WATER RESEARCH
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2022
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IF 13.4
Xiwen Liu,Penghui Shao,Shanshan Gao,Zhaoyu Bai,Jiayu Tian
Benzoquinone (BQ) is of great significance for enhancement of contaminants degradation in the homogeneous oxidation system of peroxymonosulfate (PMS). However, the role of BQ in the heterogeneous activation of PMS for contaminants oxidation is still not clear. Herein, this work reported that the addition of BQ into the Fe 3 S 4 /PMS system could effectively enhance the degradation and mineralization of bisphenol A (BPA). Mechanistic study uncovered that the BQ and PMS would form active complexes (BQ-PMS*) on the surface of Fe 3 S 4 and the excited BQ-PMS* can oxidize the BPA. To be specific, the electron of BPA was extracted by BQ-PMS* and then transfer to the surface of Fe 3 S 4 . The surface electron can induce the change of valence state of S and Fe elements, which can trigger the degradation of BPA and inhibit the decomposition of BQ itself. To the best of our knowledge, it is the first time to unveil the positive role of BQ in the heterogeneous activation of PMS, which may shed new light on the establishment of high-efficient PMS-based oxidation technology for remediation of organic pollutant.
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PubMed
高影响因子
CARBON
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2022
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IF 11.307
Huizhong Zhang,Jiayu Tian,Xiangke Cui,Jiansheng Li,Zhigao Zhu
Porous carbon with high specific surface area (SSA) has attracted considerable attention in capacitive deionization (CDI) owing to the abundant active adsorption sites. However, porous carbon dominated by the micropores tends to increase the ion transfer resistance and overlap the electrical double layers (EDLs), greatly limiting the ion adsorption rate and amount. In this work, a highly mesoporous carbon nanofiber electrode with an ultrahigh specific surface area (SSA) was prepared via electrospinning ZIF-8/benzoxazine/polyacrylonitrile (ZIF-8/BA-a/PAN) composite solution as carbon precursor. Benefiting from the cooperation of the simultaneous evaporation of Zn in ZIF-8 and activation treatment, the resultant carbon nanofibers show an ultrahigh SSA of 3066.29 m 2 /g, a pore volume of 2.23 cm 3 /g and a mesopore ratio of 72.53%, which has a high salt adsorption capacity (SAC) of 47.22 and 63.83 mg/g in 500 mg/L NaCl (50 mL) solution at 1.2 and 1.6 V, respectively. Furthermore, electrochemical measurement revealed that the high electrical double-layer capacitance facilitates ion storage in the mesoporous carbon nanofibers due to the increased nanopore size and reduced EDLs overlapping. This work provides new insight into designing novel highly mesoporous carbon with ultrahigh SSA for the next-generation electrode materials for energy and environmental applications.
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高影响因子
JOURNAL OF SEPARATION SCIENCE
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2022
·Vol. 45
·期 23
·4224-4235
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IF 3.614
Ruozhu Xu,Yuan Tao,Wang Yao,Honglin Qin,Lizhen Qiao
In this study, three-dimensional flower-like tin disulfide materials were prepared, and a highly efficient dispersive solid-phase extraction method was developed using the obtained three-dimensional tin disulfide adsorbents for the preconcentration and determination of six endocrine-disrupting phenols in combination with high-performance liquid chromatography-ultraviolet detection. Several important experimental parameters influencing extraction efficiency were investigated, including the amount of adsorbent, ultrasound time, sample solution pH, sample volume, type of elution solvent, desorption time, and the number of desorption times. Under the optimized experimental conditions, the developed method showed good linearity with the determination coefficients of 0.993–0.998 in the linear range of 0.5–400 ng/ml and low limits of detection in the range of 0.15–1.0 ng/ml, as well as satisfactory intra-day and inter-day precisions with relative standard deviations of 0.1–9.8%. Finally, the proposed method was successfully applied for the enrichment and determination of trace endocrine-disrupting phenols in milk, tea beverage, and plastic bottled water samples, and acceptable recoveries were obtained from 70.1% to 119.1% under four different spiked concentration levels. The results showed that the three-dimensional tin disulfide materials had great potential for the extraction of endocrine-disrupting phenols contaminants in environmental and food samples.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Yuanxi Huang,Lingjun Bu,Shumin Zhu,Shiqing Zhou,Zhou Shi,Jianwu Wang
Peracetic acid (PAA) is a potential disinfectant for water treatment due to its high efficiency and the limited formation of disinfection byproducts (DBPs). In PAA process of this study, bromide (Br − ) significantly enhanced the degradation of phenolic compounds , including bisphenol A (BPA), phenol , p -aminophenol, and hydroquinone. The promotion is mainly due to the formation of hypobromous acid (HOBr), which comes from the oxidation of Br − by PAA. A kinetic model of PAA treatment in the presence of Br − was established to explore the degradation mechanism of phenolic compounds with good accuracy. The removal of phenolic compounds is positively related to Br − concentration. The degradation process was pH-dependent and favored at acidic conditions. In the real water matrix, the presence of multiple water matrix components may inhibit the degradation of phenolic compounds by consuming PAA and HOBr. Further, the transformation of BPA mainly involves bromination , hydroxylation, oxidation, bond cleavage, and ring opening, resulting in the formation of organic bromines. Brominated DBPs, such as dibromoacetic acid and tribromomethane were found, suggesting the potential adverse health effects of PAA treatment in the presence of Br − . The acute toxicity of phenolic compounds initially increased and then decreased with the increase of reaction time, indicating that prolonging the reaction time may reduce the environmental risk.
