity and processing properties of PBS ionomers improved significantly with the increase of the ion group content, and the contact angle reduced to 41.1° after the introduction of ions.
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ACS Catalysis
·
2023
·
IF 12.9
Yanfen Fang,Dengyu Ying,Huibin Niu,Yan Xu,Shaobin Wang,Ran Duan,Huaiyong Zhu,Chaoyuan Deng,Chuncheng Chen,Yingping Huang
Although metal-rich biochar (M-BC) is widely used in soil remediation and pollution control, the activation mechanism of molecular oxygen (O2) by M-BC still needs to be clarified due to the low metal loading. In this study, we enhanced the manganese content of low-temperature manganese-rich biochar (Mn-BC) by treating it with hydrogen peroxide (H2O2), resulting in the formation of MnBC-Hx (where x represents the volume of H2O2 used in mL). MnBC-H5 was particularly effective in activating O2, leading to the successful degradation of phenol and dyes. Characterizations showed that the MnII in the outer layer of MnC2O4·2H2O nanoparticles evenly dispersed over Mn-BC was oxidized to MnIII by H2O2. This process was accompanied by the removal of coordinated H2O, resulting in the formation of MnIIIC2O4 on MnBC-H5. Under visible light irradiation, MnIII can bind to O2 to form MnIIIOOH species, which facilitates the transfer of charges and generates superoxide radicals (·O2–) that effectively degrade organics. Notably, MnIII of MnBC-H5 remains stable after the organic degradation reaction. This study will not only provide a theoretical basis for developing environmentally friendly biochar-based catalysts but also promote the study of the environmental effects of biochar.
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TALANTA
·
2023
·
IF 6.1
Yongzhe Niu,Kai Kang,Beibei Wang,Lanyue Wang,Congwei Li,Xiang Gao,Zhenzhen Zhao,Xueping Ji
Single-atom nanozymes (SANs) can significantly enhance the sensitivity and selectivity of electrochemical sensing platforms due to the homogeneity of their active sites, full atom utilization, and high catalytic activity. In this study, we demonstrate the synthesis and characterization of a high-density Co-based single-atom nanozyme anchored on activated MOF-derived porous carbon (Co-AcNC-3) via a cascade anchoring strategy for ultrasensitive, simultaneous electrochemical detection of catechol (CC) and hydroquinone (HQ). The Co-AcNC-3 displays a large specific surface area , high defectivity, and abundant oxygen-containing groups, with Co atoms being atomically dispersed throughout the carbon support via Co–N bonds. The Co-AcNC-3 biosensor exhibits superior electrochemical signals for CC and HQ, with linear ranges of 4.0 μM–300.0 μM. and detection limits of 0.072 μM and 0.034 μM, respectively. Moreover, the Co-AcNC-3 biosensor has shown excellent performance in accurately detecting CC and HQ in actual samples. Our findings highlight the potential of the proposed Co-AcNC-3 biosensor as a reliable and promising sensing platform for determining CC and HQ.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 43
·e2311585120
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IF 11.1
Chao-Hai Gu,Song Wang,Ai-Yong Zhang,Chang Liu,Jun Jiang,Han-Qing Yu
Single-atom Fenton-like catalysis has attracted significant attention, yet the quest for controllable synthesis of single-atom catalysts (SACs) with modulation of electron configuration is driven by the current disadvantages of poor activity, low selectivity, narrow pH range, and ambiguous structure–performance relationship. Herein, we devised an innovative strategy, the slow-release synthesis, to fabricate superior Cu SACs by facilitating the dynamic equilibrium between metal precursor supply and anchoring site formation. In this strategy, the dynamics of anchoring site formation, metal precursor release, and their binding reaction kinetics were regulated. Bolstered by harmoniously aligned dynamics, the selective and specific monatomic binding reactions were ensured to refine controllable SACs synthesis with well-defined structure–reactivity