SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Jie Zhong,Yong Feng,Bin Yang,Qian Xiong,Guang-Guo Ying
Modification using biochar as a carrier is a promising method to improve the activation of peroxymonosulfate (PMS) by magnetic nanoparticles. In this study, we provided an effective strategy to control the generation of oxygen vacancy to prepare N-doped magnetic biochar (NMB) by optimizing the heat treatment process of gas foaming. The NMB exhibited superior catalytic performance and stable recycling use in the activation of PMS to degrade sulfadiazine (SDZ). Through multiple characterization techniques and density functional theory (DFT) calculations, the mechanism of the reaction process about oxygen vacancy was explored for the first time in magnetic biochar. In addition, the degradation kinetics, recycling experiment, and removal of total organic carbon were carried out to evaluate the degradation performance of NMB/PMS system. After 15 min of reaction, the removal rate of SDZ reached 95.2%. After the fifth cycle of use, the removal rate of SDZ remained at 79.6%. In addition to SDZ, the NMB/PMS system could also efficiently remove ofloxacin, reactive brilliant red, and bisphenol A, suggesting excellent degradation reactivity for different types of pollutants. The oxygen vacancy was found to play an important role in the catalytic process probably through changing the electronic structure of the NMB catalyst and thereby activating the charge transfer to participate in the degradation. The results from this study might deepen the understanding of the activation mechanism driven by magnetic biochar and provide insights into the development of low-cost wastewater treatment technologies.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Xinxin Long,Chuanping Feng,Shengjiong Yang,Dahu Ding,Jinpeng Feng,Meng Liu,Yang Chen,Jihua Tan,Xingjie Peng,Jinan Shi,Rongzhi Chen
Oxygen atoms with lone pair electrons have been used to improve the photocatalytic activity of graphitic carbon nitride (g-C 3 N 4 ). Herein, a one-step annealing strategy without co precursor is used to prepare O-doped graphitic carbon nitride (OCN) for photocatalytic degradation of bisphenol A (BPA). The band structure and photocatalytic performance are tuned by simply controlling the heating time. The degradation rate constant for OCN6 is improved by 29 times compared to the original CN. Experimental and the density functional theory calculated results prove that the doped-O is the key factor in promoting photocatalytic performance. The introduced O not only adjusts local electron density, but also decreases the band gap to boost e - transfer and carrier generation and separation. The elevated conductive band energy is responsible for producing O 2 ∙ - , which is the dominated reactive oxygen species. This work offers a simple and effective way for the self-modification of metal-free catalysts to resolve environmental issues.
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JOURNAL OF CHROMATOGRAPHY A
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2022
·
IF 4.601
Yan Wu,Kaixing Luo,Yanjuan Liu,Wei Chen,Zhengwu Bai,Sheng Tang
Developing a versatile stationary phase to achieve the purpose of efficiently separating various target analytes is of great significance. In this work, ureido/dodecyl dual-functionalized silica (Sil-Ur-DD) was synthesized and employed as a new mixed-mode stationary phase for high-resolution chromatographic analysis. It was observed that multiple interactions, including hydrophobic, hydrophilic, hydrogen bonding, electrostatic and π-π interactions, contributed to the retention. Nucleosides and nucleobases could be effectively determined in hydrophilic interaction chromatography mode, and the separation performance of the Sil-Ur-DD was found to be even superior to that of the commercial XAmide column. Environmental endocrine disruptors, including alkylphenols, bisphenols, steroid hormones and phthalates, were more favorably separated in reversed-phase chromatography mode with highly aqueous mobile phases compared with the commercial C18-silica column. The experimental results indicated that the combined effect of ureido and long-chain alkyl groups obviously enhanced separation efficiency and selectivity. More significantly, the proposed method concerning the preparation of an efficient separation material with powerful separation ability is economical and environmentally friendly, which provides a proven and effective way for the recycling and utilization of the discarded chromatographic packing materials, thereby showing a good application prospect.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wenwei Feng,Yousef Faraj,Yuan Yan,Yaoxiao An,Ruzhen Xie,Bo Lai