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DIAMOND AND RELATED MATERIALS
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2022
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IF 3.806
Qian Zhang,Si Chen,Zhi Huang,Yanying Liu,Jun-ming Hong
In this research, a novel insight was provided for oriented low-temperature S and N doping into graphene oxide (GO).Given the gradual concern in the high-temperature dependence of traditional annealing method for the oriented design of heteroatom doping, utilizing O 3 etching-assisted heteroatom doping can simultaneously resolve the problems of energy consumption and doping species design. In this research, with O 3 etching, 100 at.% marginal S (C-SO X -C) and 92 at.% graphitic N co-doped O 3 -S/NGO were successfully synthesized at annealing temperature of 200 °C. Characterization results showed that S and N doping via O 3 etching maintained the sheet-like structure of GO without much stacking (layer thickness of 4–5 nm). In addition, active defects were formed by O 3 etching and S/N atom doping to provide active center for catalytic reaction . The electrocatalytic degradation behavior proved that 100 % bisphenol A degradation efficiency could be achieved by O 3 -S/NGO within 30 min and that the main active species generated during the reaction were O 2 •− , 1 O 2 and active chlorine. The possible pathways of bisphenol A degradation were also determined to complete the discussion. This project was based on the environmental demand of organic pollution control and suggested an optimal preparation strategy for high-performance catalyst preparation and utilization.
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CHEMISTRY OF MATERIALS
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2022
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IF 10.508
Shengda Wang,Hanqing Jiang,Ronghua Yu,Shenghui Lou,Li Ma,Jie Liu,Tao Tang
A series of epoxy resins containing aromatic imine are synthesized via the Duff reaction by using various bisphenols, which show significantly reduced heat release capacity (HRC) and total heat release (THR) after curing. Compared to diglycidyl ether bisphenol A/4,4-diaminodiphenyl methane (DGEBA/DDM), the HRC and THR of phenolphthalein-based epoxy resin containing aromatic imine/DDM (BPP-E/DDM) are reduced by 87% (464 J/g K vs 58 J/g K) and 62% (30.2 kJ/g vs 11.4 kJ/g), respectively. Furthermore, the BPP-E/DDM exhibits a UL-94 V-0 rating (1.6 mm) and a limiting oxygen index of 48% (3.2 mm). Compared to DGEBA/DDM in the cone calorimeter test, the peak heat release rate, THR, peak smoke produce rate, and total smoke production of BPP-E/DDM were reduced by 91% (1006 kW/m2vs 87 kW/m2), 51% (89 MJ/m2vs 44 MJ/m2), 89% (0.36 m2/s vs 0.09 m2/s), and 79% (38 m2vs 8 m2), respectively. The influences of aromatic imine and the chemical structures between two benzene rings in the bisphenols on HRC and THR of the resultant epoxy thermosets are investigated. The mechanism studies show that the presence of aromatic imine in the epoxy resins completely changes the decomposition process to generate the products containing aromatic N-heterocycle, which contributes greatly to the improved char-forming ability and flame retardancy. Meanwhile the thermosets bearing carbonyl, 3-phthalidylene, and sulfonyl between two benzene rings in the bisphenols show better char-forming ability and flame retardancy among the resultant epoxy resins containing aromatic imine, due to more polycyclic aromatic hydrocarbons produced in the condensed phase.