relationship. A copious quantity of monatomic dispersed metal became deposited on the C3N4/montmorillonite (MMT) interface and surface with accessible exposure due to the convenient mass transfer within ordered MMT. The slow-release effect facilitated the generation of targeted high-quality sites by equilibrating the supply and demand of the metal precursor and anchoring site and improved the utilization ratio of metal precursors. An excellent Fenton-like reactivity for contaminant degradation was achieved by the Cu1/C3N4/MMT with diminished toxic Cu liberation. Also, the selective ·OH-mediated reaction mechanism was elucidated. Our findings provide a strategy for regulating the intractable anchoring events and optimizing the microenvironment of the monatomic metal center to synthesize superior SACs.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Fa-Peng Wu,Le-Le Qiu,Yun-Peng Zhao,Zong-Pin Fu,Jian Xiao,Jian Li,Fang-Jing Liu,Jing Liang,Jing-Pei Cao
Catalytic hydrodeoxygenation (HDO) of phenolic compounds is a promising strategy for bio-oil upgradation to produce high-value chemicals and fuels. Herein, a series of NiFeAlO x catalysts prepared by a co-precipitation method were applied in HDO of guaiacol as a typical model compound. The characterization results revealed that the catalyst with Ni/Fe/Al ratio of 3/0.5/2.5 possessed developed textural properties, small metal particles, abundant oxygen vacancies and acid sites. HDO of guaiacol occurred in two pathways with different hydrogen sources : the direct hydrogenation of benzene ring to 2-methoxycyclohexanone and the further hydrogenolysis and dehydration of intermediates to cyclohexane at 260 °C in n -hexane under H 2 for 6 h, while demethoxylation affording phenol followed by hydrogenation of phenol to cyclohexanol at 220 °C in isopropanol under N 2 for 2 h. The different product composition results from the type of reactive H species, where active hydrogen species are hydrogen radicals using H 2 as the hydrogen source and hydrogen ions with opposite charges using isopropanol as the H-donor solvent, respectively. The Ni 3 Fe 0.5 Al 2.5 O x catalyst maintained good performance after five recycle experiments with a slight decrease in the conversion of guaiacol. Moreover, the catalyst showed excellent universality for selective HDO of other phenolic compounds to cycloalkanes or cycloalkanols.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xi Chen,Yunfeng Chen,Songrong Li,Cheng Xue,Dongfang Liu,Wenli Huang
Phthalic acid esters (PAEs) pose serious health risks to humans and are difficult to remove by conventional sewage treatment processes. Herein, Fe 2 Mo 3 O 8 /MoO 2 /Mo 2 N composite (FMON) derived from bimetallic organic framework was used to activate peroxymonosulfate (PMS) for dibutyl phthalate (DBP) degradation. FMON exhibited an excellent catalytic effect with DBP removal efficiency of 92.4 % within 60 min. Mo 2 N showed a superior ability in promoting Fe 3+ /Fe 2+ redox cycle. The reduction efficiencies of Fe 3+ by Mo 2 N/MoO 2 composite and MoO 2 were 67 %–94 % and 11 %–23 %, respectively, in the homogeneous comparative experiment. Moreover, the ratio of Fe 2+ /Fe 3+ in FMON increased significantly after the catalytic reaction. Fe element doping also enhanced the reuse stability and reduced the metal ion leaching of the catalyst. The degradation of DBP was mediated by a variety of reactive species, of which SO 4 − , OH and O 2 − were dominant. Fe element, Mo element and O vacancies were confirmed to exert significant contributions as active sites in the catalytic process. Three degradation pathways of DBP were obtained by DFT calculation and HPLC-MS analysis. And the toxicity of DBP degradation products was significantly reduced based on the assessment result of Toxicity Estimation Software Tool (T.E.S.T.). This study explored a novel Fe/Mo bimetallic catalyst with friendly Fe 3+ /Fe 2+ cycling for environmental catalysis and provided new ideas for the treatment of PAEs wastewater.
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