The design of a high-efficiency and ecofriendly persulfate (PS) activator with low cost and superior performance in water decontamination still remains a big challenge. Herein, we report a facile strategy for the synthesis of novel pyrolusite-templated mesoporous catalyst (PMC), and used it as a green PS activator for the outstanding removal of bisphenol A (BPA) in water. The N2 adsorption–desorption curves and SEM-EDS images show that pyrolusite templating can successfully modulate the mesoporous structure of the catalyst; the XRD and XPS spectra indicate that pyrolusite templating renders the catalyst with enriched active sites and faster electron transfer. The mechanism studies suggest that both the radical and nonradical pathway [singlet oxygen (1O2)] contributed to BPA degradation, and 86.81% of the total organic carbon (TOC) of 100 mg/L BPA was removed using merely 0.4 g/L PMC, without detectable metal ion leaching. This work provides a new strategy for the structural design and property adjustment of an efficient persulfate catalyst for green environmental remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Zenglong Wu,Wenkai Song,Xiangwei Xu,Jiangnan Yuan,Weiyang Lv,Yuyuan Yao
Applicating co-catalyst into Fenton-like advanced oxidation processes to improve the performance for wastewater remediation has attracted widespread attention. Among them, developing highly active and green heterogeneous catalyst integrating homogeneous ferrous ions and inorganic co-catalyst is a great challenge. Herein, ascorbic acid additive was creatively introduced into the precursor composed of thiourea, sodium molybdate and ferric chloride to synthesize carbon intercalated molybdenum disulfide anchoring iron (C-MoS 2 @Fe) by a simple one-step hydrothermal method. C-MoS 2 @Fe exhibited an amazing apparent first-order constant as high as 0.739 min −1 about 10 times higher than that of the homogeneous Fe 2+ /MoS 2 system for the sulfamethoxazole (SMX) removal and achieved 68.7% removal of TOC in 6 min, which was attribute to the synergistic enhancement of high 1T phase (82.0%) and sulfur vacancies induced by the introduction of ascorbic acid. Notably, the C-MoS 2 @Fe was also capable of efficiently degrading multiple organic contaminants such as pharmaceuticals, phenolic compounds, and organic dyes. Compared with the homogeneous Fe 2+ /PMS system, the C-MoS 2 @Fe/PMS system expanded the effective pH range (2.0 ∼ 9.0) and the ultralow iron ions leaching (0.204 mg L -1 ) avoided the formation of iron containing sludge. The results of electron paramagnetic resonance (EPR), radical quenching and probe experiments indicated that •OH was the main active species with the contribution rate about 60.3%. Furthermore, possible degradation pathways were proposed based on the intermediate products of SMX investigated by LC-MS. This study provides novel insights for the development of highly active and green catalysts for wastewater remediation.
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CHINESE JOURNAL OF POLYMER SCIENCE
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2022
·Vol. 40
·期 3
·310-320
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IF 3.815
Duan Zheng-Yu,Wang Yan-Yan,Pan Qi-Wei,Xie Yun-Feng,Chen Zhi-Yong
Microporous organic polymers with high surface area are widely used in many applications. Among them, hypercrosslinked polymers have been extensively concerned because of their simple processes and low-cost reagents. However, due to most state-of-the-art strategies for HCPs based on condensation reactions, the release of small molecules such as hydrochloric acid and methanol involved in such strategies brings about new hazards to environment. Herein, we propose a method of fabrication of hypercrosslinked polymers via self-addition polymerization of divinyl benzene and its crosslinking with polar aromatic molecules. The hypercrosslinked polyDVB-based products are demonstrated by Friedel-Crafts addition reaction of double bonds on DVB that can connect adjacent phenyl rings of aromatic molecules to form the crosslinked networks. The HCPDVB-CB obtained in 1-chlorobutane as solvent has a high micropore content and displays high surface area up to 931 m 2 /g. Following this finding, DVB is used as a novel external crosslinker for knitting polar aromatic molecules. When L-phenylalanine and bisphenol A are used as the aromatic units, the obtained HCP(Phe-DVB) and HCP(BPA-DVB) could reach surface area of 612 and 471 m 2 /g, and have hydrogen uptake of 0.62 wt% and 0.58 wt% at 77 K and 1.13 bar by comparison with HCPDVB-CB having hydrogen uptake of 0.30 wt%, respectively.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2022