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高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Wei Zhong,Jin Zou,Yanyu Xie,Jing Yang,Mingfang Li,Shuwu Liu,Yansha Gao,Xiaoqiang Wang,Limin Lu
Herein, a highly sensitive and selective electrochemical sensor for the detection of benomyl (BN), a typical benzimidazole fungicide was proposed based on hierarchical nano-Cu x O decorated MWCNTs-COOH/MXene (nano-Cu x O-MWCNTs-COOH /MXene) composite. The ternary heterostructure presents good electrical conductivity, large specific surface area, and high catalytic activity, exhibiting excellent electrocatalytic activity with enhanced electrochemical signals towards the oxidation of BN. Besides, the embedded nano-Cu x O particles possess strong affinity toward benzimidazole molecules, which could promote the preconcentration of BN, further enhancing the sensitivity, as well as ensuring the high selectivity. Benefitting from the synergistic effect of components in the composite, the developed sensor presents a broad linear range from 10.0 nM to 10.0 μM with a low limit of detection of 3.0 nM (S/N = 3). Meanwhile, the nano-Cu x O-MWCNTs-COOH/MXene electrode also displays good long-term stability and repeatability. Furthermore, this method was successfully applied for the detection of BN in apple samples, illustrating its promising practicability.
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2022
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IF 6.449
Xin Zhao,Zeyu Zhang,Jinyin Pang,Ling Su
Formaldehyde attacks the ortho phenolic hydroxyl groups on the p-hydroxyphenyl and guaiac-based structures in the lignin, shedding the hydrogen atom on the ortho-position carbon and grafting hydroxymethyl group to obtain the hydroxymethylated modified lignin (HMKL). The infrared spectroscopy , hydrogen NMR spectroscopy, thermogravimetric (TG), and derivative thermogravimetric (DTG) analysis show that the hydroxymethylation modification of alkali lignin is successful. Then, lignin nanoparticles (LNPs) are prepared by the acid precipitation self-assembly method in ethylene glycol solution of hydroxymethylated modified lignin. The particle size and shape of lignin nanoparticles are determined by scanning electron microscopy and dynamic light scattering (DLS) analysis. In the liquefaction agent prepared from polyethylene glycol 400 and glycerol, the graft polyol is liquefied under methanesulfonic acid . The Fourier transform infrared spectroscopy , hydrogen NMR, and thermogravimetric analysis indicate the successful formation of nano-lignin polyols. In addition, epoxy resin is synthesized by two-step epoxidation of nano-lignin polyols including ring-opening and closed-loop epoxidation in an alkaline environment. The prepared epoxy resin from nano-lignin polyol exhibits excellent performance and wide application prospects. The optimum process conditions are the mass fraction of LNP-P is 19.98 %, the amount of catalyst (NaOH) is 20.10 %, the reaction time is 6.99 h, the solid content of the epoxy resin is 57.05 %, the viscosity is 615.58 mPa.s, the tensile strength is 44.80 MPa, the elastic modulus is 2.77 GPa.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Qikai Shentu,Zenglong Wu,Wenkai Song,Shiyuan Pan,Zhenyang Zhou,Weiyang Lv,Changsheng Song,Yuyuan Yao
Developing metal-free catalysts for persulfate-mediated oxidation process has been extensively pursued in environmental remediation, yet the activity of these catalysts is typically low and the mechanism is ambiguous. Herein, a facile one-step pyrolysis method was employed to synthesize the carbon doped boron nitride (C-BN) derived from polydopamine coated BN nanosheets. The C-BN could readily activate peroxymonosulfate (PMS) with the activation energy as low as 14.95 kJ/mol, giving rise to admirable performance for bisphenol A removal even at 0 ℃, which was superior to most reported metal-free catalysts. The combined experimental and density functional theory (DFT) analyses pointed out that the remarkable performance of C-BN originated from the B-N-C moieties, which could induce the electron transfer from catalyst to PMS to promote the fast generation of superoxide radicals (O 2 •− ) as the dominant reactive species. These findings take a step toward exploring the highly efficient metal-free catalysts for realistic applications.
