JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 29
·期 2
·331-340
·
IF 2.496
Zheng Tao,Li Meisheng,Zhou Shouyong,Zhao Yijiang,Zhong Zhaoxiang,Chen Chenglung
Two-dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets are widely used in photocatalysis, energy storage and membrane separation owing to their high specific surface area, rapid photogenic carrier migration rate and numerous active sites. In this study, high performance g-C 3 N 4 nanosheets with a particle size of about 290 nm were prepared by gas exfoliation. It was observed that the structure and properties of g-C 3 N 4 nanosheets prepared at 500 °C were superior as compared to 300 °C and 400 °C. The state of g-C 3 N 4 layers at different temperatures was also studied by molecular dynamics simulation. It was revealed that the liquid nitrogen (L-N 2 ) molecules could only penetrate the edge space between g-C 3 N 4 layers at 500 °C, however, no penetration took place in the layers. The traditional gas exfoliation mechanisms were observed to be incapable in explaining this phenomenon. Combining the experimental studies and molecular dynamics simulations, a novel gas exfoliation mechanism was proposed in this study so as to prepare few-layered g-C 3 N 4 nanosheets. Based on this, the L-N 2 molecules entered the edge space in g-C 3 N 4 layers and subsequently pushed deeper to exfoliate the nanosheets.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Chuankun Yin,Qianna Xia,Jiao Zhou,Bowen Li,Yu Guo,Aimal Khan,Xiaoxia Li,Aihua Xu
The development of efficient and eco-friendly Mn-based catalysts for peroxymonosulfate (PMS) activation and revealing the mechanism are highly desired for pollutants removal in wastewater. In this study, a ternary mullite oxide YMn 2 O 5 (YMO) was synthesized for bisphenol A (BPA) degradation in the presence of PMS for the first time. Combined with XPS, EPR and TG, abundant surface labile oxygen species (O lab ) with a ratio of 39.7% were identified in the mullite materials, which was higher than that for α-, β-, γ- and δ-MnO 2 . YMO also exhibited higher interfacial conductivity and stronger interactions among the catalyst, PMS and BPA than other MnO 2 . Superior performance in BPA degradation was observed with YMO, and O lab was suggested as the main active sites, for the normalized first-order rate constant was linearly dependent on the ratio of the oxygen species. Chemical quenching experiments, EPR and open circuit potential suggested that the degradation of BPA was mainly caused by the direct electron transfer process through the reactive O lab -PMS complexes. The influence of YMO concentration, PMS concentration, solution pH, different anions and reaction temperature was thoroughly studied. Moreover, the intermediates were identified and the possible degradation pathways were proposed. This work demonstrated that mullite oxide YMO with enriched O lab species can be used as eco-friendly catalysts for efficient PMS activation to remove recalcitrant organic compounds in wastewater.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Jihong Xu,Peisheng Zhou,Penghui Shi,Yulin Min,Qunjie Xu
Concern about nitrogen-doped carbon materials for pollutant removal via nonradical pathway is mounting. In this study, graphite carbon nitride (g-C 3 N 4 ) was transformed into a high nitrogen-doped three-dimensional carbon material (N-CM) through the “metal template method”. The synthesized N-CM showed high efficiency in removing 2,4-dichlorophenol (2,4-DCP) via the activation of peroxymonosulfate (PMS). Under neutral condition, 2,4-DCP (0.2 g/L) was completely eliminated with 0.3 g/L PMS and 0.1 g/L N-CM900 in 30 min. Initial pH value, inorganic anions, and cycle experiments were selected to explore the availability of N-CM900/PMS. In addition, 1 O 2 dominated 2,4-DCP oxidation (about 60–70%), while the remaining 30–40% was contributed by the mediated electron transfer and N-CM-PMS*. Mechanism investigation suggested that graphitic nitrogen, the electron-rich ketonic groups and defects play a pivotal role in peroxymonosulfate activation . Combined with byproducts analysis, small-molecule acids, H 2 O and CO 2 were predominant. Overall, this study unveils a novel direction for the design of high nitrogen-doped carbon materials and improves the understanding of the coexistence of multiple mechanisms in the activation of PMS by nitrogen-doped carbon materials.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Shanshuai Chen,Weichen Wang,Xue Li,Puxiang Yan,Wanying Han,Tian Sheng,Tiansheng Deng,Wanbin Zhu,Hongliang Wang