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IF 4.383
Bing Xiao,Minghao Xu,Bin Lu,Yun Wang,Hui Liu,Rufen Chen
Economical elimination of organic pollutants from waste water has be paid more attention owing to its environmental and ecological significance. In this study, an easily achievable process to in-situ fabricate copper and co-modified Z-scheme BiOCl/Bi 2 O 3 heterojunction was proposed. The study on the formation mechanism indicated that the introduction of copper ions is favorable for the formation of Bi-based catalyst with flaky morphology while the addition C-dots makes the nanosheets loosely be packed and intercrossed each other. The composite exhibited a high degradation efficiency for Bisphenol A (BPA) and 91% of BPA was removal within 35 min under xenon lamp irradiation. The excellent photocatalytic performance was attributed to the synergistic effect of the in-situ formation Z-scheme BiOCl/β-Bi 2 O 3 heterojunction, multiple charge transfer channels including Cu 2+ /Cu + and C-dots, and efficient charge separation. The electron paramagnetic resonance (EPR) analysis and quenching tests revealed that O 2 •− play a main role in degradation of BPA. Based on the experimental results, the photo-catalytic mechanism is proposed and the degradation path of BPA is revealed.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Zizhao Qian,Yuanxiang Xiao,Xujun Zhang,Qing Li,Lujie Wang,Feiya Fu,Hongyan Diao,Xiangdong Liu
Bisphenol A (BPA) is the main precursor in the synthesis of epoxy resins. However, because of its toxic and nonrenewable nature, BPA is unsuitable in the sustainable preparation of epoxy resins. In contrast, Diphenolic acid (DPA) is renewable but its carboxyl group limits its applications in bio-based thermosets. In this study, we report a novel amidation route to tailor DPA to produce epoxide monomers that present epoxy resins with a high performance. The diphenolic amides exhibited very low toxicities when compared with that of BPA, and also provided an unexpected autocatalytic effect on the curing reactions when succinic anhydride (SA) was used as the hardener. Dynamic mechanical analyses (DMA) and tensile test results confirmed the remarkable thermomechanical properties of the cured epoxy resins, which may be attributed to the increased cross-linking density and enhanced hydrogen bonding by the amide groups. Among the SA-cured epoxy resins, diglycidyl ether of diphenolic ethylamide exhibited the best performance, which included a high T g of 114 °C, char yield (CY) of 20%, tensile strength of 60.2 MPa, and toughness value of 185 MPa. In addition, the DPA-derived epoxy resins have great potential in the preparation of bio-based composites because they act as excellent interfaces between the resin and cotton fibers (CoFs). Our study presents a new strategy to prepare bio-based epoxy resins with a high performance, emphasizing the greater potential of amidated DPA derivatives to replace BPA in the epoxy resin market.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Wenwu Zhou,Bing Yang,Guo Liu,Chenmin Xu,Qiuyi Ji,Weiming Xiang,Dunyu Sun,Qiang Zhong,Huan He,Liu Yazi,Zhe Xu,Chengdu Qi,Shiyin Li,Shaogui Yang
Employing perylene diimide supermolecule (PDI) as metal-free cocatalyst, a novel PDI/g-C 3 N 4 /Bi 2 WO 6 (PCB) photocatalyst was constructed for the effective degradation of antibiotics. Both the photocatalytic activity and photostability of g-C 3 N 4 /Bi 2 WO 6 (gCB) were further improved after loading PDI. Under simulated sunlight illumination, the apparent rate constant of tetracycline (TC) degradation by PCB reached 2.6 times that of gCB. The photocatalytic activity of PCB still kept over 80% after 4 cycle experiments, while gCB only remained around 21%. The superior activity of PCB was ascribed to the synergism between the extended visible light absorption range through the participation of PDI cocatalyst and facilitated gCB-to-PDI photoelectron transfer. TC would finally be transformed into non-toxic ring opening products and mineralized. This work demonstrated that PDI was an excellent metal-free cocatalyst and exhibited great potential to boost the activity of photocatalysts.