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APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Jiabai Cai,Qi Jing,Huan Li,Lin Wang,Yingchao Cheng,Masaki Takaoka
In this study, a novel catalytic air oxidation (CAO) process is proposed based on a facilely synthesized nanocomposite catalyst. The catalyst was prepared using Cu single atoms (Cu SA ) embedded on multiwalled carbon nanotubes (CNTs), denoted as CNTs@Cu SA , with mass ratio of Cu SA up to 10.02 %. Humic acid (HA) and other typical refractory contaminents were used to investigate the ability of CNTs@Cu SA in CAO. The catalysts were pre-excited to cross the energy barrier at 120 °C for 10 min, and then used to catalyze the oxidation of HA at 90 °C in 50 min. The CNTs@Cu SA with Cu SA mass ratio 8.39 % showed a superior catalytic activity, and 99 % of HA in solution was degraded with 98 % of organic carbon mineralization. Aberration-corrected transmission electron microscopy, electron paramagnetic resonance spectroscopy, and density functional theory calculations were applied to detect the mechanism. The results showed that the Cu-N coordination sites on CNT walls and the confinement effect of CNTs activated O 2 to produce ·OH radicals, with a high activation efficiency. Moreover, this catalyst remained active after multiple cycles. This result provides a new catalyst to support low-temperature catalytic air oxidation for organic wastewater treatment.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Xiaotong Zhu,Yuanyuan Zhang,Shengxiao Zhang,Shuangshuang Yang,Qiang Xu
In this study, biomass carbon supported with iron and cobalt bimetal (FeCo/BC) was synthesized by a one-pot calcination method to activate peroxymonosulfate (PMS) and peroxydisulfate (PDS) for bisphenol A (BPA) degradation. Characterization with X-ray diffraction, X-ray photoelectron spectroscopy and high resolution transmission electron microscopy showed that Fe 0 , Fe 3 O 4 , Co 0 and CoO nanocrystals were included in FeCo/BC materials. The degradation results showed Fe 0.6 Co 0.4 /BC had excellent catalytic activation performance for PMS or PDS. The Fe 0.6 Co 0.4 /BC (0.0050 g) combined with 0.25 g·L −1 of PMS could completely degrade 20 mg·L −1 BPA within 8 min, and the same amount of BPA could be removed with 0.020 g Fe 0.6 Co 0.4 /BC in the presence of 0.25 g·L −1 PDS within 20 min. The corresponding total organic carbon removal rates reached 83.49% and 77.5% respectively after 2 h. The Fe 0.6 Co 0.4 /BC also had good adaptability to solution pH and practical water body. After five cycles, the degradation rates of BPA in the two systems were all over 90%, and excellent magnetism was beneficial to the reuse of catalysts. Electron paramagnetic resonance and free radical quenching tests indicated that SO 4 •- , •OH, and 1 O 2 were the main active species involved in the BPA degradation. This work not only provided a promising catalyst for the degradation of organic pollutants, but also elucidated the synergistic effect between Fe-Co bimetal alloys during PMS and PDS activation, which would facilitate the design, synthesis, and application of catalytic materials with high efficiency.
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Environmental Science-Water Research & Technology
·
2022
·Vol. 8
·期 10
·2231-2244
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IF 5.819
Jun Zhao,Jingquan Wang,Erdeng Du,Yijie Ai,Jingjing Liu,Hongguang Guo
The increasing need for water decontamination under high salinity conditions calls for alternative processes with high efficiency and cost-effective performance, of which electrochemical technologies hold continuous attraction. Compared to several studies under chloride background, contaminant degradation in high sulfate concentrations using electrochemical methods has rarely been studied. In this study, a facile and cost-effective TiO2 nanotube (NT) electrode, coated with a PbO2 layer was fabricated to serve as an anode to degrade the selected contaminant under the condition of high sulfate concentration. 100% removal of 0.05 mM 2,4-dichlorophenol (2,4-DCP) was achieved within 50 minutes at a relatively low current density. Degradation of 2,4-DCP followed pseudo-first-order kinetics in the electrochemical system, and the parameter of current density was proved to have the biggest effect on the pollutant removal performance compared to pH and salt concentrations. The mechanism of 2,4-DCP degradation followed the radical and direct electron transfer (DET) pathways. Even though the sulfate radical was generated in water containing high sulfate, the theoretical energy barrier calculated from density functional theory (DFT) simulation indicates the priority of hydroxyl radical on pollutant degradation, and the comparison of reaction energy based on experiments and DFT also suggested that the sulfate radical is more prone to act as a precursor for more hydroxyl radical formation. The degradation performance under various salt conditions was also investigated in this study. High content of chloride in water resulted in extremely fast removal performance, while high content of nitrate in water resulted in the apparent inhibition of pollutant removal. The as-made electrodes exhibited excellent performance for the degradation of different contaminants and reliable stability after rounds of use. This study provides an insight into the application of an electrochemical oxidation system in high salinity wastewater treatment.
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