Catalytic hydrodeoxygenation (HDO) of biomass-derived oxy-compounds to advanced hydrocarbon fuels usually requires bifunctional catalysts containing metals and acidic sites. The appropriate tuning of metal and/or acidic active sites at interfaces of bifunctional catalysts can significantly improve catalyst activity and product selectivity. Here, 4-trifuoromethyl salicylic acid (TFMSA), as a hydrothermal stable organic acid, was employed to tailor the bifunctional interface of Ru/γ-Al 2 O 3 to enhance the catalytic performance on converting lignin-derived phenols to jet fuel range cycloalkanes. More than 80% phenol was converted into cyclohexane at 230 °C for 1 h over Ru/γ-Al 2 O 3 modified by TFMSA, which was about three times higher than that over unmodified Ru/γ-Al 2 O 3 . X-ray diffraction (XRD), Transmission electron microscope (TEM), H 2 chemisorption, and energy dispersive X-ray spectroscopy (EDS) elemental mapping results indicated that Ru nanoparticles and TFMSA were well distributed on γ-Al 2 O 3 , and a nanoscale intimacy between Ru and TFMSA was reached. Meanwhile, Fourier transform infrared spectroscopy after pyridine adsorption (Py-FT-IR) analysis proved that Brønsted acidic sites on the catalytic interfaces of TFMSA modified Ru/γ-Al 2 O 3 had been improved. Moreover, the kinetic and density functional theory (DFT) results suggested that the synergistic effects of adjacent Ru nanoparticles and acidic sites were crutial for promoting the rate-limiting conversion step of phenol HDO to cyclohexane.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2021
·
IF 4.952
Li Li,Yafan Zhao,Jiaqi Li,Lanzhen Ban,Lina Yang,Shengnan Wang,Lijie Zhu,Hong Song,He Liu
Soy hull insoluble dietary fiber (SHIDF) extracted from soybean water-soluble polysaccharides enzymatically is a good carbon source for the growth of gut microbiota. Genomics, co-precipitation and proteomics analyses were used to investigate adhesion behavior of the gut microbiota toward SHIDF in vitro. After gut microbiota fermentation, the content of total and reducing sugars decreased with increasing fermentation time, but the content of NH 3 –N first increased and then decreased, and gas was produced mainly during 8–16 h. The structure and abundance of the gut microbiota were regulated after fermentation. Proliferation of beneficial bacteria increased, particularly Lactobacillus and Bifidobacterium . The adhesion of Lactobacillus plantarum and Bifidobacterium longum to SHIDF increased gradually with increasing adhesion time. The adhesion of two probiotics to IDF first increased and then decreased with increasing bacterial age (6, 12, 24, and 36 h). SDS, EDTA, bile salts, trypsin and proteinase K in the adhesion environment affected probiotic adhesion to SHIDF to a certain extent. Lactobacillus plantarum and Bifidobacterium longum showed significant differences in adhesion membrane proteins after SHIDF treatment. The 30S ribosomal protein S21 and GAPDH (glyceraldehyde 3-phosphate dehydrogenase), a surface protein involved in intestinal adhesion, were found to be significantly upregulated through label free proteomic analysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Junxin Chen,Caijin Zhou,Bingqi Xie,Jisong Zhang
Dean vortices generated through the curved paths have been demonstrated to be beneficial to enhance gas–liquid mass transfer in membrane contactors. However, the effect of Dean vortices in liquid–liquid membrane extraction was seldom studied. This work implemented a numerical model describing the liquid–liquid extraction process in curved membrane contactors with the software of COMSOL. The liquid–liquid extraction experiments were first performed verifying the applicability of the simulation. Firstly, the discussion about the role of membrane resistance revealed the fact that enhancement provided by Dean flows would be more pronounced for systems with lower membrane resistance. A parametric study was then conducted including geometric parameters and physical properties of the fluid, which indicated smaller pitch, smaller curvature diameter, and less viscous fluid led to a better enhancement. The intensification factor was in the range of 1 ∼ 1.8, corresponding to the Dean number range of 5 ∼ 30. Considering the energy consumption, the values of modified intensification factors were lower than 1 only when the Dean numbers were smaller than 8. Finally, the performance of four curved geometries: helically-wound, 90-degree bend, meander-shaped, knotted were compared. The presented model yielded new insights into the liquid–liquid exaction enhancement in the curved membrane contactors.