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高影响因子
RSC Advances
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2022
·Vol. 12
·期 8
·4550-4561
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IF 4.036
Yun Liu,Haihua Yang,Tao Chen
It is highly desirable to explore efficient catalysts for reducing toxic Cr6+ to benign Cr3+ under mild and eco-friendly conditions. This article describes a facile fabrication of nitrogen doped carbon (N@C-g-C3N4) as a metal-free catalyst for Cr6+ reduction using lignin as a carbon source and g-C3N4 nanosheets as a nitrogen source. The structural properties of the N@C-g-C3N4 catalyst are characterized by TEM, HR-TEM, XRD, TGA, Raman, EDS-mapping, XPS and BET techniques. The summation of these analyses sheds light on the high surface area (903 m2 g−1), mesopore size (17.3 nm) and defects (ID/IG = 0.97) of N@C-g-C3N4, which contribute to its excellent catalytic activity in HCOOH-mediated reduction of Cr6+ to Cr3+ with high rate constant (2.98 min−1) and turnover frequency (2.21 molK2Cr2O7 gcatalyst−1 min−1) and complete degradation (100%) within 5 min. The catalytic performance of the catalyst reveals that the reduction activity is significantly dependent on the concentration of Cr6+ and HCOOH, catalyst loading, pH, temperature, and foreign ions. Particularly, the N@C-g-C3N4 catalyst shows superior stability and renewability with little loss of activity (≥95%) after 8 months storage and five repeated uses. Furthermore, N@C-g-C3N4 can be applied in other hydrogenation reactions involving K3[Fe(CN)6], 4-NP and BPA using NaBH4 as a hydrogen donor, and the removal of organic dyes. These findings illustrate that N@C-g-C3N4 as a metal-free catalyst is effective, versatile and eco-friendly for the reduction of Cr6+ from contaminated environments.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Abdul Latif,Ahsan Maqbool,Runzhan Zhou,Muhammad Arsalan,Kai Sun,Youbin Si
This study represents one of the first attempts towards bisphenol A (BPA) degradation by Trametes versicolor laccase immobilized on Ba-alginate beads. The effect of input variables including temperature (20–40 °C), BPA concentration (2–10 mg/L) and time (10–90 min) were studied using Box-Behnken design (BBD) and artificial neural network (ANN). The maximum BPA degradation of 84.34% was obtained when the temperature was 40 °C, BPA concentration 2 mg/L and time 50 min, which was accurately predicted by BBD (83.48%) and ANN (84.33%), proving the accuracy of prediction for both models. The values of R 2 and MSE for BBD were found to be 0.98, 9.88, while for ANN were 0.97, 38.25, respectively. Based on higher R 2 value and lower MSE, BBD was slightly better than ANN. The immobilized laccase showed higher storage stability than free laccase by retaining 68.64% and 44.62% of their activity at the same experimental conditions. Furthermore, BPA transformation was confirmed by Fourier-transform infrared spectroscopy (FTIR) analysis. GC-MS had detected the oxidative degradation products from BPA. Results showed that Ba-alginate immobilized laccase could be a promising biocatalyst in treating organic pollutants .
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ACS ES&T Water
·
2022
·
IF 0
Yibing Sun,Hongchao Li,Shengli Zhang,Ming Hua,Jieshu Qian,Bingcai Pan
Heterogeneous peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are under extensive investigation for their great potential in water remediation. The understanding of the PMS activation mechanism is crucial but still debatable. Here, we describe a thorough investigation of the mechanism involved in PMS activation by using molybdenum disulfide (MoS2) as a catalyst. This MoS2/PMS system exhibited intriguing target-dependent reactivity. Further comprehensive experimental results excluded the major contributions of various possible species, including HO•, SO4•–, O2•–, 1O2, homogeneous Mo(VI), and heterogeneous Mo(VI). We then proposed a surface ≡Mo–OOSO3– complex as the major reactive species, while SO4•– derived from the decomposition of ≡Mo–OOSO3– acted as the secondary reactive species for pollutant removal. This complex could oxidize pollutants through the oxygen-atom-transfer mechanism and perform both nucleophilic and electrophilic attacks. This work provides novel perspectives for the mechanistic understanding of heterogeneous PMS-based AOPs for water remediation.
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