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CHEMOSPHERE
·
2021
·
IF 7.086
Jingju Cai,Jinxin Xie,Qizhan Zhang,Minghua Zhou
A flow-through system was constructed for 2,4-dichlorophenoxyacetic acid (2,4-D) degradation for the first time using efficient boron and cobalt co-doped TiO 2 nanotubes (B, Co-TNT) as the anode and carbon black doped carbon felt (CB-CF) that had a high H 2 O 2 yield as the cathode. Compared with dimensionally stable anode (DSA), whether in anodic oxidation (AO) or AO-electro-Fenton (EF) system, 2,4-D degradation in B, Co-TNT anode system was more efficient accompanying with a lower energy consumption (Ec). Different operating parameters including applied current density, initial pH and flow rate were explored, supporting that the optimal Fe 2+ dosage was 0.5 mM while decreasing the initial pH and increasing the current intensity and flow rate were beneficial to 2,4-D removal. In this AO-EF system, the involved mechanisms for 2,4-D degradation were anodization and Fenton oxidation, possessing the comprehensive effect of • OH and SO 4 •- with their contribution of 92.7% and 4.8%, respectively. This flow-through AO-EF system performed a stable performance, and an efficient degradation performance with low Ec (5.8–29.5 kWh (kg TOC) −1 ) was obtained for different kinds of contaminants (methylene blue, phenol, p -nitrophenol and sulfamethazine). Therefore, B, Co-TNT anode coupled with CB-CF cathode in flow-through system was effective for contaminants degradation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Mengyue Li,Yi Zhai,Xubin Zhang,Fumin Wang,Guojun Lv,Mengyao Li,Qing Zhang,Yongkui Liu
It is of great significance to develop a novel strategy to synthesize hollow zeolite without using mesoporogens due to its extremely short diffusion length. Ferric nitrate as a common iron source and structure direction agent has been used for synthesizing Fe-doped zeolite. However, the effect of ferric nitrate on the morphology of zeolite has not yet been elaborated. Here, we successfully synthesized hollow MFI zeolite with a framework iron-rich surface by using ferric nitrate as an iron source and seed-assistant strategy. It is the first time to propose that inorganic iron has the hollow structure-directing effect. Herein, by comparatively investigated the effect of iron content on the structure and evolution process of hollow zeolite, a novel crystallization mechanism has been proposed based on the competitive relationship between crystallization and dissolution rates. When the Si/Fe ratio reaches 25, the internal dissolution rate of seeds is faster than the surface crystallization rate of zeolite, the hollow structures are acquired. The obtained Fe-doped hollow zeolite exhibits superior catalytic performance for the reaction of phenol degradation. In this reaction, the higher effectiveness factor (η) close to 1 of Fe-doped hollow zeolite confirmed by calculations indicates its superior mass transferability.
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EUROPEAN POLYMER JOURNAL
·
2021
·
IF 4.598
Wenjian Guo,Shuxin Bai,Yicong Ye
Although numerous efforts have been focused on the high-value-added reutilization of resin matrix in abandoned composites, the evidence chain of whether high-value-added resin pyrolysis oil can be reused has not been comprehensively presented. Herein, the epoxy resin (EP) matrix in composite wastes was pyrolyzed into EP pyrolytic oil (EPO), and its detailed composition and effects on the microstructure, strength, and ablation of remanufactured carbon fiber (CF) composites were analyzed and evaluated. According to the results, more than half (57.8 wt%) of the EP matrix was converted into EPO, which mainly included phenol and its derivatives. Given that EPO contains a certain amount of phenol derivatives, the viscosity and wettability of EPO-formaldehyde (EPOF) prepolymer with CF was slightly poorer than that of industrial grade phenol formaldehyde (PF). In addition, CF reinforced EPOF (CF/EPOF) composites with strengths and ablation rates comparable to those of CF/PF composites were fabricated successfully, owing to good process performance of the EPOF prepolymer. The present work provides a comprehensive feasibility data support and basis for high-value-added reutilization of an abandoned resin matrix composite for the manufacture of composites.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Xia Zhang,Xitong Yang,Bing Liu,Guifen Zhu,Jing Fan
An approach of simultaneous iodine doping and heterojunction fabricating with basic bismuth salt was proposed, Based on this, a novel I/BiOIO 3 /[Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O (I/BiOIO 3 /BHN) photocatalyst was prepared. The photocatalytic activity was evaluated by the degradation of multiple refractory pollutants (rhodamine B, methyl orange, phenol , bisphenol A, bisphenol B, bisphenol Z) in water under solar light irradiation. Compared with single photocatalyst, the optimized sample displayed the reaction rate constant of 0.1606 min −1 , which was 69.8, 11.4 and 2.2 times of individual [Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O, BiOI and BiOIO 3 , respectively. The performance improvement was attributed to the inhibition of charge carrier recombination by type II heterojunction formation and the expanded solar capture range caused by the springboard effect of iodine impurity level. The photocatalytic mechanism of I/BiOIO 3 /BHN was hole oxidation , followed by·OH oxidation. Besides, the I/BiOIO 3 /BHN photocatalyst in bulk structure with micrometer size and high-density could be easily separated and recovered by simple sedimentation, confirming its good application prospect in the wastewater treatment .
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Vietnam Journal of Chemistry
·
2021
·Vol. 59
·期 6
·813-822
·
IF 0
Nguyen Trung Dung,Vu Dinh Thao,Nguyen Nhat Huy
In this study, the CuCoFe-layered double hydroxide was employed for the degradation of glyphosate in water via peroxymonosulfate (PMS) activation. Scanning electron microscopy, X-ray powder diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectroscopy, and Brunauer-Emmett-Teller analyses were used to characterize the material. The effects of the catalytic system, initial solution pH, and catalyst and PMS dose on the degradation efficiency of glyphosate were investigated. The results indicated that after 6 min the CuCoFe-LDH/PMS system can degrade 99.54 % of glyphosate (100 mg/L) using 100 mg/L of CuCoFe-LDH, 200 mg/L of PMS, and pH 11. In addition, radical quenching experiments prove that the reactive oxygen species (e.g., SO 4 ●- , HO ● , O 2 ●– , and 1 O 2 ) are formed and SO 4 ●- plays a decisive role in glyphosate degradation. Moreover, the CuCoFe-LDH catalyst is reusable and stable with a glyphosate removal efficiency of 90.34 % after five continuous degradation cycles.
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ACS Nano
·
2021
·
IF 15.881
Yunyan Peng,Weiwei Zhao,Feng Ni,Wenjie Yu,Xiaoqing Liu
To achieve high solar energy utilization efficiency, photothermal materials with broadband absorption of sunlight and high conversion efficiency are becoming a fast-growing research focus. Inspired by the forest structure with efficient sunlight utilization, we designed and fabricated a graphene film consisting of densely arranged porous graphene though laser scribing on polybenzoxazine resin (poly(Ph-ddm)). This hierarchical structure significantly reduced the light reflection of graphene as a 2D material. With a combination of advanced photothermal conversion properties of graphene, the 3D structured graphene film, named forest-like laser-induced graphene (forest-like LIG), was endowed with a very high light absorption of 99.0% over the whole wavelength range of sunlight as well as advanced light-to-heat conversion performance (reaching up to 87.7 °C within 30 s under the illumination of simulated sunlight and showing an equilibrium temperature of 90.7 ± 0.4 °C). As a further benefit of its superhydrophobicity, a photothermal actuator with quick actuated response and high motion velocity, as well as a solar-driven interfacial desalination membrane with durable salt-rejecting properties and high solar evaporation efficiencies, was demonstrated.
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